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Dipolar collisions in cooling and trapping of paramagnetic atoms

Zoran Miroslav Pavlovic

Published Jan 1, 2011• 1 citation
OpenAlex

Abstract

In this dissertation, I present ab initio theoretical results on cold and ultra-cold collision of atomic and molecular systems with magnetic and electric dipole moments. The collisions of different isotopes of maximally spin-polarized chromium atoms (52Cr and 53Cr), alkali-metal atom (Rb) - chromium atom, and magnetically trapped hydroxide (OH) with cold supersonic helium beam are considered in this thesis. Spin-changing cross sections and rate constants in Cr-Cr isotopic collision in the presence of a magnetic field are calculated by propagating a set of multichannel equations in the field. The coupling between dipole-dipole allowed and hyperfine channels are included. The short range electrostatic interactions between atoms and atom-molecule are represented with highly-accurate Born-Oppenheimer (BO) potential energy curves. Due to the large spin multiplicity in Cr-Cr and Rb-Cr interactions, more than the usual singlet and triplet channels are obtained. The long-range van der Waals (vdW) interactions between atoms are calculated, for Cr, by including accurate transition frequencies, discrete dipole matrix elements, and photoionization continuum oscillator strengths, and for Rb, using published dynamic polarizabilities. The vdW coefficients for Cr-Cr and Rb-Cr are obtained. In the cold collision regime, I investigate the influence of angular momentum shape resonances on the elastic and inelastic (loss channel) rate coefficients, and when the Zeeman relaxation, resulting in the loss of atoms from the trap, dominates elastic collision. Dipolar collisions are crucial to achieving quantum degeneracy. Magnetically tuned Fano-Feshbach closed-channel resonances are used to obtain zero-energy scattering lengths in comparison with observation of trap loss. In bosonic chromium collisions, resonances appear due only to dipolar interaction. The interplay between hyperfine and dipolar resonances in mixed-species Cr-Cr and Rb-Cr collisions is studied. In Rb-Cr, it is found that the molecule has broken symmetry and therefore contains a large permanent electric dipole moment in the ground state. A recent collisional experiment at JILA of a supersonic helium beam with a magnetically trapped OH radical found the onset of a quantum threshold in the total OH loss rate. Using ab initio BO energy surfaces, I calculated the spin-changing collisions which removed OH from the trap. Only after including the effect of the trapping potential on the collision dynamics, some agreement with observation was found. ^

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Collisional properties of a dipolar gas of ultracold chromium atoms

S. Hensler, Piet O. Schmidt, J. Werner +3 more

Temperature dependence of the cross-section for elastic ground-state collisions of /sup 52/Cr- and /sup 50/Cr-atoms using the method of cross-dimensional relaxation, respectively is determined. The corresponding absolute values of the scattering length are on the order of 100a/sub 0/ for /sup 52/Cr and /sup 50/a/sub 0/ for /sup 50/Cr, respectively. However, to use evaporative cooling to increase the phase space density and achieve Bose-Einstein condensation with chromium atoms, have been limited to values below 10/sup -2/. Unusuually high inelastic collisio rates due to dipolar relaxation cause atom loss and heating of the sample. These losses are investigated and found similar magnetic-field-dependent rate coefficients (/spl ap/10/sup -11/ cm/sup 3//s @ 50 G offset field) for the two isotopes /sup 50/Cr and /sup 52/Cr indicating that the strongly enhanced dipolar relaxation is a generic feature of the dipole-dipole interaction. This conclusion is supported by theoretical calculations. To circumvent these losses, an optical dipole trap is currently being set up. Here, chromium can be trapped in the energetically lowest state where dipolar relaxation is absent.

