Second-harmonic Signal Research Articles

Inline UV pulse synthesizer

We demonstrated an inline synthesizer for generating ultrashort pulses in the ultraviolet (UV) range. The inline UV pulse synthesizer comprised three nonlinear crystals located in the propagation path of the fundamental driving laser pulse. Second-harmonic signals with central wavelengths of 420, 375, and 345 nm were generated in turn in the three BBO crystals, resulting in a synthesized UV pulse subsequent to the final nonlinear crystal. Its temporal amplitude and phase could be manipulated easily by changing the relative positions of the crystals, allowing for flexibility of the waveform. The minimum pulse duration of the synthesized UV pulse was 4.7 fs, which was close to the Fourier-transform-limited pulse duration. This ultrashort UV pulse with 19 μ\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\upmu$$\\end{document}J energy can be utilized in various applications such as high harmonic generation and frustrated tunneling ionization.

Theory of the interference tunability of second harmonic generation for two-dimensional materials in layered structures

We theoretically study how the intensity of second harmonic generation (SHG) for a sheet of two-dimensional (2D) material is controlled by an underlying layered structure. By utilizing the transfer matrix method with the inclusion of a nonlinear sheet current to describe the response of the 2D material, an explicit expression for the intensity of upward propagating second harmonic (SH) light is obtained, and the effects of the layered structure can be identified by a structure factor β, defined as the ratio of SH intensity from such a structure to that from a freely suspended 2D material. Our results show that the influence of a layered structure on the SHG intensity arises from interference effects of both the fundamental light and the SH light; the value of the structure factor is 0 ≤ β ≤ 64. Furthermore, when the incident light is pulsed, the interference effects are partially canceled due to the existence of many wave vectors and frequencies, and the cancellation becomes severe for thick films, small beam spots, and short pulses. For a specific structure of 2D material/dielectric film/substrate, the thickness of the dielectric film can effectively tune the value of β in an interval [βmin, βmax], and detailed discussions are performed for the thicknesses when these two extreme values can be obtained. When there is optical loss or the substrate is not perfectly reflective, the extreme value of βmax or βmin cannot reach 64 or 0. A large βmax requires two conditions to be fulfilled: (1) the substrate should be highly reflective, and (2) the refractive indices of the dielectric film at the fundamental and the SH frequencies should differ. Our results indicate how practical substrate structures can be used to achieve high SH signals, and the simple expression we give for the SH enhancement will be useful in characterizing the nonlinear susceptibility of 2D materials.

Even-order optical harmonics generated from centrosymmetric-material metasurfaces

Generation of even-order optical harmonics requires noncentrosymmetric structures being conventionally observed in crystals lacking the center of inversion. In centrosymmetric systems, even-order harmonics may arise, e.g., at surfaces but such effects are usually very weak. Here we observe optical harmonics up to fourth order generated under the normal incidence from centrosymmetric dielectric metasurfaces empowered by resonances. We design silicon metasurfaces supporting optical quasibound states in the continuum and guided-mode resonances, and demonstrate the enhancement of second-harmonic signals by over three orders of magnitude compared to nonresonant thin films. Under the optimal conditions, the brightness of the second harmonic approaches that of the third harmonic, and the fourth-order harmonic becomes detectable. Published by the American Physical Society 2024

Plasmonic electro-optic modulators on lead zirconate titanate platform

Abstract The advancement in material platforms exhibiting strong and robust electro-optic effects is crucial for further progress in developing highly efficient and miniaturized optoelectronic components with low power consumption for modern optical communication systems. In this work, we investigate thin-film lead zirconate titanate (PZT) substrates grown by a chemical solution deposition technique as a potential platform for on-chip plasmonic electro-optic modulators. A high modulation depth (>40 %) is achieved with 15 μm-long electro-optic directional coupler modulators. An unusual cutoff in the modulation frequency response at ∼200 kHz is observed and further studied with respect to possible reorientation effects. Second-harmonic generation signals are found influenced by the externally applied electric field, indicating that the domain reorientation effect can be responsible for the unusual frequency response observed.

Polarization-resolved super-resolution second-harmonic generation imaging based on multifocal structured illumination microscopy.

Polarization-resolved second-harmonic generation (PSHG) microscopy is widely used in investigating the structural and morphological alterations of collagen. However, the resolution of second-harmonic generation (SHG) imaging remains constrained by optical diffraction, resulting in the polarization extraction of collagen characteristics from the average properties of collagen fibers. In this study, multifocal structured illumination microscopy (MSIM) was combined with PSHG to achieve polarization-resolved super-resolution imaging of second-harmonic generation signals. For the first time to our knowledge, periodic structures with an average pitch of 277 nm were observed in mouse tail tendons using optical microscopy, and the orientation angle of fibrils within each period was found to exhibit an alternating arrangement along the axis in a regular pattern.

