Photothermal spectroscopy: A promising

tool for nanofluids

Cite as: J. Appl. Phys. 128, 190901 (2020); https://doi.org/10.1063/5.0024332
Submitted: 06 August 2020 . Accepted: 28 October 2020 . Published Online: 16 November 2020

Liliya O. Usoltseva, Mikhail V. Korobov, and Mikhail A. Proskurnin

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Paper published as part of the special topic on Photothermics PHOTOTHERMICS2020

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J. Appl. Phys. 128, 190901 (2020); https://doi.org/10.1063/5.0024332 128, 190901

© 2020 Author(s).
 Journal of PERSPECTIVE scitation.org/journal/jap
Applied Physics

Photothermal spectroscopy: A promising

tool for nanofluids
Cite as: J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
Submitted: 6 August 2020 · Accepted: 28 October 2020 · View Online Export Citation CrossMark
Published Online: 16 November 2020

Liliya O. Usoltseva, Mikhail V. Korobov, and Mikhail A. Proskurnina)

AFFILIATIONS
Chemistry Department, Lomonosov Moscow State University, Moscow 119991, Russia

Note: This paper is part of the Special Topic on Photothermics.

a)
Author to whom correspondence should be addressed: proskurnin@gmail.com

ABSTRACT
In recent years, the demand for more efficient cooling circuits has resulted in active studies of nanofluids, two-component liquids consisting of
a base fluid, and dispersed nanoparticles with high thermal conductivity. From the viewpoint of both physics and chemistry, nanofluids are
systems that require the characterization of many interconnected thermal and chemical properties. This perspective article sums up the state of
the art and recent trends in the development and applications of nanofluids and especially carbon nanofluids. A focus of the paper is the pos-
sibilities of photothermal and photoacoustic methods—as techniques combining molecular spectroscopy and thermal characterization—for the
assessment of thermal conductivity and thermal diffusivity of nanofluids. The possibilities of photothermal spectroscopy for wider characteri-
zation of nanofluids and related materials are discussed and compared with other techniques. As nanofluids are one of the examples of
complex objects dedicated to photothermal spectroscopy, more general outlooks of phototermics are also discussed.

Published under license by AIP Publishing. https://doi.org/10.1063/5.0024332

I. INTRODUCTION summing up nanofluid composition and properties2,3,7–12,14–17,19–26

Many state-of-the-art industries as well as critical technologies
such as nuclear and solar energetics, microelectronics, and com-
puter technologies require efficient cooling systems, which mainly
rely on liquid circuits.1–5 Most often, the coolant fluids in such cir-
cuits are water, ethylene glycol, and various oils.6–8 However, their
thermal conductivity is not always sufficient, which gives an incen-
tive to search for ways to enhance the heat transport. Over the past
15 years, two-component liquid coolants consisting of a base fluid
and dispersed nanoparticles (NPs) with a size range of 1–100 nm,
nanofluids (NFs) have been actively studied and implemented.4,5
Such coolants increase the heat-transfer efficiency due to high
thermal conductivity of the disperse phase. Of special interest are
carbon nanofluids (CNFs), which are very advantageous due to
their high thermal conductivity and chemical inertness.
In the past three to four years, the number of papers in this
field has increased significantly, both in the field of new materials
to create NFs and in approaches to use NFs for solving topical
problems. According to Web of Science®, there has been an expo-
nential increase in the number of publications on this topic, and
over the past five years, more than 12 000 publications have been
issued. The research on NFs has resulted in numerous reviews9–18
as well as their applications2,3,18 or dedicated to specific types of
NFs such as CNFs.14,23,27–29
From the viewpoint of both physics and chemistry, nanofluids
have many interconnected properties. For both technological and
medical applications, the key NF parameters are thermal conduc-
tivity, viscosity, and heat capacity of dispersions. It is thus impor-
tant to have methods that can adequately determine these
parameters. Moreover, the application of NFs in industry and at
some facilities require the chemical composition, size, and concen-
tration of nanoparticles along with thermal parameters. Finally, an
important practical task is the constant control or monitoring of
thermal parameters, concentrations, and the composition of the
dispersed phase during their prolonged operation as the chemical
transformation, aggregation, or other processes may seriously
change the properties of the nanofluid.
A single method is incapable of solving all these tasks; thus, the
development of methods that provide a comprehensive diagnosis of
NF is required. Photothermal methods combine the possibilities of
both optical/IR techniques of molecular spectroscopy and thermal
characterization. Photothermal spectroscopy (PTS) has a high sensi-
tivity for the determination of small amounts of substances, provides

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a high accuracy of thermal parameters, and is not destructive.30–37
Photothermal spectroscopy is promising for the characterization of
disperse systems of various nature, from natural to engineered nano-
size objects.30,38–43 Thus, the development of the methodology of
photothermal spectroscopy for nanofluids and their use in nanofluid
applications is relevant.
The aim of this perspective paper is to review the recent trends
in development and applications of nanofluids, especially carbon
nanofluids, and discuss the outlooks of photothermal methods in the
characterization of thermal parameters of nanofluids as well as in a
more comprehensive characterization of these materials.
II. NANOFLUIDS
The term “nanofluids” is somewhat ambiguous as it may refer
to heat-transfer nanofluids as well as “nanofluidics” as the minia-
turized flow techniques in nanometer-size channels (We avoid the
term “nanofluidic” in this paper due to this ambiguity.). Moreover,
nanofluids used for heat transfer are divided into two types: heat-
conducting and heat-accumulating (thermal storage) nanofluids.
Heat-conducting nanofluids provide an explicit gain in the thermal
conductivity in comparison with the base fluid, thus improving the
critical heat flux. Thermal-storage nanofluids are used for heat
accumulation by the fluid followed by their release after a certain
time or in a specific place of the circuit by forced heat transfer.44,45
An increase in the thermal conductivity of the medium as a
whole in a NF may be explained by the contribution of the disperse
phase through an effective medium theory, with the most conven-
tional static model based on Maxwell’s equations,46
3wnp (x  1)
knf /kbf ¼ 1 þ : (1)
(x þ 2  wnp (x  1))
Here, the increase in the thermal conductivity of NF knf over the
base fluid kbf is determined by the volume fraction of nanoparti-
cles wnp and the constant x ¼ knp /kbf , where knp is the thermal
conductivity of nanoparticles. The developed model considers sta-
tionary spherical nanoparticles in the base fluid and take into
account only the volume fraction of nanoparticles.47,48 However,
in many cases, the effect of nanoparticle concentrations cannot be
described by this simple equation as the heat transfer in
nanofluids may be the result of nanostructures formed (Fig. 1)
involving multiple heat-transfer mechanisms: Brownian motion
(still controversial since it is too slow in comparison with heat
diffusion; however, it could have an important indirect role in
particle clustering), liquid layering at a liquid–particle interface,
heat transport in nanoparticles (ballistic conduction), or nano-
particle clustering.49–51
Sometimes the dispersed nanoparticles act as thermal insula-
tors; for example, even metallic powders can be as insulating as
ceramic powders.52 Also, aerogels are considered one of the most
promising insulation materials.9 For nanoscale objects, interfacial
contact resistance plays an important role in heat transfer.
Basically, certain attempts are made to reduce the resistance and
enhance thermal conductivity. Molecular-dynamics simulations
reveal that ordered water layers around nanoparticles53 and polar
functional groups54 lead to a low Kapitza resistance and enhance local
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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thermal conductivity of the water shell adjacent to the nanoparticle.55
However, some scientific groups are interested in systems, in which
thermal diffusivity decreases with nanoparticle concentrations.
Studies reveal carbon56 and CdTe57 quantum dots to be promising
candidates as thermal insulating materials.
Thus, to be considered a practical heat-conducting nanofluid,
a disperse system must have not only a high thermal conductivity
but also a low viscosity, ideally equal to the viscosity of the base
fluid. The latest advances in nanoscale fabrication make it possi-
ble to produce metallic and nonmetallic particles with a wide
range of mechanical, optical, electrical, and thermal properties,
which can be used as a disperse phase of nanofluids.2 The main
types of nanoparticles and NFs and their applications are pre-
sented in Fig. 2.
Metal nanoparticles usually include but not limited to alumi-
num, copper, silver, and gold since they were quite widespread and
well-known colloidal systems.4,5,58,59 However, they are chemically
active, which leads to the impossibility of using them in a number
of areas, as well to their rapid deterioration.1,2,23,60 Their use is
most widespread in nuclear energetics and closed circuits.1,61 For
noble-metal particles, the disadvantage of NFs is the price of large
volumes of nanoparticles. The second type of NFs is nanoparticles
of metal oxides, such as Al2O3, Fe3O4, CuO, TiO2, etc.4,58,59 They
are less expensive than metal particles but also have lower thermal
conductivities.
In the past decade, the number of publications devoted to the
study of thermally conductive CNFs increased dramatically.4,9,23,62–73
Here, main carbon nanomaterials—single-wall (SW) and multiwall
(MW) carbon nanotubes (CNTs), nanodiamonds, graphene oxide,
carbon dots, etc.—serve as the disperse phase. They are less reactive
in comparison with metals and oxides69,74–81 and are stable and
environmentally friendly;82,83 thus, they cause less corrosion, are less
prone to sedimentation, do not clog communication lines, etc. They
are discussed in more detail in Subsection II D.
The above-mentioned nanofluids belong to the single-phase
class. In recent years, a novel NF class consisting of two solid mate-
rials dispersed in a fluid has appeared, hybrid nanofluids.12,16 These
NFs lead to a further increase in thermal conductivity. Among
hybrid NFs are all mixtures, of the same or different types of nano-
particles: from metals and oxides to CNTs, carbon dots, and micro-
encapsulated phase-change materials (MEPCMs).12,16 For example,
the authors of the paper73 succeeded in producing nanofluids
based on hybrid nanoparticles from functionalized MWCNTs and
graphene in de-ionized water and ethylene glycol without stabil-
izers. For a system on de-ionized water, an increase in thermal con-
ductivity of 20% relative to the base fluid was observed at a volume
fraction of hybrid nanoparticles of 0.05%.73 However, hybrid nano-
fluids, even more than single-phase ones, require the research of
combinations of nanoparticles, their mixing ratio, the stability of
hybrid nanofluids, etc., as well as understanding the mechanisms
that contribute to the total heat-transfer enhancement.12,84
As a whole, three major research directions of NF are (1) the
search for systems of new potential nanofluids; (2) applying the
well-studied nanofluids in various industries, e.g., in the field of
energetics; and (3) describing and predicting the thermophysical
properties of nanoparticle-based fluid systems using models such
as the Maxwell or Hamilton–Crosser models.25,58,69
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FIG. 1. Nanofluid types: TEM images of the microstructures of (a) ordinary and (b) functionalized nanofluids of silica nanoparticles and (c) an Al2O3–water nanofluid.
Reproduced with permission from X.-F. Yang and Z.-H. Liu, Nanoscale Res. Lett. 6, 494 (2011). Copyright 2011 Author(s). Reproduced with permission from
Khaleduzzaman et al., Procedia Eng. 105, 406 (2015). Copyright 2015 Author(s).
A. Methods for nanofluid preparation
Regardless of type, two-stage or one-stage approaches are
used to produce nanofluids. Naturally, depending on the nature
of nanoparticles and the base fluid, the conditions, e.g., the treat-
ment protocol, time, or concentrations, may change, but the prin-
ciple does not. Most often, a two-stage production approach is
used. Here, nanoparticles are first synthesized in a dry form by a
chemical or physical technology. At the second stage, the result-
ing nanoparticles are dispersed into a liquid by stirring, solvent
replacement, or sonication.5,7,58,59,85 To increase the system stabil-
ity, cationic or anionic surfactants are often used as additional
components.
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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If producing nanofluids by a two-stage method is difficult,
e.g., due to the impossibility of direct “dissolution” of nanoparticles
in the base liquid, a one-stage method is used, which omits the
stage of nanoparticle isolation after their synthesis. This involves
several approaches to producing nanofluids.
(a) The method of direct evaporation consists of the evaporation
of the material and the subsequent condensation of nanoparti-
cles right in the base liquid, which produces more stable dis-
persions due to a decrease in aggregation.5,7,25,58,59,85
(b) Chemical reduction is mainly used for nanofluids based on
metals and metal oxides. For this, a solution of a metal salt in
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FIG. 2. Types of nanofluids, their disperse phases, and their common applications and limitations.

