Journal of Physics: Condensed Matter

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Effect of quantum confinement on lifetime of anharmonic decay of optical

phonons in semiconductor nanostructures
To cite this article before publication: Debopam Datta et al 2018 J. Phys.: Condens. Matter in press https://doi.org/10.1088/1361-648X/aad104

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Page 1 of 10 AUTHOR SUBMITTED MANUSCRIPT - JPCM-111418.R1

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8

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9 Effect of quantum confinement on lifetime of anharmonic decay
10
11 of optical phonons in semiconductor nanostructures
12
13

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14
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16
D Datta1,4, K Krishnababu1,4,5, M A Stroscio1,2,3 and M Dutta1,3
1
17 University of Illinois at Chicago Department of Electrical and Computer Engineering
2
18 University of Illinois at Chicago Department of Bioengineering
3
19 University of Illinois at Chicago Department of Physics
20 E-mail: D Datta (ddatta2@uic.edu) and M A Stroscio (stroscio@uic.edu)

us
21
22 Abstract. The anharmonic decay of phonons underlies many important effects in semiconductor, e.g.,
23 hotspot formation, phonon bottleneck and thermal resistivity. In this article, we evaluate the effect of
24 quantum confinement on the anharmonic decay transition probability in a cubic isotropic material. This
25 article mainly focuses on the anharmonic decay of longitudinal optical phonons, generated from hot
electrons, are directly related to formation of hotspots in the active region of semiconductor devices. The
26
27
28
29
an
confinement effect has been realized in double interface heterostructure quantum well (DHSQW) (e.g.,
AlAs/GaAs/AlAs) and free-standing quantum well (FSQW) (e.g., GaAs) structures as the confined
phonon modes have different properties inside the structures. The LO phonon decay rate is reduced for
the case of a DHSQW compared to bulk material and for a FSQW the decay rate has a strong dependence
30 on wavevector value of the three phonons involved.
31
32
dM
Keyword: Anharmonic decay rate, confined optical phonon, confined acoustic phonon, double
33
interface heterostructure quantum well, free standing quantum well
34
35
36
37
38
39 1. Introduction
40 With advent of fabrication technology- as the devices are shrinking- phonons are emerging as one of the
41 key elements that control device performance. Both optical and acoustic phonons have pervasive importance
42 in carrier transport and energy dissipation in modern electronic devices [1]. For last three decades, GaAs, AlAs
43
pte

and their alloy compounds have been used extensively as the active material in high electron mobility
44 transistors [2], monolithic microwave integrated circuits due to high electron mobility of the order of
45 𝑐𝑚2
46
20 × 107 𝑉−𝑆 [3] in GaAs and in multi-junction solar cells, photoconductive sources, and laser sources due to
47 its direct bandgap at 1.42 eV. These materials have also found applications in future quantum information
48 processing devices via coherent manipulation of spins of double AlGaAs/GaAs double quantum dots [4,5].
49 Electron spin-phonon interaction [6] plays an important role in determining the electrical or optical properties
50 of these quantum devices. On the other hand, high frequency and high-speed operation of traditional electronic
51
ce

and optoelectronic devices results in hot electrons which produce a lot of hot LO phonons which eventually
52 decay into lower energy acoustic phonon to facilitate heat conduction, hence the study of the later phonon-
53 phonon interactions or LO phonon decay leads to a proper understanding of the device dynamics.
54
55 The decay lifetime of LO phonons in bulk GaAs has been evaluated extensively theoretically and
56 experimentally [7-10] unlike the case for nanostructured GaAs. In principle, the cubic anharmonicity of the
Ac

57 harmonic oscillator energy the phonon modes lead to phonon decay and interaction with other phonons.
58
59
60 4
These authors have equal contribution to the work.
5
Current address: Apple Inc., 320 S. Capital of Texas Highway, Building A, Austin, Texas 78746.
 AUTHOR SUBMITTED MANUSCRIPT - JPCM-111418.R1 Page 2 of 10

Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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Employing regular perturbation theory, Klemens demonstrated decay of zone center longitudinal optical
4 phonons in bulk GaAs where it decays into two longitudinal acoustic phonons with the same energies but
5 opposite momentum [7]. Like Klemens channel, optical phonons in bulk GaAs can also decay in a transverse
6 acoustic phonon and Brillouin zone edge optical phonon according to the experimental work of Valley and
7 Bogani (VB) [10]. Barman et al. have shown that in zincblende GaAs [8], VB channel plays a significant role
8 in optical phonon decay. Other decay channels are of important in other materials systems. For example, in

pt
9 the GaN the LO and LA branches are separated by more than twice the LA energies, so that the Klemens
10 channel is not operative but the Ridley channel takes on key importance [11]. However, both processes being
11 N-processes, the crystal momentum and phonon energy remain conserved. Though decay process of the
12 optical phonons has been evaluated theoretically and experimentally to understand various material properties,
13 very few efforts have been directed towards understanding the modification of these processes due to spatial

