Intra-pulse Difference Frequency Generation Research Articles

Ultra-broadband spectroscopy using a 2–11.5 µm IDFG-based supercontinuum source

Supercontinuum sources based on intrapulse difference frequency generation (IDFG) from mode-locked lasers open new opportunities in mid-infrared gas spectroscopy. These sources provide high power and ultra-broadband spectral coverage in the molecular fingerprint region with very low relative intensity noise. Here, we demonstrate the performance of such a light source in combination with a multipass cell and a custom-built Fourier transform spectrometer (FTS) for multispecies trace gas detection. The light source provides a low-noise, ultra-broad spectrum from 2–11.5 µm with ∼3 W output power, outperforming existing mid-infrared supercontinuum sources in terms of noise, spectral coverage, and output power. This translates to an excellent match for spectroscopic applications, establishing (sub-)ppb sensitivity for molecular hydrocarbons (e.g., CH4, C2H4), oxides (e.g., SO2, NOx), and small organic molecules (e.g., acetone, ethyl acetate) over the spectral range of the supercontinuum source with a measurement time varying from seconds to minutes. We demonstrate a practical application by measuring the off-gas composition of a bioreactor containing an acidic ammonia-oxidizing culture with the simultaneous detection of multiple nitrogen oxides (NO, NO2, N2O, etc.). As the different species absorb various parts of the spectrum, these results highlight the functionality of this spectroscopic system for biological and environmental applications.

Ultra-phase-stable infrared light source at the watt level.

Ultrashort pulses at infrared wavelengths are advantageous when studying light-matter interaction. For the spectral region around 2 µm, multi-stage parametric amplification is the most common method to reach higher pulse energies. Yet it has been a key challenge for such systems to deliver waveform-stable pulses without active stabilization and synchronization systems. Here, we present a different approach for the generation of infrared pulses centered at 1.8 µm with watt-level average power utilizing only a single nonlinear crystal. Our laser system relies on a well-established Yb:YAG thin-disk technology at 1.03 µm wavelength combined with a hybrid two-stage broadening scheme. We show the high-power downconversion process via intra-pulse difference frequency generation, which leads to excellent passive stability of the carrier envelope phase below 20 mrad-comparable to modern oscillators. It also provides simple control over the central wavelength within a broad spectral range. The developed infrared source is employed to generate a multi-octave continuum from 500 nm to 2.5 µm opening the path toward sub-cycle pulse synthesis with extreme waveform stability.

Maximizing the efficiency of intrapulse difference frequency generation by pulse shaping and recycling

Maximizing the efficiency of intrapulse difference frequency generation by pulse shaping and recycling

Compact mid-infrared dual-comb spectrometer over 3–4 μm via intra-pulse difference frequency generation in LiNbO3 waveguides

Abstract The mid-infrared optical frequency comb is a powerful tool for gas sensing. In this study, we demonstrate a simple mid-infrared dual-comb spectrometer covering 3–4 μm in LiNbO3 waveguides. Based on a low-power fiber laser system, the mid-infrared comb is achieved via intra-pulse difference frequency generation in the LiNbO3 waveguide. We construct pre-chirp management before supercontinuum generation to control spatiotemporal alignment for pump and signal pulses. The supercontinuum is directly coupled into a chirped periodically poled LiNbO3 waveguide for the 3–4 μm idler generation. A mid-infrared dual-comb spectrometer based on this approach provides a 100 MHz resolution over 25 THz coverage. To evaluate the applicability for spectroscopy, we measure the methane spectrum using the dual-comb spectrometer. The measured results are consistent with the HITRAN database, in which the root mean square of the residual is 3.2%. This proposed method is expected to develop integrated and robust mid-infrared dual-comb spectrometers on chip for sensing.

