Difference Frequency Generation Research Articles

6.7-8.1 μm tunable single frequency difference frequency generation in ZGP for high-resolution spectroscopy

6.7-8.1 μm tunable single frequency difference frequency generation in ZGP for high-resolution spectroscopy

Purifying quantum-dot light in a coherent frequency interface

Abstract Quantum networks typically operate in the telecom wavelengths to take advantage of low-loss transmission in optical fibres. However, bright quantum dots (QDs) emitting highly indistinguishable quantum states of light, such as InGaAs QDs, often emit photons in the near infrared thus necessitating frequency conversion (FC) to the telecom band. Furthermore, the signal quality of quantum emissions is crucial for the effective performance of these networks. In this work we report a method for simultaneously implementing spectral purification and frequency shifting of single photons from QD sources to the c-band in a periodically poled lithium niobate waveguide. We consider difference frequency generation in the counter-propagating configuration to implement FC with the output emission bandwidth in units of GHz. Our approach establishes a clear path to integrating high-performance single-emitter sources in a hybrid quantum network.

Stripe Soliton in All‐Fiber Lasers

AbstractStripe solitons (SSs), the special localized wavepackets exhibiting periodic modulations, are identified in condensed matter physics and nonlinear science. Here, giant‐chirp and chirp‐free SSs in all‐fiber lasers are demonstrated composed of single‐mode fiber and polarization‐maintaining fiber. The chirp property of SSs depends on the cavity dispersion while the stripe period relies on the fiber birefringence. Theoretical and numerical results coincide with experimental findings, revealing that the filtering and frequency shift of two vector modes is governed by the mode coupling related to birefringence and the nonlinear coupling induced by the phase modulation, respectively, which disrupts their complementarity and ultimately leads to modulation of the overall spectrum. With the aid of the saturable absorption and cross‐phase modulation effects, the multi‐color pulses synergistically overlap, giving rise to the unique SSs. These results present a simple approach for generating chirp‐controllable SSs in all‐fiber lasers, which is crucial for applications in difference frequency generation and soliton physics.

Digitally generated high-resolution mid-infrared dual-comb spectroscopy system based on electro-optic modulation.

In this Letter, we propose a high-resolution dual-comb spectroscopy (DCS) in the mid-infrared (MIR) region. A broadband electro-optic frequency comb (EOFC) with a line spacing of 13 GHz is generated in the near-infrared region. The injection locking technique is employed to lock the distributed feedback (DFB) laser to each comb line of the 34 comb lines as the seed laser for the subsequent electro-optic modulation. A dual radio frequency (RF) comb source with a 50 MHz line spacing and a 13 GHz bandwidth drives a single IQ Mach-Zehnder modulator (IQ-MZM), functioning as a single-sideband (SSB) generator and producing a DCS with high spectrum flatness and resolution flexibility. The generated DCS is converted to the MIR region via a nonlinear difference frequency generation (DFG) system. A DCS with a bandwidth of 442 GHz and a resolution of 50 MHz is achieved in the 3.3 µm region, and the figure of merit reaches 2.94×106 H z 12 in a 183.6 ms measurement time.

Monolithic top emitting room temperature THz DFG QCL with index grating for wavelength selection

We present a high performance top emitting room temperature monolithic terahertz (THz) quantum cascade laser based on difference frequency generation (DFG) and a buried modulated distributed feedback grating. Using a semi-insulating InP:Fe substrate combined with an index-coupled grating could minimize the internal losses for the THz mode. The laser consists of two separate transversely superimposed gratings. The first grating provides selective feedback for the mid-infrared pump modes and is realized in an index-coupled DFG grating designed for single-mode operation for two distinct MIR wavelengths. The second metallic grating for THz extraction is carefully aligned to the spatial distribution of the MIR modes. The resulting device lases pulses up to 150 °C in the single mode. The maximum THz output power at RT is 100 μW measured at 3.37 THz. A THz wavelength tuning of around 0.065 nm/K was achieved through thermal tuning of the MIR pump lasers.

Extending mid-infrared wavelength to 6.84 μm in oxide nonlinear optical crystal via birefringence dispersion management.

