Attosecond Transient Absorption Spectroscopy of Strongly Correlated Mott Insulators: Signature of the Creation and Annihilation of Double Occupancy

Abstract

We applied the time-resolved attosecond transient absorption spectroscopy to systematically investigate ultrafast optical responses of condensed matter systems. Under an intense pump pulse, absorption spectra indicate that the non-interacting electrons of band insulators produce a field-induced redshift, known as the dynamical Franz-Keldysh effect, as commonly expected. In contrast to the band insulators, in Mott insulators, unconventional spectra are observed which do not fully reflect the dynamical Franz-Keldysh effect. While it still exhibits the fishbone-like structures mimicking the dynamical Franz-Keldysh effect, the spectra show a negative difference absorption below the band edge, rendering a blueshift. In addition, the decomposed difference absorption reveals the creation and the annihilation of double occupancy mainly contribute to the negative signal, implying that the unconventional spectra are purely driven by the electron-correlations. These demonstrations of unconventional responses would guide us to the correlation-embedded attosecond electron dynamics in condensed matter systems.