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Conference on Lasers and Electro-Optics

Third-order nonlinear optical spectroscopy in two-dimensional Mott-insulators

Hideo Kishida, Atsushi Maeda, Yoshinori Tokura, Akihito Sawa, M. Kawasaki, Hiroshi Okamoto

Published Jan 1, 2005• 0 citations
Publisher
DOI
10.1109/iqec.2005.1560917

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We study the third-order nonlinear optical susceptibility ${\ensuremath{\chi}}^{(3)}$ and photoexcited states of two-dimensional (2D) Mott insulators by using an effective model in the strong-coupling limit of a half-filled Hubbard model. In the numerically exact diagonalization calculations on finite-size clusters, we find that the coupling of charge and spin degrees of freedom plays a crucial role in the distribution of the dipole-allowed states with odd parity and the dipole-forbidden states with even parity in the photoexcited states. This is in contrast with the photoexcited states in one dimension, where the charge and spin degrees of freedom are decoupled. In the third-harmonic generation (THG) spectrum, the main contribution is found to come from the process of three-photon resonance associated with the odd-parity states. As a result, the two-photon resonance process is less pronounced in the THG spectrum. The calculated THG spectrum is compared with recent experimental data. We also find that ${\ensuremath{\chi}}^{(3)}$ with a cross-polarized configuration of pump and probe photons shows spectral distributions similar to ${\ensuremath{\chi}}^{(3)}$ with a copolarized configuration, although the weight is small. These findings will help analyses of the experimental data of ${\ensuremath{\chi}}^{(3)}$ in 2D Mott insulators.
We prepare and study a metastable attractive Mott-insulator state formed with bosonic atoms in a three-dimensional optical lattice. Starting from a Mott insulator with Cs atoms at weak repulsive interactions, we use a magnetic Feshbach resonance to tune the interactions to large attractive values and produce a metastable state pinned by attractive interactions with a lifetime on the order of 10 s. We probe the (de)excitation spectrum via lattice modulation spectroscopy, measuring the interaction dependence of two- and three-body bound-state energies. As a result of increased on-site three-body loss we observe resonance broadening and suppression of tunneling processes that produce three-body occupation.
Solid-state high-harmonic spectroscopy is becoming an emerging tool for probing nonequilibrium many-body dynamics. Yet, direct measurements of strongly driven, sub-optical-cycle dynamics in correlated materials during high-harmonic emission remain largely unexplored. Here, we measure high-harmonic emission chirp in a prototypical one-dimensional Mott insulator, which encodes strongly driven doublon-holon dynamics at sub-optical-cycle timescales. We observe a positive chirp for above band gap harmonics, indicating that high harmonics are dominated by doublon-holon recombinations. We further show a harmonic order-dependent dephasing, which can be understood through different doublon-holon excursion distances associated with each harmonic. These results reveal coherent doublon-holon dynamics and their ultrafast dephasing in Mott insulators, which is relevant to other nonequilibrium light-induced phenomena, such as Floquet engineering.