Ab initio calculations of the high-order harmonic enhancement in small noble-gas clusters

We report calculations of the high-order harmonic spectra of few-atomic clusters of two noble gases, helium and krypton, subjected to laser pulses of intensities above 1013 W/cm2. We employ a fully ab intio framework, namely, the real-time time-dependent configuration interaction singles coupled to a discrete Gaussian basis set. Our model reproduces the observed higher-than-quadratic dependence between the high-order harmonic yield and the number of atoms, and the obtained value of the enhancement rate is in quantitative agreement with experimental results. We suggest a mechanism responsible for the high-order harmonic enhancement, according to which, after the tunneling ionization, the residual ion polarizes the electron densities of surrounding atoms in the cluster, which leads to increased electron-electron repulsion during the recollision. The proposed mechanism is not only fully consistent with both our calculations and the experimental data, but can also explain the limitations of previous theoretical studies on high-order harmonic generation in clusters.