DC Voltage Induces Quadratic Optical Nonlinearity in Ion-Exchanged Glasses at Room Temperature

We demonstrate that applying DC voltage at room temperature to an ion-exchanged glass induces quadratic optical nonlinearity in a subsurface region of the glass. We associate this with the EFISH (Electric-Field-Induced Second Harmonic) effect due to the Maxwell–Wagner charge accumulation in the subsurface region of the glass, in which a conductivity gradient forms as a result of the ion exchange processing. The second harmonic (SH) signal from the soda–lime glass subjected to potassium-for-sodium ion exchange is comparable with one from the same glass after thermal poling. The signal linearly increases with the duration of the ion exchange. The lower mobility of the potassium ions results in a higher SH signal from the potassium-for-sodium exchanged glass than that from the silver-for-sodium ion-exchanged one. This phenomenon is resistant to thermal annealing: only a 500 °C anneal caused noticeable degradation of the SH signal after “charging” the specimen. The phenomenon found is of interest for characterizing graded conductivity regions and providing and controlling second-order optical nonlinearity in transparent isotropic media.

Electric Tuning of Vortex Ratchet Effect in NbSe2.

Inversion symmetry breaking has played an important role in recent discoveries of nonreciprocal charge transport. Niobium diselenide, for example, lacks an inversion center in the monolayer form and can host prominent nonreciprocal transport property. Here, however, we observe a nonreciprocal transport signal in the second-harmonic channel of bulk-like NbSe2, in which inversion symmetry of the lattice seems preserved. The second-harmonic signal occurs along different in-plane current orientations and appears not only in the vortex-liquid regime but also even in the superconducting fluctuation regime without an applied magnetic field. By adding a direct current (DC) bias, we quantify the symmetry breaking effect in the vortex-liquid regime. The DC bias also suggests that the rectification effect at the contacts may account for the seemingly nonreciprocal transport at zero magnetic field. Our results demonstrate that DC biasing is a useful knob for addressing nonreciprocal charge transport in a wide range of materials.

Development of continuous monitoring of ambient carbon dioxide using near-infrared quartz-enhanced photoacoustic spectroscopy

We demonstrate continuous measurement of carbon dioxide (CO2) in the atmosphere using quartz-enhanced photoacoustic spectroscopy (QEPAS) at 2.008 μm with a fiber-coupled distributed-feedback laser. The QEPAS sensor is composed of a quartz tuning fork with a resonance frequency f 0 of 12.4 kHz. The photoacoustic second-harmonic (2f) signal resulting from CO2 absorption was detected using a digital lock-in amplifier. The photoacoustic signal is proportional to the laser power. The limit of detection at an absorption line of 4980.13161 cm−1 with a line strength of 3.87 × 10−22 cm2 molecule−1 cm−1 was 12 parts per million with an integration time of 10 s. The results of the continuous monitoring of ambient CO2 using the QEPAS sensor corresponded to those obtained using a nondispersive IR sensor. The QEPAS sensor exhibited a suitable performance for field measurements of the CO2 mixing ratio.

A Multi-Scale Approach to Simulate the Nonlinear Optical Response of Molecular Nanomaterials.

Nonlinear optics is essential for many recent photonic technologies. Here, a novel multi-scale approach is introduced to simulate the nonlinear optical response of molecular nanomaterials combining ab initio quantum-chemical and classical Maxwell-scattering computations. In this approach, the first hyperpolarizability tensor is computed with time-dependent density-functional theory and incorporated into a multi-scattering formalism that considers the optical interaction between neighboring molecules. Such incorporation is achieved by a novel object: the Hyper-Transition(T)-matrix. With this object at hand, the nonlinear optical response from single molecules and also from entire photonic devices can be computed, including the full tensorial and dispersive nature of the optical response of the molecules, as well as the optical interaction between different molecules as, for example, in the lattice of a molecular crystal. To demonstrate the applicability of the novel approach, the generation of a second-harmonic signal from a thin film of an Urea molecular crystal is computed and compared to more traditional simulations. Furthermore, an optical cavity is designed, which enhances the second-harmonic response of the molecular film up to more than two orders of magnitude. This approach is highly versatile and accurate and can be the working horse for the future exploration of nonlinear photonic molecular materials in structured photonicenvironments.

