The Weyl-Kondo semimetal: high-harmonic generation and extreme topological tunability
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Material Science↗
SEARCH · Engineering Papers
Results for “high harmonic generation”
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High-harmonic generation from artificially stacked 2D crystals
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Heide, Christian↗
Cavity-enhanced high-order harmonic generation for high-performance time-resolved photoemission experiments
Recent breakthroughs in high repetition-rate extreme ultraviolet (XUV) light sources and photoelectron analyzers have led to dramatic advances in the performance of time-resolved photoemission experiments. In this perspective article, we discuss the application of cavity-enhanced high-order harmonic generation, with repetition rates exceeding 10 MHz, to photoemission experiments using advanced endstations incorporating time-of-flight photoelectron analyzers. We discuss recent results, perspective on future areas for further technological improvement, and the wide array of science enabled by ultrafast XUV photoemission experiments, now in a qualitatively new regime.
Allison, Thomas K. (ORCID:0000000302898830)↗
Phase-matching analysis in high-order harmonic generation with nonzero orbital angular momentum Laguerre-Gaussian beams
Through high-order harmonic generation driven by intense ultrashort vortex infrared or midinfrared lasers, a nonzero orbital angular momentum can be imprinted onto extreme ultraviolet (XUV) or soft-x-ray (SXR) light pulses. Here we simulate the generation of vortex XUV harmonics in the gas medium as well as their propagation in vacuum till reaching the far field. In this work, we find that the intensity and phase of generated high harmonics are very sensitive to the position of gas jet with respect to the laser focus. The topological charge of the $\textit{q}$th harmonic is found to be $\textit{q}$ times that of the driving Laguerre-Gaussian beam. Each harmonic in the far field appears as a single ring in the transverse plane with an invariant diameter which is scalable with the fundamental topological charge only when the gas jet is placed after the laser focus. The underlying phase-matching mechanism is analyzed by examining the spatial map of the coherence length and by calculating the evolution of harmonic emission in the medium. We anticipate this work to stimulate interest in generating intense vortex XUV or SXR attosecond pulses for probing dynamics of molecules where special molecular features are difficult to be detected with linear or circular XUV or SXR pulses.
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
A tutorial on high-order harmonic generation in atoms, molecules, and condensed matter
This tutorial introduces strong-field-driven high-order harmonics, their experimental generation and characterization techniques, and their main applications including attosecond pulse generation and ultrafast spectroscopy of the target material. We begin from the use of atomic targets, where the first high-order harmonic generation (HHG) experiments were realized in the late 1980s. Then, we briefly discuss the basics of the microscopic generation mechanism and how various steps of the mechanism were exploited in applications such as generating isolated attosecond pulses and probing molecular orbitals. We introduce and describe the standard experimental approaches for condensed phase HHG, where we discuss unique technical challenges of the use of solid-state materials, such as the mitigation of plasma formation and laser damage. We cover the fundamentals of high-harmonic spectroscopy in condensed matter systems, such as wide bandgap dielectrics, semiconductors, liquid media, and 2D-crystals. We provide some examples of rapidly emerging spectroscopic capabilities, such as for probing crystal symmetries, Berry phases, and associated non-trivial topological properties of the source material. Finally, we provide an overview of the research field, including some of the challenges, opportunities, and open questions.
Attosecond pulses↗
Enhancing high-order harmonic generation by controlling the diffusion of the electron wave packet
We experimentally study the enhancement of high-order harmonic generation (HHG) driven by synthesized ω <#comment/> − <#comment/> 3 ω <#comment/> laser fields, where we control whether the ionization rate or the electron wave packet’s diffusion is the dominant enhancement mechanism. When minimizing the electron wave packet’s diffusion, the excursion times of the corresponding electron trajectories are reduced by a factor of 2 or more. This result is important for imaging techniques that use the returning electron wave packet to probe the remaining ion. Furthermore, we achieve a 10 × <#comment/> to 3800 × <#comment/> enhancement of the harmonic yield driven by the bichromatic fields relative to that of an optimized single-color field, showing that the bichromatic fields improve HHG’s capability as a light source. We also measure that the two-color field’s harmonics have half the divergence angle compared to their single-color counterpart, suggesting that the “short” electron trajectories play a more prominent role compared to their “long” trajectory counterparts, thus improving the wavefront of the emerging harmonic beam.
