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Frontiers in Optics

Laser Cooling of a Diatomic Molecule

David P. DeMille, E.S. Shuman, John F. Barry

Published Jan 1, 2010• 22 citations
Publisher

Abstract

We report experiments demonstrating the laser cooling of a diatomic molecule. A cryogenic molecular beam of strontium monofluoride (SrF) is subjected to one-dimensional transverse laser cooling. We observe both Doppler and Sisyphus-type cooling mechanisms.
DOI
10.1364/ls.2010.lthh1

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Laser Cooling and Slowing of a Diatomic Molecule

John F. Barry

Laser cooling and trapping are central to modern atomic physics. It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields and a number of Nobel prizes. Prior to the work presented in this thesis, laser cooling had not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. The first direct laser cooling of a molecule and further results we present here provide a new route to ultracold temperatures for molecules. In particular, these methods bridge the gap between ultracold temperatures and the approximately 1 kelvin temperatures attainable with directly cooled molecules (e.g. with cryogenic buffer gas cooling or decelerated supersonic beams). Using the carefully chosen molecule strontium monofluoride (SrF), decays to unwanted vibrational states are suppressed. Driving a transition with rotational quantum number R=1 to an excited state with R'=0 eliminates decays to unwanted rotational states. The dark ground-state Zeeman sublevels present in this specific scheme are remixed via a static magnetic field. Using three lasers for this scheme, a given molecule should undergo an average of approximately 100,000 photon absorption/emission cycles before being lost via unwanted decays. This number of cycles should be sufficient to load a magneto-optical trap (MOT) of molecules. In this thesis, we demonstrate transverse cooling of an SrF beam, in both Doppler and a Sisyphus-type cooling regimes. We also realize longitudinal slowing of an SrF beam. Finally, we detail current progress towards trapping SrF in a MOT. Ultimately, this technique should enable the production of large samples of molecules at ultracold temperatures for molecules chemically distinct from competing methods.

•Dec 1, 2013•21 citations

Transverse Laser Cooling of SrF

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This thesis discusses an experiment, which has demonstrated transverse laser cooling of a pulsed supersonic beam of strontium monofluoride (SrF) molecules. Producing ultracold molecules is important because they could advance many fields including many-body physics, quantum chemistry and precision measurements to explore fundamental forces in nature. Direct laser cooling of molecules is a new and promising way to produce molecules with temperatures in the sub-millikelvin range. In the experiment, SrF molecules produced from a pulsed supersonic source were cooled in the transverse direction using light from just two lasers. The molecular beam brightness was increased by about 20%. I discuss the detailed experimental setup, laser system and data analysis. I also present several theoretical models, which give insight into the cooling experiment. Finally, I discuss improvements to this experiment, which should enable higher yields of ultracold molecules to be produced.

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We perform magnetically assisted Sisyphus laser cooling of the triatomic free radical strontium monohydroxide (SrOH). This is achieved with principal optical cycling in the rotationally closed P(N^{''}=1) branch of either the X[over ˜]^{2}Σ^{+}(000)↔A[over ˜]^{2}Π_{1/2}(000) or the X[over ˜]^{2}Σ^{+}(000)↔B[over ˜]^{2}Σ^{+}(000) vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the B[over ˜](000) state for both the (100) level of the Sr-O stretching mode and the (02^{0}0) level of the bending mode. The transverse temperature of a SrOH molecular beam is reduced in one dimension by 2 orders of magnitude to ∼750 μK. This approach opens a path towards creating a variety of ultracold polyatomic molecules by means of direct laser cooling.

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Towards Ultracold Chiral Molecules

Timur A. Isaev, Robert Berger

Atoms can be cooled and trapped efficiently with the help of lasers. So-called Doppler cooling takes advantage of momentum transfer upon absorption and emission of photons and of Doppler shifts to facilitate effectively closed optical absorption-emission loops, by which atoms are slowed down and cooled. Due to the wealth of internal degrees of freedom accessible in molecules, it was assumed for a long time that similarly closed optical loops cannot be realised for molecules. After an early theoretical proposal by Di Rosa for diatomic molecules, such cooling has been achieved in this decade for SrF, YO, CaF and YbF. It has been outlined recently that also polyatomic molecules should be coolable with lasers and classes of molecules expected to be amenable to this have been proposed by the present authors. Experimental success in laser cooling of SrOH has been reported. The status of cooling polyatomic molecules with lasers and the prospects for obtaining ultracold chiral molecules is reviewed herein.

