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Nathalie Picqué

Publications and source records attributed to Nathalie Picqué.

At least 19 recordsLinked to original sources

Three-dimensional hyperspectral imaging with optical microcombs

Optical frequency combs have revolutionised time and frequency metrology [1, 2]. The advent of microresonator-based frequency combs ('microcombs' [3-5]) is set to lead to the miniaturisation of devices that are ideally suited to a wide range of applications, including microwave generation [6, 7], ranging [8-10], the precise calibration of astronomical spectrographs [11], neuromorphic computing [12, 13], high-bandwidth data communications[14], and quantum-optics [15, 16] platforms. Here, we introduce a new microcomb application for three-dimensional imaging. Our method can simultaneously determine the chemical identity and full three-dimensional geometry, including size, shape, depth, and spatial coordinates, of particulate matter ranging from micrometres to millimetres in size across nearly $10^5$ distinct image pixels. We demonstrate our technique using millimetre-sized plastic specimens (i.e. microplastics measuring less than 5 mm). We combine amplitude and phase analysis and achieve a throughput exceeding $1.2~10^6$ pixels per second with micrometre-scale precision. Our method leverages the defining feature of microcombs - their large line spacing - to enable precise spectral diagnostics using microcombs with a repetition frequency of 1 THz. Our results suggest scalable operation over several million pixels and nanometre-scale axial resolution. Coupled with its high-speed, label-free and multiplexed capabilities, our approach provides a promising basis for environmental sensing, particularly for the real-time detection and characterisation of microplastic pollutants in aquatic ecosystems [17].

physics.optics↗

Near-ultraviolet photon-counting dual-comb spectroscopy

Ultraviolet spectroscopy provides unique insights into the structure of matter with applications ranging from fundamental tests to photochemistry in the earth's atmosphere and astronomical observations from space telescopes. At longer wavelengths, dual-comb spectroscopy with two interfering laser frequency combs has evolved into a powerful technique that can offer simultaneously a broad spectral range and very high resolution. Here we demonstrate a photon-counting approach that can extend the unique advantages of this method into ultraviolet regions where nonlinear frequency-conversion tends to be very inefficient. Our spectrometer, based on two frequency combs of slightly different repetition frequencies, provides broad span, high resolution, frequency calibration within the accuracy of an atomic clock, and overall consistency of the spectra. We demonstrate a signal-to-noise ratio at the quantum limit and optimal use of the measurement time, provided by the multiplex recording of all spectral data on a single photo-counter. Our initial experiments are performed in the near-ultraviolet and in the visible spectral ranges with alkali-atom vapor, with a power per comb line as low as a femtowatt. This crucial step towards precision broadband spectroscopy at short wavelengths clears the path to extreme-ultraviolet dual-comb spectroscopy and, more generally, generates a new realm of applications for diagnostics at photon level, as encountered e.g., when driving single atoms or molecules.

physics.optics↗

Time-resolved dual-comb spectroscopy with a single electro-optic modulator

Time-resolved near-infrared absorption spectroscopy of single non-repeatable transient events is performed at high spectral resolution with a dual-comb interferometer using a continuous-wave laser followed by a single electro-optic amplitude modulator. By sharing high-speed electrical/optical components, our spectrometer greatly simplifies the implementation of dual-comb spectroscopy and it offers a high mutual coherence time, measured up to 50-s, without any active stabilization system and/or data processing. The time resolution, which can be reconfigured a posteriori, is as short 100 microseconds in our experimental demonstration. For a span of 36 GHz, the mean signal-to-noise ratio of 80, at 100-MHz spectral resolution and 100-microsecond measurement time, enables the precise determination of the parameters of rovibrational lines, including intensity or concentration.

