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Nanoscale chemical heterogeneity dominates the optoelectronic response of alloyed perovskite solar cells

Authors: Stuart Macpherson; Tiarnan Doherty; Jooyoung Sung; Jooyoung Sung; Kieran W. P. Orr; Kyle Frohna; Paul Quinn; +7 Authors

Nanoscale chemical heterogeneity dominates the optoelectronic response of alloyed perovskite solar cells

Abstract

Halide perovskites perform remarkably in optoelectronic devices including tandem photovoltaics. However, this exceptional performance is striking given that perovskites exhibit deep charge carrier traps and spatial compositional and structural heterogeneity, all of which should be detrimental to performance. Here, we resolve this long-standing paradox by providing a global visualisation of the nanoscale chemical, structural and optoelectronic landscape in halide perovskite devices, made possible through the development of a new suite of correlative, multimodal microscopy measurements combining quantitative optical spectroscopic techniques and synchrotron nanoprobe measurements. We show that compositional disorder dominates the optoelectronic response over a weaker influence of nanoscale strain variations even of large magnitude. Nanoscale compositional gradients drive carrier funneling onto local regions associated with low electronic disorder, drawing carrier recombination away from trap clusters associated with electronic disorder and leading to high local photoluminescence quantum efficiency. These measurements reveal a global picture of the competitive nanoscale landscape, which endows enhanced defect tolerance in devices through spatial chemical disorder that outcompetes both electronic and structural disorder.

Countries
United Kingdom, Korea (Republic of)
Keywords

34 Chemical Sciences, PHASE SEGREGATION, IMPACT, 500, Bioengineering, PERFORMANCE, LIMIT, 530, LUMINESCENCE, 3406 Physical Chemistry, LOSSES

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