Phonon State Tomography of Electron Correlation Dynamics in Optically Excited Solids

• Published in: Nano letters Vol. 24; no. 49; pp. 15693 - 15699
• Main Authors: Moroder, Mattia, Mitrano, Matteo, Schollwöck, Ulrich, Paeckel, Sebastian, Sous, John
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 26.11.2024
• Subjects: tensor networks; pump−probe spectroscopy; tomography; electron−phonon interaction
• ISSN: 1530-6984; 1530-6992; 1530-6992
• DOI: 10.1021/acs.nanolett.4c04314

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.