physics.optics↗

Dual-Comb Hyperspectral Digital Holography

Holography has always held special appeal, for it is able to record and display spatial information in three dimensions. Here, we show how to augment the capabilities of digital holography by using a large number of narrow laser lines at precisely-defined optical frequencies simultaneously. Using an interferometer based on two frequency combs of slightly different repetition frequencies and a lens-less camera sensor, we record time-varying spatial interference patterns that generate spectral hypercubes of complex holograms, revealing, for each comb line frequency, amplitudes and phases of scattered wave-fields. Unlike with previous multi-color holography and low-coherence holography (including with a frequency comb), the unique synergy of broad spectral bandwidth and high temporal coherence in dual-comb holography opens up novel optical diagnostics, such as precise dimensional metrology over large distances without interferometric phase ambiguity, or hyperspectral 3-dimensional imaging with high spectral resolving power, as we illustrate by molecule-selective imaging of an absorbing gas.

physics.optics↗

Roadmap on multimode light shaping

Our ability to generate new distributions of light has been remarkably enhanced in recent years. At the most fundamental level, these light patterns are obtained by ingeniously combining different electromagnetic modes. Interestingly, the modal superposition occurs in the spatial, temporal as well as spatio-temporal domain. This generalized concept of structured light is being applied across the entire spectrum of optics: generating classical and quantum states of light, harnessing linear and nonlinear light-matter interactions, and advancing applications in microscopy, spectroscopy, holography, communication, and synchronization. This Roadmap highlights the common roots of these different techniques and thus establishes links between research areas that complement each other seamlessly. We provide an overview of all these areas, their backgrounds, current research, and future developments. We highlight the power of multimodal light manipulation and want to inspire new eclectic approaches in this vibrant research community.

physics.optics↗

An on-chip III-V-semiconductor-on-silicon laser frequency comb for gas-phase molecular spectroscopy in real-time

Frequency combs, spectra of evenly-spaced narrow phase-coherent laser lines, have revolutionized precision measurements. On-chip frequency comb generators hold much promise for fully-integrated instruments of time and frequency metrology. While outstanding developments are being reported with Kerr, quantum cascade and microring electro-optic combs, the field of high-resolution multiplexed gas-phase spectroscopy has remained inaccessible to such devices, because of their large line spacing, their small number of usable comb lines, the intensity variations between their comb lines, and their limited photonic integrability. Here we identify a path to broadband gas-phase spectroscopy on a chip. We design a low-noise III-V-on-silicon comb generator on a photonic chip, that emits a flat-top spectrum of 1400 lines at a repetition frequency of 1.0 GHz, a feature never approached by other ultra-miniaturized comb synthesizers. With dual-comb spectroscopy, our near-infrared electrically-pumped laser records high-resolution (1 GHz) sensitive multiplexed spectra with resolved comb lines, in times as short as 5 microseconds. Isotope-resolved 12C/13C detection in carbon monoxide is performed within 1 millisecond. With further developments, entire high-resolution spectroscopy laboratories-on-a-chip may be manufactured at the wafer scale. In environmental sensing, broad networks of spectrometers could be densely field-deployed to simultaneously monitor, in real time, sources and sinks of greenhouse gases, industrial pollution or noxious emissions of motor vehicles.

physics.optics↗

Dual-comb thin-disk oscillator

For the first time to our knowledge, a dual-comb laser based on thin-disk technology and its application to direct frequency comb spectroscopy are presented. The peak power (0.6 MW) and the average power (12 W) of our Yb:YAG thin-disk dual-comb system are more than one-order-of-magnitude higher than in any previous systems. The scheme allows easy adjustment of the repetition frequency difference during operation. A time-domain signal recorded over 10 μs without any active stabilization was sufficient to resolve individual comb lines after Fourier transformation. The demonstration should enable a wider adoption of dual-comb systems towards practical applications in research laboratories. Its simplicity and compactness especially for the realization of tri- and multi-comb systems and conversion into the still poorly covered UV and VUV ranges makes it a promising next-generation technology.

