Sub-cycle control of terahertz high-harmonic generation by dynamical Bloch oscillations

Ultrafast charge transport in strongly biased semiconductors is at the heart of high-speed electronics, electro-optics and fundamental solid-state physics1,2,3,4,5,6,7,8,9,10,11,12,13. Intense light pulses in the terahertz spectral range have opened fascinating vistas14,15,16,17,18,19,20,21. Because terahertz photon energies are far below typical electronic interband resonances, a stable electromagnetic waveform may serve as a precisely adjustable bias5,11,17,19. Novel quantum phenomena have been anticipated for terahertz amplitudes, reaching atomic field strengths8,9,10. We exploit controlled (multi-)terahertz waveforms with peak fields of 72 MV cm−1 to drive coherent interband polarization combined with dynamical Bloch oscillations in semiconducting gallium selenide. These dynamics entail the emission of phase-stable high-harmonic transients, covering the entire terahertz-to-visible spectral domain between 0.1 and 675 THz. Quantum interference of different ionization paths of accelerated charge carriers is controlled via the waveform of the driving field and explained by a quantum theory of inter- and intraband dynamics. Our results pave the way towards all-coherent terahertz-rate electronics. Terahertz waveforms with peak fields of 72 MV cm−1 and a central frequency of 30 THz drive interband polarization in bulk GaSe off-resonantly and accelerate excited electron–hole pairs, inducing dynamical Bloch oscillations. This results in the emission of phase-stable, high-harmonic transients over the whole frequency range of 0.1–675 THz.