Terahertz photonics

Abstract:

We have used optical-pump-terahertz-probe spectroscopy (OPTPS) to study a range of novel of semiconductors including III-V nanowires and metal halide perovskites. We show that OPTPs allows key figures of merit to be extracted in a non-contact manner, including charge mobility, surface recombination velocity, and doping density. Furthermore, the technique allows charge recombination dynamics to be followed on a picosecond time-scale. This knowledge is useful in the design of new optoelectronic devices from lasers to solar cells as well as for the development and optimisation of new semiconductors.

Abstract:

Reliable doping in GaAs nanowires is essential for the development of novel optoelectronic devices. Previously, GaAs nanowires have been shown to exhibit extremely short photoconductivity lifetimes of a few picoseconds due to their high surface recombination velocity, which is detrimental for nanowire devices, such as solar cells and nanowire lasers. Here, we show that, by exploiting engineered band-bending via selective doping, this parasitic surface recombination can be reduced. We utilise non-contact time-resolved terahertz spectroscopy to characterise the doping efficiency in n-type and p-type doped GaAs nanowire8 and show high carrier concentrations of the order of 1018 cm-3. The carrier lifetimes were increased by an order of magnitude from 0.13ns for undoped to 3.8ns and 2.5ns for n-doped and p-doped GaAs nanowires respectively; showing that surface recombination is greatly suppressed as a result of shell doping. We also present a novel effect of p-doping in GaAs nanowires: a rapid decay in photoconductivity within 25ps after photoexcitation. This fast decay is attributed to rapid electron trapping at the nanowire surface due to doping related band bending. Thus, we demonstrate the advantages of selective doping for enhancement of desirable transport properties in GaAs nanowires, as well as highlighting terahertz spectroscopy as a reliable technique for characterising doped GaAs nanowires1.

Abstract:

We demonstrate four- and two-terminal perovskite-perovskite tandem solar cells with ideally matched band gaps. We develop an infrared-absorbing 1.2-electron volt band-gap perovskite, FA0.75Cs0.25Sn0.5Pb0.5I3, that can deliver 14.8% efficiency. By combining this material with a wider-band gap FA0.83Cs0.17Pb(I0.5Br0.5)3 material, we achieve monolithic two-terminal tandem efficiencies of 17.0% with >1.65-volt open-circuit voltage. We also make mechanically stacked four-terminal tandem cells and obtain 20.3% efficiency. Notably, we find that our infrared-absorbing perovskite cells exhibit excellent thermal and atmospheric stability, not previously achieved for Sn-based perovskites. This device architecture and materials set will enable "all-perovskite" thin-film solar cells to reach the highest efficiencies in the long term at the lowest costs.

Abstract:

Hybrid metal-halide perovskites are promising new materials for use in solar cells; however, their chemical stability in the presence of moisture remains a significant drawback. Quasi two-dimensional (2D) perovskites that incorporate hydrophobic organic interlayers offer improved resistance to degradation by moisture, currently still at the cost of overall cell efficiency. To elucidate the factors affecting the optoelectronic properties of these materials, we have investigated the charge transport properties and crystallographic orientation of mixed methylammonium (MA)-phenylethylammonium (PEA) lead iodide thin films as a function of the MA-to-PEA ratio and, thus, the thickness of the "encapsulated" MA lead-halide layers. We find that monomolecular charge-carrier recombination rates first decrease with increasing PEA fraction, most likely as a result of trap passivation, but then increase significantly as excitonic effects begin to dominate for thin confined layers. Bimolecular and Auger recombination rate constants are found to be sensitive to changes in electronic confinement, which alters the density of states for electronic transitions. We demonstrate that effective charge-carrier mobilities remain remarkably high (near 10 cm(2)V(-1)s(-1)) for intermediate PEA content and are enhanced for preferential orientation of the conducting lead iodide layers along the probing electric field. The trade-off between trap reduction, electronic confinement, and layer orientation leads to calculated charge-carrier diffusion lengths reaching a maximum of 2.5 μm for intermediate PEA content (50%).