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Surface exciton polaritons: Following in the footsteps of plasmonics

Surface exciton polaritons: Following in the footsteps of plasmonics

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An essay for the 2012 Undergraduate Awards (International Programme) Competition by Howard Moshtael. Originally submitted for Physics at University of St. Andrews, with lecturer Dr Graham Turnbull in the category of Mathematical & Physical Sciences
An essay for the 2012 Undergraduate Awards (International Programme) Competition by Howard Moshtael. Originally submitted for Physics at University of St. Andrews, with lecturer Dr Graham Turnbull in the category of Mathematical & Physical Sciences

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Published by: Undergraduate Awards on Aug 31, 2012
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10/27/2013

 
1
 
Surface exciton polaritons: Following in the footsteps of plasmonics
The surface exciton polariton (SEP) is a surface electromagnetic wave that arises due to the coupling of light todelocalized excitons at the surface of materials. They show promise for use in applications such as non-linear opticsand nanophotonics, analogous to the use of surface plasmon polaritons in these areas. SEPs can be excited at a singleinterface, but have longer propagation lengths when two SEPs couple across a thin film of absorbing dielectric. Thisreview essay will consider the dispersion relations for both single and double interfaces. This will allow somecharacteristic length scales, which are important for their analysis, to be defined. The two principal methods forexciting SEPs are prism coupling and grating coupling. The principles for these techniques are described andevaluated, and measurements from early implementations of these methods are presented.
1. Introduction
Light is playing an increasingly important role in themodern world. Gone are the days when it was simplyused for illumination. We are now dependent on lightfor telecommunications, various medicinal applicationsand many forms of entertainment. As ourunderstanding of how it interacts with matter isdeepening, its technological uses are becoming evermore ubiquitous, particularly since the advent of thelaser. And as this interaction becomes ever more direct,for example by using light to control matter as is donewith optical tweezers, we can expect this trend tocontinue.When light propagates along the interfacebetween two media, and if its amplitude decaysexponentially into the media, then it is defined as asurface electromagnetic wave [1]. When this wave iscoupled to a polarization excitation it is defined as asurface polariton [2 - 3]. There are various types of elementary excitation, such as plasmons, whichdescribe the collective vibrations of electrons, andexcitons, which describe electron-hole excitations [4].When one of the media is a metal and the other adielectric, the surface polariton is called a surfaceplasmon polariton (SPP) [5]. SPPs have beenthoroughly investigated and have various applicationssuch as to characterize the optical properties of complex structures [6], sub-wavelength optics inmicroscopy [7], lithography beyond the diffractionlimit [8] and bio-molecular sensors [9].A more recent topic of investigation is thesurface exciton polariton (SEP), which does not requireany of the media to be metallic. The fundamentalscience for the SEP was developed by Maradudin andMills in 1973 [10,11] who drew on earlier work byRuppin and Englman [12]. The first experimentalobservation of the SEP was achieved by Lagois andFischer in 1975 [13]. This early work done on SEPsassumed it was necessary to use the boundary betweena dielectric medium and a crystal with Wannier-typeexcitons [14] as elementary bulk excitation [4].Little attention was paid to the SEP untilpioneering work was done by Fuzi, Sambles andBradberry in 1990 [15]. They used thin films of vanadium at the infrared frequency, where this materialbehaves as a strongly absorbing dielectric, anddemonstrated the excitation of SEPs. In later work,they showed the generation of SEPs using othermaterials such as organic films and palladium. [1, 16].Takabayashi
et al.
used silicon at 633nm, thoughwhether or not their results showed SEPs rather thansimply TM
0
modes was contested by Giannini
et al.
 [5]. In 2008 Chu
et al.
used electron energy-lossspectroscopy to excite SEPs in gold nanoparticles atfar-ultraviolet frequencies where gold is a stronglyabsorbing dielectric [17]. In the same year, Giannini
et al.
excited SEPs in ultra-thin layers of amorphoussilicon [5].Until 2009, conventional understanding of SEPs assumed it was necessary to use materials with asharp excitonic absorption, in other words to have theimaginary component of the dielectric constant,
,much larger than the real component,
. However,Liou
et al.
demonstrated the excitation of SEPs inmonoclinic HfO
2
which has only a weak excitonicabsorption [18]. This led to the relaxed SEP-excitationcondition of 
. This has opened up a widerspectrum of materials which could support SEPs,including the recent discovery by Huang
et al.
of theexcitation of SEPs in ZnO [19].In section 2 the relevant dispersion relationsfor SEPs will be derived for both a single interface anda thin film. From this the various modes of SEPs willbe found and the relevant length scales will be defined.In section 3 the principal experimental techniques forexciting SEPs, prism and grating coupling, will bedescribed and evaluated. Section 4 will present someimportant experimental results that demonstrate theirexcitation, and section 5 will look towards futuredevelopments in this field and possible applications.
2. The dispersion relations
Central to the understanding of SEPs is knowledge of the appropriate dispersion relation for the geometry of media being used. Here, we derive and discuss thedispersion relations for two geometries: First, thesingle interface between two semi-infinite media; andsecond, a thin film of material sandwiched betweentwo semi-infinite media. The special case where thesurrounding materials to the thin film are identical willbe highlighted.The electromagnetic surface wave propagatesalong the surface of the medium as a longitudinalsurface charge density wave, which can be pictured asillustrated by figure 1. These waves are thereforetransverse magnetic (TM), with the magnetic vectorlying in the plane of the interface. The dispersion
relations can be derived starting from Maxwell’s
equations:

 
 
