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Xinhua Xie

Publications and source records attributed to Xinhua Xie.

At least 19 recordsLinked to original sources

Dichography: Two-frame Ultrafast Imaging from a Single Diffraction Pattern

We experimentally demonstrate that pairs of time-delayed ultrabright and ultrashort X-ray pulses of two different colors, delivered by modern X-ray Free Electron Lasers, can provide two time-delayed snapshots of a sample. We introduce Dichography, a method that algorithmically separates the diffraction signals overlapping on the detector and independently retrieves the two images of the specimen. We employ Dichography to reconstruct two views of individual xenon-doped helium nanodroplets with 20 nm spatial resolution. The consistency of structures observed in both images at delays up to 750 fs provides evidence that, under these illumination conditions, significant structural damage only occurs at longer timescales. We further validate the method by imaging pairs of silver nanoparticles intercepted by the same light pulse. Dichography enables a new class of experiments across physics, chemistry, and materials science, making a significant step toward the original promise of X-ray free-electron lasers to capture ultrafast movies of nanomatter.

physics.optics↗

Electron Orbital Angular Momentum Polarization in Neutral Atoms

We demonstrate the polarization of electron orbital angular momentum (OAM) in neutral atoms by integrating the Zeeman effect with attosecond transient absorption spectroscopy (ATAS). Using density matrix simulations, we show that in a helium atom, the absorption probability asymmetry between mj=-1 and mj = 1 in the 1s2p state can be precisely controlled by adjusting the time delay between infrared (IR) and extreme ultraviolet (XUV) fields, the strength of an applied static magnetic field, as well as the angle between laser polarization and magnetic field direction. This approach has significant implications across various fields, including quantum computing, quantum communication, and spintronics. Moreover, it paves the way for advancements in applications such as manipulating chemical reactions control, tailoring the magnetic properties of matter, and enabling novel laser emissions.

physics.atom-ph↗

Strong-Field-Assisted X-ray Second Harmonic Generation

We theoretically demonstrate x-ray second harmonic generation (SHG) with strong-field-driven high harmonic generation (HHG) from core electrons in gas-phase atoms, highlighting its potential as a powerful spectroscopic tool for studying atomic and molecular systems. Our simulations confirm the generation of HHG with x-ray SHG (HHG-XSHG) from atomic core electrons through the rescattering of electrons from x-ray two-photon excitation and subsequent tunneling ionization in an optical laser field. The resulting HHG-XSHG spectrum features a broadband multi-peak structure and a distinct spectral cutoff in the x-ray regime. These findings indicate that HHG-XSHG is a valuable technique for probing core-electron dynamics, generating attosecond x-ray pulses, and exploring nonlinear interactions, effectively merging laser-driven attosecond technology with nonlinear x-ray methodologies provided by x-ray free-electron lasers.

physics.atom-ph↗

Resolving Rydberg-Electron Recapture Dynamics via Laser-driven Frustrated Tunneling Ionization

By employing two-color counter-rotating circularly polarized laser fields, we investigate the dynamics of electron recapture into Rydberg states under strong, ultrashort laser pulses, probed via coherent extreme-ultraviolet free-induction decay (XFID). Our study reveals significant distinctions between XFID and above-threshold high-order harmonic generation in terms of their ellipticity dependence on the driving-laser waveforms, yield variations with the laser-intensity ratios, and sensitivity to the driving-laser ellipticity. All these differences arise from the fundamentally distinct electron trajectories underlying the two processes. More importantly, our findings provide compelling evidence that Rydberg-electron recapture predominantly occurs at the end of the driving laser field, offering the first direct experimental confirmation of this long-proposed mechanism.

physics.optics↗

Coherent all X-ray four wave mixing at core shell resonances

Nonlinear wave mixing in the X-ray range can provide valuable insights into the structural and electron dynamics of atomic and molecular systems on ultrafast time scales, with state- and site-selectivity and atomic resolution. This promising experimental toolbox was so far limited by requiring at least one near-visible laser, thus preventing core-shell two-dimensional X-ray spectroscopy. In this work, we demonstrate the generation of background-free all-X-ray four-wave mixing (XFWM) signals from a dilute gaseous sample (Ne). The measured and simulated two-dimensional spectral maps ($ω_{\text{in}},ω_{\text{out}}$) show multiple contributions involving the coherent response from core electrons. Notably, two-color resonant XFWM signals, essential for generalized multi-color schemes that allow to locally probe the electronic excitation of matter, are observed in neutral Ne. Moreover, stimulated Ne$^+$ emission in each of the propagating X-ray pulses leads to an increase of the temporal coherence in a narrow-bandwidth, which results in the coherent mixing of three X-ray lasers. Preliminary X-ray excitation experiments making use of multi-color time-delayed X-ray pulses demonstrate temporal resolution capability and show a time dependency consistent with a signal dominated by resonant XFWM processes. This first all-X-ray four-wave-mixing approach represents a major breakthrough towards multidimensional X-ray correlation spectroscopy and the general application of nonlinear all-X-ray wave-mixing.

