Progress in Energy and Combustion Science 37 (2011) 422e461

Contents lists available at ScienceDirect

Progress in Energy and Combustion Science

journal homepage: www.elsevier.com/locate/pecs

Review

Thermographic phosphors for thermometry: A survey of combustion applications

Marcus Aldén, Alaa Omrane, Mattias Richter*, Gustaf Särner
Department of Combustion Physics, Lund University, P.O.BOX 118, 221 00 Lund, Sweden

a r t i c l e i n f o a b s t r a c t

Article history: Temperature is a fundamental thermodynamic parameter used to describe physical, chemical and biological
Received 10 April 2010 processes. In combustion as in many other applications, knowledge about temperature plays a substantial role
Accepted 13 July 2010 in helping to maintain an efficient and clean environment. Being able to measure temperature accurately in
Available online 28 September 2010
combustion and in fire-related applications is important for giving a better understanding of heat transfer
phenomena and improving existing models.
Keywords:
In the present review paper a method based on the spectroscopy of inorganic luminescent materials is
Thermographic
described and exemplified in experiments related to combustion. The method involves the use of
Phosphor
Laser
thermographic phosphors which enable remote temperature diagnostics to be performed with a high
Surface degree of sensitivity and accuracy. The technique is superior to those based on thermocouples and
Temperature pyrometry, particularly in the vicinity of flames and when the measured surface is subjected to random
movements. Several phosphor materials suitable for temperature probing are described. The application
of thermographic phosphors to temperature measurements in one-point and in two-dimensions in flame
spread scenarios, and in pyrolysis experiments involving different construction materials and polymers
are described. Many thermographic phosphors have the property of being insensitive to variations in
pressure up to 1 GPa. This property extends the use and development of thermographic thermometry to
other domains, such as internal combustion engines. The temperature has been measured in a point and
in two-dimensions inside the combustion chamber. The complex procedures required to implement the
use of thermocouples on moving objects inside an engine make thermocouples an expensive choice. It
also limits the possibilities of altering the measurement locations and thereby also complicating the
investigation of different engine geometries and components.
Thermographic phosphors have also been employed in gas turbine applications. Temperature probing
in the afterburner of a full-size aircraft engine is described with the aim to study the effects of various
engine loads on the wall temperature. Furthermore, the application of thermographic phosphors to study
the temperature of droplets in relation to sprays is described. In spray dynamics, temperature is a crucial
parameter for gaining an understanding of atomisation, evaporation and heat convection from the
surrounding gases. Finally the application of thermographic phosphors for gas temperature measure-
ment by seeding the particles into a gas flow is described together with the challenges associated with
seeding the particles for in-situ flame measurements.
Ó 2010 Published by Elsevier Ltd.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 423
2. Thermographic phosphors (TP) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 424
3. Thermometry methods using TP . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 426
3.1. Lifetime methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 426
3.2. Lifetime evaluation using amplitude-modulated light sources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 427
3.3. Spectral intensity ratio method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 427
3.4. Sensitivity improvements of the ratio method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 428

* Corresponding author. Tel.: þ46 462224565; fax: þ46 462224542.

E-mail address: mattias.richter@forbrf.lth.se (M. Richter).

0360-1285/$ e see front matter Ó 2010 Published by Elsevier Ltd.

doi:10.1016/j.pecs.2010.07.001
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 423

4. Different thermographic phosphors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 428

4.1. YAG:Dy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 430
4.2. YAG:Tb . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 431
4.3. La2O2S:Eu . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 431
4.4. Y2O3:Eu . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 432
4.5. Y2O2S:Sm . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 432
4.6. YVO4:Dy . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 432
4.7. Mg4FGeO6:Mn . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 432
4.8. BaMg2Al10O17:Eu . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 432
4.9. Y2SiO5:Ce . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 433
4.10. LuSiO5:Ce . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 433
4.11. (Sr,Mg)2SiO4:Eu . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 433
4.12. ZnS:Ag . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 434
4.13. YALO3:Ce . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 434
4.14. CdWO4 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 435
4.15. ZnO:Zn . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 435
4.16. ZnO:Ga . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 436
4.17. Up-conversion phosphors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 436
4.18. Binder materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 436
5. Applied measurements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . .437
5.1. Flamespread and fire protection . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 437
5.1.1. One-point temperature measurements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 437
5.1.2. Two-dimensional temperature measurements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 439
5.1.3. Applications to intumescent paint . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 440
5.2. Pyrolysis of decomposing materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 441
5.3. Thermographic phosphor thermometry in a gas turbine afterburner . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 443
5.4. Droplets and sprays . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 445
5.5. Internal combustion engines . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 450
5.6. Additional applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 455
5.6.1. TP on a heated plate . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 455
5.6.2. TP on a moving target . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 455
5.6.3. Measurements through diffusive scattering in solid materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 456
5.6.4. Free flow applications . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 456
6. Conclusion and outlook . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 458
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 458
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 458

1. Introduction of using CFD and/or modelling the appropriate chemical kinetics

which have made considerable progress as the computing power
Combustion has for a long time been the major source of energy has increased. Another approach is to use advanced optical diag-
for heating, transportation and production of electricity. It will nostic techniques to characterize the combustion process. The
surely remain so in the foreseeable future as well, despite the advantages with these techniques are their inherent non-intru-
attempts that are made to find and to develop new energy sources. siveness in combination with high temporal and spatial resolution.
In a world of increasing energy needs and rapidly diminishing oil Various techniques have been developed for measurements of
resources, it is of increasing importance to make combustion more species concentrations, temperatures and velocities, see e.g [1e3].
effective. In particular temperature is one of the most frequently measured
A challenge of today is to increase the efficiency of processes parameter in a wide variety of combustion applications. It enables
involving combustion in order to decrease the carbon dioxide a trade-off to be made between efficient combustion and pollution
emission Further challenges are to optimize combustion properties reduction. Traditional techniques for measuring temperature such
when new fuels are to be combusted, e.g. biomass and renewable as those relying on thermocouples or pyrometry suffer from certain
fuels. Also combustion processes produce various kinds of pollut- serious limitations. Thermocouples in combustion applications are
ants, e.g. unburnt hydrocarbons, nitrogen oxides and soot are some not only intrusive but prone to a multitude of possible errors,
of the pollutants that are hazardous both for the environment and including those of radiation, conduction along the wires, catalytic
for human health and which must be minimized. Legislations effects and the slow response. Pyrometry is a non-contact sensing
during the last few decades in particular have regulated pollutants, method based on measuring the naturally emitted electromagnetic
forcing the combustion industry to develop means of lowering radiation by all objects. In combustion applications, emissivity
emissions. In order to be able to build better combustion devices variations stemming from walls and flames and absorption by gases
and to remedy in various ways the drawbacks of existing tech- and soot, become inevitable making the results questionable. The
nology, it is necessary to gain a better understanding of combustion present paper reviews research directed towards an alternative
processes. During the last decades two different but complemen- measurement technique based on the use of temperature sensitive
tary ways of gaining a deepened knowledge of combustion phosphors known as (thermographic phosphors) for temperature
phenomena have been developed. One way is to apply advanced measurements in various combustion environments as well as in
modelling approaches, e.g. modelling of turbulent flows by means related areas, e.g. sprays.
424 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Phosphor materials have a long history of use in modern society.
The first documented occurrence of a phosphorescent material is
dated back to the 17th century. An alchemist in Bologna, by the
name Vincetinus Cascuarolo, found a strange, heavy crystalline
stone and discovered that it emitted red light when exposed to
sunlight. Following this, other findings of similar nature were
made, the stones being referred to as phosphors, the Greek name
for “light bearer”. Although phosphors were known that early and
rare-earth elements were discovered at the end of the 18th century,
the development of thermographic phosphors and rare-earth
materials did not become very active before about 1930e1940,
when a strong industrial interest in the commercialisation and
development of them in connection with mercury lamps was
awakened. Thorington [4] found when studying the temperature
dependence of excitation and emission spectra of magnesium
doped with manganese, that adding fluorine to the host material
improved the efficiency of the phosphor by a factor of three.
Bradley [5] employed phosphor thermometry in wind tunnel tests
by monitoring a thermographic phosphor emission intensity.
In modern times, use of the term “light bearer” has been com-
plemented by a more stringent definition of the concept of phos-
phors. A phosphor is now considered to be a “solid luminescent
material” or a “powder synthesized for purpose of practical appli-
cation” [6]. Phosphorescence, or the emission of radiation, is
defined, however, as an extended afterglow following excitation,
one that originates from a quantum mechanically forbidden tran-
sition. The emission can last up to several hours, a very long duration
as compared with that of fluorescence. Some materials designated as
phosphors can, however, have very short emission lifetimes, down
to picoseconds. The physical explanation of phosphorescence is very
similar to that of fluorescence, namely of its originating from
a radiation emitting transition of excited electrons to a lower energy
level in the molecules or atoms in question. The only difference
between the two is that phosphorescence originates from a triplet-
to-singlet transition, causing the long emission lifetimes, whereas
fluorescence originates from a singlet-to-singlet transition [6].
Phosphors have traditionally been used in such everyday applica-
tions as fluorescent-tube lamps, CRTetelevision sets and fluorescent
paint. Today when the Edison light bulb is considered to be too
inefficient, phosphors have become increasingly important for the
shift in radiation spectra they produce in fluorescent-tube lamps
and in LED-lamps, which are able to serve as more efficient light
sources with the desired emission colour shade.
Although the temperature dependence of phosphors was
discovered in the 1950s, it took more than 20 years before
a genuine interest in thermometry in which phosphor particles
were employed. Such interest was encouraged by the availability of
new tools e.g. lasers and optics which helped accelerate the
development of thermographic phosphors thermometry. In
1978e1980, the first applications in biology [7e9] appeared.
During 1980s, scientists (Cates and Allison [10e13] and Bugos et al.
[14e16]) realised the potential of the technique in connection with
moving surfaces and also pushed for its further use for measuring
high temperatures [17]. During the 1990s several publications in
the area appeared, mainly related to gas turbine [18e23] and fibre
optic applications [24e27]. After more than a decade of using
thermographic phosphors for the remote sensing of temperatures,
Allison and Gillies [28] published a review article in which they
summarised their very extensive work they had conducted in the
area. This article serves today as a valuable source of information on
different thermometric methods utilising thermographic phos-
phors. Recently, new complex fibre temperature probes have been
gaining increasing interest [29e33]. Finding new thermographic
phosphors based on nanoparticles is of particular interest [34e36].
The development of thermographic phosphors now continues
because of the expanding use and development of rare-earth
materials for various applications [37].
During recent years the technique has become an important tool
also in combustion applications and related phase-changing
processes, e.g. droplets, sprays and pyrolysis. Today laser-induced
phosphorescence has thus become an established technique for
obtaining temperature measurements with very high precision in
both one-point and 2D mapping in a wide range of applications. A
variety of approaches to phosphor thermometry can be used
depending upon the situation and the temperature response
a particular phosphor shows. Different methods that are available, as
well as the properties of a number of thermographic phosphors are
addressed in this paper. In this context the authors would also like to
refer to another review article on thermographic phosphors to
appear [38].
After a detailed description of physics related to phosphores-
cence, the various approaches for thermometry are outlined after
which various different applications are reviewed.
2. Thermographic phosphors (TP)
The rare-earth elements (RE), divided into the Lanthanides and
Actinides, are a group of elements that display remarkably similar
chemical and physical properties and were discovered as early as in
the late 18th century. Almost 100 years later, the luminescence
obtained from them was observed for the first time, applications
based on these materials being born.
Rare-earths ions are characterised by their distinct spectra and
spectral lines. When doped in a crystal, the rare-earth emissions
appear as sharp spectral lines, due to the transitions in the 4f shell
being unaffected by perturbations of the crystal. The various rare-
earth ions differ in the number of electrons in the 4f shell. Although
the numbers differ from one rare-earth to another, variation only
occurs in the inner shell, 4f. Since all of the rare-earths have three
electrons in the outer shell they are regarded as chemically similar.
Since the transition metals and the rare-earth elements have
inversion symmetry, Laporte’s selection rule states that transitions
between states of the same parity only occur on the basis of
a magnetic dipole process. The rule forbids the electric dipole
transitions usually observed as sharp radiative transitions in the case
of RE. The fact that the electric dipole transition that is forbidden
occurs, may be related to the lack of inversion symmetry, which in
turn favours a mixing between states of 4f(n1)5d and 4fn. The mixing
is usually small in magnitude but the resulting electrical dipole
transition is usually five times as strong as the allowed magnetic
dipole transition. The permanent occurrence of the electrical dipole
transition within forbidden states, even when the ions occupy
a centre of inversion symmetry, implies that a small distortion or
perturbation usually occurs close to rare-earth ions in the crystal
field, which in turn either influences or destroys the inversion
symmetry. The distortion is so small, however, that it has no
significant effect on the energy levels of the rare-earth elements. The
metal elements, because of their strong coupling to the transitions
occurring in the crystal, are more strongly influenced by the lack of
symmetry in the lattice and the distortion of it. For the rare-earth
ions, only magnetically based dipole transitions are allowed if the
host material is considered to have an inversion symmetry. In the
crystal, the neighbouring ions can affect this rule so that it becomes
slightly relaxed. The electric dipole transition is then allowed due to
the intermixing (e.g. 3d(n1)4p and 3dn) of opposite components of
the crystal field and due to the interaction between the eletronic and
the vibrational wave functions, known as vibronic coupling. Many
researchers have become interested in better understanding the
unusual behaviour of rare-earth elements in a crystal field. The
JuddeOfelt theory [39,40] is one of the most successful methods of
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
calculating the radiative transition probabilities between different
energy levels of a rare-earth element. It has contributed very much
to prediction of the observed radiation intensities, and of radiative
and non-radiative lifetimes [41,42,45]. The line strength and spon-
taneous emission of an electrical dipole is given as [41];
X i gi expðDE=kTÞ
2
Sed ¼ e2 Ul j < ikU ðlÞ kf > j
l ¼ 2;4;6
64p4 e2 s3 c X
Aed ¼ Ul j < ikU ðlÞ kf > j2
3hð2J þ 1Þ
l ¼ 2;4;6
where Ul is the intensity parameter characterising the strength and
the nature of the odd-parity crystal field, U(l) is the unit tensor
operator, s3 is the average transition frequency, and c is a correc-
tion factor for the refractive medium of the lattice. The spontaneous
emission line strengths originating from magnetic dipole transi-
tions can be given as [41];
4p2 e2 s3 n3 h
Amd ¼ j < ikL þ 2Skf > j2
3m2 c2 ð2J þ 1Þ
where h is Planck’s constant, n is the refractive index of the
medium, and m is the mass of the electrons. The total radiative
lifetime is deduced from Eq. (3) and Eq. (2) as follows;
1
srad ¼ ðAed þ Amd Þ
Weber [41] compared the modelled radiative lifetime and the
experimentally measured lifetime. The difference was attributed to
multi-phonon decay contributions. Since non-radiative decay of an
excited state through phonon emission dominates when the frac-
tional rare-earth concentration is less than 1%, the ion-ion inter-
action, although possibly still found, would be very moderate. The
phonon decay rate in different crystal hosts has been investigated
thoroughly in a number of studies [41,42,44e48]. In crystals it has
been observed spectroscopically that light emission between two
levels fails to occur when those are sufficiently close to each other.
This minimum gap is known to be very host dependent. When the
crystal lattice vibrates with a frequency proportional to the energy
difference between two levels, de-excitation within a one-phonon
scheme can occur. When the energy gap increases and become
greater than the maximum phonon energy in the material, emis-
sion through several phonons is necessary in order for the energy to
be conserved. In several studies the dependence of multi-phonon
emission on the energy-level gap has been observed and has been
shown experimentally to follow an exponential form [41e45]. The
spontaneous phonon emission occurring is given as a function of
the energy gap;
Wo ¼ bexpðaDEÞ
where b and a are constants characterising the crystal. When the
band gap increases the probability of spontaneous phonon emission
decreases. At the same time, the radiative emission increases when
the energy difference becomes greater. The rate of multi-phonon
emission is very host dependent because of the various vibrational
spectra found in the host lattice, the different phonon frequency
distributions that are present and the coupling between the dopant
and the crystal host. For rare-earth ions found in crystals, the average
rate is around 500 cm1, whereas for glass materials [43] the rate is
much higher [700e1400 cm1 . Riseberg and Moos [44] have
investigated the dependence of the multi-phonon relaxation of
different rare-earth ions found in crystals on the temperature and on
the energy band gap. The temperature dependence of the multi-
phonon emission rate is given by [44]:
425
 p
expðZui =kTÞ
Wi ðTÞ ¼ Wo (6)
expðZui =kTÞ  1
P
i Wi gi expðDE=kTÞ
P
W ¼ (7)
(1)
where Wi and gi are the individual decay rate and the degeneracy of
the ith level, respectively. DE is the energy separation between the
ground level and the excited state, and p denotes the phonon order,
(2) involving the numbers of phonons undergoing the transition. This
model takes into account all the rates at the separate levels, induced
by the Stark effect. Good fits to the observed temperature dependence
have been claimed for use of this model. As the temperature in the
solid rises, the vibrational energy of the lattice increases, magnifying
the modulation of the crystal field. The stronger the modulation of the
crystal field is the higher the probability is for non-radiative transi-
tions, with an accompanying decrease in quantum efficiency h ¼ Arad/
(Arad þ W). For transition metals, because of their strong interaction
with the lattice, the temperature can also induce small changes in the
(3) energy levels, resulting in a temperature-dependent shift. The total
lifetime of an excited state (i) in the transition to a lower state (j) can
be deduced by use of both the radiative (Eq. (4)) and non-radiative
(Eq. (6)) emission probabilities.
X 1
si;total ¼ Aij;rad þ Wij (8)
(4) j
where Aij and Wij are the probability of radiative and of non-radiative
decay, respectively. The lifetime of the excited state (i) is summed
over all the terminal states (j). This lifetime is the one measured for
thermographic phosphors in assessing the temperature.
The charge transfer state (CTS) is an intersystem energy band
connecting the host lattice with the dopant ion directly. For ions with
a strong electron affinity, such as trivalent lanthanides Eu3þ and Yb3þ
[49], this band can be found at very low energies 40,103 cm1.
Luminescence from a metal ion can originate not only from the 4f(n)
states but also from the CTS and 3f(n1)5d(1) states, which are optically
permitted. Most research concerns the attempt to gain a better
understanding of the 4f(n) levels. Interest in the luminescence from CTS
and 3f (n1)5d(1) has also been increasing recently [50]. Since the CTS in
the Eu-ions is close to the 4f state, an intersystem crossing takes place,
no luminescence from the CTS occurs. Fonger and Struck [51] have
studied the CTS and its effect on the luminescence of Eu3þ-ions. When
the charge transfer state absorbs UV light efficiently, relaxation occurs
non-radiatively, to the lowest energy level of CTS, where it feeds the DJ
states, D0 in particular. The transition from the D0 state to the ground
states FJ occurs radiatively. As the temperature increases, higher energy
levels of the excited states DJ can be populated, so that the crossover
point to the CTS is reached where rapid thermalisation to the lowest
(5)
energy state D0 occurs. Consequently, the quenching temperature of
the DJ states increases as J ¼ 3,2,1,0 decreases [51,52].
There is no charge transfer state for the divalent lanthanide Eu2þ
due to its low electron affinity. Its luminescence behaviour is
strongly influenced by the 4f65d1 state, which is the closest excited
state at the 4f level. Its spectrum is broad and is highly dependent
upon the host material involved. Europium activated barium
magnesium aluminate (BaMgAl10O17:Eu2þ) is a thermographic
phosphor with these characteristics which has been investigated,
see below.
More information regarding the relationship between the CT
and 5d states for various rare earths is given in [53] where it is
stated that the overlap, or separation, of intershell (4fe5d) and
charge transfer spectra of trivalent rare earths depend upon
properties of the host, not upon the rare earths themselves.
426 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
3. Thermometry methods using TP
The luminescence properties of thermographic phosphors are
very sensitive to variations in temperature. Most thermographic
phosphors exhibit a broadband absorption in the UV region and few
more narrow absorption lines in the visible region. Several methods
can be used for excitation, such as laser radiation (pulsed or contin-
uous), particle beams, chemical reactions or thermal excitation in
flames. In this review the excitation is usually performed by an
ultraviolet or a visible laser beam. Following excitation, the subse-
quent emission due to the relaxation of electrons from the excited
state to the ground state can be used for non-intrusive thermometry.
Two methods of inferring the temperature can be employed, the
temporal and the spectral method. Both methods allow one-point or
two-dimensional measurements to be performed.
3.1. Lifetime methods
As indicated above the radiation from most thermographic
phosphors has a lifetime which is dependent on the temperature.
The intensity decays exponentially and is in the most simple case
single exponential in accordance with;
I ¼ Io expð  t=sÞ;
where I0 is the initial emission intensity, t is time and s is the lifetime
time constant of the phosphorescence involved, i.e. the time taken for
the intensity to decrease to 1/e of the initial emission I0 [28]. For some
thermographic phosphors the intensity decay is not single expo-
nential depending on material molecule properties. In those cases an
expanded model of the intensity decay can be employed to assess all
lifetimes present. The phosphorescence lifetime of the phosphor
material decrease with increasing temperature, see Fig. 1. The
temperature can thus be calibrated to the lifetime or lifetimes and be
retrieved by calculating the phosphorescence lifetime(s) from the
measured decay in intensity. This is normally done by fitting the
intensity decay to a theoretical model (e.g. Eq. (9)), using a nonlinear
fitting procedure. The error in temperature in such a measurement is
ideally less than 1% [54]. When performing the calibration procedure,
a single exponential fit is often appropriate also for phosphors that
show multi-exponential features, i.e. the fit itself does not need to be
perfect as long as it provides robust results.
The lifetime method is usually employed for point temperature
measurements using a Photo Multiplier Tube (PMT) for detection.
An example of a PMT signal is shown in Fig. 1. It can also be noted
that the intensity decay of CdWO4 in Fig. 1 is very close to being
single exponential.
Fig. 1. Normalized PMT signals from CdWO4 at 294, 376 and 478 K, corresponding to lifetime constants, s, of 15.8 ms, 2.26 ms and 55.6 ns, respectively. The single exponential decay
shows a linear behaviour when logarithmic values are used on the y-axis.
Lifetime evaluation from a recorded emission decay is best
performed using least-square nonlinear fitting procedures based on
the Levenberg-Marquardt algorithm [55]. In evaluating a recorded
decay signal, it is important to isolate the part containing the
exponential behaviour. Evaluation of a signal should ideally start at
the point of maximum signal intensity. Due to occasional distur-
bances from the excitation laser pulse which penetrates the filters
that are employed, it is sometimes necessary to eliminate the first
part. If the lifetime of the phosphor is much longer than the laser
pulse, this does not introduce any significant evaluation error.
Mainly two different approaches are used to choose the endpoint of
the fitting procedure. The most common one is to fit to the point at
which the signal intensity is 1% of the initial intensity, in order to
avoid the part in which the signal to noise ratio is too small. The
other approach is to optimize the fit endpoint by iteration keeping
the endpoint within 4se10s from the beginning of the fitting range.
The signal length evaluated should in any case be longer than 4
times the lifetime constants, s. [56e58].
The length and temporal shape of the excitation pulse is of
importance when measuring short emission lifetimes. Pulsed
Nd:YAG lasers, which are the type used primarily in the reviewed
applications, have Gaussian-shaped laser pulses in the time domain.
The second half of the laser pulse thus resembles an exponential
(9) decay. When using pulsed lasers, the decay time of the laser pulse
needs to be shorter than the emission lifetime, unless a deconvolu-
tion of the laser pulse shape is made from the signal. When using an
excitation source with a square pulse, such as a pulsed laser diode or
a LED, the pulse length is of no great importance as long as the
excited state of the phosphor is not saturated and the pulse decay
time is shorter than the emission lifetime. When measuring very
short lifetimes; in the nanosecond range or below, either the phase
shift method described below or a short-pulsed laser needs to be
employed.
In addition to one-point measurements there is also a great need
of two-dimensional measurement techniques for investigating
temperature behaviour and temperature gradients in unsteady
environments, as well as to provide modellers with experimental
data (such as in connection with computational fluid dynamics, CFD)
[56,59e62]]. Lifetime based 2D-imaging in combustion using ther-
mographic phosphors was demonstrated for the first time in [63,64].
After excitation by a laser pulse the phosphorescence emission was
recorded consecutively at short time intervals during the decay
using a framing camera with eight individual detectors. The phos-
phorescence emission entering the camera was divided equally over
all the eight detectors by use of a pyramidal beam splitter. The
exposure time and the time delay between each detector could be
configured to meet the experimental needs. The time delay between
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
each CCD could be adjusted to fit the optimum of 1 < s/Dt < 5, as
discussed in Ref. [56,65], s being the lifetime and Dt the time delay
between the individual detectors. An example of the lifetime
imaging procedure is presented in Fig. 2. The intensity of the
ICCD1(x, y) detector at each pixel position (x,y) was related to the
corresponding intensity ICCD2(x, y). ICCD8(x, y) for each of the
other ICCD detectors. The lifetime and thus the temperature were
extracted using an exponential fitting procedure and fitting of the
measured decays to calibration data. The time separation between
the detectors could be adjusted to improve the accuracy of the
temperature measurements. This implies that one should have
a prior estimate of the temperature which is being investigated.
3.2. Lifetime evaluation using amplitude-modulated light sources
The exponential lifetime can be measured not only by using
pulsed light sources but also by using an intensity modulated con-
tinous wave (cw) light source. If the excitation-light source is
amplitude-modulated and is of sinusoidal shape in accordance with;
Isrc ¼ I0 ð1 þ asin UtÞcos ut; (10)
where U is the angular frequency of modulation and u is the
angular frequency of the light, an induced emission signal using
such a light source is delayed relative to the excitation radiation due
to its lifetime. This results in a phase shift relative to the excitation
modulation. At the same time when emission is delayed it also loses
contrast in terms of modulation depth see Fig. 3. The same lifetime
as calculated from an emission decay curve can be calculated from
either the phase shift or the contrast loss in the emission. This can
be derived by extrapolating from a single exponential intensity
decay to the new conditions. If it is assumed that the signal
intensity decreases single exponentially at every point, the
following expression can be calculated by integrating Eq. (10) over
the sine shaped excitation source [66,67]:
!
a
Iem ¼ bI0 1 þ qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffisinðUt þ fÞ cos ut (11)
1 þ U s2
2 obtaining the temperature [17,22,29,30,69e72]. After excitation,
where
tan f ¼ Us (12)
and 4 is the phase shift and s is the same lifetime as for the intensity
decay method [68]. The lifetime can thus be calculated either from
Fig. 2. Lifetime based imaging procedure. The lifetime is computed from the single
exponential decay at each pixel position. Exposure with a temporal overlap of 50% was
employed [63].
427
Excitation
φ Emission
1
1 + Ω2τ 2
Fig. 3. Illustration of using a modulated light source to generate a phase shifted signal
for lifetime measurements.
qffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
the loss of contrast by 1= 1 þ U s2 or from the phase shift
2
(assuming the frequency of the modulation to be much smaller
than the frequency of the light).
Utilizing this method requires the use of a continuous excitation
source which is possible to modulate, such as a laser diode or a LED.
The detector is often a PMT. The signal can either be sampled by an
oscilloscope for later processing or by the use of a lock-in amplifier.
In either case a Fourier analysis is used to determine the frequency
and phase content of the signal. It should also be possible to obtain
two-dimensional measurements using a camera trigged at a slightly
different frequency so that for every image the camera gate slides
a bit relative to the modulation. The sinusoidal shape should then be
possible to interpolate for each pixel in the successive images.
An example of using the phase shift method is shown in Fig. 4.
As can be seen the phase shift decreases as expected with
temperature. The measurements shown are performed utilizing the
phosphor (Sr, Mg)2SiO4:Eu excited by a laser diode producing
415 nm light. The laser was sinusoidal modulated at 10 MHz.
3.3. Spectral intensity ratio method
The spectral method is based on ratioing two or more lines in
the emission (Sj) from one energy state can be given as;
 