2
 

 
Figure 1: Illustration of the SEP propagating as a surfacecharge density wave along the surface of a medium. Theelectric field lines are drawn and the magnetic field is into thepage.
The coordinate axes are chosen such that the
 z
-axis is perpendicular to the surface and the
 x
-axis isin the direction of propagation, as shown in figure 2.For TM waves there are only three components of theelectric and magnetic fields:
 H 
 y
 ,
 x
 
and
 z
. Themagnetic field is given by,
 
 where

is the complex wavevector, orpropagation constant,
is the angular frequency,
isthe normalization constant, and
 
is the
 z
 dependence of the magnetic field. Putting this intoequation 1 yields expressions for the electric fieldcomponents:


 


 Putting these expressions into equation 2 yields a onedimensional wave equation:

 
 where
is the vacuum wavevector. Thesolution to this equation depends on the geometry of the media.
2.1 A single interface
Figure 2 shows the simplest configuration: two planarmedia joined at a single interface. One of the media istaken to be an absorbing dielectric with complexpermittivity, and the other a non-absorbing dielectric.As we want to find a solution such that the field decaysaway from the surface we set
 
as such:
 
 
 
 
 
 where, from the wave equation,
 
8)
Maxwell’s equations require the tangential
electric field,
 E 
 x
, to be continuous across the interfaceof two isotropic media. This requirement yields thedispersion relation,
 
 
Figure 2: Schematic representation of the configuration of anabsorbing medium and a non-absorbing medium broughttogether at a single interface. The coordinate system is alsoshown, with
 z
= 0 taken to be at the interface.
In order for a surface wave to exist on a singleinterface, this dispersion relation must be satisfied. Inaddition, it should be noted that for the field to decayinto the two media, rather than be radiative, we require,


 from equations 7a and 7b. The solution of interest hereis for medium 2 to be an absorbing dielectric, with acomplex dielectric constant, though it should be notedthat this is not the only solution (See reference [1] for amore detailed analysis). If we take
, then

, and we find,
 

 


 
 
 


 


 
This is the surface exciton polariton mode. As
is the vacuum wavevector, and
is the dielectricconstant of medium
 j
, then
 
is the wavevector of light in material
 j
. From equation 10a it can be seenthat
 
. In other words, the wavevector of thelight in the non-absorbing medium, which is incidentupon the interface, is larger than the wavevector of theSEP. This is in direct contrast to the surface plasmonpolariton where
 
, which would be obtainedif medium 2 was a metal [1]. This suggests that theSEP can be directly excited from a light wave incidentfrom the ordinary dielectric, medium 1 [15]. An earlyobservation of this type of mode was made by Brillante
et al.
in 1978 [20].In deriving the expressions for the real andimaginary components of the wavevector the specialcase of 
was used. However, it can be shownthrough numerical evaluation that this is not necessaryfor the SEP to be excited. This is illustrated in figures3a and 3b which show the dependence on
of 
and
respectively. Thus for a region around
themode can be excited, so long as
.

 
 
 
 
 
 
+ + +- -
H
 
3
 
Figure 3: Variation of a)
and b)
with
.

,

,
 


. Curve 1,
;curve 2,

; curve 3,

; curve 4,

. [1]
2.2 Thin film surrounded by non-absorbingdielectrics
We will now consider what happens when two of thesesurface modes are brought close enough together tocouple. Figure 4 shows the configuration of this secondcase to be considered: that of a thin absorbing dielectricwith a complex dielectric constant,
, surrounded bynon-absorbing dielectrics characterized by
and
.Coupling can occur when the thickness of the film,
,is smaller than the penetration depth of the field.
 
In thiscase, the
 z
-dependence of the fields would be given by,
 

 
 
 


 
 
 

 
 where
,
 j
= 1,2,3 are as in equation 8.Using the boundary conditions that thetangential electric and magnetic fields,
 E 
 x
and
 H 
 y
, mustbe continuous across the boundaries at
 z =
0 and
 z
= -
,the dispersion relation is found to be,



 
Figure 4: A representation of the geometry of the second caseconsidered: that of an absorbing dielectric of thickness
 sandwiched between two non-absorbing dielectrics.
 z
= 0 istaken to be at the interface between mediums 1 and 2.
In the case of a symmetrically surroundedabsorbing dielectric,
and
. In this case,there are two dispersion relations corresponding to thefield being symmetric and antisymmetric in
 H 
 y
. Byusing these conditions, these symmetric andantisymmetric dispersion relations are analyticallyderived as equations 13 and 14 and respectively.


 


 
These are known respectively as the longrange surface exciton polariton (LRSEP) and the shortrange surface exciton polariton (SRSEP). For the longrange mode, the tangential component of electric field,
 E 
 x
, is antisymmetric with respect to the middle of thefilm at
 z
=
 /2, and thus is largely excluded from theabsorbing layer. Consequently it has a longerpropagation length than both short range modes andSEPs at a single interface, because they interact onlyweakly with the absorbing layer. As the short rangemode has a tangential electric field component that issymmetric at
 z =
 /2 it has a shorter propagationlength.It is useful to have analytical expressions forthe real and imaginary components of the wavevector,as was obtained for the single interface in equations10a and 10b. Not only would the expressions giveinsight into the nature of the mode, but they would alsoenable direct calculation of the wavelength of the SEPand their propagation length. This cannot be foundexactly from the dispersion relations but Fuzi
et al.
derived approximate analytical expressions for the longrange mode by taking the thin film limit, in otherwords, when

. This enables equation 13 tobe expanded out to first order,
 
to obtain,
 




 
 




 
 
 
 
 
 

 
 
d

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