The theory of exciton states in quasi-zero-dimensional semiconductor systems
For a semiconductor quantum dot (QD), the contributions made to the exciton energy spectrum by the electron and hole kinetic energies, the energy of Coulomb interaction between them, and the energy of their polarization interaction with the spherical interface between the QD and the dielectric mediu...
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України
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irk-123456789-1216382017-06-16T03:03:37Z The theory of exciton states in quasi-zero-dimensional semiconductor systems Pokutnyi, S.I. For a semiconductor quantum dot (QD), the contributions made to the exciton energy spectrum by the electron and hole kinetic energies, the energy of Coulomb interaction between them, and the energy of their polarization interaction with the spherical interface between the QD and the dielectric medium have been analyzed. 2006 Article The theory of exciton states in quasi-zero-dimensional semiconductor systems / S.I. Pokutnyi // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2006. — Т. 9, № 4. — С. 1-6. — Бібліогр.: 17 назв. — англ. 1560-8034 PACS 71.35; 73.20; 73.40 http://dspace.nbuv.gov.ua/handle/123456789/121638 en Semiconductor Physics Quantum Electronics & Optoelectronics Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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For a semiconductor quantum dot (QD), the contributions made to the exciton energy spectrum by the electron and hole kinetic energies, the energy of Coulomb interaction between them, and the energy of their polarization interaction with the spherical interface between the QD and the dielectric medium have been analyzed. |
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The theory of exciton states in quasi-zero-dimensional semiconductor systems |
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The theory of exciton states in quasi-zero-dimensional semiconductor systems |
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Інститут фізики напівпровідників імені В.Є. Лашкарьова НАН України |
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The theory of exciton states in quasi-zero-dimensional semiconductor systems / S.I. Pokutnyi // Semiconductor Physics Quantum Electronics & Optoelectronics. — 2006. — Т. 9, № 4. — С. 1-6. — Бібліогр.: 17 назв. — англ. |
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Semiconductor Physics, Quantum Electronics & Optoelectronics, 2006. V. 9, N 4. P. 1-6.
© 2006, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
1
PACS 71.35; 73.20; 73.40
The theory of exciton states
in quasi-zero-dimensional semiconductor systems
S.I. Pokutnyi
Illichivsk Institute of the Mechnikov Odessa National University,
17A, Danchenko str., Illichivsk, Odessa Reg., 68001 Ukraine
E-mail: Pokutnyi_Sergey@inbox.ru
Phone: +380(4868) 4-30-76; fax: +380(4868) 6-01-54
Abstract. For a semiconductor quantum dot (QD), the contributions made to the exciton
energy spectrum by the electron and hole kinetic energies, the energy of Coulomb
interaction between them, and the energy of their polarization interaction with the
spherical interface between the QD and the dielectric medium have been analyzed.
Keywords: exciton state, semiconductor quantum dot, exciton energy spectrum.
Manuscript received 10.04.06; accepted for publication 23.10.06.
1. Introduction
Optical properties of quasi-zero-dimensional semicon-
ductor structures, consisting of the semiconductor QDs
of the spherical shape with radii nm10...1≈a , grown in
transparent dielectric media have been intensively
studied recently [1-5]. Such heterostructures attract
attention owing to their nonlinear optical properties and
the prospects of their application in optoelectronics and
quantum electronics, in particular, as novel materials
perspective for the creation of elements which control
optical signals in semiconductor injection lasers [1, 2]
and in optical bistable elements and transistors [2].
Since the energy gap in a semiconductor QD is
essentially narrower than that in semiconductor
(dielectric) matrices, the motion of charge carriers is
confined to the QD volume in all three directions, i.e.,
charge carriers move in a three-dimensional spherical
potential well. As a result, both an electron and a hole as
well as an exciton have no quasi-momenta in a QD.
Therefore, it is possible to speak only about quasi-
particle states in a QD. Below, as regards to excitons in a
QD, we understand such an exciton state that has no
quasi-momentum.
