Enhanced optoelectronic quality of metal halide perovskite via additive engineering
Mojtaba Abdi-Jalebi a, Zahra Andaji-Garmaroudi a, Stefania Cacovich b, Giorgio Divitini b, Samuel D. Stranks a, Richard H. Friend a
a Cavendish Laboratory, University of Cambridge - UK, JJ Thomson Avenue, 9, Cambridge, United Kingdom
b University of Cambridge, Department of Materials Science and Metallurgy, UK, Cambridge, United Kingdom
NIPHO
Proceedings of International Conference on Perovskite Thin Film Photovoltaics, Photonics and Optoelectronics (ABXPV18PEROPTO)
Perovskite Thin Film Photovoltaics (ABXPV18). 27-28 Feb
Rennes, France, 2018 February 27th - March 1st
Organizer: Jacky Even
Oral, Mojtaba Abdi-Jalebi, presentation 063
DOI: https://doi.org/10.29363/nanoge.abxpvperopto.2018.063
Publication date: 11th December 2017

Metal halide perovskites display remarkable intrinsic properties including high absorption coefficient, sharp and tunable bandedge, long charge carrier diffusion length, low trap densities, high luminescence quantum yields, and the photon recycling capability. These materials have shown a relatively fast evolution in the performance of both light emitting diodes and solar cells (e.g. power conversion efficiency (PCE) exceeding 22%) since their first appearance in the devices. However, non-radiative losses originating from sub gap charge carrier trap states on the grain surfaces (e.g. halide vacancies) and low luminescence efficiency of metal halide perovskite in a complete device are the main barriers against reaching the efficiency limit in both solar cells and LEDs.

Here, we explore the impact of doping with different cation additives on the optoelectronic quality and structural properties of metal halide perovskite. We find significant enhancement in both micro-photoluminescence and photoluminescence quantum efficiency (e.g. internal yields exceeding 95%) while maintaining high mobilities over 42 cm2V-1s-1, giving the elusive combination of both high luminescence and excellent charge transport. We also demonstrate the inhibition of transient photo-induced ion migration processes via decorating the grain boundaries and interfaces with self-assembly passivating species. We validate these enhancements in operating solar cells where we obtain a remarkable increase in PCE along with entire elimination of hysteresis upon addition of cation additives. We also analyse the local structural changes and the corresponding effects on the electronic structure and chemical bonding of metal-iodide in the additive based perovskite using periodic DFT calculations where the corresponding negative formation energies confirm the feasibility of formation of the doped structures.

Our findings pave the way for further improvements in the optoelectronic quality of metal halide perovskite thin films and subsequent devices. It also reveals promising approaches to eliminate non-radiative losses and maximize luminescence efficiency in metal halide perovskite. 

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