Intense, carrier frequency and bandwidth tunable quasi single-cycle pulses from an organic emitter covering the Terahertz frequency gap

In Terahertz (THz) science, one of the long-standing challenges has been the formation of spectrally dense, single-cycle pulses with tunable duration and spectrum across the frequency range of 0.1–15 THz (THz gap). This frequency band, lying between the electronically and optically accessible spectra hosts important molecular fingerprints and collective modes which cannot be fully controlled by present strong-field THz sources. We present a method that provides powerful single-cycle THz pulses in the THz gap with a stable absolute phase whose duration can be continuously selected between 68 fs and 1100 fs. The loss-free and chirp-free technique is based on optical rectification of a wavelength-tunable pump pulse in the organic emitter HMQ-TMS that allows for tuning of the spectral bandwidth from 1 to more than 7 octaves over the entire THz gap. The presented source tunability of the temporal carrier frequency and spectrum expands the scope of spectrally dense THz sources to time-resolved nonlinear THz spectroscopy in the entire THz gap. This opens new opportunities towards ultrafast coherent control over matter and light.