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At least 73 records · Page 4

Two-dimensional coherent spectrum of high-spin models via a quantum computing approach

Here in this work we present and benchmark a quantum computing approach to calculate the two-dimensional coherent spectrum (2DCS) of high-spin models. Our approach is based on simulating their real-time dynamics in the presence of several magnetic field pulses, which are spaced in time. We utilize the adaptive variational quantum dynamics simulation algorithm for the study due to its compact circuits, which enables simulations over sufficiently long times to achieve the required resolution in frequency space. Specifically, we consider an antiferromagnetic quantum spin model that incorporates Dzyaloshinskii-Moriya interactions and single-ion anisotropy. The obtained 2DCS spectra exhibit distinct peaks at multiples of the magnon frequency, arising from transitions between different eigenstates of the unperturbed Hamiltonian. By comparing the one-dimensional coherent spectrum with 2DCS, we demonstrate that 2DCS provides a higher resolution of the energy spectrum. We further investigate how the quantum resources scale with the magnitude of the spin using two different binary encodings of the high-spin operators: the standard binary encoding and the Gray code. At low magnetic fields both encodings require comparable quantum resources, but at larger field strengths the Gray code is advantageous. Numerical simulations for spin models with increasing number of sites indicate a polynomial system-size scaling for quantum resources. Lastly, we compare the numerical 2DCS with experimental results on a rare-earth orthoferrite system. The observed strength of the magnonic high-harmonic generation signals in the 2DCS of the quantum high-spin model aligns well with the experimental data, showing significant improvement over the corresponding mean-field results.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Propagation effects in polarization-gated attosecond soft-X-ray pulse generation

Accurate estimation of the duration of soft-x-ray pulses from high-harmonic generation (HHG) remains challenging given their higher photon energies and broad spectral bandwidth. The carrier-envelope-phase (CEP) dependence of generated soft-x-ray spectra is indicative of attosecond pulse generation, but advanced simulations are needed to infer the pulse duration from such data. Here, we employ macroscopic propagation simulations to reproduce experimental polarization-gated CEP-dependent soft-x-ray spectra. The simulations indicate chirped pulses, which we theoretically find to be compressible in hydrogen plasmas, suggesting this as a viable compression scheme for broadband soft-x-rays from HHG.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

A beamline for ultrafast extreme ultraviolet magneto-optical spectroscopy in reflection near the shot noise limit

High harmonic generation (HHG) makes it possible to measure spin and charge dynamics in materials on femtosecond to attosecond timescales. However, the extreme nonlinear nature of the high harmonic process means that intensity fluctuations can limit measurement sensitivity. Here we present a noise-canceled, tabletop high harmonic beamline for time-resolved reflection mode spectroscopy of magnetic materials. We use a reference spectrometer to independently normalize the intensity fluctuations of each harmonic order and eliminate long term drift, allowing us to make spectroscopic measurements near the shot noise limit. Here, these improvements allow us to significantly reduce the integration time required for high signal-to-noise (SNR) measurements of element-specific spin dynamics. Looking forward, improvements in the HHG flux, optical coatings, and grating design can further reduce the acquisition time for high SNR measurements by 1–2 orders of magnitude, enabling dramatically improved sensitivity to spin, charge, and phonon dynamics in magnetic materials.

47 OTHER INSTRUMENTATION↗

Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗

Enhanced cutoff energies for direct and rescattered strong-field photoelectron emission of plasmonic nanoparticles