the base fluid is obtained, and then a reduction reaction is
carried out, leading to the formation of the solvate into the
nanoparticle phase.25
(c) Nanofluids based on noble metals, silver, and gold are pro-
duced by laser ablation. A metal plate is placed in a base liquid
and a laser beam is focused on its surface, as a result of which
the metal evaporates and condenses in the base fluid.25
(d) Interfacial transfer is also used, which consists of dissolving the
precursor and its further transfer by carrier reagents (usually
amines) into the base fluid, where the chemical reaction of
nanoparticle synthesis occurs.25,59
The main disadvantage of a one-stage method is the difficulty of
removing impurities of unreacted substances from the resulting
nanofluid, which can affect the stability, thermal parameters, and
chemical and environmental properties.25
B. Nanofluid applications
The main areas of application of nanofluids are presented in
Fig. 3.9 In recent years, there has been a tendency toward the
miniaturization of already existing devices and machinery, which
also leads to a decrease in cooling circuits, in which a small
amount of refrigerant can no longer cope with the task of remov-
ing heat. The development of methods for obtaining energy from
alternative sources, in particular, the use of solar energy, is also a
prerequisite for the study of nanofluids and their application in
this field.
One of the industries in need of better cooling systems is
nuclear energetics, as the low thermal conductivity of water and
mineral oil, which are often used as base fluids, is a major limiting
factor toward greater compactness and efficiency of reactors.
Now, NFs with nanoparticles of metal oxides, copper, or aluminum
are often used.1,61

