First-Principles Study on Hole Mobility in Antimony Selenide

doi:10.16553/j.cnki.issn1000-985x.2025.0243

Abstract

Abstract: Antimony selenide （Sb₂Se₃） is a promising photovoltaic thin-film material， owing to its abundant reserves， non-toxicity， and good stability. Despite substantial advances in its power conversion efficiency， the underlying carrier transport mechanism—particularly the key scattering processes that limit the hole mobility—remains unclear. To address this， first-principles density functional theory （DFT） combined with Boltzmann transport theory was used to quantitatively evaluate the contributions of acoustic deformation potential （ADP）， ionized impurity （IMP）， and polar optical phonon （POP） scattering to Sb₂Se₃ hole mobility. The calculated room-temperature hole mobility is 42.8 cm²·V^-1·s^-1. The results show that POP scattering dominated the limitation of hole mobility over a temperature range of 105~650 K. The mobility exhibits distinct anisotropy along the three principal crystallographic directions （x， y and z）， with the highest mobility in the y-axis direction and the lowest in the z-axis direction. It is also found that at low carrier concentrations， the hole mobility remains essentially unchanged as carrier concentration increases； at high carrier concentrations， the hole mobility decreases as carrier concentration increases. This work clarifies the dominant factors restricting the hole mobility of Sb₂Se₃ and offers a theoretical foundation for further performance optimization.

Key words: Sb₂Se₃; solar cell; scattering mechanism; hole mobility; first principle; density functional theory; Boltzmann transport theory

CLC Number:

O469

ZHANG Leng, HUANG Jiajian, SHEN Hui, WU Kongping. First-Principles Study on Hole Mobility in Antimony Selenide[J]. Journal of Synthetic Crystals, 2026, 55(4): 627-633.

Figures/Tables 7

Fig.1 Structure of primitive cell in antimony selenide

Table 1 Optimized lattice parameters （a， b， c） and volume （V） of Sb2Se3

Material	Lattice constant
Material	a/Å	b/Å	c/Å	V/Å³
Reference ［16］	3.977	11.643	11.788	545.83
Reference ［17］	3.833	11.189	11.291	484.24
This work	3.99	11.35	11.67	527.17

Fig.2 Band structure （a） and projected density of states （PDOS）（b） of Sb2Se3 obtained using the PBE functional

Table 2 Calculated elastic constants （C） and deformation potentials （DA） for Sb2Se3

Material	C/GPa			D_A/eV
Material	a	b	c	a	b	c
Reference ［22］	81.65	55.20	30.9	0.53	2.86	2.47
This work	80.97	59.72	37.17	0.47	2.38	2.28

Fig.3 Variation curves of the mobility of each branch （a） and the total mobility （b） with temperature， resulting from three scattering mechanisms

Table 3 Comparison of POP scattering parameters for Sb2Se3 with literature data

Material	ε_∞				ε_s				ω_po/THz
Material	a	b	c	Average	a	b	c	Average	ω_po/THz
Reference ［25］	15.11	14.92	10.53	13.52	85.64	128.18	15.00	76.27	2.57
This work	24.61	25.85	15.56	22.01	94.29	135.91	20.80	83.67	2.98

Fig.4 Incorporating ADP， IMP， and POP scattering mechanisms， temperature-dependent hole mobility of Sb2Se3 at various concentrations （a）， and temperature-dependent hole mobility of Sb2Se3 along the x-， y-， and z-directions （b）

