Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons

Yazdani, Nuri; Bodnarchuk, Maryna I.; Bertolotti, Federica; Masciocchi, Norberto; Fureraj, Ina; Guzelturk, Burak; Cotts, Benjamin L.; Zajac, Marc; Rainò, Gabriele; Jansen, Maximilian; Boehme, Simon C.; Yarema, Maksym; Lin, Ming-Fu; Kozina, Michael; Reid, Alexander; Shen, Xiaozhe; Weathersby, Stephen; Wang, Xijie; Vauthey, Eric; Guagliardi, Antonietta; Kovalenko, Maksym V.; Wood, Vanessa; Lindenberg, Aaron M.

doi:10.1038/s41567-023-02253-7

Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons

Journal Article · Wed Nov 08 23:00:00 EST 2023 · Nature Physics

DOI:https://doi.org/10.1038/s41567-023-02253-7· OSTI ID:2280850

^[1]; ^[2]; ^[3]; ^[3]; ^[4]; ^[5]; ^[6]; ^[5]; ^[2]; ^[7]; ^[2]; ^[7]; ^[8]; Kozina, Michael ^[8]; ^[8]; ^[8]; Weathersby, Stephen ^[8]; ^[8]; ^[4]; ^[9] more »

Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES); Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); SLAC
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland); Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
Universita degli Studi dell'Insubria, Como (Italy)
Univ. of Geneva (Switzerland)
Argonne National Laboratory (ANL), Argonne, IL (United States)
Stanford Univ., CA (United States); Middlebury College, VT (United States)
Eidgenoessische Technische Hochschule (ETH), Zurich (Switzerland)
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Consiglio Nazionale delle Ricerche (CNR), Como (Italy)
Stanford Univ., CA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Institute for Materials and Energy Science (SIMES) and Photon Ultrafast Laser Science and Engineering Institute (PULSE)

Understanding the origin of electron–phonon coupling in lead halide perovskites is key to interpreting and leveraging their optical and electronic properties. Here we show that photoexcitation drives a reduction of the lead–halide–lead bond angles, a result of deformation potential coupling to low-energy optical phonons. We accomplish this by performing femtosecond-resolved, optical-pump–electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in nanocrystals of FAPbBr₃. Our results indicate a stronger coupling in FAPbBr₃ than CsPbBr₃. We attribute the enhanced coupling in FAPbBr₃ to its disordered crystal structure, which persists down to cryogenic temperatures. We find the reorganizations induced by each exciton in a multi-excitonic state constructively interfere, giving rise to a coupling strength that scales quadratically with the exciton number. This superlinear scaling induces phonon-mediated attractive interactions between excitations in lead halide perovskites.

View Accepted Manuscript (DOE)

Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231; SC0019140

OSTI ID:: 2280850

Journal Information:: Nature Physics, Journal Name: Nature Physics Journal Issue: 1 Vol. 20; ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)Copyright Statement

Country of Publication:: United States

Language:: English

References (67)

