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Hongcheng Ni

Publications and source records attributed to Hongcheng Ni.

16 recordsLinked to original sources

Nonlinear atomic tunnelling boosted by bright squeezed vacuum

Nonlinear optical processes, mediated by multiphoton interactions rather than single-photon response, are routinely exploited to enable a range of light-based functionalities in devices and applications. Nonlinear effects are enhanced through higher intensity fields, which is a limiting strategy owing to potential radiation damage. An alternative strategy relies on the fluctuation redistribution typical of quantum light, but experimental demonstrations at the most fundamental level have been limited. Here we report experimental nonlinear tunnelling ionization of isolated atoms, a pivotal nonlinear process that drives high-harmonic generation and forms the basis of attosecond science, boosted by quantum light -- bright squeezed vacuum (BSV). A BSV light with an average pulse energy of 300 nJ achieves an effective intensity equivalent to that of a coherent light with 7.1 {\textmu}J, demonstrating a more than 20-fold quantum boost in nonlinear effect from BSV light. This boost is revealed by matching the peaks of the photoelectron momentum spectra produced by the BSV and coherent light using angular streaking. Furthermore, we demonstrate control of the effective intensity of the BSV by tuning the correlation function at fixed average pulse energy, establishing a robust method to tailor nonlinear processes via quantum statistics rather than classical intensity scaling. These findings may facilitate the development of quantum-controlled strong-field dynamics using tailored quantum light sources.

quant-ph

Over-Barrier Ionization Dynamics Studied by Backpropagation

Tunneling and over-barrier ionization are the primary processes of strong-field ionization of atoms and molecules. While the dynamics of tunneling ionization have been extensively studied, exploration of over-barrier ionization dynamics has remained a significant challenge. In this study, we investigate the dynamics of over-barrier ionization using the backpropagation method specifically adapted for this context. By analyzing the topology of the backpropagating trajectories, we differentiate the contributions of tunneling and over-barrier ionizations to the distributions of photoelectron momentum and ionization time. While the transition from tunneling to over-barrier ionization is known to depend on the field strength, our results reveal that it is also influenced by the initial transverse momentum of the outgoing electron. We clarify how ionization probabilities vary with intensity for each mechanism, highlighting a competitive relationship between them. We further find that accounting for the Stark shift is essential for accurately determining the threshold field strength for over-barrier ionization. Our work provides a detailed understanding of the dynamics of over-barrier ionization and lays the groundwork for exploring new mechanisms in intense laser-matter interactions.

physics.atom-ph

eTraj.jl: Trajectory-Based Simulation for Strong-Field Ionization

The dynamics of light-matter interactions in the realm of strong-field ionization has been a focal point and has attracted widespread interest. We present the eTraj.jl program package, designed to implement established classical/semiclassical trajectory-based methods to determine the photoelectron momentum distribution resulting from strong-field ionization of both atoms and molecules. The program operates within a unified theoretical framework that separates the trajectory-based computation into two stages: initial-condition preparation and trajectory evolution. For initial-condition preparation, we provide several methods, including the Strong-Field Approximation with Saddle-Point Approximation (SFA-SPA), SFA-SPA with Non-adiabatic Expansion (SFA-SPANE), and the Ammosov-Delone-Krainov theory (ADK), with atomic and molecular variants, as well as the Weak-Field Asymptotic Theory (WFAT) for molecules. For trajectory evolution, available options are Classical Trajectory Monte-Carlo (CTMC), which employs purely classical electron trajectories, and the Quantum Trajectory Monte-Carlo (QTMC) and Semi-Classical Two-Step model (SCTS), which include the quantum phase during trajectory evolution. The program is a versatile, efficient, flexible, and out-of-the-box solution for trajectory-based simulations for strong-field ionization. It is designed with user-friendliness in mind and is expected to serve as a valuable and powerful tool for the community of strong-field physics.

physics.atom-ph

Attosecond Ionization Time Delays in Strong-Field Physics

Electronic processes within atoms and molecules reside on the timescale of attoseconds. Recent advances in the laser-based pump-probe interrogation techniques have made possible the temporal resolution of ultrafast electronic processes on the attosecond timescale, including photoionization and tunneling ionization. These interrogation techniques include the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. While the former two are usually employed to study photoionization processes, the latter is typically used to investigate tunneling ionization. In this Topical Review, we briefly overview these timing techniques towards an attosecond temporal resolution of ionization processes in atoms and molecules under intense laser fields. In particular, we review the backpropagation method, which is a novel hybrid quantum-classical approach towards full characterization of tunneling ionization dynamics. Continued advances in the interrogation techniques promise to pave the pathway towards the exploration of ever faster dynamical processes on an ever shorter timescale.

