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Coherent vibrational dynamics reveals lattice anharmonicity in organic-inorganic halide perovskite nanocrystals.

作者信息

Debnath Tushar, Sarker Debalaya, Huang He, Han Zhong-Kang, Dey Amrita, Polavarapu Lakshminarayana, Levchenko Sergey V, Feldmann Jochen

机构信息

Chair for Photonics and Optoelectronics, Nano-Institute Munich, Physics Department, Ludwig Maximilians-Universität (LMU), Munich, Germany.

Center for Energy Science and Technology, Skolkovo Institute of Science and Technology, Moscow, Russia.

出版信息

Nat Commun. 2021 May 11;12(1):2629. doi: 10.1038/s41467-021-22934-2.


DOI:10.1038/s41467-021-22934-2
PMID:33976185
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8113605/
Abstract

The halide ions of organic-inorganic hybrid perovskites can strongly influence the interaction between the central organic moiety and the inorganic metal halide octahedral units and thus their lattice vibrations. Here, we report the halide-ion-dependent vibrational coherences in formamidinium lead halide (FAPbX, X = Br, I) perovskite nanocrystals (PNCs) via the combination of femtosecond pump-probe spectroscopy and density functional theory calculations. We find that the FAPbX PNCs generate halide-dependent coherent vibronic wave packets upon above-bandgap non-resonant excitation. More importantly, we observe several higher harmonics of the fundamental modes for FAPbI PNCs as compared to FAPbBr PNCs. This is likely due to the weaker interaction between the central FA moiety and the inorganic cage for FAPbI PNCs, and thus the PbI unit can vibrate more freely. This weakening reveals the intrinsic anharmonicity in the Pb-I framework, and thus facilitating the energy transfer into overtone and combination bands. These findings not only unveil the superior stability of Br-based PNCs over I-based PNCs but are also important for a better understanding of their electronic and polaronic properties.

摘要
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/198024f5a5d3/41467_2021_22934_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/6180b7fc9114/41467_2021_22934_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/2c3858a65088/41467_2021_22934_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/1d10df751fa0/41467_2021_22934_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/198024f5a5d3/41467_2021_22934_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/6180b7fc9114/41467_2021_22934_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/2c3858a65088/41467_2021_22934_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/1d10df751fa0/41467_2021_22934_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a744/8113605/198024f5a5d3/41467_2021_22934_Fig4_HTML.jpg

相似文献

[1]
Coherent vibrational dynamics reveals lattice anharmonicity in organic-inorganic halide perovskite nanocrystals.

Nat Commun. 2021-5-11

[2]
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[3]
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[5]
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[6]
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[7]
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引用本文的文献

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[2]
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[3]
Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons.

Nat Phys. 2024

[4]
Uncovering the mechanisms of efficient upconversion in two-dimensional perovskites with anti-Stokes shift up to 220 meV.

Sci Adv. 2023-9-29

[5]
Synthesis of centimeter-size two-dimensional hybrid perovskite single crystals with tunable, pure, and stable luminescence.

RSC Adv. 2023-7-28

[6]
Carriers, Quasi-particles, and Collective Excitations in Halide Perovskites.

Chem Rev. 2023-7-12

[7]
Phonon-driven intra-exciton Rabi oscillations in CsPbBr halide perovskites.

Nat Commun. 2023-2-24

[8]
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[9]
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[10]
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本文引用的文献

[1]
Transfer of Direct to Indirect Bound Excitons by Electron Intervalley Scattering in CsAgBiBr Double Perovskite Nanocrystals.

ACS Nano. 2020-5-26

[2]
Comparing the excited-state properties of a mixed-cation-mixed-halide perovskite to methylammonium lead iodide.

J Chem Phys. 2020-3-14

[3]
Broadband Impulsive Stimulated Raman Scattering Based on a Chirped Detection.

J Phys Chem Lett. 2019-12-19

[4]
Ultrafast Charge Carrier Relaxation in Inorganic Halide Perovskite Single Crystals Probed by Two-Dimensional Electronic Spectroscopy.

J Phys Chem Lett. 2019-9-19

[5]
Polaron-Mediated Slow Carrier Cooling in a Type-1 3D/0D CsPbBr@CsPbBr Core-Shell Perovskite System.

J Phys Chem Lett. 2019-9-19

[6]
Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites.

Nat Mater. 2019-4

[7]
Vibrational Coupling between Organic and Inorganic Sublattices of Hybrid Perovskites.

Angew Chem Int Ed Engl. 2018-10-8

[8]
Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite.

Nat Commun. 2018-6-28

[9]
Probing femtosecond lattice displacement upon photo-carrier generation in lead halide perovskite.

Nat Commun. 2018-5-17

[10]
Investigating the Role of the Organic Cation in Formamidinium Lead Iodide Perovskite Using Ultrafast Spectroscopy.

J Phys Chem Lett. 2018-2-15

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