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arXiv:1804.04184 · Physical Review A

Deflection of a molecular beam using the bichromatic stimulated force

Scott Galica, Leland Aldridge, Daniel McCarron, Edward E. Eyler, P. L. Gould

Published Aug 13, 2018• 22 citations
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Abstract

We demonstrate that a bichromatic standing-wave laser field can exert a significantly larger force on a molecule than ordinary radiation pressure. Our experiment measures the deflection of a pulsed supersonic beam of CaF molecules by a two-frequency laser field detuned symmetrically about resonance with the nearly closed $X(v=0)\ensuremath{\rightarrow}B({v}^{\ensuremath{'}}=0)$ transition. The inferred force as a function of relative phase between the two counterpropagating beams is in reasonable agreement with numerical simulations of the bichromatic force in this multilevel system. The large magnitude of the force, coupled with the reduced rate of spontaneous emission, indicates its potential utility in the production and manipulation of ultracold molecules.

DOI
10.1103/physreva.98.023408

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arXiv:1108.3543•Physical Review A•Dec 2, 2011•42 citations
We demonstrate that a bichromatic standing-wave laser field can exert a significantly larger force on a molecule than ordinary radiation pressure. Our experiment measures the deflection of a pulsed supersonic beam of CaF molecules by a two-frequency laser field detuned symmetrically about resonance with the nearly closed X(v=0)\ensuremath→B(v\ensuremath′=0)X(v=0)\ensuremath{\rightarrow}B({v}^{\ensuremath{'}}=0)X(v=0)\ensuremath→B(v\ensuremath′=0) transition. The inferred force as a function of relative phase between the two counterpropagating beams is in reasonable agreement with numerical simulations of the bichromatic force in this multilevel system. The large magnitude of the force, coupled with the reduced rate of spontaneous emission, indicates its potential utility in the production and manipulation of ultracold molecules.
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.
Stimulated optical forces offer a simple and efficient method for providing optical forces far in excess of the saturated radiative force. The bichromatic force, using a counterpropagating pair of two-color beams, has so far been the most effective of these stimulated forces for deflecting and slowing atomic beams. We have numerically studied the evolution of a two-level system under several different bichromatic and polychromatic light fields, while retaining the overall geometry of the bichromatic force. New insights are gained by studying the time-dependent trajectory of the Bloch vector, including a better understanding of the remarkable robustness of bi- and polychromatic forces with imbalanced beam intensities. We show that a four-color polychromatic force exhibits great promise. By adding new frequency components at the third harmonic of the original bichromatic detuning, the force is increased by nearly 50% and its velocity range is extended by a factor of 3, while the required laser power is increased by only 33%. The excited-state fraction, crucial to possible application to molecules, is reduced from 41% to 24%. We also discuss some important differences between polychromatic forces and pulse trains from a high-repetition-rate laser.
The bichromatic force is a coherent optical force that has been demonstrated to exceed the saturated radiative force from a monochromatic cw laser by orders of magnitude in atomic systems. By stimulating photon emission between two states, the bichromatic force allows us to increase the photon scattering rate beyond the spontaneous emission rate while also suppressing decays into dark states. We present studies of the efficacy of the bichromatic force on molecular systems using the test cases of BBB-XXX (0,0), P11(1.5)/PQ12(0.5)P_{11}(1.5)/^PQ_{12}(0.5)P11​(1.5)/PQ12​(0.5) in CaF and A~\tilde{A}A~(000)−X~-\tilde{X}−X~(000), P11(1.5)/PQ12P_{11}(1.5)/^PQ_{12}P11​(1.5)/PQ12​(0.5) in the linear triatomic molecule SrOH. Computational results from detailed multilevel models indicate that both of these molecular systems are suitable for the use of the bichromatic force, with neither repumping nor magnetic destabilization of dark states interrupting the coherent cycling at the heart of the force. We comment on the applicability of the bichromatic force to arbitrary polyatomic molecules, and present our experimental progress in demonstrating the bichromatic force on CaF and possibly on SrOH.\footnote{Supported by the National Science Foundation.}
The spontaneous decay rate $\ensuremath{\gamma}$ of excited atomic states limits the radiative force on atoms to $\ensuremath{\Elzxh}k\ensuremath{\gamma}/2.$ This bottleneck in the dissipative exchange of momentum between atoms and light can be overcome by coherent control of the momentum exchange interactions. The bichromatic force provides such control by using stimulated instead of spontaneous emission to produce the force, while at the same time exploiting spontaneous emission to enable a dissipative interaction. It is implemented with two counterpropagating light beams, each containing two frequencies, whose phases, amplitudes, and frequency difference are carefully chosen. We have made precise measurements of the extremely large magnitude and velocity range of this bichromatic force, and have shown that its velocity dependence near the edge of its range is suitable for atomic beam slowing and laser cooling. Our measurements have corroborated various models and calculations of this bichromatic force.
We demonstrate the effect of the coherent optical bichromatic force on a molecule, the polar free radical strontium monohydroxide (SrOH). A dual-frequency retroreflected laser beam addressing the X[over ˜]^{2}Σ^{+}↔A[over ˜]^{2}Π_{1/2} electronic transition coherently imparts momentum onto a cryogenic beam of SrOH. This directional photon exchange creates a bichromatic force that transversely deflects the molecules. By adjusting the relative phase between the forward and counterpropagating laser beams we reverse the direction of the applied force. A momentum transfer of 70ℏk is achieved with minimal loss of molecules to dark states. Modeling of the bichromatic force is performed via direct numerical solution of the time-dependent density matrix and is compared with experimental observations. Our results open the door to further coherent manipulation of molecular motion, including the efficient optical deceleration of diatomic and polyatomic molecules with complex level structures.
We examine the prospects for utilizing the optical bichromatic force (BCF) to greatly enhance laser deceleration and cooling for near-cycling transitions in small molecules. We discuss the expected behavior of the BCF in near-cycling transitions with internal degeneracies, then consider the specific example of decelerating a beam of calcium monofluoride molecules. We have selected CaF as a prototype molecule both because it has an easily accessible near-cycling transition and because it is well suited to studies of ultracold molecular physics and chemistry. We also report experimental verification of one of the key requirements, the production of large bichromatic forces in a multilevel system with significant energy level splittings, by performing tests in an atomic beam of metastable helium.