Extending the defect tolerance of halide perovskite nanocrystals to hot carrier cooling dynamics
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 CsPbX<sub>3</sub> 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 CsPbX<sub>3</sub>, but are strongly correlated to the defect tolerance of cold carriers, requiring shallow traps to be present (as in CsPbI<sub>3</sub>). 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.
Authors
- Clara Otero‐Martínez (ORCID: https://orcid.org/0000-0002-2110-5632)
- Jian Mao (ORCID: https://orcid.org/0000-0001-8780-4252)
- Lakshminarayana Polavarapu (ORCID: https://orcid.org/0000-0002-9040-5719)
- Junzhi Ye (ORCID: https://orcid.org/0000-0001-8919-9236)
- Neil C. Greenham (ORCID: https://orcid.org/0000-0002-2155-2432)
- Lars van Turnhout (ORCID: https://orcid.org/0000-0002-5222-6250)
- Yi‐Teng Huang (ORCID: https://orcid.org/0000-0002-4576-2338)
- Zhiqiang Cui (ORCID: https://orcid.org/0000-0002-0769-8937)
- Robert L. Z. Hoye (ORCID: https://orcid.org/0000-0002-7675-0065)
- Zhongzheng Yu (ORCID: https://orcid.org/0000-0003-0941-3357)
- Ben P. Carwithen (ORCID: https://orcid.org/0000-0002-3140-1793)
- Navendu Mondal (ORCID: https://orcid.org/0000-0001-5002-9678)
- Artem A. Bakulin (ORCID: https://orcid.org/0000-0002-3998-2000)
- Xiang‐Bing Fan
- Linjie Dai (ORCID: https://orcid.org/0000-0002-1467-3041)
- Pratyush Ghosh (ORCID: https://orcid.org/0000-0001-5780-3718)
- Akshay Rao (ORCID: https://orcid.org/0000-0003-4261-0766)
- Samuel D. Stranks (ORCID: https://orcid.org/0000-0002-8303-7292)
- Ziming Chen (ORCID: https://orcid.org/0000-0001-5008-3498)
- Yunwei Zhang (ORCID: https://orcid.org/0000-0001-7856-9190)
Institutions
- Sun Yat-sen University (CN)
- University of Cambridge (GB)
- Fudan University (CN)
- University of Oxford (GB)
- Bridge University (SS)
- Imperial College London (GB)
- Universidade de Vigo (ES)
Publication Details
- Journal
- Nature Communications
- Published
- 2024-09-16
- DOI
- https://doi.org/10.1038/s41467-024-52377-4
- Citations
- 50
- Primary Topic
- Perovskite Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 10.43
Funders
- Cambridge Philosophical Society
- UK Research and Innovation
- Leverhulme Trust
- Royal Academy of Engineering
- European Commission
- National Natural Science Foundation of China
- Sun Yat-sen University
- China Scholarship Council
- Ministerio de Ciencia e Innovación
- Tata Sons
- Xunta de Galicia
- Horizon 2020 Framework Programme
- HORIZON EUROPE Framework Programme
- Engineering and Physical Sciences Research Council
- Agencia Estatal de Investigación
- Fundamental Research Funds for the Central Universities
- Basic and Applied Basic Research Foundation of Guangdong Province
- H2020 Marie Skłodowska-Curie Actions