We develop a general framework for describing the interaction of molecules with a nonperturbative intensity gradient and note several limits, including the two-level Hamiltonian of atom trapping and the quasistatic Hamiltonian of molecular optics. The theory is used to propose a new molecular optics scheme which complements previous work in the area of spatial manipulation of molecules in intense fields by introducing the possibility of reflecting molecules with light. Repulsive interaction obtains in the limit of small level spacings as compared to the field frequency, attained by exciting the molecules to high Rydberg states. Some of the potential applications of the repulsive interaction are illustrated and others are noted. We address the problem of molecular alignment in intense laser fields and describe the possibility of simultaneously focussing the center-of-mass motion of molecules and aligning their figure axis after exit from the laser focus, under field-free conditions.
We develop a general framework for describing the interaction of molecules with a nonperturbative intensity gradient and note several limits, including the two-level Hamiltonian of atom trapping and the quasistatic Hamiltonian of molecular optics. The theory is used to propose a new molecular optics scheme which complements previous work in the area of spatial manipulation of molecules in intense fields by introducing the possibility of reflecting molecules with light. Repulsive interaction obtains in the limit of small level spacings as compared to the field frequency, attained by exciting the molecules to high Rydberg states. Some of the potential applications of the repulsive interaction are illustrated and others are noted. We address the problem of molecular alignment in intense laser fields and describe the possibility of simultaneously focussing the center-of-mass motion of molecules and aligning their figure axis after exit from the laser focus, under field-free conditions.
We discuss the possibility of manipulating the center-of-mass motion of molecules using the nonlinear interaction of a moderately intense, long-pulse laser field with the molecular polarizability tensor. Recent theoretical work demonstrating the possibility of focusing and trapping molecules is extended to consider the effects of circularly and elliptically polarized light and the effect of nonspherical laser optics. The aberrations affecting the quality of the “molecular lens” are analyzed and the means by which they can be minimized are discussed. Molecular focusing is extended to a general field of molecular optics; the possibilities of steering, reflecting, and collimating molecular beams are illustrated. Application of the mechanical force of light to disperse and separate species according to their mass, velocity, or quantum state is proposed.
The possibility of focusing and trapping molecules in the intensity gradient of a moderately intense laser field is shown. A fully quantum-mechanical and a hybrid quantum-classical model are developed and both the case of a near-resonance and that of a far-off-resonance field are studied numerically and analytically. Molecular focusing is obtained when the ratio between the kinetic energy and the field-matter interaction exceeds unity (but remains small). In this energy regime the laser beam serves as a lens for a beam of molecules. The properties of the “molecular lens” are analyzed and the experimental conditions required to focus molecules are examined. We propose the application of laser focusing to nanoscale deposition onto, and etching of a substrate and describe a possible setup to that end. Molecular trapping is obtained as the strong interaction limit of a general “molecular optics” scheme.
We introduce a time-dependent self-consistent-field approach for studying the coupled rotational–translational motion of molecules subject to the macroscopic potential induced by a spatially inhomogeneous, polarized laser field. A hybrid classical-quantum-mechanical variation of the scheme is employed to investigate the possibility of simultaneously focussing the center-of-mass motion of molecules and aligning their figure axis in a field-free region of space. A semiclassical-quantum-mechanical variation is used to describe the rotational–translational dynamics of cold molecules confined to an optical trap.
The goal of the present article is to review the major developments that have led to the current understanding of molecule–field interactions and experimental methods for manipulating molecules with electromagnetic fields. Molecule–field interactions are at the core of several, seemingly distinct areas of molecular physics. This is reflected in the organisation of this article, which includes sections on field control of molecular beams, external field traps for cold molecules, control of molecular orientation and molecular alignment, manipulation of molecules by non-conservative forces, ultracold molecules and ultracold chemistry, controlled many-body phenomena, entanglement of molecules and dipole arrays, and stability of molecular systems in high-frequency super-intense laser fields. The article contains 852 references.
