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Intriguing dynamics pattern in F + HD
Despite decades of studies, the role of relativistic spin-orbit interactions in the dynamics of chemical reactions remains an intriguing topic. Using a high-resolution velocity map imaging crossed beams technique, Chen et al. observed an interesting pattern in the differential cross sections in the F + HD → HF + D reaction near the partial wave resonances (see the Perspective by Rakitzis). Further theoretical analysis showed that this pattern originates from quantum interference between spin-orbit split partial wave resonances with different total parities. The effect of the fine structure of the partial waves observed for this long known yet not completely explored three-atom system represents one more remarkable demonstration of the truly quantum nature of chemical reaction dynamics.
Abstract
The effect of electron spin-orbit interactions on chemical reaction dynamics has been a topic of much research interest. Here we report a combined experimental and theoretical study on the effect of electron spin and orbital angular momentum in the F + HD → HF + D reaction. Using a high-resolution imaging technique, we observed a peculiar horseshoe-shaped pattern in the product rotational-state–resolved differential cross sections around the forward-scattering direction. The unusual dynamics pattern could only be explained properly by highly accurate quantum dynamics theory when full spin-orbit characteristics were considered. Theoretical analysis revealed that the horseshoe pattern was largely the result of quantum interference between spin-orbit split–partial-wave resonances with positive and negative parities, providing a distinctive example of how spin-orbit interaction can effectively influence reaction dynamics.
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