Optical and electrooptical properties of similar
heterophase systems are determined to a great extent by
the energy spectrum of a spatially-bounded electron-hole
pair (the exciton) [1-5]. The energy spectrum of the
charge carriers in a QD will be completely discrete for
the QD dimension a smaller than that of the order of the
Bohr radii of an electron ea and a hole ha [6-8]. Under
these conditions, the influence of the interface between
the QD and the dielectric matrix can cause the
dimensional quantization of the electron and hole energy
spectra in the QD, which is related to both the mere
spatial confinement of a quantization region [4, 5, 9] and
the polarization interaction of charge carriers with the
QD surface [3, 6-14].
The theory of exciton states in quasi-zero-
dimensional structures has not yet been sufficiently
developed so far. To fill this gap, the contributions to the
exciton energy spectrum, made by the electron and hole
kinetic energies and the Coulomb interaction energies
between them, as well as the energy of their polarization
interaction with the spherical interface between the QD
and the dielectric medium, have been analyzed in this
paper. In addition, the limit transition from the energy
spectrum of the exciton in the QD to that of the exciton
in the unlimited bulk has been traced.
The exciton, the structure (the effective mass, Bohr
radius, and bond energy) of which in the QD does not
differ from that in an infinite semiconductor, will be
called as the "bulk" exciton.
2. Exciton energy spectrum in a quasi-zero-
dimensional system
Following papers [3, 6-14], let us consider a simple
model of the quasi-zero-dimensional system: a neutral
spherical semiconductor QD of the radius a and
dielectric permittivity (DP) 2ε imbedded into a
dielectric matrix with DP 1ε . In the bulk of such a QD,
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2006. V. 9, N 4. P. 1-6.
© 2006, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
2
moving are an electron e and a hole h with effective
masses em and hm , respectively. The variables er and
hr denote the distances of the electron and the hole,
respectively, from the center of the QD. The electron
and hole bands are supposed parabolic. The typical
dimensions of the problem are the quantities a, ea , ha ,
and exa , where
( )22
2 / ema ee hε= , ( )22
2 / ema hh hε= ,
( )22
2ex / ea με h= (1)
are the Bohr radii of the electron, hole, and exciton,
respectively, in an infinite semiconductor with DP ε2; e
is the electron charge; and ( )( )hehe mmmm += /μ is
the reduced effective mass of the exciton. The
circumstance that all the typical dimensions of the
problem are considerably larger than the interatomic
distance a0:
a , ea , ha , 0ex aa >> , (2)
allows us to consider the motions of the electron and the
hole in the QD in the effective mass approximation.
In the model concerned, the Hamiltonian of the
exciton in the QD, in the framework of the
approximations stated above, looks like [10-14]
( ) ( ),,,,
22
22
arrUrrVE
mm
H
heheehg
h
h
e
e
+++
+Δ−Δ−=
hh
(3)
where the first two terms define the kinetic energies of
the electron and the hole, and gE is the energy gap
width in an unconfmed semiconductor with DP 2ε . In
Eq. (3), the energy of the electron-hole Coulomb
interaction ( )heeh rrV , is defined as
( )
eh
heeh rr
errV
−
−=
2
2
,
ε
(4)
Provided that 21 εε >> , the polarization interaction
energy ( )arrU he ,, in Eq. (3) can be written down as an
algebraic sum of the energies of the hole and electron
interactions with their own images, ( )arV hhh ,′ and
( )arV eee ,′ , respectively, and with the images of
“foreign” quasi-particle ( )arrV hehe ,, rr
′ = ( )arrV heeh ,, rr
′
[10-14]:
( ) ( ) ( )
( ) ( ),,,,,
,,,,
arrVarrV
arVarVarrU
heehhehe
eeehhhhe
rrrr
rr
′′
′′
++
++=
(5)
where
( ) ⎟
⎟
⎠
⎞
⎜
⎜
⎝
⎛
+
−
=′
1
2
22
2
2
2
2
,
ε
ε
ε h
hhh ra
a
a
earV , (6)
( ) ⎟⎟
⎠
⎞
⎜⎜
⎝
⎛
+
−
=′
1
2
22
2
2
2
2
,
ε
ε
ε e
eee ra
a
a
earV , (7)
( )[ ] 2
1
222
2
cos2/2 arrarr
a
a
eVV
hehe
ehhe
+Θ−
⋅−== ′′ ε
,
he rr rr ,∠=Θ . (8)
Although, in our model of the quasi-zero-
dimensional system, the electron and the hole do not go
beyond the space of the semiconductor QD, the potential
energy of their interaction with the spherical interface of
two media ( )arrU he ,, (5) depends not only on the DP
2ε of the QD, but also on the DP 1ε of the matrix, into
which the QD is imbedded [3, 10-14]. Such a
dependence is connected to the penetration of the
electrostatic field created by the electron and the hole
beyond the boundaries of the QD.