European Quantum Electronics Conference (EQEC)•Jan 1, 2003•0 citations

Cold Polar Molecules for Novel Collision Experiments at Low Energies

Brian C. Sawyer

Research in the field of cold polar molecules is progressing rapidly. An array of interesting\ntopics is being developed including precision measurement and fundamental tests, quantum phase transitions, and ultracold chemistry. In particular, dipolar molecules in well-defined quantum states enable exquisite control of their interactions via applied electric fields. The long-range, anisotropic interaction between dipolar molecules leads to new collision dynamics that could be used for novel collective effects, quantum state engineering, and information processing. The focus of this Thesis is the production of cold samples of neutral OH molecules via Stark deceleration and magnetic trapping for novel collision experiments. This novelty results from our combination of cold external beams and trapped target molecules which facilitates observation of dipolar effects as well as low temperature collision resonances. The large permanent electric dipole moment of OH allows us to precisely tune the lab-frame velocity of the molecular packets from ∼ 500 m/s to rest. We have magnetically trapped OH packets at the terminus of our Stark decelerator at a temperature of 70 mK and density of 106 cm−3. With improved understanding of Stark deceleration, we optimize the decelerator efficiency and its coupling to the magnetic trap. Our latest trap design uses permanent ring magnets to create a three-dimensional magnetic quadrupole field. Use of magnetically trapped OH molecules for collision experiments with external beams allow us the unique opportunity of observing both elastic and inelastic collisions. In addition, the trap confinement yields sensitivity to differential elastic cross sections at low collision energies. This open magnetic trap has allowed measurement of collision cross sections between trapped OH and external supersonic beams of He and D2, the latter of which is of astrophysical interest due to the role of H2-OH collisions in pumping interstellar OH megamasers. The combination of trapped OH molecules and temperature tuned beams of He and D2 has facilitated measurement of the lowest-energy D2-OH collision cross sections yet reported. More recently, we report the first observation of electric-field dependent cross sections between two different species of cold polar molecules - OH and ND3 - thereby demonstrating control over molecular scattering in the cold regime. By combining for the first time the production techniques of Stark deceleration and buffer gas cooling, we increase the molecular interaction time by∼ 105 over traditional crossed-beam experiments to gain enhanced sensitivity at the characteristic densities of cold molecule production.

•Jan 1, 2010•2 citations

Cold magnetically trapped 2Dg scandium atoms. II. Scattering dynamics

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Scattering properties of ultra-cold chromium atoms

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In this work a gas of ultra-cold chromium atoms in a magnetic trap has been prepared and its elastic and inelastic scattering properties have been investigated with regard to Bose-Einstein condensation. Bose-Einstein condensation of dilute atomic gases is achieved using different cooling and trapping techniques. Deviating from the standard way we were able to devise a continuous loading mechanism for a magnetic trap as a result of the spectroscopic properties and the large magnetic dipole moment of chromium. It not only allows us to trap more atoms but also facilitates the subsequent preparation steps. After loading, the magnetic trap is compressed to increase the atomic density. In doing so we also increases the temperature of the atomic cloud. Doppler cooling of the atoms in the compressed trap reduces the temperature and increases the density. Subsequent evaporative cooling further reduces the temperature. The efficiency of the cooling mechanism is determined by the elastic and inelastic scattering properties of atomic species. Ultra-cold collisions between ground state atoms are dominated by s-wave collisions. They are characterized by a single parameter, the scattering length a. We were able to determine the temperature dependence of the elastic collision rate for the two bosonic isotopes 52Cr and 50Cr in a relaxation experiment. Comparing our results with the effective range theory allowed us not only to extract the magnitude of the scattering length, but also its sign. The sign of the scattering length is important since only condensates with a positive scattering length are stable. Our efforts to achieve Bose-Einstein condensation in chromium by evaporative cooling in a magnetic trap resulted in a maximum phase space density of 0.04. Further cooling reduced the phase space density due to increased loss of atoms from dipolar relaxation. We were able to obtain preliminary results on the magnetic field dependence of dipolar relaxation. Our experimental data is in excellent agreement with theory. These experiments confirm the theoretical prediction that the dipolar relaxation rate is independent from the details of the interaction potential but rather scales with the magnetic offset field and the magnetic dipole moment of the atoms. The findings of this work mark an important step towards the realization of a Bose-Einstein condensate with chromium atoms. Especially the knowledge of the elastic and inelastic scattering properties allow now to devise a successful strategy.

•Jan 1, 2003•5 citations

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Rigorous calculations of magnetic Feshbach resonances and Zeeman relaxation cross sections in an ultracold and cold chromium gas are reported. This work presents the calculation of such inelastic processes in collisions of atoms with large magnetic moments. Using our recently constructed accurate interaction potentials for the chromium dimer, we compute the positions and widths of magnetically tuned resonances in an optically trapped ultracold Cr gas. We find good agreement with recent experimental data and report that spin-change collision cross sections quickly increase with decreasing collision energy and magnetic-field strength at energies below 1 K and magnetic fields larger than 40 G.