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14 confinement of test device structure.
15
16 For last two decades, the effect of dimensional confinement on electron and phonon transport have been
17 comprehensively estimated [12-15]. During this period, the focus of the phonon research community was on
18 anharmonic decay of phonons in bulk structures specifically, only Li et al. [16] evaluated the lifetime of LO
19
phonon in GaAs quantum dots and Dyson et al. in GaN heterostructure [17]. Only recently researchers have
20

us
started to investigate the lifetime and dynamics of anharmonic decay of acoustic phonons in other acoustic
21
22
phonons in confined structures [18,19] to evaluate the heat transport in materials like Si and Ge, important for
23 thermoelectric applications. To the best of our knowledge none of the prior efforts has been directed towards
24 the investigation of the effect of phonon confinement on anharmonic decay of optical phonons in GaAs, which
25 has been considered in this work. The continuum phonon formulation used in this article for GaAs can be
26 extended to isotropic materials with cubic crystal symmetry.
27
28
29
an
In this article, we have considered the effect of both optical phonon and acoustic phonon confinement on
the anharmonic decay rate of the confined optical phonons through Klemens channel and Valle-Bogani
30 channel using the three-phonon interaction Hamiltonian and employed the Fermi golden rule to evaluate the
31 transition probability (TP). The effect of confinement on the TP value has been evaluated in comparison to
32 the bulk case through the calculation of interaction matrix (IM) squared. The first section of the article
dM
33 summarizes the transition probability expression for the bulk case. Thereafter, this paper presents an
34 evaluation of the expression for the relative displacement for a confined optical phonon and the TP has been
35 evaluated for AlAs- and GaAs- based double interface heterostructure quantum well (DHSQW) where
36 acoustic phonons are not confined. The penultimate section, sheds some light on specialized cases where
37 acoustic phonons are also confined in a GaAs free-standing quantum well (FSQW) structure. The average IM
38 squared values in the article are marked as following:
39
40
Table 1. Different notation for IM related to different decay process in DHSQW and FSQW
41
42
decay process mentioned volume average IM notation
43
pte

Decay of LO phonon in bulk system

44 MB,K , MB,VB
45 (K= Klemen’s channel; VB= Vallee-Bogani Channel)
46 Klemens type decay in DHSQW MCD
47 Vallee - Bogani type decay in FSQW
MCF,VB,1 , MCF,VB,2
48 (cases 1 and 2 = asymmetric and symmetric CAP*)
49 Klemens type decay in FSQW
50 (cases 1, 2, and 3= 2 dilatational type CAP, 2 flexural type CAP, and MCF,K,1 , MCF,K,2 , MCF,K,3
51
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1dilatational and 1 flexural type CAP)

52 *
CAP: Confined Acoustic phonon
53
54
2. Continuum theory of three-phonon process
55
56 The interaction Hamiltonian within the continuum approximation for three phonon processes can be written
as [9]
Ac

57
58 1
H3 = P(k, j; k ′ , j′ ; k ′′ , j′′ ) uk,j uk′ ,j′ uk′′ ,j′′ (1)
59 3! √N
60 where 𝑘, 𝑘 ′ , 𝑘 ′′ are the three phonon wave vectors involved in the annihilation or creation process, 𝑗, 𝑗 ′ , 𝑗 ′′ are
the polarizations of the three phonons and N is the number of unit cells present. P describes the cubic
Page 3 of 10 AUTHOR SUBMITTED MANUSCRIPT - JPCM-111418.R1

Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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(anharmonic) coupling and 𝑢𝑘,𝑗 signifies the displacement field associated with the annihilated or emitted
4 phonons. The phonon displacement in normal coordinates can be represented as:
1
5
h̅ 2
⃗ ⃗
6 uk,j =( ) e′k,j (ak,j eikr⃗ + a†k,j e−ik⃗r ) (2a)
7 2mωk,j
8 1
1 h̅ 2 1

pt
9 ⃗ † −ik ⃗ r⃗ ∗
𝑢(r) = ∑ ∑ ( ) (ak,j eik⃗r ê
k,j + a k,j e ê
k,j ) = ∑ ∑ ⃗⃗⃗⃗⃗⃗uk,j (2b)
10 √N k j=1,2,3 2mωq,j √N k j=1,2,3
11 † ′
12 where 𝑎𝑘,𝑗 , 𝑎𝑘,𝑗 denotes the annihilation and creation operator, respectively, 𝑒𝑘,𝑗 is the polarization vector, m
13 is the reduced mass of the lattice atoms and 𝜔𝑘,𝑗 is the frequency of the normal mode [22]. Substituting the

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14 normalized displacement expression in (1) the three-phonon anharmonic interaction term for type 2 phonon
15 interaction where one phonon decays into two phonons can be written as:
16 3 1
17 1 1 h̅ 2 1 2
† † ∗ ∗
18 H3 = ∫ d3 r ( ) ( ) P (ak,j ak′ ,j′ ak′′ ,j′′ ) (ê
k,j . e
̂ k′ ,j′ . ê
k′′ ,j′′ ) exp(i(k − k
′
(3)
V √N 2m ωk,j ωk′ ,j′ ωk′′ ,j′′
19 ′′ ).
− k r)
20
where 𝑉 is the volume of the structure under consideration. Assumption of linear dispersion of the acoustic

us
21
22
phonons enforces the polarization vectors to vanish if the longitudinal optical phonon decays into two
23 longitudinal acoustic phonons are considered. The TP for any quantum processes can be calculated using
24 Fermi golden rule and given by:
25 2π
Γ= |⟨nk − 1, nk′ , nk′′ |H3 |nk , nk′ + 1, nk′′ + 1⟩|2 δ(h̅(ωk − ωk′ − ωk′′ )) (4)
26 h̅
27
28 expressed as:
3
an
The average value of IM, |⟨𝑖|𝑉3|𝑓⟩| for above mentioned type 2 decay (LO->LA+LA) in the (4) can be

