Electron-nuclear correlated multiphoton-route to Rydberg fragments of molecules

Wenbin Zhang, Xiaochun Gong, Hui Li, Peifen Lu, Fenghao Sun, Qinying Ji, Kang Lin, Junyang Ma, Hanxiao Li, Junjie Qiang, Feng He () and Jian Wu ()
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Wenbin Zhang: East China Normal University
Xiaochun Gong: East China Normal University
Hui Li: East China Normal University
Peifen Lu: East China Normal University
Fenghao Sun: East China Normal University
Qinying Ji: East China Normal University
Kang Lin: East China Normal University
Junyang Ma: East China Normal University
Hanxiao Li: East China Normal University
Junjie Qiang: East China Normal University
Feng He: Shanghai Jiao Tong University
Jian Wu: East China Normal University

Nature Communications, 2019, vol. 10, issue 1, 1-8

Abstract: Abstract Atoms and molecules exposed to strong laser fields can be excited to the Rydberg states with very high principal quantum numbers and large orbitals. It allows acceleration of neutral particles, generate near-threshold harmonics, and reveal multiphoton Rabi oscillations and rich photoelectron spectra. However, the physical mechanism of Rydberg state excitation in strong laser fields is yet a puzzle. Here, we identify the electron-nuclear correlated multiphoton excitation as the general mechanism by coincidently measuring all charged and neutral fragments ejected from a H2 molecule. Ruled by the ac-Stark effect, the internuclear separation for resonant multiphoton excitation varies with the laser intensity. It alters the photon energy partition between the ejected electrons and nuclei and thus leads to distinct kinetic energy spectra of the nuclear fragments. The electron-nuclear correlation offers an alternative visual angle to capture rich ultrafast processes of complex molecules.

Date: 2019
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DOI: 10.1038/s41467-019-08700-5

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