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Ultrafast photo-induced phonon hardening due to Pauli blocking in MAPbI 3 single-crystal and polycrystalline perovskites
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Xia, Chelsea Q., Poncé, Samuel, Peng, Jiali, Ulatowski, Aleksander M., Patel, Jay B., Wright, Adam D., Milot, Rebecca L., Kraus, Hans, Lin, Qianqian, Herz, Laura M, Giustino, Feliciano and Johnston, Michael B (2021) Ultrafast photo-induced phonon hardening due to Pauli blocking in MAPbI 3 single-crystal and polycrystalline perovskites. Journal of Physics: Materials, 4 (4). 044017. doi:10.1088/2515-7639/ac22b9 ISSN 2515-7639.
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WRAP-ultrafast-photo-induced-phonon-hardening-due-Pauli-blocking-MAPbI-3-single-crystal-polycrystalline-perovskites-Milot-2021.pdf - Published Version - Requires a PDF viewer. Available under License Creative Commons Attribution 4.0. Download (975Kb) | Preview |
Official URL: https://doi.org/10.1088/2515-7639/ac22b9
Abstract
Metal-halide perovskite semiconductors have attracted intense interest over the past decade, particularly for applications in photovoltaics. Low-energy optical phonons combined with significant crystal anharmonicity play an important role in charge-carrier cooling and scattering in these materials, strongly affecting their optoelectronic properties. We have observed optical phonons associated with Pb–I stretching in both MAPbI3 single crystals and polycrystalline thin films as a function of temperature by measuring their terahertz conductivity spectra with and without photoexcitation. An anomalous bond hardening was observed under above-bandgap illumination for both single-crystal and polycrystalline MAPbI3. First-principles calculations reproduced this photo-induced bond hardening and identified a related lattice contraction (photostriction), with the mechanism revealed as Pauli blocking. For single-crystal MAPbI3, phonon lifetimes were significantly longer and phonon frequencies shifted less with temperature, compared with polycrystalline MAPbI3. We attribute these differences to increased crystalline disorder, associated with grain boundaries and strain in the polycrystalline MAPbI3. Thus we provide fundamental insight into the photoexcitation and electron–phonon coupling in MAPbI3.
| Item Type: | Journal Article | ||||||||||||||||||
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| Subjects: | Q Science > QD Chemistry | ||||||||||||||||||
| Divisions: | Faculty of Science, Engineering and Medicine > Science > Physics | ||||||||||||||||||
| SWORD Depositor: | Library Publications Router | ||||||||||||||||||
| Library of Congress Subject Headings (LCSH): | Metal halides, Perovskite (Mineral), Semiconductors, Photovoltaic power generation, Optoelectronic devices, Photonics | ||||||||||||||||||
| Journal or Publication Title: | Journal of Physics: Materials | ||||||||||||||||||
| Publisher: | IOP Publishing | ||||||||||||||||||
| ISSN: | 2515-7639 | ||||||||||||||||||
| Official Date: | 22 September 2021 | ||||||||||||||||||
| Dates: |
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| Volume: | 4 | ||||||||||||||||||
| Number: | 4 | ||||||||||||||||||
| Article Number: | 044017 | ||||||||||||||||||
| DOI: | 10.1088/2515-7639/ac22b9 | ||||||||||||||||||
| Status: | Peer Reviewed | ||||||||||||||||||
| Publication Status: | Published | ||||||||||||||||||
| Access rights to Published version: | Open Access (Creative Commons) | ||||||||||||||||||
| Date of first compliant deposit: | 27 October 2021 | ||||||||||||||||||
| Date of first compliant Open Access: | 27 October 2021 | ||||||||||||||||||
| RIOXX Funder/Project Grant: |
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