187 research outputs found
Transient absorption and reshaping of ultrafast XUV light by laser-dressed helium
We present a theoretical study of transient absorption and reshaping of
extreme ultraviolet (XUV) pulses by helium atoms dressed with a moderately
strong infrared (IR) laser field. We formulate the atomic response using both
the frequency-dependent absorption cross section and a time-frequency approach
based on the time-dependent dipole induced by the light fields. The latter
approach can be used in cases when an ultrafast dressing pulse induces
transient effects, and/or when the atom exchanges energy with multiple
frequency components of the XUV field. We first characterize the dressed atom
response by calculating the frequency-dependent absorption cross section for
XUV energies between 20 and 24 eV for several dressing wavelengths between 400
and 2000 nm and intensities up to 10^12 W/cm^2. We find that for dressing
wavelengths near 1600 nm, there is an Autler-Townes splitting of the 1s ---> 2p
transition that can potentially lead to transparency for absorption of XUV
light tuned to this transition. We study the effect of this XUV transparency in
a macroscopic helium gas by incorporating the time-frequency approach into a
solution of the coupled Maxwell-Schr\"odinger equations. We find rich temporal
reshaping dynamics when a 61 fs XUV pulse resonant with the 1s ---> 2p
transition propagates through a helium gas dressed by an 11 fs, 1600 nm laser
pulse.Comment: 13 pages, 8 figures, 1 table, RevTeX4, revise
Resonance fluorescence in ultrafast and intense x-ray free-electron-laser pulses
The spectrum of resonance fluorescence is calculated for a two-level system excited by an intense, ultrashort x-ray pulse made available for instance by free-electron lasers such as the Linac Coherent Light Source. We allow for inner-shell hole decay widths and destruction of the system by further photoionization. This two-level description is employed to model neon cations strongly driven by x rays tuned to the 1s 2p-1 --> 1s-1 2p transition at 848 eV; the x rays induce Rabi oscillations which are so fast that they compete with Ne 1s-hole decay. We predict resonance fluorescence spectra for two different scenarios: first, chaotic pulses based on the self-amplified spontaneous emission principle, like those presently generated at x-ray free-electron-laser facilities and, second, Gaussian pulses which will become available in the foreseeable future with self-seeding techniques. As an example of the exciting opportunities derived from the use of seeding methods, we predict, in spite of above obstacles, the possibility to distinguish at x-ray frequencies a clear signature of Rabi flopping in the spectrum of resonance fluorescence
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
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
Quasiparticle band structure of infinite hydrogen fluoride and hydrogen chloride chains
We study the quasiparticle band structure of isolated, infinite HF and HCl
bent (zigzag) chains and examine the effect of the crystal field on the energy
levels of the constituent monomers. The chains are one of the simplest but
realistic models of the corresponding three-dimensional crystalline solids. To
describe the isolated monomers and the chains, we set out from the Hartree-Fock
approximation, harnessing the advanced Green's function methods "local
molecular orbital algebraic diagrammatic construction" (ADC) scheme and "local
crystal orbital ADC" (CO-ADC) in a strict second order approximation, ADC(2,2)
and CO-ADC(2,2), respectively, to account for electron correlations. The
configuration space of the periodic correlation calculations is found to
converge rapidly only requiring nearest-neighbor contributions to be regarded.
Although electron correlations cause a pronounced shift of the quasiparticle
band structure of the chains with respect to the Hartree-Fock result, the
bandwidth essentially remains unaltered in contrast to, e.g., covalently bound
compounds.Comment: 11 pages, 6 figures, 6 tables, RevTeX4, corrected typoe
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