Harmonic Generation Process Research Articles

Highly Nonlinear Light-Nucleus Interaction.

The interaction between light and atomic nuclei is typically weak and confined within the linear and perturbative regime, which limits the achievable nuclear excitation probability and impedes potential applications such as nuclear optical clocks, nuclear lasers, and nuclear energy storage. In this Letter we show that the interaction between hydrogenlike thorium-229 ions (^{229}Th^{89+}) and contemporary intense lasers propels light-nucleus interaction into a highly nonlinear and nonperturbative regime. This interaction unlocks remarkably efficient nuclear excitation: over 10% of the ^{229}Th nuclei can be excited to the isomeric state by a single femtosecond laser pulse. Moreover, the laser-driven ^{229}Th^{89+} ions radiate multiple wavelengths of light that are high-order harmonics of the laser frequency, akin to the high harmonic generation process from laser-driven atoms but with distinct characteristics. These results pioneer a new frontier for exploring light-matter interaction, furnish a powerful method for efficient control over atomic nuclei, and pave a new way of nuclear coherent light emission.

Metrological robustness of high photon number optical cat states

Abstract In the domain of quantum metrology, cat states have demonstrated their utility despite their inherent fragility with respect to losses. Here, we introduce noise robust optical cat states which exhibit a metrological robustness for phase estimation in the regime of high photon numbers. These cat states are obtained from the intense laser driven process of high harmonic generation (HHG), and show a resilience against photon losses. Focusing on a realistic scenario including experimental imperfections we opt for the case in which we can maximize the lower bound of the quantum Fisher information (QFI) instead of analyzing the best case scenario. We show that the decrease of the QFI in the lossy case is suppressed for the HHG-cat state compared to the even and odd counterparts. In the regime of small losses of just a single photon, the HHG-cat state remains almost pure while the even/odd cat state counterparts rapidly decohere to the maximally mixed state. More importantly, this translates to a significantly enhanced robustness for the HHG-cat against photon loss, demonstrating that high photon number optical cat states can indeed be used for metrological applications even in the presence of losses.

Harmonic‐Assisted Super‐Resolution Rotational Measurement

AbstractEnhancing rotational measurement resolution and broadening the detectable spectral range are two critical and unresolved matters within the realm of motion perception. The rotational Doppler effect (RDE) is combined with the harmonic generation process to create a rotational measurement scheme that offers flexible detection wavelength conversion, exponential improvement of measurement resolution, and real‐time display of detection results. In the experiments, a cascaded second harmonic generation process is employed to attain a fourfold enhancement in rotational resolution and demonstrate how low‐cost silicon‐based detectors can be used for real‐time detection of infrared objects. This scheme employs a Gaussian beam within the nonlinear process to achieve high conversion efficiency, thereby enabling potential for subsequent cascade amplification. Additionally, it is fully compatible with existing RDE schemes, allowing for co‐amplification of rotational resolution at both the front‐end and back‐end. This research could offer a more precise and cost‐effective method for remote sensing detection.

Tabletop Tunable Chiral Photonic Emitter.

The increasing interest in chiral light stems from its spiral trajectory along the propagation direction, facilitating the interaction between different polarization states of light and matter. Despite tremendous achievements in chiral light-related research, the generation and control of chiral pulses have presented enduring challenges, especially at the terahertz and ultraviolet spectral ranges, due to the lack of suitable optical elements for effective pulse manipulation. Conventionally, chiral light can be obtained from intricate optical systems, by an external magnetic field, or by metamaterials, which necessitate sophisticated optical configurations. Here, leveraging the high harmonic generation process, we propose a versatile tunable chiral emitter, composed of only two planar Weyl semimetals slabs, addressing the challenges in both spectral ranges. Our results open the way to a compact tunable chiral emitter platform in both terahertz and ultra-violet frequency ranges. This advancement holds the potential to serve as the cornerstone for integrated chiral photonics.

Bloch-Wave Phase Matching of High Harmonic Generation in Solids.

