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Microresonator-based soliton frequency combs - microcombs - have recently emerged to offer low-noise, photonic-chip sources for optical measurements. Owing to nonlinear-optical physics, microcombs can be built with various materials and tuned or stabilized with a consistent framework. Some applications require phase stabilization, including optical-frequency synthesis and measurements, optical-frequency division, and optical clocks. Partially stabilized microcombs can also benefit applications, such as oscillators, ranging, dual-comb spectroscopy, wavelength calibration, and optical communications. Broad optical bandwidth, brightness, coherence, and frequency stability have made frequency-comb sources important for studying comb-matter interactions with atoms and molecules. Here, we explore direct microcomb atomic spectroscopy, utilizing a cascaded, two-photon 1529-nm atomic transition of rubidium. Both the microcomb and the atomic vapor are implemented with planar fabrication techniques to support integration. By fine and simultaneous control of the repetition rate and carrier-envelope-offset frequency of the soliton microcomb, we obtain direct sub-Doppler and hyperfine spectroscopy of the $4^2D_{5/2}$ manifold. Moreover, the entire set of microcomb modes are stabilized to this atomic transition, yielding absolute optical-frequency fluctuations of the microcomb at the kilohertz-level over a few seconds and < 1 MHz day-to-day accuracy. Our work demonstrates atomic spectroscopy with microcombs and provides a rubidium-stabilized microcomb laser source, operating across the 1550 nm band for sensing, dimensional metrology, and communication.
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Spectroscopy in the molecular fingerprint spectral region (6.5-20 $mu$m) yields critical information on material structure for physical, chemical and biological sciences. Despite decades of interest and effort, this portion of the electromagnetic spectrum remains challenging to cover with conventional laser technologies. In this report, we present a simple and robust method for generating super-octave, optical frequency combs in the fingerprint region through intra-pulse difference frequency generation in an orientation-patterned gallium phosphide crystal. We demonstrate the utility of this unique coherent light source for high-precision, dual-comb spectroscopy in methanol and ethanol vapor. These results highlight the potential of laser frequency combs for a wide range of molecular sensing applications, from basic molecular spectroscopy to nanoscopic imaging.
Dual-comb spectroscopy has been proven a powerful tool in molecular characterization, which remains challenging to implement in the mid-infrared (MIR) region due to difficulties in the realization of two mutually locked comb sources and efficient photodetection. An effective way to overcome those limitations is optical upconversion; however, previously reported configurations are either demanding or inefficient. Here we introduce and experimentally demonstrate a variant of dual-comb spectroscopy called cross-comb spectroscopy, in which a MIR comb is upconverted via sum-frequency generation (SFG) with a near-infrared (NIR) comb with a shifted repetition rate and then interfered with a spectral extension of the NIR comb. We experimentally demonstrate a proof-of-concept measurement of atmospheric CO2 around 4.25 micrometer, with a 350-nm instantaneous bandwidth and 25000 resolved comb lines. Cross-comb spectroscopy can be realized using up- or down-conversion and offers an adaptable and efficient alternative to dual-comb spectroscopy outside the well-developed near-IR region, where having two mutually coherent sources and efficient photodetection is challenging. Moreover, the nonlinear gating in cross-comb spectroscopy promises a superior dynamic range compared to dual-comb spectroscopy.
We analyze several possibilities for precisely measuring electronic transitions in atomic helium by the direct use of phase-stabilized femtosecond frequency combs. Because the comb is self-calibrating and can be shifted into the ultraviolet spectral region via harmonic generation, it offers the prospect of greatly improved accuracy for UV and far-UV transitions. To take advantage of this accuracy an ultracold helium sample is needed. For measurements of the triplet spectrum a magneto-optical trap (MOT) can be used to cool and trap metastable 2^3S state atoms. We analyze schemes for measuring the two-photon $2^3S to 4^3S$ interval, and for resonant two-photon excitation to high Rydberg states, $2^3S to 3^3P to n^3S,D$. We also analyze experiments on the singlet-state spectrum. To accomplish this we propose schemes for producing and trapping ultracold helium in the 1^1S or 2^1S state via intercombination transitions. A particularly intriguing scenario is the possibility of measuring the $1^1S to 2^1S$ transition with extremely high accuracy by use of two-photon excitation in a magic wavelength trap that operates identically for both states. We predict a ``triple magic wavelength at 412 nm that could facilitate numerous experiments on trapped helium atoms, because here the polarizabilities of the 1^1S, 2^1S and 2^3S states are all similar, small, and positive.
We demonstrate coherent storage and retrieval of pulsed light using the atomic frequency comb quantum memory protocol in a room temperature alkali vapour. We utilise velocity-selective optical pumping to prepare multiple velocity classes in the $F=4$ hyperfine ground state of caesium. The frequency spacing of the classes is chosen to coincide with the $F=4 - F=5$ hyperfine splitting of the $6^2$P$_{3/2}$ excited state resulting in a broadband periodic absorbing structure consisting of two usually Doppler-broadened optical transitions. Weak coherent states of duration $2,mathrm{ns}$ are mapped into this atomic frequency comb with pre-programmed recall times of $8,mathrm{ns}$ and $12,mathrm{ns}$, with multi-temporal mode storage and recall demonstrated. Utilising two transitions in the comb leads to an additional interference effect upon rephasing that enhances the recall efficiency.
Microresonator Kerr frequency combs, which rely on third-order nonlinearity ($chi^{(3)}$), are of great interest for a wide range of applications including optical clocks, pulse shaping, spectroscopy, telecommunications, light detection and ranging (LiDAR) and quantum information processing. Many of these applications require further spectral and temporal control of the generated frequency comb signal, which is typically accomplished using additional photonic elements with strong second-order nonlinearity ($chi^{(2)}$). To date these functionalities have largely been implemented as discrete off-chip components due to material limitations, which come at the expense of extra system complexity and increased optical losses. Here we demonstrate the generation, filtering and electro-optic modulation of a frequency comb on a single monolithic integrated chip, using a thin-film lithium niobate (LN) photonic platform that simultaneously possesses large $chi^{(2)}$ and $chi^{(3)}$ nonlinearities and low optical losses. We generate broadband Kerr frequency combs using a dispersion-engineered high quality factor LN microresonator, select a single comb line using an electrically programmable add-drop filter, and modulate the intensity of the selected line. Our results pave the way towards monolithic integrated frequency comb solutions for spectroscopy data communication, ranging and quantum photonics.
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