Time-dependent momentum expectation values from different quantum probability and flux densities.

Based on the Ehrenfest theorem, the time-dependent expectation value of a momentum operator can be evaluated equivalently in two ways. The integrals appearing in the expressions are taken over two different functions. In one case, the integrand is the quantum mechanical flux density j̲, and in the other, a different quantity j̲̃ appears, which also has the units of a flux density.

Detecting and Characterizing the Nonadiabaticity of Laser-Induced Quantum Tunneling.

The nonadiabaticity of quantum tunneling through an evolving barrier is relevant to resolving laser-driven dynamics of atoms and molecules at an attosecond timescale. Here, we propose and demonstrate a novel scheme to detect the nonadiabatic behavior of tunnel ionization studied in an attoclock configuration, without counting on the laser intensity calibration or the modeling of the Coulomb effect. In our scheme, the degree of nonadiabaticity for tunneling scenarios in elliptically polarized laser fields can be steered continuously simply with the pulse ellipticity, while the critical instantaneous vector potentials remain identical.

Deformation of Atomic p_{±} Orbitals in Strong Elliptically Polarized Laser Fields: Ionization Time Drifts and Spatial Photoelectron Separation.

We theoretically investigate the deformation of atomic p_{±} orbitals driven by strong elliptically polarized (EP) laser fields and the role it plays in tunnel ionization. Our study reveals that different Stark effects induced by orthogonal components of the EP field give rise to subcycle rearrangement of the bound electron density, rendering the initial p_{+} and p_{-} orbitals deformed and polarized along distinctively tilted angles with respect to the polarization ellipse of the EP field. As a consequence, the instantaneous tunneling rates change such that for few-cycle EP laser pulses the bound electron initially counterrotating (corotating) with the electric field is most likely released before (after) the peak of the electric field.

Probability and Flux Densities in the Center-of-Mass Frame.

For an arbitrary nonstationary wave function of a nonrelativistic closed many-body system consisting of arbitrary interacting particles, the general expressions for the time-dependent one-particle probability and flux densities in the center-of-mass frame without applying Born-Oppenheimer approximation are obtained. Even the wave function for the translation is additionally introduced; it disappears in the center-of-mass frame automatically. It is shown that for the rotational ground state the time-dependent probability and flux densities of an arbitrary particle in the center-of-mass frame are isotropic.

Identifying the Tunneling Site in Strong-Field Ionization of H_{2}^{+}.

The tunneling site of the electron in a molecule exposed to a strong laser field determines the initial position of the ionizing electron and, as a result, has a large impact on the subsequent ultrafast electron dynamics on the polyatomic Coulomb potential. Here, the tunneling site of the electron of H_{2}^{+} ionized by a strong circularly polarized (CP) laser pulse is studied by numerically solving the time-dependent Schrödinger equation. We show that the electron removed from the down-field site is directly driven away by the CP field and the lateral photoelectron momentum distribution (LPMD) exhibits a Gaussian-like distribution, whereas the corresponding LPMD of the electron removed from the up-field site differs from the Gaussian shape due to the Coulomb focusing and scattering by the down-field core.

Helicity sensitive enhancement of strong-field ionization in circularly polarized laser fields.

We investigate the strong-field ionization from p± orbitals driven by circularly polarized laser fields by solving the two-dimensional time-dependent Schrödinger equation in polar coordinates with the Lagrange mesh technique. Enhancement of ionization is found in the deep multiphoton ionization regime when the helicity of the laser field is opposite to that of the p electron, while this enhancement is suppressed when the helicities are the same. It is found that the enhancement of ionization is attributed to the multiphoton resonant excitation.

Translational effects on electronic and nuclear ring currents.

