Rotational spectrum of asymmetric top molecules in combined static and laser fields.

We examine the impact of the combination of a static electric field and a non-resonant linearly polarized laser field on an asymmetric top molecule. Within the rigid rotor approximation, we analyze the symmetries of the Hamiltonian for all possible field configurations. For each irreducible representation, the Schrödinger equation is solved by a basis set expansion in terms of a linear combination of symmetric top eigenfunctions respecting the corresponding symmetries, which allows us to distinguish avoided crossings from genuine ones. Using the fluorobenzene and pyridazine molecules as prototypes, the rotational spectra and properties are analyzed for experimentally accessible static field strengths and laser intensities. Results for energy shifts, orientation, alignment, and hybridization of the angular motion are presented as the field parameters are varied. We demonstrate that a proper selection of the fields gives rise to a constrained rotational motion in three Euler angles, the wave function being oriented along the electrostatic field direction, and aligned in other two angles.

Theoretical description of adiabatic laser alignment and mixed-field orientation: the need for a non-adiabatic model.

We present a theoretical study of recent laser-alignment and mixed-field-orientation experiments of asymmetric top molecules. In these experiments, pendular states were created using linearly polarized strong ac electric fields from pulsed lasers in combination with weak electrostatic fields. We compare the outcome of our calculations with experimental results obtained for the prototypical large molecule benzonitrile (C(7)H(5)N) [J. L. Hansen et al., Phys. Rev. A, 2011, 83, 023406.] and explore the directional properties of the molecular ensemble for several field configurations, i.e., for various field strengths and angles between ac and dc fields. For perpendicular fields one obtains pure alignment, which is well reproduced by the simulations. For tilted fields, we show that a fully adiabatic description of the process does not reproduce the experimentally observed orientation, and it is mandatory to use a diabatic model for population transfer between rotational states. We develop such a model and compare its outcome to the experimental data confirming the importance of non-adiabatic processes in the field-dressed molecular dynamics.

Giant enhancement of photodissociation of polar diatomic molecules in electric fields.

We explore the photodissociation of polar diatomic molecules in static electric fields in the rotationally cold regime using the example of the LiCs molecule. A giant enhancement of the differential cross section is found for laboratory electric field strengths, and analyzed with varying rovibrational bound states, continuum energies as well as field strengths.

Fermionic collective excitations in a lattice gas of Rydberg atoms.

We investigate the many-body quantum states of a laser-driven gas of Rydberg atoms confined to a large spacing ring lattice. If the laser driving is much stronger than the van der Waals interaction among the Rydberg atoms, these many-body states are collective fermionic excitations. The first excited state is a spin wave that extends over the entire lattice. We demonstrate that our system permits us to study fermions in the presence of disorder although no external atomic motion takes place. We analyze how this disorder influences the excitation properties of the fermionic states. Our work shows a route towards the creation of complex many-particle states with atoms in lattices.

Shannon entropy as an indicator of atomic avoided crossings in strong parallel magnetic and electric fields.

Avoided crossings are the most distinctive atomic spectroscopic features in the presence of magnetic and electric fields. We point out the role of Shannon's information entropy as an indicator or predictor of these phenomena by studying the dynamics of some excited states of hydrogen in the presence of parallel magnetic and electric fields. Moreover, in addition to the well-known energy level repulsion, it is found that Shannon's entropy manifests the informational exchange of the involved states as the magnetic field strength is varied across the narrow region where an avoided crossing occurs.