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Gas samples relevant to health and environment typically contain a plethora of molecular species that span a huge concentration dynamic range. High-concentration molecules impose a strong absorption background that hinders robust identification of low-concentration species. While mid-infrared frequency comb spectroscopy with high-finesse cavity enhancement has realized many of the most sensitive multi-species trace gas detection to date, its robust performance requires gas samples to contain only weak absorption features to avoid dispersing cavity resonances from the comb line frequencies. Here we introduce a new technique that is free from this restriction, thus enabling the development of next-generation multi-species trace gas sensing with broad applicability to complex and dynamic molecular compositions. The principle of Modulated Ringdown Comb Interferometry is to resolve ringdown dynamics carried by massively parallel comb lines transmitted through a length-modulated cavity. This method leverages both periodicity of the field dynamics and Doppler frequency shifts introduced from a Michelson interferometer. Scalable enhancement of both spectral coverage and cavity finesse is enabled with dispersion immune and high-efficiency data collection. Built upon this platform, we realize in the mid-infrared a product of finesse and spectral coverage that is orders of magnitude better than all prior experiments. We demonstrate the power of this technique by measuring highly dispersive exhaled human breath samples over a vastly expanded spectral coverage of 1,010 cm-1 and with cavity finesse of 23,000. This allows for the first time simultaneous quantification of 20 distinct molecular species at > 1 part-per-trillion sensitivity with their concentrations varying by 7 orders of magnitude.

Parametric amplifiers have allowed breakthroughs in ultrafast, strong-field, and high-energy density laser science and are an essential tool for extending the frequency range of powerful emerging diode-pumped solid-state laser technology. However, their impact is limited by inherently low quantum efficiency due to nonuniform light extraction. Here we demonstrate a new type of parametric amplifier based on hybridized nonlinear optics. Hybridization of parametric amplification with idler second harmonic generation induces unusual evolution dynamics for a fully parametric amplifier - with saturating rather than cyclic gain - observed here for the first time. This allows highly uniform light extraction enabling unprecedented efficiency for a lossless amplifier with Gaussian-like intensity profiles - a 48-dB single-stage gain with 68% quantum efficiency and 44% pump-to-signal energy conversion - a several-fold improvement over the standard. Possessing both laser-like high quantum efficiency and the advantages of thermal-loading free parametric systems, this simple approach can be implemented widely and have significant impact by increasing several-fold the power available for science and industry.

We report a study of high-order multi-photon absorption, nonlinear refraction, and their anisotropy in four notable mid-infrared \c{hi}(2) crystals: GaP, ZnSe, GaSe and ZGP using the Z- scan method and 2.35-{\mu}m femtosecond pulses with peak intensity in excess of 200 GW/cm2. We found that the nonlinear absorption obeys a perturbation model with multi-photon absorption (MPA) orders from N = 4 to 6, in good agreement with the bandgaps of the crystals. A study of the role of free carrier absorption, performed by varying the pulse duration between 30 and 70 fs while maintaining a constant peak intensity showed that at our intensity levels, free carriers generated in the process of MPA absorb much stronger than would be expected from their linear absorption cross section. Possible mechanisms include high-field effects, such as intra-valley scattering in the conduction band and absorption to higher lying bands. Nonlinear refractive indices were measured using (i) closed aperture Z-scan and (ii) spectral broadening due to self-phase modulation, both methods agreeing well with each other., Comment: 10 pages, 5 figures, 3 tables

The potential of frequency comb spectroscopy has aroused great interest in generating mid-infrared frequency combs in the integrated photonic setting. However, despite remarkable progress in microresonators and quantum cascade lasers, the availability of suitable mid-IR comb sources remains scarce. Here, we present a new approach for the generation of mid-IR microcombs through cascaded three-wave-mixing. By pumping a CdSiP$_2$ microresonator at 1.55 $\mu$m wavelength with a low power continuous wave laser, we generate $\chi^{(2)}$ frequency combs at 3.1 $\mu$m wavelength, with a span of about 30 nm. We observe ordinary combs states with a line spacing of the free spectral range of the resonator, and combs where the sideband numbers around the pump and half-harmonic alternate, forming staggered patterns of spectral lines. Our scheme for mid-IR microcomb generation is compatible with integrated telecom lasers. Therefore, it has the potential to be used as a simple and fully integrated mid-IR comb source, relying on only one single material.