physics.optics↗

Hyper Spectral Resolution Stimulated Raman Spectroscopy with Amplified fs Pulse Bursts

We present a novel approach to achieve hyper spectral resolution, high sensitive detection, and high speed data acquisition Stimulated Raman Spectroscopy by employing amplified offset-phase controlled fs-pulse bursts. In this approach, the Raman-shift spectrum is obtained through the direct mapping between the bursts offset phase and the Raman-shift frequency, which requires neither wavelength-detuning as in the long-pulse method nor precise dispersion management and delay scanning with movable parts as in the spectral focusing technique. This method is demonstrated numerically by solving the coupled non-linear Schroedinger equations and the properties of this approach are systematically investigated. The product of the spectral resolution and the pixel dwell time in this work is below 2 microsiemens/centimeter, which is at least an order of magnitude lower than previous methods. This previously untouched area will greatly expand the applications of SRS and holds the potential for discovering new science.

physics.optics↗

Exploring photoelectron angular distributions emitted from molecular dimers by two delayed intense laser pulses

We describe the results of experiments and simulations performed with the aim of extending photoelectron spectroscopy with intense laser pulses to the case of molecular compounds. Dimer frame photoelectron angular distributions generated by double ionization of N$_2$-N$_2$ and N$_2$-O$_2$ van der Waals dimers with ultrashort, intense laser pulses are measured using four-body coincidence imaging with a reaction microscope. To study the influence of the first-generated molecular ion on the ionization behavior of the remaining neutral molecule we employ a two-pulse sequence comprising of a linearly polarized and a delayed elliptically polarized laser pulse that allows distinguishing the two ionization steps. By analysis of the obtained electron momentum distributions we show that scattering of the photoelectron on the neighbouring molecular potential leads to a deformation and rotation of the photoelectron angular distribution as compared to that measured for an isolated molecule. Based on this result we demonstrate that the electron momentum space in the dimer case can be separated, allowing to extract information about the ionization pathway from the photoelectron angular distributions. Our work, when implemented with variable pulse delay, opens up the possibility of investigating light-induced electronic dynamics in molecular dimers using angularly resolved photoelectron spectroscopy with intense laser pulses.

physics.chem-ph↗

Photoelectron spectroscopy of laser-dressed atomic helium

Photoelectron emission from excited states of laser-dressed atomic helium is analyzed with respect to laser intensity-dependent excitation energy shifts and angular distributions. In the two-color XUV (exteme ultra\-violet) -- IR (infrared) measurement, the XUV photon energy is scanned between \SI{20.4}{\electronvolt} and the ionization threshold at \SI{24.6}{\electronvolt}, revealing electric dipole-forbidden transitions for a temporally overlapping IR pulse ($\sim\!\SI{e12}{\watt\per \centi\meter\squared}$). The interpretation of the experimental results is supported by numerically solving the time-dependent Schrödinger equation in a single-active-electron approximation.

physics.atom-ph↗

Laser-induced Electron-Transfer in the Dissociative Multiple Ionization of Argon Dimers

We report on an experimental and theoretical study of the ionization-fragmentation dynamics of argon dimers in intense few-cycle laser pulses with a tagged carrier-envelope phase. We find that a field-driven electron transfer process from one argon atom across the system boundary to the other argon atom triggers sub-cycle electron-electron interaction dynamics in the neighboring atom. This attosecond electron-transfer process between distant entities and its implications manifest themselves as a distinct phase-shift between the measured asymmetry of electron emission curves of the $\text{Ar}^{+}+\text{Ar}^{2+}$ and $\text{Ar}^{2+}+\text{Ar}^{2+}$ fragmentation channels. Our work discloses a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving inter-molecular electron-transfer processes.

physics.atm-clus↗

Generalized phase-sensitivity of directional bond-breaking in laser-molecule interaction

We establish a generalized picture of the phase-sensitivity of laser-induced directional bond-breaking using the H$_2$ molecule as the example. We show that the well-known proton ejection anisotropy measured with few-cycle pulses arises as an amplitude-modulation of an intrinsic anisotropy that is sensitive to the laser phase at the ionization time and determined by the molecule's electronic structure. Our work furthermore reveals a strong electron-proton correlation that may open up a new approach to experimentally accessing the laser-sub-cycle intramolecular electron dynamics also in large molecules.

physics.chem-ph↗

Experimental Separation of Sub-Cycle Ionization Bursts in Strong-Field Double Ionization of H$_2$

We report on the unambiguous observation of the sub-cycle ionization bursts in sequential strong-field double ionization of H$_2$ and their disentanglement in molecular frame photoelectron angular distributions. This observation was made possible by the use of few-cycle laser pulses with a known carrier-envelope phase in combination with multi-particle coincidence momentum imaging. The approach demonstrated here will allow sampling of the intramolecular electron dynamics and the investigation of charge-state specific Coulomb-distortions on emitted electrons in polyatomic molecules.

