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At least 613 records · Page 34

Limitations and improvements for harmonic generation measurements

A typical acoustic harmonic generation measurement comes with certain limitations. Firstly, the use of the plane wave-based analysis used to extract the nonlinear parameter, β, ignores the effects of diffraction, attenuation and receiver averaging which are common to most experiments, and may therefore limit the accuracy of a measurement. Secondly, the method usually requires data obtained from a through-transmission type setup, which may not be practical in a field measurement scenario where access to the component is limited. Thirdly, the technique lacks a means of pinpointing areas of damage in a component, as the measured nonlinearity represents an average over the length of signal propagation. Here we describe a three-dimensional model of harmonic generation in a sound beam, which is intended to provide a more realistic representation of a typical experiment. The presence of a reflecting boundary is then incorporated into the model to assess the feasibility of performing single-sided measurements. Experimental validation is provided where possible. Finally, a focusing acoustic source is modelled to provide a theoretical indication of the afforded advantages when the nonlinearity is localized.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Second harmonic generation from direct band gap quantum dots pumped by femtosecond laser pulses

We report on nonlinear optical experiments performed on Cu{sub 2}S quantum dots (QDs) pumped by femtosecond laser pulses. We conduct a theoretical simulation and experiments to determine their second harmonic generation characteristics. Furthermore, we demonstrate that the QDs have a second harmonic generation conversion efficiency of up to 76%. Our studies suggest that these Cu{sub 2}S QDs can be used for solar cells, bioimaging, biosensing, and electric detection.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Advanced properties of extended plasmas for efficient high-order harmonic generation

We demonstrate the advanced properties of extended plasma plumes (5 mm) for efficient harmonic generation of laser radiation compared with the short lengths of plasmas (∼0.3–0.5 mm) used in previous studies. The harmonic conversion efficiency quadratically increased with the growth of plasma length. The studies of this process along the whole extreme ultraviolet range using the long plasma jets produced on various metal surfaces, particularly including the resonance-enhanced laser frequency conversion and two-color pump, are presented. Such plasmas could be used for the quasi-phase matching experiments by proper modulation of the spatial characteristics of extended ablating area and formation of separated plasma jets.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Current collapse imaging of Schottky gate AlGaN/GaN high electron mobility transistors by electric field-induced optical second-harmonic generation measurement

Two-dimensional current collapse imaging of a Schottky gate AlGaN/GaN high electron mobility transistor device was achieved by optical electric field-induced second-harmonic generation (EFISHG) measurements. EFISHG measurements can detect the electric field produced by carriers trapped in the on-state of the device, which leads to current collapse. Immediately after (e.g., 1, 100, or 800 μs) the completion of drain-stress voltage (200 V) in the off-state, the second-harmonic (SH) signals appeared within 2 μm from the gate edge on the drain electrode. The SH signal intensity became weak with time, which suggests that the trapped carriers are emitted from the trap sites. The SH signal location supports the well-known virtual gate model for current collapse.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Increased efficiency of ion acceleration by using femtosecond laser pulses at higher harmonic frequency

The influence of laser frequency on laser-driven ion acceleration is investigated by means of two-dimensional particle-in-cell simulations. When ultrashort intense laser pulse at higher harmonic frequency irradiates a thin solid foil, the target may become re lativistically transparent for significantly lower laser pulse intensity compared with irradiation at fundamental laser frequency. The relativistically induced transparency results in an enhanced heating of hot electrons as well as increased maximum energies of accelerated ions and their numbers. Our simulation results have shown the increase in maximum proton energy and increase in the number of high-energy protons by a factor of 2 after the interaction of an ultrashort laser pulse of maximum intensity 7 × 10{sup 21 }W/cm{sup 2} with a fully ionized plastic foil of realistic density and of optimal thickness between 100 nm and 200 nm when switching from the fundamental frequency to the third harmonics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Franck-Condon factors perturbed by damped harmonic oscillators: Solvent enhanced X {sup 1}A{sub g} ↔ A{sup 1}B{sub 1u} absorption and fluorescence spectra of perylene

