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Spectral evidence for unidirectional charge density wave in detwinned BaNi2As2

Physical Review B 2023年第8期108卷 L081104-L081104页

作者： Yucheng Guo Mason Klemm Ji Seop Oh Yaofeng Xie Bing-Hua Lei Luca Moreschini Cheng Chen Ziqin Yue Sergey Gorovikov Tor Pedersen Matteo Michiardi Sergey Zhdanovich Andrea Damascelli Jonathan Denlinger Makoto Hashimoto Donghui Lu Chris Jozwiak Aaron Bostwick Eli Rotenberg Sung-Kwan Mo Rob G. Moore Junichiro Kono Robert J. Birgeneau David J. Singh Pengcheng Dai Ming Yi Department of Physics and Astronomy Rice University Houston Texas 77005 USA Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA Department of Physics University of California Berkeley California 94720 USA Department of Physics and Astronomy University of Missouri Columbia Missouri 65211 USA Materials Science Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA Department of Physics University of Oxford Oxford OX1 3PU United Kingdom Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston Texas 77005 USA Canadian Light Source Inc. 44 Innovation Boulevard Saskatoon SK S7N 2V3 Canada Department of Physics and Astronomy University of British Columbia Vancouver British Columbia V6T 1Z1 Canada Quantum Matter Institute University of British Columbia Vancouver British Columbia V6T 1Z4 Canada Max Planck Institute for Chemical Physics of Solids Nöthnitzer Straße 40 01187 Dresden Germany Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park California 94025 USA Materials Science and Technology Division Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Department of Electrical and Computer Engineering Rice University Houston Texas 77005 USA Smalley-Curl Institute Rice University Houston Texas 77005 USA Department of Materials Science and NanoEngineering Rice University Houston Texas 77005 USA Department of Chemistry University of Missouri Columbia Missouri 65211 USA

In the iron-based superconductors, unconventional superconductivity emerges in proximity to intertwined electronic orders consisting of an electronic nematic order and a spin density wave (SDW). Recently, BaNi2As2, like its well-known iron-based analog BaFe2As2, has been discovered to host a symmetry-breaking structural transition but coupled to a unidirectional charge density wave (CDW) instead of SDW, providing a novel platform to study intertwined orders. Here, through a systematic angle-resolved photoemission spectroscopy study combined with a detwinning B1g uniaxial strain, we identify distinct spectral evidence of band evolution due to the structural transition as well as CDW-induced band folding. In contrast to the nematicity and spin density wave in BaFe2As2, the structural and CDW order parameters in BaNi2As2 are observed to be strongly coupled and do not separate in the presence of uniaxial strain. Furthermore, no nematic band splitting is resolved above the structural transition. Our measurements point to a likely lattice origin of the CDW order in BaNi2As2.

关键词： Charge density waves Nematic phase transition Iron-based superconductors Angle-resolved photoemission spectroscopy

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Two-step electronic response to magnetic ordering in a van der Waals ferromagnet

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Physical Review B 2024年第4期109卷 045416-045416页

作者： Han Wu Jian-Xin Zhu Lebing Chen Matthew W. Butcher Ziqin Yue Dongsheng Yuan Yu He Ji Seop Oh Bin Gao Jianwei Huang Shan Wu Cheng Gong Yucheng Guo Sung-Kwan Mo Jonathan Denlinger Donghui Lu Makoto Hashimoto Matthew B. Stone Alexander I. Kolesnikov Songxue Chi Junichiro Kono Andriy H. Nevidomskyy Robert J. Birgeneau Pengcheng Dai Ming Yi Department of Physics and Astronomy and Rice Center for Quantum Materials Rice University Houston Texas 77005 USA Theoretical Division Los Alamos National Laboratory Los Alamos New Mexico 87545 USA Center for Integrated Nanotechnologies Los Alamos National Laboratory Los Alamos New Mexico 87545 USA Department of Physics University of California at Berkeley Berkeley California 94720 USA Applied Physics Graduate Program Smalley-Curl Institute Rice University Houston Texas 77005 USA Materials Sciences Division Lawrence Berkeley National Laboratory Berkeley California 94720 USA National Institute for Materials Science 1-1 Namiki Tsukuba Ibaraki 305-0044 Japan Department of Applied Physics Yale University New Haven Connecticut 06511 USA Department of Electrical and Computer Engineering and Quantum Technology Center University of Maryland College Park Maryland 20742 USA Advanced Light Source Lawrence Berkeley National Laboratory Berkeley California 94720 USA Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo Park California 94025 USA Neutron Scattering Division Oak Ridge National Laboratory Oak Ridge Tennessee 37831 USA Department of Electrical and Computer Engineering Rice University Houston Texas 77005 USA Smalley-Curl Institute Rice University Houston Texas 77005 USA Department of Material Science and Nanoengineering Rice University Houston Texas 77005 USA Department of Materials Science and Engineering University of California Berkeley California 94720 USA

