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Competition and cooperation among orders is at the heart of many-body physicsin strongly correlated materials and leads to their rich physical properties.It is crucial to investigate what impact many-body physics has on extremenonlinear optical phenomena, with the possibility of controlling materialproperties by light. However, the effect of competing orders andelectron-electron correlations on highly nonlinear optical phenomena has notyet been experimentally clarified. Here, we investigated high-order harmonicgeneration from the Mott-insulating phase of Ca2RuO4. Changing the gap energyin Ca2RuO4 as a function of temperature, we observed a strong enhancement ofhigh order harmonic generation at 50 K, increasing up to several hundred timescompared to room temperature. We discovered that this enhancement can bewell-reproduced by an empirical scaling law that depends only on the materialgap energy and photon emission energy. Such scaling law cannot be explained bya simple two-band model under the single electron approximation. Our resultssuggest that the highly nonlinear optical response of strongly correlatedmaterials is deeply coupled to their electron-electron correlations andresultant many-body electronic structure.

High-order Harmonic Generation and its Unconventional Scaling Law in the Mott-insulating $\rm{Ca_2RuO_4}$