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Results for “Strong-field approximation”

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At least 19 records

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↗

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↗

Partial-wave decomposition of the Keldysh ionization amplitude

We present an alternative way of calculating the Keldysh amplitude, i.e., the length-gauge form of the ionization amplitude in the strong-field approximation. The amplitude is evaluated exactly by expanding it in Fourier components and partial waves. Comparisons of the semianalytic model predictions with results of ab initio numerical simulations of the time-dependent Schrödinger equation for the interaction of electrons in short-range potentials with intense laser light yield excellent agreement, for wavelengths from the single photon to the multiphoton to the tunneling regime. Specifically, for ionization from initial states with higher angular momentum quantum number, e.g., p states, a significant improvement over predictions based on the popular saddle-point approximation is found. Furthermore, the current model rate allows for interpretation of the strong-field ionization process in terms of multiphoton absorption pathways and angular momentum selection rules.

74 ATOMIC AND MOLECULAR PHYSICS↗

Probing two-path electron quantum interference in strong-field ionization with time-correlation filtering

We report attosecond dynamics in strong-field tunnel ionization are encoded in intricate holographic patterns in the photoelectron momentum distributions. These patterns show the interference between two or more superposed quantum electron trajectories, which are defined by their ionization times and subsequent evolution in the laser field. We determine the ionization time separation between interfering pairs of electron orbits by performing a differential Fourier analysis on the measured momentum spectrum. We identify electron holograms formed by trajectory pairs whose ionization times are separated by less than a single quarter cycle, between a quarter cycle and half cycle, between a half cycle and three fourths of a cycle, and a full cycle apart. We compare our experimental results to the predictions of the Coulomb quantum orbit strong-field approximation (CQSFA) with significant success. We also time-filter the CQSFA trajectory calculations to demonstrate the validity of the technique on spectra with known time correlations. As a general analysis technique, the filter can be applied to all energy- and angularly resolved data sets to recover time correlations between interfering electron pathways, providing an important tool to analyze any strong-field ionization spectra. Moreover, it is independent of theory and can be applied directly to experiments, without the need of a direct comparison with orbit-based theoretical methods.

74 ATOMIC AND MOLECULAR PHYSICS↗

Direct reconstruction of isolated XUV or soft x-ray attosecond pulses from high-harmonic generation streaking spectra

Characterization of an isolated attosecond pulse (IAP) in the extreme ultraviolet (XUV) or soft x-ray (SXR) region is essential for its applications. Here we propose to retrieve an IAP in the time domain directly through the modulation of high-harmonic generation (HHG) spectra in the presence of a time-delayed intense few-cycle infrared or mid-infrared laser. The retrieval algorithm is derived based on the strong-field approximation and an extended quantitative rescattering model. We show that both isolated XUV pulses with a narrow spectral bandwidth and isolated SXR pulses with a broad bandwidth can be well characterized through the HHG streaking spectra. Such an all-optical method for characterizing the IAP differs from the commonly used approach based on the streaked photoelectron spectra that would require electron spectrometers. We check the robustness of the retrieval method by changing the dressing laser or by adjusting the steps of time delay. We also show that the XUV pulse can be accurately retrieved by treating the HHG streaking spectra calculated from solving the time-dependent Schrödinger equation for single atoms as the ‘experimental’ data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Nonadiabatic strong-field photoionization revisited: Detailed analysis

We develop a theoretical framework to interpret “bump-like” enhancements in the energy distribution of electrons emitted from cesium atoms subjected to intense infrared laser fields, as observed in a recent experiment. These emissions, detected at energies approaching twice the ponderomotive energy (2⁢𝑈 p ), indicate a mechanism where electrons are nonadiabatically ejected with substantial inward velocity following ionization. The bump-like features arise from returning trajectories that scatter off the residual ion. We interpret these experimental results classically using a periodically driven version of the Bohr model and quantum mechanically through Keldysh's adiabaticity parameter (𝛾 K ) and Reiss's continuum-state intensity parameter 𝒵 in a Coulomb-corrected version of the strong-field approximation (SFA) that incorporates “complex” electronic trajectories. Notably, our theoretical analysis shows that these emissions are independent of the specific short-range form of the atomic potential.