In our papers [10-14], when considering
Hamiltonian (3) of the exciton in the QD, the
polarization interaction (5) of charge carriers with the
surface charge induced by them at the spherical interface
"QD-dielectric matrix" was taken into account for the
first time. Later on, such a polarization interaction was
taken into account when calculating the exciton [3, 10]
and biexciton [9] energy spectra in the QD.
On the basis of papers [10-14], we will obtain the
energy spectrum of an exciton in a QD making use of
the approximation, where the QD is an infinitely deep
spherical potential well for an electron and a hole that
move inside its space. The radius a of the QD is taken as
confined within the limits
exaaaa eh ≈≤<< . (9)
Then, the polarization interaction (5) plays a
dominating role in the potential energy of Hamiltonian
(3). Provided that condition (9) holds true, we use the
adiabatic approximation, supposing the kinetic energy of
an electron to have the largest value and considering the
last two terms in Hamiltonian (3), as well as the operator
of nonadiabaticity, in the framework of the perturbation
theory.
Confining ourselves to the first order of the
perturbation theory, we obtain the following expression
for the exciton energy spectrum ( )SE hhh
eee
mln
mln
0,,
0,0,
=
== in the
state ( )0,,;0,0, === hhheee mlnmln in the QD
with the radius S [3, 10-14]:
( ) ( ) ( ) ( )SSVSTESE hh
eelen
hh
e
ln
nee
e
g
ln
n
0,,
0,0,
0,,
0,0, 0,
λ+++= ′=
,
(10)
where
( )ST e
ne 0, ( ) 2
22
0,
π
S
n
SE ee
ne
== (11)
is the kinetic energy of the electron in the infinitely deep
spherical well, ( )SV ee ′ is the average value of the
interaction energy of the electron with its own image
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2006. V. 9, N 4. P. 1-6.
© 2006, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
3
calculated using the wave functions of the electron in the
infinitely deep spherical well of the QD,
( ) ( ) ⎟
⎠
⎞
⎜
⎝
⎛ ++=
2
3,0,
0,0, he
nt
n tnS
S
P
S eh
e
ωλ (12)
is the oscillator-type hole spectrum,
( ) ( )( )
( ) ( )( ),0,0,0,0,
0,0,0,
SVSV
SVSV
S
P
ee
ee
n
eh
n
he
n
ehhh
n
′′
′
++
+
′
+=
(13)
( ) 2/3
2/12/1
22π
3
212, −
⎟⎟
⎠
⎞
⎜⎜
⎝
⎛
⎟
⎠
⎞
⎜
⎝
⎛ += S
m
m
nnS
h
e
eeω (14)
is the frequency of oscillations of the hole,
K,2,1,02 =+= hrh lnt
h
is the main quantum number
of the hole, and K,2,1,0=
hrn is the radial quantum
numbers of the hole. Provided that the hole energy
spectrum ( )Sh
e
t
n 0,0,λ (12) can be described by the
spectrum of a three-dimensional harmonic oscillator, the
requirement
2/1
22
2/1
2/1
π
3
21
2/3
⎟
⎠
⎞
⎜
⎝
⎛ +
+
⎟⎟
⎠
⎞
⎜⎜
⎝
⎛
>>
e
h
h
e
n
t
m
m
S (15)
must be fulfilled [10-14].