Extending lasing wavelengths to the mid-infrared (MIR) spectrum is vital for both civilian and military applications; however, it remains challenging when employing oxide nonlinear optical crystals. In this study, we report the generation of MIR nanosecond pulses via difference frequency generation (DFG) with a near-IR pump using a newly designed langasite (LGS) crystal, La3(Nb0.6Ta0.4)0.5Ga5.5O14 (LGNT0.4), which incorporates birefringence dispersion management techniques with La3Ga5.5Nb0.5O14 (LGN) as a template. Due to the improved effective nonlinear coefficients and the maintained IR cutoff relative to LGN, the tunable DFG laser in LGNT0.4 extended from 4.24 to 6.84 μm, delivering a maximum pulse energy of 16.3 μJ at 5.02 μm. To the best of our knowledge, this is the first known oxide material capable of generating tunable nanosecond pulsed lasers beyond 6 μm at μJ-level energies, demonstrating promising potential for high-intensity MIR laser systems owing to its high laser damage threshold.

Efficient and widely tunable mid-infrared sources using GaAs and AlGaAs integrated platforms for second-order frequency conversion

Integrated coherent mid-infrared (mid-IR) sources are crucial for spectroscopy and quantum frequency conversion (QFC) to facilitate scalable fiber-based application of single photons. Direct mid-IR emission with broad tunability poses fundamental challenges from the gain media and mirror components. This paper presents a characterization of a second-order nonlinear platform. It showcases a mid-IR parametric coherent source with a continuous tuning range exceeding 230 nm centered around 2425 nm, achieved through difference-frequency generation (DFG). The nonlinear coefficient d14 of gallium arsenide (GaAs) and aluminum gallium arsenide (AlGaAs) on insulator is experimentally determined via second-harmonic generation (SHG) in waveguides of various lengths, and the tolerance of the process is investigated. These materials are explored for their high conversion efficiency, utilizing monolithic epitaxial quantum dots and integrated waveguides for QFC. The results demonstrate efficient and tunable mid-IR emission suitable for compact, scalable quantum emitters, with applications in environmental and health monitoring.

Difference‐Frequency Generation of 0.2‐mJ 3‐Cycle 9‐µm Pulses from Two 1‐kHz Multicycle OPCPAs

AbstractIntense long‐wave infrared (LWIR) femtosecond pulses within the 8−14 µm atmospheric window present an array of applications, such as in strong‐field physics, ultrafast nonlinear spectroscopy, and self‐guided atmospheric propagation. However, the realization of an LWIR source capable of delivering millijoule‐class energy, few‐cycle duration, and kHz repetition rate concurrently remains challenging. Here, such an LWIR source via the combination of different nonlinear parametric processes is reported, driven by a 1 kHz Yb:YAG thin‐disk laser. The system comprises two parallel multi‐cycle optical parametric chirped‐pulse amplifiers (OPCPAs) operating at 2.3 and 3.1 µm, respectively, alongside a stage of ZnGeP2‐crystal‐based difference‐frequency generation (DFG). The resulting 9 µm DFG pulses have a record energy of 0.21 mJ, a 3‐cycle duration, a 1 kHz repetition rate, and long‐term energy stability. The simultaneous output of three synchronized intense lasers at short‐wave infrared (2.3 µm), mid‐wave infrared (3.1 µm), and LWIR (9 µm) renders the source particularly appealing for multicolor ultrafast applications.

Harnessing complexity: Nonlinear optical phenomena in L-shapes, nanocrescents, and split-ring resonators.

