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Royal Society of Chemistry eBooks

Manipulation of Molecules by Combined Permanent and Induced Dipole Forces

Břetislav Friedrich

Published Mar 5, 2021• 3 citations
Publisher

Abstract

This chapter describes a versatile technique to control molecular rotation and translation. The technique is based on the combined effect of external electric fields that act concurrently on the molecular permanent and induced dipole moments. This synergistic effect arises for any polar molecule, as only an anisotropic polarizability, along with a permanent dipole moment, is required. This is always available in polar molecules. The effect of the combined fields can be achieved either by superimposing an electrostatic and a far-off resonant optical field (i.e., one that supplies electric field strength but does not cause transitions) that act, respectively, on the molecule's permanent and induced electric dipole, or by making use of a unipolar electromagnetic pulse that seizes the permanent and induced dipole moments simultaneously. If the combined electric fields are homogeneous, only molecular rotation is affected, whereas inhomogeneous fields affect both molecular rotation and translation. As noted in the chapter, the ability to manipulate molecular rotation and translation has wide-ranging applications – in research areas as diverse as reaction dynamics, spectroscopy, higher harmonic generation and molecular orbital imaging, the focusing and trapping of molecules, as well as quantum simulation and computing.

DOI
10.1039/9781839163043-00317

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OH Trapped by Magnets

Confining atoms with a combination of optical and magnetic fields has led to the formation of new states of matter and provided a tunable test bed to explore many-body atomic and electronic interactions; however, its extension to molecules has been slow. Ultracold molecules (milikelvin temperatures and below) are of interest for a number of additional applications, including studies of quantum phase transitions and precision spectroscopy. One approach to confining polar molecules has relied on inhomogeneous electric fields. Sawyer et al. present an alternative method that traps molecules magnetically. They demonstrate the technique on hydroxyl (OH) radicals, which have appreciable magnetic as well as electric dipole moments. Lifetimes in the magnetoelectrostatic trap ranged from 20 to 500 ms, depending on the background pressure. The technique allows the additional degree of freedom of an electrical field to be superimposed onto the trapped molecules and should facilitate further studies in the direction of controlled molecular collisions and chemical reactions. — ISO

