Frequency combs enable precision measurements across timekeeping, spectroscopy, ranging and astronomy, and are now extending to integrated and field-deployable platforms. Realizing their full performance demands a comprehensive account of the quantum noise that arises when broadband optical fields are converted into finite-bandwidth electrical signals. Here we present a rigorous first-principles quantum-mechanical framework for optical frequency-comb metrology based on continuous-mode field quantization and a comb-line-resolved description of quantum fluctuations. The theory describes how quantum fluctuations of the comb field are transduced into electrical measurement noise. We apply the framework to two canonical settings, optical frequency division (OFD) and dual-comb spectroscopy (DCS), where it reveals two effects beyond semiclassical reach: a dependence of the OFD standard quantum limit on the comb spectral envelope, and a cyclostationary noise penalty that obstructs straightforward squeezing in DCS. These insights identify practical, resource-efficient routes to quantum enhancement through engineered comb states, laying a foundation for the design of next-generation frequency combs operating at and beyond standard quantum limits.
Frequency combs enable precision measurements across timekeeping, spectroscopy, ranging and astronomy, and are now extending to integrated and field-deployable platforms. Realizing their full performance demands a comprehensive account of the quantum noise that arises when broadband optical fields are converted into finite-bandwidth electrical signals. Here we present a rigorous first-principles quantum-mechanical framework for optical frequency-comb metrology based on continuous-mode field quantization and a comb-line-resolved description of quantum fluctuations. The theory describes how quantum fluctuations of the comb field are transduced into electrical measurement noise. We apply the framework to two canonical settings, optical frequency division (OFD) and dual-comb spectroscopy (DCS), where it reveals two effects beyond semiclassical reach: a dependence of the OFD standard quantum limit on the comb spectral envelope, and a cyclostationary noise penalty that obstructs straightforward squeezing in DCS. These insights identify practical, resource-efficient routes to quantum enhancement through engineered comb states, laying a foundation for the design of next-generation frequency combs operating at and beyond standard quantum limits.
Optical frequency combs have emerged as a cornerstone for a wide range of areas, including spectroscopy, ranging, optical clocks, time and frequency transfer, waveform synthesis, and communications. However, quantum-mechanical fluctuations of the optical carrier impose fundamental performance limits on the precision of classical optical frequency combs, particularly in their use for interferometry and spectroscopy. Entanglement, as a quintessential quantum resource, allows for surpassing the fundamental limits of classical systems. Here, we introduce entanglement into the realm of optical frequency combs, formulating entangled dual-comb spectroscopy (EDCS) that surmounts the fundamental limits of classical DCS. EDCS capitalizes on tailored entangled structures across the frequency comb, enabling simultaneous detection of all comb lines below the standard quantum limit of classical DCS. Applying EDCS in gas detection, we achieve a 2.6-dB enhancement in signal-to-noise ratio and a 1.7-fold reduction in integration time over classical DCS, rendering EDCS particularly suited for dynamic chemical and biological sensing, where fast, precise measurements subject to power constraints are required. EDCS opens a new avenue for exploiting quantum frequency combs, underscoring their prospects in a plethora of applications in precision metrology, spectroscopy, and timekeeping.
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.
Optical frequency combs, named for their comblike peaks in the spectrum, are essential for various sensing applications. As the technology develops, its performance has reached the standard quantum limit dictated by the quantum fluctuations of coherent light field. Quantum combs, with their quantum fluctuation engineered via squeezing and entanglement, are the necessary ingredient for overcoming such limits. We develop the theory for designing and analyzing quantum combs, focusing on dual-comb interferometric measurement. Our analyses cover both squeezed and entangled quantum combs with division receivers and heterodyne receivers, leading to four protocols with quantum advantages scalable with squeezing/entanglement strength. In the spectroscopy of a single absorption line, the division receiver with the squeezed comb suffers from entanglement-mismatching-induced amplified noise, while the other three protocols demonstrate a surprising robustness to loss at a few comb lines. Such a unique loss-robustness of a scalable quantum advantage has not been found in any traditional quantum sensing protocols.
The fields of precision timekeeping and spectroscopy increasingly rely on optical-frequency-comb interferometry. However, comb-based measurements are not described by existing quantum theory because they exhibit both large mode mismatch and finite-strength local oscillators. To establish this quantum theory, we derive measurement operators for homodyne detection with arbitrary mode overlap. These operators are a combination of quadrature and intensity-like measurements, which inform a filter that maximizes the quadrature-measurement signal-to-noise ratio. Furthermore, these operators establish a foundation to extend frequency-comb interferometry to a wide range of scenarios, including metrology with nonclassical states of light.
Precision metrology is one application of optical frequency combs. Classical noise in their properties typically limits achievable measurement sensitivity. Amplitude and phase noise in optical frequency combs have already been studied extensively. So far, noise sidebands close to the carrier of either individual optical frequencies or of the mean field have been considered. This thesis develops methods to precisely characterize amplitude and phase noise down to the quantum limit. To this aim a transmissive, broadband passive cavity is developed. It filters and inter-converts amplitude and phase noise. The analysis of its signal by the use of homodyne detection provides a quantum limited measurement of phase noise. The application of ultrafast pulse shaping enables the measurement of the spectral correlations of amplitude and phase noise. Being represented by the use of covariance matrices, the entire noise correlations over the optical spectrum are characterized on the example of a Ti:Sapph oscillator. The measured noise correlations exhibit spectral structures, so-called modes. Their shape matches with the theoretical prediction. This concept known from multi-partite optical quantum systems is consequently applicable to classical noise in frequency combs. The knowledge of the intrinsic noise modes is likely provide an improvement of precision metrology experiments with combs.
Abstract Dual-comb spectroscopy (DCS) is a powerful technique for spectroscopic sensing, offering exceptional resolution, precision, and speed. However, its performance is fundamentally limited by quantum noise inherent to coherent-state optical combs. Here, we overcome this barrier by introducing quantum correlation-enhanced DCS using correlated twin combs generated via seeded four-wave mixing. One comb acts as a local oscillator to decode molecular signals, while the twin suppresses shot noise through intensity-difference squeezing, achieving a 2 dB signal-to-noise ratio improvement beyond the shot-noise limit—equivalent to a 2.6× measurement speed enhancement. Notably, when paired with up-conversion spectroscopy, our approach achieves comb-line-resolved, high-resolution spectra (0.0067 cm⁻¹, 7.5 pm) in the critical 3 μm region for molecular fingerprinting. These results bridge quantum optics and frequency comb spectroscopy, offering great potential for trace gas detection, precision metrology, and chemical analysis. Future developments in detector efficiency and nanophotonic integration could further enhance its scalability and impact.