hcEj
Sj ¼ Cj Te sj I exp  (13)
kT
where Cj is the detection efficiency of the (j) transition, Te is the
exposure time of the detector, sj is the optical filter transmission,
and I is the laser pulse intensity, and h is the Planck constant, c is the
speed of light, k is the Boltzmann constant, and Ej is the energy of
the emitting state. Each of these factors can be eliminated by
dividing the intensities of two different energy states by each other
as follows:
 
Sj hcDE
R ¼ ¼ z exp  (14)
Sjþ1 kT
where R is the measured ratio, DE is the energy gap between the
two states, and z is a constant determined experimentally. Like the
temporal method, the ratio technique can also be extended to two-
dimensional measurements [22,71e75]. For this purpose, two
images corresponding to two different energy states need to be
acquired simultaneously in unsteady state measurements. One way
of doing this is to use two ICCD detectors for registering emissions
through use of a beam splitter and two band-pass filters. Here,
a calibration measurement of the light sensitivity of both ICCDs is
needed to enable the pixel intensities in the different cameras to be
balanced. Another method is to use an imaging stereoscope which
428 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

(Sr,Mg) SiO :Eu (Sr,Mg) SiO :Eu

2 4 2 4
1.1
1
1 Excitation source
0.8
0.9
0.6
Emission at 639 K
0.8 0.4
PhaseShift [rad]

Intensity / a.u.
0.7 0.2 Emission at 475 K

0.6 0

0.5 −0.2

0.4 −0.4

−0.6
0.3
−0.8
0.2
−1
0.1
450 500 550 600 650 700 750 0 0.2 0.4 0.6 0.8 1 1.2
s −7
Temperature [K] Time / s x 10

Fig. 4. Left: emission phase shift of Europium activated magnesium silicate, (Sr, Mg)2SiO4:Eu, as a function of temperature. A laser diode at 415 nm modulated with 10 MHz
sinusoidal was used as excitation source. Right: example of normalized signals for two points in the left graph. A moving average filter of 20 samples is applied to the signals shown.

uses mirrors to split the image into two identical images that can be
recorded with a single camera. An imaging stereoscope (Lavision,
GmbH, Göttingen, Germany) permitting two-colour operation by
way of image doubling is shown in Fig. 5.
The stereoscope can be adapted to the objective of an ICCD
camera. After excitation, the incoming phosphorescence emission
passes through separate filters before encountering a 45-degree
mirror and a prism. This results in two identical images of the same
object on the CCD chip. After recording of the images, both back-
ground measurement and spatial reference images are needed. The
latter, known as flat-field images, are used for correcting for the
non-uniformity introduced by the detector, the stereoscope, and
the optics employed. Since the reference images are very important
for obtaining high accuracy and precision, special care in obtaining
them is needed. A uniform light source is usually chosen for this
purpose. The reference images need then to be subtracted from the
background and be divided by the phosphorescence images as
follows:
Iphos1  B1 Ref 2
Ratio ¼ $ (15)
Ref 1 Iphos2  B2
obtained using the ratio-imaging technique (using a stereoscope)
depends on the sensitivity to temperature of the thermographic
phosphors, but in general it is found to be 5e10%.
3.4. Sensitivity improvements of the ratio method
A scheme for improving the accuracy of the ratio method by
using the temporal sensitivity in the ratio measurements, delaying
one of the cameras to the other is also possible. This would in a way
combine a spectral measurement with a temporal one. If assuming
a spectral ratio where the two emission wavelengths used having
the same lifetime, as, e.g. BaMg2Al10O17:Eu, see Section 4.8 and if
one of the camera gates is delayed a few nanoseconds this will not
yield any effect at low temperatures where the emission lifetime is
long. It will, however, give rise to a big signal difference at high
temperatures where the lifetime is short.
As mentioned before the signal emission decay can be described
by Eq. (9)
To calculate the effect of a delay in one of the signal camera
gates, a perfect exponential decay was assumed and the signal was
integrated over the two camera exposure times according to;

where I denotes the phosphorescence images, B the background, Zt2

and Ref. the reference images. The accuracy of the measurements I0 expð  t=sÞdt;
t1

where t1 and t2 are the opening and closing time of camera gate,
respectively. Using this expression on the spectral data at different
temperatures, where interference filters with rectangular trans-
mission profiles are simulated by summarizing over the filter
bandwidth, an estimation of the effect of different delays can be
simulated. The resulting sensitivity improvements are shown in
Fig. 6. The sensitivity can be increased at high temperatures at the
expense of collected signal strength.

