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DOE OSTI2011

First-principles prediction of optical second-order harmonic generation in the endohedral N-C{sub 60} compound

Non-linear-optical properties in C{sub 60} have attracted enormous attention for over two decades. The endohedral complex N-C{sub 60}, with its remarkable thermal stability and spin-quartet ground state, is a candidate for future room-temperature quantum computing, but there has been no investigation of its non-linear-optical properties. Here, a first-principles calculation shows that N-C{sub 60} is a promising material for nanoscale and ultrafast modulations. Excitation by a pump laser pulse of the nitrogen-atom vibration inside the C{sub 60} cage transiently breaks inversion symmetry and can enable second-harmonic generation (SHG) from a probe pulse. Unlike the SHG observed in C{sub 60} thin films, this harmonic signal is switched on and off periodically every 345 fs. For an fcc crystal of N-C{sub 60}, the second-order susceptibility {chi}{sup (2)} is on the order of 10{sup -8} esu, similar to commercially used nonlinear materials.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2011

Quantum path control in harmonic generation by temporal shaping of few-optical-cycle pulses in ionizing media

Temporal reshaping of the electric field of few-optical-cycle pulses in a low-density ionizing gas has been used to achieve control of the electron trajectories in the process of high-order harmonic generation. As a result of such a quantum path control mechanism, isolated or multiple attosecond pulses have been produced, depending on the carrier-envelope phase of the driving field. In particular, complete spectral tunability of the harmonic peaks over the whole spectral range has been demonstrated. Experimental results have been interpreted using a nonadiabatic three-dimensional propagation model and a nonadiabatic stationary phase model.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2011

High-order-harmonic generation in gas with a flat-top laser beam

We present experimental and numerical results on high-order-harmonic generation with a flat-top laser beam. We show that a simple binary tunable phase plate, made of two concentric glass plates, can produce a flat-top profile at the focus of a Gaussian infrared beam. Both experiments and numerical calculations show that there is a scaling law between the harmonic generation efficiency and the increase of the generation volume.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2017

High-order-harmonic generation of vibrating H 2 + and D 2 +

In this work, we study the isotope effect on high-order-harmonic generation (HHG) of vibrating H 2 + and D 2 + molecular ions aligned parallel to the polarization of the laser field. The time-dependent Schrödinger equation is solved accurately and efficiently by the time-dependent generalized pseudospectral and Fourier grid methods in three spatial coordinates, one of them being the internuclear separation and the other two describing the electronic motion. The laser pulses have a carrier wavelength of 800 nm and duration of 10 or 16 optical cycles. The peak intensities used in the calculations are 2×10 14 and 3×10 14 W/cm 2 . The effect of nuclear vibration is visible in both H 2 + and D 2 + but more pronounced in the lighter H 2 + molecule. Striking differences from the fixed nuclei case are a total disappearance of the traditional plateau in the HHG spectrum at the higher intensity and significant redshift of the harmonic peaks in the central part of the spectrum. These phenomena are explained based on the analysis of the dynamics of the nuclear vibrational wave packet.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2017

High-order-harmonic generation by Laguerre-Gaussian laser modes: Control of the spectra by manipulating the spatial medium distribution

In this work, we study high-order-harmonic generation (HHG) by the incident laser beam in the Laguerre-Gaussian mode with a nonzero topological charge. We find that the harmonic signal in the central spot on the beam axis does not always vanish and depends on the distribution of the medium in the focal region of the incident laser beam. The HHG spectra on the beam axis can be controlled by changing the spatial medium distribution. General theoretical results are confirmed by calculations of HHG in the medium of argon atoms, with the single-atom response obtained by means of the time-dependent density functional theory.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2018

Wavelength and intensity dependence of recollision-enhanced multielectron effects in high-order harmonic generation

