Theory of x-ray absorption by laser-aligned symmetric-top molecules

dc.creatorButh, Christian
dc.creatorSantra, Robin
dc.date2007-11-20
dc.date2008-02-01
dc.date.accessioned2026-07-07T09:22:37Z
dc.date.available2026-07-07T09:22:37Z
dc.descriptionWe 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.
dc.description14 pages, 4 figures, 1 table, RevTeX4, revised
dc.identifierhttps://arxiv.org/abs/0711.3203
dc.identifierhttp://arxiv.org/abs/0711.3203
dc.identifierPhys. Rev. A 77, 013413 (2008) (13 pages), republication in Virtual Journal of Ultrafast Science 7, issue 2 (2008)
dc.identifierdoi:10.1103/PhysRevA.77.013413
dc.identifier.urihttp://salesiana.dossiersoluciones.com/handle/123456789/155438
dc.subjectChemical Physics
dc.subjectOptics
dc.titleTheory of x-ray absorption by laser-aligned symmetric-top molecules
dc.typetext

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