Let us write down the expressions for the average
values of the energy of the electron interaction with its
own image [10-14]
( )
S
Z
SV ee nn
ee
0,0,0, =′ ,
( )
⎟
⎟
⎠
⎞
⎜
⎜
⎝
⎛
−
+= ∫
1
0
2
2
1
2
0,
1
πsin
2
x
xndx
Z e
ne ε
ε
, (16)
the energy of the hole interaction with its own image
( ) ( )
S
SV hh
12 /1 εε+
=′ , (17)
the energies of the electron and hole interactions with
the images of "foreign" quasi-particle
( ) ( )
S
SVSV ee n
eh
n
he
20,0,0,0, −=+ ′′ , (18)
and the electron-hole Coulomb interaction energy
( )( ) ( ) ( )[ ]ee
n
eh nn
S
SV e π2Ciπ2ln20,0, −+−=
′
γ ,
( ) ( )( ) ( )
( ) ( )[ ] ( ) ,
2
3,π2Ciπ2ln2
2
3,
~ 0,0,;0,0,
⎟
⎠
⎞
⎜
⎝
⎛ ++−+−=
=⎟
⎠
⎞
⎜
⎝
⎛ ++
′
=
heee
he
n
eh
tn
eh
tnSnn
S
tnSSVSV ehe
ωγ
ω
(19)
where ( )γCi is the cosine-integral function,
K577.0=γ is the Euler constant.
It should be noted that the formulae (12)-(19) were
obtained by averaging the corresponding expressions
(4), (6)-(8) using the wave functions of the infinitely
deep spherical well of a QD [3, 10-14].
The polarization interaction energy (5), averaged
using the electron wave functions in the infinitely deep
spherical well, looks like
( ) ( ) ( )
( ) ( )( )=++
++=
′′
′′
SVSV
SVSVSU
ee
ee
n
eh
n
he
n
eehh
n
0,0,0,0,
0,0,0,0,
pol
.
1)/( 120,
S
Z
en −+
=
εε
(20)
Hereafter, the energy is measured in terms of
( )22 2/Ry eee amh= , and the dimensionless variables
( )arx h /= and ( )eaaS /= are used.
Taking into account Eqs (12), (13) and (19), (20),
we write down the expression (10) for the exciton
spectrum ( )SE h
e
t
n 0,0, in the state ( )he tn ;0,0, in the
QDs, the radii S of which satisfy conditions (9) and (15)
simultaneously, as follows:
( ) ( )
( )
( )
( )
( )
.
~
1
0,
;0,0,
0,
0,0,
pol
0,0,0,
⎥
⎥
⎥
⎦
⎤
⎢
⎢
⎢
⎣
⎡
−+×
×+=
ST
SV
ST
SU
STESE
e
n
tn
eh
e
n
n
e
ng
t
n
e
he
e
e
e
h
e
(21)
It should be pointed out that the exciton spectrum
(21) was obtained in the framework of the adiabatic
approximation, where the kinetic energy of the electron
( )ST e
ne 0, (11) was supposed to give the main
contribution to the energy spectrum of the exciton in the
QD. Therefore, formula (21) for the exciton energy
spectrum ( )SE h
e
t
n 0,0, allows one to trace the
contributions, given to the exciton spectrum by the
electron-hole Coulomb interaction (19) and the
polarization interaction (20) and to compare them with
the contribution of the electron kinetic energy (11).
The obtained exciton spectrum (21) can be applied
only to weakly excited exciton states ( )he tn ;0,0, , for
which the inequality
( ) ( )SVESE g
t
n
h
e
Δ<<−0,0, ,
where ( )SVΔ is the depth of the potential well for
electrons in the QD holds true (for example, in a CdS
QD with dimensions obeying condition (9), the value of
VΔ is eV5.2...3.2 [15]).
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2006. V. 9, N 4. P. 1-6.
© 2006, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
4
In [14], the spectrum of an exciton in a QD of the
radius a for a simple model of the quasi-zero-
dimensional system, where the Hamiltonian of the
exciton H is given by the formula (3), was found using
the variational method and not being restricted to the
framework of the adiabatic approximation. Moreover,
the radius a of the QD, contrary to [3, 10-14], was not
bounded by condition (9). The results of variational
calculations of the energy spectrum for the exciton
( )aE0 in the QD of the radius a are shown in the figure.
