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Coulomb-Enhanced Multi-Photon Processes in Quantum Materials

You Lin Wu, C. Ayala, Peiyan Wang, Zetian Mi, Steven T. Cundiff, M. Kira

Published Jan 1, 2023• 0 citations
Publisher

Abstract

Theory for multi-photon processes is presented to determine extreme nonlinear effects in quantum materials. Our systematic quantum theory predicts that Coulombic many-body effects massively enhance high harmonics and multi-photon absorption.
DOI
10.1364/cleo_fs.2023.ftu4m.5

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Competition and cooperation among orders is at the heart of many-body physics in strongly correlated materials and leads to their rich physical properties. It is crucial to investigate what impact many-body physics has on extreme nonlinear optical phenomena, with the possibility of controlling material properties by light. However, the effect of competing orders and electron-electron correlations on highly nonlinear optical phenomena has not yet been experimentally clarified. Here, we investigated high-order harmonic generation from the Mott-insulating phase of Ca_{2}RuO_{4}. Changing the gap energy in Ca_{2}RuO_{4} as a function of temperature, we observed a strong enhancement of high order harmonic generation at 50 K, increasing up to several hundred times compared to room temperature. We discovered that this enhancement can be well reproduced by an empirical scaling law that depends only on the material gap energy and photon emission energy. Such a scaling law can hardly be explained by the electronic structure change in the single particle model and has not been predicted by previous theoretical studies on HHG in the simple Mott-Hubbard model. Our results suggest that the highly nonlinear optical response of strongly correlated materials is influenced by competition among the multiple degrees of freedom and electron-electron correlations.
Multi-photon processes are extremely important in optics. Optical harmonics generation, multi-photon absorption, ionization, polymerization or spectroscopy are widely used in practical applications. The efficiency of these processes depends on many factors, one of them being the statistics of the incident light. Indeed, the rate of an n-photon effect scales as the nth-order autocorrelation function g(n)of the incident light [1]. Therefore light sources with high correlation functions can enhance the efficiency of such effects by several orders in magnitude compared to coherent light with the same wavelength, pulse duration and energy per pulse. Here we demonstrate this enhancement in the generation of optical harmonics from bright squeezed vacuum (BSV), which can have thermal (g(n)=n!) or superbunched (g(n)=(2n-1)!!) statistics depending on the spectral filtering [2].
Many-body Coulomb interactions dominate nonlinear optical properties of semiconductor structures in many respects. Resulting effects show up most distinct in the temporal evolution of transient four-wave mixing signals. The simplest example in systems with homogeneously broadened absorption is the static exchange interaction, which prevents the occurrence of pure free polarization decay and gives rise to an additional interaction induced signal. For inhomogeneous broadening one obtains photon echo-like behaviour. The temporal duration of the signal, however, is not determined by the width of the inhomogeneous broadening, as is predicted by theory if interaction effects are neglected, but is much smaller due to exciton-exciton interaction. Additional to the static interaction effects electron-electron correlations give rise to laser induced renormalization and dephasing processes which depend sensitively on the polarizations of the driving fields. These effects are analyzed on the basis of quantum-kinetic equations, which allow to describe the temporal evolution of the nonlinear polarizations. Numerical results are presented for various excitation conditions and material systems.