Dual-comb spectroscopy (DCS) is useful for gas spectroscopy due to high potential of optical frequency comb (OFC). However, fast Fourier transform (FFT) calculation of a huge amount of temporal data spends significantly longer time than the acquisition time of an interferogram. In this article, we demonstrate frequency-domain DCS by a combination of DCS with lock-in detection, namely LID-DCS. LID-DCS directly extracts an arbitrary OFC mode from a vast number of OFC modes without the need for FFT calculation. Usefulness of LID-DCS is demonstrated in rapid monitoring of transient signal change and spectroscopy of hydrogen cyanide gas.
Broadband dual-comb spectroscopy (DCS) based on portable mode-locked fiber frequency combs is a powerful tool for in situ, calibration free, multi-species spectroscopy. While the acquisition of a single spectrum with mode-locked DCS typically takes microseconds to milliseconds, the applications of these spectrometers have generally been limited to systems and processes with time changes on the order of seconds or minutes due to the need to average many spectra to reach a high signal-to-noise ratio (SNR). Here, we demonstrate high-speed, continuous, fiber mode-locked laser DCS with down to 11 $…
We demonstrate a cost-effective, fully software-based lock-in amplifier (LIA) implemented on a commercial computer. The device is designed for application in nonlinear spectroscopy, such as transient absorption and coherent multidi-mensional spectroscopy, but may be also used in any other application. The performance of our device is compared to a state-of-the-art commercial LIA with nearly identical results for both devices. Advantages of our device over commercial hardwired electronic lock-in amplifiers is the improved flexibility in the data analysis and the possibility of arbitrary up-scal…
We report the first experimental demonstration of frequency-locking of an extended-cavity quantum-cascade-laser (EC-QCL) to a near-infrared frequency comb. The locking scheme is applied to carry out absolute spectroscopy of N2O lines near 7.87 μm with an accuracy of ~60 kHz. Thanks to a single mode operation over more than 100 cm^{-1}, the comb-locked EC-QCL shows great potential for the accurate retrieval of line center frequencies in a spectral region that is currently outside the reach of broadly tunable cw sources, either based on difference frequency generation or optical parametric oscil…
We present a method to measure quadratic Terahertz optical nonlinearities in Terahertz time-domain spectroscopy. We use a rotating linear polarizer (a polarizing chopper) to modulate the amplitude of the incident THz pulse train. We use a phase-sensitive lock-in detection at the fundamental and the second harmonic of the modulation frequency to separate the materials' responses that are linear and quadratic in Terahertz electric field. We demonstrate this method by measuring the quadratic Terahertz Kerr effect in the presence of the much stronger linear electro-optic effect in the (110) GaP cr…
A combination of optical feedback self-locking of a continuous-wave distributed feedback diode laser to a V-shaped high finesse cavity, laser phase modulation at a frequency equal to the free spectral range of the V-cavity and detection of the transmitted laser beam at this high modulation frequency is described for possible application in cavity-enhanced absorption spectroscopy.In order to estimate an absorbance baseline noise of laser intensity and frequency modulated light triplet passed through the V-cavity in open air, a 1.5-cm long optical cell filled by C2H2 at low pressure was placed b…
Dual-comb sources with equally spaced and low phase noise frequency lines are of great importance for high resolution spectroscopy and metrology. In the terahertz frequency range, electrically pumped semiconductor quantum cascade lasers (QCLs) are suitable candidates for frequency comb and dual-comb operation. For a single laser frequency comb, the repetition rate can be locked using a microwave injection locking and the carrier frequency can be locked to a highly stable source. However, for the locking of two laser combs, four frequencies (two repetition rates and two carrier offset frequenci…
We present a novel remote gas detection and identification technique based on correlation spectroscopy with a piezoelectric tunable fibre-optic Fabry-Pérot filter. We show that the spectral correlation amplitude between the filter transmission window and gas absorption features is related to the gas absorption optical depth, and that different gases can be distinguished from one another using their correlation signal phase. Using an observed telluric-corrected, high-resolution near-infrared spectrum of Venus, we show via simulation that the Doppler shift of gases lines can be extracted from th…
Ultraviolet (UV) diode lasers are widely used in many photonics applications. But their frequency stabilization schemes are not as mature as frequency-doubling lasers, mainly due to some limitations in the UV spectral region. Here we developed a high-performance UV frequency stabilization technique implemented directly on UV diode lasers by combining the dichroic atomic vapor laser lock and the resonant transfer cavity lock. As an example, we demonstrate a stable locking with frequency standard deviations of approximately 200 KHz and 300 KHz for 399nm and 370nm diode lasers in 20 minutes. We a…
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 $μ$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 stabi…
We present homogeneous quantum cascade lasers (QCLs) emitting around 3 THz which display bandwidths up to 950 GHz with a single stable beatnote. Devices are spontaneously operating in a harmonic comb state, and when in a dense mode regime they can be injection locked at the cavity roundtrip frequency with very small RF powers down to -55 dBm. When operated in the electrically unstable region of negative differential resistance, the device displays ultra-broadband operation exceeding 1.83 THz ($Δf/f=50\%$) with high phase noise, exhibiting self-sustained, periodic voltage oscillations. The low …
