Resonance-enhanced optical nonlinearity in the Weyl semimetal TaAs

Abstract

The second-order conductivity of a material, ${\ensuremath{\sigma}}^{(2)}$, relating current to the square of electric field, is nonzero only when inversion symmetry is broken, unlike the conventional linear conductivity. Second-order nonlinear optical responses are thus powerful tools in basic research as probes of symmetry breaking; they are also central to optical technology as the basis for generating photocurrents and frequency doubling. The recent surge of interest in Weyl semimetals with acentric crystal structures has led to the discovery of a host of ${\ensuremath{\sigma}}^{(2)}$-related phenomena in this class of materials, such as polarization-selective conversion of light to dc current (photogalvanic effects) and the observation of giant second-harmonic generation (SHG) efficiency in TaAs at photon energy 1.5 eV. Here, we present measurements of the SHG spectrum of TaAs, revealing that the response at 1.5 eV corresponds to the high-energy tail of a resonance at 0.7 eV, at which point the second harmonic conductivity is approximately 200 times larger than seen in the standard candle nonlinear crystal, GaAs. This remarkably large SHG response provokes the question of ultimate limits on ${\ensuremath{\sigma}}^{(2)}$, which we address by a new theorem relating frequency-integrated nonlinear response functions to the third cumulant (or ``skewness'') of the polarization distribution function in the ground state.