A method is proposed for extracting ionization amplitudes from the solution of the time-dependent Schrödinger equation (TDSE) describing a system in a time-dependent external field. The method is a hybrid of two earlier developed methods, the time-dependent surface flux (t-SURFF) method and the method using the propagated wavepacket as the source term in a time-independent driven Schrödinger equation with the field-free Hamiltonian. It is demonstrated that the method combines the advantages of the parent ones and allows the extraction of ionization amplitudes by solving the TDSE within a small spatial domain (with the boundary conditions provided by exterior complex scaling) and a time interval, not exceeding the external field pulse duration.
The structure of approximate two electron wavefunction is deeply investigated, both theoretically and numerically, in the strong-field driven ionization dynamics. Theoretical analyses clarify that for two electron singlet systems, the previously proposed time-dependent extended Hartree-Fock (TD-EHF) method [Phys. Rev. A 51, 3999 (1995)] is equivalent to the multiconfiguration time-dependent Hartree-Fock method with two occupied orbitals. The latter wavefunction is further transformed into the natural expansion form, enabling the direct propagation of the natural orbitals (NOs). These methods, …
We implement a full nonlinear optimization method to fit continuum states with complex Gaussians. The application to a set of regular scattering Coulomb functions allows us to validate the numerical feasibility, to explore the range of convergence of the approach, and to demonstrate the relative superiority of complex over real Gaussian expansions. We then consider the photoionization of atomic hydrogen, and ionization by electron impact in the first Born approximation, for which the closed form cross sections serve as a solid benchmark. Using the proposed complex Gaussian representation of th…
The problem of time delay in tunneling ionization is revisited. The origin of time delay at the tunnel exit is analysed, underlining the two faces of the concept of the tunnelling time delay: the time delay around the tunnel exit and the asymptotic time delay at a detector. We show that the former time delay, in the sense of a delay in the peak of the wavefunction, exists as a matter of principle and arises due to the sub-barrier interference of the reflected and transmitted components of the tunneling electronic wavepacket. We exemplify this by describing the tunnelling ionization of an elect…
The $N$-particle wavefunction has too many dimensions for a direct time propagation of a many-body system according to the time-dependent Schrödinger equation (TDSE). On the other hand, time-dependent density functional theory (TDDFT) tells us that the single-particle density is, in principle, sufficient. However, a practicable equation of motion (EOM) for the accurate time evolution of the single-particle density is unknown. It is thus an obvious idea to propagate a quantity which is not as reduced as the single-particle density but less dimensional than the $N$-body wavefunction. Recently, w…
The dissociative ionization of $H_2^+$ in linearly polarized, 400 nm laser pulses is simulated by solving a three-particle time-dependent Schrödinger equation in full dimensionality. The joint energy spectra (JES) are computed for $\cos^8$ and flat-top envelopes using the time-dependent surface flux (tSurff) methods. In JES, the energy sharing $n$ photon energies $ω$ of nuclear kinetic energy release (KER) $E_N$ and electronic KER $E_e$ are well represented by $E_N+E_e=nω-U_p+E_0$ for $\cos^8$ pulses, but satisfy $E_N+E_e=nω+E_0$ for flat-top envelope, exposing a deviation of the ponderomotive…
We present a theoretical method for calculating multiphoton ionization amplitudes and cross sections of few-electron atoms. The present approach is based on an extraction of partial wave amplitudes from a scattering wave function, which is calculated by solving a system of driven Schroedinger equations. The extraction relies on a description of partial waves in terms of a small number of Coulomb waves with fixed wave numbers. The method can be used for photon energies below and above the ionization threshold and to treat resonance-enhanced multiphoton ionization. We use it to calculate two-, t…
Relative phases of atomic above-threshold ionization wavepackets have been investigated in a recent experiment [L. J. Zipp, A. Natan, and P. H. Bucksbaum, Optica \textbf{1}, 361-364 (2014)] exploiting interferences between different pathways in a weak probe field at half the frequency of the strong ionization pulse. In this work we theoretically explore the extraction of phase delays and time delays of attosecond wavepackets formed in strong-field ionization. We perform simulations solving the time-dependent Schrödinger equation and compare these results with the strong-field and Coulomb-Volko…