Abstract The efficient generation, accurate detection, and detailed physical tracking of energetic electrons are of applied interest for high harmonics generation, electron-impact spectroscopy, and femtosecond time-resolved scanning tunneling microscopy. We here investigate the generation of photoelectrons (PEs) by exposing plasmonic nanostructures to intense laser pulses in the infrared (IR) spectral regime and analyze the sensitivity of PE spectra to competing elementary interactions for direct and rescattered photoemission pathways. Specifically, we measured and numerically simulated emitted PE momentum distributions from prototypical spherical gold nanoparticles (NPs) with diameters between 5 and 70 nm generated by short laser pulses with peak intensities of 8.0 × 10 12 and 1.2 × 10 13 W/cm 2 , demonstrating the shaping of PE spectra by the Coulomb repulsion between PEs, accumulating residual charges on the NP, and induced plasmonic electric fields. Compared to well-understood rescattering PE cutoff energies for strong-field photoemission from gaseous atomic targets (10× the ponderomotive energy), our measured and simulated PE spectra reveal a dramatic cutoff-energy increase of two orders of magnitude with a significantly higher contribution from direct photoemission. Our findings indicate that direct PEs reach up to 93 % of the rescattered electron cutoff energy, in contrast to 20 % for gaseous atoms, suggesting a novel scheme for the development of compact tunable tabletop electron sources.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Extended quantitative rescattering model for simulating high-order harmonic streaking spectra by synchronization of an intense IR laser and a time-delayed attosecond XUV pulse

In this work, we theoretically investigate the modulated high-harmonic generation (HHG) driven by an intense few-cycle infrared (IR) laser field and a weak extreme-ultraviolet (XUV) pulse at a delayed time. We establish an extended quantitative rescattering (EQRS) model to simulate the HHG streaking spectra, with the ideas of correcting the IR ionization and the transition from the ground to continuum states in the strong-field approximation. The EQRS model has an accuracy comparable to that from “exactly” solving the time-dependent Schrödinger equation (TDSE). We reveal that the fringes in the streaking spectra are caused by the interference between the attosecond XUV pulse and harmonics resulting from different recombination pathways under the intense IR laser. We then demonstrate that the XUV pulse can be accurately retrieved by treating the single-atom TDSE results or macroscopic propagation results as the “input” data. This work provides with a tool for efficiently simulating and thoroughly analyzing the XUV-assisted HHG, which could also enhance its capability for tracing the electron dynamics involved in the strong-field phenomena.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Efficient generation and extreme compression of multidimensional solitary states in molecular gas-filled hollow-core fibers driven by picosecond Yb lasers

We present an in-depth study on the impact of spatiotemporal Raman enhancement in molecular gas-filled hollow-core fibers (HCFs), demonstrating the efficient generation and post-compression of multidimensional solitary states (MDSS). Through different experimental scenarios—employing large-core HCFs filled with molecular gases (N 2 and N 2 O) and driven by high energy, sub-picosecond and picosecond Fourier transform-limited ytterbium laser pulses—this work leverages multimode propagation and enhanced spatiotemporal interactions to achieve significant spectral broadening and asymmetric redshift, contrasting sharply with self-phase modulation. Our findings reveal that, beyond the regime of maximum nonadiabatic molecular alignment, spatiotemporal nonlinear enhancement primarily governs spectral broadening for input pulse durations up to 1 ps. The process shows limited sensitivity to input pulse duration and the two investigated molecular gases (N 2 and N 2 O), with only subtle differences in broadening arising from their distinct Raman spectroscopic properties. Furthermore, post-compression of MDSS was achieved in various cases. Notably, using 7 mJ, 1 ps laser pulses, we generated 22 fs pulses with a 47% energy conversion efficiency of the input pulse energy. These results position MDSS as a powerful platform for generating high-energy, ultrashort pulses with tunable wavelengths, offering a robust solution for applications such as high harmonic generation.

47 OTHER INSTRUMENTATION↗

EUV and Hard X-ray Hartmann Wavefront Sensing for Optical Metrology, Alignment and Phase Imaging

For more than 15 years, Imagine Optic have developed Extreme Ultra Violet (EUV) and X-ray Hartmann wavefront sensors for metrology and imaging applications. These sensors are compatible with a wide range of X-ray sources: from synchrotrons, Free Electron Lasers, laser-driven betatron and plasma-based EUV lasers to High Harmonic Generation. In this paper, we first describe the principle of a Hartmann sensor and give some key parameters to design a high-performance sensor. We also present different applications from metrology (for manual or automatic alignment of optics), to soft X-ray source optimization and X-ray imaging.