We conduct systematic studies of the optical characteristics of plasmonic nanoparticles that exhibit C2v symmetry. In particular, we analyze three distinct geometric configurations: an L-type shape, a crescent, and a split-ring resonator shaped like the Greek letter π. Optical properties are examined using the finite-difference time-domain method. It is demonstrated that all three shapes exhibit two prominent plasmon modes associated with the two axes of symmetry. This is in addition to a wide range of resonances observed at high frequencies corresponding to quadrupole modes and peaks due to sharp corners. Next, to facilitate nonlinear analysis, we employ a semiclassical hydrodynamic model, where the electron pressure term is explicitly accounted for. This model goes beyond the standard Drude description and enables capturing nonlocal and nonlinear effects. Employing this model enables us to rigorously examine the second-order angular resolved nonlinear optical response of these nanoparticles in each of the three configurations. Two pumping regimes are considered, namely, continuous wave (CW) and pulsed excitations. For CW pumping, we explore the properties of the second harmonic generation (SHG). Polarization and angle-resolved SHG spectra are obtained, revealing strong dependence on the nanoparticle geometry and incident wave polarization. The C2v symmetry is shown to play a key role in determining the polarization states and selection rules of the SHG signal. For pulsed excitations, we discuss the phenomenon of broadband terahertz (THz) generation induced by the difference-frequency generation . It is shown that the THz emission spectra exhibit unique features attributed to the plasmonic resonances and symmetry of the nanoparticles. The polarization of the generated THz waves is also examined, revealing interesting patterns tied to the nanoparticle geometry. To gain deeper insight, we propose an analytical theory that agrees very well with the numerical experiments. The theory shows that the physical origin of the THz radiation is the mixing of various frequency components of the fundamental pulse by the second-order nonlinear susceptibility. An expression for the far-field THz intensity is derived in terms of the incident pulse parameters and the nonlinear response tensor of the nanoparticle. The results presented in this work offer new insights into the linear and nonlinear optical properties of nanoparticles with C2v symmetry. The demonstrated strong SHG response and efficient broadband THz generation hold great promise for applications in nonlinear spectroscopy, nanophotonics, and optoelectronics. The proposed theoretical framework also provides a valuable tool for understanding and predicting the nonlinear behavior of other related nanostructures.

Sub-attosecond-precision optical-waveform stability measurements using electro-optic sampling

The generation of laser pulses with controlled optical waveforms, and their measurement, lie at the heart of both time-domain and frequency-domain precision metrology. Here, we obtain mid-infrared waves via intra-pulse difference-frequency generation (IPDFG) driven by 16-femtosecond near-infrared pulses, and characterise the jitter of sub-cycle fractions of these waves relative to the gate pulses using electro-optic sampling (EOS). We demonstrate sub-attosecond temporal jitter at individual zero-crossings and sub-0.1%-level relative amplitude fluctuations in the 10-kHz–0.625-MHz band. Chirping the nearly-octave-spanning mid-infrared pulses uncovers wavelength-dependent attosecond-scale waveform jitter. Our study validates EOS as a broadband (both in the radio-frequency and the optical domains), highly sensitive measurement technique for the jitter dynamics of optical waveforms. This sensitivity reveals outstanding stability of the waveforms obtained via IPDFG and EOS, directly benefiting precision measurements including linear and nonlinear (infrared) field-resolved spectroscopy. Furthermore, these results form the basis toward EOS-based active waveform stabilisation and sub-attosecond multi-oscillator synchronisation/delay tracking.

Simultaneous transmission of multi-format signals in the mid-infrared over free space

Mid-infrared (MIR) light within the 3–5 μm spectrum offers distinct advantages over the 1.5 μm band, particularly in adverse atmospheric conditions, rendering it a favorable option for free-space optical (FSO) communication. The transmission capacity within the 3–5 μm band is relatively low due to the immature state of its devices. In this study, we demonstrate multi-format signals FSO transmission with a total of 40 Gbps capacity in the 3 μm band, utilizing our developed MIR transmitter and receiver modules. These modules facilitate wavelength conversion between the 1.5 μm and 3 μm bands through the utilization of difference-frequency generation (DFG) effect. The MIR transmitter effectively produces three MIR signals: On-Off Keying (OOK), Binary Phase Shift Keying (BPSK), and Quadrature Phase Shift Keying (QPSK) optical signals. The generated MIR power is 7.8 dBm, covering a wavelength range from 3.5864 to 3.5885 μm. The MIR receiver regenerates the three format signals with a power of −29.6 dBm. Relevant results of regenerated signal demodulation have been collected in detail, including bit error ratio (BER), constellation diagram, and eye diagram. The required powers for the 10 Gbps OOK, BPSK, and QPSK are −37.82, −40.24, and −39.4 dBm at BER of 1 × 10−6. It is expected to further push the data capacity to the terabit-per-second level by adding more 1.5 μm band laser sources and using wider-bandwidth chirped nonlinear crystals.

