Cavity-Enhanced Ultrafast Transient Absorption Spectroscopy

Abstract

We present a new technique using a frequency comb laser and optical cavities for performing ultrafast transient absorption spectroscopy with improved sensitivity. Resonantly enhancing the probe pulses, we demonstrate a sensitivity of $\Delta$OD $ = 1 \times 10^{-9}/\sqrt{\mbox{Hz}}$ for averaging times as long as 30 s per delay point ($\Delta$OD${}_{min}=2\times 10^{-10}$). Resonantly enhancing the pump pulses allows us to produce a high excitation fraction at high repetition-rate, so that signals can be recorded from samples with optical densities as low as OD $\approx 10^{-8}$, or column densities $<10^{10}$ molecules/cm${}^2$. This high sensitivity enables new directions for ultrafast spectroscopy.

References in corpus (11)

• Mid-infrared frequency combs
• Electrodynamics of Correlated Electron Materials
• Cavity-enhanced dual-comb spectroscopy
• Human breath analysis via cavity-enhanced optical frequency comb spectroscopy
• Quantum-noise-limited optical frequency comb spectroscopy
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• Cavity-enhanced optical frequency comb spectroscopy in the mid-infrared - application to trace detection of H2O2
• The Impact of Dispersion on Amplitude and Frequency Noise in a Yb-fiber Laser Comb
• Simple piezoelectric-actuated mirror with 180 kHz servo bandwidth
• Spatial distribution of ions in a linear octopole radio-frequency ion trap in the space-charge limit
• Cavity-enhanced field-free molecular alignment at a high repetition rate

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• Tunable visible frequency combs from a Yb-fiber-laser-pumped optical parametric oscillator
• Simulating Ultrafast Transient Absorption Spectra from First Principles using a Time-Dependent Configuration Interaction Probe
• A Cavity-Enhanced Spectroscopist's Lens on Molecular Polaritons
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• Interferometric Differential High-Frequency Lock-In Probe for Laser-Induced Vacuum Birefringence
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