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FIG. 4. Maximum temperature of the CPU surface in terms of the Reynolds
number in different liquid blocks for the water and a hybrid nanofluid containing
graphene nanoplatelets decorated with silver nanoparticles. Reproduced with
permission from M. Bahiraei and S. Heshmatian, Appl. Therm. Eng. 127, 1233
(2017). Copyright 2017 Elsevier Ltd.
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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FIG. 3. Widespread application fields
for nanofluids. Reproduced with permis-
sion from Qiu et al., Phys. Rep. 843, 1
(2020). Copyright 2020 Author(s).
The next topical task in the development of NFs is solar
energetics. In this area, such NFs as Cu–water, Al2O3–water, CuO–
ethylene glycol, carbon nanotubes–oil, and Fe3O4–water are being
developed.2,86 Here, commercial solutions such as JJ Bioenergy Ltd
(UK) have appeared in the market.
Third, the power of computers constantly increases and the
advances in instrument making results in more and more miniature
electronic devices. However, during the operation of these devices,
a large amount of heat is produced, and the existing systems of air
and water cooling are not efficient, which leads to reduced stability
and a shortened service life of expensive computing systems. The
replacement of water with nanofluids results in a 10 ° lower tem-
perature of the processor (Fig. 4).4,5 NFs used in computer cooling
circuits include some commercially available solutions such as Ice
Dragon Cooling (http://www.icedragoncooling.com).
NFs are considered promising for various industrial appara-
tuses (evaporators, concentrating installations, etc.) and in many
chemical-industry processes to increase the efficiency and reduce
operating costs.87 To improve the cooling system, nanoparticles
such as Al2O3, Cu, and CuO can be used.60 As well, commercial
solutions such as HTF Compact Nano Thermo Fluid (HTF
Compact, TCT Nanotech, Italy) and Advanced Thermal Solutions,
Inc. (USA) have entered the market recently.
Nanofluids can be used as thermally conductive lubricants
for electric motors and other mechanisms as contributing to the
reduction of friction than traditional lubricants, which leads to
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the increased lifetime of mechanisms.23,60 Also, they start to find
applications in deep-hole drilling as heat sink and lubricant
solutions.88
In the regions where the average daily temperature is quite
low, heating systems for houses are used. They work due to the cir-
culation of, most often, a mixture of water and ethylene glycol.
The use of nanofluids in such systems makes them more compact
without a loss of efficiency of heat transfer; also, due to the lubricat-
ing properties of nanofluids, the service life of pumps for the circula-
tion of the liquid increases.59 This direction is interconnected with
the next stage of development of Internet of Things, in which smart
cooling circuits at the appliance and house levels are required.89
Finally, tests of NFs in two-phase thermosyphons as advanced
heat-transfer technologies in applications from energy conversion
systems to electronics cooling have started.90 A closed two-phase
thermosyphon utilizes the countercurrent flow of a liquid and a
vapor for heat transfer and consists of a liquid pool contained in
the heated section or evaporator, an adiabatic section, and a cooled
or condenser section.91 NFs may play a crucial role in thermosy-
phon efficiency.
The use of heat-conducting nanofluids is not limited only
to the tasks of efficient heat removal. Many nanofluids, espe-
cially CNFs based on carbon nanoparticles, are considered
potential biocompatible thermal or photothermal materials for
thermal-transport drug delivery, therapeutic purposes,92–94 or as
theranostic agents—bio-nanofluids.95–98 Bio-nanofluids based
on nanodiamonds and carbon dots are advantageous due to
their low cytotoxicity, high water solubility, favorable biocom-
patibility, and good photostability;99 in several cases, they
provide other important properties such as light absorption, IR
emission, or fluorescence.100,101 Due to these features as well as
easy bioconjugation and a high specific surface area, they are
perspective materials in biomedical imaging and sensing. This
requires reliable and much more detailed information about the
physicochemical and thermophysical properties of bio-nanofluids. In
particular, precise values of thermal diffusivity and thermal conduc-
tivity are required for understanding the mechanism of laser therapy
and theranostics, e.g., for switching between photochemical and pho-
tothermal modes,102–104 calculating the dose and irradiation parame-
ters, predicting the risk factors, etc.105
C. Nanofluid target parameters
The main characteristics of both technological and biomedical
purposes of thermally conductive NFs are thermal conductivity
and thermal diffusivity.9,11,19,85,106,107 The latter characterizes the
rate of heat transfer throughout the material; thus, it is usually
obtained from the measurements (transient methods), and it is
directly related to thermal conductivity. Thermal conductivity k
and thermal effusivity eT can be calculated from the experimental
thermal diffusivity DT and from the specific heat and density
(or volume heat capacity CV ¼ ρCP ) of the test sample,
k ¼ ρCP DT , (2)
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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pffiffiffiffiffiffiffiffiffiffi pffiffiffiffiffiffi
eT ¼ kρCP ¼ ρCP DT : (3)
Thermal effusivity is somewhat undervalued in NF research,
but it is very important as a measure of ability of the sample to
exchange heat with the materials in contact and determines the
contact temperature Tc of two objects that touch each other as
T1 e1 þ T2 e2
Tc ¼ , (4)
e1 þ e2
where T1 and T2 are temperatures and e1 and e2 are thermal effu-
sivities of objects. It is important that this property can be directly
measured by photothermal techniques such as photopyroelectric
(PPE) and thermal-wave resonator cavity (TWRC) techniques as
well as photoacoustic (PA) modalities (Sec. IV A).
The volume fraction of the dispersed phase is one of the
parameters that can be varied to obtain disperse systems with the
required thermophysical properties. This parameter affects the
thermal conductivity of the colloidal system, which begins to
increase starting from a certain concentration of nanoparticles,
while below which the thermal conductivity remains indistinguish-
able from the base fluid.5,29,47,106 With a large volume fraction of
the dispersed phase, sedimentation processes begin to occur, which
result in a decrease in the stability and efficiency of NFs. The con-
centration of nanoparticles as well as the conditions for preparing
dispersions affect the size of nanoparticles,108 which alters the ther-
mophysical properties of NFs. Typically, thermal conductivity
increases with a decrease in the nanoparticle size.5,47,106 Thus, it is
necessary to determine the volume fraction of the dispersed phase
and monitor its change during NF operation (Fig. 5).
The introduction of the dispersed phase into the base fluid
makes it possible to aim other properties of the fluid.5–8,24 An
important parameter of nanofluids that has received less attention
compared to thermal conductivity is the volume heat capacity.
Different nanoparticles may decrease or increase the specific heat
compared to the base fluid.21,85 Also, the nature of nanoparticles
affects the temperature dependence of Cp; it can either increase or
decrease with temperature. The Cp value is also affected by the
volume fraction of dispersed particles in the nanofluid. To date,
there is no fully reliable model for the heat capacity of nanofluids.
Nanoparticles increase the dynamic viscosity of the fluid,
which is a negative effect for any heat-sink and heat-transfer appli-
cations. Thus, the dynamic viscosity is the second most important
parameter that determines the applicability of nanofluids.109,110 As
a rule, the dynamic viscosity increases with a decrease in the size of
nanoparticles.
Even if a disperse system has thermophysical parameters that
ensure an efficient heat transfer, it cannot be called a nanofluid if it
has a low sedimentation stability.10,70 The aggregation leads to sedi-
mentation and may reduce the thermal conductivity due to a lower
mobility of nanoparticles. The presence of a stabilizer (dispersant)
increases the stability of the colloidal system and makes it possible
to obtain dispersions with a larger volume fraction of the dispersed
phase.5,29 However, the amount of dispersant also affects the
thermal conductivity; as the dispersant concentration increases, the
thermal conductivity may decrease.5,29 For this, the methods of
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light scattering, sedimentation, or spectrophotometry are used, and
the electrokinetic potential is also measured.10,15,22,25 This parame-
ter provides a value characterizing the stability of nanofluids and
also shows the surface charge of nanoparticles in the system.25,85
Thus, an important task is to find the optimum content of
nanoparticles and extra reagents and the conditions for obtaining
the most efficient system with the highest possible stability. Most
studies are directed toward devising new nanofluids rather than
finding the optimal parameters for the efficient use of already
designed dispersed systems.
D. Carbon nanofluids
The special interest of CNFs results from high thermal con-
ductivities of carbon nanomaterials and chemical properties
(Fig. 6).64 This also makes CNFs more stable in time and
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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FIG. 5. The intrinsic mechanisms for
the influence of various factors on the
thermal conductivity of nanofluids.
Reproduced with permission from Qiu
et al., Phys. Rep. 843, 1 (2020).
Copyright 2020 Author(s).
environmentally friendly. Nanodiamonds and fullerenes and their
aqueous dispersions raise even a more serious interest as promising
biocompatible materials.95–98
Clinical studies impose other requirements on CNFs. Of
special control is the chemical composition and purity, toxicity,
etc.; thus, CNFs with the optimum thermophysical properties
cannot be directly proposed as bio-nanofluids.99,111–114 However,
many target properties of carbon nanofluids for heat sink and
medical problems match (stability in time, concentration of nano-
particles, low aggregation, etc.). Today, the research of CNFs is pro-
gressing in the following directions:
(a) Techniques for preparing CNFs with different concentrations
of nanoparticles are developed; the attempts to increase the
concentration in different ways (surfactant admixtures, ultra-
sound treatment, etc.) are made; and the stability of CNFs
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reveals itself as an important and not fully investigated
problem. It is noteworthy that stable aqueous CNFs find wide
applications in biomedical research. Carbon nanoparticles that
are stable in water are used for drug delivery, as contrast
agents, in photodynamic therapy, etc.115,116
(b) The studies of the effect of concentration, size, shape, surface
condition, type of nanoparticles, solvent, temperature on
thermal conductivity, heat capacity, and viscosity of CNFs are
performed;14,80,81,117,118 however, the systematic research in
this direction is almost not carried out.
(c) Methods of physicochemical characterization of CNFs are devel-
oped, in particular, reliable measurements of thermal conductiv-
ity in a wide range of concentrations.11,48,119,120 A challenging
task is the measurement of particle size in colloidal solutions
and monitoring the inevitable aggregation of nanoparticles in
CNFs. The existing methods (e.g., dynamic light scattering)
sometimes do not provide reproducible results.121
(d) Physical models that seek to describe the observed patterns,
especially the dependence of thermal conductivity of CNFs on
the type, concentration, shape, and size of nanoparticles, and
the properties of the base fluid are in development.9,20,107
Noteworthy is the proposed models that do not give an ade-
quate description of the thermal properties of CNFs and, in
most cases, are adapted for the description of systems contain-
ing metal rather than carbon nanoparticles.122,123
Carbon nanotubes are the most widespread materials for producing
CNFs. The disperse phase in this case, most often, is a mixture of
multi-walled carbon nanotubes as most accessible and cheap.124
However, single-walled CNTs are characterized by the highest (up
to 6000 W/m/K)64 thermal conductivity coefficient. As CNTs are
hydrophobic, stable dispersions (up to 1% v/v) require ultrasonic
treatment and a stabilizer surfactant.9 In this case, to correctly
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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FIG. 6. Thermal properties of carbon
allotropes and their derivatives (the
diagram based on average values
reported in the literature). Reproduced
with permission from A. A. Balandin,
Nat. Mater. 10, 569 (2011). Copyright
2011 Nature Publishing Group.
assess the increase in the thermal conductivity coefficient, it is nec-
essary to measure the base fluid with the same amount of the sur-
factant. In general, the addition of a surfactant does not affect
thermophysical properties; however, up to 6 wt. % cetyltrimethylam-
monium bromide may lead to a decrease down to 5% in the thermal
conductivity coefficient.65 An important parameter of carbon nano-
tubes is the length-to-diameter ratio; prolonged ultrasonic treatment
can decrease it and, as a consequence, degrade the thermal conduc-
tivity coefficient. As a rule, an increase in the number of walls also
negatively affects thermal conductivity.118,125 However, this regularity
is not observed in all the experimental studies.65 Since carbon nano-
tubes are two-dimensional flat structures rolled into a tube, the
models for the thermal conductivity of nanofluids need to be seri-
ously modified compared to other nanoparticles.9 Finally, CNTs are
toxic, which significantly limits their use.
For dispersions of hydrophilic nanoparticles, nanodiamonds
are widely used among CNFs capable of forming stable aqueous
solutions. Diamond has many unique properties,99 including a
high thermal conductivity coefficient (up to 2000 W/m/K).64
However, nanodiamonds are sp3 diamond cores covered with sp2
graphite-like phase shells, which are responsible for lowering
thermal conductivity.126,127 Therefore, the thermal conductivity of
nanodiamond-based CNFs directly depends on the purity and the
method of production of both nanodiamonds and the nanofluid.
Also, it is not entirely correct to translate the thermal properties of
bulk materials to nanostructures since the contact resistance is of
paramount importance, and the thermal conductivity regime can
change from a diffuse to a quasi-ballistic (collisionless heat trans-
fer). In addition, nanodiamond is a powder, and the heat-
conducting properties of the powder are formed by surface contacts
of spherical particles and the thermal conductivity of the gas gaps
in the vicinity of thermal contacts. The thermal conductivity of
powders is much lower (by a factor of 10–100) than the bulk
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material. Not many studies deal with the thermal conductivity of
nanodiamonds. Composites obtained from detonation nanodia-
monds sintered at pressures of 5–7 GPa and temperatures of 1100–
1900 °C were studied; rather low (of the order of 10–50 W/m/K)
values of the thermal conductivity of detonation nanodiamonds
were found.126 They used a home-made setup for measuring
thermal conductivity by a stationary heat flux. Another research
group used a commercial analyzer based on a modified transient
plane source (TPS) method and equipped with a special kit for
testing powders and liquids.127 Even lower (tenths of W/m/K for a
porosity of 88% or a relative density of 12%) values of thermal con-
ductivity for nanodiamond powders were obtained. The authors
theoretically calculated the thermal conductivity according to the
modified Maxwell model. The calculations are in good agreement
with the experimental data, and the extrapolation of the model to
low (0.1%) porosity indices showed that the thermal conductivity
strongly increases when the nanodiamond powder becomes a solid
material. The values are in good agreement with the previous
data.126 The thermal conductivity of nanodiamonds was also calcu-
lated by molecular dynamics.127 The thermal conductivity of nano-
diamonds decreased from 28 to 10 W/m/K with a decrease in the
sp3 carbon fraction until the number of sp2 bonds exceeded the
number of sp3 bonds. Furthermore, the thermal conductivity is less
sensitive to a further increase in the sp2 fraction of carbon.
Due to a developed surface of nanodiamond particles, it is
possible to control their physicochemical properties. The thermo-
physical properties of ND nanofluids based on water,69,75–80,128,129
water–glycol,81,130–137 and other organic solvents were
studied.68,80,81,138–140 However, the heat-conducting properties of
two-phase systems containing nanodiamonds have not been
studied systematically, and one of the recent reviews on nanodia-
mond nanofluids14 shows a clear tendency of a relative increase in
thermal conductivity with concentration and temperature; however,
the values are quite scattered showing a rather contradictory 5%–
20% increase;69,74–78,80,141 therefore, it is almost impossible to
determine a priori how effective would be the addition of nanodia-
monds to a base fluid. The same situation is with other carbon
nanofluids. Of importance is the fact that the majority of studies
relied on a rather unprecise implementation of the non-stationary
