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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Resonance Effect in Brunel Harmonic Generation in Thin Film Organic Semiconductors

Abstract Nonlinear optical properties of organic semiconductors (OSCs) have been extensively investigated in the perturbative regime, while strong light induced high‐order processes in solid‐state OSCs are less studied. Here, below‐threshold harmonic generation is examined, both experimentally and theoretically, in two solid‐state thin film OSCs, that is, tetraphenylporphyrin and zinc tetraphenylporphyrin. Results show that the π–π* excitations of the porphyrin ring system generate the harmonic emission. The contribution of the Brunel harmonic to the 5th harmonic emission is uncovered, where the resonant 5‐photon transition ( S 0 → S 2 transition) is found to lead to an early onset of non‐perturbative behavior. A similar resonance effect is expected in Brunel harmonic generation in other organic materials.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Dynamics of harmonically-confined systems: Some rigorous results

In this paper we consider the dynamics of harmonically-confined atomic gases. We present various general results which are independent of particle statistics, interatomic interactions and dimensionality. Of particular interest is the response of the system to external perturbations which can be either static or dynamic in nature. We prove an extended Harmonic Potential Theorem which is useful in determining the damping of the centre of mass motion when the system is prepared initially in a highly nonequilibrium state. We also study the response of the gas to a dynamic external potential whose position is made to oscillate sinusoidally in a given direction. We show in this case that either the energy absorption rate or the centre of mass dynamics can serve as a probe of the optical conductivity of the system. -- Highlights: •We derive various rigorous results on the dynamics of harmonically-confined atomic gases. •We derive an extension of the Harmonic Potential Theorem. •We demonstrate the link between the energy absorption rate in a harmonically-confined system and the optical conductivity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

Vortices in a rotating two-component Bose–Einstein condensate with tunable interactions and harmonic potential

We consider a pair of coupled nonlinear Schrödinger equations modeling a rotating two-component Bose–Einstein condensate with tunable interactions and harmonic potential, with emphasis on the structure of vortex states by varying the strength of inter-component interaction, rotational frequency, and the aspect ratio of the harmonic potential. Our results show that the inter-component interaction greatly enhances the effect of rotation. For the case of isotropic harmonic potential and small inter-component interaction, the initial vortex structure remains unchanged. As the ratio of inter- to intra-component interactions increases, each component undergoes a transition from a vortex lattice (vortex line) in an isotropic (anisotropic) harmonic potential to an alternatively arranged stripe pattern, and eventually to the interwoven “serpentine” vortex sheets. Moreover, in the case of anisotropic harmonic potential the system can develop to a rotating droplet structure. -- Highlights: •Different vortex structures are obtained within the full parameter space. •Effects of system parameters on the ground state structure are discussed. •Phase transition between different vortex structures is also examined. •Present one possible way to obtain the rotating droplet structure. •Provide many possibilities to manipulate vortex in two-component BEC.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Polarization-Dependent Second Harmonic Diffraction from Resonant GaAs Metasurfaces

Resonant semiconductor metasurfaces are an emerging versatile platform for nonlinear photonics. Here, we investigate second-harmonic generation from metasurfaces consisting of two-dimensional square arrays of gallium arsenide nanocylinders as a function of the polarization of the fundamental wave. To this end, we perform nonlinear second harmonic microscopy, where the pump wavelength is tuned to the resonances of the metasurfaces. Furthermore, imaging the generated nonlinear signal in Fourier space allows us to analyze the spatial properties of the generated second harmonic. Our experiments reveal that the second harmonic is predominantly emitted into the first diffraction orders of the periodic arrangements, and that its intensity varies with the polarization angle of the fundamental wave. While this can be expected from the structure of the GaAs nonlinear tensor, the characteristics of this variation itself are found to depend on the pump wavelength. Interestingly, we show that the metasurface can reverse the polarization dependence of the second harmonic with respect to an unstructured GaAs wafer. These general observations are confirmed by numerical simulations using a simplified model for the metasurface. In conclusion, our results provide valuable input for the development of metasurface-based classical and quantum light sources based on parametric processes.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Bright high-repetition-rate source of narrowband extreme-ultraviolet harmonics beyond 22 eV

Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. In this article, we demonstrate a highly-efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harmonic focused tightly into Kr gas. In this cascaded scheme, a photon flux beyond ≈3 × 10 13 s -1 is generated at 22.3 eV, with 5 × 10 -5 conversion efficiency that surpasses similar harmonics directly driven by the fundamental by two orders-of-magnitude. The enhancement arises from both wavelength scaling of the atomic dipole and improved spatio-temporal phase matching, confirmed by simulations. Finally, spectral isolation of a single 72-meV-wide harmonic renders this bright, 50-kHz extreme-ultraviolet source a powerful tool for ultrafast photoemission, nanoscale imaging and other applications.

36 MATERIALS SCIENCE↗
DOE OSTI2017

High-harmonic generation in amorphous solids

High-harmonic generation in isolated atoms and molecules has been widely utilized in extreme ultraviolet photonics and attosecond pulse metrology. Recently, high-harmonic generation has been observed in solids, which could lead to important applications such as all-optical methods to image valance charge density and reconstruct electronic band structures, as well as compact extreme ultraviolet light sources. So far these studies are confined to crystalline solids; therefore, decoupling the respective roles of long-range periodicity and high density has been challenging. Here we report the observation of high-harmonic generation from amorphous fused silica. We also decouple the role of long-range periodicity by comparing harmonics generated from fused silica and crystalline quartz, which contain the same atomic constituents but differ in long-range periodicity. These results advance current understanding of the strong-field processes leading to high-harmonic generation in solids with implications for the development of robust and compact extreme ultraviolet light sources.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ultrafast high-harmonic spectroscopy of solids

High-harmonic spectroscopy, an ultrafast all-optical technique initially conceptualized in atomic and molecular systems, has now emerged as a powerful platform for studying the structure and dynamics of condensed matter. Unlike that in the gas phase, solid-state high-harmonic generation relies on the fundamental response from high atomic density and periodicity, leading to interband transitions and coherent driving of electrons and holes in their respective bands. These mechanisms make high-harmonic spectroscopy particularly sensitive to the electronic band structure, topological properties and many-body correlations in condensed media. An advantage of high-harmonic spectroscopy over other spectroscopic methods is its ability to probe ultrafast phenomena, capturing femto- to attosecond dynamics of multi-band and strongly correlated electron interactions in solids. Furthermore, in this Review, we discuss the latest experimental and theoretical advances in ultrafast high-harmonic spectroscopy of solids and provide perspectives for future research in this field.

High-harmonic generation↗
DOE OSTI2026

Efficiency-optimized relativistic plasma harmonics for extreme fields

Bright harmonic radiation from relativistically oscillating laser plasmas offers a direct route for generating extreme electromagnetic fields. Theory predicts that under optimized conditions, the plasma medium can support strong spatiotemporal compression of laser energy in a coherent harmonic focus (CHF), delivering intensity boosts many orders of magnitude greater than the incident driving laser pulse. Although diffraction-limited performance (spatial compression) and attosecond phase locking (temporal compression) have been demonstrated experimentally, efficient coupling of relativistically intense laser pulse energy into the emitted harmonic cone has not been realized so far. Here we demonstrate that this highly nonlinear interaction can be tailored to deliver the maximum conversion efficiencies predicted from simulations. By fine-tuning the temporal profile of the driving laser on sub-picosecond (<10 −12 s) timescales, energies >9 mJ between the 12th and 47th harmonics are observed. These results are in agreement with the theoretically expected efficiency dependence on harmonic order, verifying that optimal conditions have been achieved in the generation process. This is the important final element required to achieve the expected intensity boosts from a CHF in experiments. Although obtaining spatiotemporal compression and optimal efficiency simultaneously remains challenging, the path to realizing extreme optical field strengths approaching the critical field of quantum electrodynamics (the Schwinger limit at >10 16 V cm −1 or >10 29 W cm −2 ) is now open, permitting all-optical studies of the quantum vacuum and new frontiers for intense attosecond science.