4. Different thermographic phosphors

Phosphors can be both organic and inorganic. Phosphors having

Fig. 5. Schematic view of the stereoscope.
temperature-dependent emissions are mostly inorganic, however,
often made of some ceramic material. Thermographic phosphors are
composed of a carrier material doped with some activator material.
The activator is often a rare-earth metal. The doping concentration is
typically around one percent, which is a low enough concentration
for the activator atoms to be isolated from one other by the host
matrix. The host material is microcrystalline and mostly transparent
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Ratio of 400/455 nm for different delays of the 455 nm camera
2 Delay: 0ns
10 Delay: 10ns
Delay: 20ns
Delay: 30ns
Delay: 40ns
Delay: 50ns
Delay: 60ns
Ratio 400/455
Delay: 70ns
1
10
Delay: 110ns
Delay: 150ns
0
10
200 300 400 500 600 700 800 900 1000
Temperature / K
Fig. 6. The simulated effect of delaying the exposure of one camera when performing
spectral intensity ratio measurements on BaMg2Al16O27:Eu. The ratio of 400 nm  20
to 455 nm  5 is assumed and an exposure time of 10 ms with a start delay for the
455 nm exposure time.
to visible radiation, i.e. it is usually the activators that absorb and
emit radiation. In their isolation from each other, the activators
cannot de-excite the absorbed energy non-radiatively, i.e. most of
the de-excitation is in the form of radiation emission. When
designing an accurate temperature sensor the doping concentration
becomes a key factor since it slightly alters the photo-physical
properties of the thermographic phosphor such as line intensities
and decay times [80,81]. In general a low doping concentration
would yield a better rate. This is even more relevant, and has to be
considered when the mean particle diameter is below 1um. In
addition, since dopant concentration and particle size can influence
both decay time and spectral properties it is advised to always
perform a calibration for each new batch of phosphor material.
Most phosphors used for thermometry can be excited by laser
radiation. In an electron excitation, the energy is absorbed by the
rare-earth metal in question. The electron is then non-radiatively
relaxed to a meta-stable energy level, i.e. a level at which no tran-
sitions are quantum mechanically allowed. Accordingly to the Hei-
senberg uncertainty principle, some of the transitions that do occur
exhibit long-lived phosphorescence [83]. Not all phosphor emis-
sions have a long lifetime, however. Phosphors with an extremely
short lifetime, often used as scintillator material, however, have
transitions that are allowed.
The emission spectra of any material change with temperature,
since the Boltzmann distribution affects vibrational levels in both
the ground and excited states. The strong temperature dependen-
cies of thermographic phosphors are due to several factors, often
specific to the phosphor or the rare-earth metal ion in question. The
specific reasons for the temperature dependence of the phosphors
used in the present work will be addressed in the sections dealing
with the separate phosphors. A high temperature results, in
general, in an increase in vibrations in the crystal lattice of the host
material. This broadens the line-widths of the emitting transitions
in the phosphorescent process. Thermal expansion in the host
lattice often induces frequency shifts in the phosphorescence
spectra as well, which in some cases is useful for thermometry [28].
Thermometry using thermographic phosphors can currently be
carried out at temperatures up to about 2000 K using phosphors
known to possess temperature sensitivity. This section summarizes
several new thermographic phosphors that can be used for
429
thermometry. Special efforts have been made to find fast phosphors
having blue emission and short life times. Blue emission is desirable
in being less vulnerable to spectral interferences from black body
radiation at high temperatures. For two reasons in particular,
a short emission lifetime is also desirable. For one thing, it provides
the possibility of time-gating the signal collection to discriminate
from interfering background radiation and it provides high time
resolution with the possibilities this creates of making sharp 2D
measurements in turbulent situations or on fast-moving objects.
Some of the commercially available phosphors presented have
just recently been reported as temperature dependant [84]. The
information collected can be useful in choosing a phosphor and
may possibly provide certain guidance in the increasingly chal-
lenging projects in combustion diagnostics using thermographic
phosphors. The extremely harsh conditions that can be encoun-
tered makes it highly important to choose a phosphor that suits the
measurement situation in question, a phosphor with the appro-
1100
priate temperature sensitivity and the emission properties needed
to minimize background interference and achieve adequate
temporal and spatial resolution. More detailed information con-
cerning each phosphor is provided later in the paper. For two-
dimensional ratio measurements of temperature, the choice of
phosphors available is limited, see Fig. 7. The phosphors useful for
ratio measurements often cover large temperature ranges,
however, serving to compensate to some extent for limits in the
types of phosphors available. For measurements making use of
lifetime measurements, there are a large number of phosphors to
choose from. Single point measurements can be recorded using
a PMT or an avalanche photo-diode. Using a framing camera, as
described above, 2D lifetime measurements can be performed, as
exemplified in Section 5.1.2. This provides many opportunities for
finding adequate phosphors. Lifetime measurements are generally
more accurate than ratio measurements, with the exception of the
zinc oxide phosphors. This can be seen on the basis of the sensi-
tivity plots in Fig. 7 by how much the lifetime or the ratio changes
over the temperature range involved, i.e. how steep the curves are.
There are also examples where CMOS-cameras (high-speed video)
have been used for decay-time based 2D-imaging, see e.g. [85].
However, in order to achieve an adequate frame rate, the number of
useful pixels is still significantly reduced for these detectors. In [85]
for example the read out matrix was 208  64 pixels at 150 kHz.
After deciding on a measurement method, the first and most
obvious criterion for choosing a phosphor is that it has sufficient
sensitivity to temperature in the expected temperature range of the
measurement object. The next factor to consider is the measure-
ment environment expected. If measurements are to be made in
a burning environment, care should be taken to avoid the most
intense chemiluminescence emission peaks. If this is not possible or
if black body radiation interferes with the measurements, a fast
phosphor, of high quantum yield should be used. In this case the
collecting measurement equipment can be time gated to only
collect signal during the short emission period. Zinc oxide phos-
phors with emission lifetimes in the range of picoseconds are good
examples of this. In that case, the camera exposure time can be set
to a few nanoseconds without a loss of signal. Due to the very high
quantum yield of these phosphors most conceivable background
contribution is then negligible in comparison with the strong signal.
In measurements at high temperatures, black body radiation
interference can create problems. Even if the measurement object
itself is fairly cool, hot surrounding objects can interfere with
thermal emissions. Many of the thermographic phosphors that are
sensitive at high temperatures, such as manganese activated
magnesium fluorogermanate (Mg4FGeO6:Mn) and Y2O3:Eu, emit in
the red spectral region. These phosphors also have long emission
lifetimes, in the millisecond range, making it very difficult to use
430 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Temperature / °C
−200 0 200 400 600 800 1000 1200
Mg4FGeO6:Mn →
← Lifetime
Ratio →

−3 4
10 10

← Y2O3:Eu

La O S:Eu 624 →
2 2
YVO4:Dy →
−4 3
10 10
La O S:Eu 538 →
2 2

← YAG:Tb
CdWO4 →
−5 2
10 ZnO:Zn → 10
La 2O2S:Eu 512 →
Lifetime / s

← ZnO:Ga

Ratio
ZnO:Zn 510 →
−6 1
10 10

← BAM

← YAG:Dy
−7 0
10 ← LuSiO5:Ce 10
Y2SiO5:Ce → ← YAlO3 2
↑
Y2O2S:Sm

← BAM

−8 −1
10 ← ZnS:Ag ← YAlO3 1 10
↑
(Sr,Mg)2SiO4:Eu

© Gustaf Särner 2008

−9 −2
10 10
0 200 400 600 800 1000 1200 1400 1600
Temperature / K

Fig. 7. Temperature sensitivity for some of the phosphors surveyed in the paper. Ratio calibrations are dashed and can be read on the y-axis at the right [84].

time-gating for suppression of the background. For two-dimen-
sional measurements, background subtraction can often be used to
minimize the background disturbance, but the most effective
approach is to combine this with use of a short exposure time. Even
the green emission of Terbium activated yttrium aluminum garnet
(YAG:Tb) is vulnerable to black body radiation, but at high
temperatures its lifetime is reasonably short for effective time-
gating of the measurements. The high temperature phosphor
Dysprosium activated yttrium aluminum garnet (YAG:Dy) emits in
the upper blue region at 455 nm and 497 nm, a rather good emis-
sion wavelength region. A problem involved, however, is that
YAG:Dy has several groups of emission lines, see description below,
making the quantum efficiency of the few lines that are being used
low. In combination with its long lifetime of several hundred
microseconds, this makes YAG:Dy vulnerable to background
interferences and black body radiation. The large range and high-
temperature abilities of ratio measurements nevertheless often
make YAG:Dy a good choice for high temperature measurements.
For measurements on fast-moving objects, such as turbine
blades in a gas turbine, it is important to choose a phosphor with
a short emission lifetime. This is especially the case when 2D
measurements are being made since it serves to avoid a motion blur
caused by a long emission lifetime. Most of the blue or UV-emitting
phosphors have lifetimes that are short enough for this purpose.
Again, the zinc oxides are the best choice, both in terms of precision
and of lifetime. If the measurement situation requires a tempera-
ture higher than 870 K, the upper limit of sensitivity of the zinc
oxides, BaMg2Al10O17:Eu, with its strong and short-lived emission
at 440 nm, could be taken advantage of.
An important issue when using various thermographic phos-
phors is to what degree they are toxic and could induce various
health effects and being carcinogen. Since in general the potential
health effects are not known, we have in our experiments on new as
well as established phosphors used taken a safety attitude and
always treated the articles with care and not used them in exper-
iments without proper ventilation and safety precautions.
4.1. YAG:Dy
Y3Al5O12:Dy is one of the most commonly used thermographic
phosphors for high-temperature measurements. It has emission
lines in three groups, at 480, 580, and 680 nm, originating from
transitions from the 4F9/2 level to the 6H15/2, 6H13/2, and 6H11/2 levels,
respectively [87]. The phosphor emissions have lifetimes around 1
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 431

Fig. 8. Left: spectra of YAG:Dy emission as a function of temperature. Right: the ratio of the 458 nm to the 497 nm emission line measured using 10 nm wide interference filters at
455 nm and 493 nm [88].

ms and a temporal response to temperature in the range of
1500e2000 K for its 480 nm and 580 nm bands [86]. YAG:Dy is,
however, used in 2D measurements in most cases, where the ratio
of the spectral line at 458 nm and the line at 497 nm shows
a temperature dependence between 400 K and 1700 K [17,54,88]. In
Fig. 8 is shown how the phosphorescence spectra change as
a function of temperature and how the ratio of the peak at 455 and
493 depends on temperature.
YAG:Dy is effectively excited to high-energy bands by 355 nm
laser radiation. The energy is quickly relaxed, through radiative and
non-radiative de-excitation, to the 4F9/2 level. The F-level thermally
pumps the nearby G-level, 4I15/2, leading to a temperature-depen-
dent relationship between the emissions of these two levels, i.e.
between the 497 nm and 458 nm lines. Non-radiative de-excitation
is, however, also possible through quenching by vibrations of the
surrounding host lattice, so called phonon quenching. This leads to
a decrease in the signal with an increase in temperature, until the
signal finally disappears at about 1700 K.
4.2. YAG:Tb
Terbium activated yttrium aluminum garnet (Y3Al5O12:Tb) is
the host. In most phosphor host materials the CTS lies well above
the dopant energy levels, but in La2O2S the FranckeCondon-shif-
ted minima of the CTS overlap the Eu3þ 5D states as shown in
Fig. 10 [96]. Energy transferred to the CTS will feed the 5D levels
from which relaxation occurs in form of radiation. The Charge
Transfer State is located at very low energies (<40,000 cm1)
accessible from some energy states of Eu3þ, meaning that the CTS
also can absorb and transfer thermally excited 5D state electrons to
lower states, making the process complex [96]. The CTS process is
quenched thermally, however, leading to temporal temperature
sensitivity for three of the 5De7F transitions lines.
The strong temperature sensitivity at low temperatures of the
emission lines at 512 nm, 538 nm, and 624 nm, respectively, cor-
responding to the transition from the 5D2, 5D1, and 5D0 states covers
the temperature range from room temperature up to 600 K, see
Fig. 11. Because of this, La2O2S:Eu has been used in a variety of
thermometry applications, both by calibrating ratios of the
different lines to one another and by use of the lifetime decay
sensitivity [64,72,97,98].
Yag:Tb
10
−2

a green phosphor that has found use in projection CRTs, although its
use in Field Emission Displays (FED) has also been investigated
[89e92]. It is a phosphor that is useful for high-temperature decay −3
10
time measurements. It has been shown that YAG:Tb can be used for
thermometry up to 1700 K [28,93,94]. The green emission originates
from the 5D4e7Fj transition (J ¼ 6,.,0), where the main emission peak −4
is at 545 nm [95]. As can be seen in Fig. 9, the initially long lifetime 10
Lifetime / s

decreases rapidly after the quenching point at 1000 K, which reveals

a high temperature sensitivity. The initially long emission wavelength
−5
makes the signal vulnerable to black body disturbances, but since at 10
high temperatures the lifetime decreases to sub-microsecond time-
scales, a short time gate in the collecting system can be used to
effectively suppress the background. When using a PMT, that can be 10
−6

achieved by adding a gatable micro-channel plate.

−7
4.3. La2O2S:Eu 10
400 600 800 1000 1200 1400 1600
Temperature / K
In Europium activated lanthanum oxysulfide (La2O2S:Eu),
electrons are excited to the so called Charge Transfer State (CTS) of Fig. 9. The emission lifetime constant of YAG:Tb as a function of temperature.
432 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Energy / been used to excite the phosphor through a Thermal Barrier

103 cm-1 Coating, that is not transparent to UV radiation most often neces-
sary for excitation of phosphors [78]. It has, however, recently been
40
discovered that Y2O3:Eu is strongly quenched by oxygen above
900 K, severely diminishing the potential use of this phosphor in
Host CTS
combustion [102]. Y2O3:Eu also suffers irreversible damage at
pressure levels of a few bar, making it unsuitable for engine
3 applications [102,103]. Calibration data is shown in Fig. 12.
30
5 2 4.5. Y2O2S:Sm
D
1
0 The emission from samarium activated yttrium oxysulfide
(Y2O2S:Sm) originates mainly from the Sm3þ ion, see energy levels
20 in Fig. 13. The energy levels show similarities to those of dyspro-
sium. The energy gap between 4F3/2 and 4G5/2 is similar to the
Eu3+-levels energy gap between the 4I15/2 and the 4F9/2 in Dy3þ. In a manner
similar to the process occurring in YAG:Dy, the 4G5/2 state thermally
pumps the 4F3/2 state, providing a temperature sensitive relation-
6 ship between the emission lines of the two states.
10 5
4 Fig. 14 shows the temperature sensitivity of the spectra with
7 3
F emphasis to the 607 nm and the 645 nm lines corresponding to the
2
1 transitions discussed above. The ratio of the two peaks as measured
0
through 10 nm wide filters is shown at the right in the figure. The
sensitivity is not as high, however, as for YAG:Dy, also the emission
0
wavelength has a less favorable spectral position with regard to
Fig. 10. Diagram of the charge transfer state (CTS) as it affects de-excitation in the black body disturbances. The lifetime of Y2O2S:Sm is about 300 ms
La2O2S:Eu phosphor [96]. The CTS feeds the 5De7F transitions. [72]. at room temperature, the quenching point being at about 1000 K,
after which the signal strength decreases rapidly until it disappears
at about 1450 K. [104].
4.4. Y2O3:Eu
4.6. YVO4:Dy
Europium activated yttrium oxide (Y2O3:Eu) is a common red
phosphor used in fluorescent lamps, CRT projector tubes, and FEDs Dysprosium activated yttrium vanadate (YVO4:Dy) has a main
[89,99]. It has a strong emission band at 610e630 nm with the main emission line at 575 nm and a second emission line at 481 nm. [105]
emission line at 611 nm originating from the 5D0e7F2 transition The response to temperatures of 650e930 K, is in the same range as
[100]. Y2O3:Eu has long been used for thermometry [101]. Y2O3:Eu the much more sensitive Mg4FGeO6:Mn phosphor, see Fig. 15.
has a broad absorption spectrum in the UV with two main
absorption peaks centered at 395 and 466 nm, respectively. A very 4.7. Mg4FGeO6:Mn
interesting feature of Y2O3:Eu is, however, that it also has a small
absorption peak at 532 nm, coinciding with the green emission of Manganese activated magnesium fluorogermanate (Mg4FGeO6:
the second harmonic of the Nd:YAG laser. The absorption peak has Mn) is a phosphor useful for thermometry purposes and possible to
utilize for both decay time and spectral ratio measurements.
Already in the 1960s it was discovered that Mn4þ in magnesium
La2O2S:Eu
fluorogermane could emit light and that its emission was temper-
ature dependent [89,106]. The emission originates from transitions
512 nm
538 nm from the 4F2 state to the 4A2 ground level. The 4F2 state is split in
−4
10 624 nm two due to a distortion in the crystal (JahneTeller effect) [106],
leading to two dominating emission bands, the 631 nm and 657 nm
lines. Since the two emission bands originate from the split excited
state, they are thermally coupled by the Boltzmann distribution, so
−5 that the 631 nm line increases in intensity as the temperature
10
Lifetime / s

increases, at the intensity of the 657 nm line decreases. This can be

utilized for ratio measurements using the ratio of the mentioned
lines [98]. The 657 nm line also has a strong temporal dependence
with temperature between 700 and 1050 K, see Fig. 16
−6
10
4.8. BaMg2Al10O17:Eu

