Molecular Additives Improve the Selectivity of CO2 Photoelectrochemical Reduction over Gold Nanoparticles on Gallium Nitride.

Photoelectrochemical CO2 reduction (CO2R) is an appealing solution for converting carbon dioxide into higher-value products. However, CO2R in aqueous electrolytes suffers from poor selectivity due to the competitive hydrogen evolution reaction that is dominant on semiconductor surfaces in aqueous electrolytes. We demonstrate that functionalizing gold/p-type gallium nitride devices with a film derived from diphenyliodonium triflate suppresses hydrogen generation from 90% to 18%. As a result, we observe increases in the Faradaic efficiency and partial current density for carbon monoxide of 50% and 3-fold, respectively. Furthermore, we demonstrate through optical absorption measurements that the molecular film employed herein, regardless of thickness, does not affect the photocathode's light absorption. Altogether, this study provides a rigorous platform for elucidating the catalytic structure-property relationships to enable engineering of active, stable, and selective materials for photoelectrochemical CO2R.

Silicon Heterojunction Microcells.

We report the design, fabrication, and characterization of silicon heterojunction microcells, a new type of photovoltaic cell that leverages high-efficiency bulk wafers in a microscale form factor, while also addressing the challenge of passivating microcell sidewalls to mitigate carrier recombination. We present synthesis methods exploiting either dry etching or laser cutting to realize microcells with native oxide-based edge passivation. Measured microcell performance for both fabrication processes is compared to that in simulations. We characterize the dependence of microcell open-circuit voltage (Voc) on the cell area-perimeter ratio and examine synthesis processes that affect edge passivation quality, such as sidewall damage removal, the passivation material, and the deposition technique. We report the highest Si microcell Voc to date (588 mV, for a 400 µm × 400 µm × 80 µm device), demonstrate Voc improvements with deposited edge passivation of up to 55 mV, and outline a pathway to achieve microcell efficiencies surpassing 15% for such device sizes.

A new metal transfer process for van der Waals contacts to vertical Schottky-junction transition metal dichalcogenide photovoltaics.

Two-dimensional transition metal dichalcogenides are promising candidates for ultrathin optoelectronic devices due to their high absorption coefficients and intrinsically passivated surfaces. To maintain these near-perfect surfaces, recent research has focused on fabricating contacts that limit Fermi-level pinning at the metal-semiconductor interface. Here, we develop a new, simple procedure for transferring metal contacts that does not require aligned lithography. Using this technique, we fabricate vertical Schottky-junction WS2 solar cells, with Ag and Au as asymmetric work function contacts. Under laser illumination, we observe rectifying behavior and open-circuit voltage above 500 mV in devices with transferred contacts, in contrast to resistive behavior and open-circuit voltage below 15 mV in devices with evaporated contacts. One-sun measurements and device simulation results indicate that this metal transfer process could enable high specific power vertical Schottky-junction transition metal dichalcogenide photovoltaics, and we anticipate that this technique will lead to advances for two-dimensional devices more broadly.