We theoretically investigate the effects of laser polarization on photoelectron angular distribution through laser-induced continuum structure. We focus on a polarization geometry where the probe and dressing lasers are both linearly polarized, and change the relative polarization angle between them. We find that the total ionization yield and the branching ratio into different ionization channels change as a function of the relative polarization angle, and accordingly the photoelectron angular distribution is altered. We present specific results for the $4p_{1/2}$-$6p_{1/2}$ and $4p_{3/2}$-$6p_{3/2}$ systems of the K atom, and show that the change of the polarization angle leads to the significant modification of photoelectron angular distribution.
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.
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 t…
We measure the photoelectron energy spectra from strong-field ionization of Kr in a two-color laser pulse consisting of a strong 400-nm field and a weak 800-nm field. The intensities of the main above-threshold ionization (ATI) and sideband peaks in the photoelectron energy spectra oscillate roughly oppositely with respect to the relative phase between the two-color components. We study the photoelectron interferometry in strong-field ATI regime from the view of interference of different electron trajectories in order to extend RABBITT type analysis to the strong-field regime. Based on the str…
We consider atomic strong-field ionization in the long-pulse limit for linearly polarized infrared laser fields. We show how nondipole effects in the plane formed by the propagation and polarization directions lead to (i) a shift of the origin of the rings describing the energetically allowed final electron momenta for individual above-threshold ionization channels and (ii) a redistribution in the continuum population on each ring.
Multiphoton ionization of sodium by laser pulses of 800 nm wavelength and 57 fs duration is studied in the range of laser peak intensities belonging to over-the-barrier ionization regime. Photoelectron momentum distributions (PMD) and the energy spectra are determined numerically by solving the time dependent Schrödinger equation. The calculated spectra agree well with the spectra obtained experimentally by Hart et al. [Phys. Rev. A 93, 063426 (2016)]. The contributions of photoelectrons with different values of the orbital quantum number in the PMD are determined by expanding the photoelectro…
Recent experiments [D. Pengel, S. Kerbstadt, L. Englert, T. Bayer, and M. Wollenhaupt, \href{https://journals.aps.org/pra/abstract/10.1103/PhysRevA.96.043426}{{\PRA} {\bf 96} 043426 (2017)}] have measured the photoelectron momentum distribution for three-photon ionization of potassium by counter-rotating circularly polarized 790-nm laser pulses. The distribution displays spiral vortices, arising from the interference of ionizing wavepackets with different magnetic quantum numbers. The high level of multidimensional detail observed in the distribution makes this an ideal case in which to demons…
The phenomenon of spatial (polar) asymmetry of produced photoelectron emission due to strong-field multiphoton process of above-threshold ionization (ATI) in atoms irradiated by a linearly polarized two-color (bichromatic) laser field consisting of coherent superposition of two commensurate harmonics (of frequencies and is considered and studied theoretically. The problem is addressed within the conventional strong-field approximation (SFA) in standard velocity gauge (VG) formulation under condition of arbitrary value of the so-called Keldysh parameter $γ$ , including both the multiphoton (for…
Photoelectron spectroscopy of 3s3p doubly excited helium dressed with strong near-infrared laser fields
Nagoya University（名古屋大学）；RIKEN, SPring-8 Center（理化学研究所 SPring-8 中心）；Fu-Jen Catholic University（辅仁大学）；Japan Synchrotron Radiation Research Institute（日本同步辐射研究机构）；University of Toyama（富山大学）
Over the last three decades numerous numerical methods for solving the time-dependent Schrödinger equation within the single-active electron approximation have been developed for studying ionization of atomic targets exposed to an intense laser field. In addition, various numerical techniques for extracting the photoelectron spectra from the time-dependent wave function have emerged. In this paper we compare photoelectron spectra obtained by either projecting the time-dependent wave function at the end of the laser pulse onto the continuum state having proper incoming boundary condition or by …
Laser-induced electron tunneling underlies numerous emerging spectroscopic techniques to probe attosecond electron dynamics in atoms and molecules. The improvement of those techniques requires an accurate knowledge of the exit momentum for the tunneling wave packet. Here we demonstrate a photoelectron interferometric scheme to probe the electron momentum longitudinal to the tunnel direction at the tunnel exit by measuring the photoelectron holographic pattern in an orthogonally polarized two-color laser pulse. In this scheme, we use a perturbative 400-nm laser field to modulate the photoelectr…
A novel and universal interference structure is found in the photoelectron momentum distribution of atoms in intense infrared laser field. Theoretical analysis shows that this structure can be attributed to a new form of Coulomb-field-driven backward-scattering of photoelectrons in the direction perpendicular to the laser field, in contrast to the conventional rescattering along the laser polarization direction. This transverse backward-scattering process is closely related to a family of photoelectrons initially ionized within a time interval of less than 200 attosecond around the crest of th…