Powerful and efficient optical frequency combs in the mid-infrared (MIR) spectral region are highly desirable for a broad range of applications. Despite extensive efforts utilizing various techniques, MIR frequency comb sources are still lacking power, efficiency, or bandwidth for many applications. Here, we report the generation of an intrinsically locked frequency comb source centered at 4.18 {\mu}m from an optical parametric oscillator (OPO) operating in the simulton regime, in which formation of purely quadratic solitons lead to enhanced performance. We show advantages of operation in the simulton regime in direct experimental comparisons to the conventional regime, which are also supported by simulation and theory. We achieve 565 mW of average power, 900 nm of instantaneous 3-dB bandwidth, 350% of slope efficiency, and 44% of conversion efficiency; a performance that is superior to previous OPO demonstrations and other sources in this wavelength range. This work opens a new avenue toward MIR frequency comb generation with high power and efficiency and suggests the great potential of soliton generation based on quadratic nonlinearity in the MIR spectral region., Comment: 12 pages, 6 figures (main text); 3 pages, 0 figure (supplementary materials)

Broadband mid-infrared (MIR) molecular spectroscopy demands a bright and broadband light source in the molecular fingerprint region. To this end, intra-pulse difference frequency generation (IDFG) has shown excellent properties among various techniques. However, previous IDFG systems have mainly used unconventional long-wavelength 2-${\mu}$m ultrashort pulsed lasers. A few systems have been demonstrated with 1-${\mu}$m lasers, but they use bulky 100-W-class high-power Yb thin-disk lasers. In this work, we demonstrate a simple and robust approach of 1-${\mu}$m-pumped broadband IDFG with a conventional mode-locked Yb-doped fiber laser. We first generate 3.3-W, 12.1-fs ultrashort pulses at 50 MHz by a simple combination of spectral broadening with a short single-mode fiber and pulse compression with chirped mirrors. Then, we use them for pumping a thin orientation-patterned gallium phosphide (OP-GaP) crystal, generating 1.2-mW broadband MIR pulses with the -20-dB bandwidth of 480 cm$^{-1}$ in the fingerprint region (760-1240 cm$^{-1}$, 8.1-13.1 ${\mu}$m). The 1-${\mu}$m-based IDFG system allows for simultaneous generation of ultrashort pulses in the ultraviolet and visible regions, enabling, for example, 100-MHz-level high-repetition-rate vibrational sum-frequency generation spectroscopy or pump-probe spectroscopy.

Terahertz time-domain spectroscopy is employed to investigate temperature-dependent properties of bulk chalcopyrite crystals (CdGeP$_2$, ZnGeP$_2$ and CdSiP$_2$). The complex spectra provide the refraction and absorption as a function of temperature, from which electron-phonon coupling and average phonon energies are extracted and linked to the mechanics of the A- and B-site cations. Also, AC conductivity spectra provide carrier densities and electron scattering times, the temperature dependence of which is associated with unintentional shallow dopants. Temperature dependence of the scattering time is converted into carrier mobility and modeled with microscopic transport mechanisms such as polar optical phonon, acoustic phonons, deformation potential, ionized impurity and dislocation scattering. Hence, analysis links the THz optical and electronic properties to relate microscopic carrier transport and carrier-lattice interactions., Comment: 12 pages, 5 figures, journal submission preprint

Frequency combs have triggered an impressive evolution of optical metrology across diverse regions of the electromagnetic spectrum, from the ultraviolet to the terahertz frequencies. An unexplored territory, however, remains in the region of vibrational bending modes, mostly due to the lack of single-mode lasers in the long-wavelength (LW) part of the mid-infrared (MIR) spectrum. We fill this gap through a purely MIR-based nonlinear laser source with tunability from 12.1 to 14.8 $\mu$m, optical power up to 110 $\mu$W, MHz-level linewidth and comb calibration. This enables the first example of bending modes metrology in this region, with the assessment of several CO$_2$-based frequency benchmarks with uncertainties down to 30 kHz, and the accurate study of the $\nu_{11}$ band of benzene, which is a significant testbed for the resolution of the spectrometer. These achievements pave the way for LW-MIR metrology, rotationally-resolved studies and astronomic observations of large molecules, such as aromatic hydrocarbons., Comment: 36 pages including Supplementary Materials, 4 figures (paper), 3 figures (SM)