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Interactions and collisions of cold molecules: lithium + lithium dimer

Marko T. Cvitaš

There is at present great interest in the properties of ultracold molecules. Molecules are created in traps in excited rovibrational states and any vibrational relaxation results in the trap loss. This thesis provides a theoretical study of interactions and collisions in the spin-polarized lithium -b lithium dimer system at ultralow energies. Potential energy surface of the electronic quartet ground state of lithium trimer is generated ab initio using the CCSD(T) method and represented by an IMLS/Shepard fit. Long-range nonadditive interactions are modelled using a symmetric global form with coefficients taken from a fit to the atom-molecule dispersion coefficients. The surface allows barrierless atom-exchange reactions. It has a global minimum of ≈ 4000 cm(^-1) at equilateral geometries with r(_e) = 3.1 Å. The nonadditive interactions are very strong near equilibrium. They increase the well depth by a factor of 4 and reduce the interatomic distance by ≈ 1 Å. Another surface of À symmetry in C(_s) meets the ground state surface at linear geometries at short range. Part of the seam, near D(_ooh) geometries, is in an energetically accessible region for cold collisions. Inside the seam, the lowest À surface correlates with (^4)II rather than (^4)Σ state. Inelastic and reactive collisions are investigated using a quantum mechanical coupled channel method in hyperspherical coordinates. Bosonic and fermionic systems in the spin-stretched states are considered. The inelastic rate coefficients from the rovibrationally excited states of dimer at ultralow collision energies are large, often above 10-(^-10) cm(^3)s(^-1) The elastic cross sections are ≈ 3 orders of magnitude lower at 1 nK. Atom-molecule mixtures, at the densities found in Bose-Einstein condensates of alkali metal atoms that were recently produced, would last only a fraction of a second. Classical Langevin model describes semi-quantitatively the energy dependence of inelastic cross sections above ≈ 50 mK. No systematic differences between the bosonic and fermionic systems were found. Sensitivity of the results on potential was investigated. Reactions in isotopic mixtures of lithium may be exothermic even from the molecular ground state. The reactive rate coefficients are 1 - 2 orders of magnitude smaller than those in systems involving an initially vibrationally excited dimer.

