Nonlinear Conversion Processes Research Articles

Intra-oscillator high harmonic source reaching 100-eV photon energy

Resonant enhancement inside an optical cavity has been a wide-spread approach to increase efficiency of nonlinear optical conversion processes while reducing the demands on the driving laser power. This concept has been particularly important for high harmonic generation XUV sources, where passive femtosecond enhancement cavities allowed significant increase in repetition rates required for applications in photoelectron spectroscopy, XUV frequency comb spectroscopy, including the recent endeavor of thorium nuclear clock development. In addition to passive cavities, it has been shown that comparable driving conditions can be achieved inside mode-locked thin-disk laser oscillators, offering a simplified single-stage alternative. This approach is less sensitive to losses thanks to the presence of gain inside the cavity and should thus allow higher conversion efficiencies through tolerating higher intensity in the gas target. Here, we show that the intra-oscillator approach can indeed surpass the much more mature technology of passive enhancement cavities in terms of XUV flux, even reaching comparable values to single-pass sources based on chirped-pulse fiber amplifier lasers. Our system operates at 17 MHz repetition rate generating photon energies between 60 eV and 100 eV. Importantly, this covers the highly attractive wavelength for the silicon industry of 13.5 nm at which our source delivers 60 nW of outcoupled average power per harmonic order.

Design Considerations for Continuous Wave Intracavity Backwards Optical Parametric Oscillators

In this paper, we report a theoretical systematic study of continuous wave intracavity backwards optical parametric oscillators based on periodically poled lithium niobate (PPLN) for mid-infrared (mid-IR) light generation. We study the effects of varying different cavity parameters including nonlinear crystal length, cavity size, pump laser diode spot size, output coupler radius, and cavity loss values on the output power and threshold of the proposed mid-IR laser. The effects of different physical phenomena are included in the model including pump depletion due to the nonlinear conversion process, the thermal lens effect, and mode overlap between the beams in the nonlinear crystal. We show that high output powers in the mid infrared (>500 mW at 3.2 μm) can be achieved with proper cavity design and that a laser threshold with a PPLN as short as 2 cm can be reached.

Few-cycle 65-µJ pulses at 11.4 µm for ultrafast nonlinear longwave-infrared spectroscopy

Low-energy excitations can provide insight into the basic ultrafast nonequilibrium dynamics of condensed matter. High-energy femtosecond pulses in the long-wavelength infrared are required to induce such processes, and can be generated in an optical parametric chirped pulse amplification (OPCPA) system comprising three GaSe stages. A femtosecond Cr:ZnS laser serves as the front-end, providing the seed for the 2.0-µm pump and the 2.4-µm signal pulses without nonlinear conversion processes. The OPCPA system is pumped at 2.05 µm by a picosecond Ho:YLF regenerative amplifier at a 1-kHz repetition rate. The recompressed idler pulses at 11.4 µm have a duration of 185 fs and an unprecedented energy of 65 µJ, corresponding to a pump-to-idler conversion efficiency of 1.2%. Nonlinear transmission experiments in the range of the L2 infrared band of liquid water demonstrate the potential of the pulses for nonlinear vibrational spectroscopy of liquids and solids.

Topological aspects in nonlinear optical frequency conversion

Nonlinear optical frequency conversion, observed more than half a century ago, is a corner stone in modern applications of nonlinear and quantum optics. It is well known that frequency conversion processes are constrained by conservation laws, such as momentum conservation that requires phase matching conditions for efficient conversion. However, conservation laws alone could not fully capture the features of nonlinear frequency conversion. Here it is shown that topology can provide additional constraints in nonlinear multi-frequency conversion processes. Unlike conservation laws, a topological constraint concerns with the conserved properties under continuous deformation, and can be regarded as a new indispensable degree of freedom to describe multi-frequency processes. We illustrate such a paradigm by considering sum frequency generation under a multi-frequency pump wave, showing that, akin topological phases in topological insulators, topological phase transitions can be observed in the frequency conversion process both at classical and quantum level.