physics.chem-ph↗

Sub-femtosecond tracing of molecular dynamics during strong-field interaction

We introduce and experimentally demonstrate a method, where the two intrinsic time scales of a molecule, the slow nuclear motion and the fast electronic motion, are simultaneously measured in a photo-electron photo-ion coincidence experiment. In our experiment, elliptically polarized, 750~nm, 4.5~fs laser pulses were focused to an intensity of $9\times10^{14}\mathrm{W/cm}^2$ onto H$_2$. Using coincidence imaging, we directly observe the nuclear wavepacket evolving on the \ssg{} state of H$_2^+$ during its first roundtrip with attosecond temporal and picometer spatial resolution. The demonstrated method should enable insight into the first few femtoseconds of the vibronic dynamics of ionization-induced unimolecular reactions of larger molecules.

physics.chem-ph↗

Laser-Induced Dissociative Recombination of Carbon Dioxide

We experimentally investigate laser-induced dissociative recombination of CO$_2$ in linearly polarized strong laser fields with coincidence measurements. Our results show laser-induced dissociation processes originate from an electron recombination process after laser-induced double ionization. After double ionization of CO$_2$, one electron is recaptured by the CO$_2^{2+}$ and localized to O$^+$ or CO$^+$ in the following dissociation process. We found that the probability of electron localization to O$^{+}$ is much higher than that to CO$^+$. Further, our measurements reveal that the recombination probability of the first ionized electron is three times as high as that of the second ionized electron. Our work may trigger further experimental and theoretical studies on involved nuclear and electron dynamics in laser-induced dissociative recombination of molecules and their applications in controlling molecular dissociation with ultrashort laser pulses.

physics.chem-ph↗

Zero-energy proton dissociation of H$_2^+$ through stimulated Raman scattering

We show that (near-)zero energy proton emission from H$_2^+$ in strong two-color and broadband laser fields is dominated by a stimulated Raman scattering process taking place on the electronic ground state. It is furthermore shown that in the (near-)zero energy region the asymmetry in proton ejection induced by asymmetric laser fields is due to the interplay of several processes, rather than only pathway interferences, with vibrational trapping (or bond-hardening) taking a key role.

physics.chem-ph↗

Frustrated Double Ionization of Argon Atoms in Strong Laser Fields

We demonstrate kinematically complete measurements on frustrated double ionization of argon atoms in strong laser fields with a reaction microscope. We found that the electron trapping probability after strong field double ionization is much higher than that after strong field single ionization, especially in case of high laser intensity. The retrieved electron momentum distributions of frustrated double ionization show a clear transition from the nonsequential to the sequential regime, similar to those of strong field double ionization. The dependence of electron momentum width on the laser intensity further indicates that the second released electron has a dominant contribution to frustrated double ionization in the sequential regime.

physics.atom-ph↗

Disentangling intra-cycle interferences in photoelectron momentum distributions using orthogonal two-colour laser fields

We use orthogonally polarized two-colour (OTC) laser pulses to separate quantum paths in multiphoton ionization of Ar atoms. Our OTC pulses consist of 400~nm and 800~nm light at a relative intensity ratio of 10:1. We find a hitherto unobserved interference in the photoelectron momentum distribution, which exhibits a strong dependence on the relative phase of the OTC pulse. Analysis of model calculations reveal that the interference is caused by quantum pathways from non-adjacent quarter cycles.

physics.atom-ph↗

Localizing High-Lying Rydberg Wave Packets with Two-Color Laser Fields

We demonstrate control over the localization of high-lying Rydberg wave packets in argon atoms with phase-locked orthogonally polarized two-color (OTC) laser fields. With a reaction microscope, we measured ionization signals of high-lying Rydberg states induced by a weak dc field and black-body radiation as a function of the relative phase between the two-color fields. We find that the dc-field ionization yields of high-lying Rydberg argon atoms oscillate with the relative two-color phase with a period of $2π$ while the photoionization signal by black-body radiation shows a period of $π$. These observations are a clear signature of the asymmetric localization of electrons recaptured into high-lying Rydberg states after conclusion of the laser pulse and are supported by a semiclassical simulation of argon-OTC laser interaction. Our findings thus open an effective pathway to control the localization of high-lying Rydberg wave packets.

physics.atom-ph↗

Channel-resolved subcycle interferences of electron wave packets emitted from H$_2$ in two-color laser fields

We report on the observation of subcycle interferences of electron wave packets released during the strong field ionization of H$_2$ with cycle-shaped two-color laser fields. With a reaction microscope, channel-resolved photoelectron momentum distribution are obtained for different final products originating from single ionization of H$_2$. Our results show that the subcycle interference structures of electron wave packet are very sensitive to the cycle-shape of the two-color laser field. The reason is that the ionization time within an optical cycle is determined by the cycle-shape of the laser field. The subcycle interference structures can be further used to get the subcycle dynamics of molecules during strong field interaction.

physics.chem-ph↗