Back contact optimization for Sb<sub>2</sub>Se<sub>3</sub> solar cells

Li Xue-Rui; Lin Jun-Hui; Tang Rong; Zheng Zhuang-Hao; Su Zheng-Hua; Chen Shuo; Fan Ping; Liang Guang-Xing

doi:10.7498/aps.72.20221929

Abstract

Antimony selenide (Sb₂Se₃) has advantages of low-toxicity, abundant and excellent photoelectric properties. It is widely considered as one of the most promising light-harvesting materials for thin-film solar cells. However, the power conversion efficiency of the Sb₂Se₃ thin-film solar cell is still far inferior to that of cadmium telluride, copper indium gallium selenium and perovskite solar cells. As is well known, the Sb₂Se₃ solar cell performance is closely related to the light absorber layer (crystallinity, composition, bulk defect density, etc.), PN heterojunction quality (charge carrier concertation, energy band alignment, interface defect density, etc.) and back-contact barrier formation, which determines the process of carrier generation, excitation, relaxation, transfer and recombination. The low fill factor is one of the core problems that limit further efficiency improvement of Sb₂Se₃ solar cells, which can be attributed to the high potential barrier at the back contact between the Mo electrode and Sb₂Se₃ absorption layer. In this work, a heat treatment is applied to the Mo electrode to generate a MoO₂ buffer layer. It can be found that this buffer layer can inhibit MoSe₂ film growth, exhibiting better Ohmic contact with Sb₂Se₃, and reducing the back contact barrier of the solar cell. The Sb₂Se₃ thin film is prepared by an effective combination reaction involving sputtered and selenized Sb precursor. After introducing the MoO₂ buffer layer, it can also promote the formation of (hk1) (including (211), (221), (002), etc.) preferentially oriented Sb₂Se₃ thin films with average grain size over 1 μm. And the ratio of Sb to Se is optimized from 0.57 to 0.62, approaching to the stoichiometric ratio of Sb₂Se₃ thin film and inhibiting the formation of V_se and Sb_Se defects. Finally, it enhances the open-circuit voltage (V_OC) of solar cells from 0.473 to 0.502 V, the short-circuit current density (J_SC) from 22.71 to 24.98 mA/cm², and the fill factor (FF) from 46.90% to 56.18%, thereby increasing the power conversion efficiency (PCE) from 5.04% to 7.05%. This work proposes a facile strategy for interfacial treatment and elucidates the related carrier transport enhancement mechanism, thus paving a bright avenue to breaking through the efficiency bottleneck of Sb₂Se₃ thin film solar cells.

Keywords:

Authors and contacts

College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518060, China

Corresponding author: Liang Guang-Xing, lgx@szu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 62074102), the Natural Science Foundation of Guangdong Province, China (Grant No. 2022A1515010979), and the Science and Technology Plan Project of Shenzhen, China (Grant No. 20220808165025003).

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References

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图 1 Sb₂Se₃薄膜太阳电池制备流程　(a) MoO₂制备过程; (b) Mo/MoO₂/Sb₂Se₃背接触结构图; (c) 磁控溅射制备Sb薄膜; (d) 采用后硒化工艺生长Sb₂Se₃薄膜; (e) 化学水浴法制备CdS薄膜; (f) 磁控溅射制备ITO薄膜; (g) Sb₂Se₃薄膜太阳电池结构图

Figure 1. Fabrication process of Sb₂Se₃ solar cells: (a) MoO₂ preparation; (b) back contact structure of Mo/MoO₂/Sb₂Se₃; (c) sputtering Sb thin film; (d) post-selenation for Sb₂Se₃ thin film; (e) chemical bath deposition for CdS thin film; (f) sputtering ITO thin film; (g) Sb₂Se₃ solar cell sturcture.

