Orientation-Dependent Enhanced Ionization in Acetylene Revealed by Ultrafast Cross-Polarized Pulse Pairs

• URL: http://arxiv.org/abs/2411.04144v1
• Date: Tue, 05 Nov 2024 10:15:08 GMT
• Title: Orientation-Dependent Enhanced Ionization in Acetylene Revealed by Ultrafast Cross-Polarized Pulse Pairs
• Authors: S. A. Mohideen, A. J. Howard, C. Cheng, I. Gabalski, A. M. Ghrist, E. Weckwerth, P. H. Bucksbaum,
• Abstract summary: We probe molecular dynamics in acetylene with intense 6-fs cross-polarized pulse pairs. We find two distinct pathways that both contribute to a large increase in the multiple ionization yield.
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• Abstract: We investigate the orientation dependence of Enhanced Ionization (EI) during strong-field-driven nuclear motion in acetylene (C$_2$H$_2$). Here, we both initiate and probe molecular dynamics in acetylene with intense 6-fs cross-polarized pulse pairs, separated by a variable delay. Following multiple ionization by the first pulse, acetylene undergoes simultaneous elongation of the carbon-carbon and carbon-hydrogen bonds, enabling further ionization by the second pulse and the formation of a very highly charged state, [C$_2$H$_2]^{6+}$. At small inter-pulse delays ($<$20 fs), this enhancement occurs when the molecule is aligned to the probe pulse. Conversely, at large delays ($>$40 fs), formation of [C$_2$H$_2]^{6+}$ occurs when the molecule is aligned to the pump pulse. By analyzing the polarization and time dependence of sequentially ionized [C$_2$H$_2]^{6+}$, we resolve two distinct pathways that both contribute to a large increase in the multiple ionization yield. This cross-polarized pulse pair scheme uniquely enables selective probing of deeply bound orbitals, providing new insights on orientation-dependent EI in highly charged hydrocarbons.

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