•Jan 1, 2004•0 citations
In this dissertation, I present ab initio theoretical results on cold and ultra-cold collision of atomic and molecular systems with magnetic and electric dipole moments. The collisions of different isotopes of maximally spin-polarized chromium atoms (52Cr and 53Cr), alkali-metal atom (Rb) - chromium atom, and magnetically trapped hydroxide (OH) with cold supersonic helium beam are considered in this thesis. Spin-changing cross sections and rate constants in Cr-Cr isotopic collision in the presence of a magnetic field are calculated by propagating a set of multichannel equations in the field. The coupling between dipole-dipole allowed and hyperfine channels are included. The short range electrostatic interactions between atoms and atom-molecule are represented with highly-accurate Born-Oppenheimer (BO) potential energy curves. Due to the large spin multiplicity in Cr-Cr and Rb-Cr interactions, more than the usual singlet and triplet channels are obtained. The long-range van der Waals (vdW) interactions between atoms are calculated, for Cr, by including accurate transition frequencies, discrete dipole matrix elements, and photoionization continuum oscillator strengths, and for Rb, using published dynamic polarizabilities. The vdW coefficients for Cr-Cr and Rb-Cr are obtained. In the cold collision regime, I investigate the influence of angular momentum shape resonances on the elastic and inelastic (loss channel) rate coefficients, and when the Zeeman relaxation, resulting in the loss of atoms from the trap, dominates elastic collision. Dipolar collisions are crucial to achieving quantum degeneracy. Magnetically tuned Fano-Feshbach closed-channel resonances are used to obtain zero-energy scattering lengths in comparison with observation of trap loss. In bosonic chromium collisions, resonances appear due only to dipolar interaction. The interplay between hyperfine and dipolar resonances in mixed-species Cr-Cr and Rb-Cr collisions is studied. In Rb-Cr, it is found that the molecule has broken symmetry and therefore contains a large permanent electric dipole moment in the ground state. A recent collisional experiment at JILA of a supersonic helium beam with a magnetically trapped OH radical found the onset of a quantum threshold in the total OH loss rate. Using ab initio BO energy surfaces, I calculated the spin-changing collisions which removed OH from the trap. Only after including the effect of the trapping potential on the collision dynamics, some agreement with observation was found. ^
Temperature dependence of the cross-section for elastic ground-state collisions of /sup 52/Cr- and /sup 50/Cr-atoms using the method of cross-dimensional relaxation, respectively is determined. The corresponding absolute values of the scattering length are on the order of 100a/sub 0/ for /sup 52/Cr and /sup 50/a/sub 0/ for /sup 50/Cr, respectively. However, to use evaporative cooling to increase the phase space density and achieve Bose-Einstein condensation with chromium atoms, have been limited to values below 10/sup -2/. Unusuually high inelastic collisio rates due to dipolar relaxation cause atom loss and heating of the sample. These losses are investigated and found similar magnetic-field-dependent rate coefficients (/spl ap/10/sup -11/ cm/sup 3//s @ 50 G offset field) for the two isotopes /sup 50/Cr and /sup 52/Cr indicating that the strongly enhanced dipolar relaxation is a generic feature of the dipole-dipole interaction. This conclusion is supported by theoretical calculations. To circumvent these losses, an optical dipole trap is currently being set up. Here, chromium can be trapped in the energetically lowest state where dipolar relaxation is absent.
Research in the field of cold polar molecules is progressing rapidly. An array of interesting\ntopics is being developed including precision measurement and fundamental tests, quantum phase transitions, and ultracold chemistry. In particular, dipolar molecules in well-defined quantum states enable exquisite control of their interactions via applied electric fields. The long-range, anisotropic interaction between dipolar molecules leads to new collision dynamics that could be used for novel collective effects, quantum state engineering, and information processing. The focus of this Thesis is the production of cold samples of neutral OH molecules via Stark deceleration and magnetic trapping for novel collision experiments. This novelty results from our combination of cold external beams and trapped target molecules which facilitates observation of dipolar effects as well as low temperature collision resonances. The large permanent electric dipole moment of OH allows us to precisely tune the lab-frame velocity of the molecular packets from ∼ 500 m/s to rest. We have magnetically trapped OH packets at the terminus of our Stark decelerator at a temperature of 70 mK and density of 106 cm−3. With improved understanding of Stark deceleration, we optimize the decelerator efficiency and its coupling to the magnetic trap. Our latest trap design uses permanent ring magnets to create a three-dimensional magnetic quadrupole field. Use of magnetically trapped OH molecules for collision experiments with external beams allow us the unique opportunity of observing both elastic and inelastic collisions. In addition, the trap confinement yields sensitivity to differential elastic cross sections at low collision energies. This open magnetic trap has allowed measurement of collision cross sections between trapped OH and external supersonic beams of He and D2, the latter of which is of astrophysical interest due to the role of H2-OH collisions in pumping interstellar OH megamasers. The combination of trapped OH molecules and temperature tuned beams of He and D2 has facilitated measurement of the lowest-energy D2-OH collision cross sections yet reported. More recently, we report the first observation of electric-field dependent cross sections between two different species of cold polar molecules - OH and ND3 - thereby demonstrating control over molecular scattering in the cold regime. By combining for the first time the production techniques of Stark deceleration and buffer gas cooling, we increase the molecular interaction time by∼ 105 over traditional crossed-beam experiments to gain enhanced sensitivity at the characteristic densities of cold molecule production.
