Difference Frequency Generation Research Articles

Continuous-wave long-wavelength infrared difference-frequency generation in ZGP driven by near-infrared fiber lasers.

We report the continuous-wave (cw) difference-frequency generation (DFG) in a ZnGeP2 (ZGP) crystal that produces tunable long-wavelength infrared (LWIR) lasing. Particularly, we experimentally demonstrate the feasibility to drive DFG in ZGP by all-fiber near-infrared fiber lasers consisting of a 1.3 µm tunable cw random Raman fiber laser (RRFL) and a 1.5 µm erbium-doped fiber amplifier seeded by a tunable distributed feedback (DFB) laser, making the whole system compact and robust. As a result, the demonstrated LWIR DFG presents a broadband spectral tuning range spanning from 9.5 to 11.5 µm, and the output powers in the spectral range of 9.5-11 µm are larger than 40 µW pumped by watt-level fiber lasers. Meanwhile, as a typical application, a proof-of-concept demonstration of gas sensing of SF6 is executed based on the generated cw LWIR source. Our work demonstrates that the combination of ZGP crystal and fiber lasers can provide an effective and robust approach for the generation of cw LWIR radiation with useful power and broadband wavelength tunability.

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.

High-SNR mid-infrared dual-comb spectroscopy using active phase control cooperating with CWs-dependent phase correction.

Mid-infrared (MIR) dual-comb spectroscopy (DCS) is a highly effective method for molecular metrology of rovibrational transition spectra in a quick accurate manner. However, due to limited comb frequency instability, manipulating coherence between two frequency combs to accomplish high-quality spectral analysis in the MIR region is a huge challenge. Here, we developed a comb-teeth resolved MIR DCS based on active phase control cooperating with a CWs-dependent (CWD) interferogram timing correction. Firstly, four meticulously engineered actuators were individually integrated into two near-infrared (NIR) seed combs to facilitate active coherence maintenance. Subsequently, two PPLN waveguides were adopted to achieve parallel difference frequency generations (DFG), directly achieving a coherent MIR dual-comb spectrometer. To improve coherence and signal-to-noise ratio (SNR), a CWD resampled interferogram timing correction was used to optimize the merit of DCS from 7.5 × 105 to 2.5 × 106. Meanwhile, we carried out the measurement of MIR DCS on the methane hot-band absorption spectra (v3 band), which exhibited a good agreement with HITRAN by a standard deviation on recording residual of 0.76%. These experimental results confirm that this MIR DCS with CWD interferogram timing correction has significant potential to characterize the rovibrational transitions of MIR molecules.

Simultaneous generation and manipulation of terahertz waves based on nonlinear leaky-waveguide antennas with integrated bianisotropic metasurfaces.

We hereby propose and theoretically investigate a new scheme for simultaneous generation and manipulation of terahertz (THz) waves through difference frequency generation facilitated by a metasurface-assisted nonlinear leaky waveguide antenna. The proposed structure integrates a nonlinear optical waveguide, composed of multiple AlxGa1-xAs layers, with a THz leaky waveguide, wherein a bianisotropic metasurface realizes the radiating aperture. By explicitly utilizing the electric, magnetic, and magnetoelectric coupling responses of the metasurface, we demonstrate that the generated THz wave can be induced as a tightly confined, phase-matched guided mode for efficient generation of the THz wave. Additionally, this approach allows the THz wave to be transformed into a directive beam, radiating at a user-defined leakage rate and direction. Our numerical analyses suggest that THz beams ranging from 2.85 THz to 3.05 THz can be steered from 4 ∘ to 40 ∘, utilizing the inherent beam-steering capabilities of the leaky-waveguide antenna. Within this THz frequency spectrum, the phase matching condition is achieved by adjusting the optical wavelengths between 1.6μm and 1.52μm. In particular, the nonlinear conversion efficiency is 2.9 × 10-5 [1/W] at 3 THz.