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This chapter describes a versatile technique to control molecular rotation and translation. The technique is based on the combined effect of external electric fields that act concurrently on the molecular permanent and induced dipole moments. This synergistic effect arises for any polar molecule, as only an anisotropic polarizability, along with a permanent dipole moment, is required. This is always available in polar molecules. The effect of the combined fields can be achieved either by superimposing an electrostatic and a far-off resonant optical field (i.e., one that supplies electric field strength but does not cause transitions) that act, respectively, on the molecule's permanent and induced electric dipole, or by making use of a unipolar electromagnetic pulse that seizes the permanent and induced dipole moments simultaneously. If the combined electric fields are homogeneous, only molecular rotation is affected, whereas inhomogeneous fields affect both molecular rotation and translation. As noted in the chapter, the ability to manipulate molecular rotation and translation has wide-ranging applications – in research areas as diverse as reaction dynamics, spectroscopy, higher harmonic generation and molecular orbital imaging, the focusing and trapping of molecules, as well as quantum simulation and computing.
The realization of rovibrationally stable dense samples of ultracold diatomic molecules remains one of the main stepping stones to achieve the next slate of major goals in the field of atomic and molecular physics. Though obtaining diatomic alkali molecules was seen as a logical next step following the optical cooling of atoms, many of the possible applications currently under investigation extend beyond atomic and molecular physics. For example, spectroscopy of ultracold molecules can help in testing extensions of the Standard Model via the search for a permanent electric dipole moment of the electron (1; 2), or the energy difference between enantiomers of chiral molecules (3). Various molecular transitions can be utilized to track the time dependence of fundamental constants, including the fine structure constant and the proton to electron mass ratio (4). They also open the way for cold and ultracold chemistry, where the interacting species and products are in a coherent quantum superposition state (5) and reactions can happen via quantum tunneling. Dipolar ultracold quantum gases promise to show a plethora of new phenomena due to anisotropic long-range dipole-dipole interactions (6). Dipolar molecules in optical lattices can be employed as a quantum simulator of condensed matter systems, and they are predicted to demonstrate new quantum phases such as a dipolar crystal, supersolid, checkerboard and collapse phases (7; 8). Ultracold polar molecules also represent an attractive platform for quantum computation (9). They offer a variety of long-lived states for qubit encoding, including rotational, spin and hyperfine (if electronic and nuclear spins are non-zero), Λ and Ω-doublet states (10) and scalability to a large number of qubits. Polar molecules can be easily controlled by DC electric and magnetic fields, as well as bymicrowave and optical fields, allowing the design of various traps (11; 12). The main appeal of polar molecules for quantum information processing, however, comes from their permanent electric dipole moment, permitting them to interact via a long-range dipole-dipole interaction. The dipole-dipole interaction offers a tool to construct two-qubit gates, required for universal quantum computation (9; 13). Ultracold molecules in their ground vibrational state v = 0 (and even in specific rotational, hyperfine or Zeeman states) are required formany of these applications since they have a large permanent electric dipole moment and are stable with respect to collisions and spontaneous emission. Currently translationally ultracold (100 nK 1 mK) molecules are produced by magneto(14) and photo-association (15) techniques. In a typical photoassociation scheme, 3
We show that the electric dipole–dipole interaction between a pair of polar molecules undergoes an all-out transformation when superimposed by a far-off-resonant optical field. The combined interaction potential becomes tunable by variation of wavelength, polarisation and intensity of the optical field and its dependence on the intermolecular separation exhibits a crossover from an inverse-power to an oscillating behaviour. The ability thereby offered to control molecular interactions opens up avenues toward the creation and manipulation of novel phases of ultracold polar gases among whose characteristics is a long-range entanglement of the dipoles' mutual orientation. We devised an accurate analytic model of such optical-field-dressed dipole–dipole interaction potentials, which enables a straightforward access to the optical-field parameters required for the design of intermolecular interactions in the laboratory.
We show that the electric dipole–dipole interaction between a pair of polar molecules undergoes an all-out transformation when superimposed by a far-off-resonant optical field. The combined interaction potential becomes tunable by variation of wavelength, polarisation and intensity of the optical field and its dependence on the intermolecular separation exhibits a crossover from an inverse-power to an oscillating behaviour. The ability thereby offered to control molecular interactions opens up avenues toward the creation and manipulation of novel phases of ultracold polar gases among whose characteristics is a long-range entanglement of the dipoles' mutual orientation. We devised an accurate analytic model of such optical-field-dressed dipole–dipole interaction potentials, which enables a straightforward access to the optical-field parameters required for the design of intermolecular interactions in the laboratory.
We show that congruent electric, magnetic and non-resonant optical fields acting concurrently on a polar paramagnetic (and polarizable) molecule offer possibilities to both amplify and control the directionality of the ensuing molecular states that surpass those available in double-field combinations or in single fields alone.At the core of these triple-field effects is the lifting of the degeneracy of the projection quantum number M by the magnetic field superimposed on the optical field and a subsequent coupling of the members of the 'doubled' (for states with ≠ M 0) tunneling doublets due to the optical field by even a weak electrostatic field.
The properties of molecule-optical elements such as lenses or prisms based on the interaction of molecules with optical fields depend in a crucial way on the molecular quantum state and its alignment created by the optical field. Herein, we consider the effects of state-dependent alignment in estimating the optical dipole force acting on the molecules and, to this end, introduce an effective polarizability which takes proper account of molecular alignment and is directly related to the alignment-dependent optical dipole force. We illustrate the significance of including molecular alignment in the optical dipole force by a trajectory study that compares previously used approximations with the present approach. The trajectory simulations were carried out for an ensemble of linear molecules subject to either propagating or standing-wave optical fields for a range of temperatures and laser intensities. The results demonstrate that the alignment-dependent effective polarizability can serve to provide correct estimates of the optical dipole force, on which a state-selection method applicable to nonpolar molecules could be based. We note that an analogous analysis of the forces acting on polar molecules subject to an inhomogeneous static electric field reveals a similarly strong dependence on molecular orientation.
Confining atoms with a combination of optical and magnetic fields has led to the formation of new states of matter and provided a tunable test bed to explore many-body atomic and electronic interactions; however, its extension to molecules has been slow. Ultracold molecules (milikelvin temperatures and below) are of interest for a number of additional applications, including studies of quantum phase transitions and precision spectroscopy. One approach to confining polar molecules has relied on inhomogeneous electric fields. Sawyer et al. present an alternative method that traps molecules magnetically. They demonstrate the technique on hydroxyl (OH) radicals, which have appreciable magnetic as well as electric dipole moments. Lifetimes in the magnetoelectrostatic trap ranged from 20 to 500 ms, depending on the background pressure. The technique allows the additional degree of freedom of an electrical field to be superimposed onto the trapped molecules and should facilitate further studies in the direction of controlled molecular collisions and chemical reactions. — ISO