Romain Géneaux^1,2*, Iurii Timrov^3*, Christopher Kaplan^1*, Andrew Ross^1*, Peter Kraus^1,4*, Stephen Leone^1,5,6*

1 Department of Chemistry, University of California, Berkeley, 94720, USA

2 Université Paris-Saclay, CEA, CNRS, LIDYL, 91191 Gif-sur-Yvette, France

3 Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne, CH-1015 Lausanne, Switzerland

4 Advanced Research Center for Nanolithography, Science Park 106, 1098 XG Amsterdam, Netherlands

5 Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA

6 Department of Physics, University of California, Berkeley, 94720, USA

* Corresponding authors emails: romain.geneaux@cea.fr, iurii.timrov@epfl.ch, ckap35@gmail.com, adross@berkeley.edu, P.Kraus@arcnl.nl, srl@berkeley.edu

DOI10.24435/materialscloud:m2-31 [version v1]

Publication date: Jul 16, 2021

How to cite this record

Romain Géneaux, Iurii Timrov, Christopher Kaplan, Andrew Ross, Peter Kraus, Stephen Leone, Coherent energy exchange between carriers and phonons in Peierls-distorted bismuth unveiled by broadband XUV pulses, Materials Cloud Archive 2021.111 (2021), https://doi.org/10.24435/materialscloud:m2-31

Description

In Peierls-distorted materials, photoexcitation leads to a strongly coupled transient response between structural and electronic degrees of freedom, always measured independently of each other. Here we use transient reflectivity in the extreme ultraviolet to quantify both responses in photoexcited bismuth in a single measurement. With the help of first-principles calculations based on density-functional theory (DFT) and time-dependent DFT, the real-space atomic motion and the temperature of both electrons and holes as a function of time are captured simultaneously, retrieving an anticorrelation between the A1g phonon dynamics and carrier temperature. The results reveal a coherent, bi-directional energy exchange between carriers and phonons, which is a dynamical counterpart of the static Peierls-Jones distortion, providing first-time validation of previous theoretical predictions.

Materials Cloud sections using this data

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Keywords

bismuth density-functional theory time-dependent density-functional theory absorption spectrum transient reflectivity extreme ultraviolet photoexcitation real-space atomic motion density of states SNSF MARVEL/OSP CSCS Investissements d'Avenir