Design and Applications of a Decade-Spanning Terahertz Frequency Comb Spectrometer: Doppler-limited Rotational Spectroscopy of Methanol and Methanol-OD

This thesis details the design and applications of a terahertz (THz) frequency comb spectrometer. The spectrometer employs two offset locked Ti:Sapphire femtosecond oscillators with repetition rates of approximately 80 MHz, offset locked at 100 Hz to continuously sample a time delay of 12.5 ns at a maximum time delay resolution of 15.6 fs. These oscillators emit continuous pulse trains, allowing the generation of a THz pulse train by the master, or pump, oscillator and the sampling of this THz pulse train by the slave, or probe, oscillator via the electro-optic effect. Collecting a train of 16 consecutive THz pulses and taking the Fourier transform of this pulse train produces a decade-spanning frequency comb, from 0.25 to 2.5 THz, with a comb tooth width of 5 MHz and a comb tooth spacing of ~80 MHz. This frequency comb is suitable for Doppler-limited rotational spectroscopy of small molecules. Here, the data from 68 individual scans at slightly different pump oscillator repetition rates were combined, producing an interleaved THz frequency comb spectrum, with a maximum interval between comb teeth of 1.4 MHz, enabling THz frequency comb spectroscopy.

The accuracy of the THz frequency comb spectrometer was tested, achieving a root mean square error of 92 kHz measuring selected absorption center frequencies of water vapor at 10 mTorr, and a root mean square error of 150 kHz in measurements of a K-stack of acetonitrile. This accuracy is sufficient for fitting of measured transitions to a model Hamiltonian to generate a predicted spectrum for molecules of interest in the fields of astronomy and physical chemistry. As such, the rotational spectra of methanol and methanol-OD were acquired by the spectrometer. Absorptions from 1.3 THz to 2.0 THz were compared to JPL catalog data for methanol and the spectrometer achieved an RMS error of 402 kHz, improving to 303 kHz when excluding low signal-to-noise absorptions. This level of accuracy compares favorably with the ~100 kHz accuracy achieved by JPL frequency multiplier submillimeter spectrometers. Additionally, the relative intensity performance of the THz frequency comb spectrometer is linear across the entire decade-spanning bandwidth, making it the preferred instrument for recovering lineshapes and taking absolute intensity measurements in the THz region. The data acquired by the Terahertz Frequency Comb Spectrometer for methanol-OD is of comparable accuracy to the methanol data and may be used to refine the fit parameters for the predicted spectrum of methanol-OD.

Nonlinear optics in planar silica-on-silicon disk resonators

Optical frequency combs (OFCs) provide direct phase-coherent link between optical and RF frequencies, and enable precision measurement of optical frequencies. In recent years, a new class of frequency combs (microcombs) have emerged based on parametric frequency conversions in dielectric microresonators. Micocombs have large line spacing from 10's to 100's GHz, allowing easy access to individual comb lines for arbitrary waveform synthesis. They also provide broadband parametric gain bandwidth, not limited by specific atomic or molecular transitions in conventional OFCs. The emerging applications of microcombs include low noise microwave generation, astronomical spectrograph calibration, direct comb spectroscopy, and high capacity telecommunications.

In this thesis, research is presented starting with the introduction of a new type of chemically etched, planar silica-on-silicon disk resonator. A record Q factor of 875 million is achieved for on-chip devices. A simple and accurate approach to characterize the FSR and dispersion of microcavities is demonstrated. Microresonator-based frequency combs (microcombs) are demonstrated with microwave repetition rate less than 80 GHz on a chip for the first time. Overall low threshold power (as low as 1 mW) of microcombs across a wide range of resonator FSRs from 2.6 to 220 GHz in surface-loss-limited disk resonators is demonstrated. The rich and complex dynamics of microcomb RF noise are studied. High-coherence, RF phase-locking of microcombs is demonstrated where injection locking of the subcomb offset frequencies are observed by pump-detuning-alignment. Moreover, temporal mode locking, featuring subpicosecond pulses from a parametric 22 GHz microcomb, is observed. We further demonstrated a shot-noise-limited white phase noise of microcomb for the first time. Finally, stabilization of the microcomb repetition rate is realized by phase lock loop control.

For another major nonlinear optical application of disk resonators, highly coherent, simulated Brillouin lasers (SBL) on silicon are also demonstrated, with record low Schawlow-Townes noise less than 0.1 Hz^2/Hz for any chip-based lasers and low technical noise comparable to commercial narrow-linewidth fiber lasers. The SBL devices are efficient, featuring more than 90% quantum efficiency and threshold as low as 60 microwatts. Moreover, novel properties of the SBL are studied, including cascaded operation, threshold tuning, and mode-pulling phenomena. Furthermore, high performance microwave generation using on-chip cascaded Brillouin oscillation is demonstrated. It is also robust enough to enable incorporation as the optical voltage-controlled-oscillator in the first demonstration of a photonic-based, microwave frequency synthesizer. Finally, applications of microresonators as frequency reference cavities and low-phase-noise optomechanical oscillators are presented.