The two-dimensional material Cr2Ge2Te6 is a member of the class of insulating van der Waals (vdW) magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te p-orbital-dominated bands to undergo changes at the Curie transition temperature TC while the Cr d-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets.

关键词： Electronic structure Magnetic order Magnetic phase transitions Van der Waals systems Angle-resolved photoemission spectroscopy

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Beyond-Hubbard Pairing in a Cuprate Ladder

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Physical Review X 2025年第2期15卷 021049-021049页

作者： Hari Padma Jinu Thomas Sophia F. R. TenHuisen Wei He Ziqiang Guan Jiemin Li Byungjune Lee Yu Wang Seng Huat Lee Zhiqiang Mao Hoyoung Jang Valentina Bisogni Jonathan Pelliciari Mark P. M. Dean Steven Johnston Matteo Mitrano Department of Physics Harvard University Cambridge Massachusetts USA Department of Physics and Astronomy University of Tennessee Knoxville Tennessee USA Institute of Advanced Materials and Manufacturing University of Tennessee Knoxville Tennessee USA John A. Paulson School of Engineering and Applied Sciences Harvard University Cambridge Massachusetts USA Condensed Matter Physics and Materials Science Department Brookhaven National Laboratory Upton New York USA National Synchrotron Light Source II Brookhaven National Laboratory Upton New York USA Department of Physics Pohang University of Science and Technology Pohang Korea Max Planck POSTECH/Korea Research Initiative Center for Complex Phase Materials Pohang Korea 2D Crystal Consortium Materials Research Institute Pennsylvania State University University Park Pennsylvania USA Department of Physics Pennsylvania State University University Park Pennsylvania USA PAL-XFEL Pohang Accelerator Laboratory POSTECH Pohang Korea

The Hubbard model is believed to capture the essential physics of cuprate superconductors. However, recent theoretical studies suggest that it fails to reproduce a robust and homogeneous superconducting ground state. Here, using resonant inelastic x-ray scattering and density matrix renormalization group calculations, we show that magnetic excitations in the prototypical cuprate ladder Sr14Cu24O41 are inconsistent with those of a simple Hubbard model. The magnetic response of hole carriers, contributing to an emergent branch of spin-flip excitations, is strongly suppressed. This effect is the consequence of strong d-wavelike pairing, enhanced by nearly an order of magnitude through a large nearest-neighbor attractive interaction and persisting up to at least 260 K. The close connection between the physics of cuprate ladders and that of the two-dimensional compounds suggests that such an enhanced hole pairing may be a universal feature of superconducting cuprates.

关键词： Hubbard model

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Quantum critical behavior of the hyperkagome magnet Mn3CoSi

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Physical Review Research 2024年第1期6卷 013144-013144页

