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arXiv:quant-ph/0107103

Laser Cooling of Molecules by Repeated Velocity Selective Deceleration

C. H. Raymond Ooi, Karl-Peter Marzlin, Jürgen Audretsch

Published Jul 20, 2001• 0 citations
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Abstract

We propose a laser cooling concept for the translational motion of molecules which does not require repeated spontaneous emission by each molecule. The cooling works by repetition of three main steps; velocity selection of a narrow momentum width, deceleration of velocity selected molecules by repeated STIRAP and accumulation of decelerated molecules via one time spontaneous emission. We use single spontaneous emission for irreversible accumulation of narrow velocity selected and decelerated populations. We develop an analytical model to describe the evolution of the molecular gas system, internal subsystem and external (center of mass) subsystem density matrices and entropies. Simulation results show cooling from an arbitrary momentum width towards final width of about $\\hbar k$. The external entropy is reduced while the internal entropy is increased. The external entropy is shown to decrease during coherent laser interactions, a possibility of translational cooling via unitary evolution. The system entropy increases in consistency with the Araki-Lieb inequality.

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A theoretical analysis of one-dimensional cooling of atoms is presented. The method of cooling is based on velocity-selective coherent population trapping. Both internal and translational degrees of freedom of the atoms are treated quantum mechanically. The analytic expression for atomic density matrix is obtained in the limit of large interaction time and small kinetic momentum of atom. It is demonstrated that: (i) there is a limit on the lowest temperature that can be achieved by such a method and it is determined by the small but finite rate of decay of the coherence between two low-lying states in the three-level Lambda -configuration; (ii) the fraction of atoms involved in the cooling process decreases to zero as the atom-field interaction time increases, because of the presence of such a relaxation which always takes place in real experimental systems.

Journal of Physics B Atomic Molecular and Optical Physics•Nov 14, 1993•7 citations
We propose a laser cooling concept for the translational motion of molecules which does not require repeated spontaneous emission by each molecule. The cooling works by repetition of three main steps; velocity selection of a narrow momentum width, deceleration of velocity selected molecules by repeated STIRAP and accumulation of decelerated molecules via one time spontaneous emission. We use single spontaneous emission for irreversible accumulation of narrow velocity selected and decelerated populations. We develop an analytical model to describe the evolution of the molecular gas system, internal subsystem and external (center of mass) subsystem density matrices and entropies. Simulation results show cooling from an arbitrary momentum width towards final width of about hbark\\hbar khbark. The external entropy is reduced while the internal entropy is increased. The external entropy is shown to decrease during coherent laser interactions, a possibility of translational cooling via unitary evolution. The system entropy increases in consistency with the Araki-Lieb inequality.
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.
We present an approach to laser cooling of internal molecular degrees of freedom for vibrationally hot molecules using a sequence of ultrashort laser pulses. It is assumed that the molecules initially occupy different vibrational states with a substantial portion of the molecules being in excited vibrational states. We show that the ultimate aim of increasing the vibrational ground-state population through a reduction of the system's entropy can be achieved through a multistep process. In the first step, we design an ultrashort laser pulse that selectively transfers most of the population of the excited vibrational states to an excited electronic surface; then the field is switched off and the system allowed to relax until most of the excited electronic state population has decayed due to spontaneous emission. By repeating this procedure a few times, the entropy of the system can be substantially reduced and the population of the vibrational ground state increased considerably, even if the lifetimes of the excited electronic states are much greater than the length of a control pulse, i.e., if dissipative effects are negligiable on the time scales of coherent control.
A novel scheme is proposed for sequential cooling of rotation, translation, and vibration of molecules. More generally, this scheme manipulates and controls the states and energies of molecules. The scheme, while somewhat complex, is simpler and more feasible than simply providing a large number of synchronously but independently tunable lasers. The key component is a multiple single frequency laser (MSFL) in which a single narrow band pump laser generates an ensemble of resonant ‘‘stimulated Raman’’ (RSR) sidebands (subsequently amplified and selected) in a sample of the molecules to be cooled. Starting with a relatively cold molecular sample (e.g., a supersonic beam of Cs2), the rotation of molecules is cooled by sequential application of P branch electronic transition frequencies transverse to the molecular beam beginning at higher rotational angular momentum J. Then translation of molecules is cooled by application of multiple low J, P, and R branch transition frequencies which counterpropagate with the molecular beam and are synchronously chirped over their Doppler profiles. Finally, vibration of molecules is cooled by blocking the R(0) line of the 0–0 band. Only this specific order of rotation–translation–vibration appears feasible (using molecules produced by photoassociation of ultracold atoms avoids the requirement for translational cooling). Each step employs true dissipative cooling (i.e., reduction of system entropy in three degrees of freedom) by spontaneous emission and should yield a large translationally cold sample of molecules in the lowest (v=0, J=0) level of the ground electronic state, suitable for studies such as molecule trapping, ‘‘molecule optics,’’ or long range intermolecular states.
In the last several years we have discovered a variety of remarkable pulse strategies for manipulating molecular motion by employing a design strategy we call “local optimization.'' Here we review the concept of local optimization and contrast it with optimal control theory. By way of background, we give highlights from two recent examples of the method: (1) a strategy for eliminating population transfer to one or many excited electronic states during strong field excitation, an effect we call ‘optical paralysis’; (2) a generalization of the counterintuitive STIRAP (stimulated Raman adiabatic passage) pulse sequence from three levels to N levels, a strategy we call ‘straddling STIRAP.' We then turn to a third example, which is the main subject of this paper: laser cooling of molecular internal degrees of freedom. We study a model that includes both coherent interaction with the radiation field and spontaneous emission; the latter is necessary to carry away the entropy from the molecule. An optimal control calculation was performed first and succeeded in producing vibrational cooling, but the resulting pulse sequence was difficult to interpret. Local optimization subsequently revealed the cooling mechanism: the instantaneous phase of the laser is locked to the phase of the transition dipole moment between the excited state amplitude and v=0 of the ground state. Thus, the molecules that reach v=0 by spontaneous emission become decoupled from the field, and no longer absorb, while molecules in all other states are continually repumped. The mechanism could be called “vibrationally selective coherent population trapping,'' in analogy to the corresponding mechanism of velocity selective coherent population trapping in atoms for sub-Doppler cooling of translations.
A theoretical analysis of one-dimensional cooling of atoms is presented. The method of cooling is based on velocity-selective coherent population trapping. Both internal and translational degrees of freedom of the atoms are treated quantum mechanically. The analytic expression for atomic density matrix is obtained in the limit of large interaction time and small kinetic momentum of atom. It is demonstrated that: (i) there is a limit on the lowest temperature that can be achieved by such a method and it is determined by the small but finite rate of decay of the coherence between two low-lying states in the three-level Lambda -configuration; (ii) the fraction of atoms involved in the cooling process decreases to zero as the atom-field interaction time increases, because of the presence of such a relaxation which always takes place in real experimental systems.