(1) Manipulation of molecules by means of external fields
(2) Molecular collisions in fields
(3) Spectroscopy and imaging of molecules in fields
(4) Cold/slow molecules
(5) Quantum computing with molecules
(6) Supersymmetry and topology of molecules in combined electric, magnetic, and optical fields
Directional states of molecules are at the core of all methods to manipulate molecular trajectories. This is because only in directional states are the body-fixed multipole moments 'available' in the laboratory frame where they can be acted upon by space-fixed fields. In the case of polar molecules, the body-fixed permanent dipole moment is put to such a full use in the laboratory by creating oriented states characterized by as complete a projection of the body-fixed dipole moment on the space-fixed axis as the uncertainty principle allows. In the past, in order to achieve a high degree of orientation, one had to rely on special properties of particular molecules. The need for such a reliance has been superseded by the development of a versatile techniques that combines a static electric field with a nonresonant optical field. The combined fields give rise to an amplification effect which occurs for any polar molecule, as only an anisotropic polarizability, along with a permanent dipole moment, is required. This is always available in polar molecules. Thus, for a number of molecules in their rotational ground state, a very weak static electric field can convert second-order alignment by a laser into a strong first-order orientation that projects about 90% of the body-fixed dipole moment on the static field direction. If the polar molecule is also paramagnetic, combined static electric and magnetic fields yield similar amplification effects, which are indeed the subject of our present work.
Ketan Sharma (Berlin), Mikhail Lemeshko (Cambridge, MA), Marko Härtelt (Berlin).
are nearly ubiquitous in nature as well as in the laboratory. Molecules colliding in the Earth's atmosphere or in interstellar space are commonly subject to magnetic and radiative fields; in the laboratory, collisions in fields appear with particular prominence in stereodynamics, coherent control, and molecular trapping and cooling. Molecular collisions in fields have been the subject of a number of theoretical studies. However, analytic models of such collisions are scarce and limited to the collision regime near the Wigner limit. Recently, we have developed an analytic model of state-to-state rotationally inelastic collisions of atoms with molecules in fields, applicable at thermal and hyperthermal collision energies. The model, based on Fraunhofer scattering of matter waves, is inherently quantum and makes it possible to separate dynamical and geometric effects in collisions. Our current effort is being directed at identifying form factors in vector correlations observed in state-of-the-art experiments and/or full-fledged computations.
Mikhail Lemeshko (Cambridge, MA), Marcelo de Miranda (Leeds), Javier Aoiz (Madrid), Millard Alexander (Maryland).
Oriented states have a unique spectroscopic behavior, due to their sui generis energy level patterns and modified Hönl-London factors. Our effort is directed towards identifying oriented states of molecules in the combined fields, characterizing their spectroscopic response in both the time and frequency domain, and devising means to enhance the spatial resolution of molecular imaging.
Burkhard Schmidt (Berlin), Henrik Stapelfeldt (Aarhus), Rosario Gonzalez-Ferez (Granada), Jochen Küpper (Hamburg).
Over the last two decades, atomic and molecular physics has come into a spectacular bloom, much of which sprang from the newfashioned techniques to translationally cool (or slow down) gaseous atoms and molecules. The study of slow atoms and molecules, which ensued, has led to uncharted territories - not just of atomic and molecular physics, but of physics and chemistry at large. We've been engaged in developing techniques of slowing and trapping molecules based on time-varying inhomogeneous electric fields, either due to a pulsed laser or due to switched electrostatic fields. So far we worked out an analytic model of the Stark deceleration process and proposed an AC trap for high-field seeking molecules, which has meanwhile been implemented.
John Doyle (Cambridge, MA), David Patterson (Cambridge, MA).
Since the original proposal by David DeMille, arrays of ultracold polar molecules have been counted among the most promising platforms for the implementation of a quantum computer. The qubit of such an array is realized by a single dipolar molecule entangled via its dipole-dipole interaction with the rest of the array's molecules. The electric dipole interaction ensures that each qubit is interacting not only with its neighbors but also with every other qubit in the system. Previous studies of entanglement of electric dipoles have not adequately considered how the external electric field affects both the qubit states and the dipole-dipole interaction. In our current work we consider entanglement for ultracold polar and paramagnetic molecules trapped in a two-dimensional optical lattice in congruent electric and magnetic fields. The presence of the unpaired electron in a, say, doublet Sigma molecule can be used for encoding quantum information as in other spin-1/2 particles. Understanding the dynamics of spin excitation transfer between molecules in the combined fields will allow us to tune the entanglement in such a system. We are also investigating methods of designing quantum logical gates, one-qubit gates, and two-bit quantum gates (such as the CNOT gate) for molecular dipole arrays.
Sabre Kais (West Lafayette), Dudley Herschbach (Cambridge, MA).
We made use of supersymmetric quantum mechanics (SUSY QM) to find sets of conditions under which the problem of a polar paramagnetic molecule subject to combined electric, magnetic, and optical fields is analytically solvable. The analytic forms of the eigenfuntions made it possible to find analytic expressions for the observables of interest, such as the expectation values of the angular momentum squared and of the orientation and alignment cosines as well as of the eigenenergy. Furthermore, we found that the topology of the intersections of the molecule's eigenenergy surfaces can be characterized by a single integer index whose values correspond to the sets of conditions under which the analytic solutions to the quantum pendulum problem exist. We invoke both algebraic methods and the correspondence principle between quantum and classical mechanics in our attempt to identify the reasons that underlie the connection between supersymmetry and topology.
Burkhard Schmidt (Berlin), Sabre Kais (West Lafayette).
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