74 ATOMIC AND MOLECULAR PHYSICS↗

Nonadiabatic Strong-Field Photoionization Revisited

We measure strong field ionization of cesium atoms, observing a robust feature near 2⁢𝑈p in the photoelectron spectrum, which we call the intermediate energy structure (IES). Using a Coulomb-corrected strong-field approximation, we show it arises from electrons born with large inward velocities that rapidly undergo forward scattering off the Coulomb potential. The IES is similar to the previously identified low energy structure in that they are both due to forward scattering. However, it is different in that IES requires both nonadiabatic ionization conditions (as defined by the Keldysh parameter) and a more weakly bound initial state. Furthermore, our joint experimental and theoretical study supports the need for an additional parameter in characterization of strong field ionization, which depends both on nonadiabaticity of the process and the principal quantum number of the target. Together with Reiss and Keldysh parameters, this dimensionless parameter expands the description of strong field ionization across a broad range of atomic targets and incorporates ionization from excited states.

74 ATOMIC AND MOLECULAR PHYSICS↗

Dissecting subcycle interference in photoelectron holography

Multipath holographic interference in strong-field quantum tunnel ionization is key to revealing subangstrom attosecond dynamics for molecular movies. This critical subcycle motion is often obscured by longer timescale effects such as ring-shaped patterns that appear in above-threshold ionization (ATI). In the present work, we overcome this problem by combining two techniques in theory and experimental analysis: unit-cell averaging and time-filtering data and simulations. Together these suppress ATI rings and enable an unprecedented highly detailed quantitative match between strong-field ionization experiments in argon and the Coulomb-quantum orbit strong-field approximation (CQSFA) theory. Velocity map images reveal fine modulations on the holographic spiderlike interference fringes that form near the polarization axis. CQSFA theory traces this to the interference of three types of electron pathways. The level of agreement between experiment and theory allows sensitive determination of quantum phase differences and symmetries, providing an important tool for quantitative dynamical imaging in quantum systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

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↗

The Kinetic-Energy–Momentum–Mass 5-Flux of a Baryon Fluid in Bargmann Spacetimes

A Bargmann spacetime is a constrained five-dimensional setting that, while introducing no new physical degrees of freedom beyond those of ordinary four-dimensional spacetime, permits Galilei physics to be expressed with a tensor formalism that respects the distinction between mass and energy while affording the conceptual and technical advantages of a spacetime metric. This framework offers a route to a strong-field ‘Galilei general relativity’ approximating the usual Poincaré general relativity introduced by Einstein. In preparation for modeling core-collapse supernovae, where such an approximation would be useful, this work generalizes the kinetic-energy–momentum–mass 5-flux 𝒯 and its associated spacetime tensor law from a simple fluid of constant particle mass to a baryon fluid whose multiple nuclear species can interconvert rest mass and internal energy. The spacetime tensor law on Bargmann–Galilei spacetime 𝐵𝒢 and its decompositions relative to comoving (‘Lagrangian’) and fiducial (‘Eulerian’) observers are derived in detail. The formalism is rendered more suitable for core-collapse supernova modeling by an extension from strict 𝐵𝒢 to a regime that might be denoted as 𝐵𝒢+: microscopically Poincaré yet macroscopically Galilei. This extension accommodates energy generation by nuclear composition changes and allows comoving energy density and pressure to contribute relative to mass density, while preserving the simplifications of Galilei bulk fluid flow and the streamlined geometry governed by the Bargmann–Galilei spacetime metric.