hot-wire method (a KD-2 pro instrument proposed for technical
solutions), which requires a large volume of the solution, is
convection-dependent in low-viscosity solutions, and provides the
accuracy of ±5% at best.
Over the past decade, an increasing number of studies
on CNFs have been associated with colloidal solutions of
graphene,142,143 graphene oxide,117,137,144,145 and their hybrid nano-
fluids.27,28 A rather high (5000 W/m/K)146 coefficient of thermal
conductivity was experimentally determined for this material.
Ultrasonic treatment is required to produce graphene-based nano-
fluids; less often the stabilizers are used. Still, there is an acute
problem of producing stable dispersions147 containing sufficient
quantities to change the thermophysical properties of the base
fluid. As in the case of nanodiamonds, the maximum achievable
concentrations and the corresponding increases in thermal conduc-
tivity differ greatly between the reports, which may be a conse-
quence of the use of different methods for producing nanoparticles.
Also, the actual values of the thermal conductivity of the dispersed
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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phase are much lower than assumed.143 This is due to the fact that
the size of small sheets of graphene in solution can be less than
the mean free path of quasi-particles, phonons responsible for
heat transfer. In addition, the contact resistance is high, and the
oxidation leads to the appearance of defects at which, as well as at
the boundaries of the nanostructure, phonons are scattered, which
prevents heat transfer. Estimation of the thermal conductivity of
in-plane graphene and graphene oxide resulted in rather small
(4.9 ± 0.6 and 6.8 ± 0.8 W/m/K, respectively) values.143
The addition of fullerenes to water does not lead to an increase
in thermal conductivity as the thermal conductivity coefficient of
fullerene is lower (0.4 W/m/K) than the values typical for water.
An increase in the thermal conductivity of toluene upon the addi-
tion of fullerenes (a mixture of C60 and C70, less than 0.4% v/v)
was less than 1%,148 and the addition of 5% v/v C60 to a mineral
oil (0.1 W/m/K) led to an increase in the thermal conductivity by
6%.70 A fullerene–mineral oil system turned out to be promising
for use in compressors of freezing systems since it has good lubri-
cating properties, which increases the compressor life, and also has
a higher thermal conductivity than the mineral oil, which is neces-
sary for more efficient cooling.72
Still, the potentialities of carbon-based dispersions are an
open discussion. First, their application demands assessing the con-
centration of the nanophase and total composition of the disper-
sion as well as the knowledge of the characteristic size and the
aggregation state. Their thermal parameters, first of all thermal
conductivity, are sometimes rather contradictory and doubtful.1,60
The accuracy and precision of the existing data often suffer from
the errors in calculation, changes in the sample by an immersible
measurement system,11,119 and convective effects at long measure-
ment times or for large volumes. Understanding heat transfer in
carbon-based dispersions still lacks experimental techniques pro-
viding the accurate data in situ.
III. NON-PHOTOTHERMAL TECHNIQUES FOR THERMAL
CONDUCTIVITY AND DIFFUSIVITY OF NANOFLUIDS
Measuring the thermal conductivity and thermal diffusivity of
nanofluids is carried out with various methods. Experimental tech-
niques are divided usually into two principal groups: (i) the steady-
state techniques performing a measurement when the sample
reaches the thermal equilibrium and (ii) transient methods.26
Among the latter, photothermal techniques will be considered sep-
arately (see Sec. IV). In this section, the most common techniques
are briefly listed. They are the transient hot-wire (THW) method,
the 3ω method, the transient plane source (TPS), the temperature
oscillation, and laser flash (LF) methods.11 The relevance of these
methods depends on the availability of commercial equipment,
price, versatility, and practical simplicity.
A. Hot-wire method
The most common is THW (both commercially available and
homemade apparatuses);9,11,19,20,26 however, this method should be
considered more critically. Even for a homogeneous medium,
certain conditions must be fulfilled to eliminate forced convection;
e.g., the fluid sample and the thermal sensor must be kept
completely still during the measurement. Thus, it may be necessary
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to place the sample on a vibration-isolation table and shut down
heating, ventilating, and air conditioning systems in the measure-
ment room. Thus, the water bath should be turned off before the
data acquisition and the temperature must not exceed 50 °С for
aqueous solutions. The method suffers from practical drawbacks
due to the need for a large volume of liquid; also, the accuracy may
be affected by the presence of ions of the conducting fluids around
the hot wire so often that the wire should be electrically insulated
(usually implemented in a transient short hot wire, an improved
design of the method).149
In the case of nanofluids, additional problems appear. Gravity
effects can cause inhomogeneous nanoparticle dispersity over the
fluid producing a temperature gradient along the hot wire, which
increases the measurement error. Such complications may lead to a
serious measurement bias: an anomalous enhancement of the effec-
tive nanofluid thermal conductivity and as a result to large discrep-
ancies.119 To avoid these problems, a standardized methodology for
nanofluid measurement is on demand. The information on sample
preparation, sample size, all measuring conditions, as well as the
number of replicate measurements, the data on the basic fluid, and
uncertainty must be pointed out.
B. 3ω and hot ball methods
Other transient techniques find applications on nanofluid
characterization, but they are not so widespread. Just as THW, the
3ω method uses a radial flow of heat but applies a temperature
oscillation instead of a time-dependent response. Basically, a short
wire immersed in the test fluid or liquid is placed on a quartz sub-
strate on which a thin metal heater is attached, thereby allowing the
use of small (droplet) liquid volumes.150 Another advantage is the
possibility of studying the gravitational effect on the thermal con-
ductivity of disperse media by changing the orientation of the test
system. Low heating (0.5 K) and fast temperature-dependent mea-
surements help suppress convection interference for which the
effect decreases with frequency.151 All nanofluid measurements are
done by home-made instruments.150–156 Examples are Al2O3–H2O,150
TiO2–H2O,151,152 SiO2–H2O, ethanol, EG,151 CuO–H2O,153 hybrid
nanofluids (numerous CNTs attached to an alumina/iron oxide
sphere in poly-alpha-olefin oil),154 Bi3Te2 nanorods–oil,155 and
single-wall CNTs–H2O (the convective heat-transfer coefficient is
also measured).156 Similar to the wire in THW, a hot ball sensor is
applied to assess thermal diffusivity and conductivity of an
aqueous Ag nanofluid.157
C. Transient plane source
The transient plane source method is attractive for NFs
because test instruments are commercially available.11 TPS was
applied for various nanofluids: Al2O3–H2O, Cu–H2O, and carbon
nanotubes–R113 refrigerant.158–160 Manufacturers continue to
upgrade the measurement system by offering a special cell (a modi-
fied transient plane source).161 It should be mentioned that without
prior knowledge of density and isobaric heat capacity, thermal con-
ductivity is calculated with the iterative method by the software.
Fast response (0.8 s), small (1.25 ml) sample volume, low energy
power, and horizontal presentation of the sample to the sensor
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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help eliminate the effect of heat convection, but the better the
parameters, the higher the instrument price.162
D. Temperature oscillation method
The purely thermal technique—the temperature oscillation
method—is not widespread, perhaps, due to its specific principle,
instrumentation, and theory. The setup consists of a hollow insulating
cylinder and the central hole is closed from both sides by two metal
discs leaving a central cylindrical cavity for the test fluid. A sinusoidal
temperature input is applied at the outer faces of the metal disks. To
find the thermal conductivity of the test fluid, the amplitude attenua-
tion and the phase shift in the temperature wave at the inner face of
the disk and at the center of cavity are measured.
This technique was used to measure the thermal diffusivity of
metal-oxide fluids in water,163 ethylene glycol, and transformer
oil.164 The following advantages are claimed: (i) the use of a small
oscillation amplitude (1.5 K) to retain constant fluid properties and
to avoid natural convection and (ii) electrical components of the
apparatus are away from the test sample; therefore, any liquid, irre-
spective of its electrical conductivity, can be measured.
E. Laser flash method
The laser flash method is implemented as the most expensive
commercially available technique and is commonly used for solid
substances. Measurements of thermal diffusivity and specific heat
allows the calculation of the thermal conductivity with an external
measurement of the bulk density of the sample material only. A
special sample holder and more complicated data processing with
additional data on thermophysical parameters of the sample and
container material are required to work with fluids.165 The main
disadvantage of the method, especially for low-viscosity liquids, is
convection due to a strong increase in the temperature in a short
period of time. Also, LF lacks precision when measuring fluids
with low thermal conductivities.48
It was used for some nanofluids containing metal–oxide nano-
particles in water13,140,166 and water–alcohol mixtures,167 nanodia-
monds in silicone oil,140 carbon nanotubes, exfoliated graphite, and
heat treated nanofibers in a poly-alpha-olefin oil.168 LF was com-
pared with TPS (a good agreement between the two methods)166
and THW (results by LF were significantly lower).13 The collision-
mediated heat-transfer models were applied for explaining the dif-
ference in thermal conductivity values by various experimental
methods. The authors169 showed that Brownian motion of the
nanoparticles is limited because of the small liquid volume result-
ing in the reduction of the collision frequency of nanoparticles.
F. Steady-state techniques
Steady-state techniques can be classified into a coaxial
(concentric) cylinder method and a parallel plate method (including
a cut-bar method). The latter has been implemented commercially
in two types of equipment: guarded hot-plate instruments and
heat-flow meters (measurements of the electrical power and heat
flux, respectively). Only the second is adopted to measure liquids;
however, to date, there are almost no experimental data on the use
of this liquid cell. Some metal–oxide nanofluids were measured by
128, 190901-10
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home-made instruments.170,171 Home-made apparatuses of the
concentric-cylinder method was commonly used for fluids172 but
is rarely seen in the research on nanofluids.120,173 Steady-state
methods have a simple theory based on Fourier’s law providing the
assessment of the thermal conductivity from the measurements,
but they are time-consuming.
Fast, often portable, and relatively affordable equipment of
transient methods is generally more widespread. Under the right
conditions, they guarantee good characteristics (precision, 1% and
accuracy, 5%). Still, the measurement of thermal conductivity of
liquids, especially nanofluids, showing the complexity of the
thermal transport mechanism, is a challenging task.174
IV. PHOTOTHERMAL SPECTROSCOPY IN NANOFLUID
STUDIES
Methods referred to as photothermal spectroscopy (PTS) are
based on the detection of thermally induced changes in the sample
upon its interaction with electromagnetic radiation (photothermal
effects). This is an established group of methods, which is used
for the characterization of various materials.30,34,175–177 Thermal
relaxation of spatially encoded electromagnetic radiation absorbed
by an object under excitation leads to its nonuniform and dynamic
heating.
PTS is suitable for assessing all the thermophysical parame-
ters governing or associated with the heat distribution (thermal
conductivity, thermal diffusivity, specific heat, refractive index,
density, etc.).36,178–188 Also, PTS complements optical methods:
transmission spectrophotometry, diffuse-reflection spectroscopy,
and many IR modalities. While these methods measure transmis-
sion or reflection of the incident electromagnetic radiation
(i.e., its non-absorbed part), PTS is based on non-radiative
transitions of excited molecules, i.e., on the absorbed part of the
radiation.30,37 Thus, PTS is used to assess extinction and absorp-
tion coefficients in liquid and solid samples down to the level of
10–9–10–6 absorbance units. Also, using Beer’s law, PTS makes it
possible to assess the concentrations down to 10–11 M and detect
countable numbers of molecules.30 A small influence of the scat-
tering matrix on the signal compared to purely optical techniques
makes photothermal and especially photoacoustic spectroscopy
invaluable tools for complex samples and in biomedical
research.189–195 Moreover, the sensitivity of photothermal
methods excels both purely optical as well as purely thermal-wave
methods because PTS is based on the interdependence of changes
in optical and thermal properties acting cooperatively to enhance
the sensitivity196 and makes it possible to get the excitation
spectra of photothermal properties.197–203
Photothermal spectroscopy can be used to assess both thermal
and optical sample properties with a locality governed by the char-
acteristic rates of nonradiative heat transfer.30,34,175–177 Thus, PTS
works with both volume- and surface-absorbing samples, as well as
layered and discretely absorbing materials. As the excitation source
is usually a laser, which can be focused to down to the wavelength-
confined space (diffraction limit), all photothermal methods have a
merit of being implemented as a microscopic, imaging, or micro-
spectroscopic techniques.203–207
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These features of PTS are quite relevant for heterogeneous
objects or dispersions, where the classical thermophysical or chemi-
cal methods result in averaged parameters of the whole sample
only. A current trend is the application of photothermal and photo-
acoustic methods to the objects, for which other methods of optical
and thermal characterization are difficult to use,—such as complex
heterogeneous condensed systems in situ and in vivo.30,38–40
Photothermal studies of nanoparticle-containing materials show
that the nature, the particle concentration, and their size make a
critical effect on the development of the thermal profile in the
sample and on the formation of the photothermal response of the
material.41–43,208–212
PTS is an umbrella term for several techniques. They are com-
monly classified according to the result of the photothermally
excited heating because of energy absorption and thermal relaxa-
tion. This leads to some processes in the whole sample or its (sub)
surface layers: (1) the photothermal generation of thermal waves,
(2) the formation of a non-uniform spatial field (profile) of temper-
ature manifesting itself as a refractive-index or density fields, and
(3) the emission of secondary radiation by a heated sample surface,
photothermal radiometry (PTR).
Regardless of the detection approach used, photothermal tech-
niques can be categorized as frequency-domain and time-domain
(transient grating, forced Rayleigh scattering, laser flash, and
thermal lensing).213 Also, the methods of PTS can be divided into
two main categories: (1) contact techniques, in which the sample is
in contact with the detection system, and (2) non-contact techni-
ques, involving a remote detection system.214 The relevant feature
of PTS is its non-destructive character, and both for optical and
thermal parameters of materials, high precision of measurements
is attained.
The format of this perspective paper does not allow the dis-
cussion of general possibilities of the methods; therefore, below are
brief description of photothermal methods that have already found
their use in the studies of NFs and related materials.
A. Photopyroelectric and thermal-wave resonator
cavity techniques
The best example of a contact technique is the photopyroelec-
tric (PPE) technique based on the use of an opaque pyroelectric
transducer in thermal contact with the test material to detect the
temperature variations caused by light-induced periodic heating.
The signal depends on the optical and thermal parameters of the
test material and the PPE plate in a complex way, which is why
usually some approximations and calibration are used. Usually
thermal diffusivity and thermal effusivity of the sample are evalu-
ated by making an excitation frequency scan and fitting the experi-
mental curves for the dependence of the signal amplitude and
phase on the frequency.
The back and front PPE techniques (BPPE and FPPE, respec-
tively) allow the measurements of the thermal diffusivity and
thermal effusivity of fluids, and the experimental uncertainty is as
low as 2% and 1% for thermal diffusivity and effusivity, respec-
tively.215,216 Other advantages of this method include its relatively
low cost, and only a small (0.2–0.3 ml) volume of the sample is
required with a short measurement time, where the concentration
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Applied Physics

