Time-Reversal Symmetry-Protected Coherent Control of Ultracold Molecular Collisions

TL;DR

This paper demonstrates that time-reversal symmetry can protect coherent control of ultracold molecular collisions from partial wave scrambling and energy distribution issues, enabling robust manipulation even in complex, anisotropic systems.

Contribution

It introduces a novel approach leveraging time-reversal symmetry to enhance coherent control in ultracold molecular collisions, overcoming previous limitations due to complex dynamics.

Findings

Control is robust against partial wave scrambling.

Time-reversal symmetry protects control across energy distributions.

Control is more feasible in trap experiments than in crossed-molecular beams.

Abstract

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, incoherent addition of different partial wave contributions to the integral cross sections (partial wave scrambling), commonly encountered in systems with complex collisional dynamics, poses a significant challenge, often limiting control. This work demonstrates that time-reversal symmetry can overcome these limitations by constraining the relative phases of S-matrix elements, thereby protecting coherent control against partial wave scrambling, even for collisions mediated by highly anisotropic interactions. Using the example of ultracold O$_2$-O$_2$ scattering, we show that coherent control is robust against short-range dynamical complexity. Furthermore, the time-reversal symmetry also protects the control against a distribution of collisional energy. These findings show that ultracold scattering into the final states that are time-reversal-invariant, such as the J = 0, M = 0 rotational state, can always be optimally controlled by using time-reversal-invariant initial superpositions. Beyond the ultracold regime, we observe significant differences in the controllability of crossed-molecular beam vs. trap experiments with the former being easier to control, 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.