Europium activated barium magnesium aluminate (BaMg2A-

−7
10 l10O17:Eu), or BAM, is a very stable phosphor with a strong blue
emission line at 440 nm originating from the 4f65d / 4f7 transition
300 350 400 450 500 550 600 of Eu2þ [89]. BAM also emits light at temperatures up to about
Temperature / K
1200 K [107] making the phosphor suitable for combustion appli-
Fig. 11. Temporal response to temperature for the 512 nm, 538 nm, and 624 nm lines cations. Its high melting point, 2190 K, ensures that it will not be
of La2O2S:Eu. destroyed even at temperatures outside its sensitivity range. It has
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Fig. 12. Left: energy level diagram for Y2O3:Eu [100]. Right: temporal response to temperature for Y2O3:Eu.
a slight red shift at very high pressures, one that is negligible at
pressures under 1 kbar [108].
A spectral investigations of the temperature dependence of the
BAM phosphorescence reveals a blue-shift with a rise in tempera-
ture, see Fig. 17, one that can be utilized for temperature measure-
ments through use of narrowband transmission filters [109]. The
emission peak broadens towards the UV, but the peak wavelength
remains at 440 nm. A small blue-shift is also visible around 450 nm.
The ratio of 450 nm to any position on the short wavelength slope
provides a clear indication of temperature sensitivity. An oven
calibration using a 40 nm wide interference filter centered at
400 nm and a 10 nm wide interference filter centered at 456 nm is
shown in Fig. 17.
The temporal investigations of BAM with regard to temperature
show that there is a strong temperature dependence between 700
and 1150 K, where the lifetime decreases from 1 ms to 10 ns. BAM is
thus suitable for temporal measurement techniques as well in that
particular temperature range, see Fig. 18. It should be mentioned,
however, that the authors have on some occasions seen inconsis-
tent behaviour regarding the stability of BAM at elevated temper-
atures. Problems with oxidations are also treated in [110].
Fig. 13. Sm3þ energy diagram [104].
433
4.9. Y2SiO5:Ce
The blue emission from Cerium activated yttrium silicate
(Y2SiO5:Ce) originates from the 5d1 / 4f1 transition of the Ce3þ ion.
The transition is both parity-allowed and spin-allowed since the
two states are spin doublets [111], which results in short emission
lifetimes. Accordingly, this phosphor is used for flying-spot scan-
ners and fast CRTs. The spectral response is shown in Fig. 19. As can
be seen there is a slight broadening of the emission on the green
side of the emission peak, but not sufficient for thermometry to be
practical. The temporal response shown in Fig. 19 reveals a certain
sensitivity between 600 and 1020 K. This phosphor is thus useful
for thermometry, but its sensitivity is lower than that of
Mg2FGeO4:Mn, which is sensitive in the same temperature region.
An advantage of Y2SiO5:Ce, however, is its very short lifetime, less
than 1 ms, making the signal-to-background ratio higher than for
many other thermographic phosphors.
4.10. LuSiO5:Ce
The emission from cerium activated lutetium silicate
(LuSiO5:Ce) originates, just as for Y2SiO5:Ce, from the 5d1 / 4f1
transition in the Ce3þ ion. The central wavelength and lifetime of
the emission are also very similar to Y2SiO5:Ce, see Figs. 20 and 21.
The red shift accompanying an increase in temperature is more
distinct in LuSiO5:Ce, however. The ratio of 398 nm to 440 nm
shows certain sensitivity to temperature, but at high temperatures
the signal is very noisy giving lower precision, see Fig. 20.
4.11. (Sr,Mg)2SiO4:Eu
The blue-green phosphorescence of Europium activated
magnesium silicate, (Sr,Mg)2SiO4:Eu, excited by a 355 nm pulsed
light source is slightly broadened by an increase in temperature,
providing the possibility for the phosphor to be used for ther-
mometry at moderate temperatures.
There is a temporal temperature response between 500 and
700 K, see Fig. 22. One reason for selecting this phosphor could be
the advantage it has in possessing a short lifetime with a time
constant of about 400 ns at 500 K that is reduced to 5 ns at 700 K.
434 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 14. Left: spectral response to temperature for Y2O2S:Sm. Right: ratio of the 645 nm to the 607 nm peaks for Y2O2S:Sm.

The fact that there are few thermographic phosphors with
temperature sensitivity in that region makes this phosphor of
interest for thermometry at moderate temperatures. Note that the
levelling out of the lifetime in Fig. 22 is due to the limitation of the
laser pulse duration. A laser with a pulse length of about 5 ns was
used in the investigations. The lifetime most probably continues to
decrease for temperatures above 700 K, likely to sub-nanosecond
lifetimes at 850 K. This could be utilized by using a pulsed laser
with shorter pulse duration or of an amplitude-modulated
continuous excitation source and signal phase shift evaluation.
4.12. ZnS:Ag
The blue emission from Silver activated zinc sulphide (ZnS:Ag)
have traditionally (since 1939) been used in black and white CRTs,
mixed then with (Zn, Cd)S:Ag to obtain a white colour. ZnS:Ag was
used later as the original blue colour for colour CRT TV:s and is still
used for that purpose. This phosphor is also used as a scintillator in
a-detectors, due to its relatively short emission lifetime. [89]
The spectral response to temperature of ZnS:Ag is shown in
Fig. 23. The spectral shift is not large enough for use in thermom-
etry, although the temporal response can be used for that purpose.
The lifetime is very short with sensitivity to temperature in the
range 520e770 K.
4.13. YALO3:Ce
Cerium activated Yttrium Aluminum oxide (YAlO3:Ce), also
termed YAP, is used for flying-spot scanners and fast CRT, and as
scintillator. YAP can stand very high temperatures without a change
in emission properties. No obvious shift in frequency or in spectral
intensity ratio at up to 1170 K is apparent, see Fig. 24. The rugged
emission with regard to temperature could be used for measure-
ment of the spectral intensity ratio through use of this phosphor
together with another high temperature phosphor, such as the
YAG:Dy 455 nm line. YAP has an absorption peak within the
UV range at 305 nm, but absorbs up to about 10% of the maximum
at 266 nm, making the fourth harmonic of an Nd:YAG laser a possi-
ble excitation source. Temporal measurements reveal a double

YVO4:Dy Mg FGeO :Mn

−3 4 6
10 −2
10

−3
10

−4
10
−4
10
Lifetime / s

Lifetime / s

−5
10
−5
10

−6
10

−6 −7
10 10
550 600 650 700 750 800 850 900 950 200 300 400 500 600 700 800 900 1000 1100
Temperature / K Temperature / K

Fig. 15. Temporal response to temperature of the 575 nm line of YVO4:Dy. Fig. 16. Temporal response to temperature for the 657 nm line of Mg4FGeO6:Mn.
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 435

Fig. 17. Left: BAM emission at different temperatures when excited by 355 nm laser radiation. The broad blue emission band broadens towards the UV at increasing temperature.
Right: calibration of BAM for 2D measurements. The ratio of the signals collected through the 400 nm  20 to those collected through the 456 nm  5 interference filters as
a function of temperature shows a high level of sensitivity [84].

exponential decay. The temperature sensitivity of the two life-
time constants is shown in Fig. 24.
4.14. CdWO4
Cadmium tungstate (CdWO4) is a blue phosphor used in such
X-ray applications as X-ray Computed Tomography, XCT. This
phosphor is thus clearly excited by X-rays, but it also has an
absorption peak at 295 nm; 266 nm laser radiation from an Nd:YAG
laser is absorbed at up to 65% of the maximum absorption level.
CdWO4 shows no spectral response to temperature but reveals
a strong temporal sensitivity to temperature, as reported in [84],
see Fig. 25. The lifetime is about 11 ms at room temperature
decreasing to 4 ns at 570 K. At low temperatures this phosphor
could thus be used for thermometry as a complement to the weak
514 nm line from La2O2S:Eu. The sensitivity to temperature is
equally high but CdWO4 has a much higher quantum yield since all
emission is concentrated to one broadened emission peak. It should
also be noted that this phosphor contains cadmium and should be
treated as a carcinogen.
−5 BAM
10
−6
10
Lifetime / s
4.15. ZnO:Zn
Zinc activated zinc oxide (ZnO:Zn) is a zinc oxide crystal with
the defect of occasionally missing oxygen atoms being replaced in
the crystal structure by zinc atoms. It has been used as UV-sun-
blocking, as LEDs [112] and FEDs [113], in thin-film solar cells [114],
as nano-structure gas sensors [115,116], and as scintillators in
detectors [117]. ZnO:Zn shows exceptional temperature sensitive
line shifts, usable for very accurate 2D temperature determinations
using spectral ratio measurements.
ZnO:Zn has two emission lines, one at 389 nm and the other at
510 nm. The green emission line has an emission decay time
constant of about 1 ms, whereas the UV-emission line at 389 nm has
a time constant of less than 1 ns. Liu et al. [118] has shown that the
proportion of green and UV-emission is dependant on the excita-
tion energy density. In the present work a 10 Hz pulsed Nd:YAG
laser running on its third harmonic was employed, producing
355 nm light, with a fluence of 18 mJ/cm2, resulting primarily in UV
phosphorescence and in only a small amount of green emission, the
green being visible only at low temperatures.
The UV-emission line originates from near-band-edge emission
due to exciton states [119]. The green long-lived emission originates
from the defect of missing oxygen atoms in the crystal. The peak
wavelength of the UV-emission line has very strong temperature
dependence and a basically linear red shift with an increase in
temperature, see Fig. 26. Excitation was achieved by means of
a pulsed Nd:YAG laser having a pulse duration of 4.5 ns. A dichroic
mirror was used to prevent 355 nm laser radiation from entering the
spectrometer. The green 510 nm line shows temperature sensitivity

to be possible to use for decay-time measurements, see Fig. 26

−7
10 In other work ZnO:Zn has been found to function as a gas
detector when grown to nano-wires [115,116]. The phosphor was
thus tested for oxygen sensitivity. Tests were performed using an
optical quartz fibre coated at the tip with the phosphor inserted
−8
10 into a temperature and gas composition controlled container. No
spectral changes could be detected at oxygen concentrations
ranging from 0% to 100% at pressures up to 4.5 bar and tempera-
tures up to 400 K.
−9
10 Calibrations for 2D ratio measurements were made using an ICCD
200 400 600 800 1000 1200 camera and a stereoscope. An interference filter at 390  5 nm was
Temperature /K used for the short wavelength part. Two types of long pass filter sets
were used for the long wavelength part of the ratio: a GG420 filter
Fig. 18. Temporal response of BAM. A quenching point is visible at 700 K. The phos-
phorescence lifetime reveals a strong temperature dependence between 700 and and a long pass edge filter cutting at 441.6 nm. A dichroic mirror was
1150 K [84]. used to reflect any 355 nm laser light propagating together with the
436 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

−6 Y2SiO5:Ce
10
1

0.8
Intensity /. a.u

Lifetime / s
0.6
1020 K
0.4
290 K −7
10
0.2

0
300 350 400 450 500 550 600 550 600 650 700 750 800 850 900 950 1000 1050
Wavelength / nm Temperature / K

Fig. 19. Left: emission spectra from Y2SiO5:Ce between room temperature and 1020 K. Right: temporal response from Y2SiO5:Ce. The lifetime is very short throughout [84].

signal. A short camera gate was used to discriminate against the
long-lived 510 nm emission line at low temperatures. Fig. 27 shows
the ratios obtained with the two different filter sets for both ZnO:Zn
and Gallium activated zinc oxide (ZnO:Ga), the latter described
below in Section 4.16. Standard deviations of about 1% were
obtained at 800 K. At room temperature the standard deviation was
negligible, see [120].
4.16. ZnO:Ga
Gallium activated zinc oxide (ZnO:Ga) is used for a variety of
applications, such as LED [121,122], thin-film solar cells [123] and as
scintillator material in detectors [124,125]. When tested for
temperature sensitivity, ZnO:Ga revealed an exceptionally large
line shift, very similar to the one of ZnO:Zn, that could be used for
obtaining accurate 2D temperature measurements. When excited
by 355 nm radiation ZnO:Ga shows an emission peak at 386 nm at
room temperature. The lifetime of ZnO:Ga is very short, well below
1 ns and was in fact too short to be measured by use of a 35 ps long
excitation laser pulse and a streak camera. ZnO:Ga is a near-band-
edge-emitting semiconductor in which Gallium introduces a donor
band close to the edge of the conduction band [126]. Electrons
excited to the Gallium donor conduction band can recombine with
an electron hole in the valence band [127]. Fig. 28 shows a strong
red shift in emission wavelength at higher temperatures. 2D ratio
calibrations of the phosphor are shown in Fig. 27.
4.17. Up-conversion phosphors
Although not treated in detail in this paper, up-conversion
phosphors should be considered as an important complement to
the more common down-conversion phosphors. Up-conversion
phosphors are often excited at near IR and emit at shorter wave-
lengths, i.e. the resulting radiation is of higher energy than the
excitation radiation. Up-conversion phosphors are especially
interesting, due to the availability of powerful excitation sources
and low background noise in the near-IR spectral range. As an
example there are recent, still to be published, findings by Shan
et al., regarding the temperature sensitivity of the up-conversion
phosphors NaYF4:Yb,Er. The synthesis of these phosphors is
described in [128].
4.18. Binder materials
In performing surface temperature measurements using ther-
mographic phosphors, the phosphor powder needs to be attached
to the surface. This is done by mixing it with a liquid binder that
dries and cures on the surface. The mixture can be sprayed on the

LuSiO5:Ce LuSiO5:Ce
1.65
1.2 1.6

1.55
1
1.5
Intensity /. a.u

1000 K
Ratio 398/ 440

0.8 1.45

1.4
0.6
1.35
290 K
0.4 1.3

1.25
0.2
1.2

0 1.15
350 400 450 500 550 600 250 300 350 400 450 500 550 600 650 700
Wavelength / nm Temperature / K

Fig. 20. Left: spectral response to temperature for LuSiO5:Ce. Right: ratio of 398 nm to 440 nm for LuSiO5:Ce [84].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 437

LuSiO5:Ce reactive when cured. It dries at room temperature in about 20 min

−6
10 and is cured by raising the temperature. The HPC coating is soft and
can handle temperatures of up to 1500  C it is thus being used for
high temperature applications of thermographic phosphors. Sau-
ereisen #14 is a water-based binder that was developed primarily for
adjusting the viscosity of various cements in the building industry. It
Lifetime / s

is cured by heat and produces a hard coating that can handle

temperatures up to up 1200  C. Also mixtures of binders (ZYP/HPC
and ZYP/LK) have been reported to work well [82].