Detuning modulated composite segments for robust optical frequency conversion

The creation of efficient broadband frequency conversion devices while maintaining robustness to manufacturing and setup errors is crucial for accurate multiphoton spectroscopy, broadband imaging and the design of robust optical sources. Traditionally, nonlinear optical conversion processes are either efficient but narrowband or broadband but with low photon conversion yield. Several methods have been introduced in recent years to obtain both with great success, among them we can find adiabatic frequency conversion and Shaka–Pines composite segmented design. Here, we expand the composite design and introduce the detuning modulated composite segmented (DMCS) scheme in nonlinear optics, which offers a broadband, efficient and robust method for frequency conversion. We also present the constant-length DMCS scheme, which offers multiple efficient and robust wavelength regimes for broadband upconversion. We apply these schemes to a system of quasi-phase-matching crystal for the sum frequency generation process, and demonstrate the high robustness and bandwidth of the composite schemes. We show that these schemes are robust to temperature and crystal length variations and can have a superior conversion bandwidth under length and power constraints compared to other conversion schemes, such as periodically poled and adiabatic chirped crystals. We believe that the new family of DMCS schemes will have many uses in applications of frequency conversion, due to their robustness, low energy demand and compact size.

Coupling effects of the sum-frequency process and difference-frequency process on upconversion terahertz-wave detection via a DAST crystal.

Frequency upconversion technology with good performance including high sensitivity, fast response, and room-temperature operation is a promising method for terahertz-wave detection. The sum-frequency conversion and difference-frequency conversion jointly affect the detection ability for upconversion detection using organic crystals as nonlinear media. The concurrence of both processes has been ignored in past studies, which results in discrepancies between theoretical simulations and experimental results. In this paper, four-wave interaction equations involving two nonlinear conversion processes are proposed, and the effect of the sum-frequency process is analyzed in upconversion terahertz-wave detection via a 4-dimethylamino-N-methyl-4-stilbazolium tosylate (DAST) crystal. The ratio of the sum-frequency signal to the difference-frequency signal varies for different terahertz frequencies and crystal thicknesses. Experiments suggest that theoretical simulations are good at predicting physical processes. Under certain conditions, the detection efficiency can be improved by simultaneously utilizing the two signals. The total signal photon number is not sensitive to the crystal thickness. Furthermore, the theoretical exploration of terahertz single-photon detection provides a noteworthy reference for future experiments.

Quantum Sensing with Extreme Light

AbstractOptical nonlinear conversion processes are ubiquitously applied to scientific as well as industrial tasks. In particular, nonlinear processes are employed to generate radiation in many frequency ranges. In plenty of these nonlinear processes, the generation of paired photons occurs — the so‐called signal and idler photons. Although this type of generation has undergone a tremendous development over the last decades, either the generated signal or the idler radiation has been used experimentally. In contrast, novel quantum‐based measurement principles enable the usage of both partners of the generated photon pairs based on their correlation. These measurement approaches have an enormous potential for future applications, as they allow to transfer information from one spectral range to another. In particular, spectral ranges where photon generation and detection is particularly challenging can benefit from this principle. Above all, these include the extreme frequency ranges, such as on the low‐frequency side the mid to far infrared or even the terahertz spectral range, but also on the high‐frequency side the ultraviolet or X‐ray spectral range. In this review article, theoretical and experimental developments based on correlated biphotons are described specifically for the extreme spectral regions.

Graphene-based passive Q-switching of a Dy3+,Tb3+:LuLiF4 yellow laser

We report solid-state continuous-wave (cw) and Q-switched lasers directly emitting in the yellow spectral region, which include a Dy3+,Tb3+:LuLiF4 crystal as the laser material and a single-emitter blue laser diode (LD) as the pump source. Without resorting to any nonlinear conversion process, a maximum output power of 351 mW is obtained for the cw yellow laser with a slope efficiency of 15% at the wavelength of 573.9 nm. For generating the Q-switched yellow laser, a monolayer graphene is used as the saturable absorber. The maximum average output power of the Q-switched yellow laser is determined to be 85 mW. The shortest pulse width is obtained as approximately 596 ns, which corresponds to a repetition rate of 78 kHz. The calculated pulse energy and peak power are nearly 1.1 μJ and 1.8 W, respectively. Overall, the proposed approach exhibits immense potential for fabricating compact and economical solid-state cw and Q-switched yellow lasers.