thermal diffusivity is assessed by thermal-lens spectroscopy (Sec. IV E)

and thermal effusivity by PPE. The cases include Au NPs in water, eth-
ylene glycol, and ethanol;226 TiO2 NPs in water;227 biodiesel containing
Au NPs;212 and hybrid nanofluids (L-cysteine in combination with Au
nanoparticles and protoporphyrin IX).228 NFs based on Fe3O4 and
CoFe2O4 in water were investigated by both BPPE and FPPE photo-
pyroelectric configurations with the TWRC technique as a comple-
mentary high-resolution scanning procedure.229,230

B. Photoacoustic spectroscopy
The photoacoustic (PA or optoacoustic) effect consists of a
change in the pressure (acoustic pulse, PAS signal) caused by thermal
expansion of the sample upon the absorption of electromagnetic radia-
tion by its molecular structures and subsequent nonradiative relaxa-
tion. This change in pressure is detected with a microphone or
piezotransducer. PA detection first used for thermal parameters for
gases and solids214 can be applied to liquids231,232 as the physics
underlying the photoacoustic effect has been developed.233
In the assessment of parameters of liquids, usually, an open
photoacoustic cell, OPC is used: a front configuration to measure
the thermal effusivity234 and a thermal-wave transmission configu-
ration for thermal diffusivity measurements.235 Conventional PA

FIG. 7. Cross section of the photopyroelectric experimental system.

Reproduced with permission from López-Muñoz et al., Nanoscale Res. Lett. 7,
667 (2012). Copyright 2012 Springer.

of the nanofluid remains constant in the measurement process,

thus making this technique suitable for nanofluids.217 The limita-
tion of these techniques is that not all the types of liquid samples
can be used, as a reactive sample in direct contact with the trans-
ducer may damage it.
Thermal wave resonator cavity (TWRC or thermal-wave inter-
ferometry) is a simple, versatile, and accurate technique.218,219
TWRC is a kind of back-detection PPE when a thin metal foil front
wall serves as a laser-induced oscillator source (a thermal-wave gen-
erator), while a pyroelectric PVDF back wall acts as a signal trans-
ducer and a cavity standing-wave-equivalent generator. In contrast
with the frequency scans employed in conventional PPE techniques,
TWRC uses a PPE detector with a variable sample-to-source dis-
tance, usually with a micro-linear stage, which provides the cavity
length to vary with a micrometer step resolution (Fig. 7).220 The
signal phase is a linear function of the sample thickness, and the
thermal diffusivity of the sample can be determined from the slope.
Because the cavity-length scan employs a selected thermal-wave fre-
quency, it improves signal-to-noise ratios.221
A liquid-state compatible design of the TWRC was first applied
for the measurement of the thermal diffusivity of one-phase liquids
(15 ml); precision, 1% and accuracy, 1%–2%.222 Later, it has been
employed for nanofluids: TiO2 nanoparticles dispersed in polyvinyl
alcohol223 and water,224 Ag NPs in water,225 and urchin-like colloidal
gold nanofluids in water, ethanol, and ethylene glycol.220 FIG. 8. Cross section of the photoacoustic experimental system. Reproduced
with permission from López-Muñoz et al., Nanoscale Res. Lett. 7, 423 (2012).
Sometimes, these techniques are applied for nanofluid
Copyright 2012 Author(s).
characterization in combination with other photothermal techniques:

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 Journal of
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methodologies for thermal diffusivity measurement purposes in
solids rely on the scanning of the PA signal as a function of the
laser modulation frequency f. On the contrary, the PA methodology
for liquids236 makes use of linear relations among the photoacous-
tic amplitude (on a semi-log scale) and phase as functions of the
sample thickness. As in TWRC, the thermal diffusivity pffiffiffiffiffiffiffiffiffiffiffiffiof
ffi the
sample can be determined from the slope as B ¼ πf /DT . The
laser source is immersed in the sample, and the PA chamber (cell)
consists of a cylindrical cavity in a stainless-steel body and commu-
nicated with a microphone (Fig. 8). The layer of a glass sealer of
the PA chamber helps avoiding the limitation of PPE techniques to
the kind of the liquid sample to be used because there is no contact
with the transducer.235 PA techniques and the front PPE configura-
tion confine the majority of photothermal methods for direct
assessment of thermal effusivities.
The method was applied for two-phase liquids; e.g., the
thermal diffusivity of water-based Au236 and Al2O3237 nanofluids
was determined. The instrument was improved by an accurate
sample temperature control and verified the possibility to detect
slight (around 1%) thermal-diffusivity variations.237 Due to the
development of the theory, the method was used to evaluate the
thermal effusivity of a Fe3O4–ethylene glycol nanofluid (a high-
density suspension)238 and biodiesel filled with Au and Ag.239
Thermal effusivity and the refractive index of Al240 nanofluids in
ethylene glycol were measured using PA spectroscopy and
minimum deviation methods, respectively. A closed PA cell was
applied for thermal diffusivity and effusivity measurement of fluids
with low concentrations of TiO2 and Al2O3 NPs in water.241 A PA
technique with piezoelectric detection was used as a non-
destructive and noncontact tool to study thermal transport in
nanofluids formed by carbon flurooxide mesoparticles;242 this tech-
nique was also adopted for the study of heat transport across the
interface of a nanostructured solid (porous silicon) and a fluid.243
PA and thermal-lens techniques (Sec. IV E) sometimes were used
together for thermal effusivity and diffusivity evaluation of a nano-
fluid (Ag NPs in ethylene glycol and ethanol); in this case, thermal
conductivity can be calculated from this experiment alone, without
external data.244 Similarly, the TWRC technique was used to assess
the thermal diffusivity of samples and an OPC PA to the thermal
effusivity of Ag nanowires in water.245 The thermal diffusivity and
effusivity were found by fitting the theoretical expressions for each
modality as a function of the sample thickness and frequency to
the experimental data. The cell was calibrated with water to
compare with the values reported in the literature.245 Likewise, the
thermal characterization of a carbon-nanofiber–silicone based fluid
was performed using these two photothermal techniques.219
C. Photothermal radiometry
Photothermal radiometry is common in studies of solids due
to the possibility of studying the surface structure, detecting a
variety of defects, damage, heterogeneous areas in materials, etc.
The incident modulated or pulsed radiation causes fluctuations of
the temperature of the sample surface, which are dictated by the
material underneath the cover layer and are recorded by an IR
detector.204,213,246–248 By comparing the phase shift between the
original signal and the temperature variation, the thermal
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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properties can be extracted. This technique can be used in the front
(photothermal emission) and rear configurations (photothermal
radiometry), a setup similar to the laser flash technique.213 In this
case, it is necessary to deposit a black layer on both surfaces of the
sample to improve the laser absorption and increase the backside
infrared emission.213 Apart from the features common to all the
photothermal methods, the advantages of PTR are remote sensing,
the relative simplicity of the experimental setup, and a high time
resolution (10–8–10–7 s).248–250 The latter makes it possible to
measure the spectra of intermediate products and to monitor
fast processes.
Front-face modulated PTR was proposed for the estimation of
thermal conductivity of liquids (water and sunflower oil) by fitting
the experimental points of phase lag vs frequency measurement.
The system consists of three layers. The first layer is constituted of
steel (absorption of the heat flux), the second layer (thickness
500 μm) is the test liquid (opaque for thermal radiation), and the
last one is made of glass, transparent in the visible range and
opaque in the infrared. A small temperature oscillation (2 K)
ensures that no natural convection occurs in the liquid layer.251
Rear PTR was applied for thermal diffusivity measurements of
Ag NPs in water by a calibrated scanning depth profile of the heat
wave μs from the amplitude and phase signals.252 Thermal diffusiv-
ity is estimated using the dependence of the penetration depth on
the excitation frequency f,
sffiffiffiffiffiffi
DT
μs ¼ :
πf
D. Optical beam deflection techniques
These remote techniques are well suited for investigation of
thermo-optical properties including thermal diffusivity and nonde-
structive evaluation of solid samples: bulk materials, thick films as
well as thin films or multilayers.213 The concept of this method is
based on the deflection of a probe beam due to changes in the
refractive index of the contact medium—a gas (more seldom,
liquid) layer adjacent to the surface of the test sample—induced by
a temperature change produced by an absorbed excitation laser
radiation (Fig. 9). Depending on the relative position of these
beams, two configurations can be distinguished: perpendicular
FIG. 9. Schematics of the probe-beam deflection near the sample surface.
Reproduced with permission from Saadallah et al., Sens. Actuators A: Phys.
138, 335 (2007). Copyright 2007 Elsevier B.V.
128, 190901-13
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FIG. 10. Optical path of a probe laser beam in a hot wire–laser beam displace-
ment technique. Reproduced with permission from Ali et al., Rev. Sci. Instrum.
81, 074901 (2010). Copyright 2010 AIP Publishing LLC.
(mirage effect) and collinear (photothermal mirror). The former can
probe the contact medium at the front or rear surfaces, whereas the
latter preferentially probes the material. Theoretical models are
complicated; however, slopes of simple linear relations between two
measurable parameters can be used to assess thermal diffusivity;
for a more detailed information, see the paper.253
Despite the history and abilities of this method, only few
investigations were associated with liquids, especially heteroge-
neous. A technique based on a mirage effect (Fig. 9) was demon-
strated to determine the thermal diffusivity and, indirectly, the
absorption spectrum of nonabsorbent liquids (paraffin oil) by
fitting the experimental curve to the theoretical model of amplitude
vs the square root modulation frequency.254 In a glass cell fulfilled
with paraffin oil, a plexiglass plate covered with a thin black carbon
layer (radiation absorbent) is introduced. Since the thermal diffu-
sion length in liquids becomes lower than the probe-beam diameter
for high frequencies, only one part of the beam is deflected.
Therefore, a new mathematical expression of the deflection related
to the probe-beam dimensions was established to calculate the
“effective” deflection in liquids.254 The photothermal mirror tech-
nique was used for the thermal diffusivity measurement of ferro-
fluids. The samples were encapsulated in cuvettes of 0.5 cm thick
on the side and 1.0 cm large. The authors applied a linear relation
when plotting a phase collinear deflection as a function of the sepa-
ration between the excitation and probe beams at a fixed fre-
quency.255 The collinear configuration was used for detecting the
Soret (thermodiffusion) effect in ferrofluid samples with two differ-
ent surfactants. Thermodiffusion effects depend on the charge of
the coating that covers the magnetic grains; however, refractive-
index gradients for both ferrofluids presented the same trend for
the same variation of particle concentration.256
In the photothermal displacement technique, an intensity-
modulated excitation laser beam impinges onto the sample along the
normal direction like in other optical beam deflection techniques,
whereas the probe laser is incident to the surface at an oblique angle.
However, for liquids, the setup is more like in mirage-effect measure-
ments. The cell is fixed on a three-dimension position mechanism
stage. The temperature field is produced by heating a thin metal wire
immersed in the fluid and oriented vertically and perpendicularly to
the probe beam. It causes the probe beam to deflect from its original
position (the distance between the probe laser beam and the wire is
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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∼300 μm, and it is measured with a high-precision gauge); the beam
deflection is measured by a position-sensitive detector (Fig. 10).257
The detector and heater are separated from each other providing
potentially more accurate data. Thermal conductivity and thermal
diffusivity are obtained by fitting the experimental data to the
numerical simulation data.
This hot wire–laser beam displacement technique was applied
for five homogeneous liquids: thermal conductivity, thermal diffu-
sivity, and the temperature dependence of the liquid refractive
index were measured.258 The same technique was used for measur-
ing the thermophysical properties of Al NPs suspended in water,
ethylene glycol, and ethanol.257 Thin-film metal lines/heaters and
beam deflection applied for measurements of the thermal diffusiv-
ity of fluid mixtures (ethanol–water) and suspensions of nanoparti-
cles (fullerenes C60 and C70 in toluene and Au NPs in toluene and
ethanol) provided a precision of better than 1%.148 Thus, such a
configuration can be considered a prototype for the nanofluid test
measurements.
E. Thermal-lens spectrometry
Techniques referred to as thermal-lens (photothermal-lens)
spectrometry (TLS) are based on the formation of a lenslike
element (refractive-index field) upon the absorption of excitation
radiation. TLS belongs to slow photothermal techniques: the attain-
ment of a stationary photothermal state or on mid- to long-scale
(milliseconds to seconds) transient measurements. The signal is
calculated as a relative change in the probe-beam intensity Ip at a
far-field detector plane at the moment t,30
(Ip (t ¼ 0)  Ip (t))/Ip (t) ¼ Pe α  B(t)/tc  (dn/dT)/λp k: (5)
Here, Pe is the excitation laser power, α is the linear light-
absorption coefficient of the sample, dn/dT is the temperature gra-
dient of the refractive index (thermo-optical constant), k is thermal
conductivity, λp is the probe laser wavelength, and B(t) is the spec-
trometer constant determined by the geometry of the optical
scheme (the ratio of the waists of the laser beams and confocal dis-
tances). The geometrical parameters can be either strictly stable or
controlled with the use of standard software tools; in any case, they
are known. In optical and spectrochemical studies, TLS is used for
measuring light absorption30 or assessing low concentrations,259,260
especially in small volumes (thermal-lens microscopy).261–265
Among all the photothermal methods, thermal-lens spectroscopy
and microscopy have the largest pool of chemical applications, and
in biomedical studies, it is second only to state-of-the-art photoa-
coustic tomography techniques.
In thermophysical studies, such slow photothermal techniques
are used for (i) estimating macroscale thermal parameters of
various liquids266,267 from steady-state signals and (ii) assessing
heat-transfer parameters between the phases of a disperse system
from transient signals. The thermal diffusivity is assessed from the
characteristic time tc (usually, a micro- to millisecond scale) of the
thermal-lens development, which is calculated from the time-
resolved (transient) curve of thermal-lens measurements, Eq. (5),
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and the radius of the excitation beam ωe ,
tc ¼ ω2e /4DT :
The absorption of the sample α is measured with high accu-
racy simultaneously with the time-resolved curve but represents
a separate information channel. For the calculation, the radius
of the probe laser in the sample should be known, the measure-
ment of which introduces inaccuracy. Usually, thermal-lens
characteristic time is defined as a target parameter when the
experimental data are approximated by the theoretical equation
of the time-resolved signal for a homogeneous solution.
Therefore, a reference sample is sometimes used,
(6) water57,244,268–271 or toluene.272 For them, the characteristic time
is determined, and to determine the thermal diffusivity of the
sample, the ratio of the characteristic times and the known coeffi-
cient of thermal diffusivity are used. Occasionally, the thermal conduc-
tivity coefficient is obtained from a stationary thermal-lens signal;
however, in this case, it is necessary to know the thermooptical cons-
tant dn/dT with respect to temperature for each sample.273 As men-
tioned above, TLS is combined with pyroelectric detection; therefore,
the thermal diffusivity and thermal effusivity are determined from