29
2 2
1 h̅ 1
30 |MB | = |⟨i|H3 |f⟩| = ( ) ( ) P2 nk (nk′ + 1)(nk′′ + 1)δk−k′ −k′′ ,G (5)
31
N 2m ωk ωk′ ωk′′
̅𝜔 −1
32 ℎ
where 𝑛𝑘 = (exp ( 𝑘 𝑇𝑘 ) − 1) is the Bose-Einstein occupation number, 𝐺 is the reciprocal lattice vector and
dM
33 𝐵
𝑖 𝑀
34 P is the anharmonic coupling constant given by 𝑃 = − 𝛾𝜔𝑘 𝜔𝑘′ 𝜔𝑘′′ where M = atomic mass, 𝑣 sound
√3 𝑣
35
velocity (longitudinal) and 𝛾 is the Gruneisen constant [20]. The average value of IM squared |𝑀|2 for the
36
phonon interaction mentioned in (5) contains the delta function due to the integration of the Hamiltonian in
37
the whole volume as:
38
1
39 ∫ d3 r exp(i. (k − k ′ − k ′′ ). r) = δk−k′ −k′′ (6)
40 V
41 Eq. 5 can be further simplified under the assumption that ωk = k ∗ ck, i.e. linear dispersion of acoustic waves
42 elaborately discussed in Ref. 20. The average value arises from integration of the exponential term within the
43 whole volume which produces the δ function with a subscript denoting whether the process is an N-process
pte

44 or U-process, determined by G value. Using this isotropic formulation, Klemens et al. [7], Bhatt et al. [9],
45 Srivastava et al. [8] have theoretically calculated the anharmonic lifetime of LO phonons in bulk GaAs slabs
46 to be of 3.5 ps [7-9] at room temperature which has been experimentally verified with 2.2 ± 0.2 ps value [21]
47 using Raman spectroscopy.
48
49 3. Effect of confinement on phonon decay process
50
The effect of phonon confinement on anharmonic phonon decay is evaluated in two different nanostructure
51
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assemblies. The AlAs/GaAs/AlAs DHSQW is the first test structure considered where optical phonon modes
52
53
in GaAs are confined due to difference in dielectric property between the two materials but acoustic phonons
54 behave as continuum elastic modes as the two materials have almost similar elastic properties. Whereas in
55 second test structure of GaAs FSQW, the acoustic modes are confined because acoustic modes only lie within
56 the QW structure and the stress field is zero at the boundary/interface. The anharmonic coupling constant P
Ac

57 discussed in Section I. depends on three main scattering processes [20], a lattice wave can undergo scattering
58 from a point imperfection, single dislocation and grain boundaries. Due to dimensional confinement surface
59 effects become prominent, external boundary scattering of phonons increases but as for anharmonic decay of
60 confined phonons we have assumed that the anharmonic coupling coefficient does not change compared to
bulk case. A similar assumption has also been employed in Ref. 16 for the case of a quantum dot.
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Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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4 3.1. Mode pattern of confined phonons in DHSQW and FSQW structure
5 3.1.1. Mode pattern of confined optical phonons. The confinement of optical phonon arises in both DHSQW
6 and FSQW as the constituent materials have dissimilar dielectric function which in turn depends on the zone
7 center optical phonon frequency. Consideration of previously-mentioned heterostructure with dissimilar
8 dielectric properties produces two main types of phonon modes, namely: a) confined modes (bounded within

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9 the well structure) hence the phonon potential should go to zero at the two interfaces, b) Interface mode
10 (localized along the interface) i.e. the potential follows a decaying profile inside the well. Under the dielectric
11 continuum (DC) model assumption, both modes are necessary to represent the optical modes within the
12 structure. Following the DC model, the potential term for optical-phonon modes in a confined polar material
13 structure can be written as:

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14
15 2 cos(k z z)
φ(qII , z) = √ { } exp(±ik II ρ) (7)
16 Adz sin(k z z)
17
18 where 𝑘𝑧 = 𝑛𝜋/𝑑𝑧 ; 𝑑𝑧 is the thickness of the quantum well, A = Area of the quantum well and 𝑞II is the
19 wavevector parallel to the interfacial plane. The cos(𝑞𝑧 𝑧) term is obtained when n = odd and for n= even, the
20 displacement function assumes the sin(𝑞𝑧 𝑧) form in order to force the potential to zero at the interface. As

us
21 the material is assumed to be isotropic, the displacement pattern of the mode can also be written using Born-
22 Huang theory [22] as:
23 V √ε0 − ε∞
24 𝐮=√ ωTO 𝐄 and 𝐄 = −𝛁φ (8)
25 4πμN 2 2
√ωTO − ω
26
27
28
29 h̅ 2
1
cos(k z z)
an
Using Eq. 7 and 8 the displacement field for confined mode with normal coordinate is given as:

† cos(k z z) ∗ (9)
uk,j = ( ) (ak,j { } exp(ik II ρ)ê
q,j + a k,j { } exp(−ik II ρ)ê
q,j )
30 2mωk,j sin(k z z) sin(k z z)
31 The value of the constant for displacement is calculated using proper quantization condition given by
32 ̅
h
∫ u(k II , z) ∗ u∗ (k II , z)d3 r = 2mω [21] where m is based on the mass of the ions in the primitive cell.
dM
33
34
35 3.1.2. Acoustic phonon in DHSQW structure. Hard confinement of the acoustic modes inside a slab occurs in
36 presence of acoustically mismatched interfaces only. A huge difference is elastic constant causes extreme
37 confinement of acoustic modes, whereas materials with almost similar elastic constant like GaAs and AlAs
38 the interfaces behave as a continuous media hence confinement of acoustic modes is not obtained in this
39 specific structure. Hence, the DHSQW structure behaves as a continuous media for acoustic modes and the
40 mode displacements retain the bulk-type expression form given in Eq. (2).
41
42
3.1.3. Confined acoustic phonons in a FSQW structure. Unlike DHSQW structure discussed in the previous
43
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section, FSQW contains confined acoustic phonons rather than continuum acoustic phonons due to acoustic
44
45 property difference at the interface. Due to ‘hard’ confinement effect, the dispersion curves for the acoustic
46 phonons also changes from that of bulk modes. The localized acoustic modes in the slab for an isotropic
47 material using elastic continuum theory and appropriate boundary condition are of three main types: Shear
48 Mode, Dilatational Mode (Symmetric) and Flexural Mode (Anti-Symmetric) [24] which has also been
49 efficiently summarized by Stroscio and Dutta [23]. The mode shape for dilatational, flexural modes and shear
50 modes inside the slab is described in the table-II. The decaying mode shape or interface modes in the
51
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embedding material is not described because we are only considering the decay dynamics inside the quantum
52 well region.
53
54 Table 2. Displacement function of three types of confined acoustic modes
55
56 Mode Type Displacement envelope inside the slab
Ac

57 cos(k z,n z) , n = 0,2,4, . .