Damped harmonic oscillators are utilized to calculate Franck-Condon factors within displaced harmonic oscillator approximation. This is practically done by scaling unperturbed Hessian matrix that represents local modes of force constants for molecule in gaseous phase, and then by diagonalizing perturbed Hessian matrix it results in direct modification of Huang–Rhys factors which represent normal modes of solute molecule perturbed by solvent environment. Scaling parameters are empirically introduced for simulating absorption and fluorescence spectra of an isolated solute molecule in solution. The present method is especially useful for simulating vibronic spectra of polycyclic aromatic hydrocarbon molecules in which hydrogen atom vibrations in solution can be scaled equally, namely the same scaling factor being applied to all hydrogen atoms in polycyclic aromatic hydrocarbons. The present method is demonstrated in simulating solvent enhanced X {sup 1}A{sub g} ↔ A{sup 1}B{sub 1u} absorption and fluorescence spectra of perylene (medium-sized polycyclic aromatic hydrocarbon) in benzene solution. It is found that one of six active normal modes v{sub 10} is actually responsible to the solvent enhancement of spectra observed in experiment. Simulations from all functionals (TD) B3LYP, (TD) B3LYP35, (TD) B3LYP50, and (TD) B3LYP100 draw the same conclusion. Hence, the present method is able to adequately reproduce experimental absorption and fluorescence spectra in both gas and solution phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Higher harmonics generation in relativistic electron beam with virtual cathode

The study of the microwave generation regimes with intense higher harmonics taking place in a high-power vircator consisting of a relativistic electron beam with a virtual cathode has been made. The characteristics of these regimes, in particular, the typical spectra and their variations with the change of the system parameters (beam current, the induction of external magnetic field) as well as physical processes occurring in the system have been analyzed by means of 3D electromagnetic simulation. It has been shown that the system under study demonstrates the tendency to the sufficient growth of the amplitudes of higher harmonics in the spectrum of current oscillations in the VC region with the increase of beam current. The obtained results allow us to consider virtual cathode oscillators as promising high power mmw-to-THz sources.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

B-spline algebraic diagrammatic construction: Application to photoionization cross-sections and high-order harmonic generation

We present the first implementation of the ab initio many-body Green's function method, algebraic diagrammatic construction (ADC), in the B-spline single-electron basis. B-spline versions of the first order [ADC(1)] and second order [ADC(2)] schemes for the polarization propagator are developed and applied to the ab initio calculation of static (photoionization cross-sections) and dynamic (high-order harmonic generation spectra) quantities. We show that the cross-section features that pose a challenge for the Gaussian basis calculations, such as Cooper minima and high-energy tails, are found to be reproduced by the B-spline ADC in a very good agreement with the experiment. We also present the first dynamic B-spline ADC results, showing that the effect of the Cooper minimum on the high-order harmonic generation spectrum of Ar is correctly predicted by the time-dependent ADC calculation in the B-spline basis. The present development paves the way for the application of the B-spline ADC to both energy- and time-resolved theoretical studies of many-electron phenomena in atoms, molecules, and clusters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Monitoring microstructural evolution in irradiated steel with second harmonic generation

Material damage in structural components is driven by microstructural evolution that occurs at low length scales and begins early in component life. In metals, these microstructural features are known to cause measurable changes in the acoustic nonlinearity parameter. Physically, the interaction of a monochromatic ultrasonic wave with microstructural features such as dislocations, precipitates, and vacancies, generates a second harmonic wave that is proportional to the acoustic nonlinearity parameter. These nonlinear ultrasonic techniques thus have the capability to evaluate initial material damage, particularly before crack initiation and propagation occur. This paper discusses how the nonlinear ultrasonic technique of second harmonic generation can be used as a nondestructive evaluation tool to monitor microstructural changes in steel, focusing on characterizing neutron radiation embrittlement in nuclear reactor pressure vessel steels. Current experimental evidence and analytical models linking microstructural evolution with changes in the acoustic nonlinearity parameter are summarized.