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

Polarization-insensitive and polarization-controlled dual-band third-harmonic generation in silicon metasurfaces driven by quasi-bound states in the continuum

High-refractive-index nanostructures offer versatile opportunities for nonlinear optical effects, due to their ability to strongly confine field into a subwavelength scale. Herein, we propose a rhomboidal amorphous silicon metasurface to realize high-efficiency dual-band third-harmonic generation (THG), based on the supported dual quasi-bound states in the continuum (Q-BICs). Owing to the very large field confinement inside the metasurface empowered by Q-BICs, the THG efficiency up to 3.74 × 10−3 with the peak pump intensity of 30 MW/cm2 is observed. Meanwhile, thanks to the very high quality factor of Q-BICs, the ultra-narrow nonlinear process with the full width at half maximum less than 1 nm is also witnessed, suggesting the good monochromaticity. Interestingly, the dual-band THG is verified to be polarization-dependent and polarization-insensitive, respectively. The finite element method simulations exhibit that the polarization-dependent THG is attributed to the Q-BIC driven by the electric quadrupole characterized by a pair of anti-parallel electric dipoles along the x axis, which are only excited by the x-linearly polarized light. On the contrary, the polarization-insensitive THG is enabled by another Q-BIC governed by the magnetic dipole resonance with circular electric field vectors, which can be excited by any linearly polarized light. The polarization-controlled and polarization-independent dual-band THG enabled by the physics of Q-BICs would open possibilities for designing switchable nonlinear light sources. The proposed dual Q-BICs scheme undoubtedly can serve as a universal recipe for other nonlinear effects, including sum-frequency generation, difference-frequency generation, and high-order harmonics.

Novel 40 µm spot size 3050/3200 nm DFG laser versus CO2 laser for laser-assisted drug delivery.

The use of ablative fractional lasers to enhance the delivery of topical drugs through the skin is known as laser-assisted drug delivery. Here, we compare a novel 3050/3200 nm difference frequency generation (DFG) fiber laser (spot size: 40 µm) to a commercially used CO2 laser (spot size: 120 µm). The objective is to determine whether differences in spot size and coagulation zone (CZ) thickness influence drug uptake. Fractional ablation was performed on ex-vivo human abdominal skin with the DFG (5 mJ) and CO2 (12 mJ) lasers to generate 680 µm deep lesions. To evaluate drug delivery, 30 kDa encapsulated fluorescent dye was topically applied to the skin and histologically analyzed at skin depths of 100, 140, 200, 400, and 600 µm. Additionally, transcutaneous permeation of encapsulated and 350 Da nonencapsulated dye was assessed using Franz Cells. The DFG laser generated smaller channels (diameter: 56.5 µm) with thinner CZs (thickness: 22.4 µm) than the CO2 laser (diameter: 75.9 µm, thickness: 66.8 µm). The DFG laser treated group exhibited significantly higher encapsulated dye total fluorescence intensities after 3 h compared to the CO2 laser treated group across all skin depths (p < 0.001). Permeation of nonencapsulated dye was also higher in the DFG laser treated group vs the CO2 laser treated group after 48 h (p < 0.0001), while encapsulated dye was not detected in any group. The DFG laser treated skin exhibited significantly higher total fluorescence uptake compared to the CO2 laser. Additionally, the smaller spot size and thinner CZ of the DFG laser could result in faster wound healing and reduced adverse effects while delivering similar or greater amount of topically applied drugs.

Unidirectional ring laser operation and tunable single-frequency emission using differential parametric gain.

In this Letter, a novel approach for unidirectional operation of a 1064 nm solid-state ring laser is demonstrated based on difference frequency mixing. Unidirectional operation is achieved exploiting the directional parametric gain from a single-pass diode laser, facilitated through a periodically poled LiNbO3 crystal. In addition to achieving unidirectional operation, the nonlinear process further enables the generation of single-frequency mid-infrared light. Using a single-pass tapered diode laser, tunable in the range from 780 to 815 nm, the generated mid-infrared signal covers the 2.9 to 3.5 µm range while optimizing the phase-match condition of the difference frequency generation process.