An adaptive piecewise linearized weighted directed graph for the modeling and operational optimization of integrated energy systems

Operational optimization plays a vital role in ensuring the economy, security, and environmental friendliness of integrated energy systems (IES), while the nonlinear operating characteristics of energy converters have brought significant challenges to the accurate modeling and solution. Considering the nonlinear energy conversion processes, a novel adaptive piecewise linearized weighted directed graph model of IES is proposed in this paper. To accurately construct the complex energy flow relationship in IES, a weighted directed graph is first presented to describe the energy generation, conversion, storage, consumption, and demand response, thus realizing the automatic modeling of IES. On this basis, for the diverse partial-load performance of energy converters, an adaptive piecewise linearization strategy is developed to approximate the nonlinear operating characteristics of various energy converters adaptively. By taking the system operating cost, calculation time, energy mismatch, and optimization model complexity as evaluation indicators, the effectiveness of the proposed method is verified by the numerical simulations of a typical small-scale combined cooling, heating, and power (CCHP) system and a large-scale IES in a realistic industrial park. Compared with the constant efficiency method and the equispaced piecewise linearization method, the computational efficiency and accuracy are remarkably improved by the proposed method.

High efficiency 355 nm laser by employing a flat-flat cavity with improved harmonic beam quality

A high efficiency 355 nm ultraviolet (UV) laser is obtained by intracavity frequency-tripling of a 1064 nm Nd:YVO4 laser in a flat-flat cavity. The 5.6 W UV maximum average output power is obtained at the incident pump power of 29 W at 808 nm and the repetition rate of 50 kHz, corresponding to the pump-UV conversion efficiency of 19.3%. The corresponding pulse width is 14.2 ns, with the energy of a single pulse and corresponding peak power estimated to be 112 μJ and 7.89 kW, respectively. The frequency doubling and tripling lasers are obtained by employing type-I phase-matching LiB3O5 (LBO) crystal with parallel surfaces and a type-II phase-matching LBO crystal with Brewster angle-cut uncoated surface, respectively. The beam quality of the 355 nm laser is measured to be M x 2 = 1.257 and M y 2 = 1.173, respectively. The reasons for improvement of harmonic beam quality are explained by simulating the laser field intensity distribution changes in two special directions during the nonlinear conversion process.

Highly efficient difference-frequency generation for mid-infrared pulses by passively synchronous seeding

Abstract We have proposed and experimentally demonstrated a novel scheme for efficient mid-infrared difference-frequency generation based on passively synchronized fiber lasers. The adoption of coincident seeding pulses in the nonlinear conversion process could substantially lower the pumping threshold for mid-infrared parametric emission. Consequently, a picosecond mid-infrared source at 3.1 μm was prepared with watt-level average power, and a maximum power conversion efficiency of 77% was realized from pump to down-converted light. Additionally, the long-term stability of generated power was manifested with a relative fluctuation as low as 0.17% over one hour. Thanks to the all-optical passive synchronization and all-polarization-maintaining fiber architecture, the implemented laser system was also featured with simplicity, compactness and robustness, which would favor subsequent applications beyond laboratory operation.

Practical method for parametric array source evaluation at 120 kHz frequency range in the near-field region

A parametric array is a non-linear conversion process that can generate a narrow beam of low-frequency sound with a small aperture. One of the challenging issues with a parametric array is precise measurement of the sound field generated. In particular, near the transducer, it is not easy to measure the sound field generated by a parametric array precisely, because the amplitude of the difference frequency wave is much lower than the amplitude of the primary wave. In this study, the practical issues that should be considered in the design of near-distance experiments with a parametric array are examined. Limiting effects were examined, and their associated characteristics were identified by numerical simulations. Experiments were performed in a water tank (18 x 12 x 10 m) to assess these characteristics, using a custom-designed acoustic filter; the beam pattern and propagation curve of the difference frequency wave generated by the parametric array were measured and compared with simulated data.