The relevant calculation parameters in the work [14]
corresponded to experimental conditions in the
works [4, 5, 15, 16].
3. Contributions of kinetic, polarization, and
Coulomb energies to the spectra of excitons
in quantum dots
In papers [4, 16], the peaks of interband absorption in
spherical QDs with the radius a within the interval of
nm30...2.1 , which were made of CdS with DP 3.92 =ε
and dispersed in a transparent matrix of silicate glass
with DP 25.21 =ε [4], were observed. The effective
masses of the electron and hole and the reduced mass of
the exciton μ in CdS were ( ) 205.0/ 0 =mme ,
( ) 5/ 0 =mmh , and ( ) 197.0/ 0 =mμ , respectively [16].
In particular, the dependence of the positions of the
adsorption band of QDs caused by interband transitions
onto the dimensional quantization levels
( )0,1 == ee ln , ( )1,1 == ee ln , and ( )2,1 == ee ln of
the electron in the conduction band on the QD radius a
was experimentally determined [4, 16].
As was shown in [3, 10-14], the formula (21)
describes the exciton spectrum ( )SE ht
0,0,1 (5) as a
function of the QD radius S with sufficient accuracy
under the reported conditions of experiments in the CdS
[4, 16]. The parameters of the exciton spectrum
( )SE ht
0,0,1 (21) under the experimental conditions [4,
16] for the CdS QDs with the radius nm0.3...5.1=a are
listed in Table 1.
According to the formulae (11), (19), and (20), the
ratios between the polarization interaction energy and
electron kinetic energy ( ) ( )( )STSU e
0,1
0,0,1
pol / as well as
between the Coulomb interaction energy and electron
kinetic energy ( ) ( )⎟
⎠
⎞⎜
⎝
⎛ STSV e
eh 0,1
0,0,1 /
~
are proportional to
S and 2/1S , respectively. Such a behavior of the ratios
( ) ( )( )STSU e
0,1pol / (20) and ( ) ( )⎟
⎠
⎞⎜
⎝
⎛ STSV eth
0,1
;0,0,1 /
~
(19) is also confirmed by numerical data in Table 1.
From Table 1, it follows that the polarization
interaction energy ( )SU 1,0,0
pol (20) makes the dominating
contribution to the exciton energy spectrum (21),
whereas the Coulomb interaction energy ( )SV ht
eh
;0,0,1~
(19) makes a small negative one. Namely, the ratio
( ) ( )( )STSU e
0,1
1,0,0
pol / varies from 55.8 % at nm5.1=a
to 112 % at nm3=a , whereas the absolute value of the
ratio ( ) ( )⎟
⎠
⎞⎜
⎝
⎛ STSV et
eh
h
0,1
;0,0,1 /
~
from 8.5 % at nm5.1=a
to 30 % at nm3=a . The data presented in Table 1 are
also confirmed by the results of variational calculations
of the spectrum E0(a) of the exciton in the QD of the
radius ex3aa ≤ , which were obtained in the work [14]
under the experimental conditions of the works [4, 16]
and beyond the adiabatic approximation.
The main contributions to the polarization
interaction energy ( )SU 0,0,1
pol (20) are made by the
interaction energies of the electron ( )SV ee
0,0,1
′ (16)
(64.5 %) and the hole ( )SV hh
0,0,1
′ (17) (58.2 %) with their
own images, whereas the interaction energy of the
electron and hole with the images of "others"
( ) ( )( )SVSV ehhe
0,0,10,0,1
′′ + (18) gives a negative
contribution, the absolute value of which is 22.7 % (see
Table 2). It is essential that those contributions do not
depend on the QD radius S .
Table 1. Contributions to the exciton spectrum ( )aE ht
0,0,1
(10) and (21) made by the electron-hole Coulomb,
( )aV ht
eh
;0,0,1~
(19), and polarization, ( )aU 1,0,0
pol (20),
interaction energies in relation to the contribution of the
electron kinetic energy ( )aT e
0,1 (11).