Coherent laser beams in the 3 to 20 {\mu}m region of the spectrum are most applicable for chemical sensing by addressing the strongest vibrational absorption resonances of the media. Broadband frequency combs in this spectral range are of special interest since they can be used as a powerful tool for molecular spectroscopy offering dramatic gains in speed, sensitivity, precision, and massive parallelism of data collection. Here we show that a frequency comb realized through subharmonic generation in an optical parametric oscillator (OPO) based on orientation-patterned gallium phosphide (OP-GaP) pumped by a Kerr-lens mode-locked 2.35-{\mu}m laser can reach a continuous wavelength span of 3-12 {\mu}m, thus covering most of the molecular 'signature' region. The key to achieving such a broad spectrum is to use a low-dispersion cavity entailing all gold-coated mirrors, minimally dispersive and optically thin intracavity elements, and a specially designed pump injector. The system features a smooth ultra-broadband spectral output that is phase coherent to the pump laser comb, 245-mW output power with high (>20%) optical conversion efficiency, and a possibility to reach close to unity conversion from a mode-locked drive, thanks to the non-dissipative downconversion processes and photon recycling., Comment: 14 pages, 5 figures

We demonstrate mid-infrared (MIR) frequency combs at 10 GHz repetition rate via intra-pulse difference-frequency generation (DFG) in quasi-phase-matched nonlinear media. Few-cycle pump pulses ($\mathbf{\lesssim}$15 fs, 100 pJ) from a near-infrared (NIR) electro-optic frequency comb are provided via nonlinear soliton-like compression in photonic-chip silicon-nitride waveguides. Subsequent intra-pulse DFG in periodically-poled lithium niobate waveguides yields MIR frequency combs in the 3.1--4.1 $\mu$m region, while orientation-patterned gallium phosphide provides coverage across 7--11 $\mu$m. Cascaded second-order nonlinearities simultaneously provide access to the carrier-envelope-offset frequency of the pump source via in-line f-2f nonlinear interferometry. The high-repetition rate MIR frequency combs introduced here can be used for condensed phase spectroscopy and applications such as laser heterodyne radiometry.

Containment, the key strategy in quickly halting an epidemic, requires rapid identification and quarantine of the infected individuals, determination of whom they have had close contact with in the previous days and weeks, and decontamination of locations the infected individual has visited. Achieving containment demands accurate and timely collection of the infected individual's location and contact history. Traditionally, this process is labor intensive, susceptible to memory errors, and fraught with privacy concerns. With the recent almost ubiquitous availability of smart phones, many people carry a tool which can be utilized to quickly identify an infected individual's contacts during an epidemic, such as the current 2019 novel Coronavirus crisis. Unfortunately, the very same first-generation contact tracing tools have been used to expand mass surveillance, limit individual freedoms and expose the most private details about individuals. We seek to outline the different technological approaches to mobile-phone based contact-tracing to date and elaborate on the opportunities and the risks that these technologies pose to individuals and societies. We describe advanced security enhancing approaches that can mitigate these risks and describe trade-offs one must make when developing and deploying any mass contact-tracing technology. With this paper, our aim is to continue to grow the conversation regarding contact-tracing for epidemic and pandemic containment and discuss opportunities to advance this space. We invite feedback and discussion., Comment: 15 pages

We present the state of the art of a compact high-energy mid-infrared laser system for TW-level 8-cycle pulses at 7 um. This system consists of an Er:Tm:Ho:fiber MOPA which serves as the seeder for a ZGP-based OPCPA chain in addition to a Ho:YLF amplifier which is Tm:fiber pumped. Featuring all-optical synchronization, the system delivers 260-mJ pump energy at 2052 nm, 16-ps duration at 100 Hz with a stability of 0.8 % rms over 20 min. We show that chirp inversion in the OPCPA chain leads to excellent energy extraction and aids in compression of the 7-um pulses to 8 optical cycles (188 fs) in bulk BaF2 with 93.5 % efficiency. Using 21.7 mJ of the available pump energy, we generate 0.75-mJ-energy pulses at 7 um due to increased efficiency with a chirp-inversion scheme. The pulse quality of the system's output is shown by generating high harmonics in ZnSe which span up to harmonic order 13 with excellent contrast. The combination of the passive carrier-envelope phase stable mid-infrared seed pulses and the high-energy 2052 nm picosecond pulses makes this compact system a key enabling tool for the next generation of studies on extreme photonics, strong field physics and table-top coherent X-ray science., Comment: 4 pages, 5 figures