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图 2 (a) W-MoO₂和WO-MoO₂样品的XRD图谱; (b) W-MoO₂和WO-MoO₂样品的拉曼图谱; (c) WO-MoO₂样品的表面形貌; (d) W-MoO₂样品的表面形貌; (e) WO-MoO₂样品的剖面形貌图; (f) W-MoO₂样品的剖面形貌图

Figure 2. (a) XRD patterns of W-MoO₂ and WO-MoO₂ sample; (b) Raman patterns of W-MoO₂ and WO-MoO₂ sample; (c) surface morphology of WO-MoO₂ sample; (d) surface morphology of W-MoO₂ thin film; (e) cross sectional image of WO-MoO₂ sample; (f) cross sectional image of W-MoO₂ sample.

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图 3 (a) W-MoO₂和WO-MoO₂样品上生长Sb₂Se₃薄膜的XRD图谱; (b) 关于(360), (211), (221)和(002)衍射峰的TC值; (c) WO-MoO₂样品上生长Sb₂Se₃薄膜的表面形貌; (d) W-MoO₂样品上生长Sb₂Se₃薄膜的表面形貌; (e) WO-MoO₂样品上生长Sb₂Se₃薄膜太阳电池的剖面形貌图; (f) W-MoO₂样品上生长Sb₂Se₃薄膜太阳电池的剖面形貌图

Figure 3. (a) XRD patterns of Sb₂Se₃ thin film prepared on W-MoO₂ and WO-MoO₂ samples; (b) TC value comparation of the diffraction peaks (360), (211), (221) and (002); (c) morphology of Sb₂Se₃ thin film prepared on WO-MoO₂ samples; (d) morphology of Sb₂Se₃ thin film prepared on W-MoO₂ samples; (e) cross sectional image of Sb₂Se₃ solar cells based on WO-MoO₂ sample; (f) cross sectional image of Sb₂Se₃ solar cells based on W-MoO₂ sample.

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图 4 (a) MoO₂引入前后太阳电池的J - V曲线; (b) MoO₂引入前后太阳电池的外量子效率EQE (左)和相应的积分电流(右); (c) MoO₂引入前后Sb₂Se₃的禁带宽度; (d) MoO₂引入前后乌尔巴赫能量(E_u)

Figure 4. (a) J -V curve of solar cells before and after MoO₂ introduction; (b) EQE curve (left) and integrating current (right) before and after MoO₂ introduction; (c) Sb₂Se₃ bandgap calculated from EQE before and after MoO₂ introduction; (d) Urbach energy (E_u) before and after MoO₂ introduction.

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图 5 (a) MoO₂引入前后太阳电池在暗态环境下测量的J-V曲线; (b) dJ/dV-V曲线; (c) dV/dJ-(J + J_sc)^–1曲线; (d) ln(J + J_sc–GV)-(V–RJ)曲线

Figure 5. (a) J-V curves of solar cell in dark state; (b) dJ/dV-V curves; (c) dV/dJ-(J + J_sc)^–1 curves; (d) ln(J + J_sc–GV)-(V–RJ) curves

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图 6 (a) 太阳电池在暗态环境下测量的V_OC-T曲线; (b) C-V和DLCP曲线; (c) 1/C ²-V曲线; (d) 暗态环境下测量背接触I-V曲线

Figure 6. (a) V_oc-T curves of solar cell in dark state; (b) C-V and DLCP curves; (c) 1/C ²-V curves; (d) I-V curves for back-contact in dark state.

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表 1 Sb₂Se₃薄膜的化学成分

Table 1. Composition in Sb₂Se₃ thin films.

Samples Sb atomic percentage/% Se atomic percentage/% Sb/Se ratio

WO- MoO₂ 36.35 63.65 0.57
W-MoO₂ 38.27 61.73 0.62

DownLoad: CSV

表 2 太阳电池性能参数对比

Table 2. Comparison of solar cell performance.

Devices V_OC/V J_SC/(mA·cm^–2) FF/% PCE/%

WO-MoO₂ 0.473 22.71 46.90 5.04
W-MoO₂ 0.502 24.98 56.18 7.05

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表 3 太阳电池在暗态环境下测量的电学性能参数

Table 3. Solar cell performance in dark state.