Competitive Effects of Surface Plasmon Resonances and Interband Transitions on Plasmon-Enhanced Second-Harmonic Generation at Near-Ultraviolet Frequencies

The competition between plasmonic resonances and noble-metal interband transitions at near-ultraviolet (NUV) frequencies complicates nonlinear conversion processes at nanoscales. Here, we experimentally design a highly enhanced and reproducible plasmon-enhanced second-harmonic generation (PESHG) platform suitable for NUV frequencies by constructing three-dimensional silver mushroom arrays. The SHG emission from proposed platforms involved in geometrical asymmetry greatly outperforms that from unpatterned metallic films. Studies among mushroom arrays with various geometric parameters and weight ratios of component materials enable us to distinguish characteristics exhibited by plasmon-driven enhancement and interband-transition suppression, such that competitive effects on PESHG can be readily observed and quantitatively measured. Our work may provide insights for understanding the physical mechanism governing plasmon-enhanced nonlinear optical processes and may help attain efficient nonlinear wavelength conversions for quantum-optical and nonlinear metamaterial applications.

Efficient Production of Sound Waves by AGN Jets in the Intracluster Medium

Abstract We investigate the interaction between active galactic nucleus (AGN) jets and the intracluster medium (ICM) of galaxy clusters. Specifically, we study the efficiency with which jets can drive sound waves into the ICM. Previous works focused on this issue model the jet–ICM interaction as a spherically symmetric explosion, finding that ≲12.5% of the blast energy is converted into sound waves, even for instantaneous energy injection. We develop a method for measuring sound wave energy in hydrodynamic simulations and measure the efficiency of sound wave driving by supersonic jets in a model ICM. Our axisymmetric fiducial simulations convert ≳25% of the jet energy into strong, long-wavelength sound waves that can propagate to large distances. Vigorous instabilities driven by the jet–ICM interaction generate small-scale sound waves that constructively interfere, forming powerful large-scale waves. By scanning a parameter space of opening angles, velocities, and densities, we study how our results depend on jet properties. High-velocity, wide-angle jets produce sound waves most efficiently, yet the acoustic efficiency never exceeds 1/3 of the jet energy—an indication that equipartition may limit the nonlinear energy conversion process. Our work argues that sound waves may compose a significant fraction of the energy budget in cluster AGN feedback and underscores the importance of properly treating compressive wave dissipation in the weakly collisional, magnetized ICM.

Multi-octave spanning, Watt-level ultrafast mid-infrared source

We present a source of brilliant mid-infrared radiation, seamlessly covering the wavelength range between 1.33 and 18 μm (7500–555 cm−1) with three channels, employing broadband nonlinear conversion processes driven by the output of a thulium-fiber laser system. The high-average-power femtosecond frontend delivers a 50 MHz train of 250 fs pulses spectrally centered at 1.96 μm. The three parallel channels employ soliton self-compression in a fused-silica fiber, supercontinuum generation in a ZBLAN fiber, and difference-frequency generation in GaSe driven by soliton self-compressed pulses. The total output enables spectral coverage from 1.33 to 2.4 μm, from 2.4 to 5.2 μm, and from 5.2 to 18 μm with 4.5 W, 0.22 W and 0.5 W, respectively. This spatially coherent source with a footprint of less than 4 m2 exceeds the brilliance of 3rd-generation synchrotrons by more than three orders of magnitude over 90% of the bandwidth.

Visible to near-infrared octave spanning supercontinuum generation in tantalum pentoxide (Ta2O5) air-cladding waveguide.

