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Romain Cazali, Amina Alić, Matthieu Guer, Christopher J. Kaplan, Fabien Lepetit, O. Tcherbakoff, S. Guizard, Angel Rubio, N. Tancogne-Dejean, G. S. Chiuzbuaian, Romain G'eneaux
1 31. 1. 2025.

Correlations drive the attosecond response of strongly-correlated insulators

Attosecond spectroscopy of materials has provided invaluable insight into light-driven coherent electron dynamics. However, attosecond spectroscopies have so far been focused on weakly-correlated materials. As a result, the behavior of strongly-correlated systems is largely unknown at sub- to few-femtosecond timescales, even though it is typically the realm at which electron-electron interactions operate. Here we conduct attosecond-resolved experiments on the correlated insulator nickel oxide, and compare its response to a common band insulator, revealing fundamentally different behaviors. The results, together with state-of-the art time-dependent $\textit{ab initio}$ calculations, show that the correlated system response is governed by a laser-driven quench of electron correlations. The evolution of the on-site electronic interaction is measured here at its natural timescale, marking the first direct measurement of Hubbard $U$ renormalization in NiO. It is found to take place within a few femtoseconds, after which structural changes slowly start to take place. The resulting picture sheds light on the entire light-induced response of a strongly-correlated system, from attosecond to long-lived effects.


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