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ChemPhysChem

Light Gives Molecules the Chills

Adela Marian, Břetislav Friedrich

Published Jan 4, 2011• 1 citation
Publisher

Abstract

A Sisyphean task: Laser cooling of molecules is difficult, mainly due to their rich vibrational structure, typically requiring dozens of repumping lasers. However, a proof-of-principle experiment to laser cool SrF molecules has been done (see picture), showing that laser cooling of some molecules is possible with just three lasers, as Highlighted herein.

DOI
10.1002/cphc.201000967

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A Sisyphean task: Laser cooling of molecules is difficult, mainly due to their rich vibrational structure, typically requiring dozens of repumping lasers. However, a proof-of-principle experiment to laser cool SrF molecules has been done (see picture), showing that laser cooling of some molecules is possible with just three lasers, as Highlighted herein.
Recently, laser cooling methods have been extended from atoms to molecules. The complex rotational and vibrational energy level structure of molecules makes laser cooling difficult, but these difficulties have been overcome and molecules have now been cooled to a few microkelvin and trapped for several seconds. This opens many possibilities for applications in quantum science and technology, controlled chemistry, and tests of fundamental physics. This article explains how molecules can be decelerated, cooled and trapped using laser light, reviews the progress made in recent years, and outlines some future applications.
We propose a laser cooling method for atomic species whose level structure makes traditional laser cooling difficult. For instance, laser cooling of hydrogen requires single-frequency vacuum-ultraviolet light, while multielectron atoms need single-frequency light at many widely separated frequencies. These restrictions can be eased by laser cooling on two-photon transitions with ultrafast pulse trains. Laser cooling of hydrogen, antihydrogen, and many other species appears feasible, and extension of the technique to molecules may be possible.
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.
One of three priorities of the 1994 National Research Council Report Atomic, Molecular and Optical Science is promote research … to better control and manipulate atoms, molecules, charged particles, and light. Although many techniques are available for atoms, charged particles, and light, we propose here new techniques for rapidly cooling (more generally, manipulating) the vibrational, rotational, and translational energy of simple molecules. A concrete example is manipulating Cs2 by using the B1Πn-1Σg+ bands. The key component is an optically pumped amplifier (using the same molecule, here Cs2) to provide the synchronized multiple-single-frequency laser required to optically couple a significant number of rovibronic levels while rapidly (and simultaneously) tuning over all coupled Doppler profiles (as in atomic translational cooling). Proposed molecular- beam experiments providing total cooling in ~12 ms are described.