High-harmonic generation↗
DOE OSTI2016

Unravelling the dynamical origin of below- and near-threshold harmonic generation of H 2 + in an intense NIR laser field

Recently, the study of near- and below- threshold regime harmonics as a potential source of intense coherent vacuum-ultraviolet radiation has received considerable attention. However, the dynamical origin of these lower harmonics, particularly for the molecular systems, is less understood and largely unexplored. Here we perform the first fully ab initio and high precision 3D quantum study of the below- and near-threshold harmonic generation of H 2 + molecules in an intense 800-nm near-infrared (NIR) laser field. Furthermore, combining with a synchrosqueezing transform of the quantum time-frequency spectrum and an extended semiclassical analysis, we explore in-depth the roles of various quantum trajectories, including short- and long trajectories, multiphoton trajectories, resonance-enhanced trajectories, and multiple rescattering trajectories of the below- and near- threshold harmonic generation processes. Our results shed new light on the dynamical origin of the below- and near-threshold harmonic generation and various quantum trajectories for diatomic molecules for the first time.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2014

Study on higher harmonic suppression using edge filter and polished Si wafer

Higher harmonics contamination is a severe problem in synchrotron beamlines where grating monochromators are used. In these beamlines, absorption edge filters and critical angle mirrors are used to suppress the harmonic contaminations. In the present study, carried out using Indus-1 reflectivity beamline, a harmonic suppression characteristic of Al edge filter and polished silicon wafer are determined. It is found that the Al filter suppresses higher harmonics in 2–7% range whereas the polished silicon wafer can suppress the higher harmonics below 1%. The results of comparative study are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Resonant second harmonic generation in a gallium nitride two-dimensional photonic crystal on silicon

We demonstrate second harmonic generation in a gallium nitride photonic crystal cavity embedded in a two-dimensional free-standing photonic crystal platform on silicon. The photonic crystal nanocavity is optically pumped with a continuous-wave laser at telecom wavelengths in the transparency window of the nitride material. The harmonic generation is evidenced by the spectral range of the emitted signal, the quadratic power dependence vs. input power, and the spectral dependence of second harmonic signal. The harmonic emission pattern is correlated to the harmonic polarization generated by the second-order nonlinear susceptibilities χ{sub zxx}{sup (2)}, χ{sub zyy}{sup (2)} and the electric fields of the fundamental cavity mode.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Harmonic generation by circularly polarized laser beams propagating in plasma

An analytical theory is developed for studying the phenomenon of generation of harmonics by the propagation of an obliquely incident, circularly polarized laser beam in homogeneous, underdense plasma. The amplitudes of second and third harmonic radiation as well as detuning distance have been obtained and their variation with the angle of incidence is analyzed. The amplitude of harmonic radiation increases with the angle of incidence while the detuning distance decreases, for a given plasma electron density. It is observed that the generated second and third harmonic radiation is linearly and elliptically polarized, respectively. The harmonic radiation vanishes at normal incidence of the circularly polarized laser beam.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Efficient second- and third-harmonic radiation generation from relativistic laser-plasma interactions

We propose an idea to enhance the efficiency of second- and third-harmonic generation by considering the amplitude-modulation of the fundamental laser pulse. A short-pulse laser of finite spot size is modeled as amplitude modulated in time. Amplitude-modulation of fundamental laser contributes in quiver velocity of the plasma electrons and produces the strong plasma-density perturbations, thereby increase in current density at second- and third-harmonic frequency. In a result, the conversion efficiency of harmonic generation increases significantly. Power conversion efficiency of harmonic generation process is the increasing function of the amplitude-modulation parameter of the fundamental laser beam. Harmonic power generated by an amplitude modulated laser is many folds higher than the power obtained in an ordinary case.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Raman parametric excitation effect upon the third harmonic generation by a metallic nanoparticle lattice