58 Shear (S) uS,y (z) = (10)
59 sin(k z,n z) , n = 1,3,5, …
60
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Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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2
3 k t dz k t dz
uD,x (z) = ik II [(k 2II − k 2t ) sin ( ) cos(k l z) + 2k l k t cos(k t z) sin ( )]
4 Dilatational/ 2 2
5 Symmetric (D) k t dz k t dz
6 uD,z (z) = k l [−(k 2II − k 2t )sin( ) sin(k l z) + 2k 2II sin(k t z) sin ( )]
2 2
7 k t dz k t dz
8 u F,x (z) = ik II [(k 2II − k 2t ) cos ( ) sin(k l z) + 2k l k t sin(k t z) cos ( )]
Flexural/Anti- 2 2

pt
9
Symmetric(F) k t dz k t dz
10 uF,z (z) = k l [(k 2II − k 2t ) cos ( ) cos(k l z) − 2k 2II cos(k t z) cos ( )]
11 2 2
ω 2 ω 2
12 where k l,n = (k ∥ 2 − n2 )1/2 and k t,n = (k ∥ 2 − n2 )1/2 with cl and ct are the longitudinal and transverse
cl ct
13

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14 sound velocity in the isotropic slab medium. The confined acoustic mode displacements are eigenfunctions
15 solution to a eigen-value equation, hence the modes are needed to be orthogonalized for an eigen frequency.
16 The orthogonalized mode displacements for Shear, Dilatational and Flexural modes are given by, wn,S =
17 FS uS,y, wn,D = FD (uD,x x̂ + uD,z ẑ), and wn,F = FS (uF,x x̂ + uF,z ẑ) respectively. The normalized mode
18 ∗
displacements follow the condition given by ∫ wn,i wm,i = δmn . Using the normalized modes, the quantized
19 ̅
h
20 shear, dilatational and flexural modes can be represented as √2mω (ak + a†k ) ∗ FS ∗ (uS,y 𝐲̂)exp(ik II ρ) ,

us
n
21
̅
h ̅
h
22 √
2mωn
(ak + a†k ) ∗ FD ∗ (uD,x 𝐱̂ + uD,z 𝐳̂)exp(ik II ρ) and √
2mωn
(ak + a†k ) ∗ Ff ∗ (uF,x 𝐱̂ + uF,z 𝐳̂)exp(ik II ρ)
23
24 respectively, three orthonormal modes [25] obtained using Gram Schmidt orthogonalization and second
25 quantization. The normalization constants FS , FD and Ff are given in the appendix section and these constants
26 are only dependent on in-plane, wavevector, frequency of the phonon mode, longitudinal or transverse sound
27
28
29
an
velocity and thickness of the well. The x-component of Flexural mode and Dilatational mode was found to be
symmetric and asymmetric respectively; similarly, for z component the modes are found to be asymmetric
and symmetric respectively. Due to quantum confinement in the z direction the acoustic wavevector along z-
30 direction will be quantized i.e. for all value of k II there will be only few k l,n and k t,n possible which are given
31 by the dispersion curves. The k l,n is imaginary and k t,n is real for fundamental dilatational mode and both are
32
imaginary for fundamental flexural mode for low k ∥ value [23]. For a FSQW structure, the confined mode
dM
33
34
pattern will also depend on the boundary condition (BC) as free boundary condition will force the stress at the
35 interfaces to be zero. Whereas the clamped boundary condition (GaAs is embedded in a very dissimilar
36 material) will enforce that the displacement at interface goes to zero.
37
38 3.2. Calculation of optical phonon decay rate in DHSQW structure
39 In DHSQW structures, the confinement is only in the z-direction and in the x-y direction wave
40 properties behave as bulk or unconfined. Hence, assuming type-2 phonon interaction the Hamiltonian for three
41 phonon interactions can be written as:
42 3 1
43 1 dρ h̅ 2 1 2
pte

44
H3′ = ∫ ( ) ( ) P (ak,j a†k′ ,j′ a†k′′ ,j′′ ) (ê
k,j . e
̂ ∗
k′ ,j′ . ê
∗
k′′ ,j′′ )
A √N 2m ωk,j ωk′ ,j′ ωk′′ ,j′′
45 (11)
46 cos(k z z) ′ ′′
47 { } exp(−i(k ′z + k ′′
z )z) exp(i(k II − k II − k II ). ρ)
sin(k z z)
48
49
50 where 𝐤 𝐚 = k az 𝐳̂ + k aII 𝛒
̂. Using similar arguments as mentioned for the bulk case, the interaction Hamiltonian
51 is obtained after integrating the last term in the expression as:
ce

52
3 1
53
1h̅ 2 1 2
† † ∗ ∗
54 H3′ = ( ) ( ) P (ak,j ak′ ,j′ ak′′ ,j′′ ) (ê k,j . e
̂ k′ ,j′ . ê
k′′ ,j′′ )
55 √N 2m ωk,j ωk′ ,j′ ωk′′ ,j′′
cos(k z z) (12)
56
{ } exp(−i(k ′z + k ′′z )z)δkII −k′II −k′′
Ac

