Multidentate anchoring through additive engineering for highly efficient Sb2S3 planar thin film solar cells

doi:10.1016/j.jmst.2021.01.078

Abstract

Abstract:

Sb₂S₃ is a promising candidate for the flexible solar cells or the top subcells in tandem solar cells due to its wide-bandgap, less toxic, acceptable cost and progressive power conversion efficiency (PCE). However, the poor quality and high trap states of Sb₂S₃ films limit the device performance further enhancement. Herein, we adopt a multidentate ionic liquid, tetramethylammonium hexafluorophosphate ([TMA][PF₆]) as a novel additive to address this issue. The octahedral [PF₆]^- contains six different oriented fluorine atoms with the lone pair electrons, which could coordinate with Sb atoms due to the multidentate anchoring. Thus, the high-quality Sb₂S₃ film with low trap states has been achieved. Moreover, the Fermi level of the Sb₂S₃ film has been upshifted, thereby showing an effective charge transfer. As a result, all photovoltaic parameters of the optimized Sb₂S₃ devices are obviously enhanced, boosting the final PCE from 4.43 (control device) to 6.83 %. Our study about the multidentate anchoring is manifested to be an effective method to enhance the Sb₂S₃ device performance.

Key words: Sb₂S₃, Solar cells, Additive engineering, Multidentate anchoring, Passivation

Jian Han, Xingyu Pu, Hui Zhou, Qi Cao, Shuangjie Wang, Jiabao Yang, Junsong Zhao, Xuanhua Li. Multidentate anchoring through additive engineering for highly efficient Sb₂S₃ planar thin film solar cells[J]. J. Mater. Sci. Technol., 2021, 89: 36-44.

Figures/Tables 7

Fig. 1. (a) Schematic diagram of the preparation process for [TMA][PF6]-assisted Sb2S3 film and device structure. (b) Cross-sectional SEM image of Sb2S3 solar cell without Au electrode. (c) Crystal structure of Sb2S3 (showing the distances of interribbons and intersheets) and the molecular structure of the [TMA][PF6]. (d) Working mechanism schematic of [PF6]- in Sb2S3: [PF6]- coordinate with Sb to form multidentate anchoring structure at the grain boundaries of Sb2S3. The Sb2S3 films with different concentrations of [TMA][PF6] additives: (e) surface SEM images; (f) XRD patterns, and the inset is the zoom-in of the 24.5°-26.0° region around (130) peak.

Table 1 Photovoltaic parameters (best) of Sb2S3 devices with different concentrations of [TMA][PF6] additives.

Condition	V_OC (V)	J_SC (mA cm^-2)	FF (%)	PCE (%)
0 %	0.57 ± 0.006 (0.58)^(a)	14.87 ± 0.24 (14.94)	50.32 ± 0.46 (51.13)	4.27 ± 0.14 (4.43)
2 %	0.60 ± 0.007 (0.61)	16.33 ± 0.22 (16.48)	53.75 ± 0.47 (54.65)	5.27 ± 0.14 (5.49)
10 %	0.65 ± 0.005 (0.66)	17.57 ± 0.18 (17.65)	58.03 ± 0.43 (58.66)	6.63 ± 0.12 (6.83)
30 %	0.62 ± 0.005 (0.63)	16.76 ± 0.20 (16.83)	55.31 ± 0.48 (56.21)	5.75 ± 0.13 (5.96)

Fig. 2. (a) Raman spectra (containing the Raman spectrum of the [TMA][PF6]). High-resolution of (b) P 2p and F 1 s, (c) Sb 3d, and (d) S 2p XPS spectra for Sb2S3 films without and with 10 % additive.

Fig. 3. The AFM topography maps of (a) the optimized Sb2S3 (the addition of 10 % [TMA][PF6]) and (c) control Sb2S3 film, and their corresponding KPFM maps of (b) optimized Sb2S3 and (d) control Sb2S3 film. (e) The line profile of surface potential of (b) and (d). The schematic about the crystallization process of (f) the control Sb2S3 and (g) optimized Sb2S3. Yellow, brown, purple and gray spheres represent S, Sb, P and F, respectively.

Fig. 4. Photovoltaic performance: (a) J-V curves of different Sb2S3 devices measured under standard AM 1.5 G simulated sunlight, (b) UV-vis absorption spectra of different Sb2S3 films (the inset is the Tauc plot for the bandgap calculations), (c) EQE and their integrated current plots, and (d) IQE of different Sb2S3 devices.

Fig. 5. (a) UPS characterizations for the control and optimized Sb2S3 films. (b) Energy level diagram of control and optimized Sb2S3 devices. (c) I-V curves in dark conditions (the inset shows the structure of the devices), (d) 1/C2 versus V curves.

Fig. 6. (a) PL of the Sb2S3 films, and (b) dark J-V characterizations of Sb2S3 devices with different concentrations of [TMA][PF6] additives. (c) EIS of Sb2S3 devices measured in the darkness (the inset shows the equivalent circuit), and (d) bias voltage dependent Rrec curves for the Sb2S3 devices with different concentrations of [TMA][PF6] additives.

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Multidentate anchoring through additive engineering for highly efficient Sb₂S₃ planar thin film solar cells

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