4.8 Article

Unambiguous Signature of the Berry Phase in Intense Laser Dissociation of Diatomic Molecules

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JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 9, 期 9, 页码 2271-2277

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AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b00607

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  1. Deutsche Forschungsgemeinschaft (DFG) [BO 4623/1-1]

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We report strong evidence of Berry phase effects in intense laser dissociation of D-2(+) molecules, manifested as Aharonov-Bohm-like oscillations in the photofragment angular distribution (PAD). Our calculations show that this interference pattern strongly depends on the parity of the diatom initial rotational state, (-1)(j). Indeed, the PAD local maxima (minima) observed in one case (j odd) correspond to local minima (maxima) in the other case (j even). Using simple topological arguments, we clearly show that such interference conversion is a direct signature of the Berry phase. The sole effect of the latter on the rovibrational wave function is a sign change of the relative phase between two interfering components, which wind in opposite senses around a light-induced conical intersection (LICI). Therefore, encirclement of the LICI leads to constructive (j odd) or destructive (j even) self-interference of the initial nuclear wavepacket in the dissociative limit. To corroborate our theoretical findings, we suggest an experiment of strong-field indirect dissociation of D-2(+) molecules, comparing the PAD of the ortho and para molecular species in directions nearly perpendicular to the laser polarization axis.

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