( )
( )S
a nm ( )
( )e
e ST
Ry
0,1
ht
( )
( )
( )%
~
0,1
;0,0,1
ST
SV
e
t
eh
h
( )
( )
( )%
0,1
1,0,0
pol
ST
SU
e ( )[
]( )eg
t
E
SE h
Ry
0,0,1
−
−
0 17.4 55.8 35.08 1.5
(0.624) 25.35
1 8.5 37.34
0 25.6 74..4 21.21 2.0
(0.83) 14.26
1 15.3 22.68
0 34.0 93.0 14.51 2.5
(1.04) 9.13
1 22.5 15.56
0 42.6 111.5 10.71 3.0
(1.25) 6.34
1 30.0 11.51
Note. The ratio ( ) ( )aTaV et
eh
h
0,1
;0,0,1 /
~
is negative. The data are
listed for the CdS QDs with the radii ( ) nm0.3...5.1=a under
the conditions of experiments in [4, 16]. eV1068.7Ry 1−⋅=e .
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2006. V. 9, N 4. P. 1-6.
© 2006, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
5
Table 2. Contributions to the polarization interaction energy ( )aU 1,0,0
pol (20) made by the interaction of the electron with
its own image, ( )aV ee
0,0,1
′ (16), by the interaction of the hole with its own image, ( )aV hh
0,0,1
′ (17), and by the interactions of
the electron and the hole with the hole and electron images, respectively, ( ) ( )aVaV ehhe
0,0,10,0,1
′′ + (18), as well as the ratio
( ) ( )aUaV ht
eh
0,0,1
pol
;0,0,1 /
~
between the Coulomb and polarization interaction energies (19) and (20).
( )
( )S
a nm
( )
( )e
SU
Ry
1,0,0
pol
( )
( )
( )%
1,0,0
pol
0,0,1
SU
SV ee ′
( )
( )
( )%
1,0,0
pol
0,0,1
SU
SV hh ′
( ) ( )
( )
( )%
0,0,1
pol
0,0,10,0,1
SU
SVSV ehhe ′′ +
ht
( )
( )
( )%
~
1,0,0
pol
;0,0,1
SU
SV ht
eh
0 31.2 1.5
(0.624) 14.14 64.5 58.2 22.7
1 15.2
0 34.4 2.0
(0.83) 10.61 64.5 58.2 22.7
1 20.5
0 36.6 2.5
(1.04) 8.49 64.5 58.2 22.7 1 24.2
0 38.2 3.0
(1.25) 7.07 64.5 58.2 22.7 1 26.9
Note. The ratios ( ) ( )( ) ( )( )SUSVSV ehhe
1,0,0
pol
0,0,10,0,1 /′′ + and ( ) ( )⎟
⎠
⎞⎜
⎝
⎛ SUSV ht
eh
1,0,0
pol
;0,0,1 /
~
are negative. The data are listed for the CdS QDs
with radii nm0.3...5.1=a under the conditions of experiments in [4, 16].
The Coulomb interaction energy ( )SV ht
eh
;0,0,1~
(19)
makes a considerably smaller contribution to the excilon
spectrum (10) and (21) in comparison with the
polarisation interaction energy ( )SU 0,0,1
pol (20). The ratio
of these energies ( ( ) ( ))SUSV ht
eh
1,0,0
pol
;0,0,1 /
~
becomes
negative (its absolute value changes from 31 and 15 % at
nm5.1=a to 38 and 27 % at nm3=a for 0=ht and
1, respectively (see Table 2).
The experimental exciton spectrum was stated in
papers [4, 16] to be described with sufficient accuracy by
the kinetic energy of the electron in the QD ( )aT e
0,1 (11) as
the radius a of the CdS QD increases above 2.0 nm.
