arXiv subjects
Publications and source records attributed to Guy Guelachvili.
The feasibility of sub-Doppler broadband multi-heterodyne spectroscopy with two laser frequency combs is demonstrated with two-photon excitation spectra of the 5S-5D transitions of rubidium vapor.
We demonstrate a novel technique of coherent Raman spectroscopy with a femtosecond laser. We apply to a molecular sample a sequence of pairs of ultrashort excitation and probe pulses, with a linearly increasing time delay between the two pulses from one pair to the next. We measure, as a function of the delay, the intensity modulation in the signal resulting from the differential detection of the Stokes and anti-Stokes radiations generated at the sample. The Fourier transform of such time-domain signal reveals the spectrum of the excited vibrational Raman transitions. The experimental proof-of-principle demonstrates high resolution, broad spectral span and suppression of the non-resonant background, as well as sensitivity enhancement due to the differential detection.
We characterize a new mid-infrared frequency comb generator based on difference frequency generation around 3.2 microns. High power per comb mode (>10-7 W/mode) is obtained over a broad spectral span (>700 nm). The source is used for direct absorption spectroscopy with a Michelson-based Fourier transform interferometer.
Optical spectroscopy and imaging of microscopic samples have opened up a wide range of applications throughout the physical, chemical, and biological sciences. High chemical specificity may be achieved by directly interrogating the fundamental or low-lying vibrational energy levels of the compound molecules. Amongst the available prevailing label-free techniques, coherent Raman scattering has the distinguishing features of high spatial resolution down to 200 nm and three-dimensional sectioning. However, combining fast imaging speed and identification of multiple - and possibly unexpected- compounds remains challenging: existing high spectral resolution schemes require long measurement times to achieve broad spectral spans. Here we overcome this difficulty and introduce a novel concept of coherent anti-Stokes Raman scattering (CARS) spectro-imaging with two laser frequency combs. We illustrate the power of our technique with high resolution (4 cm-1) Raman spectra spanning more than 1200 cm-1 recorded within less than 15 microseconds. Furthermore, hyperspectral images combining high spectral (10 cm-1) and spatial (2 micrometers) resolutions are acquired at a rate of 50 pixels per second. Real-time multiplex accessing of hyperspectral images may dramatically expand the range of applications of nonlinear microscopy.
With the advent of laser frequency combs, coherent light sources that offer equally-spaced sharp lines over a broad spectral bandwidth have become available. One decade after revolutionizing optical frequency metrology, frequency combs hold much promise for significant advances in a growing number of applications including molecular spectroscopy. Despite its intriguing potential for the measurement of molecular spectra spanning tens of nanometers within tens of microseconds at Doppler-limited resolution, the development of dual-comb spectroscopy is hindered by the extremely demanding high-bandwidth servo-control conditions of the laser combs. Here we overcome this difficulty. We experimentally demonstrate a straightforward concept of real-time dual-comb spectroscopy, which only uses free-running mode-locked lasers without any phase-lock electronics, a posteriori data-processing, or the need for expertise in frequency metrology. The resulting simplicity and versatility of our new technique of adaptive dual-comb spectroscopy offer a powerful transdisciplinary instrument that may spark off new discoveries in molecular sciences.
Dual-comb spectroscopy is extended to the visible spectral range with a set-up based on two frequency-doubled femtosecond ytterbium-doped fiber lasers. The dense rovibronic spectrum of iodine around 19240 cm-1 is recorded within 12 ms at Doppler-limited resolution with a simple scheme that only uses free-running femtosecond lasers.
We report on the first demonstration of nonlinear dual-frequency-comb spectroscopy. In multi-heterodyne femtosecond Raman-induced Kerr-effect spectroscopy, the Raman gain resulting from the coherent excitation of molecular vibrations by a spectrally-narrow pump is imprinted onto the femtosecond laser frequency comb probe spectrum. The birefringence signal induced by the nonlinear interaction of these beams and the sample is heterodyned against a frequency comb local oscillator with a repetition frequency slightly different from that of the comb probe. Such time-domain interference provides multiplex access to the phase and amplitude Raman spectra over a broad spectral bandwidth within a short measurement time. Experimental demonstration, at a spectral resolution of 200 GHz, a measurement time of 293 μs and a sensitivity of 10^-6, is given on liquid samples exhibiting a C-H stretch Raman shift.
The sensitivity of molecular fingerprinting is dramatically improved when placing the absorbing sample in a high-finesse optical cavity, thanks to the large increase of the effective path-length. As demonstrated recently, when the equidistant lines from a laser frequency comb are simultaneously injected into the cavity over a large spectral range, multiple trace-gases may be identified within a few milliseconds. Analyzing efficiently the light transmitted through the cavity however still remains challenging. Here, a novel approach, cavity-enhanced frequency comb Fourier transform spectroscopy, fully overcomes this difficulty and measures ultrasensitive, broad-bandwidth, high-resolution spectra within a few tens of $μ$s. It could be implemented from the Terahertz to the ultraviolet regions without any need for detector arrays. We recorded, within 18 $μ$s, spectra of the 1.0 $μ$m overtone bands of ammonia spanning 20 nm with 4.5 GHz resolution and a noise-equivalent-absorption at one-second-averaging per spectral element of 3 10^-12 cm^-1Hz^-1/2, thus opening a route to time-resolved spectroscopy of rapidly-evolving single-events.