Mid-IR narrow bandwidth tuneable laser source for the FAMU experiment

The FAMU (Fisica degli Atomi MUonici) collaboration aims to measure the proton Zemach radius through muonic hydrogen (μp) spectroscopy. The experimental setup relies on a custom-developed pulsed mid-IR laser source that can be tuned over a specific 6780-6790 nm wavelength range needed to ignite the hyperfine transition of the μp ground state 1S (also known as spin-flip transition). The excitation is observed as a distinctive muonic X-rays emission resulting from the oxygen impurity present in the hydrogen target. The mid-IR emission is produced by Difference Frequency Generation (DFG) in a non-linear crystal, pumped with a fixed wavelength 1064 nm Nd-YAG laser and a tuneable Cr:forsterite laser centred on 1262 nm. This setup produces more than 1.2 mJ at 6780 nm with a linewidth smaller than 30 pm. The experiment requires the laser to run continuously 24/7 in a restricted/radiation-controlled area and for this reason a specifically developed control software permits to remotely act on the laser. The characterization of a series of different non-linear crystals was performed during the development of the laser, resulting in the choice of BaGa4Se7.

Wavelength Dependence of Output Energy in Terahertz Wave Difference Frequency Generation Pumped by a Tunable Dual-KTiOPO$_{4}$ Optical Parametric Oscillator Source

Wavelength Dependence of Output Energy in Terahertz Wave Difference Frequency Generation Pumped by a Tunable Dual-KTiOPO$_{4}$ Optical Parametric Oscillator Source

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.

Coherent FIR/THz wave generation and steering via surface-emitting thin film lithium niobate waveguides.

Generating narrowband, continuous wave FIR/THz light via difference frequency generation (DFG) remains challenging due to material absorption and dispersion from optical phonons. The relatively new platform of thin film lithium niobate enables high-confinement nonlinear waveguides, reducing device size and potentially improving efficiency. We simulated surface-emitting DFG from 10 to 100 THz in a thin film lithium niobate waveguide with fixed poling period, demonstrating reasonable efficiency and bandwidth. Furthermore, adjusting wavelength and relative phase in an array of these waveguides enables beam steering along two directions. Continuous wave FIR/THz light can be efficiently generated and steered using these integrated devices.

Resonant x-ray difference frequency generation

Resonantly enhanced x-ray difference-frequency generation (re-XDFG) is a second-order nonlinear effect that involves illuminating a molecule with two-color x-ray pulses with photon energies Ω1 and Ω2. The energy difference is tuned to match an x-ray absorption edge of an atom in the molecule. We have numerically studied the re-XDFG effect considering different individual molecules in the gas phase using density functional theory calculations and have verified the non-centrosymmetric character of the target transitions. Two-level molecular systems with permanent dipoles are evaluated for the description of re-XDFG taking into account different two-color input pulse geometries. This innovative nonlinear x-ray methodology offers a means to measure the K-edge NEXAFS spectrum of light elements, such as carbon, nitrogen, or oxygen, in dense media using non-resonant x-rays. It can also be used to investigate chemical material dynamics that are inaccessible by linear spectroscopy. These findings enable the combination of atomic-scale structure with chemical specificity and the selective and local access to x-ray excitations using hard x-ray pulses.

Precise parameter control of multicycle terahertz generation in PPLN using flexible pulse trains.

The low (sub %) efficiencies so-far demonstrated for nonlinear optical down-conversion to terahertz (THz) frequencies are a primary limiting factor in the generation of high-energy, high-field THz-radiation pulses (in particular narrowband, multicycle pulses) needed for many scientific fields. However, simulations predict that far higher conversion efficiencies are possible by use of suitably-optimized optical sources. Here we implement a customized optical laser system producing highly-tunable trains of infrared pulses and systematically explore the experimental optimization of the down-conversion process. Our setup, which allows tuning of the energy, duration, number and periodicity of the pulses in the train, provides a unique capability to test predictions of analytic theory and simulation on the parameter dependences for the optical-to-THz difference-frequency generation process as well as to map out, with unprecedented precision, key properties of the nonlinear crystal medium. We discuss the agreements and deviations between simulation and experimental results which, on the one hand, shed light on limitations of the existing theory, and on the other hand, provide the first steps in a recipe for development of practical, high-field, efficiency-optimized THz sources.