Molecular spectroscopy in the mid-infrared portion of the electromagnetic spectrum (3--25 um) has been a cornerstone interdisciplinary analytical technique widely adapted across the biological, chemical, and physical sciences. Applications range from understanding mesoscale trends in climate science via atmospheric monitoring to microscopic investigations of cellular biological systems via protein characterization. Here, we present a compact and comprehensive approach to infrared spectroscopy incorporating the development of broadband laser frequency combs across 3--27 um, encompassing the entire mid-infrared, and direct electric-field measurement of the corresponding near single-cycle infrared pulses of light. Utilizing this unified apparatus for high-resolution and accurate frequency comb spectroscopy, we present the infrared spectra of important atmospheric compounds such as ammonia and carbon dioxide in the molecular fingerprint region. To further highlight the ability to study complex biological systems, we present a broadband spectrum of a monoclonal antibody reference material consisting of more than 20,000 atoms. The absorption signature resolves the amide I and II vibrations, providing a means to study secondary structures of proteins. The approach described here, operating at the boundary of ultrafast physics and precision spectroscopy, provides a table-top solution and a widely adaptable technique impacting both applied and fundamental scientific studies.

Spectroscopy in the molecular fingerprint spectral region (6.5-20 $\mu$m) yields critical information on material structure for physical, chemical and biological sciences. Despite decades of interest and effort, this portion of the electromagnetic spectrum remains challenging to cover with conventional laser technologies. In this report, we present a simple and robust method for generating super-octave, optical frequency combs in the fingerprint region through intra-pulse difference frequency generation in an orientation-patterned gallium phosphide crystal. We demonstrate the utility of this unique coherent light source for high-precision, dual-comb spectroscopy in methanol and ethanol vapor. These results highlight the potential of laser frequency combs for a wide range of molecular sensing applications, from basic molecular spectroscopy to nanoscopic imaging.

Infrared spectroscopy in the spectral fingerprint region from 6-12 um accesses the largest molecular absorption cross-sections, permitting sensitive, quantitative and species-specific measurements. Here, we show how dual-comb spectroscopy--a form of high-speed Fourier-transform spectroscopy involving no moving parts and capable of very high resolutions--can be extended to the 6-8um wavelength band using femtosecond optical parametric oscillators (OPOs). By acquiring dual-comb interferograms faster than the mutual decoherence time of the OPO combs we implement line-shape-preserving averaging to obtain low-noise, high-fidelity spectra of H2O and CH4 at approximately 0.3 cm-1 resolutions from 1285-1585 cm-1.

We report on the first singly-resonant (SR), synchronously pumped optical parametric oscillator (OPO) based on orientation-patterned gallium arsenide (OP-GaAs). Together with a doubly resonant (DR) degenerate OPO based on the same OP-GaAs material, the output spectra cover 3 to 6 ${\mu}$m within ~3 dB of relative power. The DR-OPO has the highest output power reported to date from a femtosecond, synchronously pumped OPO based on OP-GaAs. We discovered strong three photon absorption with a coefficient of 0.35 ${\pm}$ 0.06 cm${^3}$/GW${^2}$ for our OP-GaAs sample, which limits the output power of these OPOs as mid-IR light sources. We present a detailed study of the three photon loss on the performance of both the SR and DR-OPOs, and compare them to those without this loss mechanism.

