Antimony selenide (Sb 2 Se 3) is an emerging chalcogenide photovoltaic absorber material that has been the subject of increasing interest in recent years, demonstrating rapid efficiency increases with a material that is simple, abundant, and stable. This paper examines the material from both a theoretical and practical standpoint. The theoretical viability of Sb 2 Se 3 as a solar photovoltaic material is assessed and the maximum spectroscopically limited performance is estimated, with a 200 nm film expected to be capable of achieving a photon conversion efficiency of up to 28.2%. By adapting an existing CdTe close-spaced sublimation (CSS) process, Sb 2 Se 3 material with large rhubarb-like grains is produced and solar cells are fabricated. We show that the established CdS window layer is unsuitable for use with CSS, due to intermixing during higher temperature processing. Substituting CdS with the more stable TiO 2 , a power conversion efficiency of 5.5% and an open-circuit voltage V o c of 0.45 V are achieved; the voltage exceeding current champion devices. This paper demonstrates the potential of CSS for scalable Sb 2 Se 3 deposition and highlights the Manuscript

The carrier-type of the emerging photovoltaic Sb2Se3 was evaluated for both thin films and bulk crystals via a range of complementary techniques. X-ray photoelectron spectroscopy (XPS), hot probe, Hall effect, and surface photovoltage spectroscopy showed films and crystals synthesized from the Sb2Se3 granulate material to be n-type with chlorine identified as an unintentional n-type dopant via secondary ion mass spectrometry analysis. The validity of chlorine as a dopant was confirmed by the synthesis of intrinsic crystals from metallic precursors and subsequent deliberate n-type doping by the addition of MgCl2. Chlorine was also shown to be a substitutional n-type shallow dopant by density functional theory calculations. TiO2/Sb2Se3 n–n isotype heterojunction solar cells with 7.3% efficiency are subsequently demonstrated, with band alignment analyzed via XPS.

Transparent conducting oxides (TCOs) are ubiquitous in modern consumer electronics. SnO2 is an earth abundant, cheaper alternative to In2O3 as a TCO. However, its performance in terms of mobilities and conductivities lags behind that of In2O3. On the basis of the recent discovery of mobility and conductivity enhancements in In2O3 from resonant dopants, we use a combination of state-of-the-art hybrid density functional theory calculations, high resolution photoelectron spectroscopy, and semiconductor statistics modeling to understand what is the optimal dopant to maximize performance of SnO2-based TCOs. We demonstrate that Ta is the optimal dopant for high performance SnO2, as it is a resonant dopant which is readily incorporated into SnO2 with the Ta 5d states sitting ∼1.4 eV above the conduction band minimum. Experimentally, the band edge electron effective mass of Ta doped SnO2 was shown to be 0.23m 0, compared to 0.29m 0 seen with conventional Sb doping, explaining its ability to yield higher mobilities and conductivities.

The presence of a lone pair of 5s electrons at the valence band maximum (VBM) of Sb2Se3 and the resulting band alignments are investigated using soft and hard x-ray photoemission...

Sb2Se3 is a promising material for use in photovoltaics, but the optimum device structure has not yet been identified. This study provides band alignment measurements between Sb2Se3, identical to that used in high-efficiency photovoltaic devices, and its two most commonly used window layers, namely, CdS and TiO2. Band alignments are measured via two different approaches: Anderson’s rule was used to predict an interface band alignment from measured natural band alignments, and the Kraut method was used in conjunction with hard X-ray photoemission spectroscopy to directly measure the band offsets at the interface. This allows examination of the effect of interface formation on the band alignments. The conduction band minimum (CBM) of TiO2 is found by the Kraut method to lie 0.82 eV below that of Sb2Se3, whereas the CdS CBM is only 0.01 eV below that of Sb2Se3. Furthermore, a significant difference is observed between the natural alignment- and Kraut method-determined offsets for TiO2/Sb2Se3, whereas there is little difference for CdS/Sb2Se3. Finally, these results are related to device performance, taking into consideration how these results may guide the future development of Sb2Se3 solar cells and providing a methodology that can be used to assess band alignments in device-relevant systems.