physics.atom-ph

PyStructureFactor: A Python code for the molecular structure factor in tunneling ionization rates

Tunneling ionization is at the core of strong-field and attosecond science. In this paper, we present PyStructureFactor - a general Python code towards the calculation of the structure factor in the tunneling ionization rate of common molecules under intense laser fields. The numerical implementation is based on the well-developed weak-field asymptotic theory in the integral representation. The information of the electronic structure of the molecules is obtained via the PySCF quantum chemistry package. PyStructureFactor is a general computational framework that can be utilized to compute the molecular structure factor of various types of molecules, including polar and non-polar diatomic molecules, degenerate molecules, and open-shell molecules. Examples are given that are benchmarked against known results with good agreements. The present PyStructureFactor is implemented in an efficient manner and is easily applicable towards larger molecules.

physics.atom-ph

Instantaneous Quasiphoton in Strong-Field Ionization

Photon is a concept that does not apply at the instantaneous level when light is described by classical electromagnetic fields. Exploiting the dynamical rotational symmetry of circularly or elliptically polarized classical light pulses, however, we demonstrate the existence of instantaneous quasiphotons down to the subcycle level. We illustrate the concept of quasiphotons in strong-field ionization through the correlated spectrum of angular momentum and energy of photoelectrons, both at the tunnel exit and in the asymptotic region. Moreover, we propose a protocol based on electron vortices to directly visualize the existence of quasiphotons. Our work paves the pathway towards a deeper understanding of fundamental light-matter interactions with photonic characteristics on the subcycle scale.

physics.atom-ph

Ionization Induced by the Ponderomotive Force in Intense and High-Frequency Laser Fields

Atomic stabilization is a universal phenomenon that occurs when atoms interact with intense and high-frequency laser fields. In this work, we systematically study the influence of the ponderomotive (PM) force, present around the laser focus, on atomic stabilization. We show that the PM force could induce tunneling and even over-barrier ionization to the otherwise stabilized atoms. Such effect may overweight the typical multiphoton ionization under moderate laser intensities. Our work highlights the importance of an improved treatment of atomic stabilization that includes the influence of the PM force.

physics.atom-ph

Wave-Packet Surface Propagation for Light-Induced Molecular Dissociation

Recent advances in laser technology have enabled tremendous progress in photochemistry, at the heart of which is the breaking and formation of chemical bonds. Such progress has been greatly facilitated by the development of accurate quantum-mechanical simulation method, which, however, does not necessarily accompany clear dynamical scenarios and is rather often a black box, other than being computationally heavy. Here, we develop a wave-packet surface propagation (WASP) approach to describe the molecular bond-breaking dynamics from a hybrid quantum-classical perspective. Via the introduction of quantum elements including state transitions and phase accumulations to the Newtonian propagation of the nuclear wave-packet, the WASP approach naturally comes with intuitive physical scenarios and accuracies. It is carefully benchmarked with the H2+ molecule and is shown to be capable of precisely reproducing experimental observations. The WASP method is promising for the intuitive visualization of strong-field molecular dynamics and is straightforwardly extensible toward complex molecules.

physics.chem-ph

Subcycle resolved strong-field tunneling ionization: Identification of magnetic dipole and electric quadrupole effects

Interaction of a strong laser pulse with matter transfers not only energy but also linear momentum of the photons. Recent experimental advances have made it possible to detect the small amount of linear momentum delivered to the photoelectrons in strong-field ionization of atoms. Linear momentum transfer is a unique signature of the laser-atom interaction beyond its dipolar limit. Here, we present a decomposition of the subcycle time-resolved linear momentum transfer in term of its multipolar components. We show that the magnetic dipole contribution dominates the linear momentum transfer during the dynamical tunneling process while the post-ionization longitudinal momentum transfer in the field-driven motion of the electron in the continuum is primarily governed by the electric quadrupole interaction. Alternatively, exploiting the radiation gauge, we identify nondipole momentum transfer effects that scale either linearly or quadratically with the coupling to the laser field. The present results provide detailed insights into the physical mechanisms underlying the subcycle linear momentum transfer induced by nondipole effects.