36 MATERIALS SCIENCE↗

Continuous third harmonic generation in a terahertz driven modulated nanowire

We consider the possibility of observing continuous third-harmonic generation using a strongly driven, single-band one-dimensional metal. In the absence of scattering, the quantum efficiency of frequency tripling for such a system can be as high as 93%. Combining the Floquet quasi-energy spectrum with the Keldysh Green's function technique, we derive a semiclassical master equation for a one-dimensional band of strongly and rapidly driven electrons in the presence of weak scattering by phonons. The power absorbed from the driving field is continuously dissipated by phonon modes, leading to a quasi-equilibrium in the electron distribution. We use the Kronig-Penney model with varying effective mass to establish the growth parameters of an InAs/InP nanowire near optimal for third harmonic generation at terahertz frequency range.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrashort pulse chirp measurement via transverse second-harmonic generation in strontium barium niobate crystal

Pulse compression in dispersive strontium barium niobate crystal with a random size and distribution of the anti-parallel orientated nonlinear domains is observed via transverse second harmonic generation. The dependence of the transverse width of the second harmonic trace along the propagation direction allows for the determination of the initial chirp and duration of pulses in the femtosecond regime. This technique permits a real-time analysis of the pulse evolution and facilitates fast in-situ correction of pulse chirp acquired in the propagation through an optical system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

On square-integrability of solutions of the stationary Schrödinger equation for the quantum harmonic oscillator in two dimensional constant curvature spaces

In this work, one provides a justification of the condition that is usually imposed on the parameters of the hypergeometric equation, related to the solutions of the stationary Schrödinger equation for the harmonic oscillator in two-dimensional constant curvature spaces, in order to determine the solutions which are square-integrable. One proves that in case of negative curvature, it is a necessary condition of square integrability and in case of positive curvature, a necessary condition of regularity. The proof is based on the analytic continuation formulas for the hypergeometric function. It is observed also that the same is true in case of a slightly more general potential than the one for harmonic oscillator.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Direct optical detection of current induced spin accumulation in metals by magnetization-induced second harmonic generation

Strong spin-orbit coupling in non-magnetic heavy metals has been shown to lead to large spin currents flowing transverse to a charge current in such a metal wire. This in turn leads to the buildup of a net spin accumulation at the lateral surfaces of the wire. Spin-orbit torque effects enable the use of the accumulated spins to exert useful magnetic torques on adjacent magnetic layers in spintronic devices. We report the direct detection of spin accumulation at the free surface of nonmagnetic metal films using magnetization-induced optical surface second harmonic generation. The technique is applied to probe the current induced surface spin accumulation in various heavy metals such as Pt, β-Ta, and Au with high sensitivity. The sensitivity of the technique enables us to measure the time dynamics on a sub-ns time scale of the spin accumulation arising from a short current pulse. The ability of optical surface second harmonic generation to probe interfaces suggests that this technique will also be useful for studying the dynamics of spin accumulation and transport across interfaces between non-magnetic and ferromagnetic materials, where spin-orbit torque effects are of considerable interest.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

HELIOS—A laboratory based on high-order harmonic generation of extreme ultraviolet photons for time-resolved spectroscopy

In this paper, we present the HELIOS (High Energy Laser Induced Overtone Source) laboratory, an in-house high-order harmonic generation facility which generates extreme ultraviolet (XUV) photon pulses in the range of 15-70 eV with monochromatized XUV pulse lengths below 35 fs. HELIOS is a source for time-resolved pump-probe/two-color spectroscopy in the sub-50 fs range, which can be operated at 5 kHz or 10 kHz. An optical parametric amplifier is available for pump-probe experiments with wavelengths ranging from 240 nm to 20 000 nm. The produced XUV radiation is monochromatized by a grating in the so-called off-plane mount. Together with overall design parameters, first monochromatized spectra are shown with an intensity of 2 ⋅ 10{sup 10} photons/s (at 5 kHz) in the 29th harmonic, after the monochromator. The XUV pulse duration is measured to be <25 fs after monochromatization.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Nanostructure induced changes in lifetime and enhanced second-harmonic response of organic-plasmonic hybrids

