Ab initio calculations of the linear and nonlinear susceptibilities of N2 , O2 , and air in midinfrared laser pulses

Abstract

We present first-principles calculations of the linear and nonlinear susceptibilities of N$_2$, O$_2$, and air in the mid-infrared wavelength regime, from $1-4$ $\mu$m. We extract the frequency-dependent susceptibilities from the full time-dependent dipole moment that is calculated using time-dependent density functional theory. We find good agreement with curves derived from experimental results for the linear susceptibility, and with measurements for the nonlinear susceptibility up to 2.4 $\mu$m. We also find that the susceptibilities are insensitive to the laser intensity even in the strong field regime up to $5\times 10^{13}$ W/cm$^2$. Our results will allow accurate calculations of the long-distance propagation of intense MIR laser pulses in air.