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Register a new userMid-Infrared Cross-Comb Spectroscopy
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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.
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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.
We present a new method for accurate mid-infrared frequency measurements and stabilization to a near-infrared ultra-stable frequency reference, transmitted with a long-distance fibre link and continuously monitored against state-of-the-art atomic fountain clocks. As a first application, we measure the frequency of an OsO4 rovibrational molecular line around 10 $mu$m with a state-of-the-art uncertainty of 8x10-13. We also demonstrate the frequency stabilization of a mid-infrared laser with fractional stability better than 4x10-14 at 1 s averaging time and a line-width below 17 Hz. This new stabilization scheme gives us the ability to transfer frequency stability in the range of 10-15 or even better, currently accessible in the near-infrared or in the visible, to mid-infrared lasers in a wide frequency range.
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.
The method of Doppler - free comb - spectroscopy for dipole transitions was proposed. The calculations for susceptibility spectrum for moving two-level atoms driving by strong counter propagating combs have been done. The used theoretical method based on the Fourier expansion of the components of density matrix on two rows on kv (v-velocity of group of atoms, k-projection of wave vector) and {Omega} (frequency between comb components). For testing of validity of this method the direct numerical integration was done. The narrow peaks with homogeneous width arise on the background of Doppler counter. The contrast of these peaks is large for largest amplitudes of comb-components. Power broadening is increasing with increase of field amplitudes. The spectral range of absorption spectrum is determined by the spectral range of comb generator and all homogeneous lines arise simultaneously. The spectral resolution is determined by the width of homogeneously-broadening lines. The physical nature of narrow peaks is in the existence of multi-photon transitions between manifolds of quasi-energy levels arising for different groups of atoms moving with velocities that satisfy to the resonant conditions 2kv= (n+l){Omega}, where n, l - are integers and {Omega} - frequency difference between comb teeth.
We demonstrate a high-accuracy dual-comb spectrometer centered at 3.4 mu m. The amplitude and phase spectra of the P, Q, and partial R-branch of the methane { u}3 band are measured at 25 MHz to 100 MHz point spacing with ~kHz resolution and a signal-to-noise ratio of up to 3500. A fit of the absorbance and phase spectra yield the center frequency of 132 rovibrational lines. The systematic uncertainty is estimated to be 300 kHz, which is 10-3 of the Doppler width and a tenfold improvement over Fourier transform spectroscopy. These data are the first high- accuracy molecular spectra obtained with a direct comb spectrometer.
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