Photoelectron circular dichroism (PECD) is a fascinating phenomenon both from a fundamental science aspect but also due to its emerging role as a highly sensitive analytic tool for chiral recognition in the gas phase. PECD has been studied with single-photon as well as multi-photon ionization. The latter has been investigated in the short pulse limit with femtosecond laser pulses, where ionization can be thought of as an instantaneous process. In this contribution, we demonstrate that multiphoton PECD still can be observed when using an ultra-violet nanosecond pulse to ionize chiral showcase f…
We calculate two-dimensional photoelectron momentum distributions and energy spectra after multiphoton ionization of Li atoms subject to intense laser fields in one-photon Rabi-flopping regime. The time-dependent Schrödinger equation is solved within the single-active-electron approximation using a model potential which reproduces accurately the binding energies and dipole matrix elements of the Li atom. Interaction with the external electromagnetic field is treated within the dipole approximation. We show that the Rabi oscillations of the population between the ground $2s$ state and the excit…
High-order above-threshold ionization (HATI) spectrum in IR+XUV two-color laser fields has been investigated. We found that the quantum features corresponding to the absorption of the XUV photon is well illustrated by a peculiar dip structure in the second plateau of the HATI spectrum. By the channel analysis, we show that the angular distribution of the spectrum is attributed to the coherent summation over contributions of different channels, and the dip structure in the spectrum is directly related to the absorption of one XUV photon of the ionized electron during the laser-assisted collisio…
Exact Nondipole Kramers-Henneberger Form of the Light-Atom Hamiltonian: An Application to Atomic Stabilization and Photoelectron Energy Spectra
将原子与时空相关激光场相互作用的精确非偶极最小耦合哈密顿量转化为经典自由电子在激光场中的静止坐标系，即，Kramers-Henneberger框架。新形式的哈密顿量被用来研究在高强度，高频率制度的非偶极效应。全三维非偶极{ \it ab initio}波包计算表明，电离几率随场强的增加而减小.我们确定了一个独特的签名，这种动态稳定的影响，在光电子能谱的发病。
Continuum-electron interferometry for enhancement of photoelectron circular dichroism and measurement of bound, free, and mixed contributions to chiral response
We investigate the influence of relativistic nondipole effects on the photoelectron spectra of argon, particularly in the low kinetic energy region (0 eV - 5 eV). In our experiment, we use intense linearly polarised 800 nm laser pulse to ionise Ar from a jet and we record photoelectron energy and momentum distributions using a reaction microscope (REMI). Our measurements show that nondipole effect can cause an energy-dependent asymmetry along the laser propagation direction in the photoelectron energy and momentum spectra. Model simulation based on time-dependent Dirac equation (TDDE) can repr…
Initial-state symmetry has been underappreciated in strong-field spectroscopies, where laser fields dominate the dynamics. We demonstrate numerically that the transverse photoelectron phase structure, arising from this symmetry, is robust in strong-field rescattering, and manifests in strong-field photoelectron spectra. Interpretation of rescattering experiments need to take these symmetry effects into account. In turn, transverse photoelectron phase structures may enable attosecond super-resolution imaging with structured electron beams.
We study ionization dynamics of aligned diatomic molecules N$_2$ in strong elliptical laser fields experimentally and theoretically. The alignment dependence of photoelectron momentum distributions (PMDs) of N$_2$ measured in experiments is highlighted with comparing to Ar measured synchronously. Our results show that the PMDs of N$_2$ depend strongly on the alignment of the molecule, relative to the main axis of the laser ellipse. In particular, the most-probable electron-emission angle which is often used in attosecond measurement, differs remarkably when changing the molecular alignment. We…
In this paper, we discuss the possibility of imaging molecular orbitals from photoelectron spectra obtained via Laser Induced Electron Diffraction (LIED) in linear molecules. This is an extension of our work published recently in Physical Review A \textbf{94}, 023421 (2016) to the case of the HOMO-1 orbital of the carbon dioxide molecule. We show that such an imaging technique has the potential to image molecular orbitals at different internuclear distances in a sub-femtosecond time scale and with a resolution of a fraction of an Angström.
Wavefunction-splitting or mask method, widely used in the non-relativistic calculations of the photoelectron angular distributions, is extended to the relativistic domain within the dipole approximation. Since the closed-form expressions for the relativistic Volkov states are not available within the dipole approximation, we build such states numerically solving a single second-order differential equation. We calculate the photoelectron energy spectra and angular distributions for highly charged ions under different ionization regimes with both the direct and the relativistic mask methods. We …
Photoelectron momentum distributions (PMDs) from atoms and molecules undergo qualitative changes as laser parameters are varied. We present a model to interpret the shape of the PMDs. The electron's motion is guided by a fictitious particle in our model, clearly characterizing two distinct dynamical behaviors: direct ionization and rescattering. As laser ellipticity is varied, our model reproduces the bifurcation in the PMDs seen in experiments.