Strong field processes in the non-relativistic regime are insensitive to the electron spin, i.e. the observables appear to be independent of this electron property. This does not have to be the case for several active electrons where Pauli principle may affect the their dynamics. We exemplify this statement studying model atoms with three active electrons interacting with strong pulsed radiation, using an ab-initio time-dependent Schrödinger equation on a grid. In our restricted dimensionality model we are able, for the first time, to analyse momenta correlations of the three outgoing electron…
Several recent attoclock experiments have investigated the fundamental question of a quantum mechanically induced time delay in tunneling ionization via extremely precise photoelectron momentum spectroscopy. The interpretations of those attoclock experimental results were controversially discussed, because the entanglement of the laser and Coulomb field did not allow for theoretical treatments without undisputed approximations. The method of semiclassical propagation matched with the tunneled wavefunction, the quasistatic Wigner theory, the analytical R-matrix theory, the backpropagation metho…
Levy-Perdew-Sahni (LPS) provided a proof of the connection between the density and ionization potential of a many-electron system using the equation for the density directly. This equation employs an effective potential which is derived by LPS from the many-electron wavefunction of the system. In this paper, we calculate this potential explicitly by employing an accurate wavefunction for two-electron systems. With this wavefunction connection the LPS equation is then solved self- consistently employing this potential and shown to lead to accurate densities and chemical potentials for these sys…
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 …
We demonstrate the capabilities of time-dependent density functional theory (TDDFT) for strong-field, short wavelength (soft X-ray) physics, as compared to a formalism based on rate equations. We find that TDDFT provides a very good description of the total and individual ionization yields for Ne and Ar atoms exposed to strong laser pulses. We assess the reliability of different adiabatic density functionals and conclude that an accurate description of long-range interactions by the exchange and correlation potential is crucial for obtaining the correct ionization yield over a wide range of in…
The energy distribution of an ultracold rubidium ion beam, which is intended to be used as the source for a focused ion beam instrument, is measured with a retarding field analyzer. The ions are created from a laser-cooled and compressed atomic beam by two-step photoionization in which the ionization laser power is enhanced in a build-up cavity. Particle tracing simulations are performed to ensure the analyzer is able to resolve the distribution. The lowest achieved full width 50% energy spread is $\left(0.205\pm0.006\right)$ eV. The energy spread originates from the variation in the ionizatio…
We analyze interference processes in atomic ionization induced by a two-color laser with fundamental frequency $ω$ and its second harmonic $2ω$. The interplay between inter- and intracycle interference processes give rise to multiphoton peaks which can be named as main or ATI peaks and sidebands, in analogy to the well-known RABBIT (reconstruction of attosecond harmonic beating by interference of two-photon transitions). We use the saddle point approximation (SPA) to extract the complex ionization times of the interfering electron trajectories. Changing the relative phase between the two color…
We investigate the role of nuclear motion and strong-field-induced electronic couplings during the double ionization of deuterated water using momentum-resolved coincidence spectroscopy. By examining the three-body dicationic dissociation channel, D$^{+}$/D$^{+}$/O, for both few- and multi-cycle laser pulses, strong evidence for intra-pulse dynamics is observed. The extracted angle- and energy-resolved double ionization yields are compared to classical trajectory simulations of the dissociation dynamics occurring from different electronic states of the dication. In contrast with measurements o…
