Multiheterodyne techniques using frequency combs -- light sources whose lines are perfectly evenly-spaced -- have revolutionized optical science. By beating an unknown signal with the many lines of a comb, its spectrum is recovered. However, these techniques have been restricted to measuring coherent sources, such as lasers. In this work, we demonstrate a new multiheterodyne technique that allows for nearly any complex broadband spectrum to be retrieved using a comb. Two versions are introduced: a delayed comb technique that uses a tunable delay element, and a dual comb technique that uses a second comb. In each case, the spectrum of the source is recovered by Fourier transforming the correlation between two spectrograms. This approach is statistical in nature and is general to nearly any source (coherent or incoherent), allowing for the entire spectrum to be rapidly measured with high resolution.
Femtosecond dual-comb lasers have revolutionized linear Fourier-domain spectroscopy by offering a rapid motion-free, precise and accurate measurement mode with easy registration of the combs beat note in the RF domain. Extensions of this technique found already application for nonlinear time-resolved spectroscopy within the energy limit available from sources operating at the full oscillator repetition rate. Here, we present a technique based on time filtering of femtosecond frequency combs by pulse gating in a laser amplifier. This gives the required boost to the pulse energy and provides the…
We demonstrated combination of gapless terahertz (THz) comb with dual-comb spectroscopy, namely gapless dual-THz-comb spectroscopy, to achieve the spectral resolution equal to width of the THz comb tooth. The gapless THz comb was realized by interpolating frequency gaps between the comb teeth with sweeping of a laser mode-locked frequency. The demonstration of low-pressure gas spectroscopy with gapless dual-THz-comb spectroscopy clearly indicated that the spectral resolution was decreased down to 2.5-MHz width of the comb tooth and the spectral accuracy was enhanced to 10-6 within the spectral…
Single-shot ultrafast absorbance spectroscopy based on the frequency encoding of the kinetics is analyzed theoretically and implemented experimentally. In Part II of the series, arbitrary thickness sample is analysed theroretically. The model is then used to simulate the results for a-Si:H films.
We experimentally demonstrate four-wave-mixing spectroscopy using frequency combs. The experiment uses a geometry where excitation pulses and four-wave-mixing signals generated by a sample co-propagate. We separate them in the radio frequency domain by heterodyne detection with a local oscillator comb that has a different repetition frequency.
Electron energy-loss spectroscopy (EELS) and cathodoluminescence (CL) are widely used experimental techniques for characterization of nanoparticles. The discrete dipole approximation (DDA) is a numerically exact method for simulating interaction of electromagnetic waves with particles of arbitrary shape and internal structure. In this work we extend the DDA to simulate EELS and CL for particles embedded into arbitrary (even absorbing) unbounded host medium. The latter includes the case of the dense medium, supporting the Cherenkov radiation of the electron, which has never been considered in E…
Rapid characterization of optical and vibrational spectra with high resolution can identify species in cluttered environments and is important for assays and early alerts. In this regard, dual-comb spectroscopy has emerged as a powerful approach to acquire nearly instantaneous Raman and optical spectra with unprecedented resolution. Spectra are generated directly in the electrical domain and avoid bulky mechanical spectrometers. Recently, a miniature soliton-based comb has emerged that can potentially transfer the dual-comb method to a chip platform. Unlike earlier microcombs, these new device…
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.
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.
Dual terahertz (THz) comb spectroscopy is a promising methods for high accuracy, high resolution, and broadband THz spectroscopy because the mode-resolved THz comb spectrum possesses both characteristics of broadband THz radiation and narrow-linewidth continuous-wave THz radiation and all frequency mode of THz comb can be phase-locked to a microwave frequency standard. However, requirement of stabilized dual femtosecond lasers has often hindered wide use of this method. In this article, we demonstrated the adaptive sampling, dual THz comb spectroscopy, enabling use of free-running dual femtose…
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-band…
While being invented for precision measurement of single atomic transitions, frequency combs have also become a versatile tool for broadband spectroscopy in the last years. In this paper we present a novel and simple approach for broadband spectroscopy, combining the accuracy of an optical fiber-laser-based frequency comb with the ease-of-use of a tunable external cavity diode laser. This scheme enables broadband and fast spectroscopy of microresonator modes and allows for precise measurements of their dispersion, which is an important precondition for broadband optical frequency comb generati…
Multi-dimensional coherent spectroscopy (MDCS)1,2 is a powerful method for optical spectroscopy that has become an important tool for studying ultrafast dynamics in a wide range of systems. It is an optical analog of multidimensional nuclear magnetic resonance spectroscopy that enables the measurement of homogeneous linewidths in inhomogeneously broadened systems, many-body interactions, and coupling between excited resonances, all of which are not simultaneously accessible by any other linear or non-linear method. Current implementations of MDCS require a bulky apparatus and suffer from resol…
Frequency combs based on terahertz quantum cascade lasers feature broadband coverage and high output powers in a compact package, making them an attractive option for broadband spectroscopy. Here, we demonstrate the first multi-heterodyne spectroscopy using two terahertz quantum cascade laser combs. With just 100 $μ$s of integration time, we achieve peak signal-to-noise ratios exceeding 60 dB and a spectral coverage greater than 250 GHz centered at 2.8 THz. Even with room-temperature detectors we are able to achieve peak signal-to-noise ratios of 50 dB, and as a proof-of-principle we use these…
Fano resonance in molecular spectroscopy is reported with a dual-comb instrument. The effect is observed as asymmetric absorption lines of H12CN. Pulse chirping conditions in the gas cell are varied to show that Fano resonance is dependent on the pulse peak power. A model adding the Fano profile to Voigt lines is used to estimate Fano phase as a function of pulse peak power. A pulse peak power condition is derived from this analysis to avoid lineshape distortion in pulsed laser experiments.