physics.atom-ph

Zeptosecond Angular Streak Camera

Time-resolved electronic processes on the attosecond scale have recently become experimentally accessible through the development of laser-based pump-probe interrogation techniques such as the attosecond streak camera, the reconstruction of attosecond beating by interference of two-photon transitions, and the attoclock. In this work, we demonstrate that by combining the concepts of the attosecond streak camera and the attoclock, time resolved processes down to the time scale of tens of zeptoseconds come into reach. Key to advancing to this remarkable level of time precision by this method termed the zeptosecond angular streak camera (ZASC) is its substantial intrinsic time-information redundancy. The ZASC results in a remarkably simple streaking trace, which is largely independent of the precise temporal structure of the streaking pulse, thereby bypassing the need for detailed characterization of the streaking field. Moreover, it is capable of retrieving information on the duration of the pump pulse. It is also capable of reaching attosecond-level precision in a single-shot mode that may be useful for free-electron-laser experiments. This concept promises to open pathways towards the chronoscopy of zeptosecond-level ultrafast processes.

physics.atom-ph

Magnetic-field effect in high-order above-threshold ionization

We experimentally and theoretically investigate the influence of the magnetic component of an electromagnetic field on high-order above-threshold ionization of xenon atoms driven by ultrashort femtosecond laser pulses. The nondipole shift of the electron momentum distribution along the light-propagation direction for high energy electrons beyond the classical cutoff is found to be vastly different from that below the cutoff. A V-shape structure in the momentum dependence of the nondipole shift above the cutoff is identified for the first time. With the help of classical and quantum-orbit analysis, we show that large-angle rescattering of the electrons strongly alters the partitioning of the photon momentum between electron and ion. The sensitivity of the observed nondipole shift to the electronic structure of the target atom is confirmed by three-dimensional time-dependent Schrödinger equation simulations for different model potentials.

physics.atom-ph

Quantum Battles in Attoscience -- Tunnelling

What is the nature of tunnelling? This yet unanswered question is as pertinent today as it was at the dawn of quantum mechanics. This article presents a cross section of current perspectives on the interpretation, computational modelling, and numerical investigation of tunnelling processes in attosecond physics as debated in the Quantum Battles in Attoscience virtual workshop 2020.

quant-ph

Theory of Subcycle Linear Momentum Transfer in Strong-Field Tunneling Ionization

Interaction of a strong laser pulse with matter transfers not only energy but also linear momentum of the photons. Recent experimental advances have made it possible to detect the small amount of linear momentum delivered to the photoelectrons in strong-field ionization of atoms. We present numerical simulations as well as an analytical description of the subcycle phase (or time) resolved momentum transfer to an atom accessible by an attoclock protocol. We show that the light-field-induced momentum transfer is remarkably sensitive to properties of the ultrashort laser pulse such as its carrier-envelope phase and ellipticity. Moreover, we show that the subcycle resolved linear momentum transfer can provide novel insights into the interplay between nonadiabatic and nondipole effects in strong-field ionization. This work paves the way towards the investigation of the so-far unexplored time-resolved nondipole nonadiabatic tunneling dynamics.

physics.atom-ph

Polarization tagging of two-photon double ionization by elliptically polarized XUVs

We explore the influence of elliptical polarization on the (non)sequential two-photon double ionization of atomic helium with ultrashort extreme ultraviolet (XUV) light fields using time-dependent full ab-initio simulations. The energy and angular distributions of photoelectrons are found to be strongly dependent on the ellipticity. The correlation minimum in the joint angular distribution becomes more prominently visible with increasing ellipticity. In a pump-probe sequence of two subsequent XUV pulses with varying ellipticities, polarization tagging allows to discriminate between sequential and nonsequential photoionization. This clear separation demonstrates the potential of elliptically polarized XUV fields for improved control of electronic emission processes.

physics.atom-ph

Numerical simulation of time delays in light induced ionization

We apply a fundamental definition of time delay, as the difference between the time a particle spends within a finite region of a potential and the time a free particle spends in the same region, to determine results for photoionization of an electron by an extreme ultraviolet (XUV) laser field using numerical simulations on a grid. Our numerical results are in good agreement with those of the Wigner-Smith time delay, obtained as the derivative of the phase shift of the scattering wave packet with respect to its energy, for the short-range Yukawa potential. In case of the Coulomb potential we obtain time delays for any finite region, while - as expected - the results do not converge as the size of the region increases towards infinity. The impact of an ultrashort near-infrared probe pulse on the time delay is analyzed for both the Yukawa as well as the Coulomb potential and is found to be small for intensities below $10^{13}$ W/cm$^2$.

physics.atom-ph

Theoretical analysis of time delays and streaking effects in XUV photoionization

We apply a recently proposed theoretical concept and numerical approach to obtain time delays in extreme ultraviolet (XUV) photoionization of an electron in a short- or long-range potential. The results of our numerical simulations on a space-time grid are compared to those for the well-known Wigner-Smith time delay and different methods to obtain the latter time delay are reviewed. We further use our numerical method to analyze the effect of a near-infrared streaking field on the time delay obtained in the numerical simulations.

physics.atom-ph