Manipulation of cold atoms by lasers has so far been studied solely within the framework of the conventional dipole approximation, and the atom-light interaction has been treated using low order perturbation theory. Laser control of atomic motions has been ascribed exclusively to the corresponding light-induced dipole forces. In this work, we present a general theory to derive the potential experienced by an atom in a monochromatic laser field in a context analogous to the Born-Oppenheimer approximation for molecules in the field-free case. The formulation goes beyond the dipole approximation and gives rise to the field-atom coupling potential terms which so far have not been taken into consideration in theoretical or experimental studies. Contrary to conventional approaches, our method is based upon the many electron Floquet theory and remains valid also for high intensity laser fields (i.e., for a strongly nonperturbative atom-light interaction). As an illustration of the developed theory, we investigate the trapping of cold atoms in optical lattices. We find that for some atoms for specific laser parameters, despite the absence of the dipole force, the laser trapping is still possible due to the electric quadrupole forces. Namely, we show that by using realistic laser parameters one can form a quadrupole optical lattice which is sufficiently strong to trap Ca and Na atoms.
In this thesis, the use of pulsed laser fields to control the center-of-mass motion of neutral atoms and molecules is studied both numerically and experimentally. In particular, we consider the use of a pulsed standing wave for the deflection of atomic beams, and develop novel types of mirrors for applications in atom and molecule optics. The research work shows that pulsed laser fields can be applied to form efficient mirrors for neutral particles regardless of the details of their internal energy-level structure. Moreover, it is shown that pulsed standing waves can also be utilized to efficiently deflect atomic beams. In the first part of the thesis, we study the effects of phase fluctuations of the laser field on the momentum distribution of atoms after interaction with a standing wave. Our numerical simulations show that the coherence properties of the laser field play a major role in diffraction of atoms, especially when using pulsed lasers. It turns out that the effects caused by the limited coherence time of the optical field are clearly observable as a transfer of atoms in momentum space to the region around zero momentum rather than to high momentum states. The numerical analysis of the pulsed standing-wave diffraction was complemented by experimental measurements of the deflection profiles of a beam of thermal sodium atoms. The experimental distributions were measured for a value of the coherence time intermediate between the Rabi period and the interaction time. A comparison of the results with an expected distribution calculated for a fully coherent interaction shows that the phase fluctuations of the light field drastically affect the achievable transverse momentum values. Based on our theoretical and experimental analysis of the diffraction profiles, we conclude that large deflection angles can be reached only when laser pulses with a Fourier-limited bandwidth are applied. The second part of the thesis concentrates on the development of pulsed mirrors for neutral atoms and molecules. In particular, we consider the use of an evanescent wave, formed in total internal reflection of light on a vacuum-dielectric interface, and of a standing wave as possible mirror configurations. Our numerical simulations of the pulsed evanescent-wave mirror show that atoms with initial velocities up to several tens of meters per second can be reflected already at the moderate field intensities of a few tens of MW/cm2. This allows pulsed evanescent waves to be applied in a compact setup to control the motion of thermal atomic beams, for which the traditional atom mirrors are suited only at grazing incidence. However, since the effective interaction volume of the atomic beam and the laser field is limited by the short decay length of the evanescent wave, only a relatively small number of atoms can be reflected with a single laser pulse. Furthermore, the reflection is always inelastic, since the force exerted on the atoms varies as a function of the initial position of the particles. To solve the above problem we consider the use of a standing wave as a pulsed mirror for atoms. Our numerical simulations show that with a proper choice of the pulse duration and field intensity, each period of the standing-wave pattern functions as an elastic mirror for particles with an initial kinetic energy below the depth of the standing-wave potential. Hence, the standing-wave pattern acts as a long row of independent atom mirrors, which provides a novel route to controlling large volumes of fast atoms even with a single laser pulse. As a second application for the pulsed standing-wave mirror we consider the reflection of slow molecules, for which no efficient mirror configuration previously has been available. It is shown that pulsed standing waves of nonresonant frequencies can be used to efficiently manipulate large volumes of rotationally cold molecules. With a suitable choice of the parameter values, the molecules can be reflected nearly elastically, or with a tailored momentum distribution. This opens up a possibility to use the pulsed standing-wave mirror to control the motion of particles in various applications of atomic and molecular physics. Such a mirror could be applied, for example, to steer and image molecular beams, separate molecular species, and to form pulsed molecular beams.