Abstract The methods of laser cooling of atoms have long been applied to obtain cold and ultracold atomic gases, including degenerate states and the atomic Bose–Einstein condensate in particular. Until recently the application of laser cooling methods to molecules was assumed to be impossible because of the complex structure of molecular levels and the absence of closed cooling cycles for transitions between the electron levels of molecules in the general case. However, it has recently become clear that laser cooling can be performed for a large class of molecules, including not only the simplest diatomic molecules but also polyatomic molecules. We here present the general principles for identifying suitable molecules and discuss current studies on and further developments in the laser cooling of molecules.
Abstract The methods of laser cooling of atoms have long been applied to obtain cold and ultracold atomic gases, including degenerate states and the atomic Bose–Einstein condensate in particular. Until recently the application of laser cooling methods to molecules was assumed to be impossible because of the complex structure of molecular levels and the absence of closed cooling cycles for transitions between the electron levels of molecules in the general case. However, it has recently become clear that laser cooling can be performed for a large class of molecules, including not only the simplest diatomic molecules but also polyatomic molecules. We here present the general principles for identifying suitable molecules and discuss current studies on and further developments in the laser cooling of molecules.
Abstract The extension of laser cooling and trapping techniques from atoms to molecules is currently the subject of intense and growing interest. Molecular laser cooling and trapping offers a general technique applicable to a variety of molecules with different properties and internal structures and is well-suited to the growing list of proposed applications for ultracold molecules. The recent development of optical cycling schemes for specific molecular species now allow each molecule to scatter up to ∼10 6 photons. This has proven sufficient for multiple groups to laser cool and slow molecular beams and, notably, capture molecules in magneto-optical traps (MOTs) and cool them to ultracold temperatures. MOTs are the workhorse technique for atomic physics in the ultracold regime and today’s molecular MOTs represent a powerful starting point for the study and manipulation of ultracold molecular gases. This Topical Review presents a summary of the progress made in this new and emerging field.
The first part of this project involved continued development of theoretical models of diatomic molecular electronic level structure for application to the production of ultracold diatomic molecules via photoassociation. Recently, there has been considerable interest in producing molecules at the temperatures achieved for laser-cooled atoms, for applications to "coherent chemistry," studies of molecule-atom and molecule-molecule interactions. Bose condensates of molecules and for quantum computing. It is advantageous to produce cold molecules from laser-cooled atoms. but this requires an accurate model of the energy level structure near the dissociation limit for excited atoms, and for other intermediate states. With this in mind. we have modeled experimental photoassociation data from Rb2. spectroscopic data on the lowest excited states of Na2, and hyperfine structure of the lowest triplet state of Cs2. The second part involved continued development of experimental techniques for intense atomic beam collimation using a bichromatic laser field. We solved the equations for evolution of atoms in such a laser field, expressed the results in the form of trajectories on the Bloch sphere for a two-level atoms, and then used these results to design and perform efficient atomic beam reflection experiments. At the same time, we are developing methods to use these highly collimated beams of metastable helium atoms for precision lithography, using sensitized surfaces.
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.
Laser cooling of atoms began more than 25 years ago and has led to spectacular advances in areas such as atomic clocks, Bose-Einstein condensation, degenerate Fermi gases, and ultracold collisions. Molecules, due to their complexity relative to atoms (1), have been slower to jump on the ultracold bandwagon but are now firmly on board. Three recent papers (2-4) describe techniques for efficiently and substantially reducing the vibrational motion of molecular ensembles, thus approaching the goal of large numbers of molecules that are cold in all their degrees of freedom, both external and internal.
Slowing down atoms using laser cooling, together with techniques like magnetic trapping and evaporative cooling, has led to numerous exciting results over the last decade [1], with the realization of Bose-Einstein condensation as the most spectacular achievement [2]. Laser-cooling schemes are applicable to atoms since closed multilevel systems can be realized and many consecutive absorptionemission cycles can be induced. This leads to a significant momentum transfer from the photons of the laser to the atom, resulting in a change of the velocity of the atom. There currently is a great interest in producing cold molecules for the study of cold molecule-molecule collisions, molecular quantum collective effects, Doppler-free spectroscopy, frequency standards, as well as many other applications already realized for atoms [3]. Slowing down of neutral molecules, a prerequisite for being able to trap them, has proven to be considerably more difficult to be achieved, however. The above-mentioned laser-cooling scheme cannot be applied to slow down molecules as no simple closed-level systems can be found; the unavoidable off-resonant radiative decay of molecules from the excited state to other vibrational levels in the electronic ground state hampers efficient momentum transfer [4]. Once molecules are present at sufficiently low kinetic energies, below a fraction of a cm21, they can be trapped in various ways. Trapping of neutral molecules in inhomogeneous magnetic [3] and electric fields [5] and trapping based on the use of evanescent fields close to the dielectricvacuum interface have been proposed [6]. It has also been suggested that extremely high laser powers might be used to induce a dipole moment in polarizable molecules, leading to trapping of these molecules in the laser beam [7]. Other methods to produce slow molecules have been put forward and have recently been successfully applied to produce the first samples of trapped molecules. By injecting molecules in a cold buffer gas, sufficiently low kinetic energies of the injected molecules can be obtained after thermalization that they can subsequently be trapped in an inhomogeneous magnetic field. This has recently been demonstrated for CaH injected in 3He buffer gas at temperatures of around 0.3 K [8]. Associative collisions between ultracold trapped atoms [9] have proven to be
Slowing, cooling, and trapping molecules One of the major achievements in physics during the last two decades of the twentieth century was the ability to cool and trap atoms [1]. Laser cooling can produce previously inconceivable atomic temperatures of less than 1 μK. Atoms with sufficiently low kinetic energy can be trapped in magnetic and optical traps and thus studied for a prolonged time, thereby improving the resolution of spectroscopy by many orders of magnitude as well as reducing Doppler broadening. Furthermore, besides the external degrees of freedom, the internal degrees of freedom of the atoms can also be manipulated, leading to full control of the atoms. One of the holy grails of physics, the achievement of Bose–Einstein condensation in a dilute gas, was achieved mainly because of laser cooling and trapping of atoms. One of the natural extensions of laser cooling and trapping of atoms is the application of the techniques to molecules. Molecules offer a much richer internal structure than atoms, and thus provide extended possibilities to experimentalists. However, atomic laser cooling is based on the repetitive scattering of light and requires a closed, or at least nearly closed, two-level system. Because of the complicated internal structure of molecules, a closed two-level system cannot usually be found because they have many different electronic, vibrational, and rotational states and in general can decay to many different states after absorption of light (see Chap. 16). This requires a complete rethinking of the schemes that are used to cool atoms. Still, because of the extended possibilities cold molecules can offer with respect to cold atoms, there have been a large number of techniques developed to slow, cool, and trap them. These techniques can be divided into two classes, namely direct and indirect cooling. In the first case, molecules at cryogenic or room temperature are directly slowed and cooled. Although many different slowing techniques are used, this chapter focuses on Stark slowing of molecules since it was the first technique developed. Apart from the Stark shift of the molecules, the Zeeman and light shift of molecules can also be used to slow them. The idea behind Stark slowing is to subject the moving molecules to a continuously increasing electric field so that their kinetic energy is converted into potential energy.