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Whispering-Gallery Exciton Polaritons in Submicron Spheres
Whispering-Gallery Exciton Polaritons in Submicron Spheres
Whispering-Gallery Exciton Polaritons in Submicron Spheres
I. V. Iorsh
Ioffe Institute, Polytechnicheskaya 26, 194021 St. Petersburg, Russia
A. V. Kavokin*
Department of Physics, University of Rome II, 1 via della Ricerca Scientifica, Rome 00133, Italy
共Received 17 November 2008; revised manuscript received 16 March 2009; published 23 June 2009兲
We show that a semiconductor sphere with a radius comparable with the wavelength of light at the exciton
resonance frequency can behave as a high-quality three-dimensional microcavity or “polariton dot.” We obtain
numerical results for gallium arsenide submicron spheres and demonstrate that, in contrast to a larger sphere or
planar microcavity, they can simultaneously possess both large quality factor and high finesse. In the strong-
coupling regime the Rabi splitting approaches the bulk polariton splitting.
冑 冉
BEC.11,12 Despite the fact that the formalism describing the
interaction of excitons with the photonic modes of a sphere k m 兩m兩
ជ l,m = −
E Pl 共cos 兲eជ
is well developed, a complete and systematic analysis of the sin
冊
optical-mode spectrum is yet to be provided. In most of the
literature on exciton polaritons in spheres, the only modes 兩m兩
+i 关P 共cos 兲兴eជ V共r兲exp共im兲, 共1a兲
discussed have been those with the quantum number l, which l
ជ l,m =
H 再 l共l + 1兲
r
V共r兲P兩m兩
l 共cos 兲e
ជr + 冉
兩m兩
关P 共cos 兲兴eជ
l by
The reflection coefficient7 for the TE polarization is given
+
im 兩m兩
sin共兲
Pl 共cos 兲eជ 冊1
r r
冎
关rV共r兲兴 exp共im兲, R共TE兲 =
共1兲
Cl1
共1兲
Cl2
共1兲
− Cl2
共2兲
− Cl1
共4兲
ជ l,m = 冑k
H 冉 m 兩m兩
P 共cos 兲eជ
sin l
Substituting Eq. 共4兲 into Eq. 共3兲, one can write the equa-
tion for the eigenfrequencies of the TE modes in the form
冊 h共1兲 共1兲
l 共k2r0兲关j l共k1r0兲 + k1r0 j l⬘共k1r0兲兴 − j l共k1r0兲关hl 共k2r0兲
+ i 关P兩m兩 共cos 兲兴eជ V共r兲exp共im兲, 共2a兲
l + k2r0h共1兲
l ⬘共k2r0兲兴 = 0. 共6兲
Eជ l,m = 再 l共l + 1兲
r
V共r兲P兩m兩
l 共cos 兲e
ជr + 冉
兩m兩
关P 共cos 兲兴eជ
l
Similarly, substituting Eq. 共5兲 into Eq. 共3兲, the equation for
the eigenfrequencies of the TM modes has the form
冊 冎 2h共1兲 共1兲
1 l 共k2r0兲关j l共k1r0兲 + k1r0 j l⬘共k1r0兲兴 − 1 j l共k1r0兲关hl 共k2r0兲
im 兩m兩
+ Pl 共cos 兲eជ 关rV共r兲兴 exp共im兲. + k2r0h共1兲
sin共兲 r r l ⬘共k2r0兲兴 = 0. 共7兲
共2b兲 Equations 共6兲 and 共7兲 can also be obtained by matching the
tangential components of the electric and magnetic fields
Note that the radial dependence of the tangential component
taken from Eqs. 共1兲 and 共2兲. In the case of large sphere radius
of the electric field is given by V共r兲 = Ah共1兲 共2兲
l 共kr兲 + Bhl 共kr兲 for the asymptotic expressions for the spherical Hankel func-
the TE polarization, while this expression describes the tan-
tions, viz., h共1,2兲
l 共kr兲 → ⫿ kri exp共⫾i关kr − 2l 兴兲, can be used to
gential component of the magnetic field for TM polarization.