57 sin(k z z) II ,GII
58
59 The previously mentioned three phonon interaction suggests that the in-plane vector should be conserved to
60 produce δ00 and for all other combination the interaction Hamiltonian is zero. The IM squared value for
 AUTHOR SUBMITTED MANUSCRIPT - JPCM-111418.R1 Page 6 of 10

Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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3
calculating TP for the confined optical phonons can be obtained using Fermi golden rule similar to the bulk
4 case and the average value of that IM squared due to confinement over dz along z-direction is given by:
2
5 |MCD | = |⟨nk − 1, nk′ , nk′′ |H3 |nk , nk′ + 1, nk′′ + 1⟩|2
6 3
1 h̅ 1 cos 2(k z)
7 1 dz/2 dz ( ) ( ) P2 { 2 z } nk (nk′ + 1)(nk′′ + 1)
8 = ∫ N 2m ωk ωk′ ωk′′ sin (k z z)
dz −dz/2

pt
′ ′′
9 exp(−i(k z + k z )z)δkII −k′II −k′′
II ,GII
10 3 (13)
2 1 ̅
h 1
11 ∴ |MCD | = ( ) ( ) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II−k′′
N 2m ωk ωk′ ωk′′ II ,GII
12
13 dz /2
cos 2(k z)
∫ { 2 z } exp(−2i(k ′z + k ′′ z )z)dz

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14
15 −dz /2 sin (k z z)
16 Based on the Fuchs-Kliewer slab mode boundary condition, the z-component of the displacement can only
17 take the form of sin(k z z). Evaluation of the integral produces:
18 1 dz/2 π 1
19 k ′z = −k ′′
z ∫ sin2 ( z) dz = (14a)
dz −dz/2 dz 2
20 dz

us
21 1 2
22 ∫ sin2 (k z z) exp(−2i(k ′z + k ′′
z )z) dz
dz −dz
23 k ′z ≠ −k ′′
z 2 (14b)
24 (2(k ′z + k ′′ 2 2 2 ′ ′′
z ) dz − π ) sin((k z + k z )dz )
=
25 dz (2(k ′z + k ′′ 3 2 2 ′ ′′
z ) dz − 2π (k z + k z ))
26
27
28
29
an
In GaAs, the zone center LO phonon decays into two LA phonons of same phonon polarization with opposite
momentum through the Klemens channel. According to momentum conservation, the in-plane wavevector of
two daughter acoustic waves are related through k ′II = −k ′′ II if the parent optical phonon is zone center;
30 whereas 𝑘𝑧′ and 𝑘𝑧′′ will be equal and opposite if the two acoustic modes are in Γ − L direction. Otherwise if
31 daughter phonons are along Γ − K symmetry direction k ′z = k ′′ z = 0. Hence, for decay of zone center LO
32 phonon in GaAs, the integral is reduced to (14a). But for any other decay processes, if the acoustic phonons
dM
1
33 ωk′ 2 2
′ 2
34 are not on the same polarization branch then the k ′z and k ′′
z can be evaluated from (( c ) − k II ) and
l,t
35 1
36 ωk′′ 2 2
2
37 (( c ) − k ′′
II ) where ωk′ and ωk′′ are the acoustic phonon frequency and cl,t is the sound speed along
l,t
38
39 the direction (for longitudinal phonon) or perpendicular to the acoustic phonon wavevector. Combining Eq.
40 (13) with (14a) the IM squared can be written as:
3
41
D 2
1 h̅ 1 1
42 |MC | = ( ) ( ) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II−k′′ ,GII .
N 2m ωk ωk ωk
′ ′′ II 2 (15)
43
pte

2 2 1
44 ∴ |MCD | = |MB,K | .
45 2
2
46 where |𝑀𝐵,𝐾 | is the IM squared value bulk material for Klemens channel. Hence for the decay rate of Klemens
47 channel in a confined structure with respect to a bulk case in GaAs can be written as:
48 1 1 1
49 Γ(confined) = = Γ(bulk) = (16)
τ(confined) 2 2τ(bulk)
50
51
ce

52 3.3. Calculation of optical phonon decay rate in FSQW structure

53 Employing the mathematical description of optical phonon given in section II-A and description of
54 acoustic phonon in II-D, the three-phonon interaction Hamiltonian can be obtained analogous to the DHSQW
55 structure. Following Eq. 12 the average IM squared can be written as:
3
56
F 2
1 h̅ 1 2 (n ′
1 dz/2
|MC | = ( ) ( ) P nk k + 1)(nk + 1)δkII −k′II −k′′ ∫ v(z)dz
Ac

57 ′′ (17)
N 2m ωk ωk′ ωk′′ II ,GII d
z −dz /2
58
59 where 𝑣(𝑧) can be determined by considering the expression for optical and acoustic phonon given in (9) and
60 (17) and the decay process of interest. The frequency, wavevector and polarization of the three phonons
involved in the process are determined by considering the energy conservation principle, crystal momentum
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Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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2
3
conservation and symmetry plane of interaction. The two daughter acoustic phonons for Klemen’s channel
4 decay can be two dilatational or two flexural or one dilatational and one flexural modes and as shear modes
5 represents purely transverse vibrations it will only be participating in Vallee-Bogani (VB) channel evaluation
6 where a zone-edge LO and a TA phonon are created. For different decay processes the v(z) differs due to the
7 complicated mode pattern of the confined acoustic modes.
8

