Abstract
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.
Highlights
IntroductionThe loss-free spectral tuning of bandwidth and carrier frequency is based on adjusting the pump laser’s wavelength
The loss-free spectral tuning of bandwidth and carrier frequency is based on adjusting the pump laser’s wavelength. This simple approach represents an important advance over modern laser and accelerator based high-field T-ray sources as it offers chirp-free mono-cycle THz pulses adjustable between 68 fs and 1100 fs
We demonstrated the production of transform-limited, single-cycle THz pulses with tunable bandwidth and tunable carrier frequency by controlling the exceptional phase-matching conditions in the organic crystal HMQ-TMS via a wavelength-tunable pump pulse
Summary
The loss-free spectral tuning of bandwidth and carrier frequency is based on adjusting the pump laser’s wavelength This simple approach represents an important advance over modern laser and accelerator based high-field T-ray sources as it offers chirp-free mono-cycle THz pulses adjustable between 68 fs and 1100 fs (i.e. carrier frequency between 0.8 and 15 THz). To our best knowledge such extensive tunability in pulse duration (while keeping the pulse duration at its transform-limit) is unique and not provided by any other T-ray source. This opens novel opportunities in the emerging field of impulsive THz science as it enables a parametric match of the stimulus’ carrier oscillation frequency to the response time of the induced dynamics
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