Microresonator-based optical frequency combs have been a topic of extensive research during the last few years. Several theoretical models for the comb generation have been proposed; however, they do not comprehensively address experimental results that show a variety of independent comb generation mechanisms. Here, we present frequency-domain experiments that illuminate the transition of microcombs into phase-locked states, which show characteristics of injection locking between ensembles of comb modes. In addition, we demonstrate the existence of equidistant optical frequency combs that are …
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…
We demonstrate a compact and robust device for simultaneous absolute frequency stabilization of three diode lasers whose carrier frequencies can be chosen freely relative to the reference. A rigid ULE multi-cavity block is employed, and, for each laser, the sideband locking technique is applied. Useful features of the system are a negligible lock error, computer control of frequency offset, wide range of frequency offset, simple construction, and robust operation. One concrete application is as a stabilization unit for the cooling and trapping lasers of a neutral atom lattice clock. The device…
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 show, both experimentally and theoretically, that a slave laser injected with an optical frequency comb can undergo two distinct locking mechanisms, both of which decrease the output optical comb's frequency spacing. We report that, for certain detuning and relative injection strengths, slave laser relaxation oscillations can become undamped and lock to rational frequencies of the optical comb spacing, creating extra comb tones by nonlinear dynamics of the injected laser. We also study the frequency locking of the slave laser in between the injected comb lines, which add the slave laser's f…
We present a rapid-scanning approach to fluorescence-detected two-dimensional electronic spectroscopy that combines acousto-optic phase-modulation with digital lock-in detection. The approach shifts the signal detection window to suppress 1/f laser noise and enables interferometric tracking of the time delays to allow for correction of spectral phase distortions and accurate phasing of the data. This use of digital lock-in detection enables acquisition of linear and nonlinear signals of interest in a single measurement. We demonstrate the method on a laser dye, measuring the linear fluorescenc…
We present detailed numerical simulations of the laser dynamics that describe optical frequency comb formation by injection-locking a gain-switched laser. The typical rate equations for semiconductor lasers including stochastic carrier recombination and spontaneous emission suffice to show the injection-locking behavior of gain switched lasers, and we show how the optical frequency comb evolves starting from the free-running state, right through the final injection- locked state. Unlike the locking of continuous wave lasers, we show that the locking range for gain switched lasers is considerab…
The two-frequency problem of synchronization of the pulse train of a passively mode locked soliton laser to an externally injected pulse train is solved in the weak injection regime. The source and target frequency combs are distinguished by the spacing and offset frequency mismatches. Locking diagrams map the domain in the mismatch parameter space where stable locking of the combs is possible. We analyze the dependence of the locking behavior on the relative frequency and chirp of the source and target pulses, and the conditions where the relative offset frequency has to be actively stabilize…
Quantum cascade laser (QCL) frequency combs are a promising candidate for chemical sensing and biomedical diagnostics, requiring only milliseconds of acquisition time to record absorption spectra without any moving parts. They are electrically pumped and have a small footprint, making them an ideal platform for on-chip integration. Until now, optical feedback is fatal for frequency comb generation in QCLs and destroys intermodal coherence. This property imposes strict limits on the possible degree of integration. Here, we demonstrate coherent injection locking of the repetition frequency to a …
We present the detailed characterization of the phase dynamics of a telecom hybrid III-V-on-silicon passively mode-locked laser with a ring cavity. We explore the various regimes of operation as a function of gain current and saturable absorber bias voltage. We use a stepped-heterodyne measurement to quantify the spectral chirp and reconstruct the pulse envelop. With this technique we are able to identify regimes of near-transform-limited operation and we assess the degradation of mode-locking in the comb phase relationship when saturable absorber bias voltage is changed. Finally, we present a…
We experimentally observed self-injection locking regime of the gain-switched laser to high-Q optical microresonator. We revealed that comb generated by the gain-switched laser experiences a dramatic reduce of comb teeth linewidths in this regime. We demonstrated the Lorentzian linewidth of the comb teeth of sub-kHz scale as narrow as for non-switched self-injection locked laser. Such setup allows generation of high-contrast electrically-tunable optical frequency combs with tunable comb line spacing in a wide range from 10 kHz up to 10 GHz. The characteristics of the generated combs were studi…
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.