Intraband Cooling in All‐Inorganic and Hybrid Organic–Inorganic Perovskite Nanocrystals Diroll, Benjamin T.; Schaller, Richard D. Advanced Functional Materials, Vol. 29, Issue 37 https://doi.org/10.1002/adfm.201901725	journal	July 2019
Nonequilibrium Lattice Dynamics in Photoexcited 2D Perovskites Cuthriell, Shelby A.; Panuganti, Shobhana; Laing, Craig C. Advanced Materials, Vol. 34, Issue 44 https://doi.org/10.1002/adma.202202709	journal	October 2022
Efficiency of ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set Kresse, G.; Furthmüller, J. Computational Materials Science, Vol. 6, Issue 1, p. 15-50 https://doi.org/10.1016/0927-0256(96)00008-0	journal	July 1996
Metal Halide Perovskites in Quantum Dot Solar Cells: Progress and Prospects Yuan, Jianyu; Hazarika, Abhijit; Zhao, Qian Joule, Vol. 4, Issue 6 https://doi.org/10.1016/j.joule.2020.04.006	journal	June 2020
Pressure engineering of photovoltaic perovskites Liu, Gang; Kong, Lingping; Yang, Wenge Materials Today, Vol. 27 https://doi.org/10.1016/j.mattod.2019.02.016	journal	July 2019
Effect of static local distortions vs. dynamic motions on the stability and band gaps of cubic oxide and halide perovskites Zhao, Xin-Gang; Wang, Zhi; Malyi, Oleksandr I. Materials Today, Vol. 49 https://doi.org/10.1016/j.mattod.2021.05.021	journal	October 2021
First principles phonon calculations in materials science Togo, Atsushi; Tanaka, Isao Scripta Materialia, Vol. 108 https://doi.org/10.1016/j.scriptamat.2015.07.021	journal	November 2015
Femtosecond mega-electron-volt electron microdiffraction Shen, X.; Li, R. K.; Lundström, U. Ultramicroscopy, Vol. 184 https://doi.org/10.1016/j.ultramic.2017.08.019	journal	January 2018
Phase Behavior and Polymorphism of Formamidinium Lead Iodide Weber, Oliver J.; Ghosh, Dibyajyoti; Gaines, Sam Chemistry of Materials, Vol. 30, Issue 11 https://doi.org/10.1021/acs.chemmater.8b00862	journal	May 2018
Synthesis and Spectroscopy of Monodispersed, Quantum-Confined FAPbBr ₃ Perovskite Nanocrystals Li, Yulu; Ding, Tao; Luo, Xiao Chemistry of Materials, Vol. 32, Issue 1 https://doi.org/10.1021/acs.chemmater.9b04297	journal	November 2019
Crystal Structure Evolution and Notable Thermal Expansion in Hybrid Perovskites Formamidinium Tin Iodide and Formamidinium Lead Bromide Schueller, Emily C.; Laurita, Geneva; Fabini, Douglas H. Inorganic Chemistry, Vol. 57, Issue 2 https://doi.org/10.1021/acs.inorgchem.7b02576	journal	October 2017
Luminescence Fine Structures in Single Lead Halide Perovskite Nanocrystals: Size Dependence of the Exciton–Phonon Coupling Cho, Kenichi; Yamada, Takumi; Tahara, Hirokazu Nano Letters, Vol. 21, Issue 17 https://doi.org/10.1021/acs.nanolett.1c02122	journal	August 2021
Exciton–Phonon and Trion–Phonon Couplings Revealed by Photoluminescence Spectroscopy of Single CsPbBr₃ Perovskite Nanocrystals Cho, Kenichi; Tahara, Hirokazu; Yamada, Takumi Nano Letters, Vol. 22, Issue 18 https://doi.org/10.1021/acs.nanolett.2c02970	journal	September 2022
Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium–Lead-Halide Perovskite Quantum Dots Makarov, Nikolay S.; Guo, Shaojun; Isaienko, Oleksandr Nano Letters, Vol. 16, Issue 4 https://doi.org/10.1021/acs.nanolett.5b05077	journal	March 2016
Brightly Luminescent and Color-Tunable Formamidinium Lead Halide Perovskite FAPbX ₃ (X = Cl, Br, I) Colloidal Nanocrystals Levchuk, Ievgen; Osvet, Andres; Tang, Xiaofeng Nano Letters, Vol. 17, Issue 5 https://doi.org/10.1021/acs.nanolett.6b04781	journal	April 2017
Neutral and Charged Exciton Fine Structure in Single Lead Halide Perovskite Nanocrystals Revealed by Magneto-optical Spectroscopy Fu, Ming; Tamarat, Philippe; Huang, He Nano Letters, Vol. 17, Issue 5 https://doi.org/10.1021/acs.nanolett.7b00064	journal	April 2017
Critical Role of Methylammonium Librational Motion in Methylammonium Lead Iodide (CH ₃ NH ₃ PbI ₃ ) Perovskite Photochemistry Park, Myeongkee; Kornienko, Nikolay; Reyes-Lillo, Sebastian E. Nano Letters, Vol. 17, Issue 7 https://doi.org/10.1021/acs.nanolett.7b00919	journal	June 2017