20 metrology↗

Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides

We present a systematic study of the crystal-orientation dependence of high-harmonic generation in monolayer transition-metal dichalcogenides, WS 2 and MoSe 2 , subjected to intense linearly polarized midinfrared laser fields. The measured spectra consist of both odd- and even-order harmonics, with a high-energy cutoff extending beyond the 15th order for a laser-field strength around ~1 V/nm. In WS 2 , we find that the polarization direction of the odd-order harmonics smoothly follows that of the laser field irrespective of the crystal orientation, whereas the direction of the even-order harmonics is fixed by the crystal mirror planes. Furthermore, the polarization of the even-order harmonics shows a flip in the course of crystal rotation when the laser field lies between two of the crystal mirror planes. By numerically solving the semiconductor Bloch equations for a gapped-graphene model, we qualitatively reproduce these experimental features and find the polarization flipping to be associated with a significant contribution from interband polarization. In contrast, high-harmonic signals from MoSe 2 exhibit deviations from the laser-field following of odd-order harmonics and crystal-mirror-plane following of even-order harmonics. We attribute these differences to the competing roles of the intraband and interband contributions, including the deflection of the electron-hole trajectories by nonparabolic crystal bands.

36 MATERIALS SCIENCE↗

Searching for optimal THz generation through calculations of the asymmetry of photoelectron momentum distributions by an improved strong-field-approximation method

From the solution of the time-dependent Schrödinger equation (TDSE), it has been shown that in a two-color laser pulse the relative phase that optimizes terahertz (THz) radiation also optimizes the asymmetry of the angular distribution of photoelectrons. Here, in this work, we show that a second-order strong-field approximation can accurately calculate the asymmetry of photoelectrons and thus can locate the phase delay that optimizes THz generation, doing so four orders of magnitude faster than TDSE calculations. We further trace that this is possible because THz emission originates from a free-free radiative transition between the rescattered electron and the target ion, similar to other electron-ion collisions in the laser field, e.g., high-harmonic generation and nonsequential double ionization. Our results pave the way to locate the optimal phase delay for any typical laser pulses for maximal THz generation in the laboratory.

74 ATOMIC AND MOLECULAR PHYSICS↗

Department of Energy Project DE-SC0012198: Probing Electron-Molecule Scattering with HHG: Theory and Experiment (Final Report)

The study of the motion of atoms in molecules is important to understanding many areas of physical and life sciences. Such motion occurs on many different times scales, with electronic motion occurring on a sub-femtosecond time scale, and simple vibrational motion in tens to hundreds of femtoseconds. One way to follow such processes in real time is by the use of shortpulsed lasers, and in particular by studying time-resolved photoionization and the related process of high-harmonic generation (HHG). Thus there has been much effort to develop the tools necessary to probe molecular systems using short pulse lasers and understanding the sensitivity of the different possible probes to the time dependent geometric structure as well as the electronic structure of molecules. Our research has particularly focused on the connection between high-field processes and the more traditional weak field photoionization processes. Strong field and weak field processes can be connected through models that involve the same matrix elements. We have demonstrated in our study of HHG from SF 6 that the spectrum is sensitive to the interplay between the angular dependence of the ionization step and recombination step. In our study of rescattering spectroscopy, we have shown that with a combination of experiment and theory, we can use this high-field spectroscopy to determine molecular structure in molecules such as C 2 H 4 . We have also developed new computational tools based on overset grids to enable studies on larger molecular systems which use much more robust numerical approaches so that the resulting code can be a tool that non-specialists can use to study related systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Extension of the bright high-harmonic photon energy range via nonadiabatic critical phase matching

The concept of critical ionization fraction has been essential for high-harmonic generation, because it dictates the maximum driving laser intensity while preserving the phase matching of harmonics. In this work, we reveal a second, nonadiabatic critical ionization fraction, which substantially extends the phase-matched harmonic energy, arising because of the strong reshaping of the intense laser field in a gas plasma. We validate this understanding through a systematic comparison between experiment and theory for a wide range of laser conditions. In particular, the properties of the high-harmonic spectrum versus the laser intensity undergoes three distinctive scenarios: (i) coincidence with the single-atom cutoff, (ii) strong spectral extension, and (iii) spectral energy saturation. We present an analytical model that predicts the spectral extension and reveals the increasing importance of the nonadiabatic effects for mid-infrared lasers. These findings are important for the development of high-brightness soft x-ray sources for applications in spectroscopy and imaging.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Generation of 3.3-mJ, 2.45-µm, sub-2-cycle laser pulses via hollow-core fiber pulse compression