Effects of Temperature and Humidity on the Absorption Spectrum and Concentration of N2O Using an Open-Path Sensor System

This paper examines the effects of temperature and humidity on the absorption spectrum and concentration of nitrous oxide (N2O) using a compact, portable open optical-path gas detection sensor system. We obtained the absorption coefficient and widened the linear function of the N2O absorption spectrum related to temperature by theoretical analysis and the high-resolution transmission molecular absorption database (HITRAN). Afterward, we conducted real-time monitoring of N2O in both campus and laboratory environments using lasers for a duration of 32 h and 6 h, respectively, and the results were compared and analyzed with the theoretical derivation. The results show that the concentration of N2O increased with increasing environmental temperature but decreased with increasing humidity. Furthermore, the variations in temperature and humidity significantly affected the peak values of the second-harmonic (2f) and first-harmonic (1f) signals. Finally, the temperature N2O concentration and humidity N2O curves were calibrated separately, and temperature changes were positively correlated with the N2O concentration, while humidity changes were negatively correlated with the N2O concentration. The experimental results indicate that the concentration of N2O and its absorption spectra are influenced by humidity and temperature, which has a significant reference value in the absorption and measurement of N2O in practical applications.

All-optical generation of static electric field in a single metal-semiconductor nanoantenna

Electric field is a powerful instrument in nanoscale engineering, providing wide functionalities for control in various optical and solid-state nanodevices. The development of a single optically resonant nanostructure operating with a charge-induced electrical field is challenging, but it could be extremely useful for novel nanophotonic horizons. Here, we show a resonant metal-semiconductor nanostructure with a static electric field created at the interface between its components by charge carriers generated via femtosecond laser irradiation. We study this field experimentally, probing it by second-harmonic generation signal, which, in our system, is time-dependent and has a non-quadratic signal/excitation power dependence. The developed numerical models reveal the influence of the optically induced static electric field on the second harmonic generation signal. We also show how metal work function and silicon surface defect density for different charge carrier concentrations affect the formation of this field. We estimate the value of optically-generated static electric field in this nanoantenna to achieve ≈108V/m. These findings pave the way for the creation of nanoantenna-based optical memory, programmable logic and neuromorphic devices.

High-coherence hybrid-integrated 780 nm source by self-injection-locked second-harmonic generation in a high-Q silicon-nitride resonator

Visible, high-coherence optical sources are important to a wide range of applications spanning spectroscopy to precision timing. Integration of these sources on a semiconductor chip is a necessary step if the systems that use these devices are to be made compact, portable, and low power. Here, by self-injection-locking a 1560 nm distributed feedback semiconductor laser to a high-Q silicon-nitride resonator, a high-coherence 780 nm second-harmonic signal is generated via the photogalvanic-induced second-order nonlinearity. A record-low frequency noise floor of 4Hz2/Hz is achieved for the 780 nm emission. The approach can potentially generate signals over a wide range of visible and near-visible bands, and thereby help transition many table-top systems into a fieldable form.

Comparative study on the second-harmonic generation of thermally poled fused silica by multi-energy boron and argon ion implantations

The second-order optical nonlinearity (SON) of thermally poled fused silica was shown for the first time to be significantly improved by the implantation of multi-energy boron (B) ions, and the outcomes were compared with those obtained from the implantation of multi-energy argon (Ar) ions. Second-harmonic (SH) signals in both samples grew roughly linearly as the poling temperature rose. Samples with Ar implants showed a greater increase in SH signal with rising poling temperature. A qualitative explanation for the formation of [Formula: see text] in poled samples can be found in a model of charge hopping and migration through defects. The diminished SH signal in the B-implanted sample is probably caused by the negative charge trapping layer, as well as by B[Formula: see text] and E[Formula: see text] center defects.

In-Situ Temporal Characterization of Chirped Ultra-Broadband Laser Pulses Exciting a Dual-Light Emitter Er3+-Doped Perovskite

We take advantage of the dual emission properties of up-conversion fluorescence (UCF) and second harmonic generation (SHG) in Er3+-doped perovskite Na0.95Er0.05Nb0.9Ti0.1O3 to fully temporally characterize the ultrashort laser pulse that excites Er3+-ion fluorescence. The chirped pulses from a broadband Ti:Sa oscillator are temporally characterized using the dispersion scan (d-scan) technique by using the SHG signal in the host perovskite at the same point where UCF is being produced by the same pulse. The pulse durations obtained range from ~45 fs to ~8 fs and positive and negative spectral phases are unambiguously identified. The temporal characterization is compared using a standard non-linear crystal and perfect agreement is obtained. These results show that it is possible to temporally characterize in-situ ultrashort laser pulses while they are inducing a UCF process, as long as the host generates second-harmonic signal.