High-resolution frequency-comb spectroscopy with electro-optic sampling and instantaneous octave-wide coverage across mid-IR to THz at a video rate

Ultrabroadband electro-optic sampling using few-optical-cycle probing pulses is a sensitive technique to detect electric field amplitudes with a high dynamic range and up to near-infrared optical frequencies. By combining this method with dual-frequency-comb spectroscopy and using a new class of ultrafast lasers, we perform high-resolution, 80 MHz/0.0027 cm−1 (10 MHz/0.0003 cm−1 with spectral interleaving), spectroscopic measurements in the frequency range 1.5–45 THz (6.6–200 µm), excluding the strongly absorbing Reststrahlen band of lattice resonances at 4.5–9 THz, with an instantaneous spectral coverage exceeding an octave (e.g., 9–22 μm). As a driving source, we use a pair of mutually coherent combs from Kerr-lens mode-locked solid-state Cr:ZnS (2.35 μm) lasers. One of the combs is frequency downconverted via intrapulse difference frequency generation to produce a longwave “sensing” comb, while the second comb is frequency doubled to produce a near-IR “probe” comb for electro-optic sampling (EOS). The low intensity and phase noise of our dual-comb system allow for capturing a large amount of spectral information (200 000 comb-mode-resolved spectral lines spaced by 80 MHz) in the mid-IR portion of the spectrum at a video rate of 69 Hz, with the signal-to-noise ratio limited by the shot noise of the near-IR EOS balanced detection system. Our dual-comb spectroscopy measurements with low-pressure gaseous ethanol, isoprene, and dimethyl sulfide reveal Doppler-limited spectroscopic signatures that have never been explored before.

In-line synthesis of multi-octave phase-stable infrared light.

Parametric downconversion driven by modern, high-power sources of 10-fs-scale near-infrared pulses, in particular intrapulse difference-frequency generation (IPDFG), affords combinations of properties desirable for molecular vibrational spectroscopy in the mid-infrared range: broad spectral coverage, high brilliance, and spatial and temporal coherence. Yet, unifying these in a robust and compact radiation source has remained a key challenge. Here, we address this need by employing IPDFG in a multi-crystal in-line geometry, driven by the 100-W-level, 10.6-fs pulses of a 10.6-MHz-repetition-rate, nonlinearly post-compressed Yb:YAG thin-disk oscillator. Polarization tailoring of the driving pulses using a bichromatic waveplate is followed by a sequence of two crystals, LiIO3 and LiGaS2, resulting in the simultaneous coverage of the 800-cm-1-to-3000-cm-1 spectral range (at -30-dB intensity) with 130 mW of average power. We demonstrate that optical-phase coherence is maintained in this in-line geometry, in theory and experiment, the latter employing ultra-broadband electro-optic sampling. These results pave the way toward coherent spectroscopy schemes like field-resolved and frequency-comb spectroscopy, as well as nonlinear, ultrafast spectroscopy and optical-waveform synthesis across the entire infrared molecular fingerprint region.

Ultra-CEP-stable single-cycle pulses at 2.2  µm

Single-cycle optical pulses with controllable carrier-envelope phase (CEP) form the basis to manipulate the nonlinear polarization of matter on a sub-femtosecond time scale. Moreover, nonlinear light–matter energy exchange and frequency conversion processes benefit from longer, infrared wavelengths. We report a highly stable source of 6.9-fs, single-cycle pulses at 2.2 µm, based on a directly diode-pumped Cr:ZnS oscillator with 22.9-MHz repetition rate. Extreme spectral broadening of the oscillator output to a super-octave bandwidth (1.1–3.1 µm) is achieved in a single rutile (TiO2) plate. Excellent agreement with simulations provides a precise understanding of the underlying nonlinear pulse propagation. A comprehensive investigation of alternative broadening materials and additional simulations single out the exceptional broadening in TiO2 due to the favorable interplay of self-focusing, and plasma formation accompanied by self-phase modulation and self-compression. Unprecedented reproducibility of the single-cycle waveforms is ensured by a unique combination of active CEP stabilization with a residual CEP jitter of only 5.9 mrad (0.1 Hz to 11.45 MHz) and a relative intensity noise of 0.036% (0.1 Hz to 1 MHz). The new single-cycle source permits efficient downconversion to the mid-infrared by cascaded intra-pulse difference frequency generation, giving access to sub-femtosecond manipulation of electric currents in low-bandgap materials with an unprecedented degree of control.