obtain a simplified equation for the real part of the frequency
Now consider a sphere of radius r0 made of material hav-
of the eigenmode of the sphere,
ing a refractive index n1 surrounded by a medium with re-
fractive index n2. An electromagnetic field inside the sphere 2n1r0共TE,TM兲
can be represented as the sum of incoming and outgoing ⬇ 共2N + l兲 − arg共R共TE,TM兲兲. 共8兲
spherical waves. However, the field at the center of the mi- c
crocavity should be finite, which, in the case of an empty For a gallium arsenide 共GaAs兲 sphere in vacuum arg共R共TE兲兲
microcavity, requires that the incoming and the outgoing ⬇ 0 and arg共R共TM兲兲 ⬇ , so that
waves have equal amplitudes in the central core and the ra-
dial dependence of the field is described by a spherical c共2N + l兲
Bessel function j共1兲 共1兲 共2兲 n1r0共TE兲 ⬇ 共9a兲
l 共x兲 = 关hl 共x兲 + hl 共x兲兴 / 2. Thus, the elec-
,
2
tromagnetic field of the eigenmodes is described by Eqs. 共1兲
and 共2兲 with V共r兲 = jl共kr兲. On the other hand, at the interface
of the sphere and the surrounding medium, the amplitude of c共2N + l + 1兲
n1r0共TM兲 ⬇ . 共9b兲
the ingoing wave must be equal to the product of the ampli- 2
tude of the outgoing wave and the amplitude reflection coef-
ficient R of that spherical wave from the boundary of the In the subsequent analysis, we will use the double index lN,
sphere. Hence, the equation for the optical eigenmodes of a where N is the radial quantum number in order to define the
spherical microcavity with radius r0 can be represented in the specific mode.
form The minimum radius of the sphere at which a mode of
frequency with a specific l exists 共which will be referred to
R共TE,TM兲h共1兲 共2兲
l 共kr0兲 = hl 共kr0兲. 共3兲 subsequently as the first mode TEl0, TMl0兲, can be esti-
mated from Eq. 共9a兲 for the TE polarization by putting N
Equation 共3兲 defines the eigenfrequencies of both the TE and = 0,
TM eigenmodes. We note here that in the case of the TE
mode the reflection coefficient R共TE兲 is defined as the ratio of cl
the tangential component of electric fields for the ingoing n1r共TE兲
0
共TE兲
⬇ . 共10a兲
2
and outgoing waves, while for the TM wave R共TM兲 is the ratio
of the tangential components of the magnetic fields. For the TM polarization the corresponding result is
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WHISPERING-GALLERY EXCITON POLARITONS IN… PHYSICAL REVIEW B 79, 245322 共2009兲
1.0
0.8
TE3
|R|2
0.6
TE2
0.4 TE1
0.2
TM1
TM2
TM3
0.0
0 200 400 600 800 1000
r (nm)
c共l + 1兲
n1r共TM兲
0 共TM兲 ⬇ . 共10b兲
2
However, for radial quantum number N = 0, the radius of the FIG. 2. 共Color online兲 共a兲 Dependence on l of the minimum
sphere is comparable to the wavelength corresponding to the radius of a GaAs sphere at which a particular mode exists. The
eigenmode energy, and the formulas in Eqs. 共9兲 and 共10兲 are photon energy of the first mode with specific l and radial quantum
not good approximations. Better approximations can be number N = 0 共TEl0, TMl0兲 is chosen to be 1.515 eV. Open 共solid兲
symbols correspond to the value obtained for the TM 共TE兲 polar-
made by observing that if the refractive index of the sphere is
ization using Eqs. 共6兲 and 共7兲. The lines show the results obtained
larger than that of the outer medium, the electric field of the
using the simplified Eq. 共10兲 共dashed line兲 and Eq. 共11兲 共solid line兲
eigenmode should have an antinode at the boundary of the
for the eigenfrequencies of the cavity modes for the TM 共upper/red兲
sphere. It follows from Eqs. 共6兲 and 共7兲 that jl共kr兲 should and TE 共lower/green兲 polarizations. 共b兲 Dependence on l of the
have a maximum at the boundary of the sphere for a TE radiative decay rate of the first mode 共N = 0, photon energy
mode, while jl⬘共kr兲 has a maximum for a TM mode. Now, = 1.515 eV兲. Open 共solid line兲 symbols correspond to the value
according to a theorem of Siegel, the first root of jl共x兲 is obtained for the TM 共TE兲 polarization using Eqs. 共6兲 and 共7兲. The
confined between the values 冑共l + 1 / 2兲共l + 5 / 2兲 and lines show the results obtained using the simplified Eq. 共13兲 for the
冑2共l + 3 / 2兲共l + 7 / 2兲 while the first root of jl⬘共x兲 is confined TM 共upper/red兲 and TE 共lower/green兲 polarizations. The horizontal
between the values 冑共l + 1 / 2兲共l + 5 / 2兲 and solid line indicates the threshold between the weak-coupling and
冑2共l + 1 / 2兲共l + 3 / 2兲. Using these results it is possible to de- strong-coupling regimes.