pt
9 3.3.1. Calculation of the 𝑣(𝑧) function for FSQW. The shear mode represents pure transverse modes and the
10 mode pattern appears to be of the form cos(k z,n z) or sin(k z,n z). The two optical phonon mode patterns for
11 the VB channel will follow the sin function in order to satisfy the boundary condition on phonon potential.
12
Employing the optical phonon mode pattern given in Eq. 9 and sinusoidal shear acoustic wave mode pattern,
13
the v(z) is given by:

cri
14 πz
15 v(z) = F1 (z) = sin6 ( ) (18a)
16 dz
πz πz
17 v(z) = F2 (z) = cos2 ( ) sin4 ( ) (18b)
18 dz dz
19 where F1 (z) denoted the case where both LO and TA phonon are of sin(k z,n z) form and F2 (z) represents the
20 shear TA mode is in cos(k z,n z) form and LO mode is in sin(k z,n z) form. The corresponding IM squared for

us
21 F1 (z) and F2 (z) are obtained as following:
22 3 dz
23 F,VB,1 2 1 h̅ Fs4 2
24
|MC | = ( ) ( ) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II −k′′ ,GII ∫ F1 (z)dz
Ndz 2m ωk ωk′ ωk′′ II −d z
25 2
3
26 F,VB,1 2 5 1 h̅ Fs4 (19a)
) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II −k′′
27
28
29
|MC | = ( ) (
16 N 2m ωk ωk′ ωk′′
2
∴ |MCF,VB,1 | =
5 4
an
Fs |MB,VB |
2
II ,GII

30
16
2 1 ̅ 3
h F 4 dz /2
31 |MCF,VB,2 | = ( ) (
s
) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′ −k′′ ,GII ∫ F2 (z)dz
32 Ndz 2m ωk ωk′ ωk′′ −dz /2
dM
33 3
F,VB,2 2 1 1 h̅ Fs4 (19b)
34 |MC | = ( ) ( ) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II −k′′
16 N 2m ωk ωk′ ωk′′ II ,GII
35
36 2 1 4 2
37 ∴ |MCF,VB,2 | = Fs |MB,VB |
16
38 𝑀𝐵,𝑉𝐵 is the IM squared value for Vallee-Bogani channel in bulk GaAs material.
39
40 As for Klemens type of decay the two daughter LA phonons can be of a combination of dilatational
41 and flexural mode pattern, as mentioned earlier. For all three cases the optical and acoustic vibrations lie in
42 the x-z plane assuming z is perpendicular to the interfaces. As the two modes comprise of complimentary
43
pte

variations along both x and z axis, we considered only x-direction displacement in order to simplify the
44
problem. We have assumed the magnitude of x-displacement in a simpler form given as:
45
46
Dilatational
47 uD,x = A1 cos(k l z) + B1 cos(k t z)
48 (Symmetric)
(20)
49 Flexural
uF,x = A2 sin(k l z) + B2 sin(k t z)
50 (Asymmetric)
51
ce

kt dz kt dz kt dz
52 where A1 = FD k II (k 2II − k 2t ) sin ( ), A2 = Ff k II (k 2II − k 2t ) cos ( ), B1 = FD 2k II k l k t sin ( ) and
2 2 2
53 kd
54 B2 = Ff 2k II k l k t cos ( t2 z).
Assuming the co-linearity of three phonons displacement, the 𝑣(𝑧) function for
55 three cases are calculated using fundamental wavevector value and the IM squared for those cases. The 𝑘𝑙 and
56 𝑘𝑡 value are assumed to be real for all three cases to ensure the existence of the confined modes inside the
Ac

57 quantum well, imaginary value of the wavevector forces the modes to be only surface bound.
58
59
60
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Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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2
3 Table 3. The evaluation of the 𝑣(𝑧) function for three different acoustic modes
4 4
πz π π
5 v(z) = F3 (z) = sin2 ( ) (A1 cos ( z) + B1 cos ( z))
6 Both D dz dz dz
7 mode 1 dz/2 1
8 ∫ F (z)dz = (A + B1 )4
dz −dz/2 3 16 1

pt
9 4
πz π π
10 v(z) = F4 (z) = sin2 ( ) (A2 sin ( z) + B2 sin ( z))
11 Both F dz dz dz
12 mode 1 dz/2 5
13 ∫ F (z)dz = (A + B2 )4
dz −dz/2 4 16 2

cri
14 2 2
15 πz π π π π
v(z) = F5 (z) = sin2 ( ) (A1 cos ( z) + B1 cos ( z)) (A2 sin ( z) + B2 sin ( z))
16 (1D+1F) dz dz dz dz dz
17 dz /2
mode 1 1
18 ∫ F (z)dz = (A + B1 )2 (A2 + B2 )2
dz −dz/2 5 16 1
19
20 Replacing the three functions obtained in Table-III in (17) the IM squared for the three processes are given as:
3

us
21 F,K,1 2 1 4
1 h̅ 1
22 |MC | = (A1 + B1 ) ( ) ( ) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II−k′′
II ,GII
16 N 2m ωk ωk′ ωk′′ (21a)
23 1
F,K,1 2 4 2
24 ∴ |MC | = (A + B1 ) |MB,K |
25 16 1
3
26 F,K,2 2 5 4
1 h̅ 1
) P2 nk (nk′ + 1)(nk′′ + 1)δkII −k′II−k′′
27
28
29
|MC | =
16
(A2 + B2 ) ( ) (
N 2m
∴ |MCF,K,2 | =
2
an
ωk ωk′ ωk′′
5
(A + B2 )4 |MB,K |
2
II ,GII
(21b)