In this letter we show that the optical response of organic nanofibers, grown from functionalized para-quaterphenylene molecules, can be controlled by forming organic-plasmonic hybrid systems. The interaction between nanofibers and supporting regular arrays of nanostructures leads to a strongly enhanced second harmonic response. At the same time, the fluorescence lifetime of the nanofibers is reduced from 0.32 ns for unstructured gold films to 0.22 ns for gold nanosquare arrays, demonstrating efficient organic–plasmonic interaction. To study the origin of these effects, we applied two-photon laser scanning microscopy and fluorescence lifetime imaging microscopy. These findings provide an effective approach for plasmon-enhanced second-harmonic generation at the nanoscale, which is attractive for nanophotonic circuitry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Surface and interface states of Bi{sub 2}Se{sub 3} thin films investigated by optical second-harmonic generation and terahertz emission

We investigate the surface and interface states of Bi{sub 2}Se{sub 3} thin films by using the second-harmonic generation technique. Distinct from the surface of bulk crystals, the film surface and interface show the isotropic azimuth dependence of second-harmonic intensity, which is attributed to the formation of randomly oriented domains on the in-plane. Based on the nonlinear susceptibility deduced from the model fitting, we determine that the surface band bending induced in a space charge region occurs more strongly at the film interface facing the Al{sub 2}O{sub 3} substrate or capping layer compared with the interface facing the air. We demonstrate that distinct behavior of the terahertz electric field emitted from the samples can provide further information about the surface electronic state of Bi{sub 2}Se{sub 3}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Conversion of the optical orbital angular momentum in a plasmon-assisted second-harmonic generation

We experimentally demonstrate the plasmon-assisted second-harmonic generation of an optical orbital angular momentum (OAM) beam. Because of the shape resonance, the plasmons in a periodic array of rectangular metal holes greatly enhance the nonlinear optical conversion of an OAM state. The OAM conservation (i.e., 2l{sub 1} = l{sub 2} with l{sub 1} and l{sub 2} being the OAM numbers of the fundamental and second-harmonic waves, respectively) holds well under our experimental configuration. Our results provide a potential way to realize nonlinear optical manipulation of an OAM mode in a nano-photonic device.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Dynamic embedding of effective harmonic normal mode vibrations in all-atomistic energy gap fluctuations: Case study of light harvesting 2 complex

Environmental effects in excitation energy transfer have mostly been modeled by baths of harmonic oscillators, but to what extent such modeling provides a reliable description of actual interactions between molecular systems and environments remains an open issue. Here, we address this issue by investigating fluctuations in the excitation energies of the light harvesting 2 complex using a realistic all-atomistic simulation of the potential energy surface. Our analyses reveal that molecular motions exhibit significant anharmonic features, even for underdamped intramolecular vibrations. In particular, we find that the anharmonicity contributes to the broadening of spectral densities and substantial overlaps between neighboring peaks, which complicates the meaning of mode frequencies constituting a bath model. Thus, we develop a strategy to construct a minimally underdamped harmonic bath that has a clear connection to all-atomistic dynamics by utilizing actual normal modes of molecules but optimizing their frequencies such that the resulting bath model can best reproduce the all-atomistic simulation results. By subtracting the underdamped contribution from the entire fluctuations, we also show that identifying a residual spectral density representing all other contributions with overdamped behavior is possible. We find that this can be fitted well with a well-established analytic form of a spectral density function or, alternatively, modeled as explicit time dependent fluctuations with muti-exponential or power law type correlation functions. We provide an assessment and the implications of these possibilities. The approach presented here can also serve as a general strategy to construct a simplified bath model that can effectively represent the underlying all-atomistic bath dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