Devices G/(mS·cm^–2) R/(Ω·cm²) A J₀/(mA·cm^–2)

WO-MoO₂ 3.49 10.02 2.15 2.65×10^–2
W-MoO₂ 0.05 8.95 1.96 6.16×10^–3

DownLoad: CSV

表 4 太阳电池的界面性能参数

Table 4. Solar cell interface performance.

Devices E_a/eV N_i/cm^–3 x/nm V_bi/mV Slop/(A·V^–1) Resistance/Ω

WO-MoO₂ 1.16 2.10×10¹⁶ 272.18 525 0.072 13.89
W-MoO₂ 1.22 1.61×10¹⁶ 282.44 550 0.097 10.31

DownLoad: CSV

[1]	Duan Z T, Liang X Y, Feng Y, Ma H Y, Liang B L, Wang Y, Luo S P, Wang S F, Schropp R E I, Mai Y H, Li Z Q 2022 Adv. Mater. 34 2202969 Google Scholar
[2]	Chen S, Liu T X, Zheng Z H, Ishaq M, Liang G X, Fan P, Chen T, Tang J 2022 J Energy Chem. 67 508 Google Scholar
[3]	Zhou Y, Wang L, Chen S Y, Qin S K, Liu X S, Chen J, Xue D J, Luo M, Cao Y Z, Chen Y B, Sargent E H, Tang J 2015 Nat. Photonics 9 409 Google Scholar
[4]	Hadke S, Huang M L, Chen C, Tay Y F, Chen S Y, Tang J, Wong L 2022 Chem. Rev. 122 10170 Google Scholar
[5]	Rajpure K Y, Bhosale C H 2002 Mater. Chem. Phys. 73 6 Google Scholar
[6]	Choi Y C, Mandal T N, Yang W S, Lee Y H, Im S K, Noh J H, Seok S 2014 Angew. Chem. Int. Ed. 126 1353 Google Scholar
[7]	Zhou Y, Leng M Y, Xia Z, Zhong J, Song H B, Liu X S, Yang B, Zhang J P, Chen J, Zhou K H, Han J B, Cheng Y B, Tang J 2014 Adv. Energy Mater. 4 1301864 Google Scholar
[8]	Wang X, Tang R, Yin Y W, Ju H X, Li S A, Zhu C F, Chen T 2019 Sol. Energy Mater. Sol. Cells 189 5 Google Scholar
[9]	Wang L, Li D B, Li K H, Chen C, Deng H X, Gao L, Zhao Y, Jiang F, Li L Y, Huang F, He Y S, Song H S, Niu G D, Tang J 2017 Nat. Energy 2 17046 Google Scholar
[10]	Wen X X, Chen C, Lu S C, Li K H, Kondrotas R, Zhao Y, Chen W H, Gao L, Wang C, Zhang J, Niu G D, Tang J 2018 Nat. Commun. 9 2179 Google Scholar
[11]	Liang G X, Zheng Z H, Fan P, Luo J T, Hu J G, Zhang X H, Ma H L, Fan B, Luo Z K, Zhang D P 2018 Sol. Energy Mater. Sol. Cells 174 263 Google Scholar
[12]	Liang G X, Zhang X H, Ma H L, Hu J G, Fan B, Luo Z K, Zheng Z H, Luo J T, Fan P 2017 Sol. Energy Mater. Sol. Cells 160 257 Google Scholar
[13]	Tang R, Zheng Z H, Su Z H, Li X J, Wei Y D, Zhang X H, Fu Y Q, Luo J T, Fan P, Liang G X 2019 Nano Energy 64 103929 Google Scholar
[14]	Liang G X, Luo Y D, Chen S, Tang R, Zheng Z H, Li X J, Liu X S, Liu Y K, Li Y F, Chen X Y, Su Z H, Zhang X H, Ma H L, Fan P 2020 Nano Energy 73 104806 Google Scholar
[15]	Tang R, Chen S, Zheng Z H, Su Z H, Luo J T, Fan P, Zhang X H, Tan J, Liang G X 2022 Adv. Mater. 34 2109078 Google Scholar
[16]	Li J J, Zhang Y, Zhao W, Nam D, Cheong H, Wu L, Zhou Z Q, Sun Y 2015 Adv. Energy Mater. 5 1402178 Google Scholar
[17]	Neugebohrn N, Hammer M S, Sayed M H, Michalowski P, Stroth C, Parisi J, Richter M 2017 J. Alloys Compd. 725 69 Google Scholar
[18]	Li Z Q, Chen X, Zhu H B, Chen J W, Guo Y T, Zhang C, Zhang W, Niu X N, Mai Y H 2017 Sol. Energy Mater. Sol. Cells 161 190 Google Scholar
[19]	Zhang J Y, Guo H F, Jia X G, Ning H, Ma C H, Wang X Q, Yuan N Y, Ding J N 2021 Sol. Energy 214 231 Google Scholar
[20]	Wu H R, Zhou X C, Li J D, Li X M, Li B W, Fei W W, Zhou J X, Yin J, Guo W L 2018 Small 14 1802276 Google Scholar
[21]	Lopez S C, Lopez I O P, Lara M C, Garcia A E, Sanchez M C M, Hernandez J A R, Lopez M C 2018 Phys. Status Solidi A. 215 1800226 Google Scholar
[22]	曹宇, 刘超颖, 赵耀, 那艳玲, 江崇旭, 王长刚, 周静, 于皓 2022 物理学报 71 038802 Google Scholar Cao Y, Liu C Y, Zhao Y, Na Y L, Jiang C X, Wang C G, Zhou J, Yu H 2022 Acta Phys. Sin. 71 038802 Google Scholar
[23]	Luo Y D, Tang R, Chen S, Hu J G, Liu Y K, Li Y F, Liu X S, ZhengZ H, Su Z H, Ma X F, Fan P, Zhang X H, Ma H L, Chen Z G, Liang G X 2020 Chem. Eng. J. 393 124599
[24]	曹宇, 祝新运, 陈翰博, 王长刚, 张鑫童, 侯秉东, 申明仁, 周静 2018 物理学报 67 247301 Google Scholar Cao Y, Zhu X Y, Chen H B, Wang C G, Zhang X T, Hou B D, Shen MR, Zhou J 2018 Acta Phys. Sin. 67 247301 Google Scholar
[25]	Luo M, Leng M Y, Liu X S, Chen J, Chen C, Qin S K, Tang J 2014 Appl. Phys. Lett. 104 173904 Google Scholar