CHIMIA International Journal for Chemistry•Jun 26, 2018•14 citations
Laser cooling and trapping are central to modern atomic physics. It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields and a number of Nobel prizes. Prior to the work presented in this thesis, laser cooling had not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. The first direct laser cooling of a molecule and further results we present here provide a new route to ultracold temperatures for molecules. In particular, these methods bridge the gap between ultracold temperatures and the approximately 1 kelvin temperatures attainable with directly cooled molecules (e.g. with cryogenic buffer gas cooling or decelerated supersonic beams). Using the carefully chosen molecule strontium monofluoride (SrF), decays to unwanted vibrational states are suppressed. Driving a transition with rotational quantum number R=1 to an excited state with R'=0 eliminates decays to unwanted rotational states. The dark ground-state Zeeman sublevels present in this specific scheme are remixed via a static magnetic field. Using three lasers for this scheme, a given molecule should undergo an average of approximately 100,000 photon absorption/emission cycles before being lost via unwanted decays. This number of cycles should be sufficient to load a magneto-optical trap (MOT) of molecules. In this thesis, we demonstrate transverse cooling of an SrF beam, in both Doppler and a Sisyphus-type cooling regimes. We also realize longitudinal slowing of an SrF beam. Finally, we detail current progress towards trapping SrF in a MOT. Ultimately, this technique should enable the production of large samples of molecules at ultracold temperatures for molecules chemically distinct from competing methods.
This thesis discusses an experiment, which has demonstrated transverse laser cooling of a pulsed supersonic beam of strontium monofluoride (SrF) molecules. Producing ultracold molecules is important because they could advance many fields including many-body physics, quantum chemistry and precision measurements to explore fundamental forces in nature. Direct laser cooling of molecules is a new and promising way to produce molecules with temperatures in the sub-millikelvin range. In the experiment, SrF molecules produced from a pulsed supersonic source were cooled in the transverse direction using light from just two lasers. The molecular beam brightness was increased by about 20%. I discuss the detailed experimental setup, laser system and data analysis. I also present several theoretical models, which give insight into the cooling experiment. Finally, I discuss improvements to this experiment, which should enable higher yields of ultracold molecules to be produced.
We perform magnetically assisted Sisyphus laser cooling of the triatomic free radical strontium monohydroxide (SrOH). This is achieved with principal optical cycling in the rotationally closed P(N^{''}=1) branch of either the X[over ˜]^{2}Σ^{+}(000)↔A[over ˜]^{2}Π_{1/2}(000) or the X[over ˜]^{2}Σ^{+}(000)↔B[over ˜]^{2}Σ^{+}(000) vibronic transitions. Molecules lost into the excited vibrational states during the cooling process are repumped back through the B[over ˜](000) state for both the (100) level of the Sr-O stretching mode and the (02^{0}0) level of the bending mode. The transverse temperature of a SrOH molecular beam is reduced in one dimension by 2 orders of magnitude to ∼750 μK. This approach opens a path towards creating a variety of ultracold polyatomic molecules by means of direct laser cooling.
Laser cooling of molecules is a powerful technique for producing cold, slow beams for precision measurements and quantum control, yet its implementation remains challenging due to molecular complexity. Here, we combine a cryogenic buffer gas beam, an electrostatic hexapole lens, and 2D transverse Doppler laser cooling to produce a bright beam of barium monofluoride (138Ba19F) molecules. We study both numerically and experimentally the laser cooling effect as a function of laser detuning, laser power, laser alignment, and interaction time. We find a scattering rate of 6.1(1.4) × 105 s−1 on the laser cooling transition (14% of the expected maximum) and identify suboptimal dark Zeeman state remixing, suboptimal laser sideband powers and detunings, and a lack of vibrational repump laser intensity as possible causes of such a low rate. Using 3 tuneable lasers with appropriate sidebands and detuning, each molecule scatters approximately 400 photons during 2D laser cooling, limited by the interaction time and scattering rate. Leaks to dark states are less than 10%. Finally, we use the experimental results to benchmark the trajectory simulations to predict the achievable flux 3.5 m downstream for a planned eEDM experiment. Laser cooling is a powerful technique that enables precision measurements and quantum control, yet its implementation in molecules remains challenging due to their complex structures. Here, the authors apply 2D transverse laser cooling to a focused beam of cold barium monofluoride (138Ba19F) molecules to significantly increase beam brightness.
Atoms can be cooled and trapped efficiently with the help of lasers. So-called Doppler cooling takes advantage of momentum transfer upon absorption and emission of photons and of Doppler shifts to facilitate effectively closed optical absorption-emission loops, by which atoms are slowed down and cooled. Due to the wealth of internal degrees of freedom accessible in molecules, it was assumed for a long time that similarly closed optical loops cannot be realised for molecules. After an early theoretical proposal by Di Rosa for diatomic molecules, such cooling has been achieved in this decade for SrF, YO, CaF and YbF. It has been outlined recently that also polyatomic molecules should be coolable with lasers and classes of molecules expected to be amenable to this have been proposed by the present authors. Experimental success in laser cooling of SrOH has been reported. The status of cooling polyatomic molecules with lasers and the prospects for obtaining ultracold chiral molecules is reviewed herein.