Using a model molecular system (A 2 ) with two active electrons restricted to one dimension, we examine high-order harmonic generation (HHG) enhanced by rescattering. Our results show that even at intensities well below the single ionization saturation, harmonics generated from the cation (A 2 + ) can be significantly enhanced due to the rescattering of the electron that is initially ionized. This two-electron effect is manifested by the appearance of a secondary plateau and cutoff in the HHG spectrum, extending beyond the predicted cutoff in the single active electron approximation. We use our molecular model to investigate the wavelength dependence of rescattering enhanced HHG, which was first reported in a model atomic system [I. Tikhomirov, T. Sato, and K. L. Ishikawa, Phys. Rev. Lett. 118, 203202 (2017)]. Finally, we demonstrate that the HHG yield in the secondary cutoff is highly sensitive to the available electron rescattering energies as indicated by a dramatic scaling with respect to driving wavelength.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2024

Wavelength scaling and multicolor operation of a plasma-driven attosecond x-ray source via harmonic generation

The generation of high-power coherent soft x-ray pulses of sub-100 as duration and 10 nm wavelength using beams from a GeV energy plasma wakefield accelerator has been recently investigated in Emma []. As a future upgrade to this concept, this contribution investigates scaling to shorter x-ray wavelengths by cascading undulators tuned to higher harmonics of the fundamental. We present two simulation studies for plasma-driven attosecond harmonic generation schemes with final photon wavelengths of 2 and 0.40 nm. We demonstrate in these schemes that using undulators with retuned fundamental frequencies can produce GW-scale pulses of sub-nm radiation with tens of attosecond-scale pulse lengths, an order of magnitude shorter than current state-of-the-art attosecond x-ray free electron lasers (XFELs). This multipulse multicolor operation will be broadly applicable to attosecond pump-probe experiments. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗

DOE OSTI2020

Smooth periodic gauge satisfying crystal symmetry and periodicity to study high-harmonic generation in solids

Intense lasers can easily drive nonadiabatic transitions of excited electron wave packets across the Brillouin zones, thus transition dipole moments (TDM) between energy bands of solids should be continuous, satisfying crystal symmetry, and periodic at zone boundaries. While current ab initio algorithms are powerful in calculating band structures of solids, they all introduced random phases into the eigenfunctions at each crystal momentum k. In this work, we show how to choose a “smooth-periodic” gauge where TDMs can be smooth versus k, preserving crystal symmetry, as well as maintaining periodic at boundaries. The symmetry properties of TDMs with respect to k ensure the absence of even-order harmonics from MgO with inversion symmetry, while the TDM in the “smooth-periodic” gauge for broken-symmetry ZnO is responsible for even harmonics that were underestimated in previous simulations. These results reveal the importance of correctly treating the complex TDMs that satisfy crystal symmetry and continuous across zone boundaries in nonlinear laser-solid interactions, which has been elusive in most theories so far.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Implications of second harmonic generation for hidden order in Sr 2 CuO 2 Cl 2

Sr 2 CuO 2 Cl 2 (SCOC) is a model undoped cuprate with I4/mmm crystallographic symmetry, and a simple magnetic space group CAmca with associated magnetic point group mmm1'. However, recent second harmonic spectroscopy in the antiferromagnetic phase has challenged this picture, suggesting instead a magnetic point group 4/mm'm' that coexists with the antiferromagnetism and breaks the two orthogonal mirror planes containing the tetragonal c axis. Here, we analyze the symmetry of SCOC in light of the second harmonic results, and discuss possible ground states that are consistent with the data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Correlations between azimuthal anisotropy Fourier harmonics in PbPb collisions at sNN =2.76 TeV in the HYDJET++ model and in the multiphase transport model

Correlations between azimuthal anisotropy Fourier harmonics vn (n=2,3,4) are studied using the events from PbPb collisions at sNN=2.76 TeV generated by the HYDJET++ and multiphase transport (AMPT) models, and compared to the corresponding experimental results obtained by the ATLAS Collaboration. The Fourier harmonics vn are measured over a wide centrality range using the two-particle azimuthal correlation method. The slopes of the v2-v3 correlation from both models are in a good agreement with the ATLAS data. The HYDJET++ model predicts a stronger slope for the v2-v4 and v3-v4 correlations than the ones experimentally measured, while the results from the AMPT model are in a rather good agreement with the experimental results. In contrast to the HYDJET++ predictions, the AMPT model predicts a boomeranglike shape in the structure of the correlations as found in the experimental data. © 2020 American Physical Society.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2023

