Ultrafast Transient Absorption Spectroscopy of the Charge-Transfer Insulator NiO: Beyond the Dynamical Franz-Keldysh Effect

Abstract

We demonstrate that a dynamical modification of the Hubbard U in the model charge-transfer insulator NiO can be observed with state-of-the-art time-resolved absorption spectroscopy. Using a self-consistent time-dependent density functional theory plus U computational framework, we show that the dynamical modulation of screening and Hubbard U significantly changes the transient optical spectroscopy. Whereas we find the well-known dynamical Franz-Keldysh effect when the U is frozen, we observe a dynamical band-gap renormalization for dynamical U. The renormalization of the optical gap is found to be smaller than the renormalization of U. This work opens up the possibility of driving a light-induced transition from a charge-transfer into a Mott insulator phase.

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Cited by in corpus (10)

• Nonthermal pathways to ultrafast control in quantum materials
• Ultrafast renormalization of the onsite Coulomb repulsion in a cuprate superconductor
• Keldysh space control of charge dynamics in a strongly driven Mott insulator
• A Snapshot of Time-Dependent Density-Functional Theory
• Ultrafast creation of a light induced semimetallic state in strongly excited 1T-TiSe${}_2$
• Floquet theory and computational method for the optical absorption of laser-dressed solids
• Photo-induced charge-transfer renormalization in NiO
• Simulating Ultrafast Transient Absorption Spectra from First Principles using a Time-Dependent Configuration Interaction Probe
• Attosecond All-Optical Retrieval of Valley Polarization via Circular Dichroism in Transient Absorption
• Attosecond Transient Absorption Spectroscopy of Strongly Correlated Mott Insulators: Signature of the Creation and Annihilation of Double Occupancy