We evaluate the spectral performance of a novel continuous-wave room-temperature distributed feedback quantum cascade laser operating at the long wavelength of 17 $μ$m. By demonstrating broadband laser absorption spectroscopy of the $ν$2 fundamental vibrational mode of N2O molecules, we have determined the spectral range and established the spectroscopic potential of this laser. We have characterized the frequency noise and measured the line width of this new device, uncovering a discrepancy with the current consensus on the theoretical modeling of quantum cascade lasers. Our results confirm the potential of such novel narrow-line-width sources for vibrational spectroscopy. Extending laser spectroscopy to longer wavelength is a fascinating prospect that paves the way for a wide range of opportunities from chemical detection, to frequency metrology as well as for exploring light-matter interaction with an extended variety of molecules, from ultra-cold diatomic species to increasingly complex molecular systems.
Demonstration and frequency noise characterization of a 17 μm quantum cascade laser
We evaluate the spectral performance of a novel continuous-wave room-temperature distributed feedback quantum cascade laser operating at the long wavelength of 17 μm. By demonstrating broadband laser absorption spectroscopy of the ν2 fundamental vibrational mode of N2O molecules, we have determined the spectral range and established the spectroscopic potential of this laser. We have characterized the frequency noise and measured the line width of this new device, uncovering a discrepancy with the current consensus on the theoretical modeling of quantum cascade lasers. Our results confirm the potential of such novel narrow-line-width sources for vibrational spectroscopy. Extending laser spectroscopy to longer wavelength is a fascinating prospect that paves the way for a wide range of opportunities from chemical detection, to frequency metrology as well as for exploring light-matter interaction with an extended variety of molecules, from ultra-cold diatomic species to increasingly complex molecular systems.
We developed a fiber-laser-pumped Ti:sapphire laser system designed for quantum precision measurement applications. By employing a 35 W single-frequency 532 nm fiber laser as the pump source, the system delivered continuous-wave output powers of 4.12 W at 770.108 nm (D 1 line, K), 4.72 W at 780.244 nm (D 2 line, Rb), and 5.29 W at 794.982 nm (D 1 line, Rb), thereby fulfilling the requirements for optical pumping and probing of alkali atoms. To enhance frequency stability, saturated absorption spectroscopy was used to lock the laser frequency, resulting in frequency drifts below 1 MHz over two hours. Furthermore, since low-frequency intensity noise (DC-100 Hz) critically affects spin-relaxation-free quantum sensing, we carried out a theoretical analysis which identified the pump laser as the dominant noise source. By implementing feedback control to the pump source as well as an external noise suppression, both methods achieved over 30 dB of intensity noise suppression within the DC-4kHz frequency range. In addition, improved beam pointing stability further reduced noise below 3 Hz. These results collectively demonstrate the system’s strong potential for quantum sensing applications.
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.
Tunable single-frequency lasers are essential for high-resolution spectroscopy and quantum technologies, yet achieving narrow-linewidth performance in compact, scalable systems across the UV-visible spectrum remains a key challenge. Recent work has revealed that Raman scattering in diamond can act as a natural spectral squeezer, where phonon dynamics help suppress frequency noise and concentrates optical power into a single, narrow spectral mode. Experiments at CERN and elsewhere have demonstrated linewidth compression by orders of magnitude, frequency-noise suppression exceeding 10³-10⁴, and pathways toward Schawlow–Townes-limited performance in CW regimes. These results establish Raman phonon damping as a universal mechanism for generating ultra-coherent, widely tunable lasers, opening new opportunities in quantum metrology, optical clocks, and high-resolution spectroscopy.
Tunable single-frequency lasers are essential for high-resolution spectroscopy and quantum technologies, yet achieving narrow-linewidth performance in compact, scalable systems across the UV-visible spectrum remains a key challenge. Recent work has revealed that Raman scattering in diamond can act as a natural spectral squeezer, where phonon dynamics help suppress frequency noise and concentrates optical power into a single, narrow spectral mode. Experiments at CERN and elsewhere have demonstrated linewidth compression by orders of magnitude, frequency-noise suppression exceeding 10³-10⁴, and pathways toward Schawlow–Townes-limited performance in CW regimes. These results establish Raman phonon damping as a universal mechanism for generating ultra-coherent, widely tunable lasers, opening new opportunities in quantum metrology, optical clocks, and high-resolution spectroscopy.
Spectroscopy in the mid-infrared region is an indispensable tool for identifying molecular types in various fields, including physics, chemistry, and medical sciences. However, conventional infrared light sources, detectors, and noise from blackbody radiation have been the obstacles to miniaturization and higher sensitivity of infrared spectrometers. Quantum infrared spectroscopy, which uses visible and infrared photon pairs in a quantum entangled state, has attracted attention as a new sensing technology that enables infrared spectroscopy with detectors in the visible range. However, the bandwidth of conventional quantum entangled light sources is at most 1 µm or less, which hinders broadband measurements, which are important in spectroscopic applications. Here we have realized an ultra-broadband entangled state of visible–infrared photons with wavelengths from 2 to 5 µm, harnessing a specially designed nonlinear crystal with chirped poling structure inside. Furthermore, we constructed a nonlinear quantum interferometer using the ultra-broadband quantum entangled photons and realized broadband infrared spectroscopy of inorganic and organic materials using a visible detector made of silicon. Our results show that quantum infrared spectroscopy can achieve ultra-broadband spectroscopic measurements and pave the way for the highly sensitive, ultra-compact infrared spectrometers using quantum entangled photons.
High Resolution Image Download MS PowerPoint Slide Numerous molecules exhibit unique absorption bands in the “fingerprint” infrared (IR) region, allowing chemical identification and detection. This makes IR spectroscopy an essential tool in biomedical diagnostics, sensing, and material characterization. However, measurements in the IR range are challenging due to the relatively poor performance, need for cryogenic cooling, and high cost of IR light sources and photodetectors. Here, we demonstrate that the mid-IR fingerprints of the sample can be revealed from measurements in the near-IR range using conventional silicon photodetectors. Our approach relies on the quantum interference of correlated photon pairs produced in strong frequency nondegenerate parametric down-conversion. Our technique simultaneously measures the absorption coefficient and refractive index in the broad “fingerprint” region with high accuracy. As a proof-of-concept, we perform spectroscopy of nitrous oxide gas in the 7.4 to 8.4 μm wavelength range, with the detection in the 865 to 877 nm range. This work extends the applicability of quantum interferometry to a range of broad practical appeals, such as detection of atmosphere pollutants, breath diagnostics, chemical safety, and others.