Long-wavelength infrared upconversion time-stretch spectroscopy

High-speed spectroscopy in the molecular fingerprint spectral region (≈6–12 μm) is essential for the detection of ultrafast molecular dynamic processes, rapid combustion analysis, and biological diagnostics. However, ultrafast spectroscopy in the long-wavelength infrared (LWIR) region remains a challenge due to the limitations of laser sources and the lack of ultrafast and sensitive detectors in this wavelength region. Here, we demonstrate broadband LWIR time-stretch spectroscopy, which can realize a single-shot high-speed spectral measurement in a 8–10 μm region, by combining the LWIR femtosecond (fs) light generation and upconversion time-stretching detection with specific dispersive fiber. Broadband tunable fs light generated in the 8–10 μm region is upconverted to the 1.1–1.2 μm near-infrared wavelength via difference-frequency generation with the 1 μm chirped pump pulse. Time-stretch detection of the upconverted light can then be realized by adopting dispersion shifted fiber, which has a superior dispersion-to-loss ratio in the 1.1–1.2 μm wavelength region, as the dispersive medium. As a result, we experimentally demonstrate LWIR time-stretch spectroscopy in the 8–10 μm region with a spectral resolution of 1.07 cm−1, at a rate of 200 kSpectra s−1, which is only limited by the repetition rate of the 1 μm pump source. The demonstration of high-speed time-stretch spectroscopy in the LWIR region would open the possibility in exploring the transient dynamics of molecular fingerprint spectroscopy.

Concurrent phase-matchings for multi-wavelength conversion in coupled dual waveguides

Thin film lithium niobate, as a highly promising integrated photonics platform, has emerged as an ideal material platform for wavelength conversion owing to its exceptional second-order nonlinear characteristics. Here, we present the first demonstration of concurrent phase-matchings for multi-wavelength conversion in coupled thin film lithium niobate waveguides without poling technique. In the coupled dual waveguide system, employing modal phase-matching, we validate three effective phase-matching conditions for second harmonic generation, arising from additional momentum compensation due to the coupling of waveguides. Simultaneously, we confirm that phase-matching wavelengths can be tuned by adjusting the gap between waveguides. The concurrent phase-matchings in coupled dual waveguide systems can be readily extended to other nonlinear optical processes, such as difference frequency generation and spontaneous parametric down conversion. Our work contributes to advancing the exploration of efficient on-chip nonlinear optical processes within the realms of nanophotonics and quantum optics.

Time-resolved ARPES with probe energy of 6.0 eV and tunable MIR pump at 250 kHz

In this paper, we present a laser source designed specifically for time- and angle-resolved photoemission spectroscopy (TR-ARPES) investigations of light-induced electron dynamics in quantum materials. Our laser source is based on a ytterbium-doped laser that seeds an optical parametric amplifier (OPA) followed by a difference frequency generation (DFG) stage. This configuration enables the generation of tunable near-infrared and mid-infrared laser pulses (1.5 to 8 μm - 0.82 to 0.15 eV) at 250 kHz of repetition rate, serving as the pump for TR-ARPES measurements. The remaining energy of the laser is used to generate the ultraviolet 6 eV probe pulses, which prompt the material to emit photoelectrons. We demonstrate the long-term stability of the source, as well as the characterization of the beam profiles and pulse durations. Additionally, we present preliminary TR-ARPES results obtained on Bi2Te3, a prototypical 3D topological insulator. This paper illustrates the capability of our laser source to probe electronic dynamics in quantum materials.

Modelling of long-wave mid-infrared ultrashort pulse generation via difference frequency generation

In this paper, a model of generating mid-infrared (MIR) ultrashort laser pulse through difference frequency generation (DFG) is established. The pulse evolution relationship among the pump, signal, and idler pulses during the DFG process, as well as the effects of crystal length, pulse energy of the pump and signal lights, pulse width, and other factors on the characteristics of the MIR pulse are explored. Furthermore, through simulations from the time domain to the frequency domain, the spectral characteristics and angular distribution of MIR were analyzed. DFG experimental data are also presented to support the model.