Cardall, Christian [ORNL] (ORCID:000000020086105X)↗

Strong-field nonsequential double photoionization using virtual-detector theory with path summation

We present an ab initio study of the nonsequential strong-field ionization dynamics of a model two-electron atom with helium character. Single- and double-ionization events are characterized and displayed using detector signals extracted at different points in the two-electron two-dimensional space. The double photoelectron momentum distribution is calculated via coherent path-summation over virtual-particle trajectories. A comparison is made between the momentum distributions obtained with the virtual-detector method, the Schrödinger wave function, and the time-dependent surface flux method developed by Tao and Scrinzi [New J. Phys. 14, 013021 (2012)]. Insights into different ionization and electron recollision pathways are gained from detailed virtual-particle tracking and energy-time readouts. Furthermore, this study demonstrates the extension of virtual-detector theory to strong-field multielectron quantum dynamics and highlights the importance of the evolving quantum phase in quasiclassical electron propagation.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Measuring signatures in photon angular spectra to distinguish nonlinear Compton scattering models

The collision of a high-energy electron beam with a laser pulse may be used to study radiation reaction and nonlinear Compton scattering among many other processes in strong-field quantum electrodynamics. Predictions from simulation and theory for these interactions rely on a number of approximations and assumptions that have not been experimentally tested. Here, experimentally measurable signatures are identified that might be able to distinguish between radiation reaction models, i.e., classical or quantum, or between the local constant field and local monochromatic approximations used to calculate the properties of the nonlinear Compton process. These signatures are considered through Monte Carlo simulations of various experimental conditions that are relevant to today's laser facilities. Potential detection schemes for measuring the signatures are proposed. We find that single-photon counting of keV photons to resolve harmonics and scintillator-based detection of MeV photons may allow us to validate nonlinear Compton scattering models and radiation reaction models respectively. This will require electron beams with divergence angles less than 2 mrad and less than 20% energy spread.

Russell, Brandon K↗

Extracting doubly excited state lifetimes in helium directly in the time domain with attosecond noncollinear four-wave-mixing spectroscopy

The helium atom, with one nucleus and two electrons, is a prototypical system to study quantum many-body dynamics. Doubly excited states, or quantum states in which both electrons are excited by one photon, showcase electronic-correlation mediated effects. In this paper, the natural lifetimes of the doubly excited 1 P o 2 s n p Rydberg series and the 1 S e 2 p 2 dark state in helium in the 60–65 eV region are measured directly in the time domain with extreme-ultraviolet/near-infrared noncollinear attosecond four-wave-mixing (FWM) spectroscopy. The measured lifetimes agree with lifetimes deduced from spectral linewidths and theoretical predictions, and the roles of specific decay mechanisms are considered. While complex spectral line shapes in the form of Fano resonances are common in absorption spectroscopy of autoionizing states, the background-free and thus homodyned character of noncollinear FWM results exclusively in Lorentzian spectral features in the absence of strong-field effects. The onset of strong-field effects that would affect the extraction of accurate natural lifetimes in helium by FWM is determined to be approximately 0.3 Rabi cycles. This study provides a systematic understanding of the FWM parameters necessary to enable accurate lifetime extractions, which can be utilized in more complex quantum systems in the future. Published by the American Physical Society 2024

Rupprecht, Patrick (ORCID:000000026491793X)↗

Laser-induced electron diffraction of the ultrafast umbrella motion in ammonia

Visualizing molecular transformations in real-time requires a structural retrieval method with Ångström spatial and femtosecond temporal atomic resolution. Imaging of hydrogen-containing molecules additionally requires an imaging method sensitive to the atomic positions of hydrogen nuclei, with most methods possessing relatively low sensitivity to hydrogen scattering. Laser-induced electron diffraction (LIED) is a table-top technique that can image ultrafast structural changes of gas-phase polyatomic molecules with sub-Ångström and femtosecond spatiotemporal resolution together with relatively high sensitivity to hydrogen scattering. Here, we image the umbrella motion of an isolated ammonia molecule (NH3) following its strong-field ionization. Upon ionization of a neutral ammonia molecule, the ammonia cation (NH3+) undergoes an ultrafast geometrical transformation from a pyramidal (ΦHNH=107°) to planar (ΦHNH=120°) structure in approximately 8 femtoseconds. Using LIED, we retrieve a near-planar (ΦHNH=117 ± 5°) field-dressed NH3+ molecular structure 7.8−9.8 femtoseconds after ionization. Our measured field-dressed NH3+ structure is in excellent agreement with our calculated equilibrium field-dressed structure using quantum chemical ab initio calculations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Multi-Particle Three-Dimensional Covariance Imaging: “Coincidence” Insights into the Many-Body Fragmentation of Strong-Field Ionized D 2 O