Y-shaped tunable monolithic dual colour lasers for THz technology

Abstract. THz generation by difference frequency generation can be accomplished by many different laser systems. The most cost efficient and compact solution will be monolithic dual-colour lasers. Application of these lasers in THz metrology can suffer from several drawbacks like coupling between the modes, strong amplitude variations, low tuning capabilities, or a complicated growth process. We discuss the impact of these points for THz measurements and present a simple monolithic dual colour laser which can be used for material characterisations.

Quantum Interferometric Pathway Selectivity in Difference-Frequency-Generation Spectroscopy.

Even-order spectroscopies such as sum-frequency generation (SFG) and difference-frequency generation (DFG) can serve as direct probes of molecular chirality. Such signals are usually given by the sum of several interaction pathways that carry different information about matter. Here we focus on DFG, involving impulsive optical-optical-IR interactions, where the last IR pulse probes vibrational transitions in the ground or excited electronic state manifolds, depending on the interaction pathway. Spectroscopy with classical light can use phase matching to select the two pathways. In this theoretical study, we propose a novel quantum interferometric protocol that uses entangled photons to isolate individual pathways. This additional selectivity originates from engineering the state of light using a Zou-Wang-Mandel interferometer combined with coincidence detection.

Frequency conversion of orbital angular momentum with optimized efficiency and modal purity

The use of nonlinear optics for the creation, control, and detection of structured light has gained prominence of late, but it is plagued by low efficiency and variable modal purity. Here, we show how to optimize the efficiency and modal purity in the nonlinear conversion of structured light modes. Using difference frequency generation of orbital angular momentum carrying Laguerre–Gaussian modes as an example, we achieved more than a 40% rise in efficiency while maintaining the modal purity above 90% compared to conventional methods. To demonstrate the versatility of our approach, we show the frequency conversion of perfect vortex beams up to ℓ=40 in a topological charge, achieving a new state of the art. We believe this theoretical treatment will facilitate our work’s translation to other modal forms and nonlinear processes.

Narrow linewidth and wideband tunable continuous-wave terahertz generator based on difference frequency generation with DAST crystal.

A narrow linewidth and wideband tunable continuous-wave terahertz generator with DAST crystal has been demonstrated in this paper. Two narrow-linewidth CW fiber lasers were used as the pump sources for difference frequency generation. The terahertz wave can be continuously tunable in the range of 1.1-3 THz. The maximum output power of 2.79nW was obtained at 2.568 THz. The linewidth of the output THz wave was estimated to be 56.5 MHz by fitting transmission spectrum of CO gas at 450 Pa pressure around 80.52 cm-1 with the Vogit gas model. Furthermore, the output spectra at room temperature and pressure was in good agreement with the air absorption lines in Hitran database. Moreover, the narrower absorption characteristic spectrum of 2-Deoxy-D-Glucose sample has been obtained through the spectrum measurements. Therefore, it could promote the practical prospect of tunable CW-THz source, which will have good potential in THz high-precision spectroscopic detection and multispectral imaging.

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.

Selective BTEX detection using laser absorption spectroscopy in the CH bending mode region

BTEX (benzene, toluene, ethylbenzene, and xylene) are simple aromatics that play a major role in soot formation in combustion systems. They are widely used as aromatic representatives in fuel surrogates. Measuring BTEX in chemical reactors can give insight into the soot formation mechanisms and help mitigate its production. The similar chemical structures of BTEX make their selective detection highly challenging. These species give rise to broad and similar absorption features across most of the electromagnetic spectrum. In this work, we report the development of a selective BTEX laser-based sensor in the long-wave mid-infrared (LW-MIR) spectral region. The sensor probes the rarely accessed CH bending modes of BTEX molecules and takes advantage of the strong, spectrally isolated absorption features of aromatics in this spectral region. The developed sensor is based on a custom-designed difference-frequency generation (DFG) laser source. Wavelength selection, and the development and evaluation of the performance of the custom-designed sensor are discussed. The sensor was found to perform excellently over the mole fraction range of 0 - 1,000 ppm of each of the BTEX species. Estimated detection limits of our developed sensor are 60, 15, 40, and 50 ppm for benzene, toluene, ethylbenzene, and m-xylene, respectively.