Bichromatic extreme-ultraviolet pulses from a seeded free-electron laser enable us to measure photoelectron angular distribution (PAD) as a function of the relative phase between the different wavelength components. The time-dependent multiconfiguration self-consistent-field (TD-MCSCF) methods are powerful multielectron computation methods to accurately simulate such photoionization dynamics from the first principles. Here we propose a method to evaluate the amplitude and phase of each ionization path, which completely determines the photoionization processes, using TD-MCSCF simulation results…
We show that time ordering underlying time-dependent quantum dynamics is a physical observable accessible by attosecond streaking. We demonstrate the extraction of time ordering for the prototypical case of time-resolved two-photon double ionization (TPDI) of helium by an attosecond XUV pulse. The Eisenbud-Wigner-Smith time delay for the emission of a two-electron wavepacket and the time interval between subsequent emission events can be unambiguously determined by attosecond streaking. The delay between the two emission events sensitively depends on the energy, pulse duration, and angular dis…
Hydrogen photoionization in a magnetized medium: the rigid-wavefunction approach revisited
Instituto de Ciencias Astronómicas, de la Tierra y del Espacio (ICATE, CONICET-UNSJ)（地球与空间天体物理科学研究所）；Facultad de Ciencias Exactas, Físicas y Naturales (FCEFN, UNSJ)（理学院）
The open-shell reference relativistic equation-of-motion coupled-cluster method within its four-component description is successfully implemented with the consideration of single- and double- excitation approximation. The one-body and two-body matrix elements required for the correlation calculation are generated using Dirac-Coulomb Hamiltonian. As a first attempt, the implemented method is employed to calculate a few of the low-lying ionized states of heavy atomic (Ag, Cs, Au, Fr, Lr) and valence ionization potential of molecular (HgH, PbF) systems, where the effect of relativity does really …
An infinite dimensional canonical symplectic structure and structure-preserving geometric algorithms are developed for the photon-matter interactions described by the Schrödinger-Maxwell equations. The algorithms preserve the symplectic structure of the system and the unitary nature of the wavefunctions, and bound the energy error of the simulation for all time-steps. This new numerical capability enables us to carry out first-principle based simulation study of important photon-matter interactions, such as the high harmonic generation and stabilization of ionization, with long-term accuracy a…
We review time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method and time-dependent optimized coupled-cluster (TD-OCC) method for first-principles simulations of high-field phenomena such as tunneling ionization and high-order harmonic generation in atoms and molecules irradiated by a strong laser field. These methods provide a flexible and systematically improvable description of the multielectron dynamics by expressing the all-electron wavefunction by configuration interaction expansion or coupled-cluster expansion, using time-dependent one-electron orbital functions. The …
The newly developed method of time-of-flight (ToF) momentum microscopy was used to analyse the cold electron emission from a Cs 3D magneto-optical trap (MOT). Three-step resonant photoionization was implemented via two intermediate states (6P3/2 pumped with 852 nm laser and 7S1/2 with 1470 nm) and a tuneable femtosecond Ti:sapphire laser for the final ionization step. The magnetic field of the MOT is switched off during the photoionization step. The natural bandwidth of the fs-laser is reduced to 4 meV using optical spectral filters. Precise tuning of the photon energy makes it possible to obs…
Solution of two-center time-dependent Dirac equation in spherical coordinates: Application of the multipole expansion of the electron-nuclei interaction
We describe an ab initio and non-perturbative $R$-matrix with time-dependence theory for ultrafast atomic processes in light fields of arbitrary polarization. The theory is applicable to complex, multielectron atoms and atomic ions subject to ultrashort (particularly few-femtosecond and attosecond) laser pulses with any given ellipticity, and generalizes previous time-dependent $R$-matrix techniques restricted to linearly polarized fields. We discuss both the fundamental equations, required to propagate the multielectron wavefunction in time, as well as the computational developments necessary…
Time-dependent Hole States in Multiconfigurational Time-Dependent Hartree-Fock Approaches: Applications in Photoionization of Water Molecule
Shanghai Jiao Tong University（上海交通大学）；RIKEN Center for Interdisciplinary Theoretical and Mathematical Sciences (iTHEMS)（理化学研究所交叉理论数学科学中心（iTHEMS））；RIKEN Center for Computational Science (R-CCS)（理化学研究所计算科学中心（R-CCS））；The University of Tokyo（东京大学）
