Cs2InAgCl6: A New Lead-Free Halide Double Perovskite with Direct Band Gap.

J Phys Chem Lett (2017) 772-778

Authors:

G Volonakis, AA Haghighirad, RL Milot, WH Sio, MR Filip, B Wenger, MB Johnston, LM Herz, HJ Snaith, F Giustino

Abstract:

A2BB'X6 halide double perovskites based on bismuth and silver have recently been proposed as potential environmentally friendly alternatives to lead-based hybrid halide perovskites. In particular, Cs2BiAgX6 (X = Cl, Br) have been synthesized and found to exhibit band gaps in the visible range. However, the band gaps of these compounds are indirect, which is not ideal for applications in thin film photovoltaics. Here, we propose a new class of halide double perovskites, where the B(3+) and B(+) cations are In(3+) and Ag(+), respectively. Our first-principles calculations indicate that the hypothetical compounds Cs2InAgX6 (X = Cl, Br, I) should exhibit direct band gaps between the visible (I) and the ultraviolet (Cl). Based on these predictions, we attempt to synthesize Cs2InAgCl6 and Cs2InAgBr6, and we succeed to form the hitherto unknown double perovskite Cs2InAgCl6. X-ray diffraction yields a double perovskite structure with space group Fm3̅m. The measured band gap is 3.3 eV, and the compound is found to be photosensitive and turns reversibly from white to orange under ultraviolet illumination. We also perform an empirical analysis of the stability of Cs2InAgX6 and their mixed halides based on Goldschmidt's rules, and we find that it should also be possible to form Cs2InAg(Cl1-xBrx)6 for x < 1. The synthesis of mixed halides will open the way to the development of lead-free double perovskites with direct and tunable band gaps.

Photovoltaic mixed-cation lead mixed-halide perovskites: links between crystallinity, photo-stability and electronic properties

ENERGY & ENVIRONMENTAL SCIENCE 10:1 (2017) 361-369

Authors:

W Rehman, DP McMeekin, JB Patel, RL Milot, MB Johnston, HJ Snaith, LM Herz

Semiconductor Nanowires in Terahertz Photonics: From Spectroscopy to Ultrafast Nanowire-Based Devices

Institute of Electrical and Electronics Engineers (IEEE) (2017) 1-2

Authors:

Hannah J Joyce, Sarwat A Baig, Jennifer Wong-Leung, H Hoe Tan, C Jagadish, Jessica L Boland, Djamshid A Damry, Christopher L Davies, Laura M Herz, Michael B Johnston

Increased photoconductivity lifetimes in GaAs nanowires via n-type and p-type shell doping

41st International Conference on Infrared, Millimeter, and Terahertz waves (IRMMW-THz), 2016 IEEE 2016-November (2016)

Authors:

Jessica L Boland, A Casadei, G Tutuncouglu, F Matteini, C Davies, F Gaveen, F Amaduzzi, HJ Joyce, Laura M Herz, A Fontcuberta i Morral, Michael Johnston

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.

Perovskite-perovskite tandem photovoltaics with optimized band gaps.

Science 354:6314 (2016) 861-865

Authors:

GE Eperon, T Leijtens, KA Bush, R Prasanna, T Green, JT Wang, DP McMeekin, G Volonakis, RL Milot, R May, A Palmstrom, DJ Slotcavage, RA Belisle, JB Patel, ES Parrott, RJ Sutton, W Ma, F Moghadam, B Conings, A Babayigit, HG Boyen, S Bent, F Giustino, LM Herz, MB Johnston, MD McGehee, HJ Snaith

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.