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Back contact optimization for Sb₂Se₃ solar cells

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Corresponding author: Liang Guang-Xing, lgx@szu.edu.cn

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Samples	Sb atomic percentage/%	Se atomic percentage/%	Sb/Se ratio
WO- MoO₂	36.35	63.65	0.57
W-MoO₂	38.27	61.73	0.62

Devices	V_OC/V	J_SC/(mA·cm^–2)	FF/%	PCE/%
WO-MoO₂	0.473	22.71	46.90	5.04
W-MoO₂	0.502	24.98	56.18	7.05

Devices	G/(mS·cm^–2)	R/(Ω·cm²)	A	J₀/(mA·cm^–2)
WO-MoO₂	3.49	10.02	2.15	2.65×10^–2
W-MoO₂	0.05	8.95	1.96	6.16×10^–3

Devices	E_a/eV	N_i/cm^–3	x/nm	V_bi/mV	Slop/(A·V^–1)	Resistance/Ω
WO-MoO₂	1.16	2.10×10¹⁶	272.18	525	0.072	13.89
W-MoO₂	1.22	1.61×10¹⁶	282.44	550	0.097	10.31

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Back contact optimization for Sb2Se3 solar cells

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Corresponding author: Liang Guang-Xing, lgx@szu.edu.cn

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Back contact optimization for Sb₂Se₃ solar cells