We investigate coherent control of atomic translational motion in an applied off-resonance dipole optical potential. Since spontaneous emission can be neglected in this regime, the problem is treated as one of coherent momentum transfer. We consider both adiabatic and nonadiabatic regimes of cooling in the framework of the Wigner function formalism. For the adiabatic case, an approximate solution is obtained corresponding to the cooling envelope for an arbitrary time dependence of the external field. The nonadiabatic cooling process is formulated in terms of optimal control theory in order to define the most favorable regime of cooling under imposed constraints on the intensity of the control field. We find that the applied control field yields a significant reduction of the effective temperature of the atoms.
We investigate coherent control of atomic translational motion in an applied off-resonance dipole optical potential. Since spontaneous emission can be neglected in this regime, the problem is treated as one of coherent momentum transfer. We consider both adiabatic and nonadiabatic regimes of cooling in the framework of the Wigner function formalism. For the adiabatic case, an approximate solution is obtained corresponding to the cooling envelope for an arbitrary time dependence of the external field. The nonadiabatic cooling process is formulated in terms of optimal control theory in order to define the most favorable regime of cooling under imposed constraints on the intensity of the control field. We find that the applied control field yields a significant reduction of the effective temperature of the atoms.
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.
The usual form of electromagnetic forces is given by but for neutral atoms q = 0. The next order of force is the dipole term, but this also vanishes because neutral atoms have no inherent dipole moment. However, a dipole moment can be induced by a field, and this is most efficient if the field is alternating near the atomic resonance frequency. Since these frequencies are typically in the optical range, dipole moments are efficiently induced by shining nearly resonant light on the atoms. Laser cooling and trapping rely on the interaction between laser light and atoms to exert a controllable force on the atoms, and many sophisticated schemes have been developed using the special properties of the interaction. This chapter begins with the simplest schemes for exerting optical forces on atoms, namely a single-frequency light field interacting with a two-level atom. Although this is the simplest possible scheme, it is pedagogically valuable because it shows many of the features that will be encountered further on. The ultimate temperature using such a scheme is limited, but lower temperatures can be achieved with multilevel atoms. This topic is addressed later in the chapter. Two kinds of optical forces When an atom absorbs nearly resonant light, it makes a transition to the excited state, and its subsequent return to the ground state can be either by spontaneous or by stimulated emission. The nature of the optical force that arises from these two different processes is quite different, and will be described separately [1]. The spontaneous emission case is different from the familiar quantum mechanical calculations using state vectors to describe the state of the system, because spontaneous emission causes the state of the system to evolve from a pure state into a mixed state (see Exercise 6.9). Spontaneous emission is an essential ingredient for the dissipative nature of the optical forces in monochromatic light, and the density matrix is needed to describe it (see Chap. 6). When an atom absorbs light, its energy excites the atom and its angular momentum changes the electron's orbit. Both of these are internal atomic properties. However, the linear momentum of the light, can change only the external, translational motion of the atom.
Optimal control theory (OCT) is applied to the problem of cooling molecular rotations. The optimal field gives rise to a striking behavior, in which there is no noticeable increase in the lowest rotational state population until the last percent or so of the control interval, at which point the population jumps to 1. Further analysis of the intermediate time interval reveals that cooling is taking place all along, in the sense that the purity of the system, as measured by Tr(ρ 2 ), is increasing monotonically in time. Once the system becomes almost completely pure, the external control field can transfer the amplitude to the lowest rotational state by a completely Hamiltonian manipulation. This mechanism is interesting because it suggests a possible way of accelerating cooling, by exploiting the cooling induced by spontaneous emission to all the ground electronic state levels, not just the lowest rotational level. However, it also raises a major paradox: it may be shown that external control fields, no matter how complicated, cannot change the value of Tr(ρ 2 ); changing this quantity requires spontaneous emission which is inherently uncontrollable. What place is there then for control, let alone optimal control, using external fields? We discuss the resolution to this paradox with a detailed analysis of cooling in a two-level system.
Nonadiabatic unitary evolution with tailored time-dependent Hamiltonians can prepare systems of cold-atomic gases with various desired properties such as low excess energies. For a system of two one-dimensional quasicondensates coupled with a time-varying tunneling amplitude, we show that the optimal protocol, for maximizing any figure of merit in a given time, is bang-bang, i.e., the coupling alternates between only two values through a sequence of sudden quenches. Minimizing the energy of one of the quasicondensates with such a nonadiabatic protocol, and then decoupling it at the end of the process, can result in effective cooling beyond the current state of the art. Our cooling method can be potentially applied to arbitrary systems through an integration of the experiment with simulated annealing computations.
Optimal control theory is applied to laser cooling of molecules. The objective is to cool vibrations, using shaped pulses synchronized with the spontaneous emission. The optimal mechanism is found to operate by a “vibrationally selective coherent population trapping”. The trapping condition is that the instantaneous phase of the laser is locked to the phase of the transition dipole moment of v=0 with the excited population. The molecules that reach v=0 by spontaneous emission are then trapped, while the others are continually repumped.
Cooling of internal atomic and molecular states via optical pumping and laser cooling of the atomic velocity distribution, rely on spontaneous emission. The outstanding success of such examples, taken together with general arguments, has led to the widely held notion that radiative cooling requires spontaneous emission. We here show by specific examples and direct calculation, based primarily on breaking emission-absorption symmetry as in lasing without inversion, that cooling of internal states by external coherent control fields is possible. We also show that such coherent schemes allow us to practically reach absolute zero in a finite number of steps, in contrast to some statements of the third law of thermodynamics.