Deciphering the Role of Key Defects in Sb2Se3, a Promising Candidate for Chalcogenide-Based Solar Cells

Stoliaroff, Adrien; Lecomte, Alicia; Rubel, Oleg; Jobic, Stéphane; Zhang, Xianghua; Latouche, Camille; Rocquefelte, Xavier

doi:10.1021/acsaem.9b02192

Cited by 62 publications

(79 citation statements)

References 38 publications

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“…Recent computational studies have shown that SbSe antisite defects would occupy states at 0.4 eV above the valence band of Sb2Se3 and the suppresion of defect emission at energies close to 0.8 eV could imply the passivation of SbSe antisite defects upon sulfur treatment of Sb2Se3 films. [20] Low-frequency Raman spectroscopy (LFRS) can be used to probe the acoustic vibrational modes (AVM) of materials. Long-range order induces AVM enhancement thus revealing otherwise hidden LFRS modes.…”

Section: Resultsmentioning

confidence: 99%

Unravelling Defect Passivation Mechanisms in Sulfur-treated Sb2Se3

Prabhakar¹,

Moehl²,

Friedrich³

et al. 2021

Preprint

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Sb2Se3 has emerged as an important photoelectrochemical (PEC) and photovoltaic (PV) material due to its rapid rise in photoconversion efficiencies. However, despite its binary nature, Sb2Se3 has a complex defect chemistry, which reduces the maximum photovoltage that can be obtained. Thus, it is important to understand these defects and to develop passivation strategies in order to further improve this material. In this work, a comprehensive investigation of the charge carrier dynamics of Sb2Se3 and the influence of sulfur treatment on its optoelectronic properties was performed using time resolved microwave conductivity (TRMC), photoluminescence (PL) spectroscopy and low frequency Raman spectroscopy (LFRS). The key finding in this work is that upon sulfur treatment of Sb2Se3, the carrier lifetime is increased by the passivation of deep defects in Sb2Se3 in both the surface region and the bulk, which is evidenced by increased charge carrier lifetime of TRMC decay dynamics, increased radiative recombination efficiency and decreased deep defect level emission (PL), and improved long-range order in the material (LFRS). These findings provide crucial insights into the defect passivation mechanisms in Sb2Se3 paving the way for developing highly efficient PEC and PV devices.

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Section: Resultsmentioning

confidence: 99%

Unravelling Defect Passivation Mechanisms in Sulfur-treated Sb2Se3

Prabhakar¹,

Moehl²,

Friedrich³

et al. 2021

Preprint

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“…Then, the calculation of Sb 2 (S,Se) 3 was based on the GGA‐1/4 exchange‐correlation functional . We used the original cell of Sb 2 Se 3 for calculation and replaced one Se atom with one S atom based on the minimum energy principle …”

Section: Methodsmentioning

confidence: 99%

Over 7% Efficiency of Sb₂(S,Se)₃ Solar Cells via V‐Shaped Bandgap Engineering

et al. 2020

Solar RRL

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Antimony chalcogenides (including Sb2S3, Sb2Se3, and Sb2(S,Se)3 alloy) have emerged as promising solar absorber materials. Notably, the Sb2(S,Se)3 alloy possesses continuously tunable bandgap from 1.1 to 1.7 eV, which covers the ideal bandgap for single‐junction photovoltaics governed by the Shockley–Queisser theory. Moreover, the bandgap gradient provides effective ways for photogenerated carriers collection and has the potential for high‐efficient Sb2(S,Se)3 alloy solar cells. Herein, a V‐shaped distributional bandgap in Sb2(S,Se)3 solar cells is reported through a simple dual‐source vapor transport deposition process, enabling the synergetic increase of the open‐circuit voltage (VOC) and short‐circuit current (JSC). Through careful optimization, a power conversion efficiency of 7.27% under AM1.5G illumination is obtained, with VOC and JSC of 0.46 V and 29.6 mA cm−2, respectively. This V‐shaped bandgap engineering provides an effective method to enhance the device performance and can be extended to other chalcogenide thin‐film solar cells such as Sn–X, Ge–X, Cu–Sb–X (X = S and Se), and so on.

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“…[ 26 ] Effective mass of electrons in Sb 2 Se 3 is reported to be

m_{normale}^{*}

= 0.67 m 0 and the effective mass of holes in the upper valence bands A and B is

m_{normalh}^{*}

= 3.32 m 0 and

m_{normalh}^{*}

= 3.83 m 0 , respectively. [ 20 ] However, different values of electron and hole effective masses were also reported:

m_{normale}^{*}

= 0.365 m 0 and

m_{normalh}^{*}

= 0.316 m 0 ; [ 27 ]

m_{normale}^{*}

= 0.42 m 0 and

m_{normalh}^{*}

= 0.31 m 0 . [ 28 ] These values give the free exciton binding energy in the range of E bA = 4–9 meV and the exciton radius is about 7 nm.…”

