Terahertz photonics

Abstract:

Metal halide perovskites are promising light absorbers for multijunction photovoltaic applications because of their remarkable bandgap tunability, achieved through compositional mixing on the halide site. However, poor energy-level alignment at the interface between wide-bandgap mixed-halide perovskites and charge-extraction layers still causes significant losses in solar-cell performance. Here, the origin of such losses is investigated, focusing on the energy-level misalignment between the valence band maximum and the highest occupied molecular orbital (HOMO) for a commonly employed combination, FA_0.83Cs_0.17Pb(I_1-xBr_x)₃ with bromide content x ranging from 0 to 1, and poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA). A combination of time-resolved photoluminescence spectroscopy and numerical modeling of charge-carrier dynamics reveals that open-circuit voltage (V_OC) losses associated with a rising energy-level misalignment derive from increasing accumulation of holes in the HOMO of PTAA, which then subsequently recombine non-radiatively across the interface via interfacial defects. Simulations assuming an ideal choice of hole-transport material to pair with FA_0.83Cs_0.17Pb(I_1-xBr_x)₃ show that such V_OC losses originating from energy-level misalignment can be reduced by up to 70 mV. These findings highlight the urgent need for tailored charge-extraction materials exhibiting improved energy-level alignment with wide-bandgap mixed-halide perovskites to enable solar cells with improved power conversion efficiencies.

Abstract:

Terahertz (THz) continuous wave (CW) spectroscopy systems can offer extremely high spectral resolution over the THz band by photo-mixing high-performance telecommunications-band (1530-1565 nm) lasers. However, typical THz CW detectors in these systems use narrow band-gap photoconductors, which require elaborate material growth and generate relatively large detector noise. Here we demonstrate that two-step photon absorption in a nano-structured low-temperature grown GaAs (LT-GaAs) metasurface which enables switching of photoconductivity within approximately one picosecond. We show that LT-GaAs can be used as an ultrafast photoconductor in CW THz detectors despite having a bandgap twice as large as the telecommunications laser photon energy. The metasurface design harnesses Mie modes in LT GaAs resonators, whereas metallic electrodes of THz detectors can be designed to support an additional photonic mode, which further increases photoconductivity at a desired wavelength.