We demonstrate nonlinear compression of mid-infrared pulses from a Cr:ZnSe chirped-pulse amplifier using a gas-filled stretched hollow-core fiber followed by bulk-material compression. Starting from 90 fs, 2.45 µm pulses with 5.3 mJ energy, spectral broadening in the gas-filled capillary combined with optimized dispersion management enables compression to 15 fs, less than two optical cycles at 2.45 µm, with 3.3 mJ pulse energy, corresponding to a peak power of approximately 0.12 TW. The simplicity of the approach, based on a single hollow-core fiber stage and bulk dispersion compensation, makes it scalable to higher energies and establishes a robust route to mid-infrared drivers for high harmonic generation and attosecond applications.

Britton, Mathew [SLAC National Accelerator Laborat↗

Tailoring the Thickness‐Dependent Optical Properties of Conducting Nitrides and Oxides for Epsilon‐Near‐Zero‐Enhanced Photonic Applications

Abstract The unique properties of the emerging photonic materials, conducting nitrides and oxides, especially their tailorability, large damage thresholds, and, importantly, the so‐called epsilon‐near‐zero (ENZ) behavior, have enabled novel photonic phenomena spanning optical circuitry, tunable metasurfaces, and nonlinear optical devices. This work explores direct control of the optical properties of polycrystalline titanium nitride (TiN) and aluminum‐doped zinc oxide (AZO) by tailoring the film thickness, and their potential for ENZ‐enhanced photonic applications. This study demonstrates that TiN–AZO bilayers support Ferrell–Berreman modes using the thickness‐dependent ENZ resonances in the AZO films operating in the telecom wavelengths spanning from 1470 to 1750 nm. The bilayer stacks also act as strong light absorbers in the ultraviolet regime using the radiative ENZ modes and the Fabry–Perot modes in the constituent TiN films. The studied Berreman resonators exhibit optically induced reflectance modulation of 15% with picosecond response time. Together with the optical response tailorability of conducting oxides and nitrides, using the field enhancement near the tunable ENZ regime can enable a wide range of nonlinear optical phenomena, including all‐optical switching, time refraction, and high‐harmonic generation.

Saha, Soham↗

High‐Order Nonlinear Frequency Conversion in Transparent Conducting Oxide Thin Films

The study of conductive oxides has gained momentum within the photonics community due to their unique linear and nonlinear optical properties. Despite recent experiments reporting on high harmonic generation from thin films, the optical/electronic behavior of these compounds at the nanoscale is still not fully understood due to the lack of a suitable theoretical model. In the present work, aluminum zinc oxide is excited near its epsilon-near-zero crossing point using incident femtosecond pulses having peak power densities in the 1 TW cm −2 range. A relatively efficient frequency up-conversion including even and odd harmonics up to the seventh order is observed. A hydrodynamic-Maxwell theoretical approach is adopted, capable of simultaneously taking into account linear and nonlinear dispersions, nonlocal effects, surface, magnetic, and bulk nonlinearities in a spectral region that spans over two and a half octaves from the UV to the NIR region. The study enables a deeper understanding of the fundamental material parameters regulating optical nonlinearities, providing important insights to engineer this class of materials for applications in sensing, ultra-fast physics, and spectroscopy.

material modeling↗

Ultrafast X-ray Spectroscopy of Intersystem Crossing in Hexafluoroacetylacetone: Chromophore Photophysics and Spectral Changes in the Face of Electron-Withdrawing Groups