Determining the absolute temporal field of ultra-broadband terahertz-infrared pulses with field-induced second-harmonic spectrograms.

We demonstrate the use of spectrograms of the field-induced second-harmonic (FISH) signal generated in ambient air, to reconstruct the absolute temporal electric field of ultra-broadband terahertz-infrared (THz-IR) pulses with bandwidths exceeding 100 THz. The approach is applicable even with relatively long (150-femtosecond) optical detection pulses, where the relative intensity and phase can be extracted from the moments of the spectrogram, as demonstrated by transmission spectroscopy of very thin samples. Auxiliary EFISH/ABCD measurements are used to provide the absolute field and phase calibration, respectively. We take into account the beam-shape/propagation effects about the detection focus on the measured FISH signals, which affect the field calibration, and show how an analysis of a set of measurements vs. truncation of the unfocused THz-IR beam can be used to correct for these. This approach could also be applied to the field calibration of ABCD measurements of conventional THz pulses.

Large Spontaneous Polarization Ferroelectric Property, Switchable Second-Harmonic Generation Responses, and Magnetism in an Fe-Based Compound.

Since the switchable spontaneous polarization of ferroelectric materials endows it with many useful properties such as a large pyroelectric coefficient, switchable spontaneous polarization, and semiconductor, it has a wide range of application prospects, and the research of high-performance molecular ferroelectric materials has become a hot spot. We obtained a 0D organic-inorganic hybrid ferroelectric [(CH3)3NCH2CH2CH3]2FeCl4 (1) with well-defined ferroelectric domains and excellent domain inversion and exhibited a relatively large spontaneous polarization (Ps = 9 μC/m-2) and a Curie temperature (Tc) of 394 K. Furthermore, compound 1 belongs to the non-centrosymmetrical space group Cmc21 and has a strong second-harmonic generation signal. Interestingly, we also performed magnetic tests on 1, which confirmed that it is a magnetic material. This work provides clues for exploring the application of high-performance molecular ferroelectric materials in future multifunctional smart devices.

Suppression of coherent interference to electric-field-induced second-harmonic (E-FISH) signals for the measurement of electric field in mesoscale confined geometries.

We present spatially enhanced electric-field-induced second-harmonic (SEEFISH) generation with a chirped femtosecond beam for measurements of electric field in mesoscale confined geometries subject to destructive spurious second-harmonic generation (SHG). Spurious SHG is shown to interfere with the measured E-FISH signal coherently, and thus simple background subtraction is not sufficient for single-beam E-FISH approaches, especially in a confined system with a large surface-to-volume ratio. The results show that a chirped femtosecond beam is effective in preventing higher-order mixing and white light generation in windows near the beam focal point which further contaminates the SEEFISH signal. The successful measurements of electric field of a nanosecond dielectric barrier discharge in a test cell demonstrated that spurious SHG detected with a congruent traditional E-FISH approach can be eliminated using the SEEFISH approach.

Nonlinear circular dichroism in achiral dielectric nanoparticles

We present a theoretical study of circular dichroism in the second-harmonic signal of single dielectric nanostructures with different symmetries and noncentrosymmetric materials. We show that this effect is defined not only by macroscopic (particle) and lattice symmetries but also by their relative orientation. Using symmetry and modal analysis, we provide a general and very simple formula to determine whether the dichroism exists and a chart with the most significant cases.

Research on Noise Reduction Method of Second-Harmonic Signal

Research on Noise Reduction Method of Second-Harmonic Signal

Tuning the Čerenkov second harmonic contrast from ferroelectric domain walls via anomalous dispersion

Second harmonic (SH) microscopy represents a powerful tool for the investigation of crystalline systems, such as ferroelectrics and their domain walls (DWs). Under the condition of normal dispersion, i.e., the refractive index at the SH wavelength is larger as compared to the refractive index at the fundamental wavelength, n(2ω)>n(ω), bulk crystals will generate no SH signal. Should the bulk, however, contain DWs, an appreciable SH signal will still be detectable at the location of DWs stemming from the Čerenkov mechanism. In this work, we demonstrate both how SH signals are generated in bulk media and how the Čerenkov mechanism can be inhibited by using anomalous dispersion, i.e., n(ω)>n(2ω). This allows us to quantitatively estimate the relative strength of the Čerenkov compared to other SH contrast mechanisms in DWs, such as the interference contrast. The results are in agreement with previous experiments based on the geometric separation of the signals. Due to the observed, strong Čerenkov contrast, such signal contributions may not be neglected in polarimetry studies of ferroelectric DWs in the future.