作者： Hiroki Yamauchi Dita Puspita Sari Yukio Yasui Terutoshi Sakakura Hiroyuki Kimura Akiko Nakao Takashi Ohhara Takashi Honda Katsuaki Kodama Naoki Igawa Kazutaka Ikeda Kazuki Iida Daichi Ueta Tetsuya Yokoo Matthias D. Frontzek Songxue Chi Jaime A. Fernandez-Baca Kenji M. Kojima Donald Arseneau Gerald Morris Bassam Hitti Yipeng Cai Adam Berlie Isao Watanabe Pai-Tse Hsu Yu-Sheng Chen Min Kai Lee Amelia Elisabeth Hall Geetha Balakrishnan Lieh-Jeng Chang Shin-ichi Shamoto Materials Sciences Research Center Japan Atomic Energy Agency (JAEA) Tokai Ibaraki 319-1195 Japan Innovative Global Program College of Engineering Shibaura Institute of Technology 307 Fukasaku Minuma-ku Saitama City Saitama 337-8570 Japan Meson Science Laboratory RIKEN Nishina Center 2-1 Hirosawa Wako Saitama 351-0198 Japan School of Science and Technology Meiji University Kawasaki Kanagawa 214-8571 27 Japan Neutron Industrial Technology Center Comprehensive Research Organization for Science and Society (CROSS) Tokai Ibaraki 319-1106 Japan Institute of Multidisciprinary Research for Advanced Materials Tohoku University Sendai 980-8577 Japan Neutron Science and Technology Center Comprehensive Research Organization for Science and Society (CROSS) Tokai Ibaraki 319-1106 Japan J-PARC Center Japan Atomic Energy Agency (JAEA) Tokai Ibaraki 319-1195 Japan Institute of Materials Structure Science High Energy Accelerator Research Organization (KEK) Tsukuba Ibaraki 305-0801 Japan Neutron Scattering Division Oak Ridge National Laboratory (ORNL) Oak Ridge Tennessee 37831 USA TRIUMF Vancouver British Columbia V6T 2A3 Canada ISIS Neutron and Muon Source Science and Technology Facilities Council Rutherford Appleton Laboratory Didcot OX11 0QX United Kingdom Department of Physics National Cheng Kung University Tainan 70101 Taiwan National Synchrotron Radiation Research Center Hsinchu 300092 Taiwan Department of Physics University of Warwick Coventry CV4 7AL United Kingdom Institute of Physics Academia Sinica Taipei 115201 Taiwan Advanced Science Research Center Japan Atomic Energy Agency (JAEA) Tokai Ibaraki 319-1195 Japan

β-Mn-type family alloys Mn3TX (T=Co, Rh, and Ir; X=Si and Ge) have a three-dimensional antiferromagnetic (AF) corner-shared triangular network, i.e., the hyperkagome lattice. The antiferromagnet Mn3RhSi shows magnetic short-range order over a wide temperature range of approximately 500 K above the Néel temperature TN of 190 K. In this family of compounds, as the lattice parameter decreases, the long-range magnetic ordering temperature decreases. Mn3CoSi has the smallest lattice parameter and the lowest TN in the family. The quantum critical point (QCP) from AF to the quantum paramagnetic state is expected near a cubic lattice parameter of 6.15 Å. Although the Néel temperature of Mn3CoSi is only 140 K, the emergence of the quantum critical behavior in Mn3CoSi is discussed. We study how the magnetic short-range order appears in Mn3CoSi by using neutron scattering, μSR, and bulk characterization such as specific heat capacity. According to the results, the neutron scattering intensity of the magnetic short-range order in Mn3CoSi does not change much at low temperatures from that of Mn3RhSi, although the μSR short-range order temperature of Mn3CoSi is largely suppressed to 240 K from that of Mn3RhSi. Correspondingly, the volume fraction of the magnetic short-range order regions, as shown by the initial asymmetry drop ratio of μSR above TN, also becomes small. Instead, the electronic-specific heat coefficient γ of Mn3CoSi is the largest in this Mn3TSi system, possibly due to the low-energy spin fluctuation near the quantum critical point.