High-energy, carrier-envelope phase (CEP)-stable, sub-cycle, mid-infrared (mid-IR) pulses can provide unique opportunities of exploring phase-sensitive strong-field light-matter interactions in atoms, molecules, and solids. In the mid-IR wavelength, the ponderomotive energy of laser pulses is dramatically increased (versus the visible/near-infrared) and, therefore, the Keldysh parameter is much smaller than unity even at relatively modest laser intensities. This enables to study the sub-cycle electron dynamics in solids via high-harmonic generation (HHG) without damage. One can also control the electron emissions from nano-devices in the sub-cycle time scale. These efforts are opening a great opportunity towards petahertz electronics. Here, we present a high-energy, sub-cycle pulse synthesizer based on a mid-IR optical parametric amplifier (OPA), pumped by CEP-stable, 2.1 um femtosecond pulses, and its application to HHG in solids. The signal and idler combined spectrum spans from 2.5 to 9.0 um, which covers the whole midwave-infrared (MWIR) region. We coherently synthesize the passively CEP-stable few-cycle signal and idler pulses to generate 33 uJ, 0.88-cycle (12.4 fs), multi-GW pulses centered at ~4.2 um, which is further energy scalable. The in-line synthesis of the CEP-stable sub-cycle pulse is realized through the type-I collinear OPA with minimal temporal walk-off. The MWIR sub-cycle pulse is used for driving HHG in thin silicon samples, producing harmonics up to ~19th order with a continuous spectral coverage due to the isolated emission by the sub-cycle driver. Our demonstration offers an energy scalable and technically simple platform of laser sources generating CEP-stable sub-cycle pulses in the whole MWIR region for investigating isolated phase-sensitive strong-field interactions in solids and gases., Comment: 19 pages, 6 figures

We report a femtosecond optical parametric oscillator (OPO) based on the new semiconductor gain material orientation patterned gallium phosphide (OP-GaP), which enables the production of high-repetition-rate femtosecond pulses spanning 5-12 \mu m with average powers in the few to tens of milliwatts range. This is the first example of a broadband OPO operating across the molecular fingerprint region, and we demonstrate its potential by conducting broadband Fourier-transform spectroscopy using water vapor and a polystyrene reference standard., Comment: 4 pages, 5 figures

Collinear phase-matched optical rectification is studied in ZnGeP$_{2}$ pumped with near-infrared light. The pump-intensity dependence is presented for three crystal lengths (0.3, 1.0 and 3.0 mm) to determine the effects of linear optical absorption, nonlinear optical absorption and terahertz free-carrier absorption on the generation. Critical parameters such as the coherence length (for velocity matching), dispersion length (for linear pulse broadening) and nonlinear length (for self-phase modulation) are determined for this material. These parameters provide insight into the upper limit of pulse intensity and crystal length required to generate intense terahertz pulse without detriment to the pulse shape. It is found that for 1-mm thick ZnGeP$_{2}$(012), pumped at 1.28 micron with intensity of ~15 GW/cm2 will produce intense undistorted pulses, whereas longer crystals or larger intensities modify the pulse shape to varying degrees. Moreover, phase-matching dispersion maps are presented for the terahertz generation over a large tuning range (1.1-2.4 micron) in longer (3 mm) crystal, demonstrating the phase-matching bandwidth and phase mismatch that leads to fringing associated with multi-pulse interference. All observed results are simulated numerically showing good qualitative agreement., Comment: 7 pages, 4 figures, journal submission, version 2

The angular dependence of terahertz (THz) emission from birefringent crystals can differ significantly from that of cubic crystals. Here we consider optical rectification in uniaxial birefringent materials, such as chalcopyrite crystals. The analysis is verified in (110)-cut ZnGeP_2 and compared to (zincblende) GaP. Although the crystals share the same nonzero second-order tensor elements, the birefringence in chalcopyrite crystals cause the pump pulse polarization to evolve as it propagates through the crystal, resulting in a drastically different angular dependence in chalcopyrite crystals. The analysis is extended to {012}- and {114}-cut chalcopyrite crystals and predicts more efficient conversion for the {114} crystal cut over the {012}- and {110}-cuts., Comment: 6 pages, 3 figure, online journal article

Optical rectification is demonstrated in (110)-cut ZnGeP_2 (ZGP) providing broadband terahertz (THz) generation. The source is compared to both GaP and GaAs over a wavelength range of 1150 nm to 1600 nm and peak intensity range of 0.5 GW/cm^2 to 40 GW/cm^2. ZGP peak-to-peak field amplitude is larger than in the other materials due to either lower nonlinear absorption or larger second order nonlinearity. This material is well suited for broadband THz generation across a wide range of infrared excitation wavelengths., Comment: 4 pages, 3 figures, journal article