In this work, for the first time, to the best of our knowledge, an anomalous dispersion CMOS-compatible Ta2O5 waveguide was realized, and broadband on-chip supercontinuum generation (SCG) was accordingly demonstrated. When pumped at a center wavelength of 1056nm with pulses of 100fs duration and peak power of 396W, a supercontinuum ranging from 585nm to 1697nm was generated, comprising a bandwidth of more than 1.5 octaves and leading to an efficient SCG source. The excellent performance for Ta2O5 to generate SCG benefits mainly from its high nonlinear refractive index, which enhances the efficiency of the nonlinear conversion process.

Thermal noise in mid-infrared broadband upconversion detectors.

Low noise detection with state-of-the-art mid-infrared (MIR) detectors (e.g., PbS, PbSe, InSb, HgCdTe) is a primary challenge owing to the intrinsic thermal background radiation of the low bandgap detector material itself. However, researchers have employed frequency upconversion based detectors (UCD), operable at room temperature, as a promising alternative to traditional direct detection schemes. UCD allows for the use of a low noise silicon-CCD/camera to improve the SNR. Using UCD, the noise contributions from the nonlinear material itself should be evaluated in order to estimate the limits of the noise-equivalent power of an UCD system. In this article, we rigorously analyze the optical power generated by frequency upconversion of the intrinsic black-body radiation in the nonlinear material itself due to the crystals residual emissivity, i.e. absorption. The thermal radiation is particularly prominent at the optical absorption edge of the nonlinear material even at room temperature. We consider a conventional periodically poled lithium niobate (PPLN) based MIR-UCD for the investigation. The UCD is designed to cover a broad spectral range, overlapping with the entire absorption edge of the PPLN (3.5 - 5 µm). Finally, an upconverted thermal radiation power of ~30 pW at room temperature (~30°C) and a maximum of ~70 pW at 120°C of the PPLN crystal are measured for a CW mixing beam of power ~60 W, supporting a good quantitative agreement with the theory. The analysis can easily be extended to other popular nonlinear conversion processes including OPO, DFG, and SHG.

Metasurface-assisted phase-matching-free second harmonic generation in lithium niobate waveguides

The phase-matching condition is a key aspect in nonlinear wavelength conversion processes, which requires the momenta of the photons involved in the processes to be conserved. Conventionally, nonlinear phase matching is achieved using either birefringent or periodically poled nonlinear crystals, which requires careful dispersion engineering and is usually narrowband. In recent years, metasurfaces consisting of densely packed arrays of optical antennas have been demonstrated to provide an effective optical momentum to bend light in arbitrary ways. Here, we demonstrate that gradient metasurface structures consisting of phased array antennas are able to circumvent the phase-matching requirement in on-chip nonlinear wavelength conversion. We experimentally demonstrate phase-matching-free second harmonic generation over many coherent lengths in thin film lithium niobate waveguides patterned with the gradient metasurfaces. Efficient second harmonic generation in the metasurface-based devices is observed over a wide range of pump wavelengths (λ = 1580–1650 nm).

Coherent combining of second-harmonic generators by active phase control of the fundamental waves.

Coherent beam combining by active phase control could be useful for power scaling fiber-laser-pumped optical frequency converters. However, a fast phase modulator operating at the frequency-converted wavelength, a non-standard component, would be necessary. Fortunately, nonlinear conversion processes rely on a phase-matching condition allowing for indirect phase control using standard phase modulators. In this Letter, coherent combining of second-harmonic generators is demonstrated in both birefringent and quasi-phase-matching schemes in CW regime. Phase control operates at the fundamental wavelength, using all-fiber electro-optic modulators. An excellent beam combination is achieved with a residual phase error of λ/30 on the second-harmonic wave.

Polarization-manipulated all-optical cross-wavelength data inversion in a C-rich SiCx micro-ring

Polarization-manipulated all-optical format inversion of a 12.5 Gbit s−1 pulsed return-to-zero on-off-keying (PRZ-OOK) data stream is demonstrated through the nonlinear Kerr switching-induced wavelength conversion process.