References 26

[1]	WANG L， LI D B， LI K H， et al. Stable 6%-efficient Sb₂Se₃ solar cells with a ZnO buffer layer［J］. Nature Energy， 2017， 2： 17046.
[2]	YANG Z L， WANG X M， CHEN Y Z， et al. Ultrafast self-trapping of photoexcited carriers sets the upper limit on antimony trisulfide photovoltaic devices［J］. Nature Communications， 2019， 10： 4540.
[3]	DUAN Z T， LIANG X Y， FENG Y， et al. Sb₂Se₃ thin-film solar cells exceeding 10% power conversion efficiency enabled by injection vapor deposition technology［J］. Advanced Materials， 2022， 34（30）： e2202969.
[4]	CHEN C， LI K H， TANG J. Ten years of Sb₂Se₃ thin film solar cells［J］. Solar RRL， 2022， 6（7）： 2200094.
[5]	SINGH Y， RANI S， SHASHI， et al. Sb₂Se₃ heterostructure solar cells： techniques to improve efficiency［J］. Solar Energy， 2023， 249： 174-182.
[6]	ZHOU Y， LENG M Y， XIA Z， et al. Solution-processed antimony selenide heterojunction solar cells［J］. Advanced Energy Materials， 2014， 4（8）： 1301846.
[7]	WEN X X， CHEN C， LU S C， et al. Vapor transport deposition of antimony selenide thin film solar cells with 7.6% efficiency［J］. Nature Communications， 2018， 9： 2179.
[8]	LI Z Q， LIANG X Y， LI G， et al. 9.2%-efficient core-shell structured antimony selenide nanorod array solar cells［J］. Nature Communications， 2019， 10： 125.
[9]	WANG X M， TANG R F， JIANG C H， et al. Manipulating the electrical properties of Sb₂（S， Se）₃ film for high-efficiency solar cell［J］. Advanced Energy Materials， 2020， 10（40）： 2002341.
[10]	ZHAO Y Q， WANG S Y， JIANG C H， et al. Regulating energy band alignment via alkaline metal fluoride assisted solution post-treatment enabling Sb₂（S， Se）₃ solar cells with 10.7% efficiency［J］. Advanced Energy Materials， 2022， 12（1）： 2103015.
[11]	YUAN C C， ZHANG L J， LIU W F， et al. Rapid thermal process to fabricate Sb₂Se₃ thin film for solar cell application［J］. Solar Energy， 2016， 137： 256-260.
[12]	BLACK J， CONWELL E M， SEIGLE L， et al. Electrical and optical properties of some M₂ ^V-B N₃ ^VI-B semiconductors［J］. Journal of Physics and Chemistry of Solids， 1957， 2（3）： 240-251.
[13]	LIANG G X， CHEN X Y， REN D L， et al. Ion doping simultaneously increased the carrier density and modified the conduction type of Sb₂Se₃ thin films towards quasi-homojunction solar cell［J］. Journal of Materiomics， 2021， 7（6）： 1324-1334.
[14]	MADELUNG O. Semiconductor： data handbook［M］. 2nd ed. New York： Springer-Verlag， 1996.
[15]	张　冷，张鹏展，刘　飞，等. 基于形变势理论的掺杂计算Sb₂Se₃空穴迁移率［J］. 物理学报， 2024， 73（4）： 047101.
	ZHANG L， ZHANG P Z， LIU F， et al. Carrier mobility in doped Sb₂Se₃ based on deformation potential theory［J］. Acta Physica Sinica， 2024， 73（4）： 047101 （in Chinese）.
[16]	EL-SAYAD E A， MOUSTAFA A M， MARZOUK S Y. Effect of heat treatment on the structural and optical properties of amorphous Sb₂Se₃ and Sb₂Se₂S thin films［J］. Physica B： Condensed Matter， 2009， 404（8/9/10/11）： 1119-1127.
[17]	ZHENG X W， XIE Y， ZHU L Y， et al. Growth of Sb₂E₃ （E = S， Se） polygonal tubular crystals via a novel solvent-relief-self-seeding process［J］. Inorganic Chemistry， 2002， 41（3）： 455-461.
[18]	PONCÉ S， MARGINE E R， GIUSTINO F. Towards predictive many-body calculations of phonon-limited carrier mobilities in semiconductors［J］. Physical Review B， 2018， 97（12）： 121201.
[19]	GRIMVALL. The electron-phonon interaction in metals［M］. Amsterdam： North-Holland Pub.， 1981.
[20]	GIUSTINO F， COHEN M L， LOUIE S G. Electron-phonon interaction using Wannier functions［J］. Physical Review B， 2007， 76（16）： 165108.
[21]	GANOSE A M， PARK J， FAGHANINIA A， et al. Efficient calculation of carrier scattering rates from first principles［J］. Nature Communications， 2021， 12： 2222.
[22]	LORA DA SILVA E， SKELTON J M， RODRÍGUEZ-HERNÁNDEZ P， et al. A theoretical study of the Pnma and R3m phases of Sb₂S₃， Bi₂S₃， and Sb₂Se₃ ［J］. Journal of Materials Chemistry C， 2022， 10： 15061-15074.
[23]	EMIN D. Polarons［M］. Cambridge： Cambridge University Press， 2013.
[24]	FRÖHLICH H. Interaction of electrons with lattice vibrations［J］. Proceedings of the Royal Society of London Series A， Mathematical and Physical Sciences， 1952， 215（1122）： 291-298.
[25]	WANG X W， GANOSE A M， KAVANAGH S R， et al. Band versus polaron： charge transport in antimony chalcogenides［J］. ACS Energy Letters， 2022， 7（9）： 2954-2960.
[26]	NAG B. Electron transport in compound semiconductors［M］. Berlin， Heidelberg： Springer， 1980.