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High harmonic generation (HHG) takes place in all phases of matter. Ingaseous atomic and molecular media, it has been extensively studied and is verywell-understood. In solids research is ongoing, but a consensus is forming forthe dominant microscopic HHG mechanisms. In liquids on the other hand, noestablished theory yet exit and approaches developed for gases and solids aregenerally inapplicable, hindering our current understanding. We develop here apowerful and reliable ab-initio cluster-based approach for describing thenonlinear interactions between isotropic bulk liquids and intense laser pulses.The scheme is based on time-dependent density functional theory and utilizesseveral approximations that make it feasible yet accurate in realistic systems.We demonstrate our approach with HHG calculations in water, ammonia, andmethane liquids, and compare the characteristic response of polar and non-polarliquids. We identify unique features in the HHG spectra of liquid methane thatcould be utilized for ultrafast spectroscopy of its chemical and physicalproperties: (i) a structural minima at 15-17eV, and (ii) a well-like shape inthe perturbative region that is reminiscent of a shape resonance. Our resultspave the way to accessible calculations of HHG in liquids and illustrate theunique nonlinear nature of liquid systems.

Ab-initio cluster approach for high-harmonic generation in liquids