The broadband, coherent nature of narrow-linewidth fiber frequency combs is exploited to measure the full complex spectrum of a molecular gas through multi-heterodyne spectroscopy. We measure the absorption and phase shift experienced by each of 155,000 individual frequency comb lines, spaced by 100 MHz and spanning from 1495 nm to 1620 nm, after passing through a hydrogen cyanide gas. The measured phase spectrum agrees with Kramers-Kronig transformation of the absorption spectrum. This technique can provide a full complex spectrum rapidly, over wide bandwidths, and with hertz-level accuracy.
Frequency comb assisted diode laser spectroscopy, employing both the accuracy of an optical frequency comb and the broad wavelength tuning range of a tunable diode laser, has been widely used in many applications. In this letter we present a novel method using cascaded frequency agile diode lasers, which allows extending the measurement bandwidth to 37.4 THz (1355 to 1630 nm) at MHz resolution with scanning speeds above 1 THz/s. It is demonstrated as a useful tool to characterize a broadband spectrum for molecular spectroscopy and in particular it enables to characterize the dispersion of inte…
Mid-infrared femtosecond optical frequency combs were produced by difference frequency generation of the spectral components of a near-infrared comb in a 3-mm-long MgO:PPLN crystal. We observe strong pump depletion and 9.3 dB parametric gain in the 1.5 μm signal, which yields powers above 500 mW (3 μW/mode) in the idler with spectra covering 2.8 μm to 3.5 μm. Potential for broadband, high-resolution molecular spectroscopy is demonstrated by absorption spectra and interferograms obtained by heterodyning two combs.
Mid-infrared dual-comb spectroscopy has the potential to supplant conventional high-resolution Fourier transform spectroscopy in applications that require high resolution, accuracy, signal-to-noise ratio, and speed. Until now, dual-comb spectroscopy in the mid-infrared has been limited to narrow optical bandwidths or to low signal-to-noise ratios. Using a combination of digital signal processing and broadband frequency conversion in waveguides, we demonstrate a mid-infrared dual-comb spectrometer that can measure comb-tooth resolved spectra across an octave of bandwidth in the mid-infrared fro…
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 mul…
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.