Quantum-Path-Resolved Attosecond High-Harmonic Spectroscopy

Strong-field ionization of molecules releases electrons which can be accelerated and driven back to recombine with their parent ion, emitting high-order harmonics. This ionization also initiates attosecond electronic and vibrational dynamics in the ion, evolving during the electron travel in the continuum. Revealing this subcycle dynamics from the emitted radiation usually requires advanced theoretical modeling. Here we show that this can be avoided by resolving the emission from two families of electronic quantum paths in the generation process. The corresponding electrons have the same kinetic energy, and thus the same structural sensitivity, but differ by the travel time between ionization and recombination-the pump-probe delay in this attosecond self-probing scheme. We measure the harmonic amplitude and phase in aligned CO 2 and N 2 molecules and observe a strong influence of laser-induced dynamics on two characteristic spectroscopic features: a shape resonance and multichannel interference. This quantum-path-resolved spectroscopy thus opens wide prospects for the investigation of ultrafast ionic dynamics, such as charge migration.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2022

In-Situ Nanoscale Focusing of Extreme Ultraviolet Solid-State High Harmonics

Extreme ultraviolet light delivering radiation with a wavelength shorter than approximately 100 nm is now available from solid-state sources. However, despite exceptional progress, efficient focusing of extreme ultraviolet photons to their ultimate diffraction limit remains a formidable challenge because of the precision of the focusing by curved, optical surfaces. Here we integrate coherent short-wavelength high-order harmonics from a MgO crystal, with a high-numerical-aperture, nanostructured, focusing element etched onto the surface of the crystal itself. We focus extreme ultraviolet light, seventh harmonic of an 800-nm laser, with a zone plate of numerical aperture 0.35, down to a waist radius of 150 nm, with 18% focusing efficiency. The estimated intensity approaches 10 7 W/cm 2 . Future developments may demonstrate nanoscale laser ablation and miniaturization of extreme ultraviolet coherent sources on a chip.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2013

Polarization-resolved second-harmonic generation microscopy as a method to visualize protein-crystal domains

Polarization-resolved second-harmonic generation microscopy is applied to the identification of multiple crystalline domains within protein-crystal samples. Polarization-resolved second-harmonic generation (PR-SHG) microscopy is described and applied to identify the presence of multiple crystallographic domains within protein-crystal conglomerates, which was confirmed by synchrotron X-ray diffraction. Principal component analysis (PCA) of PR-SHG images resulted in principal component 2 (PC2) images with areas of contrasting negative and positive values for conglomerated crystals and PC2 images exhibiting uniformly positive or uniformly negative values for single crystals. Qualitative assessment of PC2 images allowed the identification of domains of different internal ordering within protein-crystal samples as well as differentiation between multi-domain conglomerated crystals and single crystals. PR-SHG assessments of crystalline domains were in good agreement with spatially resolved synchrotron X-ray diffraction measurements. These results have implications for improving the productive throughput of protein structure determination through early identification of multi-domain crystals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Low Space Harmonic Content Windings (LSHWs) Applied to Improve the Pareto Front in Design Optimization of Electric Machines

In design optimization of high performance electric machines where the power density is increasingly a key metric, it is often desirable to maximize the average torque output within a given volume. However, if a smooth output is also required, the torque ripple may become a hurdle as it tends to increase with the average torque for conventional windings. A direct benefit of low space harmonic content windings (LSHWs), featuring the suppression or elimination of targeted non-working orders in the winding magnetomotive force (MMF), is the torque ripple reduction. This paper provides a detailed analysis of torque ripple pairs and the space-time harmonic order mapping, with concise results that applies to both distributed windings and fractionalslot concentrated windings (FSCWs) of any slot/pole combination. Metamodel-based optimizations are performed to compare two LSHWs with a conventional winding. Improved Pareto fronts are validated, which confirms higher torque producing capabilities at various torque ripple thresholds for LSHWs.