Phonon Interaction and Phase Transition in Single Formamidinium Lead Bromide Quantum Dots Pfingsten, Oliver; Klein, Julian; Protesescu, Loredana Nano Letters, Vol. 18, Issue 7 https://doi.org/10.1021/acs.nanolett.8b01523	journal	June 2018
Long Exciton Dephasing Time and Coherent Phonon Coupling in CsPbBr ₂ Cl Perovskite Nanocrystals Becker, Michael A.; Scarpelli, Lorenzo; Nedelcu, Georgian Nano Letters, Vol. 18, Issue 12 https://doi.org/10.1021/acs.nanolett.8b03027	journal	November 2018
Direct Evidence of Permanent Octahedra Distortion in MAPbBr ₃ Hybrid Perovskite Bernasconi, Andrea; Malavasi, Lorenzo ACS Energy Letters, Vol. 2, Issue 4 https://doi.org/10.1021/acsenergylett.7b00139	journal	March 2017
Rationalizing and Controlling the Surface Structure and Electronic Passivation of Cesium Lead Halide Nanocrystals Bodnarchuk, Maryna I.; Boehme, Simon C.; ten Brinck, Stephanie ACS Energy Letters, Vol. 4, Issue 1 https://doi.org/10.1021/acsenergylett.8b01669	journal	November 2018
Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy Guzelturk, Burak; Utterback, James K.; Coropceanu, Igor ACS Nano, Vol. 14, Issue 4 https://doi.org/10.1021/acsnano.0c00673	journal	March 2020
Resolving the Controversy in Biexciton Binding Energy of Cesium Lead Halide Perovskite Nanocrystals through Heralded Single-Particle Spectroscopy Lubin, Gur; Yaniv, Gili; Kazes, Miri ACS Nano, Vol. 15, Issue 12 https://doi.org/10.1021/acsnano.1c06624	journal	November 2021
Direct Observation of Ultrafast Lattice Distortions during Exciton–Polaron Formation in Lead Halide Perovskite Nanocrystals Seiler, Hélène; Zahn, Daniela; Taylor, Victoria C. A. ACS Nano, Vol. 17, Issue 3 https://doi.org/10.1021/acsnano.2c06727	journal	January 2023
Coherent Nanotwins and Dynamic Disorder in Cesium Lead Halide Perovskite Nanocrystals Bertolotti, Federica; Protesescu, Loredana; Kovalenko, Maksym V. ACS Nano, Vol. 11, Issue 4 https://doi.org/10.1021/acsnano.7b00017	journal	April 2017
Study of Local Structure in Selected Organic–Inorganic Perovskites in the Pm 3̅ m Phase Worhatch, Richard J.; Kim, HyunJeong; Swainson, Ian P. Chemistry of Materials, Vol. 20, Issue 4 https://doi.org/10.1021/cm702668d	journal	February 2008
Photoinduced Vibrations Drive Ultrafast Structural Distortion in Lead Halide Perovskite Duan, Hong-Guang; Tiwari, Vandana; Jha, Ajay Journal of the American Chemical Society, Vol. 142, Issue 39 https://doi.org/10.1021/jacs.0c03970	journal	September 2020
Quantifying Photoinduced Polaronic Distortions in Inorganic Lead Halide Perovskite Nanocrystals Cannelli, Oliviero; Colonna, Nicola; Puppin, Michele Journal of the American Chemical Society, Vol. 143, Issue 24 https://doi.org/10.1021/jacs.1c02403	journal	June 2021
Monodisperse Formamidinium Lead Bromide Nanocrystals with Bright and Stable Green Photoluminescence Protesescu, Loredana; Yakunin, Sergii; Bodnarchuk, Maryna I. Journal of the American Chemical Society, Vol. 138, Issue 43 https://doi.org/10.1021/jacs.6b08900	journal	October 2016
Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites Yang, Jianfeng; Wen, Xiaoming; Xia, Hongze Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14120	journal	January 2017
Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite Park, Myeongkee; Neukirch, Amanda J.; Reyes-Lillo, Sebastian E. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-04946-7	journal	June 2018
Unraveling exciton–phonon coupling in individual FAPbI3 nanocrystals emitting near-infrared single photons Fu, Ming; Tamarat, Philippe; Trebbia, Jean-Baptiste Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05876-0	journal	August 2018
Photoinduced, reversible phase transitions in all-inorganic perovskite nanocrystals Kirschner, Matthew S.; Diroll, Benjamin T.; Guo, Peijun Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-08362-3	journal	January 2019
