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Nathalie Picqué

Publications and source records attributed to Nathalie Picqué.

At least 37 records · Page 2Linked to original sources
arXiv2015

Frequency-agile dual-comb spectroscopy

We propose a new approach to near-infrared molecular spectroscopy, harnessing advanced concepts of optical telecommunications and supercontinuum photonics. We generate, without mode-locked lasers, two frequency combs of slightly different repetition frequencies and moderate, but rapidly tunable, spectral span. The output of a frequency-agile continuous wave laser is split and sent into two electro-optic intensity modulators. Flat-top low-noise frequency combs are produced by wave-breaking in a nonlinear optical fiber of normal dispersion. With a dual-comb spectrometer, we record Doppler-limited spectra spanning 60 GHz within 13 microseconds and 80-kHz refresh rate, at a tuning speed of 10 nm.s^(-1). The sensitivity for weak absorption is enhanced by a long gas-filled hollow-core fiber.

physics.optics↗
arXiv2014

Few-cycle, Broadband, Mid-infrared Optical Parametric Oscillator Pumped by a 20-fs Ti:sapphire Laser

We report a few-cycle, broadband, singly-resonant optical parametric oscillator (OPO) for the mid-infrared based on MgO-doped periodically-poled LiNbO3 (MgO:PPLN), synchronously pumped by a 20-fs Ti:sapphire laser. By using crystal interaction lengths as short as 250 um, and careful dispersion management of input pump pulses and the OPO resonator, near-transform-limited, few-cycle idler pulses tunable across the mid-infrared have been generated, with as few as 3.7 optical cycles at 2682 nm. The OPO can be continuously tuned over 2179-3732 nm by cavity delay tuning, providing up to 33 mW of output power at 3723 nm. The idler spectra exhibit stable broadband profiles with bandwidths spaning over 422 nm (FWHM) recorded at 3732 nm. We investigate the effect of crystal length on spectral bandwidth and pulse duration at a fixed wavelength, confirming near-transform-limited idler pulses for all grating interaction lengths. By locking the repetition frequency of the pump laser to a radio-frequency reference, and without active stabilization of the OPO cavity length, an idler power stability better than 1.6% rms over >2.75 hours is obtained when operating at maximum output power, in excellent spatial beam quality with TEM00 mode profile.

physics.optics↗
arXiv2014

Differential femtosecond coherent Stokes and anti-Stokes Raman spectroscopy

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.

physics.optics↗
arXiv2013

Broadband high-resolution two-photon spectroscopy with laser frequency combs

Two-photon excitation spectroscopy with broad spectral span is demonstrated at Doppler-limited resolution. We describe first Fourier transform two-photon spectroscopy of an atomic sample with two mode-locked laser oscillators in a dual-comb technique. Each transition is uniquely identified by the modulation imparted by the interfering comb excitations. The temporal modulation of the spontaneous two-photon fluorescence is monitored with a single photodetector, and the spectrum is revealed by a Fourier transform.

physics.optics↗
arXiv2013

Coherent Raman spectro-imaging with laser frequency combs

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.

physics.optics↗
arXiv2012

Adaptive real-time dual-comb spectroscopy

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.

physics.optics↗
arXiv2012

Adaptive dual-comb spectroscopy in the green region

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.

physics.optics↗
arXiv2012

Raman-induced Kerr-effect dual-comb spectroscopy

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.

physics.optics↗
arXiv2012

Mid-infrared frequency combs

Laser frequency combs are coherent light sources that emit a broad spectrum consisting of discrete, evenly spaced narrow lines, each having an absolute frequency measurable within the accuracy of an atomic clock. Their development, a decade ago, in the near-infrared and visible domains has revolutionized frequency metrology with numerous windfalls into other fields such as astronomy or attosecond science. Extension of frequency comb techniques to the mid-infrared spectral region is now under exploration. Versatile mid-infrared frequency comb generators, based on novel laser gain media, nonlinear frequency conversion or microresonators, promise to significantly expand the tree of applications of frequency combs. In particular, novel approaches to molecular spectroscopy in the fingerprint region, with dramatically improved precision, sensitivity, recording time and/or spectral bandwidth may spark off new discoveries in the various fields relevant to molecular sciences.

physics.optics↗
arXiv2009

Cavity-enhanced dual-comb spectroscopy

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.

physics.optics↗
arXiv2008

Molecular fingerprinting with femtosecond lasers

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.

physics.optics↗
arXiv2007

Supercontinua for high resolution absorption multiplex infrared spectroscopy

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.

physics.optics↗
arXiv2007

Infrared frequency combs and supercontinua for multiplex high sensitivity spectroscopy

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.

physics.optics↗
arXiv2007

Sensitive multiplex spectroscopy in the molecular fingerprint 2.4 $μ$m region with a Cr^{2+}:ZnSe femtosecond laser

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.

physics.optics↗
arXiv2007

Frequency modulation Fourier transform spectroscopy

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.

physics.optics↗
arXiv2007

Femtosecond laser Fourier transform absorption spectroscopy

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.

physics.optics↗