Programmable generation of counterrotating bicircular light pulses in the multi-terahertz frequency range

The manipulation of solid states using intense infrared or terahertz light fields is a pivotal area in contemporary ultrafast photonics research. While conventional circular polarization has been well explored, the potential of counterrotating bicircular light remains widely underexplored, despite growing interest in theory. In the mid-infrared or multi-terahertz region, experimental challenges lie in difficulties in stabilizing the relative phase between two-color lights and the lack of available polarization elements. Here, we successfully generated phase-stable counterrotating bicircular light pulses in the 14–39 THz frequency range circumventing the above problems. Employing spectral broadening, polarization pulse shaping with a spatial light modulator, and intra-pulse difference frequency generation leveraging a distinctive angular-momentum selection rule within the nonlinear crystal, we achieved direct conversion from near-infrared pulses into the designed counterrotating bicircular multi-terahertz pulses. Use of the spatial light modulator enables programmable control over the shape, orientation, rotational symmetry, and helicity of the bicircular light field trajectory. This advancement provides a novel pathway for the programmable manipulation of light fields, and marks a significant step toward understanding and harnessing the impact of tailored light fields on matter, particularly in the context of topological semimetals.

Background-free mid-infrared absorption spectroscopy using sub-cycle pulses

We have demonstrated highly sensitive single-shot based background-free mid-infrared (MIR) absorption spectroscopy using sub-cycle MIR pulses generated through filamentation. The MIR pulse transmitted through a sample was upconverted with a fast rising and long tailing gate pulse through four-wave difference frequency generation in a silicon membrane. By recording the upconverted spectrum of the free induction decay alone, we successfully measured the absorption spectrum as a positive signal in the wavenumber range from 500 to 4500 cm−1, which covers both the fingerprint and functional group regions. We obtained an absorption spectrum of ∼50 mM of aqueous glucose, which is not detectable with a standard Fourier transform infrared spectrometer.

Nonlinear upconverted thermal emission through difference frequency generation.

Thermal radiation management is of critical importance in energy, sensing, and heat transfer. According to Planck's law, objects at room temperature predominantly emit thermal radiation within the mid- and far-infrared bands. Here, we demonstrated the upconversion of the mid- and far-infrared thermal radiation emitted by second-order nonlinear material to the easily-detectable visible band through a difference frequency process. This nonlinear broad-spectrum upconversion is facilitated by the random quasi-phase-matching technique in the nanoparticle system. Furthermore, we show the temperature measurement of thermal spots using such nonlinear thermal radiation. This scheme paves the way for applications in thermal management and sensing.

Interfacial epitaxy of multilayer rhombohedral transition-metal dichalcogenide single crystals.

Rhombohedral-stacked transition-metal dichalcogenides (3R-TMDs), which are distinct from their hexagonal counterparts, exhibit higher carrier mobility, sliding ferroelectricity, and coherently enhanced nonlinear optical responses. However, surface epitaxial growth of large multilayer 3R-TMD single crystals is difficult. We report an interfacial epitaxy methodology for their growth of several compositions, including molybdenum disulfide (MoS2), molybdenum diselenide, tungsten disulfide, tungsten diselenide, niobium disulfide, niobium diselenide, and molybdenum sulfoselenide. Feeding of metals and chalcogens continuously to the interface between a single-crystal Ni substrate and grown layers ensured consistent 3R stacking sequence and controlled thickness from a few to 15,000 layers. Comprehensive characterizations confirmed the large-scale uniformity, high crystallinity, and phase purity of these films. The as-grown 3R-MoS2 exhibited room-temperature mobilities up to 155 and 190 square centimeters per volt second for bi- and trilayers, respectively. Optical difference frequency generation with thick 3R-MoS2 showed markedly enhanced nonlinear response under a quasi-phase matching condition (five orders of magnitude greater than monolayers).

Peregrine solitons and resonant radiation in cubic and quadratic media.

We present the fascinating phenomena of resonant radiation emitted by transient rogue waves in cubic and quadratic nonlinear media, particularly those shed from Peregrine solitons, one of the main wavepackets used today to model real-world rogue waves. In cubic media, it turns out that the emission of radiation from a Peregrine soliton can be attributed to the presence of higher-order dispersion, but is affected by the intrinsic local longitudinal variation of the soliton wavenumber. In quadratic media, we reveal that a two-color Peregrine rogue wave can resonantly radiate dispersive waves even in the absence of higher-order dispersion, subjected to a phase-matching mechanism that involves the second-harmonic wave, and to a concomitant difference-frequency generation process. In both cubic and quadratic media, we provide simple analytic criteria for calculating the radiated frequencies in terms of material parameters, showing excellent agreement with numerical simulations.