Phonon State Tomography of Electron Correlation Dynamics in Optically Excited Solids.

Nano Lett

Department of Chemistry and Biochemistry, University of California San Diego, La Jolla, California 92093, United States.

Published: December 2024

We introduce phonon state tomography (PST) as a diagnostic probe of electron dynamics in solids whose phonons are optically excited by a laser pulse at initial time. Using a projected-purified matrix-product states algorithm, PST decomposes the exact correlated electron-phonon wavefunction into contributions from purely electronic states corresponding to statistically typical configurations of the optically accessible phononic response, enabling a "tomographic" reconstruction of the electronic dynamics generated by the phonons. Thus, PST may be used to diagnose electronic behavior in experiments that access only the phonon response, such as thermal diffuse X-ray and electron scattering. We study the dynamics of a metal whose infrared phonons are excited by an optical pulse at initial time and use it to simulate the sample-averaged momentum-resolved phonon occupancy and accurately reconstruct the electronic correlations. We also use PST to analyze the influence of different pulse shapes on the light-induced enhancement and suppression of electronic correlations.

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http://dx.doi.org/10.1021/acs.nanolett.4c04314DOI Listing

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