High-sensitivity Frequency Comb Carrier-Envelope-Phase Metrology in Solid State High Harmonic Generation

TL;DR

This paper demonstrates a highly sensitive, phase-sensitive method for high harmonic generation in solid state crystals using a low-energy frequency comb, enabling detailed ultrafast spectroscopy with high signal-to-noise ratio.

Contribution

It introduces a novel carrier-envelope amplitude modulation spectroscopy technique utilizing a 100 MHz Erbium-fiber frequency comb for phase-sensitive harmonic generation in solids.

Findings

Achieved harmonic spectra as short as 200 nm in a single pass.

Demonstrated phase-sensitive modulation with 85 dB SNR.

Verified non-perturbative harmonic generation via polarization gating.

Abstract

Non-perturbative and phase-sensitive light-matter interactions have led to the generation of attosecond pulses of light and the control electrical currents on the same timescale. Traditionally, probing these effects via high harmonic generation has involved complicated lasers and apparatuses to generate the few-cycle and high peak power pulses needed to obtain and measure spectra that are sensitive to the phase of the light wave. Instead, we show that nonlinear effects dependent on the carrier-envelope phase can be accessed in solid state crystals with simple low-energy frequency combs that we combine with high-sensitivity demodulation techniques to measure harmonic spectral modulations. Central to this advance is the use of a scalable 100 MHz Erbium-fiber frequency comb at 1550 nm to produce 10 nJ, 20 fs pulses which are focused to the TW/cm2 level. In a single pass through a 500 {\mu}m ZnO crystal this yields harmonic spectra as short as 200 nm. With this system, we introduce a technique of carrier-envelope amplitude modulation spectroscopy (CAMS) and use it to characterize the phase-sensitive modulation of the ultraviolet harmonics with 85 dB signal-to-noise ratio. We further verify the non-perturbative nature of the harmonic generation through polarization gating of the driving pulse to increase the effects of the carrier-envelope phase. Our work demonstrates robust and ultra-sensitive methods for generating and characterizing harmonic generation at 100 MHz rates that should provide advantages in the study of attosecond nonlinear processes in solid state systems. Additionally, as a simple and low-noise frequency comb, this broadband source will be useful for precision dual-comb spectroscopy of a range of physical systems across the ultraviolet and visible spectral regions (200 - 650 nm).