74 ATOMIC AND MOLECULAR PHYSICS↗
Two-color-driven enhanced high-order harmonic generation in solids
We theoretically investigate the emission of high-harmonic (HH) radiation in model crystals by bichromatic few-cycle driving pulses that are composed as the phase-coherent superposition of a mid-infrared fundamental pulse and its second harmonic. Adjusting the model-crystal parameters to reproduce the lowest band gap of MgO, we examine the extent to which distinct domains of the HH spectrum can be controlled and enhanced by tuning the temporal profile of the bichromatic driving laser electric field. We change the driving-pulse shape by varying its fundamental-versus-second-harmonic pulse amplitude ratio and delay, while keeping the energy of the driving laser pulse fixed. For suitable amplitude ratios and delays, we find an up to fivefold enhancement of the spectral HH yield and significant shifts of the HH cutoff frequency.
74 ATOMIC AND MOLECULAR PHYSICS↗
Role of the Porras factor in phase matching of high-order harmonic generation driven by focused few-cycle laser pulses
We investigate the role of the Porras factor (or laser focusing effect) on the macroscopic high-order harmonic generation (HHG) driven by a focused broadband few-cycle laser beam. By employing a non-adiabatic phase-matching analysis method, we reveal that phase mismatch due to the induced-dipole phase varies with the Porras factor, which is dominant in phase matching at low gas pressure. We also find that in a strongly ionized medium when gas pressure is high, the nonlinear propagation is dominated by a plasma effect such that the focusing effect is mitigated, resulting in similar poor phase matching of HHG regardless of the Porras factor. Our results are expected to assist experimentalists identifying optimal conditions for HHG using ultrashort laser pulses.
Optics↗
Genetic-algorithm retrieval of the molecular alignment distribution with high-order harmonics generated from transiently aligned CO 2 molecules
Using genetic algorithm, we propose a method to retrieve the alignment distribution of transiently aligned CO 2 molecules from the high-order harmonic generation (HHG) spectra. The retrieval method is based on the quantitative rescattering (QRS) model where averaged photorecombination transition dipole can be factored out from the parallel (or perpendicular) harmonic spectra after the propagation of the harmonic fields in the gas medium. We examine how the retrieved alignment distributions are affected by uncertainty in alignment dependent ionization probability and on multiple orbital contribution to the HHG. We further confirm that alignment distribution is more accurately retrieved by using the minima in the HHG spectra driven by a long-wavelength laser. In addition, we show that earlier experimental data on the ratios between the perpendicular and the parallel HHG components of aligned CO 2 molecules are in better agreement with the QRS model if the macroscopic propagation and multiple orbital interference are included in the theoretical calculation.
74 ATOMIC AND MOLECULAR PHYSICS↗
High-efficiency second harmonic generation of blue light on thin-film lithium niobate
The strength of interactions between photons in a χ (2) nonlinear optical waveguide increases at shorter wavelengths. These larger interactions enable coherent spectral translation and light generation at a lower power, over a broader bandwidth, and in a smaller device: all of which open the door to new technologies spanning fields from classical to quantum optics. Stronger interactions may also grant access to new regimes of quantum optics to be explored at the few-photon level. One promising platform that could enable these advances is thin-film lithium niobate (TFLN), due to its broad optical transparency window and possibility for quasi-phase matching and dispersion engineering. In this Letter, we demonstrate second harmonic generation of blue light on an integrated thin-film lithium niobate waveguide and observe a conversion efficiency of η 0 = 33, 000%/W- cm 2 , significantly exceeding previous demonstrations.
