Above-gap ultraviolet excitation of NiO produces a roughly 600 picosecond-lived state with enhanced Ni 3d-O 2p hybridization, observed as a non-thermal red shift of the Ni K-edge X-ray absorption spectrum.
Correlations drive the attosecond response of strongly-correlated insulators
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abstract
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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cond-mat.mtrl-sci 1years
2026 1verdicts
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Light-Stabilized Metastable Electronic State in NiO with Enhanced Orbital Hybridization2
Above-gap ultraviolet excitation of NiO produces a roughly 600 picosecond-lived state with enhanced Ni 3d-O 2p hybridization, observed as a non-thermal red shift of the Ni K-edge X-ray absorption spectrum.