By using two mutually phase-locked optical frequency combs with slightly different repetition rates, we demonstrate asynchronous optical-sampling terahertz time-domain spectroscopy (ASOPS THz-TDS) without using any trigger signals or optical delay lines. Due to a tight stabilization of the repetition frequencies, it was possible to accumulate the data over 48 minutes in a triggerless manner without signal degradation. The fractional frequency stability of the measured terahertz signal is evaluated to be $\sim$8.0$\times$10$^{- 17}$ after 730 s. The frequency accuracy of the obtained terahertz …
In this paper, we present an experimental study of the metrological stabilization of a solid-state frequency comb for embedded metrology applications. The comb is a passively mode-locked laser diode based on InGaAs/InP Quantum-dash structure emitting optical lines into a 9 nm bandwidth centered at 1.55 $μ$m with a repetition rate of 10.09 GHz. The frequency stabilization is achieved by optical injection locking of the comb with an external cavity laser diode referenced onto a metrological frequency standard. One observes the transfer of the spectral purity from the injection laser to the neigh…
In this letter we theoretically investigate the formation of localized temporal dissipative structures, and their corresponding frequency combs in doubly resonant dispersive optical parametric oscillators. We derive a nonlocal mean field model, and show that domain wall locking allows for the formation of stable coherent optical frequency combs.
We report on an optical frequency comb with 14nm (~1.8 THz) spectral bandwidth at -3 dB level that is generated using a passively mode-locked quantum-well (QW) laser in photonic integrated circuits (PICs) fabricated through an InP generic photonic integration technology platform. This 21.5-GHz colliding-pulse mode-locked laser cavity is defined by on-chip reflectors incorporating intracavity phase modulators followed by an extra-cavity SOA as booster amplifier. A 1.8-THz-wide optical comb spectrum is presented with ultrafast pulse that is 0.35-ps-wide. The radio frequency beat note has a 3-dB …
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 …
Laser injection locking and nanophotonic spectral translation of electro-optic frequency combs
National Institute of Standards and Technology（美国国家标准与技术研究院）；University of Maryland（马里兰大学）；Joint Quantum Institute, NIST/University of Maryland（NIST/马里兰大学联合量子研究所）
We calculate the quantum-limited shape of the comb lines from a mode-locked Ti:sapphire laser using experimentally-derived parameters for the linear response of the laser to perturbations. The free-running width of the comb lines is found across the laser spectrum. By modeling the effect of a simple feedback loop, we calculate the spectrum of the residual phase noise in terms of the quantum noise and the feedback parameters. Finally, we calculate the frequency uncertainty in an optical frequency measurement if the limiting factor is quantum noise in the detection of the optical heterodyne beat…
Microresonator frequency combs harness the nonlinear Kerr effect in an integrated optical cavity to generate a multitude of phase-locked frequency lines. The line spacing can reach values in the order of 100 GHz, making it an attractive multi-wavelength light source for applications in fiber-optic communications. Depending on the dispersion of the microresonator, different physical dynamics have been observed. A recently discovered comb state corresponds to the formation of mode-locked dark pulses in a normal-dispersion microcavity. Such dark-pulse combs are particularly compelling for advance…
Dual-comb spectroscopy allows for the rapid, multiplexed acquisition of high-resolution spectra without the need for moving parts or low-resolution dispersive optics. This method of broadband spectroscopy is most often accomplished via tight phase locking of two mode-locked lasers or via sophisticated signal processing algorithms, and therefore, long integration times of phase coherent signals are difficult to achieve. Here we demonstrate an alternative approach to dual-comb spectroscopy using two phase modulator combs originating from a single continuous-wave laser capable of > 2 hours of coh…
In this work, we describe an updated version of single arm locking, and the noise amplification due to the nulls can be flexibly restricted with the help of optical frequency comb. We show that, the laser phase noise can be divided by a specific factor with optical frequency comb as the bridge. The analytical results indicate that, the peaks in the science band have been greatly reduced. The performance of the noise suppression shows that the total noise after arm locking can well satisfy the requirement of time delay interferometry, even with the free-running laser source. We also estimate th…