duce an improved estimate of the minimum radius at which
the first mode with a given l exists. For a TE mode, r共TE兲 0 is ␥ ␣4l+12l/2−5/2
given by = 4 , 共13a兲
⌫ 共l + 3/2兲n5l+1/2
n1共TE兲r共TE兲
0 ⬇ 1.3c共l + 1兲 共11a兲 where ␣ = 1.3共l + 1兲 and n = n1 / n2.
whereas for the first TM mode, For the first TM mode the corresponding expression is
245322-3
PLATTS et al. PHYSICAL REVIEW B 79, 245322 共2009兲
10
0.1 11 21
10 11 22 13
20 21
12 31 12
22
TM20
32
0.01
20 31
41 m=0
30 41
30
51 51
10-3
γ (eV)
40 40
10-4 50
50
60
10-5 60
70
70
10-6
100 150 200 250 300 350 400 450
r0 (nm)
冉 冊
acterized by heavier effective masses.
To estimate analytically the value of the 共Rabi兲 splitting ⌬ LT
1+ 2 = ex
2
共17兲
of the polariton modes, we consider how the exciton interac- ex −
tion affects an optical mode of the spherical cavity that
would be at frequency ex in the absence of excitonic effects, or
when the cavity would simply have a relative permittivity b. 2LT
For such a bare cavity mode, the cavity and mode parameters 共 − ex兲共 + ex兲 − = 0. 共18兲
are related by Eq. 共9兲 or Eq. 共11兲, which can be rewritten in
− ex
the form Assuming that − ex Ⰶ ex we obtain
共TE,TM兲2
bex
2
r0 = A共l兲, 共15兲 exLT
共 − ex兲2 ⬇ . 共19兲
where A共l兲 is the appropriate function of l. However, when 2
excitonic effects are included, the relative permittivity of the Thus the splitting of polariton modes is
cavity is 1 ⬇ b共1 + exLT− 兲, if the nonradiative exciton decay
is neglected, and the equation for the polariton eigenenergies ⌬ = 冑2exLT . 共20兲
is This result is not exclusive to the case of spherical symmetry,
冉
b 1 +
LT
ex −
冊
2r20 = A共l兲. 共16兲
but it is worth noting that the Rabi splitting for the sphere is
generally larger than for planar microcavities with Bragg
mirrors because the electric field of the cavity mode is
Combining Eqs. 共15兲 and 共16兲 yields mostly localized inside the sphere and thus its overlap inte-
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WHISPERING-GALLERY EXCITON POLARITONS IN… PHYSICAL REVIEW B 79, 245322 共2009兲
Energy (eV)
1.520
III. RESULTS AND DISCUSSION 1.515
TE30
It follows from Eq. 共12兲 that the radiative decay of the 1.510
photon mode in a sphere depends on two factors, namely, the 1.505
reflection coefficient of the spherical wave from the bound-
ary of the sphere and the radius of the sphere. Minimization 1.500
of ␥ can be achieved either by increasing the reflection co- 1.495
efficient R toward unity or by increasing the size of the 188 190 192 194 196 198 200 202
sphere. However, increasing the size of the sphere leads to an r0 (nm)
increase in the density of photonic modes, which reduces the
finesse of each individual mode. FIG. 5. 共Color online兲 The real part of the photon energy of the
Figure 1 shows for various outgoing spherical waves the first polariton modes of a GaAs sphere as a function of its radius.
dependence of the power reflection coefficient 兩R兩2 on the Within the interval of the radii considered only two bare optical
radius r of a spherical interface between GaAs with a refrac- modes exist: TM20 and TE30 共shown by solid lines兲. The vertical
tive index n1 = 3.7 共the incident medium兲 and vacuum 共n2 bars show the values of ␥ for the modes. The horizontal line shows
the energy of the exciton resonance.