33 ADVANCED PROPULSION SYSTEMS↗

DOE OSTI2022

A Single-Stage Multilevel AC-DC Bidirectional Converter With Natural Grid Harmonic Elimination

Generally, AC-DC converters have an AC-DC stage followed by a DC-DC stage. In these two stage approaches, the AC-DC stage is hard-switched, whereas the DC-DC stage is soft-switched. Therefore, the devices in the AC-DC stage can be switched only at tens of kHz to avoid excessive switching losses, thus limiting the bandwidth of the current control loop. Hence, the control of these converters with distorted grid voltages requires multiple harmonic compensation loops or other complex control algorithms in order for the grid currents to comply with IEEE standards. By integrating both the stages, the devices in the AC-DC stage can also be soft-switched, thus facilitating higher switching frequency, and thereby higher current control bandwidth. This paper proposes an integrated multilevel bidirectional AC-DC converter with improved control bandwidth and disturbance rejection. It is shown experimentally that the high bandwidth current control loop of the converter can reject grid harmonic current disturbances, without the need for any compensation loops or complex control techniques, and comply with IEEE standards.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2015

Harmonics in a Wind Power Plant: Preprint

Wind power generation has been growing at a very fast pace for the past decade, and its influence and impact on the electric power grid is significant. As in a conventional power plant, a wind power plant (WPP) must ensure that the quality of the power being delivered to the grid is excellent. At the same time, the wind turbine should be able to operate immune to small disturbances coming from the grid. Harmonics are one of the more common power quality issues presented by large WPPs because of the high switching frequency of the power converters and the possible nonlinear behavior from electric machines (generator, transformer, reactors) within a power plant. This paper presents a summary of the most important issues related to harmonics in WPPs and discusses practical experiences with actual Type 1 and Type 3 wind turbines in two WPPs.

17 WIND ENERGY↗

DOE OSTI2020

Harmonics and Stability Evaluation of Converter-Interfaced Combined Heat and Power Units

Grid integration of medium-sized combined heat and power (CHP) units is challenging due to strict grid codes and conventional generators lack of control flexibility to meet these grid codes. Adding a two-stage ac-dc-ac power electronics interface between the generator and the utility grid will accelerate the interconnection process of CHP units. For the dc-ac stage, a voltage source converter (VSC) has been widely used as a grid-tied inverter because of its fast control and low total harmonics distortion (THD). In this paper, several topologies of generator-side rectifiers for ac-dc power conversion are explored and analyzed. The harmonics impact of various rectifiers on the CHP generator are evaluated. The overall cost of the electrical system, when using various types of rectifiers, is assessed and the VSC back-to-back converter interface configuration is found to be optimal. The overall system stability is also examined using small-signal impedance analysis to assess potential instability issues at the system level.

CHP, Harmonics, Generator Rectifier Unit, DC Imped↗

DOE OSTI2021

Cyber-Attack Detection for Photovoltaic Farms Based on Power-Electronics-Enabled Harmonic State Space Modeling

Here in this paper, a physics-data-based detection method is proposed to detect a variety of cyber-attacks in Photovoltaic (PV) farms using the power electronics-enabled harmonic state space (HSS) models, which, to our knowledge, is original. At the device level, HSS-based detection is developed to monitor harmonic vectors of individual PV converter with minimum sensor measurements, thus improving accuracy and robustness compared to Kalman Filter-based detection. At the system level that involves multiple PV converters, a clustering approach is developed to investigate attack propagation and accurately locate attack sources within a PV farm. The proposed approach is one of the first attempts to address PV security through interaction between the device and system, maximizing the accuracy and robustness at different levels. To verify the feasibility, a comprehensive attacks model is built, including single attack, coordinated attacks, and replay attacks. Besides, the impacts of irradiance changes are taken into consideration in the test scenarios. With the real-time data acquisition and hardware-in-the-loop testbed, comprehensive test results are provided to verify the feasibility of the proposed detection methodology.

42 ENGINEERING↗