Two-dimensional electronic spectroscopy reveals liquid-like lineshape dynamics in CsPbI3 perovskite nanocrystals Seiler, Hélène; Palato, Samuel; Sonnichsen, Colin Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12830-1	journal	October 2019
Coherent vibrational dynamics reveals lattice anharmonicity in organic–inorganic halide perovskite nanocrystals Debnath, Tushar; Sarker, Debalaya; Huang, He Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22934-2	journal	May 2021
Fröhlich interaction dominated by a single phonon mode in CsPbBr3 Iaru, Claudiu M.; Brodu, Annalisa; van Hoof, Niels J. J. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-26192-0	journal	October 2021
Ultra-narrow room-temperature emission from single CsPbBr3 perovskite quantum dots Rainò, Gabriele; Yazdani, Nuri; Boehme, Simon C. Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-30016-0	journal	May 2022
Genesis, challenges and opportunities for colloidal lead halide perovskite nanocrystals Akkerman, Quinten A.; Rainò, Gabriele; Kovalenko, Maksym V. Nature Materials, Vol. 17, Issue 5 https://doi.org/10.1038/s41563-018-0018-4	journal	February 2018
Present status and future prospects of perovskite photovoltaics Snaith, Henry J. Nature Materials, Vol. 17, Issue 5 https://doi.org/10.1038/s41563-018-0071-z	journal	April 2018
Phonon coherences reveal the polaronic character of excitons in two-dimensional lead halide perovskites Thouin, Félix; Valverde-Chávez, David A.; Quarti, Claudio Nature Materials, Vol. 18, Issue 4 https://doi.org/10.1038/s41563-018-0262-7	journal	January 2019
The ground exciton state of formamidinium lead bromide perovskite nanocrystals is a singlet dark state Tamarat, Philippe; Bodnarchuk, Maryna I.; Trebbia, Jean-Baptiste Nature Materials, Vol. 18, Issue 7 https://doi.org/10.1038/s41563-019-0364-x	journal	May 2019
Visualization of dynamic polaronic strain fields in hybrid lead halide perovskites Guzelturk, Burak; Winkler, Thomas; Van de Goor, Tim W. J. Nature Materials, Vol. 20, Issue 5 https://doi.org/10.1038/s41563-020-00865-5	journal	January 2021
Ultrafast relaxation of lattice distortion in two-dimensional perovskites Zhang, Hao; Li, Wenbin; Essman, Joseph Nature Physics, Vol. 19, Issue 4 https://doi.org/10.1038/s41567-022-01903-6	journal	January 2023
Significance of hydrogen bonding and other noncovalent interactions in determining octahedral tilting in the CH3NH3PbI3 hybrid organic-inorganic halide perovskite solar cell semiconductor Varadwaj, Pradeep R.; Varadwaj, Arpita; Marques, Helder M. Scientific Reports, Vol. 9, Issue 1 https://doi.org/10.1038/s41598-018-36218-1	journal	January 2019
Structural and optical properties of methylammonium lead iodide across the tetragonal to cubic phase transition: implications for perovskite solar cells Quarti, Claudio; Mosconi, Edoardo; Ball, James M. Energy & Environmental Science, Vol. 9, Issue 1 https://doi.org/10.1039/C5EE02925B	journal	January 2016
The chemical forces underlying octahedral tilting in halide perovskites Butler, Keith T. Journal of Materials Chemistry C, Vol. 6, Issue 44 https://doi.org/10.1039/C8TC02976H	journal	January 2018
Polymorphism in metal halide perovskites Alaei, Aida; Circelli, Abigail; Yuan, Yihang Materials Advances, Vol. 2, Issue 1 https://doi.org/10.1039/D0MA00643B	journal	January 2021
Femtosecond broadband fluorescence upconversion spectroscopy: Improved setup and photometric correction Zhang, X. -X.; Würth, C.; Zhao, L. Review of Scientific Instruments, Vol. 82, Issue 6 https://doi.org/10.1063/1.3597674	journal	June 2011
Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory Weathersby, S. P.; Brown, G.; Centurion, M. Review of Scientific Instruments, Vol. 86, Issue 7 https://doi.org/10.1063/1.4926994	journal	July 2015
Theory of light absorption and non-radiative transitions in F-centres Huang, Kun; Rhys, Avril Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences, Vol. 204, Issue 1078, p. 406-423 https://doi.org/10.1098/rspa.1950.0184	journal	December 1950
