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Ultracold molecules : the effect of electromagnetic fields

Alisdair O. G. Wallis

Published Jan 1, 2010• 0 citations
OpenAlex

Abstract

There is great interest within the physics and chemistry communities in the properties of ultracold molecules. Electromagnetic fields can be used to create, trap, and modify the collisional dynamics of ultracold molecules, and thus the properties of ultracold molecules in electromagnetic fields is of growing importance. This thesis examines some of the effects of externally applied electromagnetic fields on ultracold molecules. Initially, magnetic Feshbach resonances in combined electric and magnetic fields are examined in the collisions of He($^1S$)+SO($^3\Sigma^-$). Through detailed quantum scattering calculations, it is then shown that the sympathetic cooling of NH($^3\Sigma^-$) molecules with Mg atoms has a good prospect of success, a first for a neutral molecular system. Detailed quantum scattering calculations are performed for a wide range of collision energies and magnetic field strengths and it is found that the ratio of elastic to inelastic collisions is large for temperatures below 10 mK, and increases as the collision energy and magnetic field strength decrease. The near threshold collision properties of Mg+NH have been examined using a multichannel quantum defect theory approach. A new type of conical intersection, that is a function of applied electromagnetic fields only, is also demonstrated. For states of opposite parity, brought into degeneracy with a magnetic field, the degeneracy can be resolved by the addition of an electric field, forming a conical intersection. A suitable arrangement of fields could thus be used to create a conical intersection in laboratory coordinates within an ultracold trapped gas. For a Bose-Einstein condensate, in the mean-field approximation, the resultant geometric phase effect induces stable states of persistent superfluid flow that are characterized by half-integer quantized angular momentum.

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Ultracold Molecules: The E ect of Electromagnetic Fields

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There is great interest within the physics and chemistry communities in the properties of ultracold molecules. Electromagnetic fields can be used to create, trap, and modify the collisional dynamics of ultracold molecules, and thus the properties of ultracold molecules in electromagnetic fields is of growing importance. This thesis examines some of the effects of externally applied electromagnetic fields on ultracold molecules. Initially, magnetic Feshbach resonances in combined electric and magnetic fields are examined in the collisions of He(1S )+SO(3Σ−). Through detailed quantum scattering calculations, it is then shown that the sympathetic cooling of NH(3Σ−) molecules with Mg atoms has a good prospect of success, a first for a neutral molecular system. Detailed quantum scattering calculations are performed for a wide range of collision energies and magnetic field strengths and it is found that the ratio of elastic to inelastic collisions is large for temperatures below 10 mK, and increases as the collision energy and magnetic field strength decrease. The near threshold collision properties of Mg+NH have been examined using a multichannel quantum defect theory approach. A new type of conical intersection, that is a function of applied electromagnetic fields only, is also demonstrated. For states of opposite parity, brought into degeneracy with a magnetic field, the degeneracy can be resolved by the addition of an electric field, forming a conical intersection. A suitable arrangement of fields could thus be used to create a conical intersection in laboratory coordinates within an ultracold trapped gas. For a BoseEinstein condensate, in the mean-field approximation, the resultant geometric phase effect induces stable states of persistent superfluid flow that are characterized by half-integer quantized angular momentum.