TABLE I. Thermal diffusivity DT of nanofluids and related systems by thermal lensing.

Concentration,
Nanoparticle Base fluid М Results Reference
−2
Au + Rhodamine 6G Water 5.5 × 10 DT increases with the addition of NPs 274
Ag + Rhodamine 6G Water 1 × 10−3 The average DT is lower than that of water 275
Ag/Au + neutral red Ethanol 6.8 and 3.7 × DT decreases with the addition of NPs 276
10−5
Au Water 6.6 × 10−4 DT increases when the particle sizes increase 277
Au Cellular culture medium 6.6 × 10−4 DT increases with the addition of NPs 278
Au Water, ethylene glycol, 6.6 × 10−4 DT enhanced by 9%, 1%, 8% 42 and
ethanol 226
Au Biodiesel 1.0 × 10−2 DT increases with the addition of NPs 212
Au Water 1.0 × 10−4 DT decreases with the addition of NPs 268
Au Ethylene glycol : water, 50 1.5 × 10−9 DT increases with the addition of NPs 269
: 50
Au Polyvinyl alcohol–water 2.9 × 10−4 DT increases with the addition of NPs 279
Au Water 2.31 × 10−9 DT increases with the addition of NPs, depends on 271
the shape
Au, Ag Water 2 × 10−4
, 5× DT enhanced by 16%, 20%, 280
10−4
Ag Water 2.6 × 10−9 DT decreases with the addition of NPs 281
Ag (rod-shaped) Water 1.4 × 10−6 DT depends on the aspect ratio 270
Ag (25–38.5 nm) Polyvinylpyrrolidone– 3.4 × 10−3 DT increases when the particle sizes increase 282
water
Ag Ethylene glycol–water 1.6 × 10−4 DT and effusivity (by PA) measured, conductivity 244
Ethanol–water calculated (5% and 3% enhancement)
Cu Polyvinylpyrrolidone– 5 × 10−2 DT increases with the addition of NPs 272
water
TiO2 Water 4.7 × 10−2 DT and effusivity (by PPE) measured, conductivity 227
calculated (12% enhancement)
SiO2 (100–600 nm) Water 6.2 × 10−3 DT increases when the particle sizes increase 209
TiO2 4.7 × 10−2 DT increases with the addition of NPs
TiO2 Water No information DT increases with the particle size and the 283
calcination temperature
Fe3O4 (6–63 nm) Water 1.7 × 10−11 DT increases when the particle sizes increase 284
Na2C2 Water 2.9 × 10−3 DT enhanced by 87% 285
CdTe quantum dots Water 2.1 × 10−4 DT is less than that of water and decreases when the 57
particle sizes increase
A mixture of carbon Acetone 0.2 mg/ml DT enhanced by 95% with soot annealed at 300 °C 286
allotropes
Silicone Ethanol 4.5 mg/ml DT is less than that of ethanol and decreases with 287
the addition of NPs

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both methods, and then the coefficient of thermal conductivity is cal-
culated from these parameters.212,226–228
Due to simplicity and rather easy interpretation, thermal-lens
spectrometry is often used to determine the thermal diffusivity of col-
loidal solutions, especially two-phase systems containing nanoparticles
of metals and their oxides (Table I).42,57,209,212,226,227,244,268–272,274–287
Not all the cases gathered in Table I are established NFs, but this
collection shows the possibilities and problems of thermal lensing
of disperse systems. In addition to the fact that for similar systems,
the increments of thermal conductivity differ considerably, and the
regularities of thermal properties on concentration and size differ.
Unfortunately, this is typical for measurements of all the dispersed
systems regardless of whether thermal or optical methods are used
and may be associated with different physicochemical properties of
two-phase liquids.
Nevertheless, inconsistencies in thermal-lens assessment of
NFs may result from incorrect data processing; two-phase systems
require either a correction in standard homogeneous models of the
thermal-lens signal or brand-new approaches. If for homogeneous
systems, transient curves are largely symmetric, for disperse
systems, the local heating at the initial time is located around
absorbing particles followed by the heat transfer to the bulk, which
leads to much more rapid heating and reduction of the characteris-
tic time of the thermal lens. On the contrary, dissipation of the
thermal lens changes less significantly because for small heating
(10–2 K, which is characteristic for solutions used in thermal-lens
spectrometry), it is possible not to consider the dispersion medium.
As an example, studies of fullerene C60 solutions in toluene
(no aggregate formation, molecular solutions), N-methylpyrrolidone
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
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FIG. 11. Transient thermal-lens curves
(a) fullerene C60, blue line and a molec-
ular dye (Sudan) in toluene, red line; (b)
for fullerene C60, blue line and a molecu-
lar dye (ferroin) in N-methylpyrrolidone,
red line; (c) for fullerene C60, blue line
and a molecular dye (ferroin) in water,
red line; and (d) for ND (1.0 mg/ml,
NanoAmando), blue line and a molecu-
lar dye (ferroin) in water, red line;
532 nm, 150 mW. Irel (t) ¼ (Ip (0)  Ip (t))/
(Ip (0)  Ip (1)).
(NMP, C60 aggregates), and water (aggregates are formed and are sta-
bilized by charge-transfer complexes) show that the aggregation and
stabilization processes change thermooptical parameters (Fig. 11).
In toluene [Fig. 11(a)], the transient curves, Eq. (5) (normalized
values of Irel, the inital probe-beam intensity is set to 1, the equilib-
rium, to 0) for fullerene C60 and a dye of approximately the same
molecule size (1 nm), are nearly identical. This correlates well with
the theory of thermal lensing, and the estimation of the characteristic
time [Eq. (6)] shows that the values for fullerene and the dye differ
insignificantly from one another and from the value calculated using
the reference data for toluene.197 However, in NMP [Fig. 11(b)], the
situation changes drastically: the curve for fullerene C60 shows a
slower heat transfer (a less steeper transient curve) and differs from
the characteristic curve of a molecular dye. This is accounted for by
the formation of a coarse dispersion of fullerene in NMP, which sig-
nificantly decreases the rate of heat propagation. This is confirmed
by the same effect of the second part of the curve (dissipation after a
mechanical chopper switches off the excitation beam). In water
[Fig. 11(c)], the result is contrary to the case of NMP: the curve for a
fullerene solution shows a characteristic time lower than a molecular
solution of a dye (ferroin) and a quicker decrease in the probe laser
intensity due to thermal-lens effect. This can be attributed to the for-
mation of a finely dispersed solution with a cluster size of 50–
150 nm,288 which exhibits short overheating near the clusters fol-
lowed by a longer period of thermal equilibration of the whole solu-
tion.289 The same behavior, though with larger changes, is
characteristic to nanodiamond aqueous dispersions [Fig. 11(d)]. It is
interesting that the behavior of the dissipation part of the curve for
fullerene is nearly the same as for a molecular dye, which is contrary
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to the behavior of the ND dispersions. Overall, this cannot be pre-

