Higher-harmonic generation in boron-doped silicon from band carriers and bound-dopant photoionization

We investigate ultrafast harmonic generation (HG) in Si: B, driven by intense pump pulses with fields reaching∼ 100 kV cm− 1 and a carrier frequency of 300 GHz, at 4 K and 300 K, both experimentally and theoretically. We report several findings concerning the nonlinear charge carrier dynamics in intense sub-THz fields:(i) Harmonics of order up to n= 9 are observed at room temperature, while at low temperature we can resolve harmonics reaching at least n= 11. The susceptibility per charge carrier at moderate field strength is as high as for charge carriers in graphene, considered to be one of the materials with the strongest sub-THz nonlinear response.(ii) For T= 300 K, where the charge carriers bound to acceptors are fully thermally ionized into the valence subbands, the susceptibility values decrease with increasing field strength. Simulations incorporating multi-valence-band Monte Carlo and finite-difference-time-domain (FDTD) propagation show that here, the HG process becomes increasingly dominated by energy-dependent scattering rates over the contribution from band nonparabolicity, due to the onset of optical-phonon emission, which ultimately leads to the saturation at high fields. (iii) At T=4K, where the majority of charges are bound to acceptors, we observe a drastic rise of the HG yields for internal pump fields of ∼30kVcm−1, as one reaches the threshold for tunnel ionization. We disentangle the HG nonlinear response into contributions associated with the initial photoionization and subsequent motion in the bands, and show that intracycle scattering seriously degrades any contribution to HG emission from coherent recollision of the holes with their parent ions.