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Physical Review A

Molecular cooling via Sisyphus processes

D. Comparat

Published Apr 14, 2014• 41 citations
Publisher

Abstract

We present a study of Sisyphus cooling of molecules: The scattering of a single photon removes a substantial amount of the molecular kinetic energy and an optical pumping step allows one to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperatures. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase-space density by a factor of 10${}^{7}$. Even in the case of molecules with both low Franck-Condon coefficients and a nonclosed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperatures in a few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam.

DOI
10.1103/physreva.89.043410

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A Study of molecular cooling via Sisyphus processes

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We present a study of Sisyphus cooling of molecules: the scattering of a single-photon remove a substantial amount of the molecular kinetic energy and an optical pumping step allow to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperature. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using Kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase space density by a factor of 10^7 . Even in the case of molecules with both low Franck-Condon coefficients and a non-closed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperature in few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam

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Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.

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In this thesis, I study optical pumping as a powerful cooling tool for trapped ultra-cold atoms in a highly collisional regime. First application of optical pumping is a continuous loading scheme used to transfer atoms from a guided beam into a hybrid trap. Further, I introduce a Sisyphus cooling scheme based on radio-frequency transitions and optical pumping, operating simultaneously to the accumulation of atoms in the trap. The combined scheme of continuous loading and Sisyphus cooling is demonstrated for a large range of initial conditions of the guided atoms. Thereby, I show that collisional thermalization occurs in a steady-state for almost arbitrary initial conditions, provided that the first dissipative step is able to prevent the atom from leaving the trap during its first passage. On the one hand, this scheme could be applied to a wide range of atomic or molecular beams. On the other hand, phase-space density of 4*10^-4 is reached in a continuous operation mode with chromium atoms. In the second part, I investigate demagnetization cooling based on dipolar relaxation collisions driving the thermalization of the internal (spin) and the external (motional) degrees of freedom. In the case of a gas, one has the advantage that the spin degree of freedom can be cooled very efficiently using optical pumping. It is shown, that demagnetization cooling of a gas is more efficient than evaporation cooling in terms of phase-space density gain versus loss of atoms. This allows reaching a temperature of 6uK at a phase-space density of 0.03. It is observed, that both, continuous Sisyphus cooling and demagnetization cooling are limited by a density dependent loss mechanism. I present circumstantial evidence for excited-state collisions as the dominant limiting process. Finally, I discuss possible extensions to the current experimental procedures, possibly allowing reaching quantum degeneracy by optical means only.

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Abstract We propose a promising scheme to prepare ultracold MgF molecules from a slowed cold molecular beam by using three-dimensional pure intensity-gradient induced Sisyphus cooling. The cooling is based on a blue-detuned localized hollow beam and a weak repumping beam. We investigate the dynamic process in the trap with the method of the Monte-Carlo simulations, verifying the feasibility. Our results show that achieving sub-Doppler temperature should be possible in such a well-designed trap; the trapped MgF molecules with initial temperature of 1 mK can be directly cooled to the final equilibrium temperature of about 46.5 μ K , well below the Doppler limit (about 527.9 μ K for MgF); meanwhile, molecules with initial temperature of 14 mK can be even cooled to about 68.7 μ K .