In previous works, it was predicted that electronic and nuclear ring currents in degenerate excited states of atomic and molecular systems persist after the end of driven circularly polarized atto- or femtosecond laser pulses on relatively long time scales, often on pico- or nanosecond time scales, before spontaneous emission occurs. Although this conclusion is true in the center of mass frame, it is not true in the laboratory frame, where the translation has to be considered. In this theoretical work, the analytic formulas for the ring current densities, electric ring currents, mean ring current radii, and induced magnetic fields at the ring center, depending on the translational wavepacket widths, are derived.

Strong nuclear ring currents and magnetic fields in pseudorotating OsH4 molecules induced by circularly polarized laser pulses.

We design a circularly polarized laser pulse in the infrared frequency and femtosecond time domains, for excitation of the OsH(4) molecule in its first excited pseudorotational state of the triply-degenerate bend. The OsH(4) molecule need not be pre-oriented. After excitation, the central nucleus Os carries out pseudorotation about the axis parallel to the direction of propagation of the laser pulse.

Electronic quantum fluxes during pericyclic reactions exemplified for the Cope rearrangement of semibullvalene.

The outcome of a pericyclic reaction is typically represented by arrows in the Lewis structure of the reactant, symbolizing the net electron transfer. Quantum simulations can be used to interpret these arrows in terms of electronic fluxes between neighboring bonds. The fluxes are decomposed into contributions from electrons in so-called pericyclic orbitals, which account for the mutation of the Lewis structure for the reactant into that for the product, in other valence and in core orbitals.

From synchronous to sequential double proton transfer: quantum dynamics simulations for the model porphine.

Quantum dynamics simulations of double proton transfer (DPT) in the model porphine, starting from a nonequilibrium initial state, demonstrate that a switch from synchronous (or concerted) to sequential (or stepwise or successive) breaking and making of two bonds is possible. For this proof of principle, we employ the simple model of Smedarchina, Z.; Siebrand, W.

Few-cycle laser pulses to obtain spatial separation of OHF- dissociation products.

In a two-part theoretical study, field-free orientation of OHF(-) is achieved by means of moderately intense half-cycle, infrared laser pulses. In the first step, a short linearly polarized pulse excites a superposition of rigid rotor rotational eigenstates via interaction with the permanent dipole moment of OHF(-). After the field has been switched off, pronounced molecular orientation is observed for several picoseconds.

Nonadiabatic orientation, toroidal current, and induced magnetic field in BeO molecules.

It is predicted that oriented BeO molecules would give rise to unprecedentedly strong, unidirectional electric ring current and an associated magnetic field upon excitation by a right or left circularly polarized laser pulse into the first excited degenerate singlet state. The strong toroidal electric ring current of this state is dominated by the ring current of the 1pi(+/-) orbital about the molecular axis. Our predictions are based on the analysis of the orbital composition of the states involved and are substantiated by high level electronic structure calculations and wavepacket simulations of the laser-driven orientation and excitation dynamics.

Internal momentum state mapping using high harmonic radiation.

We numerically demonstrate so-far undescribed features in ionization and high harmonic generation from bound states with nonvanishing electronic angular momentum. The states' modified response to a strong laser pulse can be exploited for novel measurement and pulse production schemes. It is shown that angularly asymmetric tunneling from the states can be mapped onto variations of high harmonic intensities and that near-circularly polarized isolated attosecond extreme ultraviolet or x-ray pulses can be produced.

Unidirectional electronic ring current driven by a few cycle circularly polarized laser pulse: quantum model simulations for Mg-porphyrin.

A circularly polarized ultraviolet (UV) laser pulse may excite a unidirectional valence-type electronic ring current in an oriented molecule, within the pulse duration of a few femtoseconds (e.g., tau = 3.

Factors affecting the efficacy of peripheral blood progenitor cells collections by large-volume leukaphereses with standardized processing volumes.

Background: Peripheral blood progenitor cell (PBPC) collections should be safe and efficient. Therefore, the influence and risk factors in large-volume leukaphereses (LVL) with standardized blood volumes was investigated.

Study Design And Methods: In a total of 724 autologous LVL performed at our center, either 4x or 6x the patient's blood volume (PBV) was processed.