Intra-pulse difference frequency generation in ZnGeP2 for high-frequency terahertz radiation generation

The highly-nonlinear chalcopyrite crystal family has experienced remarkable success as source crystals in the mid-infrared spectral range, such that these crystals are primary candidates for producing high terahertz frequency (i.e., gtrsim 10 THz) electric fields. A phase-resolved terahertz electric field pulse is produced via intra-pulse difference frequency generation in a chalcopyrite (110) ZnGeP2 crystal, with phase-matching being satisfied by the excitation electric field pulse having polarizations along both the ordinary and extraordinary crystal axes. While maximum spectral power is observed at the frequency of 24.5 THz (in agreement with intra-pulse phase-matching calculations), generation nonetheless occurs across the wide spectral range of 23–30 THz. To our knowledge, this is the first time a chalcopyrite ZnGeP2 crystal has been used for the generation of phase-resolved high-frequency terahertz electric fields.

Longwave infrared (6.6-11.4 µm) dual-comb spectroscopy with 240,000 comb-mode-resolved data points at video rate.

Using sub-3-cycle pulses from mode-locked Cr:ZnS lasers at λ ≈ 2.4 µm as a driving source, we performed high-resolution dual-frequency-comb spectroscopy in the longwave infrared (LWIR) range. A duo of highly coherent broadband (6.6-11.4 µm) frequency combs were produced via intrapulse difference frequency generation in zinc germanium phosphide (ZGP) crystals. Fast (up to 0.1 s per spectrum) acquisition of 240,000 comb-mode-resolved data points, spaced by 80 MHz and referenced to a Rb clock, was demonstrated, resulting in metrology grade molecular spectra of N2O (nitrous oxide) and CH3OH (methane). The key to high-speed massive spectral data acquisition was low intensity and phase noise of the LWIR combs and high (7.5%) downconversion efficiency, resulting in a LWIR power of 300 mW for each comb.

Intensity noise in difference frequency generation-based tunable femtosecond MIR sources.

We characterize the intensity noise of two mid-infrared (MIR) ultrafast tunable (3.5-11 μm) sources based on difference frequency generation (DFG). While both sources are pumped by a high repetition rate Yb-doped amplifier delivering 200 μJ 300 fs at a central wavelength of 1030 nm, the first is based on intrapulse DFG (intraDFG), and the second on DFG at the output of an optical parametric amplifier (OPA). The noise properties are assessed through measurement of the relative intensity noise (RIN) power spectral density and pulse-to-pulse stability. The noise transfer mechanisms from the pump to the MIR beam is empirically demonstrated. As an example, improving the pump laser noise performance allows reduction of the integrated RIN (IRIN) of one of the MIR source from 2.7% RMS down to 0.4% RMS. The intensity noise is also measured at various stages and in several wavelength ranges in both laser system architectures, allowing us to identify the physical origin of their variation. This study presents numerical values for the pulse to pulse stability, and analyze the frequency content of the RINs of particular importance for the design of low-noise high repetition rate tunable MIR sources and future high performance time-resolved molecular spectroscopy experiments.

Mid-infrared pulse generation using multi-plate white-light generation and optical parametric amplification in LiGaS2 crystals

We demonstrate intense mid-infrared pulse generation with a pulse energy of up to 6.2 μJ and a tunable wavelength range of 5.3–7.4 μm. This light source is based on white-light generation by multi-plate pulse compression of the output of a commercial Yb:KGW laser pulse followed by intra-pulse difference frequency generation (DFG) and optical parametric amplification in LiGaS2 crystals. Due to the use of intra-pulse DFG, we were able to generate carrier-envelope phase (CEP)-stable mid-infrared optical pulses with a CEP standard deviation of 114 mrad, corresponding to a timing fluctuation of 360 attoseconds during the 5-hour-long measurement.

Generation of 17-32 THz radiation from a CdSiP2 crystal.