The binary collision dynamics of 2Dg,3/2{}^{2}{D}_{g,3/2}2Dg,3/2​ ground state scandium atoms is studied from first principles. We employ 30 coupled diabatic ab initio potentials in a coupled-channels study of the scattering dynamics of cold and ultracold scandium atoms in external magnetic fields. Due to the long-ranged magnetic dipolar interaction, the field dependence of the cross section does not follow the threshold laws derived by Volpi and Bohn [Phys. Rev. A 65, 052712 (2002)]. In the field-free case, the near-threshold cross section is independent of the collision energy, and hence the cross section does not follow the well-established Wigner threshold laws. The observed threshold behavior is explained in the Born approximation. For energies above $1\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}$, inelastic collisions are driven by the anisotropic nonrelativistic electronic interaction. For energies below $100\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}$, the ratio of elastic-to-inelastic collisions is likely to be favorable for evaporative cooling. Both anisotropy in the long-range interaction and in the short-range potential contribute to large cross sections for inelastic collisions at higher energies and lead to a small ratio of elastic-to-inelastic collisions. This is in agreement with the large rates for Zeeman relaxation of submerged-shell atoms observed experimentally. The effect of the uncertainty in the ab initio potential is sampled by scaling the reduced mass and is found to have little influence on the conclusions drawn from this work.
In this work a gas of ultra-cold chromium atoms in a magnetic trap has been prepared and its elastic and inelastic scattering properties have been investigated with regard to Bose-Einstein condensation. Bose-Einstein condensation of dilute atomic gases is achieved using different cooling and trapping techniques. Deviating from the standard way we were able to devise a continuous loading mechanism for a magnetic trap as a result of the spectroscopic properties and the large magnetic dipole moment of chromium. It not only allows us to trap more atoms but also facilitates the subsequent preparation steps. After loading, the magnetic trap is compressed to increase the atomic density. In doing so we also increases the temperature of the atomic cloud. Doppler cooling of the atoms in the compressed trap reduces the temperature and increases the density. Subsequent evaporative cooling further reduces the temperature. The efficiency of the cooling mechanism is determined by the elastic and inelastic scattering properties of atomic species. Ultra-cold collisions between ground state atoms are dominated by s-wave collisions. They are characterized by a single parameter, the scattering length a. We were able to determine the temperature dependence of the elastic collision rate for the two bosonic isotopes 52Cr and 50Cr in a relaxation experiment. Comparing our results with the effective range theory allowed us not only to extract the magnitude of the scattering length, but also its sign. The sign of the scattering length is important since only condensates with a positive scattering length are stable. Our efforts to achieve Bose-Einstein condensation in chromium by evaporative cooling in a magnetic trap resulted in a maximum phase space density of 0.04. Further cooling reduced the phase space density due to increased loss of atoms from dipolar relaxation. We were able to obtain preliminary results on the magnetic field dependence of dipolar relaxation. Our experimental data is in excellent agreement with theory. These experiments confirm the theoretical prediction that the dipolar relaxation rate is independent from the details of the interaction potential but rather scales with the magnetic offset field and the magnetic dipole moment of the atoms. The findings of this work mark an important step towards the realization of a Bose-Einstein condensate with chromium atoms. Especially the knowledge of the elastic and inelastic scattering properties allow now to devise a successful strategy.
Rigorous calculations of magnetic Feshbach resonances and Zeeman relaxation cross sections in an ultracold and cold chromium gas are reported. This work presents the calculation of such inelastic processes in collisions of atoms with large magnetic moments. Using our recently constructed accurate interaction potentials for the chromium dimer, we compute the positions and widths of magnetically tuned resonances in an optically trapped ultracold Cr gas. We find good agreement with recent experimental data and report that spin-change collision cross sections quickly increase with decreasing collision energy and magnetic-field strength at energies below 1 K and magnetic fields larger than 40 G.
There is at present great interest in the properties of ultracold molecules. Molecules are created in traps in excited rovibrational states and any vibrational relaxation results in the trap loss. This thesis provides a theoretical study of interactions and collisions in the spin-polarized lithium -b lithium dimer system at ultralow energies. Potential energy surface of the electronic quartet ground state of lithium trimer is generated ab initio using the CCSD(T) method and represented by an IMLS/Shepard fit. Long-range nonadditive interactions are modelled using a symmetric global form with coefficients taken from a fit to the atom-molecule dispersion coefficients. The surface allows barrierless atom-exchange reactions. It has a global minimum of ≈ 4000 cm(^-1) at equilateral geometries with r(_e) = 3.1 Å. The nonadditive interactions are very strong near equilibrium. They increase the well depth by a factor of 4 and reduce the interatomic distance by ≈ 1 Å. Another surface of À symmetry in C(_s) meets the ground state surface at linear geometries at short range. Part of the seam, near D(_ooh) geometries, is in an energetically accessible region for cold collisions. Inside the seam, the lowest À surface correlates with (^4)II rather than (^4)Σ state. Inelastic and reactive collisions are investigated using a quantum mechanical coupled channel method in hyperspherical coordinates. Bosonic and fermionic systems in the spin-stretched states are considered. The inelastic rate coefficients from the rovibrationally excited states of dimer at ultralow collision energies are large, often above 10-(^-10) cm(^3)s(^-1) The elastic cross sections are ≈ 3 orders of magnitude lower at 1 nK. Atom-molecule mixtures, at the densities found in Bose-Einstein condensates of alkali metal atoms that were recently produced, would last only a fraction of a second. Classical Langevin model describes semi-quantitatively the energy dependence of inelastic cross sections above ≈ 50 mK. No systematic differences between the bosonic and fermionic systems were found. Sensitivity of the results on potential was investigated. Reactions in isotopic mixtures of lithium may be exothermic even from the molecular ground state. The reactive rate coefficients are 1 - 2 orders of magnitude smaller than those in systems involving an initially vibrationally excited dimer.