Park, Taewon↗
Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating
High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.
attosecond science↗
Intense infrared lasers for strong-field science
The advent of chirped-pulse amplification in the 1980s and femtosecond Ti:sapphire lasers in the 1990s enabled transformative advances in intense laser–matter interaction physics. Whereas most of experiments have been conducted in the limited near-infrared range of 0.8–1 μm, theories predict that many physical phenomena such as high harmonic generation in gases favor long laser wavelengths in terms of extending the high-energy cutoff. Significant progress has been made in developing few-cycle, carrier-envelope phase-stabilized, high-peak-power lasers in the 1.6–2 μm range that has laid the foundation for attosecond X ray sources in the water window. Even longer wavelength lasers are becoming available that are suitable to study light filamentation, high harmonic generation, and laser–plasma interaction in the relativistic regime. Long-wavelength lasers are suitable for sub-bandgap strong-field excitation of a wide range of solid materials, including semiconductors. In the strong-field limit, bulk crystals also produce high-order harmonics. In this review, we first introduce several important wavelength scaling laws in strong-field physics, then describe recent breakthroughs in short- (1.4–3 μm), mid- (3–8 μm), and long-wave (8–15 μm) infrared laser technology, and finally provide examples of strong-field applications of these novel lasers. Furthermore, some of the broadband ultrafast infrared lasers will have profound effects on medicine, environmental protection, and national defense, because their wavelengths cover the water absorption band, the molecular fingerprint region, as well as the atmospheric infrared transparent window.
43 PARTICLE ACCELERATORS↗
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↗
On the Impact of High-Order Harmonic Generation in Electrical Distribution Systems
The modern power grid has seen a rise in the integration of non-linear loads, presenting a significant concern for operators. These loads introduce unwanted harmonics, leading to potential issues such as overheating and improper functioning of circuit breakers. In pursuing a more sustainable grid, the adoption of electric vehicles (EVs) and photovoltaic (PV) systems in residential networks has increased. Understanding and examining the effects of high-order harmonic frequencies beyond $1.5$ kHz is crucial to understanding their impact on the operation and planning of electrical distribution systems under varying nonlinear loading conditions. This study investigates a diverse set of critical power electronic loads within a household modeled using PSCAD/EMTdc, analyzing their unique harmonic spectra. This information is utilized to run the time-series harmonic analysis program in OpenDSS on a modified IEEE 34 bus test system model. The impact of high-order harmonics is quantified using metrics that evaluate total harmonic distortion (THD), transformer harmonic-driven eddy current loss component, and propagation of harmonics from the source to the substation transformer.
Peerzada, Aaqib A. [BATTELLE (PACIFIC NW LAB)]↗
High-order harmonic generation from ultrarelativistic s-polarized 400 nm laser-solid interactions
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Flores, V. [University of California, Irvine] (ORC↗
High-order harmonic generation in graphene quantum dots in the field of an elliptically polarized pulse
Not provided.
Materials Science↗
Ultrafast Dynamics of Molecules on Surfaces Studied with Time-Resolved XUV Photoelectron Spectroscopy (Final Report)
In this project we set out to make technical advances in time-resolved photoemission from surfaces and study molecule-surface charge transfer processes. Combining a novel light source developed at Stony Brook with a new type of time-of-flight photoemission electron microscope (TOF k-mic) developed in Mainz, Germany, we achieved the former goal. Our light source, based on cavity-enhanced high harmonic generation at 61 MHz repetition rate, enables ultrafast time-resolved photoemission experiments to be conducted with orders of magnitude higher photocurrents than otherwise possible. Critically, this provides the high dynamic range necessary to study perturbatively excited samples, such that one can study the intrinsic dynamics of electrons and holes as they would occur in a device. Combining our light source with the TOF k-mic, we’ve achieved an overall improvement in data rate of time- and angle-resolved photoemission (tr-ARPES) of approximately four orders of magnitude over the previous state-of-the-art using kHz-repetition rate sources and conventional hemispherical electron analyzers. This new instrument is now being used in experiments on 2D materials and organic semiconductors.
74 ATOMIC AND MOLECULAR PHYSICS↗