A fully stabilized mid-infrared optical frequency comb spanning from 2.9 to 3.4 um is described. The comb is based on half-harmonic generation in a femtosecond optical parametric oscillator, which transfers the high phase coherence of a fully stabilized near-infrared Er-doped fiber laser comb to the mid-infrared region. The method is simple, as no phase-locked loops or reference lasers are needed. Precise locking of optical frequencies of the mid-infrared comb to the pump comb is experimentally verified at sub-20 mHz level, which corresponds to a fractional statistical uncertainty of 2x10-16 a…
We propose and characterize experimentally a new source of optical frequency combs for performing multi-heterodyne spectrometry. This comb modality is based on a frequency shifting loop seeded with a CW monochromatic laser. The comb lines are generated by successive passes of the CW laser through an acousto-optic frequency shifter. We report the generation of frequency combs with more than 1500 mutually coherent lines, without resorting to non-linear broadening phenomena or external electronic modulation. The comb line spacing is easily reconfigurable from tens of MHz down to the kHz region. W…
Dual Comb Spectroscopy proved its versatile capabilities in molecular fingerprinting in different spectral regions, but not yet in the ultraviolet (UV). Unlocking this spectral window would expand fingerprinting to the electronic energy structure of matter.This will access the prime triggers of photo-chemical reactions with unprecedented spectral resolution. In this research article, we discuss the milestones marking the way to the first UV dual comb spectrometer. We present experimental and simulated studies towards UV dual comb spectroscopy, directly applied to planned absorption measurement…
Dual-comb spectroscopy is a powerful technique for real-time, broadband optical sampling of molecular spectra which requires no moving components. Recent developments with microresonator-based platforms have enabled frequency combs at the chip scale. However, the need to precisely match the resonance wavelengths of distinct high-quality-factor microcavities has hindered the development of an on-chip dual comb source. Here, we report the first simultaneous generation of two microresonator combs on the same chip from a single laser. The combs span a broad bandwidth of 51 THz around a wavelength …
Self-heterodyne spectroscopy via a non-uniformly spaced frequency comb
State Key Laboratory of Quantum Optics Technologies and Devices, Institute of Laser Spectroscopy（山西大学量子光学技术与器件国家重点实验室激光波谱学研究所）；Shanxi University（山西大学极端光学协同创新中心）；Collaborative Innovation Center of Extreme Optics；Shanxi University
We perform femtosecond frequency comb vernier spectroscopy in the near infrared with a femtosecond Er doped fiber laser, a scanning high-finesse cavity and an InGaAs camera. By utilizing the properties of a frequency comb and a scanning high-finesse cavity such spectroscopy provides broad spectral bandwidth, high spectral resolution, and high detection sensitivity on a short time scale. We achieved an absorption sensitivity of ~8E-8 cm-1Hz-1/2 corresponding to a detection limit of ~70 ppbv for acetylene, with a resolution of ~1.1 GHz in single images taken in 0.5 seconds and covering a frequen…
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 de…
We have carried out dual-comb spectroscopy and observed in a simultaneous acquisition a 140-THz-wide spectrum from 1.0 to 1.9 μm using two fiber-based frequency combs phase-locked to each other. This ultra-broad wavelength bandwidth is realized by setting the difference between the repetition rates of the two combs to 7.6 Hz using the sub-Hz-linewidth fiber combs. The recorded spectrum contains five vibration-rotation bands of C${_2}$H${_2}$, CH${_4}$, and H${_2}$O at different wavelengths across the whole spectrum. The determined transition frequencies of C${_2}$H${_2}$ agree with those from …
We demonstrate a high-accuracy dual-comb spectrometer centered at 3.4 μm. The amplitude and phase spectra of the P, Q, and partial R-branch of the methane ν3 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 d…
We demonstrate optical frequency comb Faraday rotation spectroscopy (OFC-FRS) for broadband interference-free detection of paramagnetic species. The system is based on a femtosecond doubly resonant optical parametric oscillator and a fast-scanning Fourier transform spectrometer (FTS). The sample is placed in a DC magnetic field parallel to the light propagation. Efficient background suppression is implemented via switching the direction of the field on consecutive FTS scans and subtracting the consecutive spectra, which enables long term averaging. In this first demonstration, we measure the e…
Dual-comb spectroscopy is emerging as one of the most appealing applications of mid-infrared frequency combs for high-resolution molecular spectroscopy, as it leverages on the unique coherence properties of frequency combs combined with the high sensitivities achievable by mid-infrared molecular spectroscopy. Here we present an on-chip dual-comb source based on mid-infrared quantum cascade laser frequency combs, where two frequency combs are integrated on a single chip. Control of the combs repetition and offset frequencies is obtained by integrating micro-heaters next to each laser. We show t…
We present a thorough analysis of the signal line shapes of Fourier transform-based noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS). We discuss the signal dependence on the ratio of the modulation frequency, f${_m}$, to the molecular line width, Γ. We compare a full model of the signals and a simplified absorption-like analytical model that has high accuracy for low f${_m}$/Γ ratios and is much faster to compute. We verify the theory experimentally by measuring and fitting NICE-OFCS spectra of CO${_2}$ at 1575 nm using a system based on an Er:fiber femtosecond lase…
