Electron Correlation Effects in Solid-state High Harmonic Generation with First-Principles Calculations

Dr. Didarul Alam, University of Missouri
Prof. Carsten Ullrich
Physics Library

High harmonic generation (HHG) is an extreme non-linear phenomenon where strong laser-field pulses interact with a medium to produce coherent and high-frequency harmonics of the incident light.  Since its first observation in solids in 2011, pioneering theoretical studies have clarified some of the details of the microscopic mechanism behind this phenomenon, like the role of intra- and inter-band transitions, the contribution of the transition dipole moments to the even and odd harmonic peaks, effects of broken symmetry, etc. However, the role of electron correlation effects in the HHG in strongly correlated materials is much less understood. This talk will discuss the role of these effects in the high-harmonic (HH) spectra of solids, using time-dependent density-functional theory and dynamical mean-field theory, for the examples of semiconductor ZnO, perovskites BaTiO3 and BiFeO3 and transition-metal oxide VO2. It is found that correlation effects significantly modify the HH spectrum of all systems, in particular through the ultrafast modification of the electronic spectrum in ZnO. In the case of BaTiO3, correlation effects generate "super-harmonics" – periodic enhancements and suppressions of specific harmonic orders that depend on the correlation strength. Memory effects in HHG were found to lead to a further extension of the harmonic cutoff. For the HH spectrum of VO2,  we find correlation-induced higher harmonics, in good agreement with experimental data. The obtained results shed light on the role of electron correlations in the HH spectrum in complex materials and may help pave the way for future advancements in the field of ultrafast science and attosecond physics.