5. Applied measurements

5.1. Flamespread and fire protection

−7
10
600 650 700 750 800 850 900
Temperature / K
Fig. 21. Temporal response to temperature for the LuSiO5:Ce broadband signal [84].
surface or painted on it with a brush, creating a coating in each case
that is a few micrometers thick. When measuring a surface
temperature it is important to keep the layer thin to avoid the
coating acting as a Thermal Barrier Coating (TBC) layer. This is
because the phosphor coating, even if applied in a very thin layer,
may have sufficient heat capacity and thermal conductivity to alter
the local thermal environment. This implies that the temperature of
the coating might be slightly different from that of the surface of
interest and especially so at high temperatures and during
temperature transients [28].
Phosphors have, however, been employed using the TBC layer
in, for example, a gas turbine as the binder material. In that case the
intended measurement object is either the TBC layer itself [76] or
the material underneath it [77]. Few phosphors, if any but Euro-
pium activated yttrium oxide (Y2O3:Eu), are, however, available for
measurements through the TBC layer, since the materials used for
TBCs do not transmit UV light [78]. This makes it hard to excite
most phosphors. More information on rare-earth doped high
temperature thermal barrier coatings can be found in [79].
In most of work presented here, two binders have been
employed, HPC (ZYP Coatings) and Thinning Liquid #14 (Sauer-
eisen). HPC is composed of magnesium aluminium silicate and is not
Fires in buildings are often tragic events that have a devas-
tating impact on human lives. The spread of flames is strongly
950 1000
dependent upon the nature of the building involved, its geom-
etry, the contents of the interior and their flammability. For
instance, buildings furnished with flame resistant materials tend
to have reduced rates of flame spread, allowing more time for
occupant evacuation. Accordingly, the study of flamespread
phenomena is highly important for the fire safety. The
phenomenon of flamespread has for long been studied with the
aim of improving theoretical models [129e132] for flame growth
and for the prediction of flame spread. Nevertheless, the
complexity of the phenomena involved makes the development
of a unified model or a set of such models a very slow process.
One way of improving current models is to develop an experi-
mental database, especially of surface temperature, which plays
a major role in heat exchange between the flame and the solid
material. Thermocouples [133] are the standard for surface
thermometry of firespread [134]. Special care needs to be put
into installing thermocouples, mounting them as close as
possible to the surface of interest [133,135,136]. However, ther-
mocouples usually detach from the surface during combustion
and erroneously measure the gas or flame temperature [137]. In
experiments on flamespread, such problems can be avoided by
use of thermographic phosphors.
5.1.1. One-point temperature measurements
Temperature measurements at the surface of combustible
materials were performed in a small-scale flame spread scenario.
The materials chosen were low-density fibreboards (LDF) and

(Sr,Mg)2SiO4:Eu (Sr,Mg) 2SiO4:Eu

−6
10
1

0.8
−7
10
Lifetime / s
Intensity/. a.u

0.6

720 K
0.4 −8
10

0.2
290 K
−9
0 10
350 400 450 500 550 600 350 400 450 500 550 600 650 700 750
Wavelength / nm Temperature / K

Fig. 22. Left: the spectral response of (Sr, Mg)2SiO4:Eu up to 720 K. Right: the dependency of lifetime on temperature for the (Sr, Mg)2SiO4:Eu phosphor. At about 700 K the lifetime
is too short to be measured using a 5 ns long laser pulses from an Nd:YAG laser [84].
438 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

ZnS:Ag ZnS:Ag
10−6
1

0.8
−7
Intensity/. a.u

770 K 10

Lifetime / s
0.6

0.4 −8
10
290 K
0.2

−9
0 10
350 400 450 500 550 600 200 300 400 500 600 700 800
Wavelength / nm Temperature / K

Fig. 23. Left: spectra for ZnS:Ag at temperatures ranging from room temperature to 770 K. Right: lifetime of ZnS:Ag as a function of temperature for [84].

Polymethylmethacrylate (PMMA) 50 mm wide, 120 mm high and
10 mm thick. A hole 5 mm deep and 1 mm wide in which
phosphor particles could be placed to be present during
combustion was drilled into the surface of the material. The
spatial resolution of the technique was limited to 1 mm (on the
surface) in order not to alter the combustion and flamespread
processes. The presence of phosphor particles inside the material
ensured that temperature measurements could be carried out,
even when the surface layers degraded, burned and fell. Fig. 29
shows how LDF and PMMA materials were investigated. They
were placed in a vertical position and were wetted at the bottom
with either alcohol or heptane and were then ignited. The flame
propagated and heated the surface of the material by convection
and radiation. The fourth harmonic beam of an Nd:YAG laser at
266 nm was used to excite the phosphor particles
(Mg4FGeO6:Mn) inside the hole. The subsequent phosphores-
cence emission, guided by an optical quartz fibre, was registered
by a photomultiplier after passing through a 632 nm interference
filter. The signal was digitised by an oscilloscope (TDS 620) and
stored in a PC through a GPIB interface. The lifetime was calcu-
lated as described earlier.
The temperature could be deduced on the basis of earlier cali-
bration data on lifetime versus temperature measurement, utilising
the thermographic phosphor Mg4FGeO6:Mn. Fig. 29 shows the
results of two different tests of low-density fibreboard. The low-
density fibreboard produced less soot than PMMA. Once it was
ignited, a steep temperature increase occurred, due to rapid prop-
agation of the flame on the surface of the material. The temperature
then levelled off at a maximum value of around 450  C. In both tests
conducted the experimental conditions were identical, only the
differences found in the ignition procedure producing a noticeable
difference in the rise in temperature.
The effects of using two different fuels as the source of ignition
were studied. It was noted that for both fuels an acceptable signal
level could be measured, although the signal was stronger with use
of alcohol as fuel, which also produced less soot. The flames orig-
inating when using heptane as a fuel were more intense than those
when using alcohol. Accordingly, the heptane also produced more
soot. This led to sediment covering phosphor particles deposited on
the surface of interest. The use of heptane is very common in large-
scale flamespread scenarios. The signal-to-background ratio (the
background originating from the flames) could be improved by
using phosphors that emit at shorter wavelengths since the Planck
radiation emitted at flame temperatures is weaker in the blue
spectral region. Also shorter emission decays are favourable,
permitting background suppression through faster gating.

YAlO3:Ce YALO3 :Ce

10−4
Lifetime 1
1 Lifetime 2
−5
10
0.8
Intensity /. a.u

Lifetime / s

−6
10
0.6

1170 K 10−7
0.4

−8
0.2 10
290 K
−9
0 10
250 300 350 400 450 500 550 600 650 700 200 400 600 800 1000 1200 1400
Wavelength / nm Temperature / K

Fig. 24. Left: spectra from YAlO3:Ce at different temperatures. Right: temporal response to temperature of the two lifetime constants in the double exponential decay of YAlO3:Ce [84].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 439

CdWO4 at room temperature CdWO4

10−4
1
−5
10
0.8
Intensity/.a.u

Lifetime / s
−6
10
0.6

−7
0.4 10

−8
0.2 10

−9
0 10
350 400 450 500 550 600 250 300 350 400 450 500 550 600
Wavelength / nm Temperature /K

Fig. 25. Left: spectrum of CdWO4 at a room temperature of 295 K. Right: the temporal response to temperature for CdWO4 [84].

5.1.2. Two-dimensional temperature measurements DT

In combustion applications precise measurements of temper- s¼ (16)
logðI1 =I2 Þ
ature are very much needed in order to enable models for realistic
applications to be developed. Combustion and pyrolysis of where DT is the time separation between the emission measured by
burning materials are complex phenomena and performing the detectors and I1 and I2 are the intensities registered by detectors
temperature measurements in just one spatial location is usually one and two, respectively. The accuracy of such measurements is
not sufficient. The development of pulsed laser sources and high- readily affected by the exposure time and by the time window
speed acquisition devices (e.g ICCD clusters) has enabled the between the individual detectors (for further information see Refs.
extension from one-point measurements to measurements in two [56,65].
and three dimensions to take place. For surface temperature Fig. 30 presents flame spread scenario identical to the one
imaging, two techniques are available. Pyrometry is a mature described in the previous section.
technique which is available commercially, whereas thermo- Thermographic phosphor particles (Mg4FGeO6:Mn) were
graphic phosphor technique is still under development. Lifetime- deposited on the surface of the low-density fibre board by
temperature imaging using thermographic phosphors had not dispersing them on the surface and then pressing them against it.
been investigated previously and was addressed for the first time The board was wetted with alcohol and was placed vertically in the
by the authors in [63]. Lifetime imaging, as described briefly in focal plane of a high-speed framing camera (Hadland). Radiation at
Section 3.1, is a sensitive technique for temperature imaging. Ni 266 nm was then used to excite the phosphor particles at the
and Melton [59] used two detectors to measure the lifetime of repetition rate of the laser (10 Hz). The subsequent emission
naphthalene in a nitrogen flow, where the estimated error was through an interference filter at around 632 nm, Dl ¼ 10 nm was
about 15  C. The lifetime was deduced as follows from the accu- detected by the camera. The time separation between the eight
mulated fluorescence intensity signals recorded for each detector; ICCDs was chosen to satisfy [56,65];

ZnO:Zn spectra at different temperatures Lifetime vs temperature, ZnO:Zn, 510nm line

1100 10−5
294 K 475 K 655 K 838 K 954 K Peak position
1 1000
900
Time constant / s

0.8 800
10−6
Temperature / K
Intensity/. a.u

700
0.6 600
500
0.4 400 −7
10
300
0.2 200
100
−8
0 0 10
350 400 450 500 550 600 280 300 320 340 360 380 400 420 440 460
Wavelength / nm Temperature / K

Fig. 26. Left: ZnO:Zn spectra as a function of temperature. Excitation was achieved by using a pulsed high energy Nd:YAG laser which at room temperature induced mainly
UV-emission. A small green emission peak at around 510 nm is visible at low temperatures. As the temperature increases the UV-emission line shows an increasingly red shift.
Right: lifetime as a function of temperature for the 510 nm emission line from ZnO:Zn [120].
440 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

temperatures of 445e455  C dominated. Comparison with Fig. 29

(right) shows the results to agree well with those of the one-
point measurements. A standard deviation over 4  4 pixels
obtained in a region of fairly constant temperature was better than
the 5  C surface temperature deviations obtained at around
450  C. For the low temperature range w400  C, where the ther-
mographic phosphors do not excel, the measurement precision was
seen to deteriorate, being in the best case around 25  C.
Many factors need to be investigated carefully during such tests in
order for a high level of accuracy to be obtained. First, the time
schemes of the separate detectors need to be examined and taken into
account. Secondly, one needs to ensure that the temporal sensitivity is
high. Third and finally, calibration measurements, reference images
and statistical procedures are needed in connection with the indi-
vidual detectors in order to take into account their differing light and
gain sensitivity and to be able to compensate for these.

5.1.3. Applications to intumescent paint

Fig. 27. 2D temperature sensitivity calibration of ZnO:Zn and ZnO:Ga using an ICCD
camera equipped with a stereoscope. The plot shows the ratio of a 390  5 nm inter-
ference filter to either an edge long pass filter or a set of Schott GG absorption high-
pass filters [120].
0:2 < s=DT < 5
dt ¼ DT
where DT is the time delay between the active gating of the indi-
vidual ICCDs and dt is the exposure time of each detector. No
overlap between the individual temporal windows of the detectors
was employed since both short and long lifetimes needed to be
measured and be evaluated correctly. Short and long lifetimes
correspond to high and low temperatures, respectively. The results
are shown in Fig. 31
After acquisition of the signals, the lifetime was deduced on the
basis of an exponential fitting procedure, the temperature being
inferred from previous calibration measurements. A temperature
snapshot taken 112 s after the start of ignition is shown in Fig. 32,
where a 40  30 mm surface on the upper part of the fibreboard
that was investigated can be seen. Temperature contours were
plotted for different temperature ranges ascertain the temperature
that dominated. As is evident, on most of the area investigated,
ZnO:Ga spectra at different temperatures
294 K 475 K 655 K 838 K 954 K
Peak position
1 1000
0.8
Intensity /.a.u
Intumescent paint is a fire-resistive coating that swells up under
the influence of heat to create insulating layers of paint. It can be
applied to the surface of the material involved, such as steel, or be
incorporated into a polymer prior to fabrication. When exposed to
heat the paint foams up 40-fold to form a thick and porous charred
layer, which protects the coated material against heat transfer. The
dense char layer not only acts as a thermal barrier but also helps both
(17) in reducing the propagation of volatiles to the flame and in shielding
the coated material from oxygen transport, thus reducing the rate of
(18) flamespread. Such paint was the subject of a variety of full-scale tests
and mathematical model developments, see Refs. [141,142]. The
surface temperature is an important parameter in the heat balance
equation concerned with the paint and the surrounding environ-
ment, i.e. it is crucial for the determination of heat transfer inwards
and outwards through the coating.
Since the coating is very fragile, no optical or physical probe
technique had succeeded previously in measuring the coating
temperature. In Ref. [139], the surface temperature of an intu-
mescent coating was investigated by use of thermographic phos-
phors, the results are compared with those of simulations in which
a simplified heat transfer model was employed.
The experimental setup is presented in Fig. 33. An intumescent
coating was applied to steel plates of differing thickness (5, 10 and
20 mm). Different numbers of paint layers were investigated (1, 2
and 3), approximately 7.2 g of wet paint being deposited in each
layer. The coated substrates were dried at room temperatures for at
least 48 hours, and the thermographic phosphor, Mg4FGeO6:Mn,
was then dispersed onto the surface of the coating, covering an area
of about 0.5 cm2. The samples were introduced under the hood of
1100
a cone calorimeter regulated to a constant radiant heat flux. The
third harmonic of a Nd:YAG laser at 355 nm was used to excite the
900 thermographic phosphor particles. The phosphorescence emission
800 was detected by a photomultiplier through a narrow band trans-
mission filter centred at 632 nm, FWHM ¼ 10 nm. To monitor the

Temperature / K

700
expansion in coating thickness, an ICCD camera was used to record
0.6 600
the evolution of the coating on a regular time basis.
500 Fig. 34 shows the measured and the modelled surface temper-
0.4 400 ature and the thickness expansion as measured for a 5 mm plate
300 coated with 3 layers of paint. During the first few seconds of heat
exposures, both the predicted and the measured surface tempera-
0.2 200
ture increased markedly. This temperature increase is due mainly
100 to the characteristics of the paint. At temperatures of around 280  C
0 0 a delay in temperature rise was observed, one due to the decom-
350 400 450 500 550 600
position of the coating accompanied by the release of volatiles. The
Wavelength / nm
release of gases induced foaming of the carbonaceous material. At
Fig. 28. ZnO:Ga spectra at different temperatures. The peak wavelength is strongly temperatures of around 640  C the rise in surface temperature
shifted to longer wavelengths [120]. levels off before the paint expansion was complete. The measured
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Fig. 29. Left: the experimental setup: a laser pulse of 266 nm was used to excite the phosphor particles deposited on the combustible material. The subsequent emission was guided
to a PMT by means of an optical fibre. Right: results of two identical tests of surface temperature measurements of LDF boards. A maximum temperature of around 450  C was
obtained [138].
temperature agreed well with predictions of the model. In
Ref. [139], the effect of different thicknesses of the steel and of the
paint layers were investigated to examine their influence on the
measured and the calculated temperature.
5.2. Pyrolysis of decomposing materials
Due to the importance of gasification and combustion of bio
materials, considerable research nowadays deals with the physical
properties of these materials and their decomposition in a low
oxygen concentration environment, such as in pyrolysis scenarios.
Pyrolysis appears when organic materials decompose at high
temperatures in absence of air producing volatile components,
mixtures of combustible gases, and carbon-rich char. At high
temperatures, the composition of wood-based materials fragments
to form complex structures, due to the strong vibrations that occur
at the atomic level in the solid structures, producing organic
materials such as methane, together with water and different
aromatic structures. Brackmann et al. [144] used optical techniques
such as LIF and absorption measurements for studying volatiles
Fig. 30. Surface temperature imaging of an LDF board during a small-scale flame
spread scenario. The fourth harmonic at 266 nm was used to excite phosphor particles
deposited on the upper part of the LDF board. The subsequent emission was detected
by the framing camera through a band-pass filter. An alcohol-based fuel was used for
igniting the material [63].
441
originating from the pyrolysis of biomass. The resulting spectra
were complex, due to the strong interference between different
molecules, making identification of the relevant species very hard.
Modelling the pyrolysis of solid organic materials is a complex
task. Many parameters that play a substantial role in the pyrolytic
processes in the heat transfer models need to be validated and
correctly assessed. The surface temperature is one of these
parameters. In Ref. [140], the surface temperature of decomposing
construction materials, together with their mass-loss rates during
pyrolysis are studied. Wood particles were studied in a single
particle reactor filled with preheated argon gas injected at a flow
rate of 1.5 dm3/min. The reactor was equipped with a cooled tube
through which the particles were introduced and a ceramic sample
holder which received the particles and held them. A balance
connected to the sample holder was used to register the particle
mass at a frequency of 5 Hz. U-shaped heaters were installed inside
the reactor close to the centre of it, a thermocouple being placed
there for temperature regulation and display. The reactor was
equipped with optical access and with a mass spectrometer for
analysis of pyrolysis gases, see the photograph in Fig. 35 (left).
Prior to introduction of the test particles into the reactor, ther-
mographic phosphors were dispersed on the material being
investigated. The test particles were dried in an oven to remove any
moisture. Single particles were introduced into the reactor one at
a time through the air-cooled falling tube. The transition time
within the cooled tube was less than 1 s in duration, ensuring that
the particles did not gain appreciably in temperature prior to the
measurements being undertaken. Ultraviolet laser light was used to
excite the phosphor particles applied on the surface of the mate-
rials. The subsequent phosphorescence emitted was collected by
a PMT and a spectrograph for temporal and spectral evaluation, see
Fig. 35 (Right). The signals were detected by the photomultiplier
and digitised by means of an oscilloscope. As soon as the first
particle landed on the sample holder, acquisition started.
The surface temperature and mass loss of the particles were
investigated at different reactor temperatures. After the material
had reached the sample holder, a small loss in mass could be noted,
followed by large and rapid loss in mass. Then, the mass-loss levelled
off producing a char component of about 20e30%. The same basic
behaviour was seen on all the tests. Increasing the reactor temper-
ature led to an increase in the mass-loss rate due to rapid decom-
position of the material. In most cases a time delay of 1e4 s occurred
between the start of the measurements and the landing of the
442 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 31. Two-dimensional surface temperatures of low-density fibre board from ignition to the extinction [63].