dicted using the generic theory for homogeneous thermal lensing,
and the new approach should be based upon, e.g., single-point
approaches.41,290 This area has not been fully studied; however, it is
crucial for thermophysical characterization of nanofluids as the
majority of information is not used in full or may be inaccurate.
The advantage of TLS in NF assessment is the simplicity of
equipment relative to other photothermal methods (for liquids,
only a cuvette is needed). There are no restrictions on the range of
determination of the thermal diffusivity; due to high accuracy and
precision (1% and 5%), it is possible to determine small differences
(of the order of 2%–3%)288 in the thermal diffusivity, which is
especially important in the analysis of nanofluids. There is a possi-
bility of measurements at different temperatures and the time range
(milliseconds) makes it possible to simultaneously record the
uneven heating of the dispersion medium and the dispersed phase.
The method is non-contact, and the effect of convection is
minimal due to low heating per cycle (10–2 K).30
The disadvantage of TLS for NFs is that any thermal-lens
spectrometer is characterized by a certain concentration region in
which the signal linearity is observed; therefore, to work with
highly concentrated (highly scattering) solutions, it is necessary
either to reduce the length of the optical path (it is impossible to
infinitely decrease the thickness of the cell) or to decrease the
power of the exciting laser. The processing of the time-resolved
curves is time-consuming and, in the case of heterogeneous media,
requires significant improvements in the theory. Also, while absor-
bance measurements by thermal lensing are calibration based and
linear, thermophysical characterization, even for one-point calibra-
tion using a reference solvent, requires several conditions (cell
length, cell wall length, measurement time, excitation beam radius)
to be selected carefully as incorrect parameters may lead to devia-
tions from the one-dimensional heat-transfer model;291–300 thus,
the use of this model for estimation of thermophysical parameters
may lead to rather serious errors.
F. Thermoreflectance and forced Rayleigh scattering
techniques
These techniques belong to the group of fast (micro-,
nanosecond, or shorter timescales) photothermal methods:
transient-grating (TG) methods,301–303 optical heterodyne detec-
tion, or impulsive stimulated scattering (ISS)157,304,305 and
related techniques.306 These fast transient modalities of PTS are
used for investigating dynamics of charge transfer,307,308
thermoelastic properties,304 or ultrafast heat transfer inside
nanoparticles.309–311
Thermoreflectance techniques (time-domain, TDTR and
frequency-domain, FDTR) have been typically used to measure the
thermal conductivity of both bulk and thin films along with inter-
facial thermal conductance.213 The excitation laser focused on the
sample generates a periodic temperature change through the
sample, which is detected by changes in probe-beam reflectivity.
The sample must be covered by a thin metallic layer highly reflect-
ing at the wavelength of the probe laser. The obtained phase signals
are fitted with the heat-transfer model to extract thermophysical
properties of solid samples.312 TDTR measures the
FIG. 12. Typical signal from a TG measurement. The acoustic response (inset)
is finished within 400 ns. The slower exponential response can be fit to extract
the thermal diffusivity of the sample. Reproduced with permission from Schmidt
et al., J. Appl. Phys. 103, 083529 (2008). Copyright 2008 AIP Publishing LLC.
thermoreflectance response as a function of the time delay between
the arrival of the probe and the excitation pulses at the sample
surface. In FDTR, the thermoreflectance change is a function of the
excitation modulation frequency.312
Only a few studies have been made for liquids and they are
based on the transient-grating technique.313,314 This time-domain
method relies on the thermal decay of a periodic variation in the
refractive index generated by the interference of two picosecond
light pulses. Optical absorption also causes thermal expansion,
which launches acoustic waves (within a few hundred nanoseconds)
into the sample; thus, the sound velocity can be measured. From
the signal decay (Fig. 12) at longer times (tens or hundreds of
microseconds), thermal diffusivity is determined.315
An impulsive stimulated scattering technique in a heterodyne
diffraction detection configuration was used to study the depen-
dence of the speed of sound and the thermal diffusivity on the con-
centration of silver nanoparticles in water with a precision better
than 1%.157 Al2O3 particles suspended in decane and isoparaffinic
poly(alpha-olefin) were assessed by TG for thermal diffusivity deter-
mination, and thermal conductivity was calculated using theoretical
effective volume heat capacity.315 The results on thermal conductivity
were compared with data obtained by THW (Sec. III A) , and good
agreement between these two dissimilar techniques was observed.
An interesting, though not fully implemented idea is the use
of fast techniques such as ISS or TG with thermal-lens measure-
ments for NF characterization. This would provide a simultaneous
use of the fast technique for the assessment of thermophysical
parameters of the base fluid and building the whole timescale for
heat transfer using ISS by acoustic and photothermal responses in
the nanosecond–microsecond range (Fig. 12) followed by thermal
lensing in the microsecond–second range.