16 2
30 3
31 F,K,3 2 1 2 2
1 h̅ 1
|MC | = (A1 + B1 ) (A2 + B2 ) ( ) ( ) P2 nk (nk′ + 1)(nk′′
32 16 N 2m ωk ωk′ ωk′′
dM
33 + 1)δkII −k′II−k′′ (21c)
II ,GII
34 2 1 2
35 ∴ |MCF,K,3 | = (A1 + B1 )2 (A2 + B2 )2 |MB,K |
36 16
where 𝑀𝐵,𝐾 is the IM squared value bulk material for Klemens channel. Using all the IM matrix squared value
37
38 the transition probability or inverse of lifetime can be calculated. The bulk IM squared value for all above
39 mentioned decay processes are decay process specific, hence calculation of the decay lifetime for confined
40 structures requires knowledge of the decay for bulk case. Using Fermi golden rule, the transition probabilities
41 are calculated as:
42 2π 2
ΓB,VB/K = |MB,VB/K | δ(h̅(ωk − ωk′ − ωk′′ ))
43 ̅h
pte

44 2π 2
D
ΓC,K = |MCD | δ(h̅(ωk,n − ωk′ − ωk′′ ))
45 ̅h
46 2π F,VB,1 2 (22)
47
F,1
ΓC,VB = |MC | δ(h̅(ωk,n − ωk′ ,n − ωk′′ ,n ))
h̅
48 2π F,K,1 2
49
F,1
ΓC,K = |MC | δ(h̅(ωk,n − ωk′ ,n − ωk′′ ,n ))
h̅
50 𝑎,𝑑
where 𝛤𝑐,𝑏 denotes the transition probability of the process under confinement and a can be {F=FSQW,
51
ce

52 D=DHSQW}, d can have values {1,2,3; depending on whether the CAPs are asymmetric or asymmetric}, c
53 denoted {C= confined, B= Bulk} and b is the {VB, K; type of decay process}. The difference between 𝜔𝑖 , 𝜔𝑖,𝑛
54 is that first term denotes frequency of the phonons in bulk and the later in confined structure.
55
56 4. Summary and Conclusion
Ac

57 In this research, the effect of dimensional confinement on the anharmonic decay of a longitudinal optical
58 phonon in isotropic cubic crystal (GaAs) is analyzed. The main decay processes considered for GaAs are the
59 Klemens channel (LO -> LA+LA) and the Valle-Bogani Channel (LO -> LO+TA). The confined optical
60 phonons and acoustic phonons are treated using the dielectric continuum model and the elastic continuum
model, thereafter the modes are second quantized. The transition probability of the decay process is calculated
Page 9 of 10 AUTHOR SUBMITTED MANUSCRIPT - JPCM-111418.R1

Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

1
2
3
for a DHSQW, where acoustic phonon modes are continuous, whereas optical phonon modes are confined
4 and FSQW structure where both acoustic and optical phonon modes are confined. The analysis is based on the
5 three-phonon interaction Hamiltonian the interaction matrix squared for both Klemens and Vallee-Bogani
6 decay processes is calculated for DHSQW and FSQW. The calculations suggest that decay probability of
7 Klemens channel reduces by half compared to bulk case for DHSQW and for FSQW the rate is significantly
8 depends on daughter phonons wavevector through non-linear relationship. The decay rate for the processes

pt
9 also depends on the mode pattern, i.e., whether the daughter acoustic phonon modes are symmetric or not.
10 This formulation can be extended to calculate anharmonic decay rate of phonons which have ubiquitous effect
11 on carrier and thermal transport and electron relaxation dynamics in the future nanostructured devices.
12
13
Acknowledgement

cri
14
15 The authors would like to acknowledge support from Air Force Office of Scientific Research through grant
16 FA9550-16-1-0227.
17
18 Appendix-A:
19
20 The quantization constant for shear, dilatational and flexural acoustic modes are given in the following section.

us
21 The constants are obtained using the second quantization where acoustic mode energies are equal to single
22 phonon energy. As we are only interested in confined modes in this problem we the constants are given for
23 real values of 𝑘𝑙 , 𝑘𝑡 .
24 Shear Mode:
25
26
27
28
29
an
1
√𝑑𝑧
,𝑛 = 0

𝐹𝑆 = (A.1)
30 2
31 √ ,𝑛 > 0
𝑑𝑧
32
dM
33
34 Dilatational mode:
35
1
36 𝐹𝑑−2 = 8𝑘 𝑘 [2𝑑𝑧 𝑘𝑙3 𝑘𝑡5 + 4𝑑𝑧 𝑘𝑙3 𝑘𝑡3 𝑘𝑥2 + 2𝑑𝑧 𝑘𝑙 𝑘𝑡5 𝑘𝑥2 + 10𝑑𝑧 𝑘𝑙3 𝑘𝑡 𝑘𝑥4 + 4𝑑𝑧 𝑘𝑙 𝑘𝑡3 𝑘𝑥4 +
𝑙 𝑡
37
38 2𝑑𝑧 𝑘𝑙 𝑘𝑡 𝑘𝑥6 − 8𝑑𝑧 𝑘𝑙3 𝑘𝑡 𝑘𝑥2 (𝑘𝑥2 + 𝑘𝑡2 ) cos(𝑑𝑧 𝑘𝑙 ) − 2𝑑𝑧 𝑘𝑙 𝑘𝑡 (𝑘𝑡2 − 𝑘𝑥2 )(𝑘𝑙2 + 𝑘𝑥2 ) cos(𝑑𝑧 𝑘𝑡 ) +
39 2𝑘𝑡 (𝑘𝑥2 − 𝑘𝑡2 )(𝑘𝑙2 𝑘𝑡2 + 7𝑘𝑙2 𝑘𝑥2 − 𝑘𝑡2 𝑘𝑥2 + 𝑘𝑥4 ) sin(𝑑𝑧 𝑘𝑙 ) + 8𝑘𝑙3 𝑘𝑥2 (𝑘𝑡2 − 𝑘𝑥2 ) sin(𝑑𝑧 𝑘𝑙 ) + (𝑘𝑙2 𝑘𝑡5 + (A.2)
40 4𝑘𝑙3 𝑘𝑡2 𝑘𝑥2 + 6𝑘𝑙2 𝑘𝑡3 𝑘𝑥2 − 𝑘𝑡5 𝑘𝑥2 − 4𝑘𝑙3 𝑘𝑥4 − 7𝑘𝑙2 𝑘𝑡 𝑘𝑥4 + 2𝑘𝑡3 𝑘𝑥4 − 𝑘𝑡 𝑘𝑥6 ) sin(𝑑𝑧 (𝑘𝑙 − 𝑘𝑡 )) +
41 (𝑘𝑙2 𝑘𝑡5 − 4𝑘𝑙3 𝑘𝑡2 𝑘𝑥2 + 6𝑘𝑙2 𝑘𝑡3 𝑘𝑥2 − 𝑘𝑙5 𝑘𝑥2 − 4𝑘𝑙3 𝑘𝑥4 − 7𝑘𝑙2 𝑘𝑡 𝑘𝑥4 + 2𝑘𝑡3 𝑘𝑥4 − 𝑘𝑡 𝑘𝑥6 ) sin(𝑑𝑧 (𝑘𝑙 +
42
43 𝑘𝑡 ))]
pte