关键词： Critical phenomena Exotic phases of matter Magnetic order Magnetism Phase diagrams Phase transitions Quantum phase transitions

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From Stoner to Local Moment Magnetism in Atomically Thin Cr2Te3

arXiv

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arXiv 2023年

作者： Zhong, Yong Peng, Cheng Huang, Haili Guan, Dandan Hwang, Jinwoong Hsu, Kuan H. Hu, Yi Jia, Chunjing Moritz, Brian Lu, Donghui Lee, Jun-Sik Jia, Jin-Feng Devereaux, Thomas P. Mo, Sung-Kwan Shen, Zhi-Xun Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Department of Applied Physics Stanford University StanfordCA94305 United States TD Lee Institute School of Physics and Astronomy Shanghai Jiao Tong University Shanghai200240 China Department of Physics Institute of Quantum Convergence Technology Kangwon National University Chucheon24341 Korea Republic of Department of Materials Science and Engineering Stanford University StanfordCA94305 United States Department of Physics University of Florida GainesvilleFL32611 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Department of Physics Stanford University StanfordCA94305 United States

The field of two-dimensional (2D) ferromagnetism has been proliferating over the past few years, with ongoing interests in basic science and potential applications in spintronic technology. However, a high-resolution spectroscopic study of the 2D ferromagnet is still lacking due to the small size and air sensitivity of the exfoliated nanoflakes. Here, we report a thickness-dependent ferromagnetism in epitaxially grown Cr2Te3 thin films and investigate the evolution of the underlying electronic structure by synergistic angle-resolved photoemission spectroscopy, scanning tunneling microscopy, x-ray absorption spectroscopy, and first-principle calculations. A conspicuous ferromagnetic transition from Stoner to Heisenberg-type is directly observed in the atomically thin limit, indicating that dimensionality is a powerful tuning knob to manipulate the novel properties of 2D magnetism. Monolayer Cr2Te3 retains robust ferromagnetism, but with a suppressed Curie temperature, due to the drastic drop in the density of states near the Fermi level. Our results establish atomically thin Cr2Te3 as an excellent platform to explore the dual nature of localized and itinerant ferromagnetism in 2D magnets. © 2023, CC BY.

关键词： Ferromagnetism

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Dissecting subcycle interference in photoelectron holography

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Physical Review A 2021年第1期104卷 013109-013109页

作者： Nicholas Werby Andrew S. Maxwell Ruaridh Forbes Philip H. Bucksbaum Carla Figueira de Morisson Faria Stanford PULSE Institute SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo Park California 94025 USA Department of Physics Stanford University Stanford California 94305 USA Institut de Ciencies Fotoniques The Barcelona Institute of Science and Technology 08860 Castelldefels (Barcelona) Spain Department of Physics & Astronomy University College London Gower Street London WC1E 6BT United Kingdom Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo Park California 94025 USA Department of Applied Physics Stanford University Stanford California 94305 USA

Multipath holographic interference in strong-field quantum tunnel ionization is key to revealing subangstrom attosecond dynamics for molecular movies. This critical subcycle motion is often obscured by longer timescale effects such as ring-shaped patterns that appear in above-threshold ionization (ATI). In the present work, we overcome this problem by combining two techniques in theory and experimental analysis: unit-cell averaging and time-filtering data and simulations. Together these suppress ATI rings and enable an unprecedented highly detailed quantitative match between strong-field ionization experiments in argon and the Coulomb-quantum orbit strong-field approximation (CQSFA) theory. Velocity map images reveal fine modulations on the holographic spiderlike interference fringes that form near the polarization axis. CQSFA theory traces this to the interference of three types of electron pathways. The level of agreement between experiment and theory allows sensitive determination of quantum phase differences and symmetries, providing an important tool for quantitative dynamical imaging in quantum systems.

关键词： Holography Multiphoton or tunneling ionization & excitation Strong-field-induced spectra Ultrafast phenomena Quantum orbits theory Strong-field approximation

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Charge order induced Dirac pockets in the nonsymmorphic crystal TaTe4

arXiv

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arXiv 2023年

作者： Zhang Zhou, Ruixiang Wu, Hanlin Oh, Ji Seop Li, Sheng Huang, Jianwei Denlinger, Jonathan D. Hashimoto, Makoto Lu, Donghui Mo, Sung-Kwan Kelly, Kevin F. McCandless, Gregory T. Chan, Julia Y. Birgeneau, Robert J. Lv, Bing Li, Gang Yi, Ming Department of Physics and Astronomy Rice University HoustonTX77005 United States School of Physical Science and Technology Shanghai Tech University Shanghai200031 China Department of Physics The University of Texas at Dallas RichardsonTX75080 United States Department of Physics University of California BerkeleyCA94720 United States Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Department of Chemistry and Biochemistry Baylor University WacoTX76798 United States Materials Science Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States