= 1兲. One can see that for kr ⬍ l the reflection coefficient 兩R兩2
approaches unity with decreasing radius; for kr ⬎ l, 兩R兩2 as- coupled with the exciton resonance, the finesse of the modes
ymptotically approaches the value 兩共n1 − n2兲 / 共n1 + n2兲兩, which is so low that they are not suitable for polariton lasing. Fig-
is the plane-wave limit. Note that the reflection coefficient ure 3 shows that one can always find a mode tuned to the
always remains less than unity 共strictly speaking, total inter- specific frequency which possesses a substantial finesse and
nal reflection never takes place in the spherical geometry兲. a sufficiently low decay rate but only for a value of l larger
Note also that for the TM modes there is a broad minimum in than unity. For example, if the radius of a GaAs sphere is just
the dependence of 兩R兩2 on r, which is associated with the below 200 nm, the TE30 mode has a decay rate below the
analog of the Brewster effect for spherical waves.7 threshold and is suitable for strong coupling, while the TM20
According to Eqs. 共10兲 and 共11兲, the critical radius at mode is characterized by a decay rate just above the thresh-
which the first mode 共TEl0, TMl0兲 of a GaAs sphere in old.
vacuum comes into resonance with the bulk exciton energy, Figure 4 shows the profile of the electric field for the
increases with increasing l, as illustrated in Fig. 2共a兲. Figure TM20 and the TE30 modes for m = 0. The TE30 mode, hav-
2共b兲 shows the field amplitude decay rate ␥ corresponding to ing a decay rate ␥ = 3 meV, is apparently almost perfectly
the photon modes, and this decreases nearly exponentially as localized within the sphere, while for the TM20 mode with
l increases. It can be seen that only the TM modes with l ␥ = 28 meV, the tail of the field outside the sphere is visible.
ⱖ 3 and TE modes with l ⱖ 2 satisfy the strong-coupling con- The difference in the penetration depth of the light field into
dition. the vacuum is responsible for the difference in their decay
Figure 3 shows the dependence on sphere radius r0 of the rates.
decay rate of the mode with the real part of the eigenfre- Figure 5 shows the dependence of the real parts of the
quency tuned to the exciton resonance in GaAs 共1.515 eV兲. It eigenfrequencies of the TE30 and TM20 modes on sphere
can be seen that with increasing radius more and more radius and the decay rates of these modes. The modes are not
modes 共with radial quantum numbers N = 1, 2, 3, etc.兲 appear. degenerate as predicted by the approximate formulae in Eqs.
Equation 共12兲 states that ␥ depends explicitly on the sphere 共9兲 and 共11兲 but the difference in their energies is less than
radius r0 and also implicitly on it through the reflection co- 5%. For the TM20 mode, ␥ exceeds the Rabi splitting given
efficient R 关see Eqs. 共4兲 and 共5兲兴. It is instructive to consider by Eq. 共18兲, which is characteristic of the weak-coupling
increasing the sphere radius from an initial very small value. regime. In contrast, for the TE30 mode the decay rate is
For a mode with specific l, the initial increase in sphere smaller than the Rabi splitting, so that the strong-coupling
radius and the corresponding rapid decrease in reflection co- regime is realized, and this explains the anticrossing of the
efficient that is seen in Fig. 1 lead to an increase in ␥. Further exciton and photon modes seen in the figure. The simple
increase in sphere radius causes the reflection coefficient for nature of semiconductor submicron spheres and the possibil-
a spherical wave at a spherical boundary to tend to the ity of achieving strong coupling of photons and excitons in
equivalent value for a planar surface, as shown in Fig. 1. At them suggest that they have significant promise for use in
this point the sphere radius itself has more bearing on ␥ than polariton lasers.
the reflection coefficient does and, due to the inverse depen-
IV. CONCLUSIONS
dence of ␥ on r0, ␥ slowly decreases. On the other hand, in
the limit of large radius, the density of modes becomes so For the optical modes of semiconductor spheres, we have
large that even if many of the modes are formally strongly considered the criteria for the simultaneous achievement of a
245322-5
PLATTS et al. PHYSICAL REVIEW B 79, 245322 共2009兲
high finesse and a sufficiently high-quality factor to produce lows the polariton dot to be considered as a promising can-
strong coupling with the exciton resonance in the semicon- didate for use in a polariton laser.
ductor material. It is demonstrated numerically for the spe-
cific case of gallium arsenide spheres that the modes with
smaller l are in the weak-coupling regime and the modes ACKNOWLEDGMENTS
with larger l are in the strong-coupling regime. We have
obtained the specific conditions required for the strong cou- The work was supported in part by the EPSRC, the Royal
pling of an exciton and an isolated photon mode which al- Society, and the EU.
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245322-6