A phase-resolved electric field pulse is produced through the second-order nonlinear process of intra-pulse difference frequency generation (DFG) in a (110) CdSiP2 chalcopyrite crystal. The generated electric field pulse exhibits a duration of several picoseconds and contains frequency components within the high-frequency terahertz regime of ∼17-32 THz. The intra-pulse DFG signal is shown to be influenced by single-phonon and two-phonon absorption, the nonlinear phase-matching criterion, and temporal spreading of the excitation electric field pulse. To date, this is the first investigation in which a CdSiP2 chalcopyrite crystal is used to produce radiation within the aforementioned spectral range.

Suppression of Pulse Intensity Dependent Dispersion during Nonlinear Spectral Broadening with Intermediate Compression for Passive CEP Stable Pulse Generation

The intensity fluctuation induced spectral phase-change of the laser pulse during nonlinear spectral broadening is theoretically investigated. The oscillation of the phase-change curves at the central part of the spectra is explained by the two-wave interference model, while the bending of the phase-change curves at the wings is considered to originate from the intensity dependent dispersion caused by the self-steepening (SST) effect. Both of them can degrade carrier envelop phase (CEP) stability after an intra-pulse difference frequency generation (IP-DFG) setup. We propose an effective approach to suppress the intensity dependent dispersion with intermediate compression. Verified by numerically simulations, well-phased spectral components at the wings can be obtained, which is highly beneficial for CEP stable pulse generation with noisy input.

Efficient generation of mid-infrared few-cycle pulses by the intrapulse difference-frequency generation in YCOB.

Yttrium calcium oxyborate (YCOB) crystals have been widely applied for generating intense near-infrared laser pulses by optical parametric amplification. Here, we show that the YCOB crystals oriented in both the XZ and XY principal planes possess broadband phase-matching property of intrapulse difference-frequency generation in the mid-infrared region. Few-cycle pulses tunable from 2 to 4 µm are experimentally produced by using a 7.5-fs pump laser at 800 nm, in which the conversion efficiency can be as high as 2.5%. With a large-size crystal and high-power pump laser, intrapulse difference-frequency generation based on YCOB may provide a new route for directly producing intense few-cycle mid-infrared pulses.

Inline amplification of mid-infrared intrapulse difference frequency generation.

We demonstrate an ultrafast mid-infrared source architecture that implements both intrapulse difference frequency generation (iDFG) and further optical parametric amplification (OPA), in an all-inline configuration. The source is driven by a nonlinearly compressed high-energy Yb-doped-fiber amplifier delivering 7.4 fs pulses at a central wavelength of 1030 nm, at a repetition rate of 250 kHz. It delivers 1 µJ, 73 fs pulses at a central wavelength of 8 µm, tunable over more than one octave. By enrolling all the pump photons in the iDFG process and recycling the long wavelength pump photons amplified in the iDFG in the subsequent OPA, we obtain an unprecedented overall optical efficiency of 2%. These performances, combining high energy and repetition rate in a very simple all-inline setup, make this technique ideally suited for a growing number of applications, such as high harmonic generation in solids or two-dimensional infrared spectroscopy experiments.

Broadband 1-GHz mid-infrared frequency comb

Mid-infrared (MIR) spectrometers are invaluable tools for molecular fingerprinting and hyper-spectral imaging. Among the available spectroscopic approaches, GHz MIR dual-comb absorption spectrometers have the potential to simultaneously combine the high-speed, high spectral resolution, and broad optical bandwidth needed to accurately study complex, transient events in chemistry, combustion, and microscopy. However, such a spectrometer has not yet been demonstrated due to the lack of GHz MIR frequency combs with broad and full spectral coverage. Here, we introduce the first broadband MIR frequency comb laser platform at 1 GHz repetition rate that achieves spectral coverage from 3 to 13 µm. This frequency comb is based on a commercially available 1.56 µm mode-locked laser, robust all-fiber Er amplifiers and intra-pulse difference frequency generation (IP-DFG) of few-cycle pulses in χ(2) nonlinear crystals. When used in a dual comb spectroscopy (DCS) configuration, this source will simultaneously enable measurements with μs time resolution, 1 GHz (0.03 cm−1) spectral point spacing and a full bandwidth of >5 THz (>166 cm−1) anywhere within the MIR atmospheric windows. This represents a unique spectroscopic resource for characterizing fast and non-repetitive events that are currently inaccessible with other sources.