Spectroscopy is the basic tool for studying molecular physics and realizing bio-chemical sensing. However, it is challenging to realize sub-femtometer resolution spectroscopy over broad bandwidth. In this paper, broadband and high-resolution spectroscopy with calibrated optical frequency is demonstrated by bridging the fields of speckle patterns and electro-optic frequency comb (EOFC). A novel wavemeter based on whispering-gallery-mode (WGM) speckles (or WGM barcodes) is proposed to link the frequency of a tunable continuous-wave (CW) laser to an optical reference provided by an ultra-stable l…
Cavity-enhanced direct frequency comb spectroscopy combines broad spectral bandwidth, high spectral resolution, precise frequency calibration, and ultrahigh detection sensitivity, all in one experimental platform based on an optical frequency comb interacting with a high-finesse optical cavity. Precise control of the optical frequency comb allows highly efficient, coherent coupling of individual comb components with corresponding resonant modes of the high-finesse cavity. The long cavity lifetime dramatically enhances the effective interaction between the light field and intracavity matter, in…
Historically, there has been a trade-off in spectroscopic measurements between high spectral resolution, broadband coverage, and acquisition time. Optical frequency combs, initially envisioned for precision spectroscopy of the hydrogen atom in the ultraviolet region, are now commonly used for probing molecular rotational-vibrational transitions throughout broad spectral bands in the mid-infrared with superior accuracy, resolution and speed. Here we demonstrate acquisition of 2.5 million spectral points over the continuous wavelength range of 3.2 to 5.1 microns (frequency span 1200 cm^{-1}, res…
Dual-comb generation from a single laser cavity provides a simple and high-performance solution to time sampling applications. We demonstrate a compact single-cavity dual-comb laser operating at gigahertz repetition rates and high repetition rate differences up to more than 100 kHz with sub-100 fs pulse duration. The single cavity approach leads to passive common noise suppression resulting in ultra-low relative timing jitter and fully resolvable comb lines in free-running operation. We showcase the laser performance with two application demonstrations: (a) time-domain spectroscopy of acetylen…
We have recently introduced the Vernier-based Direct Frequency Comb Cavity-Enhanced Spectroscopy technique and we present the corresponding formalism for quantitative broadband spectroscopy. We achieve high sensitivity and broadband performance by acquiring spectra covering more than 2000 cm$^{-1}$ around 12600 cm$^{-1}$ (800 nm), resolving the 3$ν$+$δ$ band of water vapor and the entire A-band of oxygen in ambient air. 31 300 independent spectral elements are acquired at the second time scale with an absorption baseline noise of 2$\times$10$^{-8}$ cm$^{-1}$ providing a merit figure of 1,1.10$…
We use two femtosecond Erbium-doped fiber lasers with slightly different repetition rates to perform a modern type of Fourier transform spectroscopy without moving parts. The measurements are done in real time, and it takes less than 50 microseconds. We work with somewhat different spectral outputs from two Erbium-doped fiber lasers and employ spectral filtering based on a 2f-2f grating setup to select the common spectral region of interest, thereby increasing the signal-to-noise ratio. The interferogram is taken with a 20 cm long gas cell, containing a mixture of acetylene and air at atmosphe…
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,…
In this work we present the design and characterization of a dual comb photoacoustic spectroscopy (DCPAS) set-up for ammonia detection in the near infrared. The system consists of a dual electro-optic (EO) comb generator that generates a multiheterodyne beating signal in the gas sample. The input to the dual EO comb generator is a laser diode tuned to a fixed wavelength within an absorption feature of ammonia (around 1531.6 nm, 6529 cm-1) and we show how the dual comb allows to perform PAS measurements and resolve the absorption features with high spectral resolution. We present results of the…
Confocal imaging and phase imaging are powerful tools in life science research and industrial inspection. To coherently link the two techniques with different depth resolutions, we introduce an optical frequency comb (OFC) to microscopy. Two-dimensional (2D) image pixels of a sample were encoded onto OFC modes via 2D spectral encoding, in which OFC acted as an optical carrier with a vast number of discrete frequency channels. Then, a scan-less full-field confocal image with a depth resolution of 62.4 um was decoded from a mode-resolved OFC amplitude spectrum obtained by dual-comb spectroscopy.…
Two frequency combs can be used to measure the full complex response of a sample in a configuration which can be alternatively viewed as the equivalent of a dispersive Fourier transform spectrometer, infrared time domain spectrometer, or a multiheterodyne laser spectrometer. This dual comb spectrometer retains the frequency accuracy and resolution inherent to the comb sources. We discuss, in detail, the specific design of our coherent dual-comb spectrometer and demonstrate the potential of this technique by measuring the first overtone vibration of hydrogen cyanide, centered at 194 THz (1545 n…
Dual comb spectroscopy allows for high-resolution spectra to be measured over broad bandwidths, but an essential requirement for coherent integration is the availability of a phase reference. Usually, this means that the combs' phase and timing errors must be measured and either minimized by stabilization or removed by correction, limiting the technique's applicability. In this work, we demonstrate that it is possible to extract the phase and timing signals of a multiheterodyne spectrum completely computationally, without any extra measurements or optical elements. These techniques are viable …
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.