Polymorphous nature of cubic halide perovskites Zhao, Xin-Gang; Dalpian, Gustavo M.; Wang, Zhi Physical Review B, Vol. 101, Issue 15 https://doi.org/10.1103/PhysRevB.101.155137	journal	April 2020
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium Kresse, G.; Hafner, J. Physical Review B, Vol. 49, Issue 20, p. 14251-14269 https://doi.org/10.1103/PhysRevB.49.14251	journal	May 1994
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set Kresse, G.; Furthmüller, J. Physical Review B, Vol. 54, Issue 16, p. 11169-11186 https://doi.org/10.1103/PhysRevB.54.11169	journal	October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Evidence of Large Polarons in Photoemission Band Mapping of the Perovskite Semiconductor CsPbBr 3 Puppin, M.; Polishchuk, S.; Colonna, N. Physical Review Letters, Vol. 124, Issue 20 https://doi.org/10.1103/PhysRevLett.124.206402	journal	May 2020
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Polaronic quantum confinement in bulk CsPbBr3 perovskite crystals revealed by state-resolved pump/probe spectroscopy Sonnichsen, Colin D.; Strandell, Dallas P.; Brosseau, Patrick J. Physical Review Research, Vol. 3, Issue 2 https://doi.org/10.1103/PhysRevResearch.3.023147	journal	May 2021
Absorption correction for cylindrical and annular specimens and their containers or supports Bowden, Mark; Ryan, Martin Journal of Applied Crystallography, Vol. 43, Issue 4 https://doi.org/10.1107/S0021889810021114	journal	July 2010
The MYTHEN detector for X-ray powder diffraction experiments at the Swiss Light Source Bergamaschi, Anna; Cervellino, Antonio; Dinapoli, Roberto Journal of Synchrotron Radiation, Vol. 17, Issue 5 https://doi.org/10.1107/S0909049510026051	journal	July 2010
The Materials Science beamline upgrade at the Swiss Light Source Willmott, P. R.; Meister, D.; Leake, S. J. Journal of Synchrotron Radiation, Vol. 20, Issue 5 https://doi.org/10.1107/S0909049513018475	journal	July 2013
Light-induced picosecond rotational disordering of the inorganic sublattice in hybrid perovskites Wu, Xiaoxi; Tan, Liang Z.; Shen, Xiaozhe Science Advances, Vol. 3, Issue 7 https://doi.org/10.1126/sciadv.1602388	journal	July 2017
Large polarons in lead halide perovskites Miyata, Kiyoshi; Meggiolaro, Daniele; Trinh, M. Tuan Science Advances, Vol. 3, Issue 8 https://doi.org/10.1126/sciadv.1701217	journal	August 2017
Screening in crystalline liquids protects energetic carriers in hybrid perovskites Zhu, H.; Miyata, K.; Fu, Y. Science, Vol. 353, Issue 6306 https://doi.org/10.1126/science.aaf9570	journal	September 2016
Coherent single-photon emission from colloidal lead halide perovskite quantum dots Utzat, Hendrik; Sun, Weiwei; Kaplan, Alexander E. K. Science, Vol. 363, Issue 6431 https://doi.org/10.1126/science.aau7392	journal	February 2019
Coupling to Octahedral Tilts in Halide-Perovskite Nanocrystals Induces Phonon-Mediated Attractive Interactions between Excitons Nuri, Yazdani, ETH Zurich https://doi.org/10.3929/ethz-b-000626244	collection	January 2023

Similar Records

Quasicubic model for metal halide perovskite nanocrystals

Journal Article · Fri Dec 20 23:00:00 EST 2019 · Journal of Chemical Physics · OSTI ID:1767718

Ultrafast exciton many-body interactions and hot-phonon bottleneck in colloidal cesium lead halide perovskite nanocrystals

Journal Article · Mon Sep 10 00:00:00 EDT 2018 · Physical Review B · OSTI ID:1476250

Phonon Screening of Excitons in Semiconductors: Halide Perovskites and Beyond

Journal Article · Thu Aug 05 00:00:00 EDT 2021 · Physical Review Letters · OSTI ID:1821153

Related Subjects

36 MATERIALS SCIENCE
electronic devices
electronic properties and materials
quantum dots

Coupling to octahedral tilts in halide perovskite nanocrystals induces phonon-mediated attractive interactions between excitons

Citation Formats

References (67)

Similar Records

Related Subjects