Section: Excitons and Biexcitonsmentioning

confidence: 99%

Identification of Excitons and Biexcitons in Sb₂Se₃ under High Photoluminescence Excitation Density

Krustok

Kondrotas

Nedzinskas

et al. 2021

Advanced Optical Materials

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abundant and low-cost elements like Cu, Zn, Sn, S, and Se, are also potential candidates for next-generation PV technologies. [3,4] However, kesterites have turned out to be very challenging on their way toward highly efficient thin film PV due to strong recombination of photogenerated charge carriers via various routes leading to short minority carrier lifetime (i.e., magnitude lower than in CIGS, CdTe, etc.) and diffusion length and resulting in large open circuit voltage deficit of kesterite solar cells. [3,[5][6][7][8] It is, therefore, obvious that more research is required to find the alternative inexpensive and earth abundant materials for efficient thin-film solar cells. One of the promising absorber material candidates among the inorganic semiconductors being in the spotlight these days is antimony triselenide (Sb 2 Se 3 ). The efficiencies of the corresponding thin-film solar cells have already boosted to 9.2% in a very short time. [9][10][11] Quasi-1D antimony triselenide belongs to a family of inorganic binary A V -B VI compounds and indeed has very attractive properties, such as proper optical bandgap (1.1-1.2 eV) for a solar absorber, a single phase structure, high light absorption coefficient (10 5 cm −1 ), low toxicity, and high element abundance. [12] It was shown that due to the very high absorption coefficient the photons with wavelengths λ > 800 nm are completely absorbed within the first 400 nm of Sb 2 Se 3 film, enabling much thinner absorber layers compared to the usual thin film solar cells. [13] Despite extensive research there are still problems related to various point defects or electronic band structure of this compound. Capacitance spectro scopy studies have shown the presence of various deep donor and acceptor defects. [14,15] Defect states in polycrystalline Sb 2 Se 3 have been studied also using temperature and laser intensity-dependent photoluminescence (PL). [16] The low-temperature (T = 10 K) PL spectrum was consisted of three bands at 0.94, 1.10, and 1.24 eV. The PL bands at 1.24 and 0.94 eV were found to originate from the distant and close donor-acceptor pair recombination, respectively, and the third PL band at 1.10 eV was proposed to be related to the grain boundaries. Recent theoretical calculations showed that the defect chemistry of quasi-1D Sb 2 Se 3 is rather complicated compared to conventional semiconductors. In particular, it has been discussed that the identical defects located on nonequivalent atomic sites might have different properties. [17] All kinds of defect studies are therefore extremely important as usually defects act as powerful recombination channels and reduce the performance of the solar cell.The near-band-edge emission of Sb 2 Se 3 microcrystals is studied in detail under high photoluminescence excitation density using a pulsed UV laser (λ = 266 nm, pulse width 0.6 ns). Based on the peak energy positions and the excitation power density and temperature dependencies (T = 3-110 K) of the photoluminescence spectra, the emission is interpreted as a reco...

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Deciphering the Role of Key Defects in Sb₂Se₃, a Promising Candidate for Chalcogenide-Based Solar Cells

Abstract: Herein we report a thorough investigation on Sb 2 Se 3, a promising absorber material for photovoltaic applications, using state of the art quantum methods to understand the impact of defects on its electrical properties. The results show that despite a rather small

Cited by 62 publications

References 38 publications

Unravelling Defect Passivation Mechanisms in Sulfur-treated Sb2Se3

Unravelling Defect Passivation Mechanisms in Sulfur-treated Sb2Se3

Over 7% Efficiency of Sb₂(S,Se)₃ Solar Cells via V‐Shaped Bandgap Engineering

Identification of Excitons and Biexcitons in Sb₂Se₃ under High Photoluminescence Excitation Density

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Deciphering the Role of Key Defects in Sb2Se3, a Promising Candidate for Chalcogenide-Based Solar Cells

Abstract: Herein we report a thorough investigation on Sb 2 Se 3, a promising absorber material for photovoltaic applications, using state of the art quantum methods to understand the impact of defects on its electrical properties. The results show that despite a rather small

Cited by 62 publications

References 38 publications

Unravelling Defect Passivation Mechanisms in Sulfur-treated Sb2Se3

Unravelling Defect Passivation Mechanisms in Sulfur-treated Sb2Se3

Over 7% Efficiency of Sb2(S,Se)3 Solar Cells via V‐Shaped Bandgap Engineering

Identification of Excitons and Biexcitons in Sb2Se3 under High Photoluminescence Excitation Density

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Deciphering the Role of Key Defects in Sb₂Se₃, a Promising Candidate for Chalcogenide-Based Solar Cells

Over 7% Efficiency of Sb₂(S,Se)₃ Solar Cells via V‐Shaped Bandgap Engineering

Identification of Excitons and Biexcitons in Sb₂Se₃ under High Photoluminescence Excitation Density