There has been a longstanding doubt that the conversion efficiency of high harmonics in solids is much lower than expected at such a high level of electron density. To address this issue, we revisit the dynamical process of high harmonic generation (HHG) in solids in terms of wavelet interference. We find that the constructive interference among the wavelets has intrinsic consistency with the phase matching of coupled waves in nonlinear optics, which we call Bloch-wave phase matching. Our analysis indicates that most of the wavelets are out of phase and coherently canceled out during the solid HHG process, leading to only a small fraction of excited electrons effectively contributing to HHG. Consequently, the conversion from the excited electron to HHG is fairly low. Moreover, a Bloch-wave phase-matching scheme is proposed and a nearly 3 orders of magnitude enhancement of solid HHG can be achieved by engineering the crystal structures. Our Letter addresses a longstanding doubt and provides a novel idea and theoretical guidance for realizing efficient all-solid-state tabletop ultraviolet light sources.

Laser harmonic generation with independent control of frequency and orbital angular momentum

The non-linear optical process of laser harmonic generation (HG) enables the creation of high quality pulses of UV or even X-ray radiation, which have many potential uses at the frontiers of experimental science, ranging from lensless microscopy to ultrafast metrology and chiral science. Although many of the promising applications are enabled by generating harmonic modes with orbital angular momentum (OAM), independent control of the harmonic frequency and OAM level remains elusive. Here we show, through a theoretical approach, validated with 3D simulations, how unique 2-D harmonic progressions can be obtained, with both frequency and OAM level tuned independently, from tailored structured targets in both reflective and transmissive configurations. Through preferential selection of a subset of harmonic modes with a specific OAM value, a controlled frequency comb of circularly polarised harmonics can be produced. Our approach to describe HG, which simplifies both the theoretical predictions and the analysis of the harmonic spectrum, is directly applicable across the full range of HG mechanisms and can be readily applied to investigations of OAM harmonics in other processes, such as OAM cascades in Raman amplification, or the analysis of harmonic progressions in nonlinear optics.

Harnessing collisional nonlinearity for enhanced harmonic generation by ultraviolet plasmonic nanoparticles.

We investigate the contribution of inelastic electron collisions to nonlinear (NL) dynamics in ultraviolet plasmonic nanoparticles, exploring their potential for harmonic generation. Employing the Landau weak coupling formalism to model radiation-driven electron dynamics in sodium and aluminum, we account for both electron-electron and electron-phonon scattering processes by a set of hydrodynamic equations, which we solve perturbatively to obtain third-order NL susceptibilities. Furthermore, we model high harmonic generation enhanced by localized surface plasmons in nanospheres composed of such poor metals, demonstrating their efficient operation for extreme ultraviolet generation. Our investigation reveals that plasmonic nanospheres composed of sodium and aluminum produce a large field intensity enhancement of ≃103-105, boosting the harmonic generation process. Our findings indicate that poor metals hold great promise for advanced extreme ultraviolet nano-sources with potential applications in nano-spectroscopy.

Second harmonic generation enhancement based on quasi-BICs in centrosymmetric materials

In centrosymmetric optical materials, the second-order nonlinear polarization of the bulk electric dipolar contribution is zero. More effective utilization of the contribution of the surface term is one of the key methods to efficiently obtain second-order nonlinear responses on these materials. Herein, a design of densely packed slotted nanopillar arrays based on quasi-bound states in the continuum (quasi-BICs) is proposed. The quasi-BICs are analyzed by using the finite element method as an example of silicon and the second harmonic generation (SHG) process is simulated. In the structure, normal-incidence linearly polarized light excites magnetic dipole-like quasi-BICs with a high quality factor which effectively promotes light-matter interactions. Increasing the nanopillar radius or decreasing the lattice constant within a certain range can cause the distribution of quality factors in k-space of the ky direction to contract toward the Γ point, which leads to a quasi-BIC with higher quality factors at the Γ point. By conjunctively adjusting the nanopillar radius and lattice constant or changing the slot azimuth, the resonance wavelength can be adjusted over a wide range (about several hundred nanometers) or finely (within about one nanometer) while maintaining high quality factors. When the symmetry perturbation introduced by the slot is small, it is calculated that the SHG conversion efficiency is about 10−6∼10−5 at an incident light power density of 1 MW/m2, and the SHG power is about 107∼108 times enhancement compared with the structure without slots. As the slot width decreases, higher SHG conversion efficiency with more significant SHG enhancement can be achieved at a specific slot length. The results provide new insights into the modulation of the resonant wavelength and quality factor of quasi-BICs, as well as the control of second-order nonlinear effects in centrosymmetric materials.