The interplay between charge order (CO) and nontrivial band topology has spurred tremendous interest in understanding topological excitations beyond the single-particle description. In a quasi-one-dimensional nonsymmorphic crystal TaTe4, the (2a×2b×3c) charge ordered ground state drives the system into a space group where the symmetry indicators feature the emergence of Dirac fermions and unconventional double Dirac fermions. Using angle-resolved photoemission spectroscopy and first-principles calculations, we provide evidence of the CO induced Dirac fermion-related bands near the Fermi level. Furthermore, the band folding at the Fermi level is compatible with the new periodicity dictated by the CO, indicating that the electrons near the Fermi level follow the crystalline symmetries needed to host double Dirac fermions in this system. © 2023, CC BY-NC-ND.

关键词： Ground state

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Kramers Nodal Lines and Weyl Fermions in SmAlSi

arXiv

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arXiv 2022年

作者： Zhang, Yichen Gao, Yuxiang Gao, Xue-Jian Lei, Shiming Ni, Zhuoliang Oh, Ji Seop Huang, Jianwei Yue, Ziqin Zonno, Marta Gorovikov, Sergey Hashimoto, Makoto Lu, Donghui Denlinger, Jonathan D. Birgeneau, Robert J. Kono, Junichiro Wu, Liang Law, Kam Tuen Morosan, Emilia Yi, Ming Department of Physics and Astronomy Rice University HoustonTX77005 United States Department of Physics Hong Kong University of Science and Technology Clear Water Bay Hong Kong Department of Physics and Astronomy University of Pennsylvania PhiladelphiaPA19104 United States Department of Physics University of California BerkeleyCA94720 United States Applied Physics Graduate Program Smalley-Curl Institute Rice University HoustonTX77005 United States Canadian Light Source Inc. 44 Innovation Boulevard SaskatoonSKS7N 2V3 Canada Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory 2575 Sand Hill Road Menlo ParkCA94025 United States Advanced Light Source Lawrence Berekeley National Laboratory BerkeleyCA94720 United States Materials Science Division Lawrence Berekeley National Laboratory BerkeleyCA94720 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Department of Materials Science and Nanoengineering Rice University HoustonTX77005 United States

Kramers nodal lines (KNLs) have recently been proposed theoretically as a special type of Weyl line degeneracy connecting time-reversal invariant momenta. KNLs are robust to spin orbit coupling and are inherent to all non-centrosymmetric achiral crystal structures, leading to unusual spin, magneto-electric, and optical properties. However, their existence in in real quantum materials has not been experimentally established. Here we gather the experimental evidence pointing at the presence of KNLs in SmAlSi, a non-centrosymmetric metal that develops incommensurate spin density wave order at low temperature. Using angle-resolved photoemission spectroscopy, density functional theory calculations, and magneto-transport methods, we provide evidence suggesting the presence of KNLs, together with observing Weyl fermions under the broken inversion symmetry in the paramagnetic phase of SmAlSi. We discuss the nesting possibilities regarding the emergent magnetic orders in SmAlSi. Our results provide a solid basis of experimental observations for exploring correlated topology in SmAlSi. © 2022, CC BY-NC-SA.

关键词： Temperature

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Self-Standing Co24sn0.6o4 Nano Rods as High Performance Anode Materials for Sodium-Ion Battery and Investigation on its Reaction Mechanism

