Two dimensional inorganic–organic hybrid perovskites (2D perovskites) suffer from not only quantum confinement, but also dielectric confinement, hindering their application perspective in devices involving the conversion of an optical input into current. In this report, we theoretically predict that an extremely low exciton binding energy can be achieved in 2D perovskites by using high dielectric-constant organic components. We demonstrate that in (HOCH2CH2NH3)2PbI4, whose organic material has a high dielectric constant of 37, the dielectric confinement is largely reduced, and the exciton binding energy is 20-times smaller than that in conventional 2D perovskites. As a result, the photo-induced excitons can be thermally dissociated efficiently at room temperature, as clearly indicated from femtosecond transient absorption measurements. In addition, the mobility is largely improved due to the strong screening effect on charge impurities. Such low dielectric-confined 2D perovskites show excellent carrier extraction efficiency, and outstanding humidity resistance compared to conventional 2D perovskites.

Hydrogen production via photoelectrochemical water-splitting is a key source of clean and sustainable energy. The use of one-dimensional nanostructures as photoelectrodes is desirable for photoelectrochemical water-splitting applications due to the ultralarge surface areas, lateral carrier extraction schemes, and superior light-harvesting capabilities. However, the unavoidable surface states of nanostructured materials create additional charge carrier trapping centers and energy barriers at the semiconductor-electrolyte interface, which severely reduce the solar-to-hydrogen conversion efficiency. In this work, we address the issue of surface states in GaN nanowire photoelectrodes by employing a simple and low-cost surface treatment method, which utilizes an organic thiol compound (i.e., 1,2-ethanedithiol). The surface-treated photocathode showed an enhanced photocurrent density of -31 mA/cm at -0.2 V versus RHE with an incident photon-to-current conversion efficiency of 18.3%, whereas untreated nanowires yielded only 8.1% efficiency. Furthermore, the surface passivation provides enhanced photoelectrochemical stability as surface-treated nanowires retained ∼80% of their initial photocurrent value and produced 8000 μmol of gas molecules over 55 h at acidic conditions (pH ∼ 0), whereas the untreated nanowires demonstrated only <4 h of photoelectrochemical stability. These findings shed new light on the importance of surface passivation of nanostructured photoelectrodes for photoelectrochemical applications.

Ajia I, et al. (2018) Highperformance solar-blind flexible deep-UV photodetectors based on quantum dots synthesized by femtosecond-laser ablation.

Understanding defect chemistry, particularly ion migration, and its significant effect on the surface's optical and electronic properties is one of the major challenges impeding the development of hybrid perovskite-based devices. Here, using both experimental and theoretical approaches, we demonstrated that the surface layers of the perovskite crystals may acquire a high concentration of positively charged vacancies with the complementary negatively charged halide ions pushed to the surface. This charge separation near the surface generates an electric field that can induce an increase of optical band gap in the surface layers relative to the bulk. We found that the charge separation, electric field, and the amplitude of shift in the bandgap strongly depend on the halides and organic moieties of perovskite crystals. Our findings reveal the peculiarity of surface effects that are currently limiting the applications of perovskite crystals and more importantly explain their origins, thus enabling viable surface passivation strategies to remediate them.

A droop-free nitride light-emitting diode (LED) with the capacity to operate beyond the "green gap" has been a subject of intense scientific and engineering interest. While several properties of nanowires on silicon make them promising for use in LED development, the high aspect ratio of individual nanowires and their laterally discontinuous features limit phonon transport and device performance. Here, we report on the monolithic integration of metal heat-sink and droop-free InGaN/GaN quantum-disks-in-nanowire LEDs emitting at ∼710 nm. The reliable operation of our uncooled nanowire-LEDs (NW-LEDs) epitaxially grown on molybdenum was evident in the constant-current soft burn-in performed on a 380 μm × 380 μm LED. The square LED sustained 600 mA electrical stress over an 8 h period, providing stable light output at maturity without catastrophic failure. The absence of carrier and phonon transport barriers in NW-LEDs was further inferred from current-dependent Raman measurements (up to 700 mA), which revealed the low self-heating. The radiative recombination rates of NW-LEDs between room temperature and 40 °C was not limited by Shockley-Read-Hall recombination, Auger recombination, or carrier leakage mechanisms, thus realizing droop-free operation. The discovery of reliable, droop-free devices constitutes significant progress toward the development of nanowires for practical applications. Our monolithic approach realized a high-performance device that will revolutionize the way high power, low-junction-temperature LED lamps are manufactured for solid-state lighting and for applications in high-temperature harsh environment.