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      Electron–phonon-driven three-dimensional metallicity in an insulating cuprate

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          Significance

          Elucidating the role of different degrees of freedom in a phase transition is crucial in the comprehension of complex materials. A phase transformation that attracts significant interest is the insulator-to-metal transition of Mott insulators, in which the electrons are thought to play the dominant role. Here, we use ultrafast laser spectroscopy and theoretical calculations to unveil that the correlated insulator L a 2 C u O 4 , precursor to high-temperature superconductivity, is unstable toward metallization when its crystal structure is displaced along the coordinates of specific vibrational modes. This, in turn, supports the involvement of the lattice in this phase transition. Our results pave the way toward the geometrical design of metallic states in Mott insulators, with technological potential for ultrafast switching devices at room temperature.

          Abstract

          The role of the crystal lattice for the electronic properties of cuprates and other high-temperature superconductors remains controversial despite decades of theoretical and experimental efforts. While the paradigm of strong electronic correlations suggests a purely electronic mechanism behind the insulator-to-metal transition, recently the mutual enhancement of the electron–electron and the electron–phonon interaction and its relevance to the formation of the ordered phases have also been emphasized. Here, we combine polarization-resolved ultrafast optical spectroscopy and state-of-the-art dynamical mean-field theory to show the importance of the crystal lattice in the breakdown of the correlated insulating state in an archetypal undoped cuprate. We identify signatures of electron–phonon coupling to specific fully symmetric optical modes during the buildup of a three-dimensional (3D) metallic state that follows charge photodoping. Calculations for coherently displaced crystal structures along the relevant phonon coordinates indicate that the insulating state is remarkably unstable toward metallization despite the seemingly large charge-transfer energy scale. This hitherto unobserved insulator-to-metal transition mediated by fully symmetric lattice modes can find extensive application in a plethora of correlated solids.

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          Special points for Brillouin-zone integrations

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            Self-interaction correction to density-functional approximations for many-electron systems

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              Doping a Mott insulator: Physics of high-temperature superconductivity

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                Author and article information

                Journal
                Proc Natl Acad Sci U S A
                Proc. Natl. Acad. Sci. U.S.A
                pnas
                pnas
                PNAS
                Proceedings of the National Academy of Sciences of the United States of America
                National Academy of Sciences
                0027-8424
                1091-6490
                24 March 2020
                11 March 2020
                11 March 2020
                : 117
                : 12
                : 6409-6416
                Affiliations
                aInstitute of Physics, Laboratory for Ultrafast Microscopy and Electron Scattering, École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland;
                bInstitute of Chemical Sciences and Engineering, Laboratory of Ultrafast Spectroscopy, École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland;
                cMax Planck Institute for the Structure and Dynamics of Matter, D-22761 Hamburg, Germany;
                dDepartment of Physics, King’s College London, London WC2R 2LS, United Kingdom;
                eWilhelm Ostwald Institut of Physical and Theoretical Chemistry, University of Leipzig, D-04103 Leipzig, Germany;
                fDepartment of Physics, University of Fribourg, CH-1700 Fribourg, Switzerland;
                gSolid State Chemistry Group, Laboratory for Multiscale Materials Experiments, Paul Scherrer Institute, CH-5232 Villigen PSI, Switzerland;
                hNano-Bio Spectroscopy Group, Departamento de Física de Materiales, Universidad del País Vasco, 20018 San Sebastían, Spain;
                iCenter for Computational Quantum Physics, The Flatiron Institute, New York, NY 10010
                Author notes
                1To whom correspondence may be addressed. Email: angel.rubio@ 123456mpsd.mpg.de , cedric.weber@ 123456kcl.ac.uk , or ebaldini@ 123456mit.edu .

                Contributed by Angel Rubio, February 11, 2020 (sent for review November 8, 2019; reviewed by Riccardo Comin and Zhi-Xun Shen)

                Author contributions: E.B., M.A.S., A.R., and C.W. designed research; E.B., S.A., T.B., E.S., F.L., E.P., M.v.S., A.R., and C.W. performed research; E.B. and F.C. analyzed data; and E.B., M.A.S., C.B., A.R., and C.W. wrote the paper.

                Reviewers: R.C., Massachusetts Institute of Technology; and Z.-X.S., Stanford University.

                Article
                201919451
                10.1073/pnas.1919451117
                7104249
                32161128
                Copyright © 2020 the Author(s). Published by PNAS.

                This open access article is distributed under Creative Commons Attribution-NonCommercial-NoDerivatives License 4.0 (CC BY-NC-ND).

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                Pages: 8
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                Categories
                Physical Sciences
                Physics

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