Actually, as follows from Table 1, the ratio
( ) ( ) ( )⎟
⎠
⎞
⎜
⎝
⎛ + STSVSU et
eh
h
0,1
;0,0,11,0,0
pol /
~
of the sum of the
polarization and Coulomb interaction energies to the kinetic
energy of the electron comprises a significant value of
(0.49–0.69). Even for the QD with the smallest experi-
mentally allowable radius a = 1.5 nm, such a ratio amounts
to a substantial value of about 38 % (see the figure).
4. Emergence of the bulk exciton
in a quasi-zero-dimensional system
For the QD with a small radius exaa << , the main
contribution to the exciton spectrum (21) is given by the
electron kinetic energy ( )ST e
ln ee , (11), whereas the
contributions of the terms ( )SU en 0,0,
pol (5) and
( )SV he tn
eh
;0,0,~
are small [7-14]:
( ) ( ) 1/ ,
,0,0n
pol
e <<STSU e
ln ee
,
( ) ( ) 1/
~
,
;0,0, <<STSV e
ln
tn
eh ee
he .
The exciton energy spectra ( )SE 0
0,0,1 as functions of the
nanocrystal dimension S = a/aex: 1 – the experimental exciton
spectrum [4, 16], 2 – the exciton spectrum ( )aE0 obtained by
the variational method [14], 3 – the kinetic energy of the
electron ( )ST e
0,1 (11).
Semiconductor Physics, Quantum Electronics & Optoelectronics, 2006. V. 9, N 4. P. 1-6.
© 2006, V. Lashkaryov Institute of Semiconductor Physics, National Academy of Sciences of Ukraine
6
For the QD with a large radius exaa >> , the
exciton is quantized as a whole, and its energy spectrum
is determined as [9]
( ) 2
2
2
ex 2 nlgnl aM
ΕΕaΕ ϕh
+−= ,
exE = 2
ex
2
ex μ2
Ry
a
h
−=− , (22)
where M is the translational mass of the exciton, and
nlϕ are the roots of the Bessel function ( )ϕ
2
1
+l
J .
In paper [17], an expression for the exciton
spectrum was obtained by the variational method in the
framework of the effective mass approximation but
without regard for the polarization interaction energies
of an electron and a hole with the surface of the QD,
which made it possible to trace the limit transition to the
spectrum of the bulk exciton (22), starting from the QD
radius 80
exex ≥> SS .
The spectrum of the exciton in the CdS QD, which
was found by us in the paper [14] by the variational
method in the framework of the effective mass
approximation by taking into account the polarization
interaction energy, turns into the spectrum of the bulk
exciton (22) at 44.9~0
exex ≥> SS under the experimental
conditions of the works [4, 5, 16]. In this case, the value
of 0
ex
~S differs from that of 0
exS by no more than 18 %.
Such a difference is connected to the fact that the account
of the polarization interaction energy (it has not been done
in the paper [4]) results in the exciton energy growth
proportional to 1−S . In addition, the values of the QD
radii 0
exS and 0
ex
~S , can be overestimated to a certain
extent, because the variational calculations of the exciton
spectrum yield the overestimated values of the energy.
5. Conclusions
Here, in the framework of the simple model of a quasi-
zero-dimensional system, we have shown that, even for
the QDs with the smallest experimentally allowable
radii, the kinetic energy of the electron (11) makes a
contribution to the exciton spectrum ( )aE h
e
t
n 0,0, (10)
and (21) that is comparable by the order of magnitude
with the contributions made to this spectrum by the
polarization, ( )aU ,0,0n
pol
e (20), and Coulomb,
( )aV he tn
eh
,0,0,~
(19), interaction energies. In this
connection, a description of the exciton spectrum in QDs
with radii exaa < using only the expression for the
electron kinetic energy ( )aT e
nl (11), as it has been done
in works [4, 5, 16], is not justified.
In the least studied case where the QD radius a is
comparable by its value with the Bohr radius of the
exciton, we showed [10-14] that the exciton spectrum
( )aE h
e
t
n 0,0, (10) and (21) can be described by the
complicated dependence
( )aE h
e
t
n 0,0, = ( )1122/31 ,,,, −−−−−
he mmaaaf
(see the figure). In this case, the effective masses of the
electron em and the exciton μ are the functions of the
QD radius a [12-14].
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