Extending the defect tolerance of halide perovskite nanocrystals to hot carrier cooling dynamics

Junzhi Ye, Navendu Mondal (), Ben P. Carwithen, Yunwei Zhang, Linjie Dai, Xiang-Bing Fan, Jian Mao, Zhiqiang Cui, Pratyush Ghosh, Clara Otero‐Martínez, Lars Turnhout, Yi-Teng Huang, Zhongzheng Yu, Ziming Chen, Neil C. Greenham, Samuel D. Stranks, Lakshminarayana Polavarapu, Artem Bakulin, Akshay Rao and Robert L. Z. Hoye ()
Additional contact information
Junzhi Ye: University of Cambridge
Navendu Mondal: Imperial College London, Molecular Sciences Research Hub
Ben P. Carwithen: Imperial College London, Molecular Sciences Research Hub
Yunwei Zhang: Sun Yat-sen University
Linjie Dai: University of Cambridge
Xiang-Bing Fan: University of Cambridge, 9 JJ Thomson Avenue
Jian Mao: University of Cambridge
Zhiqiang Cui: Sun Yat-sen University
Pratyush Ghosh: University of Cambridge
Clara Otero‐Martínez: Campus Universitario As Lagoas, Marcosende
Lars Turnhout: University of Cambridge
Yi-Teng Huang: University of Oxford
Zhongzheng Yu: University of Cambridge
Ziming Chen: Imperial College London, Molecular Sciences Research Hub
Neil C. Greenham: University of Cambridge
Samuel D. Stranks: University of Cambridge
Lakshminarayana Polavarapu: Campus Universitario As Lagoas, Marcosende
Artem Bakulin: Imperial College London, Molecular Sciences Research Hub
Akshay Rao: University of Cambridge
Robert L. Z. Hoye: University of Oxford

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract Defect tolerance is a critical enabling factor for efficient lead-halide perovskite materials, but the current understanding is primarily on band-edge (cold) carriers, with significant debate over whether hot carriers can also exhibit defect tolerance. Here, this important gap in the field is addressed by investigating how intentionally-introduced traps affect hot carrier relaxation in CsPbX3 nanocrystals (X = Br, I, or mixture). Using femtosecond interband and intraband spectroscopy, along with energy-dependent photoluminescence measurements and kinetic modelling, it is found that hot carriers are not universally defect tolerant in CsPbX3, but are strongly correlated to the defect tolerance of cold carriers, requiring shallow traps to be present (as in CsPbI3). It is found that hot carriers are directly captured by traps, instead of going through an intermediate cold carrier, and deeper traps cause faster hot carrier cooling, reducing the effects of the hot phonon bottleneck and Auger reheating. This work provides important insights into how defects influence hot carriers, which will be important for designing materials for hot carrier solar cells, multiexciton generation, and optical gain media.

Date: 2024
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DOI: 10.1038/s41467-024-52377-4

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