Photovoltaic & Optoelectronic Device Group

Abstract:

Silver-bismuth based semiconductors represent a promising new class of materials for optoelectronic applications because of their high stability, all-inorganic composition, and advantageous optoelectronic properties. In this study, charge-carrier dynamics and transport properties are investigated across five compositions along the AgBiI4–CuI solid solution line (stoichiometry Cu4x(AgBi)1−xI4). The presence of a close-packed iodide sublattice is found to provide a good backbone for general semiconducting properties across all of these materials, whose optoelectronic properties are found to improve markedly with increasing copper content, which enhances photoluminescence intensity and charge-carrier transport. Photoluminescence and photoexcitation-energy-dependent terahertz photoconductivity measurements reveal that this enhanced charge-carrier transport derives from reduced cation disorder and improved electronic connectivity owing to the presence of Cu+. Further, increased Cu+ content enhances the band curvature around the valence band maximum, resulting in lower charge-carrier effective masses, reduced exciton binding energies, and higher mobilities. Finally, ultrafast charge-carrier localization is observed upon pulsed photoexcitation across all compositions investigated, lowering the charge-carrier mobility and leading to Langevin-like bimolecular recombination. This process is concluded to be intrinsically linked to the presence of silver and bismuth, and strategies to tailor or mitigate the effect are proposed and discussed.

Abstract:

The use of highly-active and robust catalysts is crucial for producing green hydrogen by water electrolysis as we strive to achieve global carbon neutrality. Noble metals like platinum are currently used catalysts in industry for the hydrogen evolution, but suffer from scarcity, high price and unsatisfied performance and stability at large current density, restrict their large-scale implementations. Here we report the synthesis of a type of monolith catalyst consisting of a metal disulfide (e.g., tantalum sulfides) vertically bonded to a conductive substrate of the same metal tantalum by strong covalent bonds. These features give the monolith catalyst a mechanically-robust and electrically near-zero-resistance interface, leading to an excellent hydrogen evolution performance including rapid charge transfer and excellent durability, together with a low overpotential of 398 mV to achieve a current density of 2,000 mA cm^-2 as required by industry. The monolith catalyst has a negligible performance decay after 200 h operation at large current densities. In light of its robust and metallic interface and the various choices of metals giving the same structure, such monolith materials would have broad uses besides catalysis.

Abstract:

Metal halide perovskite nanocrystal (PNC) light-emitting devices (LEDs) are promising in the future ultra-high-definition display applications due to their tunable bandgap and high color purity. Balanced carrier injection is indispensable for realizing highly efficient LEDs. Herein, cobalt (Co) was doped into ZnO to modulate the electron mobility of a pristine electron transport layer (ETL) and to inhibit exciton quenching at the ZnO/EML interface due to the passivation of oxygen vacancies and the reduction of electron concentration resulting from the trapping of electrons by the Co²⁺-induced deep impurity level. Also, the bandgap was widened due to the size confinement effect. All of those were beneficial to achieve a balanced charge injection during the operating process. Consequently, the maximum luminance increased from 867 cd m^-2 for ZnO LEDs to 1858 cd m^-2 for Co-doped ZnO LEDs, and there was a 70% increase of external quantum efficiency (EQE). By further inserting a polyethylenimine (PEI) layer in the Co-doped ZnO LEDs, the EQE reached 13.0%.