particle. During this time, the surface temperature of the particle
increased to around 200  C. Then there was a sharp increase in
surface temperature until it reached a steady state level, see Fig. 36.
As the temperature increased, the surface temperature levelled off
more rapidly. The surface temperature measured was found to agree
very well with the reactor temperature as registered by the
thermocouples.
In some of the temperature plots in Fig. 36, for example, in cases
corresponding to 350  C and 400  C certain temperature modula-
tion could be observed, originating from the automatic temperature
control of the reactor. This temperature feedback stabilised the
reactor temperature close to the desired value through turning on
and off of the heating elements. In general, for the various wood-
based materials investigated, fast pyrolysis was found to start at
a surface temperature of around 380e430  C, where 90% of the mass
of the material had already been processed. The combined surface
temperature and mass-loss measurements were found to provide
valuable data for quantitative comparisons with the models.
In Ref. [143], surface temperature and mass loss from birch
particles were investigated and compared with results concerning
a two-dimensional model of the rapid pyrolysis of large particles.
The experimental setup was the same as described above. Birch
particles, cylindrical in form, weighting 50e90 mg, 5.4 mm both in
height and diameter were employed. The wood particles were
dried and then coated with thermographic phosphors, around
1e2% (by wt). When introduced into the reactor through the air-
cooled fall tube, the particles landed vertically because of their
shape, meaning that the direction of the wood fibres was oriented
in the direction of the cylinder axis [144]. The heat transfer model
implemented was based on a mathematical model first developed

Fig. 32. The surface temperature 112 s after ignition is shown, contour plots revealed that most temperature values were around 445e455  C [63].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Fig. 33. Experimental setup: the third harmonic from an Nd:YAG laser was used to
excite thermographic phosphors dispersed on the surface of the intumescent coating.
A photomultiplier detector and an ICCD camera were used for the temperature and
thickness measurements, respectively [139].
by Grønli [145] and modified by Larfeldt et al. [146]. The model
features the following: (1) a two-dimensional particle shape
(cylindrical in this case), (2) the particles being in a dried state, (3)
thermal equilibrium between the gas and the solid phases, (4)
anisotropy, (5) conduction, (6) convection and (7) mass transfer.
Three different pyrolytic schemes were investigated namely, (a),
(b), and (c) as described in Ref. [143]. The kinetic schemes differ in
the pathways for the decomposition of wood and its components to
gas, volatiles and char.
Scheme (a) assumes no gas phase reactions, (b) was taken from
Ref. [146] and (c) [147] uses hemicelluloses, cellulose and lignin as
the main components of the wood particle in predicting the gas,
char and remaining tar. Results of the experiments and of simula-
tions at different reactor temperatures are shown in Fig. 37. In
introducing a particle to a hot reactor, the surface temperature was
found to increase rapidly to 200  C during the first seconds prior to
acquisition. The falling tube was air-cooled to minimize heat
transport from the surroundings to the particle during free fall. The
200  C measured was believed to originate from heat conduction
from the sample holder and from heat convection from the inert
Fig. 34. Intumescent coating surface temperature and thickness are presented [139].
443
gas (Argon) surrounding it. After the particle had successfully
landed on the sample holder, the temperature increase continued
to about 400  C. When this temperature was reached, the rate of
heating decreased during the rapid pyrolysis that occurred and
increased again to approach the reactor temperature, at which
point only the char component was left. As can be seen in Fig. 37,
rapid pyrolysis started at around 400  C. At lower temperatures, the
material reached the reactor temperature already when only partial
decomposition had occurred. At temperatures above 400  C,
complete decomposition took place before the material surface
reached the steady state level. The model implemented was found
to predict the measured surface temperature well, as evident in
Fig. 37. The simulations indicated the surface temperature not to be
very sensitive to either the kinetic scheme employed or the rate of
pyrolysis. However, when the physical properties of the wood
material change from those of wood to those of char, a substantial
change in the heat transfer characteristics of the material occurs.
This transition was observed in the temperature measurements but
not in the simulations.
Recent use of optical diagnostic in general and thermographic
phosphorescence in specific for deducing temperature in gasifica-
tion experiments using biomass is reported in Ref. [148].
5.3. Thermographic phosphor thermometry in a gas turbine
afterburner
The gas turbine is one of the most important inventions of the
20th century. It is used in a wide variety of contexts, such as power
generation and propulsion of ships and airplanes. During the last 40
years, developments have progressed continuously especially in
terms of reducing fuel consumption and emissions of CO, NOx and
HC [149,150]. To improve its efficiency and reduce the CO emis-
sions, the engine needs to be operated at high temperatures to
ensure that the chemical conversion of CO to CO2 is as complete as
possible. To increase the overall temperature, either the air inlet
temperature or the pressure inside the combustion chamber is
usually increased. As a direct consequence, the emission level of
nitrogen oxides increases with increasing flame temperatures
[149]. Operating the engine at high temperatures to reduce fuel
consumption also affects the thermal load on the engine compo-
nents, shortening their lifetime and leading to their deterioration.
The components need to be cooled in order to sustain long-term
444 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Fig. 35. Experimental setup: laser radiation at 266 nm was directed onto the phosphor particles inside the reactor. The phosphorescence emission was registered by a photomultiplier
and a spectrometer [140].
operability of the engine. Different cooling systems exist. One way
of cooling the engine is to make efficient use of the air already
introduced to form a thermal barrier between the liner and the
combustion chamber. Another method, involves use of thermal
barrier coatings, which reduce heat transfer to the coated surface.
Usually, the materials used for thermal barrier coating are based on
carbon, ceramics and highly temperature-resistant alloys.
Due to the known limitations of thermocouples, being trou-
blesome to install, sensitive to electromagnetic radiation and
measuring only the local temperature, thermographic phosphors
came into use in turbine machinery already at the end of the
eighties. Alaruri et al. [21,22], Tobin et al. [18,19] and Noel et al. [20]
have investigated the use of Y2O3:Eu and YVO4:Eu for the ther-
mometry of engine components, such as rotating blades. Feist et al.
[23] investigated the use of several phosphors for high temperature
measurements inside combustors. It was found that thermographic
phosphors were useful in thermal barrier coatings, phosphor
particles were mixed with the thermal barrier coating itself to
monitor the temperature of the coating and deterioration in its
thickness.
Laser-induced phosphorescence thermometry has been applied
to the inner wall of the afterburner on a full size fighter jet engine
[88]. The measurements were aimed at testing the technique under
the extreme conditions prevailing in the test rig of an aviation gas
turbine running at full afterburner load. The engine, a Volvo RM12,
see Fig. 38, is dedicated for use in the Swedish Gripen fighter
aircraft (JAS 39). It is based on the General Electric F404 engine,
from which it has been developed to meet single-engine safety
criteria, achieve higher performance and possess greater resistance
to bird strikes.
The measurements were made under various engine-running
conditions, including use of the afterburner. Specifically the
investigations were made on the outlet cone of the afterburner
using the intensity ratio method, see Section 3, and the phosphor
YAG:Dy, which is suitable for temperature measurement from
room temperature to 1700 K. The spectral response of YAG:Dy to
temperature and the calibration curve for the measurements are
shown in Section 4.1. A Nd:YAG laser running at its third harmonic,
355 nm, was used for excitation of the 1 dm2 measurement area
coated with YAG:Dy phosphor particles. A stereoscope containing
interference filters for the wavelengths 455 and 493 nm was used
for collection of the two spectral regions onto one half each of an
image intensified CCD chip. The setup is shown in Fig. 39.
The intensity ratios of the resulting images were converted to
temperatures, using calibration curves obtained earlier. Single-shot
images of surface temperatures are shown for an afterburner of
both 62% and 100% load, shown in Fig. 40 (Left). There was
a temperature difference between the two loads of around 200  C.
After averaging 100 single-shot phosphorescence images (not
shown), the resulting temperature distribution was found to have
a triangular shape. This shape resembled to some extent the shape
of the air-cooling canals positioned behind the surface [151]. The
average surface temperature over 20  20 pixels in each single-shot
image is shown in the right part of Fig. 40.
The surface temperature at the idling of the engine (no fuelling
of the afterburner) was 517 K, whereas when the afterburner was
activated the temperature increased and levelled off at tempera-
tures around 940 K. After the engine was run at full load of the
afterburner for 50 s, the afterburner was deactivated and the
temperature decreased. Statistics from the measurements show
that at full afterburner load the standard deviation, or precision,
was about 20e30 K at about 1000 K or 2e3%.
Measurements have also been made at a single point in the
flame holder using the lifetime method [152]. The flame holder was
located at the front of the afterburner, meaning that the excitation
laser radiation and the signal both had to pass through almost the
entire afterburner flame A phosphor material having suitable
sensitivity in the expected temperature range (Mg4FGeO6:Mn) was
applied to the area of interest on the flame holder of the after-
burner, see Fig. 41.
Phosphorescence radiation was generated using the fourth
harmonic (266 nm) of a pulsed Nd:YAG laser (10 Hz) as an excita-
tion source and the signal was detected with a photo multiple tube
(PMT). Spectral filtering of the phosphorescence signal was utilized
using a band-pass filter centred at 657 nm, thus a distinct transition
in the phosphorescent material could be selected. Phosphorescence
lifetime decays were recorded with a 1GHz oscilloscope over a wide
operational range of the engine, including various use of the
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 445

Fig. 36. Temperature and mass loss at different reactor temperatures [140].

afterburner. By analyzing the lifetime decay, temperature data was
acquired through implementation of a regression equation
extracted from well-defined calibration measurements of the
phosphor used. An example is shown in Fig. 42.
5.4. Droplets and sprays
Sprays are a key element in various industrial processes such as
inkjet printing, fuel injection in internal combustion engines and
cooling processes in steel production. Once injected in a hot envi-
ronment, the liquid atomise to small droplets and evaporate as heat
is transferred to the core of the two-phase flow. Thus, spray
temperatures play an important role in determining of heat transfer
and evaporation rates. Although modelling heat transfer in
complex sprays is a far from trivial task, the problem can be
simplified to the modelling of droplets since the heat characteris-
tics of the overall spray depend upon the heat transfer properties of
individual droplets. Laser-based diagnostics has been found to be
a valuable tool for verifying and improving current models. In Refs.
[153,154,155], the temperature and the size of droplets were
investigated, using a laser-based rainbow technique. Flow velocity
measurements have been described, e.g. in Refs. [156,157]. Simul-
taneous visualization of the liquid and the gas phase were reported
in Refs. [158,159] and measurements of droplet temperatures were
demonstrated in Refs. [60,153,154,160e164].
Laser-induced fluorescence from organic molecules [159] or
exciplex [60,165] represents one of the most successful methods for
liquid thermometry and liquid-vapour visualisation. Unfortunately,
in harsh environments such as in internal combustion engines,
quantitative measurements using fluorescence-based techniques
require investigation of all the dependencies involved, such as
pressure, quenching, and temperature variations, as exemplified in
Ref. [166]. In such environments a method insensitive to pressure
variations and to quenching is highly desired.
446 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Fig. 37. Measured temperature and mass loss as compared with results from simulations [143].
In Ref. [98], a thermographic phosphor technique was applied to
mono-dispersed droplets. Both the temporal and the spectral method
were investigated using La2O2S:Eu and Mg4FGeO6:Mn, respectively.
Calibration measurements were performed in a liquid kept in
a container equipped with quartz windows and an opening for
a thermocouple. To monitor the temperature of the mono-dispersed
droplets, a free-falling scenario was arranged. The experimental
setup is shown in Fig. 43. A container was used to keep the liquid in
question and to heat it by use of heating wires. The liquid investigated
was distilled water mixed with phosphors, w1%-wt. A thermocouple
was placed inside the tank in order to obtain a reference temperature.
When the droplets that were formed left the tank, they encountered
a continuous wave (HeeNe laser), which in turn triggered acquisition
of the droplet signal at a distance 100 mm below the position where it
was located initially. Excitation was achieved by use of an Nd:YAG
laser at 355 nm, detection being performed by means of a suitable
detector, such as a PMT, a spectrometer or an ICCD camera.
Fig. 44 shows the results when droplets were seeded with
La2O2S:Eu. After excitation of the phosphor particles, the subse-
quent emission was detected by a PMT after passing through an
interference filter at 514 nm. The temperature of the liquid was
initially set to room temperature and was increased successively up
to 100  C. As already noted, comparing the measured temperature
with the results the thermocouple provided showed that up to
a temperature of around 90  C the two agreed well. The discrepancy
above this point was attributed to heat and mass loss that occurred
during the free fall. The model was calculated as in Ref. [168]
ðM2 þ M1 Þ
DT ¼ lDM  Hs (19)
2 1 2 3
where (1) is the change in variation of the heat stored in the droplet,
(2) is the mass loss term and (3) is the sensible heat transfer. This
equation was calculated using small time steps to account for
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Fig. 38. The Volvo RM12 engine [88].
acceleration of the droplet and its variation in diameter until it
reached a distance of 100 mm, which was the measurement point.
The results of calculations using the model previously described are
presented in Fig. 44. The higher the temperature of the liquid in the
container is, the greater the loss in droplet temperature becomes.
Further experiments on droplets falling in a temperature-controlled
surrounding provided further support for this.
Use of thermographic phosphors for liquid thermometry was
reported for the first time in Ref. [98]. An accuracy of better than 1%
was estimated. Several liquids involving use of different phosphor
materials were investigated.
Two-dimensional temperature measurements using the fluo-
rescence lifetime imaging technique of free falling droplets and
sprays were reported in Ref. [64]. The technique extends the one-
point measurements described in the previous chapter to two-
dimensions. Two-dimensional measurements allow gradients to be
visualized and deeper insight into the influence of temperature on
the atomisation and evaporation of sprays to be gained. Melton and
colleagues [62,159] investigated several other effects, such as
thermal diffusion, liquid-vapour separation and internal circulation
that occur inside the droplet.
The experimental setup was similar to that in Fig. 43, only the
detector being replaced. A Hadland framing camera was used
instead of a PMT. After excitation of the droplet, which was seeded
with La2O2S:Eu, the subsequent phosphorescence was detected by
the framing camera through an interference filter centred at
514.5 nm. The time delay between the individual detectors was
adjusted to satisfy 1 < s/Dt < 5 [56], where s is lifetime and Dt is the
time delay between the ICCDs. The time gate was adjusted during
the experiments to fulfil Dt ¼ s/2.5. Having an overlap of 50%
Fig. 39. Setup for thermographic phosphor wall temperature measurements in two-
dimensions using the intensity ratio method [88].
447
between the individual detectors was decided upon, although no
appreciable difference could be detected when an overlap of 75%
was employed. The 50% overlap was still preferred because of its
sensitivity to longer lifetime components being greater than in the
case of a 75% overlap. The resulting images were filtered, using
a median filter to remove spikes and dead pixels. The images were
then binned (2  2 pixels) to increase their dynamic range. After
subtraction of the background the images were then divided by
flat-field images to account for non-homogeneities and the
different sensitivity of the various ICCD cameras. An exponential
function was then fitted to the intensities originating from the
corresponding pixel positions in all the CCDs.
Fig. 45 (left) shows two-dimensional temperature measure-
ments of a free-falling droplet. As can be noted, the temperature in
the droplet, except in its lowest part, was basically homogeneous.
Possible explanations of the temperature gradients found, involves
convective heat transfer from the surrounding air having a lower
temperature, and of the slow thermal diffusion and its effect of
internal circulation.
To further investigate use of the technique in spray applications,
a simple water spray was investigated. First a quantity of 0.25%-wt
of Triton X-100 ([C16H26O2]n) was added to the water being
investigated together with thermographic phosphors. Triton X
increased the solubility and the mixing of the thermographic
phosphors with the liquid. Compressed air was used to spray the
liquid downward past the laser sheet. The phosphorescence emis-
sion was detected by the framing camera and was processed further
then to obtain the temperature, as described previously. Fig. 45
(right) shows two-dimensional temperature measurements of
a water spray. As one can note the spray was cooler in the middle
than at the edges. Another example of phosphor thermometry in
sprays is presented in [167].
Use of lifetime imaging for high spray velocities can introduce
errors due to displacement of the spray by the acquisition window
selected. Use of another phosphor, e.g. the ZnO:Zn or ZnO:Ga, with
a shorter lifetime on a nanosecond scale and to record the ratio of
two temperature emission lines may even allow burning droplets
to be studied. A series of 2D temperature measurements have thus
been performed on burning droplets of methanol [120]. A container
with methanol and 1% ZnO:Ga was heated to the boiling point of
methanol, inducing turbulence in the container and ensuring
sufficient mixing of the insoluble inorganic phosphor and the
methanol. The experimental set-up was similar to above. The
droplets were ignited by falling through a Bunsen burner flame. The
5 ns 355 nm excitation laser pulse was formed to a sheet which
penetrated the centre of the droplet. Fig. 46 shows a temperature
image of a burning droplet inside the Bunsen burner flame. The
short exposure time and strong signal reduce the chem-
iluminescence interference to negligibly intensities.
448 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 40. Left: single shot temperature measurements at different loads of the afterburner. The images corresponding to a surface area of 100  100 mm2 were taken at afterburner
loads of 100% (right figure) and 62% (left figure). Right: the average temperature value over 20  20 pixles in each single shot image is plotted versus time. An increase of surface
temperature of about 400 K is noticed when increasing the load from idling to 100% load of the afterburner [88].