Intersystem crossings between singlet and triplet states represent a crucial relaxation pathway in photochemical processes. Herein, we probe the intersystem crossing in hexafluoro-acetylacetone with ultrafast X-ray transient absorption spectroscopy at the carbon K-edge. In this study, we observe the excited state dynamics following excitation with 266 nm UV light to the 1 ππ* (S 2 ) state with element and site-specificity using a broadband soft X-ray pulse produced by high harmonic generation. These results are compared to X-ray spectra computed from orbital optimized density functional theory methods. It is found that the electron-withdrawing fluorine atoms decongest the X-ray absorption spectrum by enhancing separation between features originating from different carbon atoms. This facilitates the elucidation of structural and electronic dynamics at the chromophore. The evolution of the core-to-valence resonances at the carbon K-edge reveals an ultrafast population transfer between the 1 nπ* (S 1 ) and 3 ππ* (T 1 ) states on a 1.6 ± 0.4 ps time scale, which is similar to the 1.5 ps time scale earlier observed for acetylacetone [ J. Am. Chem. Soc. 2017, 139, 16576—16583, DOI: 10.1021/jacs.7b07532]. It therefore appears that terminal fluorination has little influence on the intersystem crossing rate of the acetylacetone chromophore. In addition, the significant role of hydrogen-bond opened and twisted rotational isomers is elucidated in the excited state dynamics by comparison of the experimental transient X-ray spectra with theory.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Attosecond Transient Grating Spectroscopy with Near-Infrared Grating Pulses and an Extreme Ultraviolet Diffracted Probe

Transient grating spectroscopy has become a mainstay among metal and semiconductor characterization techniques. Here, we extend the technique toward the shortest achievable time scales by using tabletop high-harmonic generation of attosecond extreme ultraviolet (XUV) pulses that diffract from transient gratings generated with sub-5 fs near-infrared (NIR) pulses. We demonstrate the power of attosecond transient grating spectroscopy (ATGS) by investigating the ultrafast photoexcited dynamics in an Sb semimetal thin film. ATGS provides an element-specific, background-free signal unfettered by spectral congestion, in contrast to transient absorption spectroscopy. With ATGS measurements in Sb polycrystalline thin films, we observe the generation of coherent phonons and investigate the lattice and carrier dynamics. Among the latter processes, we extract carrier thermalization, hot carrier cooling, and electron-hole recombination, which are on the order of 20 fs, 50 fs, and 2 ps time scales, respectively. Furthermore, the simultaneous collection of transient absorption and transient grating data allows us to extract the total complex dielectric constant in the sample dynamics with a single measurement, including the real-valued refractive index, from which we are also able to investigate carrier-phonon interactions and longer-lived phonon dynamics. The outlined experimental technique expands the capabilities of transient grating spectroscopy and attosecond spectroscopies by providing a wealth of information concerning carrier and lattice dynamics with an element-selective technique at the shortest achievable time scales.

Quintero-Bermudez, Rafael↗

Signatures of the Bromine Atom and Open-Shell Spin Coupling in the X-ray Spectrum of the Bromobenzene Cation

Tabletop X-ray spectroscopy measurements at the carbon K-edge complemented by ab initio calculations are used to investigate the influence of the bromine atom on the carbon core–valence transitions in the bromobenzene cation (BrBz + ). The electronic ground state of the cation is prepared by resonance-enhanced two-photon ionization of neutral bromobenzene (BrBz) and probed by X-rays produced by high-harmonic generation (HHG). Replacing one of the hydrogen atoms in benzene with a bromine atom shifts the transition from the 1s C* orbital of the carbon atom (C*) bonded to bromine by ~1 eV to higher energy in the X-ray spectrum compared to the other carbon atoms (C). Moreover, in BrBz + , the X-ray spectrum is dominated by two relatively intense transitions, 1s C →π* and 1s C* →σ*(C*–Br), where the second transition is enhanced relative to the neutral BrBz. In addition, a doublet peak shape for these two transitions is observed in the experiment. The 1s C →π* doublet peak shape arises due to the spin coupling of the unpaired electron in the partially vacant π orbital (from ionization) with the two other unpaired electrons resulting from the transition from the 1s C core orbital to the fully vacant π* orbitals. Here, the 1s C* →σ* doublet peak shape results from several transitions involving σ* and vibrational C*–Br mode activations following the UV ionization, which demonstrates the impact of the C*–Br bond length on the core–valence transition as well as on the relaxation geometry of BrBz + .

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