Strong field photoelectron holography has been proposed as a means for interrogating the spatial and temporal information of electrons and ions in a dynamic system. After ionization, part of the electron wave packet may directly go to the detector (the reference wave), while another part may be driven back to the ion where it scatters off (the signal wave). The interference hologram of the two waves may be used to retrieve the target information. However, unlike conventional optical holography, the propagations of electron wave packets are affected by the Coulomb potential as well as by the la…
The magnetic-field effect of the laser pulse is investigated in laser-assisted XUV ionization. By numerically solving the three-dimensional time-dependent Schrödinger equation, we find that the photoelectron momentum distribution is distorted by the magnetic-field effect of the IR streaking field. It results in a transverse-momentum- and time-delay-dependent longitudinal photoelectron momentum shift, which is further analytically confirmed by employing the nondipole corrected strong field approximation. We also demonstrate that the magnetic field does not affect the time shift retrieved from t…
We use the $R$-matrix with time-dependence method to study detachment from F$^-$ in circularly-polarized laser fields of infrared wavelength. By decomposing the photoelectron momentum distribution into separate contributions from detached $2p_1$ and $2p_{-1}$ electrons, we demonstrate that the detachment yield is distributed asymmetrically with respect to these initial orbitals. We observe the well-known preference for strong-field detachment of electrons that are initially counter-rotating relative to the field, and calculate the variation in this preference as a function of photoelectron ene…
The energy and the angular distributions of photoelectrons are shown to be tunable by choosing the time and the spatial phase structure of the driving fields. These conclusions are derived from quantum mechanical calculations done within a single-active electron model for an atomic target subjected to a combination of laser field and a time-asymmetric THz pulse and/or vortex-laser pulse with a spatially modulated phase of the wavefront.
Photoelectron interferometry with spectrally shaped polychromatic infrared pulses
Lund University（隆德大学）；Sorbonne Université, CNRS, Laboratoire de Chimie Physique-Matière et Rayonnement, LCPMR（索邦大学，法国国家科学研究中心，物理化学物质与辐射实验室）；Institute of Atomic and Molecular Physics, Jilin University（吉林大学原子与分子物理研究所）；Albert-Ludwigs-Universität Freiburg（弗赖堡大学）；EUCOR Centre for Quantum Science and Quantum Computing, Albert-Ludwigs-Universität Freiburg（弗赖堡大学 EUCOR 量子科学与量子计算中心）；University of Gothenburg（哥德堡大学）
This paper employs Bayesian probability theory for analyzing data generated in femtosecond pump-probe photoelectron-photoion coincidence (PEPICO) experiments. These experiments allow investigating ultrafast dynamical processes in photoexcited molecules. Bayesian probability theory is consistently applied to data analysis problems occurring in these types of experiments such as background subtraction and false coincidences. We previously demonstrated that the Bayesian formalism has many advantages, amongst which are compensation of false coincidences, no overestimation of pump-only contribution…
Nondipole effects in the atomic dynamic interference are investigated by numerically solving the time-dependent Schrödinger equation~(TDSE) of hydrogen. It is found that the inclusion of nondipole corrections in the TDSE can induce momentum shifts of photoelectrons in the opposite direction of the laser propagation. The magnitude of the momentum shift is roughly proportional to the laser peak intensity and to the momentum component of the photoelectron along the laser propagation. By including the nondipole corrections of the Volkov phase into a semi-analytical model previously developed under…
A theoretical study of ionization of the hydrogen atom due to an XUV pulse in the presence of an IR laser is presented. Well-established theories are usually used to describe the problem of laser assisted photoelectron effect. However, the well-known soft-photon approximation firstly posed by Maquet et al in Journal of Modern Optics 54, 1847 (2007) and Kazansky's theory in Phys. Rev. A 82, 033420 (2010) completely fails to predict the electron emission prependicularly to the polarization direction. Making use of a simple semiclassical model, we study the angle-resolved energy distribution of p…
Multiphoton ionization of sodium by femtosecond laser pulses of 800 nm wavelength in the range of laser peak intensities entering over-the-barrier ionization domain is studied. Photoelectron momentum distributions and the energy spectra are determined numerically by solving the time dependent Schroedinger equation for three values of the laser intensity from this domain. The calculated spectra agree well with the spectra obtained experimentally by Hart et al (Phys. Rev. A 2016 93 063426). A partial wave analysis of the spectral peaks related to Freeman resonances has shown that each peak is a …
The full three-dimensional photoelectron momentum distributions of argon are measured in intense near-circularly polarized laser fields. We observed that the transverse momentum distribution of ejected electrons by 410-nm near-circularly polarized field is unexpectedly narrowed with increasing laser intensity, which is contrary to the conventional rules predicted by adiabatic theory. By analyzing the momentum-resolved angular momentum distribution measured experimentally and the corresponding trajectories of ejected electrons semiclassically, the narrowing can be attributed to a temporary trap…