Another attractive method, besides that of studying droplets in
free fall, is levitation. There are different types of levitation, such as
electrostatic levitation [169], aerodynamic levitation [170],
diamagnetic levitation [171], and acoustic levitation [172]. The
latter is used extensively in analytical chemistry and has the
advantage of levitating either liquid or solid samples without the
use of an electrostatic field. The levitator used for thermometry
using TP was based on the acoustic levitation method APOS BA10
(Dantec Dynamics GmbH, Erlangen, Germany). This levitator
operates with a frequency of 100 kHz and generates a standing
wave with equally spaced nodes and antinodes by multiple
reflections between an ultrasonic transducer and a solid reflector,
see Fig. 47. In these nodes, liquid or solid samples of appropriate
volume and density can be positioned, either manually by use of
a syringe or by using droplet dispensers [173e175]. Droplet levi-
tation facilitates basic research aimed at providing a better
understanding of liquid mixing, internal circulation, and evapora-
tion effects under different environmental conditions, such as
varying the pressure or the surrounding temperature. The ther-
mographic phosphor approach can thus be very useful for vali-
dating models for liquid and spray evaporation, e.g. for internal
combustion engine applications.
The use of thermographic phosphors (TP) for levitated droplet
thermometry has been investigated, together with other laser-based
techniques such as Mie-scattering and laser-induced fluorescence
[176]. First, Mie-scattering and TP were performed on a water
droplet. Laser-induced fluorescence and phosphorescence were
then applied to a droplet of acetone with the aim of investigating the
potential of TP for studying droplets in levitation and also the
behaviour of phosphor particles in droplets during evaporation.
The experimental setup is shown in Fig. 47 in which the exci-
tation and detection schemes for the levitated droplet are indi-
cated. The liquid, based on water, acetone or both, was mixed with
phosphor particles, around 1% by weight. A syringe was used to
form the droplet and introduce it into the levitator. A thin laser
sheet was then formed and was directed at the centre of the

Fig. 41. Image showing the afterburner flame holder. The white dot represents the Fig. 42. Plot showing the time resolved temperature on the flame holder as the load of
coated surface. the afterburner is varied [152].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 449

Fig. 43. Experimental setup: a HeeNe laser was used to trigger the acquisition system. After a free-fall of 100 mm the phosphorescence emission was registered by a suitable
detector [98].

levitated droplet. The subsequent emission was monitored, using
an ICCD camera and a stereoscope to record two physical processes
simultaneously, TP and LIF.
Results using elastic scattering and thermographic phosphors
are shown in Fig. 48. The suspended droplet had a diameter of
2 mm initially, its diameter decreasing with time and finally
becoming 0.5 mm or less. In all the tests, the phosphor particles
were believed to remain inside the droplet while it was evapo-
rating. Only in some few cases, when a droplet was rotating rapidly,
did some of the phosphor particles precipitate to the surface and
leave the droplet. This was due to ultrasonic streaming, which
normally is used to enhance liquid mixing inside the droplet. Fig. 48
shows results of simultaneous measurement of TP and laser-
induced fluorescence in a water/acetone droplet. The fluorescence
signal decreased substantially during the first 60 s. When most of
acetone had evaporated, there were mainly only water and phos-
phor particles left. The droplets were deformed as shown in the
figure, due to a slight increase in the ultrasonic field. This was done
in order to determine whether the droplet, when exposed to forces
that deformed it as occurs normally during the breaking up and
atomisation of spray, have an influence on the thermographic
phosphors particles inside the droplet. It was noted that most of the
phosphor particles remained inside the droplet long after the
acetone had evaporated.
In Fig. 48, the diameter of the droplet can be seen to have
decreased over time. Measuring variations in droplet diameter over
time can yield information on the evaporation process which is
taking place. Usually, droplet diameter changes according to the
d-square law, d2 ¼ d20  bt, where d0 is the initial diameter, t is time
and b is the evaporation coefficient. The latter is very relevant in
estimating the evaporation and the burning rate of a droplet, for
example in Fig. 49, the square of the measured diameter was plotted
against time. As can be noted, there are two components. The first
component was identified (from the evaporation coefficient) as
being acetone and the other as being water. Since the boiling point of
acetone is 56  C, which is approximately half that of water, acetone
evaporates first and does so completely during the first 60 s, the
water remaining and evaporating only about half as fast (which

Fig. 44. Left: droplet temperature as measured by use of thermographic phosphors (TP) and by use of a thermocouple (TC). The model, as calculated Ref. [168], was used to correct
for the temperature loss from the container to the measuring point. Right: temperature for a modelled droplet travelling a distance of 100 mm in free fall. As the diameter decreases
the temperature loss to the surroundings also increases [98].
450 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 45. Left: single-shot of a freefalling droplet. The droplet temperature was fairly homogeneous, except for the lowest part of the droplet. The layers surrounding it were less
homogeneous. Right: single-shot temperature measurement of a water spray (height of imaged area: 40 mm). The core of the spray was cooler than the edges [64].

agrees well with Fig. 48). As shown in Fig. 49, the evaporation of
toluene droplets was slower than that of acetone droplets. No other
components, such as water, were observed. The evaporation coef-
ficient was close to that of water, which is reasonable, since the
boiling point of toluene is around 110  C. Both figures demonstrate
the usefulness of a levitator for measuring the droplet evaporation
coefficient of relevant fuels. Further investigation could be directed
at simultaneous measurement of the evaporation coefficients of
mixed fuels at various pressures. This could contribute considerably
to an understanding of spray and droplet evaporation in realistic
environments.
All the tests carried out were performed at room temperature
and at atmospheric pressure. This was because of the compact
geometry of the levitator, which does not support momentary
variations in temperature and pressure. Promising results should,
however, encourage to redesign the levitator to be able to operate
under high temperatures and pressures.
Despite the successful demonstrations of thermographic phos-
phors for thermometry in droplets and sprays as described above, it
should be pointed out that this application is still under investigation
and further work is needed before reliable applications in practical
devices can be presented. One aspect to investigate is the increased
phosphor concentration after droplet vaporization and to what
degree this will influence the results in a practical environment.
5.5. Internal combustion engines
The design and the performance of internal combustion engines
are strongly affected by two major factors: emission legislation and
thermal efficiency. Since 1970 exhaust emissions have been
dramatically reduced. In parallel the efficiency of the engines has
been increased. In designing engines, the thermal loads to which
the internal components are subjected need to be known as closely
as possible so that adequate predictions of their lifetime can be
made [177,178]. The temperature distribution to which the
components are exposed is non-uniform and affected in a negative
way by the high temperatures within the engine. Increasingly
strong demands are being placed on the achievements of high
power, low fuel consumption and avoidance of pollution. Operating
an engine under extreme conditions further exposes the internal
components to damage of various sorts. Wall thermometry and
measurement of heat loss are needed in order to gain better

Fig. 46. (a) A burning methanol droplet as it was falling, photographed with an ICCD camera. (b) A temperature image of a burning methanol droplet that was falling, recorded in
the middle of the Bunsen burner with a camera exposure time of 10 ns [120].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 451

Fig. 47. Left: ultrasonic levitator setup: the waves generated between the ultrasonic transducer and the solid reflector hold the droplet suspended in air. Right: experimental setup.
An acoustic levitator was used to suspend a 1 mm diameter droplet. The third and the fourth harmonic of an Nd:YAG laser were used for Mie-scattering, TP and LIF. An intensified
CCD camera and a stereoscope were used for separation and detection of the signals [176].

Fig. 48. Left: simultaneous detection of Mie-scattering and TP at different time intervals after formation of the droplet. Right: simultaneous detection of TP and LIF at different time
intervals after introduction of the droplet into the levitator [176].
452 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 49. Left: the droplet diameter squared versus time for pure acetone, 99.9%. Right: droplet diameter variation over time for a toluene droplet, 99.8%.

understanding of the thermal efficiency and the durability of the
hardware. In various studies, wall [179e181], valve [182e184], and
piston thermometry [185e189] have been applied in internal
combustion engines to assess the thermal load and heat losses
[179,183,190]. The use of thermographic phosphors in internal
combustion engines allows both one-point and two-dimensional
surface temperature measurements to be obtained. Thermocouples
are a standard tool for temperature measurement. However, in
engines thermocouples are time-consuming to install due to their
complex geometry and the harsh environment to which they are
exposed, such as inside a combustion chamber. In addition once
installed, thermocouples are difficult to shift to a different
measurement area, which increases the complexity of an experi-
ment and the time required for it. For moving targets, e.g. pistons,
valves, etc, the instrumentation of thermocouples is even more
cumbersome. Thermographic phosphors also have the advantages
of enabling two-dimensional measurements to be made and of
having high degree of applicability to highly differing geometries.
The technique is also not sensitive to engine vibrations or to typical
pressures of around 30e100 bar inside the combustion chamber.
Studies performed using either Cr3þ [191,192] or Eu [193,194] have
not revealed any noticeable changes in lifetime or in spectral line
positions at pressures under 1GPa. However, when pressure
exceeds 1 GPa the crystal field of rare-earth ions and transition
metals could conceivably be altered, affecting the line coupling, line
separation and dipole transitions, see Refs. [191e195].
Although thermographic phosphors have been employed in
a variety of applications, until the early 2000, the authors could
only find one example of applications in engines when Armfield
et al. [196] used them for thermometry of the intake valve (on the
stem side of the valve). The present authors demonstrated and
discussed both two-dimensional and one-point temperature
measurements in a direct injection gasoline engine using TP [197].
The measurements were performed on the intake and exhaust
valves, and inside the combustion chamber on the pistons. The
engine investigated, based on the AVL 528 engine, had a Volvo 4-
valve gasoline cylinder head, see Fig. 50.
The engine provided a horizontal view through the pent-roof
area (Quartz window) and a vertical view through an elongated
piston. The direct injection engine was fuelled with isooctane and
was operated at l ¼ 1(stoichiometric condition). Two different
modes of operation were employed: (1) a continuous mode in
which the engine was run continuously and (2) a skip-fire mode in
which combustion occurred every fifth cycle. In this latter mode the
engine could be operated for a longer period of time since the
thermal load on the combustion chamber was reduced when there

Fig. 50. Left: photograph of the optical engine. Right: experimental set-up [197].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
was no ignition. This mode is suitable for optical engines with
limited cooling of the optical components.
Thermographic phosphor was coated on the engine components
to be investigated, using Thinning Liquid 14. The coating was dried
by hot air for at least 30 min at temperatures of around 400  C. As
shown in Fig. 50 (Right), the phosphor particles Mg4FGeO4:Mn
deposited were excited using a laser beam at 266 nm and the
subsequent emission was used for the one-point and two-dimen-
sional measurements. In the one-point measurements, the emis-
sions that were detected were first filtered from the scattered laser
light by means of an OG 550 high-pass filter and were then detected
by a photomultiplier. The higher transmission of this filter increased
the signal compared to that obtained with use of the interference
filter. This was needed because of the small measurement area
(4 mm2) at the centre of the valves. Despite the measurements not
being obtained when the flame was present, the intensity that was
registered decreased when soot deposits on the surface increased. In
the two-dimensional measurements, a stereoscope and an ICCD
were used for acquiring two identical images, corresponding to two
different spectral lines, 631 and 657 nm.
Fig. 51 shows two-dimensional temperature measurements of
the exhaust and intake valves. The temperatures of the exhaust
valve increase earlier than those of the intake valve. During the
exhaust stroke, the burned gas leaves the combustion chamber
through the exhaust valves where heat transfer from hot gases to
the exhaust valves occurs. In the tests conducted the temperature
of the exhaust valves increased from the edges to the centre. This is
due to the high convective heat transfer from the hot gases exiting
the combustion chamber. During the intake stroke, the intake
valves opens to allow air to enter the combustion chamber. Since
heat transfer from the fresh air-cooled the intake valves, the
Fig. 51. Left: two-dimensional temperature measurements of exhaust and intake valves. Right: one-point measurement of exhaust valve temperatures under different running
conditions [197].
453
temperature of the exhaust valves reached steady state quicker
than that of the cooled intake valves. One-point measurements of
an exhaust valve are presented in Fig. 51. Different engine condi-
tions were investigated, 1200 and 2000 rpm in the continuous
mode and 2000 rpm in the skip-fire mode. When running the
engine in the continuous mode, the measurement time window of
around 300 s was not exceeded, in order not to damage the optical
windows through excessive accumulation of heat.
The upper figure, involving 2000 rpm in the continuous mode,
shows that the surface temperature of the exhaust valve to increase
markedly and to level off finally at a temperature of around 350  C.
The middle figure shows the measured surface temperatures at
1200 rpm at a lower engine load. The surface temperature
increasing rapidly the first 50e70 s and then levelling off at around
270  C. The figure at the bottom shows exhaust valve temperatures
when the engine is running in a skipfire mode. The temperature
was found to be much lower than for the continuous mode, level-
ling off at 158  C. In all three tests, a rapid temperature increase
during the first 50 s was noted. The final temperature depended, as
expected, very much on the mode and load of the engine.
Since the measurements were conducted prior to combustion,
no background interference with the phosphorescence signals
occurred. The measurement errors originated from the fitting
procedures and least-square errors in extracting the temperatures
from the calibration curve. The precision was found to be around
0.5% for one-point measurements and 3% for two-dimensional
measurements. The gradients shown for the 2D-images were not
found to be related to fluctuations of the laser or to unevenness of
the coating.
Measurements of piston temperatures in diesel engines are also
of great importance and could assist in improving current heat
454 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 52. Optical fiber probe for thermometry in a production diesel engine [97].

transfer models, and also the thermal efficiency of such engines. In
Ref. [97], thermographic phosphors were used for piston ther-
mometry of a single-cylinder heavyduty diesel engine based on the
Volvo Truck D12C motor. A production piston with an omega-sha-
ped bowl generating a compression ratio of 18.5:1 was investigated.
It was equipped with thermocouples at the surface and on the
squish area. To access the piston optically, one exhaust valve was
removed and was replaced by a quartz window or an optical fiber
based probe, which is shown in Fig. 52.
The phosphor particles were coated on the piston and the
binder was dried with hot air. The third harmonic from an Nd:YAG
laser at 355 nm, was used to excite the phosphor particles. In these
tests two phosphor particles were investigated Mg3GeO4:Mn and
La2O2S:Eu. The Mg3FGeO4:Mn particles were used to investigate
the temperature of the piston, the La2O2S:Eu was used then to
optimise the measurements. One of the advantages of La2O2S:Eu
over Mg3FGeO4:Mn is its short lifetime, which allows measure-
ments at each crank angle position to be performed at an engine
speed of 1200 rpm. Fig. 53 shows results using La2O2S:Eu. The
surface temperature was measured at different crank angle posi-
tions. Between 270 and 350 CAD, the piston was moving upwards
in the compression stroke, the air being compressed. Compression
of the air induced a temperature rise from 237 to 257  C. At TDC the
fuel was injected. Shortly thereafter, combustion began and lasted
until 380 CAD. Combustion was terminated at a crank angle greater
than 400, a cooling process being noted then. Due to the intense
background, which swamped the phosphorescence signal, no
measurements between 350 and 380 CAD could be performed.
Nevertheless, the surface temperature during combustion at 370
CAD was only w5  C higher than that at 380 CAD, as deduced from
the thermocouple measurements.