Molecular fingerprinting through absorption spectroscopy is a powerful analytical method. Wide spectral ranges are explored with Doppler-limited resolution. Fast data acquisition, accurate measurements of frequency, intensity, and line shape; time-resolved, selective spectra are achieved with excellent sensitivities. However, presently spectrometers are unable to provide all these features at once.
A TiCl_4/He plasma is observed by high resolution double-modulation FTS using concentration-modulation as a selective detection method. Analysis of the C ^4Δ- X ^4 ΦΔv=0 transitions of ^48Ti^35Cl reveals perturbations affecting the C ^4Δ_{1/2} sub-state.
Supercontinua generated in highly non-linear fibers by ultrashort-pulse lasers can be used for high resolution Fourier transform absorption spectroscopy. The practical advantages of these bright ultrabroadband light sources for spectroscopy are reported in the near-infrared region. A Cr^4+:YAG femtosecond laser broadened by an extruded soft-glass photonic crystal fiber, emitting from 1200 to 2200 nm and from 675 to 950 nm, provides a spectral radiance being 1x10^5 times higher than that of a 3000 K blackbody and 10^2 times higher than that of a synchrotron radiation. The C_2H_2 and NH_3 overtone spectra are recorded using this source within a few seconds.
An infrared high-brightness light source based on supercontinuum generation through a SF6 photonic crystal fiber seeded by a Cr^4+:YAG femtosecond oscillator is developed for high resolution multiplex spectroscopy in the 1.5 $μ$m region. Moreover, a multiplex high resolution approach based on a Cr^4+:YAG frequency comb enables to probe large spectral domains, with simultaneous sensitive measurement of the absorption and the dispersion associated with all individual spectral features.
An ultrashort-pulse Cr^{2+}:ZnSe laser is a novel broadband source for sensitive high resolution molecular spectroscopy. A 130-fs pulse allows covering of up to 380 cm^-1 spectral domain around 2.4 $μ$m which is analyzed simultaneously with a 0.12 cm^-1 (3.6 GHz) resolution by a Fourier-transform spectrometer. Recorded in 13 s, from 70-cm length absorption around 4150 cm^-1, acetylene and ammonia spectra exhibit a 3800 signal-to-noise ratio and a 2.4*10^-7 cm^-1*Hz^-1/2 noise equivalent absorption coefficient at one second averaging per spectral element, suggesting a 0.2 ppbv detection level for HF molecule. With the widely practiced classical tungsten lamp source instead of the laser, identical spectra would have taken more than one hour.
A new method, FM-FTS, combining Frequency Modulation heterodyne laser spectroscopy and Fourier Transform Spectroscopy is presented. It provides simultaneous sensitive measurement of absorption and dispersion profiles with broadband spectral coverage capabilities. Experimental demonstration is made on the overtone spectrum of C2H2 in the 1.5 $μ$m region.
A femtosecond mode-locked laser is used for the first time as a broadband infrared source for high resolution Fourier transform absorption spectroscopy. Demontration is made with a Cr^4+:YAG laser. The entire nu_1+nu_3 vibration-rotation band region of acetylene, observed after passing through a single pass 80-cm long cell, is simultaneously recorded between 1480 and 1600 nm, in 7.9 s with a signal to noise ratio equal to 1000. Two hot bands of the most abundant acetylene isotopologue and the n1+n3 band of the ^13C^12CH_2 are also present. The noise equivalent absorption coefficient at one second averaging is equal to 7 10^{-7} cm^{-1}.Hz^{-1/2} per spectral element.
A room temperature operating Vertical External Cavity Surface Emitting Laser is applied around 1550 nm to intracavity laser absorption spectroscopy analyzed by time-resolved Fourier transform interferometry. At an equivalent pathlength of 15 km, the high resolution spectrum of the semiconductor disk laser emission covers 17 nm simultaneously. A noise equivalent absorption coefficient at one second averaging equal to 1.5 10^{-10} cm^{-1}.Hz^{-1/2} per spectral element is reported for the 65 km longest path length employed.
Spectra comprised of hundreds of time-components for absorption path lengths up to 130 km have been recorded around 1050 nm by combining two recent techniques, intracavity laser spectroscopy with vertical external cavity surface emitting multiple-quantum-well lasers and time-resolved Fourier transform spectroscopy. A sensitivity of 1 10^{-10} cm^{-1}.Hz^{-1/2} is achieved, for simultaneously acquired 10^4 spectral elements, three orders of magnitude better than the sensitivity obtained in previous similar experiments. Specific advantages of the method, especially for frequency and intensity metrology of weak absorption transitions, are discussed.
Previously unobserved nitrous oxide transitions around 2.5 $μ$m are measured by intracavity laser absorption spectroscopy (ICLAS) analyzed by time-resolved Fourier transform (TRFT) spectrometer. With an accuracy of the order of 10^-3 cm^-1, measured positions of 1637 assigned weak transitions are provided. They belong to 42 vibrational transitions, among which 33 are observed for the first time. These data are believed to be useful in particular to monitoring atmosphere purposes.