GeSe photovoltaics: doping, interfacial layer and devices.

Germanium selenide (GeSe) bulk crystals, thin films and solar cells are investigated with a focus on acceptor-doping with silver (Ag) and the use of an Sb2Se3 interfacial layer. The Ag-doping of GeSe occurred by a stoichiometric melt growth technique that created Ag-doped GeSe bulk crystals. A combination of capacitance voltage measurements, synchrotron radiation photoemission spectroscopy and surface space-charge calculations indicates that Ag-doping increases the hole density from 5.2 × 1015 cm-3 to 1.9 × 1016 cm-3. The melt-grown material is used as the source for thermally evaporated GeSe films within solar cells. The cell structure with the highest efficiency of 0.260% is FTO/CdS/Sb2Se3/undoped-GeSe/Au, compared with solar cells without the Sb2Se3 interfacial layer or with the Ag-doped GeSe.

Impedance spectroscopy of Sb2Se3 photovoltaics consisting of (Sb4Se6)n nanoribbons under light illumination.

Sb2Se3, consisting of one-dimensional (Sb4Se6)n nanoribbons has drawn attention as an intriguing light absorber from the photovoltaics (PVs) research community. However, further research is required on the performance-limiting factors in Sb2Se3 PVs. In this study, we investigated the charge carrier behavior in Sb2Se3 PVs by impedance spectroscopy (IS) under light illumination. (Sb4Se6)n nanoribbons with two different orientations were used to investigate the effect of crystal orientation on the device performance. Regardless of the (Sb4Se6)n orientation, negative capacitance was observed at forward bias, representing a recombination pathway at the TiO2/Sb2Se3 interface. A comparison of the recombination resistances and lifetimes of two different Sb2Se3 PVs showed that a better interface could be formed by placing the (Sb4Se6)n ribbons parallel to the TiO2 layer. Based on these observations, an ideal structure of the Sb2Se3/TiO2 interface is proposed, which will enhance the performance of Sb2Se3 PVs toward its theoretical limit.

Hybrid photocathode based on a Ni molecular catalyst and Sb2Se3 for solar H2 production.

We report a H2 evolving hybrid photocathode based on Sb2Se3 and a precious metal free molecular catalyst. Through the use of a high surface area TiO2 scaffold, we successfully increased the Ni molecular catalyst loading from 7.08 ± 0.43 to 45.76 ± 0.81 nmol cm-2, achieving photocurrents of 1.3 mA cm-2 at 0 V vs. RHE, which is 81-fold higher than the device without the TiO2 mesoporous layer.

Interrelation of the CdTe Grain Size, Postgrowth Processing, and Window Layer Selection on Solar Cell Performance.

Recent improvements to the CdTe solar cell device structure have focused on replacing the CdS window layer with a more transparent material to reduce parasitic absorption and increase Jsc, as well as incorporating selenium into the absorber layer to achieve a graded band gap. However, altering the CdTe device structure is nontrivial due to the interdependent nature of device processing steps. The choice of the window layer influences the grain structure of the CdTe layer, which in turn can affect the chloride treatment, which itself may contribute to intermixing between the window and absorber layers. This work studies three different device architectures in parallel, allowing for an in-depth comparison of processing conditions for CdTe solar cells grown on CdS, SnO2, and CdSe. Direct replacement of the CdS window layer with a wider band gap SnO2 layer is hindered by poor growth of the absorber, producing highly strained CdTe films and a weak junction. This is alleviated by inserting a CdSe layer between the SnO2 and CdTe, which improves the growth of CdTe and results in a graded CdSexTe1-x absorber layer. For each substrate, the CdTe deposition rate and postgrowth chloride treatment are systematically varied, highlighting the distinct processing requirements of each device structure.

GeSe: Optical Spectroscopy and Theoretical Study of a van der Waals Solar Absorber.

The van der Waals material GeSe is a potential solar absorber, but its optoelectronic properties are not yet fully understood. Here, through a combined theoretical and experimental approach, the optoelectronic and structural properties of GeSe are determined. A fundamental absorption onset of 1.30 eV is found at room temperature, close to the optimum value according to the Shockley-Queisser detailed balance limit, in contrast to previous reports of an indirect fundamental transition of 1.10 eV. The measured absorption spectra and first-principles joint density of states are mutually consistent, both exhibiting an additional distinct onset ∼0.3 eV above the fundamental absorption edge. The band gap values obtained from first-principles calculations converge, as the level of theory and corresponding computational cost increases, to 1.33 eV from the quasiparticle self-consistent GW method, including the solution to the Bethe-Salpeter equation. This agrees with the 0 K value determined from temperature-dependent optical absorption measurements. Relaxed structures based on hybrid functionals reveal a direct fundamental transition in contrast to previous reports. The optoelectronic properties of GeSe are resolved with the system described as a direct semiconductor with a 1.30 eV room temperature band gap. The high level of agreement between experiment and theory encourages the application of this computational methodology to other van der Waals materials.