Resolving the controversy in biexciton binding energy of cesium lead halide perovskite nanocrystals through heralded single-particle spectroscopy
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arXiv
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| Format: | Preprint |
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2021
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| _version_ | 1866914193058299904 |
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| author | Lubin, Gur Yaniv, Gili Kazes, Miri Ulku, Arin Can Antolovic, Ivan Michel Burri, Samuel Bruschini, Claudio Charbon, Edoardo Yallapragada, Venkata Jayasurya Oron, Dan |
| author_facet | Lubin, Gur Yaniv, Gili Kazes, Miri Ulku, Arin Can Antolovic, Ivan Michel Burri, Samuel Bruschini, Claudio Charbon, Edoardo Yallapragada, Venkata Jayasurya Oron, Dan |
| contents | Understanding exciton-exciton interaction in multiply-excited nanocrystals is crucial to their utilization as functional materials. Yet, for lead halide perovskite nanocrystals, which are promising candidates for nanocrystal-based technologies, numerous contradicting values have been reported for the strength and sign of their exciton-exciton interaction. In this work we unambiguously determine the biexciton binding energy in single cesium lead halide perovskite nanocrystals at room temperature. This is enabled by the recently introduced SPAD array spectrometer, capable of temporally isolating biexciton-exciton emission cascades while retaining spectral resolution. We demonstrate that CsPbBr$_3$ nanocrystals feature an attractive exciton-exciton interaction, with a mean biexciton binding energy of 10 meV. For CsPbI$_3$ nanocrystals we observe a mean biexciton binding energy that is close to zero, and individual nanocrystals show either weakly attractive or weakly repulsive exciton-exciton interaction. We further show that within ensembles of both materials, single-nanocrystal biexciton binding energies are correlated with the degree of charge-carrier confinement. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2108_00347 |
| institution | arXiv |
| publishDate | 2021 |
| record_format | arxiv |
| spellingShingle | Resolving the controversy in biexciton binding energy of cesium lead halide perovskite nanocrystals through heralded single-particle spectroscopy Lubin, Gur Yaniv, Gili Kazes, Miri Ulku, Arin Can Antolovic, Ivan Michel Burri, Samuel Bruschini, Claudio Charbon, Edoardo Yallapragada, Venkata Jayasurya Oron, Dan Mesoscale and Nanoscale Physics Chemical Physics Optics Quantum Physics Understanding exciton-exciton interaction in multiply-excited nanocrystals is crucial to their utilization as functional materials. Yet, for lead halide perovskite nanocrystals, which are promising candidates for nanocrystal-based technologies, numerous contradicting values have been reported for the strength and sign of their exciton-exciton interaction. In this work we unambiguously determine the biexciton binding energy in single cesium lead halide perovskite nanocrystals at room temperature. This is enabled by the recently introduced SPAD array spectrometer, capable of temporally isolating biexciton-exciton emission cascades while retaining spectral resolution. We demonstrate that CsPbBr$_3$ nanocrystals feature an attractive exciton-exciton interaction, with a mean biexciton binding energy of 10 meV. For CsPbI$_3$ nanocrystals we observe a mean biexciton binding energy that is close to zero, and individual nanocrystals show either weakly attractive or weakly repulsive exciton-exciton interaction. We further show that within ensembles of both materials, single-nanocrystal biexciton binding energies are correlated with the degree of charge-carrier confinement. |
| title | Resolving the controversy in biexciton binding energy of cesium lead halide perovskite nanocrystals through heralded single-particle spectroscopy |
| topic | Mesoscale and Nanoscale Physics Chemical Physics Optics Quantum Physics |
| url | https://arxiv.org/abs/2108.00347 |