Coherent optical bichromatic forces have been shown to be effective tools for rapidly slowing and cooling simple atomic systems. While previous estimates suggest that these forces may also be effective for rapidly decelerating molecules or complex atoms, a quantitative treatment for multilevel systems has been lacking. We describe detailed numerical modeling of bichromatic forces by direct numerical solution for the time-dependent density matrix in the rotating-wave approximation. We describe both the general phenomenology of an arbitrary few-level system and the specific requirements for slowing and cooling on a many-level transition in calcium monofluoride (CaF), one of the molecules of greatest current experimental interest. We show that it should be possible to decelerate a cryogenic buffer-gas-cooled beam of CaF nearly to rest without a repumping laser and within a longitudinal distance of about 1 cm. We also compare a full 16-level simulation for the CaF $B\ensuremath{\leftrightarrow}X$ system with a simplified numerical model and with a semiquantitative estimate based on two-level systems. The simplified model performs nearly as well as the complete version, whereas the two-level model is useful for making order-of-magnitude estimates, but nothing more.
We examine two approaches for significantly extending the velocity range of the optical bichromatic force (BCF), to make it useful for laser deceleration of atomic and molecular beams. First, we present experimental results and calculations for BCF deceleration of metastable helium using very large BCF detunings and discuss the limitations of this approach. We consider in detail the constraints, both inherent and practical, that set the usable upper limit of the BCF. We then show that a more promising approach is to utilize a BCF profile with a relatively small velocity range in conjunction with chirped Doppler shifts, to keep the force resonant with the atoms as they are slowed. In an initial experimental test of this chirped BCF method, helium atoms are slowed by $\ensuremath{\sim}$370 m/s using a BCF profile with a velocity width of $\ensuremath{\lesssim}$125 m/s. Straightforward scaling of the present results indicates that a decelerator for He* capable of loading a magneto-optical trap can yield a brightness comparable to a much larger Zeeman slower.
This dissertation discusses an experiment to demonstrate the application of the stimulated bichromatic optical force (BCF) on the diatomic molecule calcium monofluoride (CaF). The research demonstrates the deflection of a supersonic beam of CaF through the application of BCF under a variety of conditions, highlighting distinctive characteristics of the force. Results show that the measured deflection of the molecular beam is consistent with the behavior of BCF under the tested conditions. In particular, we have measured a predicted reversal in the direction of the force as well as an applied force which exceeds the radiation pressure force. Detailed modeling of the BCF in multilevel systems corroborates our findings. We discuss the development and application of these models with respect to non-ideal conditions present in the experiment. The construction of the molecular beam source and BCF laser systems are discussed in detail. A brief discussion of further modeled extensions of the BCF through the addition of higher order sidebands is presented as well. Overall, our results demonstrate that the BCF is a potentially useful tool for manipulation of cold molecules.
Abstract We theoretically investigate the possibility of stimulated light force deceleration and cooling of the diatomic magnesium fluoride molecular beam with near-cycling transitions in the bichromatic standing light wave of high intensity. The weighted degeneracy and force reduction factor are considered due to the behavior of the optical bichromatic force (BCF) in near-cycling transitions with internal degeneracies, and the two-level optical Bloch equations can estimate the actual behavior of the BCF. Our simulation shows that the stimulated force exceeding the spontaneous force by a factor of 2.8 can slow down the molecular beam to several m s −1 within centimeter-scale distance, and this slowing mechanism can eliminate the need of compensation of Doppler shift during the longitudinal deceleration of the molecular beam.
The bichromatic optical force (BCF), which can greatly exceed radiative forces, seems ideal for laser slowing and cooling of molecules because it minimizes the effects of radiative decay. However, it relies on sustained coherences between optically coupled states, and molecules, with their many sublevels and decay pathways, present new challenges in maintaining these coherences compared with simple atoms. We have conducted extensive numerical simulations of BCFs in model molecular systems based on the
BleftrightarrowX transition in CaF, and have begun experimental tests in a molecular beam.\ In our modeling, the effects of fine and hyperfine structure are examined using a simplified level scheme that is still sufficiently complete to include the major pathways leading to loss or decoherence. To circumvent optical pumping into coherent dark states we explore two possible schemes: (1) a skewed dc magnetic field, and (2) rapid optical polarization switching. The effects of repumping to compensate for out-of-system radiative decay are also examined. Our results verify that the BCF is a promising method for creating large forces in molecular beams while minimizing out-of-system radiative losses, and provide detailed guidance for experimental designs. Compared to a two-level atom, the peak force is reduced by about an order of magnitude, but there is little reduction in the velocity range over which the force is effective. Our experiments on deflection and slowing using the CaF
BleftrightarrowX, (0-0) transition, still at an early stage, include studies of both the
P11(1.5)/PQ12(0.5) branch, a quasi-cycling configuration with extensive hfs, and the
R11(0.5)/RQ21(0.5) branch, which has a much simpler hfs but requires rotational repumping.