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arXiv:2012.10269 · Physical Review Letters

Complete Quantum Coherent Control of Ultracold Molecular Collisions

Adrien Devolder, Paul W. Brumer, Timur V. Tscherbul

Published Apr 13, 2021• 34 citations
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Abstract

We show that quantum interference-based coherent control is a highly efficient tool for tuning ultracold molecular collision dynamics that is free from the limitations of commonly used methods that rely on external electromagnetic fields. By varying the relative populations and phases of initial coherent superpositions of degenerate molecular states, we demonstrate complete coherent control over integral scattering cross sections in the ultracold s-wave regime of both the initial and final collision channels. The proposed control methodology is applied to ultracold O_{2}+O_{2} collisions, showing extensive control over s-wave spin-exchange cross sections and product branching ratios over many orders of magnitude.

DOI
10.1103/physrevlett.126.153403

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Coherent control of atomic and molecular scattering relies on the preparation of colliding particles in superpositions of internal states, establishing interfering pathways that can be used to tune the outcome of a scattering process. However, the incoherent addition of different partial wave contributions to the integral cross-sections, commonly encountered in systems with complex collisional dynamics, poses a significant challenge, often limiting the control. This work demonstrates that time-reversal symmetry can be used to overcome these limitations by constraining the relation between the S-matrix elements. For example, the preparation of a superposition of two states related by the time-reversal superposition can provide extensive control for transitions to a time-reversal invariant final state, such as the J = 0, M = 0. Using the example of ultracold O 2 –O 2 scattering, we show that for such states coherent control is robust against short-range dynamical complexity. Furthermore, the time-reversal symmetry also protects the control against a distribution of collisional energies. Beyond the ultracold regime, we observe significant differences in the controllability of crossed-molecular beam vs trap experiments with complete control achievable in the former case at any temperature, emphasizing the cooperative role of time-reversal and permutation symmetries in maintaining control at any temperature. These results open new avenues for the coherent control of complex inelastic collisions and chemical reactions both in and outside of the ultracold regime.

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We show that quantum interference-based coherent control is a highly efficient tool for tuning ultracold molecular collision dynamics that is free from the limitations of commonly used methods that rely on external electromagnetic fields. By varying the relative populations and phases of initial coherent superpositions of degenerate molecular states, we demonstrate complete coherent control over integral scattering cross sections in the ultracold s-wave regime of both the initial and final collision channels. The proposed control methodology is applied to ultracold O_{2}+O_{2} collisions, showing extensive control over s-wave spin-exchange cross sections and product branching ratios over many orders of magnitude.
Coherent control of atomic and molecular scattering relies on the preparation of colliding particles in superpositions of internal states, establishing interfering pathways that can be used to tune the outcome of a scattering process. However, the incoherent addition of different partial wave contributions to the integral cross-sections, commonly encountered in systems with complex collisional dynamics, poses a significant challenge, often limiting the control. This work demonstrates that time-reversal symmetry can be used to overcome these limitations by constraining the relation between the S-matrix elements. For example, the preparation of a superposition of two states related by the time-reversal superposition can provide extensive control for transitions to a time-reversal invariant final state, such as the J = 0, M = 0. Using the example of ultracold O 2 –O 2 scattering, we show that for such states coherent control is robust against short-range dynamical complexity. Furthermore, the time-reversal symmetry also protects the control against a distribution of collisional energies. Beyond the ultracold regime, we observe significant differences in the controllability of crossed-molecular beam vs trap experiments with complete control achievable in the former case at any temperature, emphasizing the cooperative role of time-reversal and permutation symmetries in maintaining control at any temperature. These results open new avenues for the coherent control of complex inelastic collisions and chemical reactions both in and outside of the ultracold regime.
We propose a general method to induce interference between scattering wave functions in atomic and molecular collisions at ultracold temperatures by using a static magnetic field. The scheme is based on the preparation of collision partners in coherent superpositions of Zeeman states. The magnetic field is used to induce interference between two incoming channels. As an illustrative example, we consider ultracold collisions between 7Li^{7}\mathrm{Li}7Li and 133Cs^{133}\mathrm{Cs}133Cs atoms, and show that ratios of state resolved collision cross sections can be enhanced by engineering the preparation of the initial coherent superpositions.
We explore coherent control of Penning and associative ionization in cold collisions of metastable He∗(23S){\mathrm{He}}^{*}(2{\phantom{\rule{4pt}{0ex}}}^{3}S)He∗(23S) atoms via the quantum interference between different states of the He2∗{\mathrm{He}}_{2}^{*}He2∗​ collision complex. By tuning the preparation coefficients of the initial atomic spin states, we can benefit from the quantum interference between molecular channels to maximize or minimize the cross sections for Penning and associative ionization. In particular, we find that we can enhance the ionization ratio by 30% in the cold regime. This work is significant for the coherent control of chemical reactions in the cold and ultracold regimes.
The optical theorem is a fundamental aspect of quantum scattering theory. Here, we generalize this theorem to the case where the incident scattering state is a superposition of internal states of the collision partners, introducing additional interference contributions and, e.g., providing a route to control the total integral cross section. As in its standard form, forward scattering plays an essential role in the multichannel optical theorem, but with interference terms being related to the inelastic forward scattering amplitudes between states in the initial superposition. Using the resultant control index, we show that extensive control is possible over ultracold collisions of oxygen molecules in their rovibrational ground states, and of $^{85}\mathrm{Rb}\text{\ensuremath{-}}^{85}\mathrm{Rb}$ collisions, promising systems for the experimental demonstration of the quantum interference control of the total scattering cross section.
The optical theorem is a fundamental aspect of quantum scattering theory. Here, we generalize this theorem to the case where the incident scattering state is a superposition of internal states of the collision partners, introducing additional interference contributions and, e.g., providing a route to control the total integral cross section. As in its standard form, forward scattering plays an essential role in the generalized optical theorem, but with interference terms being related to the inelastic forward scattering amplitudes between states in the initial superposition. Using the resultant control index, we show that extensive control is possible over ultracold collisions of oxygen molecules in their rovibrational ground states, and of 85Rb-85Rb collisions, promising systems for the first experimental demonstration of the quantum interference control of the total scattering cross section.
We show that exchange symmetry in collisions of identical particles enables symmetry-protected coherent control of the total scattering cross section. For identical fermions, antisymmetrization enforces a common control phase among contributing channels within a given parity sector, yielding maximal control visibility. For identical bosons, phase-locking persists but with reduced visibility due to additional exchange (satellite) contributions. Collisions of distinguishable particles lack this symmetry-imposed phase-locking, leading to lower controllability and visibility. We elucidate these principles through coupled-channel quantum-scattering calculations for lithium-lithium collisions, comparing the 6Li−6Li^{6}\mathrm{Li}{-}^{6}\mathrm{Li}6Li−6Li (identical fermions), 7Li−7Li^{7}\mathrm{Li}{-}^{7}\mathrm{Li}7Li−7Li (identical bosons), and 6Li−7Li^{6}\mathrm{Li}{-}^{7}\mathrm{Li}6Li−7Li (distinguishable) systems. Furthermore, in the identical-particle cases, symmetry-enforced phase-locking enables full control over the parity of the final state even beyond the ultracold regime. This mechanism is broadly applicable to identical-particle collisions, including homonuclear molecules for which established approaches--DC electric fields or microwave shielding--are ineffective or unavailable.