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There is great interest within the physics and chemistry communities in the properties of ultracold molecules. Electromagnetic fields can be used to create, trap, and modify the collisional dynamics of ultracold molecules, and thus the properties of ultracold molecules in electromagnetic fields is of growing importance. This thesis examines some of the effects of externally applied electromagnetic fields on ultracold molecules. Initially, magnetic Feshbach resonances in combined electric and magnetic fields are examined in the collisions of He(1S^1S1S)+SO(3Σ−^3\Sigma^-3Σ−). Through detailed quantum scattering calculations, it is then shown that the sympathetic cooling of NH(3Σ−^3\Sigma^-3Σ−) molecules with Mg atoms has a good prospect of success, a first for a neutral molecular system. Detailed quantum scattering calculations are performed for a wide range of collision energies and magnetic field strengths and it is found that the ratio of elastic to inelastic collisions is large for temperatures below 10 mK, and increases as the collision energy and magnetic field strength decrease. The near threshold collision properties of Mg+NH have been examined using a multichannel quantum defect theory approach. A new type of conical intersection, that is a function of applied electromagnetic fields only, is also demonstrated. For states of opposite parity, brought into degeneracy with a magnetic field, the degeneracy can be resolved by the addition of an electric field, forming a conical intersection. A suitable arrangement of fields could thus be used to create a conical intersection in laboratory coordinates within an ultracold trapped gas. For a Bose-Einstein condensate, in the mean-field approximation, the resultant geometric phase effect induces stable states of persistent superfluid flow that are characterized by half-integer quantized angular momentum.
There is great interest within the physics and chemistry communities in the properties of ultracold molecules. Electromagnetic fields can be used to create, trap, and modify the collisional dynamics of ultracold molecules, and thus the properties of ultracold molecules in electromagnetic fields is of growing importance. This thesis examines some of the effects of externally applied electromagnetic fields on ultracold molecules. Initially, magnetic Feshbach resonances in combined electric and magnetic fields are examined in the collisions of He(1S )+SO(3Σ−). Through detailed quantum scattering calculations, it is then shown that the sympathetic cooling of NH(3Σ−) molecules with Mg atoms has a good prospect of success, a first for a neutral molecular system. Detailed quantum scattering calculations are performed for a wide range of collision energies and magnetic field strengths and it is found that the ratio of elastic to inelastic collisions is large for temperatures below 10 mK, and increases as the collision energy and magnetic field strength decrease. The near threshold collision properties of Mg+NH have been examined using a multichannel quantum defect theory approach. A new type of conical intersection, that is a function of applied electromagnetic fields only, is also demonstrated. For states of opposite parity, brought into degeneracy with a magnetic field, the degeneracy can be resolved by the addition of an electric field, forming a conical intersection. A suitable arrangement of fields could thus be used to create a conical intersection in laboratory coordinates within an ultracold trapped gas. For a BoseEinstein condensate, in the mean-field approximation, the resultant geometric phase effect induces stable states of persistent superfluid flow that are characterized by half-integer quantized angular momentum.
This Thesis describes new mechanisms for controlling elastic and inelastic collisions of ultracold atoms and molecules with static electromagnetic and laser fields. The dynamical properties of ultracold atoms are usually tuned in experiments by applying an external magnetic field to induce a Feshbach resonance. The work presented in this Thesis demonstrates the possibility of inducing and manipulating Feshbach resonances with electric fields. We discuss in detail the mechanisms of electric-field-induced resonances in ultracold mixtures of alkali metal atoms and demonstrate that electric fields may shift and split the magnetic resonances. We show that electric fields may spin up the collision complex of ultracold atoms and induce anisotropic scattering which may be exploited in experiments on many-body dynamics of ultracold gaseous mixtures. The mechanisms of electric-field-induced resonances described in this Thesis allow for two-dimensional control of inter-particle interactions, leading to total control over ultracold gases. To guide future experiments, we generate accurate interaction potentials for ultracold Li--Rb mixtures by fitting positions and widths of experimentally measured Feshbach resonances. Ultracold atomic and molecular gases can be confined by laser fields in one or two dimensions which produces an optical lattice of ultracold particles. We develop a multichannel scattering theory for collisions of atoms and molecules in two dimensions and explore the effects of the confining laser potential on inelastic and reactive collisions of ultracold atoms and molecules in a 1D optical lattice. We show that ultracold collisions can be controlled in a quasi-2D geometry by varying the orientation of a magnetic field with respect to the confinement plane normal and demonstrate that the threshold energy dependence of cross sections for inelastic collisions in an optical lattice can be tuned by varying the confining potential and the magnetic field. Our results show that applying laser confinement in one dimension may stabilize ultracold systems with large scattering lengths, which may open up interesting opportunities for studies of ultracold controlled chemistry and might lead to a new research direction of ultracold chemistry in restricted geometries.