Trident edge coupler on thin-film lithium niobate for optimized coupling of octave-separated wavelengths for nonlinear applications

We introduce a trident edge coupler design optimized for the simultaneous coupling of two widely separated wavelengths (2 µm and 1 µm) between a lensed fiber and a 600-nm-thick X-cut lithium-niobate-on-insulator (LNOI) waveguide. These wavelengths are commonly encountered in nonlinear wave mixing applications, representing either the fundamental and second harmonics in second harmonic generation (SHG) processes or the leading and trailing edges of an octave-spanning spectrum generated through broadband nonlinear processes such as frequency comb or supercontinuum generation. Achieving efficient coupling between fibers and strongly confined waveguides in integrated platforms, such as LNOI, can be challenging due to the significant difference in spot sizes between the two wavelengths. Our trident edge coupler offers coupling losses below 1.4 dB for the 2 µm and 1 µm spots simultaneously, showcasing an average transmission enhancement of around 10% compared to the baseline of a single linear taper. Furthermore, it enables a reduction of transmission at 1.5 µm, a typical pump wavelength, with an attenuation of transmission over 10 dB compared to those at the 2 µm and 1 µm wavelengths.

Bound Bogoliubov quasiparticles in photon superfluids

Bogoliubov's description of Bose gases relies on the linear dynamics of noninteracting quasiparticles on top of a homogeneous condensate. Here, we theoretically explore the weakly nonlinear regime of a one-dimensional photon superfluid in which phononlike elementary excitations interact via their backreaction on the background flow. The generalized dispersion relation extracted from spatiotemporal intensity spectra reveals additional branches that correspond to Bogoliubov quasiparticles—phase-locked collective excitations originating from nonresonant harmonic generation and wave-mixing processes. These mechanisms are inherent to fluctuation dynamics and highlight nontrivial scattering channels other than resonant interactions that could be relevant in the emergence of dissipative and turbulent phenomena in superfluids. Published by the American Physical Society 2024

Efficient Time-Dependent Method for Strong-Field Ionization of Atoms with Smoothly Varying Radial Steps

We present an efficient numerical method to solve the time-dependent Schrödinger equation in the single-active electron picture for atoms interacting with intense optical laser fields. Our approach is based on a non-uniform radial grid with smoothly increasing steps for the electron distance from the residual ion. We study the accuracy and efficiency of the method, as well as its applicability to investigate strong-field ionization phenomena, the process of high-order harmonic generation, and the dynamics of highly excited Rydberg states.

A Modified Variable Power Angle Control for Unified Power Quality Conditioner in a Distorted Utility Source

The distorted supply voltage degrades the control performance of a unified power quality conditioner (UPQC). This problem causes incorrect calculations in the harmonic identification and reference signal generation processes. This paper proposes a modified harmonic identification of the UPQC. The reference compensating current calculation for the shunt active power filter (shunt APF) is developed using the sliding window with the Fourier analysis (SWFA) method. In addition, the variable power angle control (PAC) is applied to operate the reference signal generation of the series APF and the shunt APF of the UPQC. Under the distorted voltage and nonlinear load conditions, the proposed approach can provide accurate reference compensating signals and successfully share the load reactive power compensation between the shunt APF and the series APF. In this work, a three-phase, three-wire power system with linear and nonlinear loads was implemented. The proposed method was validated using the processor-in-the-loop technique on an eZdsp™ F28335 board and the MATLAB/Simulink program. The testing results indicated that SWFA has excellent filtering performance and enhances harmonic identification compared to the operation without any filter or with low pass filters (LPF). With the proposed approach, the percentage of total harmonic distortion of voltage and current could be maintained within the IEEE519-2022 standard, and the magnitude of the RMS voltage across the load was in the recommended range specified by ANSI C84.1-2016.

