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