We demonstrate the applicability of covariance analysis to three-dimensional velocity-map imaging experiments using a fast timestamping detector. Studying the photofragmentation of strong-field doubly ionized D$_2$O molecules, we show that combining high count rate measurements with covariance analysis yields the same level of information typically limited to the `gold standard' of true, low count rate coincidence experiments, when averaging over a large ensemble of photofragmentation events. This increases the effective data acquisition rate by approximately two orders of magnitude, enabling a new class of experimental studies. This is illustrated through an investigation into the dependence of three-body D$_2$O$^{2+}$ dissociation on the intensity of the ionizing laser, revealing mechanistic insights into the nuclear dynamics driven during the laser pulse. Here, the experimental methodology laid out, with its drastic reduction in acquisition time, is expected to be of great benefit to future photofragment imaging studies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Femtosecond Nonadiabatic Confinement of Molecular Dication Yield

Doubly charged molecular cations often carry signatures of electronic correlation and electron–nuclear entanglement present in the parent cation. Here, we produce ethylene dications using a combination of an extreme ultraviolet pump and near-infrared probe pulses, observing a peak in the dication yield at a pump–probe delay of approximately 15 fs. Ab-initio calculations, which explicitly take into account coupled electron–nuclear dynamics induced by the pump and the multiphoton nature of the probe-induced ionization step, reproduced the observed delay in the yield. It originates from resonant enhancement of the multiphoton ionization of the electronically excited ethylene cation as the carbon–carbon double bond expands. However, this effect is tempered by rapid nonadiabatic relaxation of the excited ionic states. Our results suggest a general mechanism whereby ultrafast nonadiabatic relaxation of a molecular ion can compete with its strong-field ionization rate, confining the dication yield to a narrow temporal window of a few femtoseconds.

74 ATOMIC AND MOLECULAR PHYSICS↗

Single particle detection system for strong-field QED experiments

Abstract Measuring signatures of strong-field quantum electrodynamics (SF-QED) processes in an intense laser field is an experimental challenge: it requires detectors to be highly sensitive to single electrons and positrons in the presence of the typically very strong x-ray and γ -photon background levels. In this paper, we describe a particle detector capable of diagnosing single leptons from SF-QED interactions and discuss the background level simulations for the upcoming Experiment-320 at FACET-II (SLAC National Accelerator Laboratory). The single particle detection system described here combines pixelated scintillation LYSO screens and a Cherenkov calorimeter. We detail the performance of the system using simulations and a calibration of the Cherenkov detector at the ELBE accelerator. Single 3 GeV leptons are expected to produce approximately 537 detectable photons in a single calorimeter channel. This signal is compared to Monte-Carlo simulations of the experiment. A signal-to-noise ratio of 18 in a single Cherenkov calorimeter detector is expected and a spectral resolution of 2% is achieved using the pixelated LYSO screens.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

All-electron molecular tunnel ionization based on the weak-field asymptotic theory in the integral representation

Tunnel ionization (TI) underlies many important ultrafast processes, such as high-harmonic generation andstrong-field ionization. Among the existing theories for TI, many-electron weak-field asymptotic theory (ME-WFAT) is by design capable of accurately treating many-electron effects in TI. An earlier version of ME-WFATrelied on an accurate representation of the asymptotic tail of the orbitals, which hindered its implementation inGaussian-basis-set-based quantum chemistry programs. In this work, we reformulate ME-WFAT in the integralrepresentation, which makes the quality of the asymptotic tail much less critical, hence greatly facilitating itsimplementation in standard quantum chemistry packages. The integral reformulation introduced here is thereforemuch more robust when applied to molecules with arbitrary geometry. Here, we present several case studies, amongwhich is the CO molecule where some earlier theories disagree with experiments. Here we find that ME-WFATproduces the largest ionization probability when the field points from C to O, as experiments suggest. Anattractive feature of ME-WFAT is that it can be used with various types of multielectron methods whether ofdensity functional or multiconfiguration types, this inturn facilitates tunnel ionization calculation in systems exhibiting a strong multireference character.

74 ATOMIC AND MOLECULAR PHYSICS↗