Ultrafast giant enhancement of second harmonic generation in a strongly correlated cobaltite

We report the observation of ultrafast photoinduced giant enhancement of optical second harmonic generation (SHG) efficiency in cobaltite YbBaCo4O7. Upon femtosecond pumping at energies above the band gap, the system exhibits an ultrafast enhancement in SHG intensity, reaching up to 60 % higher than the initial value, then decays into a long-lived excited state maintaining the enhancement. The enhancement scales linearly with pump fluence but shows no dependence on pump polarization. A pure electronic process sets in within the first ~200 fs and is accompanied by a pronounced anisotropic amplification of nonlinear susceptibility. We propose this anomalous SHG enhancement originates from ultrafast electronic band renormalization arising from dynamical modification of electron correlations. Our findings open a new avenue for ultrafast optical control of nonlinear properties in strongly correlated materials.