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Forced Rayleigh scattering is an approach that shares similar-
ity to the TG technique but takes place on a slower (millisecond)
timescale; the amplitude of the temperature modulation is small
as well (≤10 mK). The technique was applied for thermal diffusiv-
ity measurements in a citrate-stabilized Au NP suspension in
water and an Al2O3 NP suspension in a petroleum oil at a temper-
ature range of 25–75 °C. The sample (should be transparent) was
contained between optical windows separated by a Teflon spacer
having a nominal thickness of 1 mm. The samples were mounted
in an aluminum block through which oil from a temperature-
controlled bath was circulated maintaining the sample within
±0.1 K of the desired temperature. In contrast to experimental
results obtained using THW, forced Rayleigh scattering shows
that a small (2%) thermal conductivity enhancement is indepen-
dent of temperature and is consistent with effective medium
theory predictions.316
V. OUTLOOKS AND CHALLENGES
Thus, the interest in nanofluids as advanced heat-conducting
and heat-accumulating materials is growing constantly. The effect
of nanofluids in the advanced heat-transfer applications is signifi-
cant, and particles of different nature are considered dispersed
phases for nanofluids tailored for industrial, fast-transfer, or bio-
medical applications. The impact of carbon and hybrid NFs com-
bining the advantages of nanoparticles of various types of
nanoparticles and CNFs is increasing due to several advantages
over NFs of metals and metal oxides.
The well-developed technology of nanofluids is reflected in
several established production technologies of the fabrication and
characterization of common and tailored nanoparticles and nano-
fluids. This is reflected in the appearance of the innovative market
and several R&D and production companies such as PLiN
Nanotechnology (Greece), Synano (the Netherlands), JJ Bioenergy
Ltd. (UK), TCT Nanotech (Italy), Advanced Thermal Solutions,
Inc. (USA), Meliorum Technologies, Inc. (USA), and others.
Notable is the “Nanouptake” action initiative (the European
Cooperation in Science and Technology, http://www.nanouptake.
eu/is-it-possible-to-overcome-all-the-barriers-to-nanofluids-market-
uptake/), a Europe-wide network of research, development, and
industrial institutions, which get together to develop and foster the
use of nanofluids to increase the efficiency of heat-exchange and
thermal-storage systems.
However, all this progress and relevance of nanofluids makes
the problems in NF research and production that remained
unsolved or not fully unsolved rather topical. These challenges may
be summarized as follows.
(i) In many studies, empirical approaches to the estimation of
the working parameters of NFs prevail, with primary
attention being paid to the “front row” of characteristics, i.e.,
thermophysical parameters. The chemical and physicochemi-
cal properties of nanofluids have been studied to a much
lesser extent. However, the knowledge of such properties
(exact chemical composition, size, shape, surface properties
and limiting concentrations of nanoparticles, temperature
dependences of physicochemical parameters, etc.), along with
the information on thermophysical properties, will make it
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possible to purposefully design and create new nanofluid
systems and increase their efficiency. The development of
approaches to the production of new types of nanofluids
with tailored properties is rather topical.
(ii) Noteworthy is that the proposed models of NF action do not
give a whole description of the thermal properties of nano-
fluids and, in most cases, are adapted for the description of
systems containing metal rather than carbon nanoparti-
cles.122,123 Also, to date, there is no working model for the
change in specific heat during the production of nanofluids.
Thermal effusivity, though playing an important part in the
NF action, is not considered in full.
(iii) The necessity for new technologies of nanofluids with better
cost efficiency and reliable upscaling is still required. With
increasing volumes of produced nanofluids and their limited
lifetime, the questions of costs become more and more
serious and are a concern of many industrial and production
R&D initiatives.
(iv) Increasing amounts of nanofluids in an increasing number of
cooling circuits of various scale inevitably raise the problem
of NF wastes or restoration. This requires studies on the envi-
ronmental impacts of nanofluids, which include but are not
limited to biocompatibility, biodegradability, the impact on
soils and marine environments, and long-term effects on
nanoparticle accumulation. Certainly, the progress in issues
of engineering nanoparticles and their biohazards is studied
for a long time,317–319 but nanofluids as a specific type of
nanoscale systems requires certain work especially for hybrid
and core-and-shell particles.12,16,320,321
(v) Of all the dispersed systems based on carbon nanoparticles,
the most studied are systems with carbon nanotubes due to
their extremely high values of thermal conductivity; however,
other CNFs, especially hydrophilic ones based on nanodia-
monds, graphene, and graphene oxide, are probably more
versatile and promising; however, the values of thermal con-
ductivity of CNFs and carbon hybrid NFs are contradictory
and must be estimated with a standardized technology and
high accuracy. Also, the stability of CNFs is an important
and not fully resolved problem.
As a whole, nanofluids require both precise measurement and cons-
tant monitoring techniques, and the development of methods for
their comprehensive characterization becomes crucial. The accuracy
and precision of the existing data suffer from the errors in calcula-
tion, changes in the sample by the measurement system,11,119 and
convective effects. Thus, measurement techniques for thermal con-
ductivity of NFs are continuously developed or improved. Among
those, non-contact heating methods are of importance as they bypass
a frequent source of errors characteristic to contact-based thermal
measurements and thermal-contact resistances, which can be domi-
nating in nanoscale materials. A standardized methodology for
nanofluid measurement is on demand.
The progress in the development of photothermal and photoa-
coustic methods and the results obtained for the last 10–15 years
show that they are fairly promising for such non-contact thermal
measurements when heating is generated by incident UV/vis/IR
radiation.213 Apart from high sensitivity, accuracy, reproducibility,
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small required quantities or volumes of the test sample, and relative
simplicity of the detection cells and laboratory instrumentation are
other advantages of photothermal techniques, as compared to clas-
sical thermophysical methods.35 In addition, being both thermal
and optical techniques, photothermal methods provide an extended
pool of information with a small influence from a scattering
matrix. As the density and thermal expansion coefficients of nano-
fluids are determined by the base fluid, it is possible to find espe-
cially important features of the test object connected with the
heterogeneity effect of NFs. The latter is particularly important as
the majority of classical thermophysical methods can provide
average characteristics of the sample only,37,288 thus forcing empiri-
cal approaches in designing nanofluids mentioned above.
The advantages of photothermal spectroscopy are not limited
to the information on the base fluid and the possibility to assess
the disperse phase more accurately. In many cases, including NFs
and their biomedical applications, the actual spatial heterogeneity
and the mechanism of heat transfer are quite important. Here,
various microspectroscopic photothermal modalities can be of
serious value. They provide images of tissues,31,322 cells,197,323 and
single and assembled nanoparticles206,324 with a high resolution
challenging the diffraction limit due to joint use of optical as well
as thermal imaging governed by the characteristic rates of nonra-
diative heat transfer.33,207,325 This provides both thermal and
optical sample nondestructive quantitative mapping with a nano-
scale locality.30,34,175,177,326 Recent results show that photothermal
microspectroscopy is capable of non-destructive characterization of
carbon nanomaterials and nanoparticle dispersions.209,228,327–333
Photothermal imaging and microscopy techniques are closely
related with another state-of-the-art trend in photothermics, the
development of single particle photothermal modalities. These
methods include photothermal difference interference contrast,334,335
photothermal heterodyne microspectroscopy,311,336,337 and photother-
mal correlation microspectroscopy32,338,339 and are capable of mea-
suring single submicrometer particles. Nowadays, these techniques
mainly target biomedical research but may be even more relevant
for nanoparticle systems with multiple phase composition (like
hybrid NFs) or complex structural properties (like microencapsu-
lated phase-change materials).340
In these microspectroscopic modalities, the photothermal
effect upon the absorption of an excitation beam by a single nano-
object (a heated large molecule or a nanoparticle) causes the scat-
tering of a probe beam, which can be detected as a fluctuation of
its power due to the interference of the initial beam and scattered
radiation around.341 Photothermal heterodyne microspectroscopy
was introduced as imaging310,311,342,343 and spectroscopy344,345 of
nano-size particles. Photothermal correlation microspectroscopy,
an advanced technique based on photothermal heterodyne spectro-
scopy,32,338,339 is based on building an autocorrelation function
G(τ) for time-resolved photothermal signal S(t),
G(τ) ¼ hS(t)S(t þ τ)i/hS(t)i2 ,
which provides characteristic times τ of the heat-releasing processes
of the underlying photothermal phenomena. As the photothermal
processes for nanoparticle solutions depend on the thermal and
optical properties of nanoparticles and their motion velocity, this
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provides detecting, monitoring, and characterizing such objects. In
the simplest concept related to thermal lensing (Sec. IV E) and cor-
relation spectroscopy,324,346,347 a single absorber particle acts like
an analog of a “macro” thermal lens, a nanolens, which can be
detected using a scattering pattern of the probe radiation from a
“halo” of the thermally induced field around the heated particle.
The combination of the nanolens concept and a differential
mode-mismatched excitation-probe schematics30,291,348,349 is a very
promising microscopic technique called twin-focus photothermal
correlation spectroscopy.350 This technique detects two spatially sep-
arated volumes of the sample and reference building two autocorre-
lation functions for each of the volumes separately. It provides a
tool for precise measurements of a slow motion along the beam
axis or very slight changes in heterogeneities at nanometer scales in
the sample. Such measurements beyond the diffraction limit can be
used for probing nanoparticles tailored to NFs from the viewpoint
of the mechanism of heat transfer.
Finally, as we showed in Sec. IV, nondestructive and fast char-
acter of many photothermal techniques such as photoacoustic
modalities and thermal lensing along with relative simplicity of
instrumentation make them very robust monitoring techniques.
This is currently used in biomedical studies, both in vitro and ex
vivo (flow cytometry)192,351–353 and in vivo.246,354,355 Such modali-
ties can be very valuable for monitoring the workability of nano-
fluids in industrial scale (such as nuclear and solar energy), while
the development of compact photothermal instruments356,357 may
be of value for small-scale and widespread NF applications in com-
puters, appliances, etc.
Certainly, photothermal spectroscopy is not free from some
drawbacks and limitations. First, as major photothermal methods
(thermal lensing, optical beam deflection, photothermal radiome-
try) are based on thermal diffusivity, to assess the thermal conduc-
tivity coefficient of NFs, other methods for the density and specific
heat are required. These are no single measurements, as these
values are required for each concentration in the desired range at
all the working temperature range of a NF or rely on some detailed
preliminary data or precise regularities. This certainly degrades or
at least questions both accuracy and precision of the final values of
thermal conductivity by photothermics. Certainly, this is a disad-
vantage of all the methods for NFs based on thermal diffusivity
and may be a reason behind differing data for the same nanofluids
in the literature. Thus, it seems expedient to use several comple-
mentary photothermal techniques based on thermal conductivity
and thermal diffusivity229,230 or thermal effusivity and thermal dif-
fusivity. In principle, this can be implemented in a single setup;
therefore, it would provide all the key parameters of a nanofluid (as
we discussed above, in two-modality PTS measurements, thermal
conductivity can be assessed or calculated from photothermal
experiments only, without external data).
As we have shown in the main body of this paper, the applica-
tion of the methods of photothermal spectroscopy to determine the
thermal properties of liquids and, moreover, dispersed systems have
many merits. Still, a reader may say that they are rather scarce still,
and they demonstrate the possibilities for a rather limited set of
nanofluids. In our opinion, this is caused by two main reasons: (a)
lack of methodology and (b) lack of standardized photothermal
instruments.
128, 190901-19
 Journal of
Applied Physics
The analysis of the data shows that building a methodology
for nanofluids requires solving the following issues.
(i) In many photothermal modalities, the theory is based on
either homogeneous media or a single nanoscale object.30
Thus, it necessitates either to develop a theory of the genera-
tion of the photothermal signal in complex objects or correct
the existing theories. This is especially important for
ensemble-based slow techniques such as thermal lensing and
optical beam deflection.
(ii) The issues related to the experiment planning also require con-
sidering new factors both connected with nanofluids and the
possible operation modes. Therefore, the setups should be
based on flow techniques and should provide both transient
and steady-state measurements. Thermal-lens spectrometry
would require a minimum change; for other photothermal
techniques and modalities, some work is in order.
Instrumentation issues are more general as such a situation is char-
acteristic for any types of photothermal applications. In our
opinion, it requires the following:
(i) The first important issue is the unification of photothermal
apparatuses. Despite several companies in the market and
industrial applications and many excellent prototypes,357–362
many photothermal apparatuses are home-built for certain
research applications. This results in difficulty in comparing
apparatuses, even those based on the same principle. This in
turn results in the lack of standard samples and no detailed
uncertainty data in photothermics.
(ii) As the measurements of dispersed systems require a special
set of time, concentration, and excitation powers, the special-
ized setups built for specific types of nanofluids are probably
required. The techniques such as photoacoustic modalities,
optical beam deflection, and PTR require special cells or
compartments for liquid media.
(iii) A broader comment is appropriate here. The serious progress
in photothermal methods in many branches of industry
and research already demands a special initiative—alike
“Nanouptake” action for nanofluids—to photothermal
market-uptake due to large possibilities for photothermal
instrumentation.
Despite rather difficult and serious tasks of methodology and
instrumentation, they are resolvable, and they are required
for nanofluid research in photothermal spectroscopy. Witnessing
the boom in multi-spectral optoacoustic tomography
(MSOT),193,194,200,203,355,363–373 the area neighboring to photo-
thermal techniques, we believe that it will be made in the nearest
future.
Moreover, our experience in photothermal spectroscopy allow
us to state that the complex character of photothermal techniques
makes them a valuable tool, and disadvantages could be turned to
advantages. The examples below can possibly serve as other fea-
tured applications of photothermal spectroscopy in nanofluids and
related research:
• Detection of the Soret effect, which is usually a negative factor in
NFs and may be the cause of their deterioration, can be assessed
J. Appl. Phys. 128, 190901 (2020); doi: 10.1063/5.0024332
Published under license by AIP Publishing.
PERSPECTIVE scitation.org/journal/jap
using photothermal techniques in the same run of the
experiment.
• As nanofluid thermophysical properties are used in other
applications such as thermally resistant lubricants and fuels
(a nanoparticle-filled biodiesel mentioned above212), photother-
mal methods may be used for testing the two-phase thermally
conductive liquids with the same type and concentration of the
disperse phase but with a varying composition of the base fluid.
• As photothermal spectroscopy may provide the spectra of
thermal properties,186,356,374–376 this could be especially valuable
for photothermally induced NFs, e.g., in solar energetics.
All these features of photothermics may be combined in developing
areas of nanofluid research. In our opinion, new types of nanofluids
will be a subject of research. They are NFs based on natural nano-
particles such as clay minerals377 and core–shell nanoparticles.
Also, double-action heat-accumulating nanofluids such as microen-
capsulated phase-change materials should be mentioned,340 which
are introduced into building materials but may be extended to
many heat-transfer applications.
Other promising NF-related materials for photothermal
methods are thermal slurries and thermally conductive pastes that
are used in various industries such as computers and energy
storage. Microencapsulated phase-change material slurries improve
the value of critical heat flux by as much as 100%–200% as a result
of nanoparticle deposition on the surface of the component.378
Also, nanolayers formed at nanoparticle–liquid interfaces,122,379
nanoparticle clustering, and some other mechanisms of heat trans-
fer that improve the workability of NFs in addition to the primary
increase in thermal conductivity are interesting concepts that await
instrumental control and evaluation. A combination of thermal-
lens and mirage modalities can be a concept of controlling both the
solution and the surface.
Anyway, the complex problem of nanofluid design, develop-
ment, and application will undoubtedly advance and progress in
the nearest future, and it will find many new ideas and concepts.
By the phenomena beneath, abilities, and the current status as well
as the theory and instrumentation, photothermal spectroscopy
undoubtedly provides very promising tools for nanofluids.
AUTHORS’ CONTRIBUTIONS
L.O.U., M.V.K., and M.A.P. contributed equally to this work.
ACKNOWLEDGMENTS
This work was supported by the Russian Foundation for Basic
Research (Grant Nos. 18-33-00586mol_a and 19-08-00498 a).
DATA AVAILABILITY
The data that support the findings of this study are available
from the corresponding author upon reasonable request.
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