Influence of the focusing parameter on the SHG efficiency at a wavelength of 968 nm in a ZnSe polycrystal

A theoretical model for determine the optimal focusing parameter for second harmonic generation (SHG) process in a polycrystalline nonlinear medium has been constructed. Theoretical calculations were confirmed by an experiment to obtain SHG at a wavelength of 968[Formula: see text]nm in a zinc selenide polycrystal using a thulium laser.

Generation of high-energy, sub-20 fs deep-UV pulses in a twin-crystal third harmonic generation scheme.

Ultrashort deep ultraviolet (DUV) pulses serve as indispensable tools for investigating molecular dynamics on the femtosecond scale. Nonlinear frequency upconversion of near-infrared (NIR) light sources in a sequence of nonlinear crystals is a common method for their generation. However, preserving the temporal duration of the starting source encounters challenges owing to phase-matching bandwidth limitations within the harmonic generation process. Here we propose an approach for circumventing this limitation and demonstrate it for the case of generation of the third harmonic of 800 nm pulses in a two-stage scheme (second harmonic generation succeeded by sum-frequency mixing of the fundamental and second harmonic pulses). Expanding the bandwidth of the DUV pulse involves the utilization for the last mixing process of two nonlinear crystals, detuned to convert opposite sides of the spectrum. The implementation of this approach yields 20 µJ, 263 nm DUV pulses as short as 19 fs after compression. The setup is very compact and extremely stable due to the common-path scheme, which makes it very interesting for a variety of advanced ultrafast spectroscopy applications.

Entanglement and Squeezing of the Optical Field Modes in High Harmonic Generation.

Squeezed optical fields are a powerful resource for a variety of investigations in basic research and technology. However, the generation of intense squeezed light is challenging. Here, we show that intense squeezed light can be produced using strongly laser driven atoms and the so far unrelated process of high harmonic generation. We demonstrate that when the intensity of the driving field significantly depletes the ground state of the atoms, leading to dipole moment correlations, the quantum state of the driving field and the generated high harmonics are entangled and squeezed. Furthermore, we analyze how the resulting quadrature squeezing of the fundamental laser mode after the interaction can be controlled. The findings open the way for the generation of high intensity squeezed light states for a wide range of applications.

Nonlinear Photodetector Based on InSe p–n Homojunction for Improving Spatial Imaging Resolution

AbstractAn efficient nonlinear photodetector (NLPD) is demonstrated with quadratic response based on a few‐layer InSe p–n homojunction, which is beneficial from the strong second harmonic generation (SHG) process in InSe and effective harvest of photocarriers actuated by the high‐quality homojunction. The NLPD can sense light with photon energy smaller than InSe's electronic bandgap because the SHG process in InSe doubles the frequency of incident light, extending InSe's photodetection wavelength range to 1750 nm. The InSe p–n homojunction, which is electrostatically doped by two split back gates, presents a rectification ratio exceeding 106 with a dark current down to 2 pA and a high normalized responsivity of 0.534 A W−2 for the telecom‐band pulsed light at 1550 nm. The photocurrents of the SHG‐assisted photodetection have a quadratic dependence on the optical powers, making the NLPD highly sensitive to light intensity variation with improved spatial resolution. As examples, the NLPD is employed to precisely determine the localization point of a focused laser beam waist and implement spatial imaging with an improved resolution compared with the linear photodetector. These features highlight the potential of the proposed NLPD in developing advanced optical sensing and imaging systems.