This work is a theoretical study on third harmonic generation in the nonlinear propagation of an intense laser pulse through a periodic three-dimensional lattice of nanoparticles. Using a perturbative method, the nonlinear equations that describe the laser–nanoparticle interaction in the weakly relativistic regime are derived. Additionally, the nonlinear dispersion relation and the amplitude of the third harmonic are obtained. Finally, the effects of the nanoparticle radius and separation length, the distribution of the nanoparticle electron density, and the laser frequency upon the third harmonic efficiency are investigated. In addition to the expected resonance that occurs when the third harmonic resonates with the plasmon wave, another resonance appears when the nonlinear interaction of the fundamental mode with the third harmonic excites a longitudinal collective plasmon wave via the parametric Raman mechanism.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Second-harmonic generation in shear wave beams with different polarizations

A coupled pair of nonlinear parabolic equations was derived by Zabolotskaya [1] that model the transverse components of the particle motion in a collimated shear wave beam propagating in an isotropic elastic solid. Like the KZK equation, the parabolic equation for shear wave beams accounts consistently for the leading order effects of diffraction, viscosity and nonlinearity. The nonlinearity includes a cubic nonlinear term that is equivalent to that present in plane shear waves, as well as a quadratic nonlinear term that is unique to diffracting beams. The work by Wochner et al. [2] considered shear wave beams with translational polarizations (linear, circular and elliptical), wherein second-order nonlinear effects vanish and the leading order nonlinear effect is third-harmonic generation by the cubic nonlinearity. The purpose of the current work is to investigate the quadratic nonlinear term present in the parabolic equation for shear wave beams by considering second-harmonic generation in Gaussian beams as a second-order nonlinear effect using standard perturbation theory. In order for second-order nonlinear effects to be present, a broader class of source polarizations must be considered that includes not only the familiar translational polarizations, but also polarizations accounting for stretching, shearing and rotation of the source plane. It is found that the polarization of the second harmonic generated by the quadratic nonlinearity is not necessarily the same as the polarization of the source-frequency beam, and we are able to derive a general analytic solution for second-harmonic generation from a Gaussian source condition that gives explicitly the relationship between the polarization of the source-frequency beam and the polarization of the second harmonic.

42 ENGINEERING↗
DOE OSTI2015

Harmonic growth of spherical Rayleigh-Taylor instability in weakly nonlinear regime

Harmonic growth in classical Rayleigh-Taylor instability (RTI) on a spherical interface is analytically investigated using the method of the parameter expansion up to the third order. Our results show that the amplitudes of the first four harmonics will recover those in planar RTI as the interface radius tends to infinity compared against the initial perturbation wavelength. The initial radius dramatically influences the harmonic development. The appearance of the second-order feedback to the initial unperturbed interface (i.e., the zeroth harmonic) makes the interface move towards the spherical center. For these four harmonics, the smaller the initial radius is, the faster they grow.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2015

Design and optimization of a harmonic probe with step cross section in multifrequency atomic force microscopy

In multifrequency atomic force microscopy (AFM), probe’s characteristic of assigning resonance frequencies to integer harmonics results in a remarkable improvement of detection sensitivity at specific harmonic components. The selection criterion of harmonic order is based on its amplitude’s sensitivity on material properties, e.g., elasticity. Previous studies on designing harmonic probe are unable to provide a large design capability along with maintaining the structural integrity. Herein, we propose a harmonic probe with step cross section, in which it has variable width in top and bottom steps, while the middle step in cross section is kept constant. Higher order resonance frequencies are tailored to be integer times of fundamental resonance frequency. The probe design is implemented within a structural optimization framework. The optimally designed probe is micromachined using focused ion beam milling technique, and then measured with an AFM. The measurement results agree well with our resonance frequency assignment requirement.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Third harmonic generation in air ambient and laser ablated carbon plasma

We report the third harmonic generation of a nanosecond laser pulse (1.06 μm) in air ambient and in the presence of nanoparticles from laser ablated carbon plasma. Significant decrease in the threshold of third harmonic generation and multi-fold increment in the intensity of generated third harmonic is observed in presence of carbon plasma. The third harmonic in air is due to the quasi-resonant four photon process involving vibrationally excited states of molecular ion of nitrogen due to electron impact ionization and laser pulse. Following optical emission spectroscopic observations we conclude that the presence of C{sub 2} and CN in the ablated plume play a vital role in the observed third harmonic signals.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