44 Flexural mode:
45 1
46 𝐹𝑓−2 = 8𝑘 𝑘 [2𝑑𝑧 𝑘𝑙3 𝑘𝑡5 + 4𝑑𝑧 𝑘𝑙3 𝑘𝑡3 𝑘𝑥2 + 2𝑑𝑧 𝑘𝑙 𝑘𝑡5 𝑘𝑥2 + 10𝑑𝑧 𝑘𝑙3 𝑘𝑡 𝑘𝑥4 − 4𝑑𝑧 𝑘𝑙 𝑘𝑡3 𝑘𝑥4 +
𝑙 𝑡
47 2𝑑𝑧 𝑘𝑙 𝑘𝑡 𝑘𝑥6 + 8𝑑𝑧 𝑘𝑙3 𝑘𝑡 𝑘𝑥2 (𝑘𝑥2 + 𝑘𝑡2 ) cos(𝑑𝑧 𝑘𝑙 ) + 2𝑑𝑧 𝑘𝑙 𝑘𝑡 (𝑘𝑡2 − 𝑘𝑥2 )(𝑘𝑙2 + 𝑘𝑥2 ) cos(𝑑𝑧 𝑘𝑡 ) −
48
2𝑘𝑡 (𝑘𝑥2 − 𝑘𝑡2 )(𝑘𝑙2 𝑘𝑡2 + 7𝑘𝑙2 𝑘𝑥2 − 𝑘𝑡2 𝑘𝑥2 + 𝑘𝑥4 ) sin(𝑑𝑧 𝑘𝑙 ) + 8𝑘𝑙3 𝑘𝑥2 (𝑘𝑥2 − 𝑘𝑙2 ) sin(𝑑𝑧 𝑘𝑙 ) + (𝑘𝑙2 𝑘𝑡5 +
49 (A.3)
50 4𝑘𝑙3 𝑘𝑡2 𝑘𝑥2 + 6𝑘𝑙2 𝑘𝑡3 𝑘𝑥2 − 𝑘𝑡5 𝑘𝑥2 − 4𝑘𝑙3 𝑘𝑥4 − 7𝑘𝑙2 𝑘𝑡 𝑘𝑥4 + 2𝑘𝑡3 𝑘𝑥4 − 𝑘𝑡 𝑘𝑥6 ) sin(𝑑𝑧 (𝑘𝑙 − 𝑘𝑡 )) +
51 (𝑘𝑙2 𝑘𝑡5 − 4𝑘𝑙3 𝑘𝑡2 𝑘𝑥2 + 6𝑘𝑙2 𝑘𝑡3 𝑘𝑥2 − 𝑘𝑙5 𝑘𝑥2 − 4𝑘𝑙3 𝑘𝑥4 − 7𝑘𝑙2 𝑘𝑡 𝑘𝑥4 + 2𝑘𝑡3 𝑘𝑥4 − 𝑘𝑡 𝑘𝑥6 ) sin(𝑑𝑧 (𝑘𝑙 +
ce

52 𝑘𝑡 ))]
53
54 where 𝑘𝑥 denotes the in-plane wavevector which is equivalently noted here as k II for both flexural and
55 dilatational modes.
56 lowest values for 𝑘𝑥 , 𝑘𝑙 and 𝑘𝑡 are limited by the device dimensions in the in-plane direction and dimension
Ac

57 in confined direction. The lowest values for 𝑘𝑡 and 𝑘𝑡 are 3.14 × 108 for a 10 𝑛𝑚 thick quantum well. For a
58
10 nm thick quantum well:
59
60
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Effect of quantum confinement on anharmonic decay of LO phonon Datta et al.

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3
2
4 𝐹𝑆 = √ −8 = 14142 𝑚−1/2
5 10
6
7
𝑑𝑧 𝑘𝑡8
𝐹𝑑−2 , 𝐹𝑓−2 ~ ≈ 1040
8 𝑘𝑡 𝑘𝑙

pt
9 ∴ 𝐹𝐷 , 𝐹𝑆 ~10−20
10
11 The value for 𝐹𝐷 and 𝐹𝑓 are calculated approximately and obtained as very small values.
12
13 References

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dM
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