Recovering coefficients in a system of semilinear Helmholtz equations from internal data

We study an inverse problem for a coupled system of semilinear Helmholtz equations where we are interested in reconstructing multiple coefficients in the system from internal data measured in applications such as thermoacoustic imaging. The system serves as a simplified model of the second harmonic generation process in a heterogeneous medium. We derive results on the uniqueness and stability of the inverse problem in the case of small boundary data based on the technique of first- and higher-order linearization. Numerical simulations are provided to illustrate the quality of reconstructions that can be expected from noisy data.

Theoretical analysis of perturbative high harmonic wave mixing from plasma surfaces

High harmonic generation modulated by a weakly perturbing laser field enables new wave mixing frequency components, thus allowing in-situ spatiotemporal measurements and wavefront control of attosecond optical pulses. However, perturbative high harmonic wave mixing from plasma surfaces has not been investigated extensively. In this study, we theoretically analyze the plasma high harmonic generation process in the relativistic regime modulated by a perturbing laser field with an arbitrary frequency. New wave mixing frequency components satisfying the conservation laws of photon energy and momentum are observed. The wave mixing component intensities adhere to a power law for the perturbating laser photon number as the perturbing laser intensity increases, thereby revealing perturbative behaviors in the nonperturbative, extremely nonlinear optical process of high harmonic generation. Detailed studies reveal the polarization selection rule and physical mechanism of high harmonic wave mixing. The modulation of the relativistic factor or mass enhancement of electrons on the plasma surface by the perturbing laser field is believed to result in high harmonic wave mixing in the relativistic regime.

Plasmonic Enhancement of Second Harmonic Generation in Weyl Semimetal TaAs

AbstractIn this work a hybrid nanoplasmonic‐Weyl Semimetal (WSM) structure is realized for the first time utilizing silver nanopatch antennas and WSM Tantalum Arsenide (TaAs). The studied hybrid WSM‐nanoplasmonic structure demonstrated a substantial, over x4.5 enhancement of the second harmonic generation (SHG) process compared to a bare TaAs film. To realize the hybrid structure while preserving TaAs properties, a scalable, non‐destructive manufacturing approach is developed that involves the fabrication of TaAs flakes from single crystalline TaAs, overgrowth of a silicon nitride overlayer, and drop‐casting of silver nanopatch antennas. The strong polarization response of both the bare flakes, along with the hybrid‐nanoplasmonic cavities demonstrates that this approach uniquely preserves the TaAs crystal structure and its optical response while providing significant enhancement of the nonlinear properties. The developed method allows leveraging the capabilities of plasmonics to control and enhance light‐matter interactions at the nanometer scale to access and engineer WSM response. This work is the first step towards high‐performance nanophotonic devices utilizing WSM topological properties.

Macroscopic effects in generation of attosecond XUV pulses via high-order frequency mixing in gases and plasma

We theoretically study the generation of attosecond XUV pulses via high-order frequency mixing (HFM) of two intense generating fields, and compare this process with the more common high-order harmonic generation (HHG) process. We calculate the macroscopic XUV signal by numerically integrating the 1D propagation equation coupled with the 3D time-dependent Schrödinger equation. We analytically find the length scales which limit the quadratic growth of the HFM macroscopic signal with propagation length. Compared to HHG these length scales are much longer for a group of HFM components, with orders defined by the frequencies of the generating fields. This results in a higher HFM macroscopic signal despite the microscopic response being lower than for HHG. In our numerical simulations in a gas target, the intensity of the HFM signal is several times higher than that for HHG, while for a plasma target the HFM generation efficiency is up to three orders of magnitude higher than for HHG. The HFM with relatively long generating pulses provides very narrow XUV lines ( δω/ω=4.6×10−4 ) with well-defined frequencies, thus allowing for a simple extension of optical frequency standards to the XUV range. Finally, we show that the group of HFM components effectively generated due to macroscopic effects provides a train of attosecond pulses such that the carrier-envelope phase of an individual attosecond pulse can be easily controlled by tuning the phase of one of the generating fields.