294 research outputs found
Phase Measurement of Resonant Two-Photon Ionization in Helium
We study resonant two-color two-photon ionization of Helium via the 1s3p 1P1
state. The first color is the 15th harmonic of a tunable titanium sapphire
laser, while the second color is the fundamental laser radiation. Our method
uses phase-locked high-order harmonics to determine the {\it phase} of the
two-photon process by interferometry. The measurement of the two-photon
ionization phase variation as a function of detuning from the resonance and
intensity of the dressing field allows us to determine the intensity dependence
of the transition energy.Comment: 4 pages, 5 figures, under consideratio
Non-Hermitian Rayleigh-Schroedinger Perturbation Theory
We devise a non-Hermitian Rayleigh-Schroedinger perturbation theory for the
single- and the multireference case to tackle both the many-body problem and
the decay problem encountered, for example, in the study of electronic
resonances in molecules. A complex absorbing potential (CAP) is employed to
facilitate a treatment of resonance states that is similar to the
well-established bound-state techniques. For the perturbative approach, the
full CAP-Schroedinger Hamiltonian, in suitable representation, is partitioned
according to the Epstein-Nesbet scheme. The equations we derive in the
framework of the single-reference perturbation theory turn out to be identical
to those obtained by a time-dependent treatment in Wigner-Weisskopf theory. The
multireference perturbation theory is studied for a model problem and is shown
to be an efficient and accurate method. Algorithmic aspects of the integration
of the perturbation theories into existing ab initio programs are discussed,
and the simplicity of their implementation is elucidated.Comment: 10 pages, 1 figure, RevTeX4, submitted to Physical Review
Hydrogen bonding in infinite hydrogen fluoride and hydrogen chloride chains
Hydrogen bonding in infinite HF and HCl bent (zigzag) chains is studied using
the ab initio coupled-cluster singles and doubles (CCSD) correlation method.
The correlation contribution to the binding energy is decomposed in terms of
nonadditive many-body interactions between the monomers in the chains, the
so-called energy increments. Van der Waals constants for the two-body
dispersion interaction between distant monomers in the infinite chains are
extracted from this decomposition. They allow a partitioning of the correlation
contribution to the binding energy into short- and long-range terms. This
finding affords a significant reduction in the computational effort of ab
initio calculations for solids as only the short-range part requires a
sophisticated treatment whereas the long-range part can be summed immediately
to infinite distances.Comment: 9 pages, 4 figures, 3 tables, RevTeX4, corrected typo
Theory of x-ray absorption by laser-dressed atoms
An ab initio theory is devised for the x-ray photoabsorption cross section of
atoms in the field of a moderately intense optical laser (800nm, 10^13 W/cm^2).
The laser dresses the core-excited atomic states, which introduces a dependence
of the cross section on the angle between the polarization vectors of the two
linearly polarized radiation sources. We use the Hartree-Fock-Slater
approximation to describe the atomic many-particle problem in conjunction with
a nonrelativistic quantum-electrodynamic approach to treat the photon-electron
interaction. The continuum wave functions of ejected electrons are treated with
a complex absorbing potential that is derived from smooth exterior complex
scaling. The solution to the two-color (x-ray plus laser) problem is discussed
in terms of a direct diagonalization of the complex symmetric matrix
representation of the Hamiltonian. Alternative treatments with time-independent
and time-dependent non-Hermitian perturbation theories are presented that
exploit the weak interaction strength between x rays and atoms. We apply the
theory to study the photoabsorption cross section of krypton atoms near the K
edge. A pronounced modification of the cross section is found in the presence
of the optical laser.Comment: 13 pages, 3 figures, 1 table, RevTeX4, corrected typoe
Rate equations for nitrogen molecules in ultrashort and intense x-ray pulses
We study theoretically the quantum dynamics of nitrogen molecules (N2) exposed to intense and ultrafast x-rays at a wavelength of 1.1 nm (1100eV photon energy) from the Linac Coherent Light Source (LCLS) free electron laser. Molecular rate equations are derived to describe the intertwined photoionization, decay, and dissociation processes occurring for N2. This model complements our earlier phenomenological approaches, the single-atom, symmetric-sharing, and fragmentation-matrix models of 2012 (J. Chem. Phys. 136 214310). Our rate-equations are used to obtain the effective pulse energy at the sample and the time scale for the dissociation of the metastable dication . This leads to a very good agreement between the theoretically and experimentally determined ion yields and, consequently, the average charge states. The effective pulse energy is found to decrease with shortening pulse duration. This variation together with a change in the molecular fragmentation pattern and frustrated absorption - an effect that reduces absorption of x-rays due to (double) core hole formation - are the causes for the drop of the average charge state with shortening LCLS pulse duration discovered previously
Theory of x-ray absorption by laser-aligned symmetric-top molecules
We devise a theory of x-ray absorption by symmetric-top molecules which are
aligned by an intense optical laser. Initially, the density matrix of the
system is composed of the electronic ground state of the molecules and a
thermal ensemble of rigid-rotor eigenstates. We formulate equations of motion
of the two-color (laser plus x rays) rotational-electronic problem. The
interaction with the laser is assumed to be nonresonant; it is described by an
electric dipole polarizability tensor. X-ray absorption is approximated as a
one-photon process. It is shown that the equations can be separated such that
the interaction with the laser can be treated independently of the x rays. The
laser-only density matrix is propagated numerically. After each time step, the
x-ray absorption is calculated. We apply our theory to study adiabatic
alignment of bromine molecules (Br2). The required dynamic polarizabilities are
determined using the ab initio linear response methods coupled-cluster singles
(CCS), second-order approximate coupled-cluster singles and doubles (CC2), and
coupled-cluster singles and doubles (CCSD). For the description of x-ray
absorption on the sigma_g 1s --> sigma_u 4p resonance, a parameter-free
two-level model is used for the electronic structure of the molecules. Our
theory opens up novel perspectives for the quantum control of x-ray radiation.Comment: 14 pages, 4 figures, 1 table, RevTeX4, revise
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