New Journal of Physics•Feb 3, 2020•18 citations
We present a study of Sisyphus cooling of molecules: The scattering of a single photon removes a substantial amount of the molecular kinetic energy and an optical pumping step allows one to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperatures. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase-space density by a factor of 107{}^{7}7. Even in the case of molecules with both low Franck-Condon coefficients and a nonclosed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperatures in a few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam.
We present a study of Sisyphus cooling of molecules: the scattering of a single-photon remove a substantial amount of the molecular kinetic energy and an optical pumping step allow to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperature. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using Kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase space density by a factor of 10^7 . Even in the case of molecules with both low Franck-Condon coefficients and a non-closed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperature in few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam
Ultracold molecular gases are promising as an avenue to rich many-body physics, quantum chemistry, quantum information, and precision measurements. This richness, which flows from the complex internal structure of molecules, makes the creation of ultracold molecular gases using traditional methods (laser plus evaporative cooling) a challenge, in particular due to the spontaneous decay of molecules into dark states. We propose a way to circumvent this key bottleneck using an all-optical method for decelerating molecules using stimulated absorption and emission with a single ultrafast laser. We further describe single-photon cooling of the decelerating molecules that exploits their high dark state pumping rates, turning the principal obstacle to molecular laser cooling into an advantage. Cooling and deceleration may be applied simultaneously and continuously to load molecules into a trap. We discuss implementation details including multilevel numerical simulations of strontium monohydride. These techniques are applicable to a large number of molecular species and atoms with the only requirement being an electric dipole transition that can be accessed with an ultrafast laser.
Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.
In this thesis, I study optical pumping as a powerful cooling tool for trapped ultra-cold atoms in a highly collisional regime. First application of optical pumping is a continuous loading scheme used to transfer atoms from a guided beam into a hybrid trap. Further, I introduce a Sisyphus cooling scheme based on radio-frequency transitions and optical pumping, operating simultaneously to the accumulation of atoms in the trap. The combined scheme of continuous loading and Sisyphus cooling is demonstrated for a large range of initial conditions of the guided atoms. Thereby, I show that collisional thermalization occurs in a steady-state for almost arbitrary initial conditions, provided that the first dissipative step is able to prevent the atom from leaving the trap during its first passage. On the one hand, this scheme could be applied to a wide range of atomic or molecular beams. On the other hand, phase-space density of 4*10^-4 is reached in a continuous operation mode with chromium atoms. In the second part, I investigate demagnetization cooling based on dipolar relaxation collisions driving the thermalization of the internal (spin) and the external (motional) degrees of freedom. In the case of a gas, one has the advantage that the spin degree of freedom can be cooled very efficiently using optical pumping. It is shown, that demagnetization cooling of a gas is more efficient than evaporation cooling in terms of phase-space density gain versus loss of atoms. This allows reaching a temperature of 6uK at a phase-space density of 0.03. It is observed, that both, continuous Sisyphus cooling and demagnetization cooling are limited by a density dependent loss mechanism. I present circumstantial evidence for excited-state collisions as the dominant limiting process. Finally, I discuss possible extensions to the current experimental procedures, possibly allowing reaching quantum degeneracy by optical means only.
A laser-cooling scheme for molecules is presented based on repeated cycle of zero-velocity selection, deceleration, and irreversible accumulation. Although this scheme also employs a single spontaneous emission as in [Raymond Ooi, Marzlin, and Audretsch, Eur. Phys. J. D 22, 259 (2003)], in order to circumvent the difficulty of maintaining closed pumping cycles in molecules, there are two distinct features which make the cooling process of this scheme faster and more practical. First, the zero-velocity selection creates a narrow velocity-width population with zero mean velocity, such that no further deceleration (with many stimulated Raman adiabatic passage (STIRAP) pulses) is required. Second, only two STIRAP processes are required to decelerate the remaining hot molecular ensemble to create a finite population around zero velocity for the next cycle. We present a setup to realize the cooling process in one dimension with trapping in the other two dimensions using a Stark barrel. Numerical estimates of the cooling parameters and simulations with density matrix equations using OH molecules show the applicability of the cooling scheme. For a gas at temperature T=1T=1T=1 K, the estimated cooling time is only 222 ms, with phase-space density increased by about 30 times. The possibility of extension to three-dimensional cooling via thermalization is also discussed.
Abstract We propose a promising scheme to prepare ultracold MgF molecules from a slowed cold molecular beam by using three-dimensional pure intensity-gradient induced Sisyphus cooling. The cooling is based on a blue-detuned localized hollow beam and a weak repumping beam. We investigate the dynamic process in the trap with the method of the Monte-Carlo simulations, verifying the feasibility. Our results show that achieving sub-Doppler temperature should be possible in such a well-designed trap; the trapped MgF molecules with initial temperature of 1 mK can be directly cooled to the final equilibrium temperature of about 46.5 μ K , well below the Doppler limit (about 527.9 μ K for MgF); meanwhile, molecules with initial temperature of 14 mK can be even cooled to about 68.7 μ K .