Single-cycle infrared waveform control

Tailoring the electric-field waveform of ultrashort light pulses forms the basis for controlling nonlinear optical phenomena on their genuine, attosecond timescale. Here we extend waveform control from the visible and near-infrared—where it was previously demonstrated—to the mid-infrared spectral range. Our approach yields single-cycle infrared pulses over several octaves for the first time. Sub-10-fs pulses from a carrier-envelope-phase-stabilized, Kerr-lens-mode-locked, diode-pumped Cr:ZnS laser drive cascaded intrapulse difference-frequency generation and control the electric-field evolution of the resulting coherent emission over 0.9–12.0 μm. Sub-cycle field control in this wavelength range will be instrumental for launching and steering few-femtosecond electron/hole wavepackets in low-gap materials, extending the bandwidth of electronic signal processing to multi-terahertz frequencies, as well as for electric-field-resolved molecular fingerprinting of biological systems.

Simple approach to broadband mid-infrared pulse generation with a mode-locked Yb-doped fiber laser.

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. Although IDFG systems pumped with 1.5- or 2-µm ultrashort pulsed lasers have been extensively developed, few systems have been demonstrated with 1-µm lasers, which use bulky 100-W-class high-power Yb thin-disk lasers. In this work, we demonstrate a simple and robust approach of 1-µm-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 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 µm). The 1-µm-based IDFG system allows for additional generations of ultrashort pulses in the ultraviolet and visible regions, enabling, for example, 50-MHz-level high-repetition-rate vibrational sum-frequency generation spectroscopy or pump-probe spectroscopy.

Efficient generation of few-cycle pulses beyond 10\xa0\u03bcm from an optical parametric amplifier pumped by a 1-\xb5m laser system

Nonlinear vibrational spectroscopy profits from broadband sources emitting in the molecular fingerprint region. Yet, broadband lasers operating at wavelengths above 7 μm have been lacking, while traditional cascaded parametric frequency down-conversion schemes suffer from exceedingly low conversion efficiencies. Here we present efficient, direct frequency down-conversion of femtosecond 100-kHz, 1.03-μm pulses to the mid-infrared from 7.5 to 13.3 μm in a supercontinuum-seeded, tunable, single-stage optical parametric amplifier based on the wide-bandgap material Cd0.65Hg0.35Ga2S4. The amplifier delivers near transform-limited, few-cycle pulses with an average power > 30 mW at center wavelengths between 8.8 and 10.6 μm, at conversion efficiencies far surpassing that of optical parametric amplification followed by difference-frequency generation or intrapulse difference-frequency generation. The pulse duration at 10.6 μm is 101 fs corresponding to 2.9 optical cycles with a spectral coverage of 760–1160 cm−1. CdxHg1−xGa2S4 is an attractive alternative to LiGaS2 and BaGa4S7 in small-scale, Yb-laser-pumped, few-cycle mid-infrared optical parametric amplifiers and offers a much higher nonlinear figure of merit compared to those materials. Leveraging the inherent spatial variation of composition in CdxHg1−xGa2S4, an approach is proposed to give access to a significant fraction of the molecular fingerprint region using a single crystal at a fixed phase matching angle.

Enhanced intrapulse difference frequency generation in the mid-infrared by a spectrally dependent polarization state.

We present a technique to optimize the intrapulse difference frequency generation efficiency for mid-infrared generation. The approach employs a multi-order wave plate that is designed to selectively rotate the polarization state of the incoming spectral components on the relevant orthogonal axes for subsequent nonlinear interaction. We demonstrate a significant increase of the mid-infrared average power generated, of a factor ≥2.5 compared with the conventional scheme, owing to an optimally distributed number of photons enrolled in the difference frequency generation process.