Cavity-enhanced Ultrafast Transient Absorption Spectroscopy

Abstract

We introduce cavity enhanced ultrafast transient absorption spectroscopy, which employs frequency combs and high-finesse optical cavities. % The schematic of apparatus is shown in Figure 1.

Sub-100 fs pulses with a repetition rate of 90 MHz are generated by a home-built Ytterbium fiber laser. The amplified light has a power up to 10 W, which is used to pump an optical parametric oscillator, followed by second-harmonic generation(SHG) that converts the wavelength from near-IR to visible. A pump comb at 530 nm is separately generated by SHG. Both pump and probe combs are coupled into high-finesse cavities. Compared to the conventional transient absorption spectroscopy method, the detection sensitivity can be improved by a factor of $\left(\frac{\mathcal{F}}{\pi} \right)^2 \sim 10^5$, where $\mathcal{F}$ is the finesse of cavity. This ultrasensitive technology enables the direct all-optical dynamics study in molecular beams. We will apply the cavity enhanced ultrafast transient absorption spectroscopy to investigate the dynamics of visible chromophores and then extend the wavelength to mid-IR to study vibrational dynamics of small hydrogen-bonded clusters.

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%\caption{Schematic of cavity enhanced ultrafast transient absorption spectroscopy apparatus. An amplified fiber laser frequency comb is converted to visible light and pump and probe combs are coupled to high-finesse optical resonators. Transmission of the probe light is measured.}

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