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 (πF)2∼105, where 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. %\begin{wrapfigure}{I}{1\textwidth} % \centering % \includegraphics[width = 0.7\textwidth]{CETAS_details.eps} %\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.} %\end{wrapfigure}
The measurement and manipulation of coherent optical fields have been transformed by the optical frequency comb. Today, the optical frequency comb grants measurements precise enough to count individual cycles of light as well as the generation of nearly any coherent electromagnetic field from the ultraviolet through the infrared. These capabilities have enabled the most precise realizations and comparisons of time, precision spectroscopy over broad bandwidths, and the ability to convert stable signals between optical and microwave fields–seamlessly connecting the entire electromagnetic spectrum from hertz (100 ) to petahertz (1015). These applications involve the interference of a frequency comb with another coherent light source, such as another frequency comb or a single-frequency continuous-wave laser. However, coherent light represents only one type of light. The vast majority of light emanates from “black bodies” such as stars, which is in a thermal state as opposed to a coherent state, and carries profound information about the universe and humanity’s place within it. Other types of light defy classical electromagnetism and are known as non-classical or quantum light. Such quantum light may play central roles in quantum communication, quantum computation, and quantum-enhanced metrology. In this thesis, the use of the optical frequency comb in the interferometric measurement of thermal and quantum light is investigated, with a focus on assessing fundamental limits to the sensitivity of such measurements. In order to measure thermal light, a technique called dual-comb correlation spectroscopy is explored. This technique entails heterodyne measurement of the field of thermal light and subsequent correlation of the field in time. This process reveals the spectrum of thermal light at high resolution and across broad bandwidths. New theoretical work uncovers previously unknown fundamental limits on sensitivity when measuring realistically weak thermal light. Experimental investigation verifies this scaling and is accompanied by a demonstration of spectroscopy at the equivalent power spectral density of our Sun, realizing a greater than 1000-fold sensitivity increase over past demonstrations of this technique. These insights pave the way for expansion of this technique to comb-based spatial correlation of thermal fields. This advancement would allow for extended baseline synthetic aperture hyperspectral imaging throughout the optical spectrum, facilitating novel and profound observations of the universe. The use of frequency combs for the measurement of quantum light is also investigated. This scenario breaks typical quantum optics assumptions, such as large, mode-matched local oscillators, and necessitates new quantum measurement operators. Such measurement operators are derived, which not only describe homodyne measurements on any quantum state of light with a frequency comb local oscillator, but also indicate that the shot noise limit generally reached in comb-based measurements of coherent light (such as in continuous-wave laser heterodyne and dual-comb spectroscopy) does not correspond to the quadrature or coherent state-overlap description standard in quantum optics. Efforts to experimentally reach this “standard” quantum limit demonstrate a significant improvement in the signal-to-noise ratio over the conventional comb-based shot noise limit, paving the way for lower-power portable optical clocks and quantum-enhanced frequencycomb metrology.