Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr$_3$ quantum dots
Fuente:
arXiv
Saved in:
| Main Authors: | , , , , , , , , , , , , , , , , , , , , , , , , , , , , , , |
|---|---|
| Format: | Preprint |
| Published: |
2025
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866917912475860992 |
|---|---|
| author | Shen, Zhou Samoli, Margarita Erdem, Onur Bielecki, Johan Samanta, Amit Kumar E, Juncheng Estillore, Armando Kim, Chan Kim, Yoonhee Koliyadu, Jayanath Letrun, Romain Locardi, Federico Lübke, Jannik Mall, Abhishek Melo, Diogo Mills, Grant Rafie-Zinedine, Safi Round, Adam Sato, Tokushi de Wijn, Raphael Wollweber, Tamme Worbs, Lena Zhuang, Yulong Mancuso, Adrian P. Bean, Richard Chapman, Henry N. Küpper, Jochen Infante, Ivan Lange, Holger Hens, Zeger Ayyer, Kartik |
| author_facet | Shen, Zhou Samoli, Margarita Erdem, Onur Bielecki, Johan Samanta, Amit Kumar E, Juncheng Estillore, Armando Kim, Chan Kim, Yoonhee Koliyadu, Jayanath Letrun, Romain Locardi, Federico Lübke, Jannik Mall, Abhishek Melo, Diogo Mills, Grant Rafie-Zinedine, Safi Round, Adam Sato, Tokushi de Wijn, Raphael Wollweber, Tamme Worbs, Lena Zhuang, Yulong Mancuso, Adrian P. Bean, Richard Chapman, Henry N. Küpper, Jochen Infante, Ivan Lange, Holger Hens, Zeger Ayyer, Kartik |
| contents | The outstanding opto-electronic properties of lead halide perovskites have been related to the formation of polarons. Nevertheless, the observation of the atomistic deformation brought about by one electron-hole pair in these materials has remained elusive. Here, we measure the diffraction patterns of single CsPbBr$_3$ quantum dots (QDs) with and without resonant excitation in the single exciton limit using serial femtosecond crystallography (SFX). By reconstructing the 3D differential diffraction pattern, we observe small shifts of the Bragg peaks indicative of a crystal-wide deformation field. Building on DFT calculations, we show that these shifts are consistent with the lattice distortion induced by a delocalized electron and a localized hole, forming a mixed large/small exciton polaron. This result creates a clear picture of the polaronic deformation in CsPbBr$_3$ QDs, highlights the exceptional sensitivity of SFX to lattice distortions in few-nanometer crystallites, and establishes an experimental platform for future studies of electron-lattice interactions. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2502_02343 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr$_3$ quantum dots Shen, Zhou Samoli, Margarita Erdem, Onur Bielecki, Johan Samanta, Amit Kumar E, Juncheng Estillore, Armando Kim, Chan Kim, Yoonhee Koliyadu, Jayanath Letrun, Romain Locardi, Federico Lübke, Jannik Mall, Abhishek Melo, Diogo Mills, Grant Rafie-Zinedine, Safi Round, Adam Sato, Tokushi de Wijn, Raphael Wollweber, Tamme Worbs, Lena Zhuang, Yulong Mancuso, Adrian P. Bean, Richard Chapman, Henry N. Küpper, Jochen Infante, Ivan Lange, Holger Hens, Zeger Ayyer, Kartik Materials Science Mesoscale and Nanoscale Physics Data Analysis, Statistics and Probability The outstanding opto-electronic properties of lead halide perovskites have been related to the formation of polarons. Nevertheless, the observation of the atomistic deformation brought about by one electron-hole pair in these materials has remained elusive. Here, we measure the diffraction patterns of single CsPbBr$_3$ quantum dots (QDs) with and without resonant excitation in the single exciton limit using serial femtosecond crystallography (SFX). By reconstructing the 3D differential diffraction pattern, we observe small shifts of the Bragg peaks indicative of a crystal-wide deformation field. Building on DFT calculations, we show that these shifts are consistent with the lattice distortion induced by a delocalized electron and a localized hole, forming a mixed large/small exciton polaron. This result creates a clear picture of the polaronic deformation in CsPbBr$_3$ QDs, highlights the exceptional sensitivity of SFX to lattice distortions in few-nanometer crystallites, and establishes an experimental platform for future studies of electron-lattice interactions. |
| title | Direct observation of the exciton polaron by serial femtosecond crystallography on single CsPbBr$_3$ quantum dots |
| topic | Materials Science Mesoscale and Nanoscale Physics Data Analysis, Statistics and Probability |
| url | https://arxiv.org/abs/2502.02343 |