We stabilize a chip-scale Si3N4 phase-locked Kerr frequency comb via locking the pump laser to an independent stable high-Q reference microresonator and locking the comb spacing to an external microwave oscillator. In this comb, the pump laser shift induces negligible impact on the comb spacing change. This scheme is a step towards miniaturization of the stabilized Kerr comb system as the microresonator reference can potentially be integrated on-chip. Fractional instability of the optical harmonics of the stabilized comb is limited by the microwave oscillator used for comb spacing lock below 1…
We have specifically investigated the free-space mode locking dynamics of erbium-doped fiber (EDF) mode-locked ultrafast lasers via nonlinear polarization rotation (NPR) in the normal dispersion regime. To do so, we built a passively mode-locked fiber laser based on NPR with a repetition rate of 89 MHz producing an octave-spanning spectrum due to supercontinuum (SC) generation in highly nonlinear fiber (HNLF). Most significantly, we have achieved highly stable self-starting NPR mode-locked femtosecond fiber laser based frequency comb which has been running mode locked for the past one year wit…
Amplified spontaneous emission (ASE) causes fluctuations of pulse energy, of the optical phase and of the timing of the pulse intensity envelope in a mode-locked laser or frequency comb. Starting from the assumption of one ASE photon per longitudinal laser mode and roundtrip, we rederive analytic equations for the three fundamental types of quantum noise in a laser. To this end, we analyze the interference of the coherent intracavity field and a spectrally localized ASE photon as a function of wavelength and phase of the latter. Performing an integration over all wavelengths and phases and tak…
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…
We report on a mode-locked laser design using Yb-doped fiber lasers for low-noise frequency-comb generation. The frequency comb covers the spectral range from $700$ to $1400$ nm. Although this range is more practical for many measurements than that produced by the more commonly used Er-fiber lasers, it has been addressed in only a handful of reports, mainly due to the difficulty of generating a fully coherent supercontinuum at $1\;μ$m. We overcome this difficulty by a tailored design of the mode-locking dynamics that succeeds in generating energetic 33 fs-long pulses without even using higher-…
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…
Noise-immune cavity-enhanced optical frequency comb spectroscopy (NICE-OFCS) is a recently developed technique that utilizes phase modulation to obtain immunity to frequency-to-amplitude noise conversion by the cavity modes and yields high absorption sensitivity over a broad spectral range. We describe the principles of the technique and discuss possible comb-cavity matching solutions. We present a theoretical description of NICE-OFCS signals detected with a Fourier transform spectrometer (FTS), and validate the model by comparing it to experimental CO2 spectra around 1575 nm. Our system is ba…
Femtosecond frequency combs have boosted progress in various fields of precision metrology. Nevertheless, demanding applications such as front-end frequency and time standards, ultrastable microwave generation or high-resolution spectroscopy still necessitate improved stability. The spectral bandwidth and absolute position of individual comb lines are crucial in this context. Typically, both parameters are controlled on short and long time scales by tight locking to external optical and microwave references which represent costly and cumbersome additions to the entire setup. Here, we demonstra…
We present a method of phase-locking any number of continuous-wave lasers to an optical frequency comb (OFC) that enables independent frequency positioning and control of each laser while still maintaining lock to the OFC. The scheme employs an acousto-optic modulator (AOM) in a double pass configuration added to each laser before its light is compared by optical heterodyne with the comb. The only requirement is that the tuning bandwidth of the double pass AOM setup be larger than half the OFC repetition rate. We demonstrate this scheme and achieve an arbitrary frequency tuning precision, a tu…