physics.optics↗

Upconversion mid-infrared dual-comb spectroscopy

We devise a new detection technique for mid-infrared multi-heterodyne spectroscopy. As an experimental implementation, mid-infrared light interrogates a gas sample in the 3-$μ$m region of the fundamental CH, OH, NH stretch in molecules and detection is performed in the near-infrared telecommunication region. Spectra showing 18000 resolved comb lines of 100-MHz spacing are recorded at a sensitivity close to the shot-noise limit. The demonstration adds to the unique advantages of dual-comb spectroscopy, such as potential very high resolution, negligible instrumental line width, and direct calibration of the frequency scale with an atomic clock. We also show that direct mid-infrared detection with a differential photo-detector module is beneficial in the limit of low mid-infrared average power.

physics.optics↗

An integrated lithium-niobate electro-optic platform for spectrally tailored dual-comb spectroscopy

A high-resolution broad-spectral-bandwidth spectrometer on a chip would create new opportunities for gas-phase molecular fingerprinting, especially in environmental sensing. A resolution high enough to observe transitions at atmospheric pressure and the simultaneous sensitive detection of multiple atoms or molecules are the key challenges. Here, an electro-optic microring-based dual-comb interferometer, fabricated on a low-loss lithium-niobate-on-insulator nanophotonic platform, demonstrates significant progress towards such an achievement. Spectra spanning 1.6 THz (53 cm-1) at a resolution of 10 GHz (0.33 cm-1) are obtained in a single measurement without requiring frequency scanning or moving parts. The frequency agility of the system enables spectrally-tailored multiplexed sensing, which allows for interrogation of non-adjacent spectral regions, here separated by 6.6 THz (220 cm-1), without compromising the signal-to-noise ratio.

physics.app-ph↗

On-chip mid-infrared and THz frequency combs for spectroscopy

Frequency combs have revolutionized time and frequency metrology and in recent years, new frequency comb lasers that are highly compact or even on-chip have been demonstrated in the mid-infrared and THz regions of the electromagnetic spectrum. The emerging technologies include electrically pumped quantum and interband cascade semiconductor devices, as well as high-quality factor microresonators. In this guest editorial, the authors summarize recent advances in the field, the potential for rapid broadband spectroscopy, as well as the challenges and prospects for use in molecular gas sensing.

physics.optics↗

Single-photon interferometry and spectroscopy with two laser frequency combs

We demonstrate single-photon time-domain interference in a new realm. We observe interferences in the photon counting statistics with two separate mode-locked femtosecond lasers of slightly different repetition frequencies, each emitting a comb of evenly spaced spectral lines over a wide spectral span. We exploit the interference pattern for spectroscopic diagnostics over a broad spectral range. An experimental proof-of-concept shows that the emerging technique of high-resolution dual-comb Fourier transform spectroscopy can be performed at light powers that are a billion-fold weaker than those commonly employed. Our experiments challenge the intuitive concept that a photon exists before detection and they open the prospect of precise spectroscopy over broad spectral bandwidth in light-starved conditions.

physics.optics↗

Frequency comb spectroscopy

A laser frequency combs is a broad spectrum composed of equidistant narrow lines. Initially invented for frequency metrology, such combs enable new approaches to spectroscopy over broad spectral bandwidths, of particular relevance to molecules. With optical frequency combs, the performance of existing spectrometers, such as Michelson-based Fourier transform interferometers or crossed dispersers, involving e.g. virtual imaging phase array (VIPA) étalons, is dramatically enhanced. Novel types of instruments, such as dual-comb spectrometers, lead to a new class of devices without moving parts for accurate measurements over broad spectral ranges. The direct self-calibration of the frequency scale of the spectra within the accuracy of an atomic clock and the negligible contribution of the instrumental line-shape will enable determinations of all spectral parameters with high accuracy for stringent comparisons with theories in atomic and molecular physics. Chip-scale frequency-comb spectrometers promise integrated devices for real-time sensing in analytical chemistry and biomedicine. This review article gives a summary of advances in the emerging and rapidly advancing field of atomic and molecular broadband spectroscopy with frequency combs.