SSRN

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SSRN 2022年

作者： Ali, Ghulam Islam, Mobinul Bhange, Deu S. Jung, Young Hwa Ge, Mingyuan Chu, Yong S. Nam, Kyung-Wan Du, Yonghua Yang, Xiao-Qing Jung, Hun-Gi Bak, Seong-Min Chung, Kyung Yoon Hwarangno 14 gil 5 Seongbuk-gu Seoul02792 Korea Republic of Islamabad44000 Pakistan Department of Energy and Materials Engineering Dongguk University-Seoul Seoul100715 Korea Republic of Department of Chemistry Shivaji University Kolhapur416004 India Beamline Department Pohang Accelerator Laboratory Pohang37673 Korea Republic of National Synchrotron Light Source II Brookhaven National Laboratory UptonNY11973 United States Chemistry Division Brookhaven National Laboratory UptonNY11973 United States Division of Energy & Environment Technology KIST School Korea University of Science and Technology Seoul02792 Korea Republic of

The self-standing nanorod Co 2.4 Sn 0.6 O 4 is synthesized as a high-performance anode material in search of high capacity and stable anode materials for sodium-ion batteries. The Co 2.4 Sn 0.6 O 4 nanorod exhibits a high reversible capacity of 576 mAh g -1 at a current density of 80 mA g -1 and shows excellent high-rate capability. The X-ray absorption spectroscopy study reveals the mechanisms of charge storage reaction and improved cycling performance of Co 2.4 Sn 0.6 O 4 . A partially limited conversion reaction of Co- and Sn-oxide during the cycling effectively regulate the irreversible capacity loss over the cycling that is commonly observed from the conversion and alloying reaction-based anode materials. Furthermore, Co 2.4 Sn 0.6 O 4 also exhibits superior sodium-ion full cell performance when coupled with a NaNi 2/3 Bi 1/3 O 2 cathode, demonstrating an energy density of 262 Wh kg -1 . © 2022, The Authors. All rights reserved.

关键词： Nanorods

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Phonon-Mediated Attractive Interactions between Excitons in Lead-Halide-Perovskites

arXiv

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arXiv 2022年

作者： 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 Department of Materials Science and Engineering Stanford University StanfordCA United States Stanford Institute for Materials and Energy Sciences SLAC National Accelerator Laboratory Menlo ParkCA United States Department of Information Technology and Electrical Engineering ETH Zürich Zürich Switzerland Department of Chemistry and Applied Biosciences ETH Zürich ZürichCH-8093 Switzerland Empa- Swiss Federal Laboratories for Materials Science and Technology Dübendorf Dübendorf CH-8600 Switzerland Dipartimento di Scienza e Alta Tecnologia & To.Sca.Lab Università dell’Insubria Como22100 Italy Department of Physical Chemistry University of Geneva 30 Quai Ernest-Ansermet Geneva 4CH-1211 Switzerland X-ray Science Division Argonne National Laboratory LemontIL60439 United States Department of Chemistry and Biochemistry Middlebury College MiddleburyVT United States Chemistry and Materials Design Group Institute for Electronics Department of Information Technology and Electrical Engineering ETH Zurich Gloriastrasse 35 Zurich8092 Switzerland Linac Coherent Light Source SLAC National Accelerator Laboratory Menlo ParkCA United States Istituto di Cristallografia & To.Sca.Lab Consiglio Nazionale delle Ricerche Como22100 Italy The PULSE Institute for Ultrafast Energy Science SLAC National Accelerator Laboratory Menlo ParkCA United States Department of Photon Science Stanford University SLAC National Accelerator Laboratory Menlo ParkCA United States

Understanding the origin of electron-phonon coupling in lead-halide perovskites (LHP) is key to interpreting and leveraging their optical and electronic properties. Here we perform femtosecond-resolved, optical-pump, electron-diffraction-probe measurements to quantify the lattice reorganization occurring as a result of photoexcitation in LHP nanocrystals. Photoexcitation is found to drive a reduction in lead-halide octahedra tilts and distortions in the lattice, a result of deformation potential coupling to low energy optical phonons. Our results indicate particularly strong coupling in FAPbBr3, and far weaker coupling in CsPbBr3, highlighting differences in the dominant machanisms governing electron-phonon coupling in LHPs. 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 multiexcitonic state constructively interfere, giving rise to a coupling strength which scales quadratically with the exciton number. This superlinear scaling induces phonon-mediated attractive interactions between excitations in LHPs. © 2022, CC BY.

关键词： Perovskite

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