Point 1, CAD −57

200

190

180
Temperature /°C

170

160

150

140

130

120
0 2 4 6 8 10 12 14 16
Time / s (std = 0.72667)

Fig. 53. Temperature versus crank angle. The boxplot represents data from 50 samples Fig. 54. A series of 150 consecutive single-shot images measured at 10 Hz at 57 CAD
[97]. BTDC. The standard deviation is 0.73  C [198].
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 455

Mean temperature with std for wall and gas / oC emission at 538 nm, was used because of its very high sensitivity, in
the range 100e300  C. An oscilloscope, able to record the PMT signal
for every engine cycle, i.e. at a 10 Hz frequency, was used for signal
210 1400 recording. The first measurements made were to test the precision of
the technique. As shown in Fig. 54, the standard deviation when
Wall temperature / C (−x−)

measuring during motored operation at 57 CAD Before Top Dead

Gas Temperature / K
200 1200

Center (BTDC) was as small as 0.73 K, or 0.2%, at 433 K ( ¼ 160  C).

o

190 1000 Note that this data includes both measurement error and real cycle-
to-cycle temperature variations.
180 800 Measurements such as those in Fig. 54 were made at different
crank angle degrees to investigate the temperature variations due to
170 600 combustion. Mean temperatures for each of these measurements, as
shown in Fig. 55, follow the gas temperature trend rather closely. The
160 400 wall temperature was found to oscillate about 60 K in every cycle.
Investigations made of the wall temperature response to different
150 200 engine loads are reported in Ref. [198]. About 150 single shots. The
−100 −80 −60 −40 −20 0 20 40 60 80 100
gas temperature is calculated from the pressure trace [198].
CAD / deg

Fig. 55. Mean wall temperature in a single point for different CAD-values. The error-
bars represent the standard deviation for the respective single measurement series, 5.6. Additional applications
calculated in each case from about 150 single shots. The gas temperature is calculated
from the pressure trace [198].
5.6.1. TP on a heated plate
In Ref. [199] 2D temperature measurements on a hot plate heated
The probe with the optical fibres showed clear potential for by an impinging laminar flame jet were carried out to validate
production engine thermometry under conditions where more certain heat transfer models developed by Eindhoven University of
intrusive optical access is not an option. The results obtained using Technology. The measurements were conducted on the cool side of
thermocouples and those obtained using thermographic phosphors a fused silica plate, heated from underneath by an oxy-fuel flame jet,
were found to agree rather well. The differences between the two see Fig. 56. Measurements were made using YAG:Dy and the ratio
were attributed to effects, such as the non-uniformity of the piston method, see Section 3.3; 355 nm radiation from an Nd:YAG was used
temperatures and also soot deposits, which could act as a thermal to irradiate the coated 100  100 mm plate.
barrier. To develop the technique further, the blue-emitting phos- Results of measurements using a hydrogeneoxygen flame are
phors (described in Section 4) with high sensitivity cold be used. In shown in Fig. 57. After eight seconds of heating the temperature was
addition, an acquisition system monitoring the surface temperature measured as being about 700 K in the middle of the plate, decreasing
of a multi-cylinder production engine at several points simulta- radially from the center. The measurement results correspond
neously would be of interest to develop. closely to the heat model, as can be seen at the right in Fig. 57
Wall temperature measurements have also been performed in an
HCCI engine by use of TP and the lifetime method. The aim was to 5.6.2. TP on a moving target
obtain single-shot cycle-resolved measurements while altering load An investigation of the feasibility of using a reasonable fast
and EGR. The work is presented in Ref. [198]. The phosphor La2O2- phosphor, i.e. a phosphor with a short lifetime, for 2D temperature
S:Eu was used for the measurements. Phosphor spots were applied measurements on a spinning target was made in testing the
to the ceiling of the combustion chamber at 6 locations, an Nd:YAG potential for measurements on gas turbines rotor blades. To simulate
laser producing 355 nm radiation being employed for excitation. A the speed of a gas turbine rotor a rotating disc, spinning at
PMT was used for detection through an interference filter centred at 21000 rpm, was placed in a pressurized combustion rig. The disc was
540 nm and having a Full Width Half Maximum (FWHM) of 10 nm, spray-coated with BaMg2Al10O17:Eu (BAM). BAM has a lifetime of
used to suppress emission wavelengths other than the phospho- about 2 ms at room temperature. An Nd:YAG laser producing 355 nm
rescence peak of interest. For these measurements the phospho- radiation was used for excitation and an ICCD camera equipped with
rescence peak originating from the 5D1eF relaxation, producing a stereoscope and the filters discussed earlier was used.

Fig. 56. Left: the setup for 2D temperature ratio measurements of a hot plate using YAG:Dy. Right: photograph of the fused silica plate and the flame. The white phosphor coating on
the upper surface can be seen through the quartz. The red glow is due to black body radiation from the spot where the flame hits the plate [199].
456 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461

Fig. 57. Temperature distribution of the cold side of the plate after 8 s (left) and the isothermal contours obtained (middle); the center of the hot spot is indicated by the asterisk.
The plate was heated by a hydrogeneoxygen flame. Right: temperature as a function of radial distance [199].

The disc had a diameter of 90 mm and it was motored at
21,000 rpm which corresponds to a speed of 100 m/s at the edge of the
disc, or a movement of 100 mm/ms. Fig. 58 shows a photograph and
single-shot images of the disc using an exposure time of 100 ns. As can
be seen in the image there is no motion blur even at these high speeds.
The test shows that 2D measurements on fast-moving targets are
feasible given that a phosphor with a sufficiently short lifetime is used.
5.6.3. Measurements through diffusive scattering in solid materials
Very recently a new application of thermographic phosphors
relying on diffusive scattering in a solid material has been described
[200]. The phosphor material was deposited on the surface of a piece
of polystyrene. Since the polysterene is a solid material which to
a certain degree will transport light through diffusive scattering,
measurements should also be possible to perform through the
material, i.e. from the backside. When using the phosphorescence
decay time for thermometry through scattering media, the time
delay caused by scattered light has to be much shorter than the
emission lifetime. This is the case in the present application.
The experimental set-up is shown in Fig. 59 (Left).
The experiments were performed on expanded polystyrene. The
reason for choosing this material is that it is commonly used for
thermal insulation of buildings and surface temperature
measurements are of great interest for fire safety studies. It is also
one of the most favorable materials with respect to the low density
and the non-absorbing properties letting light from different
wavelengths to pass through. The emission was collected using
spherical lenses and focused onto two identical Photo Multiplier
Tubes (PMT), one directly detecting the emission from the surface
and one detecting the diffusive scattered emission through the
polystyrene. Dichroic mirrors reflecting 266 nm light and high-pass
glass filters were used to avoid any laser light reaching the PMTs.
The tests were performed in a standard cone calorimeter test rig.
The test started at room temperature and the surface temperature
of the polystyrene was measured as it was exposed to a steadily
increasing irradiance from the cone heater.
The measurements worked satisfactory up to a temperature of
about 100  C. For higher temperatures, the material formed a mel-
ted pool and some slow pyrolysis took place. Fig. 59 (Right) shows
the resulting temperature when measured by detecting the emis-
sion directly (from above) and through the styrene, when the
sample was slowly heated to 90  C.
The test series proved that it can be possible to measure the
surface temperature by analyzing the thermographic phosphores-
cence emission that is diffusively scattered through the medium.
5.6.4. Free flow applications
So far the application of LIP has been limited to surface and/or
liquid thermometry. However, it seems quite promising, especially
with the new very sensitive phosphor particles ZnO:Zn and ZnO:Ga,
also to probe the gas flow temperature. The first demonstration of this
kind was shown in [201], where the phosphor particles were seeded
to a heated gas flow and then probed both for thermometry and flow
studies. The experimental set-up is shown in Fig. 60. The thermo-
graphic phosphor Mg4FGeO6:Mn in this investigation used both for
temperature measurements and as flow tracers for simultaneous PIV
measurements, were seeded into the flow. The particles were
dispersed in alcohol and transported by compressed air streaming

Fig. 58. Images of a rotating disc mounted in the pressurized combustion rig. At the left a photograph of the disc when mounted in the pressurized chamber is shown. The disc is
coated with the thermographic phosphor BaMg2Al10O17:Eu, emitting in the blue region after excitation by 355 nm laser radiation. A single-shot TP-image, with 100 ns gate width, is
shown to the right. Note that the stripes are still clearly visible even at this high rotation speed (21,000 rpm).
 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461 457

Fig. 59. Left: experimental set-up for thermometry using diffusive scattering. Right: temperature measurements as measured from both side of the expanded polystyrene [200].

through the nebulizer creating a fine spray carrying the particles.
During the passage trough the heated tube the alcohol evaporated
and particles and air were heated gradually (to approximately 400  C)
before exiting into the ambient. Two separate laser and detector
systems were used for the simultaneous velocity (PIV) and temper-
ature measurements. The counter-propagating laser beams were
formed into overlapping sheets to illuminate a planar region along the
centerline of the flow to be investigated.
For PIV the beams from two frequency doubled Nd:YAG lasers
(Quantel) were overlapped to provide successive Mie-scattering
images from the phosphoric particles. For imaging an interline-
transfer CCD camera (PCO) was used. For the evaluation of the
velocities, a cross-correlation algorithm with an adaptive multipass
method developed by LaVision was used [202].
For temperature measurements the third harmonic generation
of an Nd:YAG laser at 355 nm, with a pulse duration of 7 ns and
a repetition rate of 10 Hz, was used to excite the particles at the
outlet. The thermometry light sheet matched the sheet for the PIV
measurements. The subsequent phosphorescence emission was
detected by an intensified CCD camera together with an imaging
stereoscope. The collected emission first passes through separate
filters before encountering the stereoscope, producing identical
images of the same object on corresponding halves of the CCD
chip.
The technique was tested on a re-circulating flow with a higher
degree of mixing. A conical bluff body was centered and placed
5 mm above the outlet from the heated tube, creating a flow with
a recirculation zone in the centre, see Fig. 60. The data were
produced by averaging 50 instantaneous samples. As can bee seen
in the figure the flow was not perfectly symmetric and the highest
velocities (and mass flow) were found on the right-hand side. This
also influences the temperature field with higher maximum
temperatures and a larger area with temperatures above 300  C. In
the central recirculation zone areas with lower average tempera-
ture than the flow passing outside are found. This could be caused
by cooling from the metallic bluff body or by entrainment of cooler
air into the recirculation zone.
This thermal flow diagnostic relying upon a seed is based on
assumption that the small seed particles should have the same
temperature relative to the surrounding medium. However, funda-
mental investigations of the sensitivity of the particles for various gas
phase measurements are necessary. The authors have addressed this
subject initially using simple heat transfer calculations based on heat
convection from the surrounding flow to a suspended or a free falling
particle, and found that particle diameter and density contribute to
the measurement sensitivity to temperature change. For example
particles having a 1 mm diameter and a density of 2 g/cm3 would yield
a response time of 10 ms when subjected to a 400  C step change.

Fig. 60. Experimental set-up (left). Simultaneous measurements of temperature and velocity of the turbulent flow behind a conical bluff body (right) [201].
458 M. Aldén et al. / Progress in Energy and Combustion Science 37 (2011) 422e461
Smaller diameters and lower densities generate a shorter response
time. For an accurate measurement of both velocity and temperature
the particles used should be as small as possible. For metal oxide
powders often used for PIV, it is vital that the size is around 1mm or
smaller for the particles to follow rapid fluctuations in a flow properly.
It should also be noted that the life time of Mg4FGeO6:Mn in the
present temperature range is of order 1 ms (see Fig.16), which is of the
same order as the integral time scales (w450 ms) in the investigated
flows. With a more sensitive phosphor (shorter decay time) the
temporal resolution and measurement accuracy could be improved.
Clearly also from this perspective the ZnO:Zn and ZnO:Ga phosphors
would be the optimum choice for future investigations.
Another example of TP’s applied for thermometry in gaseous
free-flows can be fond in [203]. In that work the possible issue of
laser-induced heating is investigated. Furthermore, the temporal
response, of the TP particles, to a step change in gas temperature is
briefly discussed and estimated to be on the microsecond scale.
This topic is of course very critical for measurements in the gas
phase and more investigations are required. Thermographic phos-
phors have also been used for gas thermometry in IC engines [204].
6. Conclusion and outlook
Thermographic phosphors have been shown to be useful for
temperature measurement under a variety of combustion condi-
tions. In flamespread experiments, UV- or blue-emitting thermo-
graphic phosphors have been found to be suitable for surface
thermometry in the vicinity of flames. Most existing UV- or blue-
emitting phosphors, however, fail to encompass the temperature
range for use of the lifetime measurement technique in flame-
spread applications (temperatures of between 20  C and w700  C).
The thermographic phosphor BaMg2Al10O17:Eu was on the other
hand shown to be a suitable candidate, providing an acceptable
degree of temperature sensitivity in the region between 300  C and
800  C, although further technical development of the use of this
phosphor is needed for applications of this sort.
In internal combustion engines, existing thermographic phos-
phors, such as La2O2S:Eu allow surface temperature measurements
at 1200 rpm to be made at a resolution of one crank angle degree.
This red-emitting phosphor has been applied to surface tempera-
ture measuremenst inside an HCCI engine during combustion. This
is possible because of the nature of the flames in HCCI engines. The
flames are here blue and less sooty than those in Diesel engines, in
which the flames are sometimes yellowish and very sooty. Still it
was found that thermographic phosphors can be used in combi-
nation with fibre-optics to probe Diesel engines in which ordinary
optical access is precluded. In multi-cylinder engines, an acquisi-
tion system based on use of thermographic phosphors and optical
fibres would allow temperature measurements to be performed at
the same time in each of the running cylinders. This would provide
extensive opportunities for thermographic phosphor based tech-
niques to be used in tests of ordinary production-type engines.
Use of thermographic phosphors for temperature measure-
ments of droplets and sprays has been demonstrated by several
groups. It was found that the need of optimising the mixing of
thermographic phosphors with the liquid could be reduced if
smaller particles are employed. Use in this connection of the
nanophosphor particles being developed today would facilitate the
measurement of sprays. Use of such nanoparticles in gas ther-
mometry would also appear promising. These nanoparticles are
more sensitive to temperature variations than microparticles in the
gas phase due to their lower mass, allowing them to reach thermal
equilibrium with the surrounding gases more quickly. Recently,
synthesis of nanophosphors has made a significant progress.
Several methods have been developed to synthesize nanosized
oxide and fluoride (with and without silica coating) phosphors, e.g.
[128,205] The availability of uniform and optically efficient nano-
particles provide opportunities for more accurate temperature
measurements using phosphors and there have been some appli-
cations of nanophosphors for thermometry, e.g. [35,36].
An area of highest interest in using thermographic phosphors for
gas phase thermometry is its potential application for in-situ
measurements in flames. With the precision shown in Ref. [120] for
single shot 2D measurements, a similar approach would certainly be
very attractive in flame environments. However, such measure-
ments have still not been demonstrated due to the lack of suitable
phosphors. Preliminary measurements have indicated challenges to
suppress background emission due to spontaneous black body
radiation as well as laser-induced incandescence, LII. Clearly new
phosphors yielding sufficient signal at flame temperatures with
shorter lifetimes as well as emission in the UV spectral regions are
still to be shown. Also issues on quenching and the high temperature
influence on emission characteristics have to be addressed.
Preliminary investigations have been made in this area, e.g investi-
gations on the influence on quenching from oxygen [102]. It has also
very recently been reported that thermographic phosphors
(YAG:Dy) captured after a flame environment “survive” the high
temperature region in the flame and show very similar emission
characteristics as before the flame [206]. Furthermore, a recent
report indicates that the use of the higher laser power needed when
using thermographic phosphors for gasphase thermometry may not
cause extra complications, e.g. heating of the particle.
LEDs and laser diodes for excitation of thermographic phos-
phors present new methods that hold particular promise. Cheap
laser diodes and LEDs are now available in the UV region. LEDs are
possible to purchase with emission wavelengths down to 250 nm.
Using LEDs and phase shift methods for lifetime evaluation,
compact probes can be developed for a fraction of the price of such
equipment using conventional high power lasers. This could
present the first true opportunity for temperature probing using
thermographic phosphors to be fully commercialized.
It is clear that the use of thermographic phosphors for ther-
mometry in combustion environments has a great potential due to
its ease of operation, strong signals and low requirement of
advanced/expensive equipment and we will see new applications
emerging along with new phosphors found as well as with the
advancements of new light sources and detectors. An interesting
approach is also to use tailor made phosphors with characteristics
optimized for each specific application. Such activities have been
presented by, e.g. Eckert et al. [207].
Acknowledgements
The authors greatly acknowledge the support from the Swedish
Energy Agency, STEM through CECOST and KCFP.
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