physics.optics↗

Mid-infrared feed-forward dual-comb spectroscopy at 3 $μ$m

Mid-infrared high-resolution spectroscopy has proven an invaluable tool for the study of the structure and dynamics of molecules in the gas phase. The advent of frequency combs advances the frontiers of precise molecular spectroscopy. Here we demonstrate, in the important 3-μm spectral region of the fundamental CH stretch in molecules, dual-comb spectroscopy with experimental coherence times between the combs that exceed half-an-hour. Mid-infrared Fourier transform spectroscopy using two frequency combs with self-calibration of the frequency scale, negligible contribution of the instrumental line-shape to the spectral profiles, high signal-to-noise ratio and broad spectral bandwidth opens up novel opportunities for precision spectroscopy of small molecules. Highly multiplexed metrology of line shapes may be envisioned.

physics.optics↗

Doppler-free Fourier transform spectroscopy

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.

physics.optics↗

A phase-stable dual-comb interferometer

Improvements to dual-comb interferometers will benefit precision spectroscopy and sensing, distance metrology, tomography, telecommunications etc. A specific requirement of such interferometers is to enforce mutual coherence between the two combs over the measurement time. With feed-forward relative stabilization of the carrier-enveloppe offset frequencies, we experimentally realize such mutual coherence over times that exceed 300 seconds, two orders of magnitude longer than state-of-the-art systems. Illustration is given with near-infrared Fourier transform molecular spectroscopy, where two combs of slightly different repetition frequencies replace a scanning two-beam interferometer. Our technique can be implemented with any frequency comb generators including microresonators or quantum cascade lasers.

physics.optics↗

Silicon-chip-based mid-infrared dual-comb spectroscopy

On-chip spectroscopy that could realize real-time fingerprinting with label-free and high-throughput detection of trace molecules is one of the 'holy grails" of sensing. Such miniaturized spectrometers would greatly enable applications in chemistry, bio-medicine, material science or space instrumentation, such as hyperspectral microscopy of live cells or pharmaceutical quality control. Dual-comb spectroscopy (DCS), a recent technique of Fourier transform spectroscopy without moving parts, is particularly promising since it measures high-precision spectra in the gas phase using only a single detector. Here, we present a microresonator-based platform designed for mid-infrared (mid-IR) DCS. A single continuous-wave (CW) low-power pump source generates two mutually coherent mode-locked frequency combs spanning from 2.6 $μ$m to 4.1 $μ$m in two silicon micro-resonators. Thermal control and free-carrier injection control modelocking of each comb and tune the dual-comb parameters. The large line spacing of the combs (127 GHz) and its precise tuning over tens of MHz, unique features of chip-scale comb generators, are exploited for a proof-of-principle experiment of vibrational absorption DCS in the liquid phase, with spectra of acetone spanning from 2870 nm to 3170 nm at 127-GHz (4.2-cm$^{-1}$) resolution. We take a significant step towards a broadband, mid-IR spectroscopy instrument on a chip. With further system development, our concept holds promise for real-time and time-resolved spectral acquisition on the nanosecond time scale.

physics.optics↗

Dual-Comb Coherent Raman Spectroscopy with Lasers of 1-GHz Pulse Repetition Frequency

We extend the technique of multiplex coherent Raman spectroscopy with two femtosecond mode-locked lasers to oscillators of a pulse repetition frequency of 1 GHz. We demonstrate spectra of liquids, which span 1100 cm$^{-1}$ of Raman shifts. At a resolution of 6 cm$^{-1}$, their measurement time may be as short as 5 microseconds for a refresh rate of 2 kHz. The waiting period between acquisitions is improved ten-fold compared to previous experiments with two lasers of 100-MHz repetition frequencies.

physics.optics↗

Mid-infrared dual-comb spectroscopy with electro-optic modulators

We demonstrate dual-comb spectroscopy based on difference frequency generation of frequency-agile near-infrared frequency combs, produced with the help of electro-optic modulators. The combs have a remarkably flat intensity distribution and their positions and line spacings can be selected freely by simply dialing a knob. We record, in the 3-micron region, Doppler-limited absorption spectra with resolved comb lines within milliseconds. Precise molecular line parameters are retrieved. Our technique holds promise for fast and sensitive time-resolved studies e.g. of trace gases.

physics.optics↗