The research field of cold and ultracold atoms and molecules is rapidly growing and expanding into different areas of research such as quantum information science and condensed matter physics. The success of this field is due to the possibility of precisely controlling and manipulating atoms and molecules at low temperatures. The progress in this field relies on the development of new methods for controlling collisional dynamics and interactions of particles with electromagnetic fields. This Thesis describes research on modification of the collisional dynamics of ultracold atoms and molecules by external laser and microwave fields as well as new methods for the detection of weak electromagnetic fields. First, we study the scattering of atoms and molecules confined in a 2D geometry by optical lattices. In particular we develop a theory for scattering in 2D and derive the equations for the threshold dependence of the collision cross sections. We show that inelastic processes and chemical reactions can be suppressed under strong confinement in one dimension and can be controlled by varying the orientation of the external field with respect to the plane of confinement. Next, we present a rigorous theory of low-temperature molecular collisions in the presence of a microwave field. The microwave field can theoretically be used to trap and control polar molecules. The molecular collisions may lead to trap loss and decoherence. We develop a rigorous quantum theory for molecular scattering in the presence of microwave fields. We study inelastic, spin-changing molecular collisions and Feshbach resonances in the presence of microwave fields. We demonstrate that inelastic collisions accompanied by absorption of microwave photons can be significant. The detection of weak electromagnetic fields is very important for various applications ranging from fundamental measurements to biomagnetic imaging, and for tests of microwave chips. We present a method for the detection of weak electromagnetic fields in a wide range of frequencies from sub-kHz to THz with ultracold polar molecules. We show that using ultracold molecules one can achieve the sensitivity of two orders of magnitude larger than with a similar method based on ultracold Rb atoms.
For two states of opposite parity that cross as a function of an external magnetic field, the addition of an electric field will break the symmetry and induce an avoided crossing. A suitable arrangement of fields may be used to create a conical intersection as a function of external spatial coordinates. We consider the effect of the resulting geometric phase for ultracold polar molecules. For a Bose-Einstein condensate in the mean-field approximation, the geometric phase effect induces stable states of persistent superfluid flow that are characterized by half-integer quantized angular momentum.
This article reviews the current state of the art in the field of cold and ultracold molecules and demonstrates that chemical reactions, inelastic collisions and dissociation of molecules at subkelvin temperatures can be manipulated with external electric or magnetic fields. The creation of ultracold molecules may allow for spectroscopy measurements with extremely high precision and tests of fundamental symmetries of nature, quantum computation with molecules as qubits, and controlled chemistry. The probability of chemical reactions and collisional energy transfer can be very large at temperatures near zero kelvin. The collision energy of ultracold atoms and molecules is much smaller than perturbations due to interactions with external electric or magnetic fields available in the laboratory. External fields may therefore be used to induce dissociation of weakly bound molecules, stimulate forbidden electronic transitions, suppress the effect of centrifugal barriers in outgoing reaction channels or tune Feshbach resonances that enhance chemical reactivity.
We present an accurate quantum mechanical study of molecule–molecule collisions in the presence of a magnetic field. The work focuses on the analysis of elastic scattering and spin relaxation in collisions of O 2 ( 3 Σ g – ) molecules at cold (∼0.1 K) and ultracold (∼10 –6 K) temperatures. Our calculations show that magnetic spin relaxation in molecule–molecule collisions is extremely efficient except at magnetic fields below 1 mT. The rate constant for spin relaxation at T =0.1 K and a magnetic field of 0.1 T is found to be as large as 6.1 × 10 –11 cm –3 s –1 . The magnetic field dependence of elastic and inelastic scattering cross sections at ultracold temperatures is dominated by a manifold of Feshbach resonances with the density of ∼100 resonances per Tesla for collisions of molecules in the absolute ground state. This suggests that the scattering length of ultracold molecules in the absolute ground state can be effectively tuned in a very wide range of magnetic fields. Our calculations demonstrate that the number and properties of the magnetic Feshbach resonances are dramatically different for molecules in the absolute ground and excited spin states. The density of Feshbach resonances for molecule–molecule scattering in the low-field-seeking Zeeman state is reduced by a factor of 10.