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We thank Dr M E Corrales for her participation in the first stages of this project. MLMS acknowledges financial support through a predoctoral contract from Universidad Complutense de Madrid (Spain) and FULMATEN-CM project funded by Madrid Regional Government under programme Y2018/NMT-5028. GR thanks the Netherlands Organization for Scientific Research (NWO) for financial support (Rubicon 68-50-1410). This project has received funding (SMP) from the European Union's Horizon 2020 Research and Innovation Programme under the Marie Sklodowska-Curie Grant agreement No. 842539 (ATTO-CONTROL) and has been financed in part by the Spanish State Research Agency (AEI/10.13039/501100011033), Grants PGC2018-096444-B-I00, PID2019-106125GB-I00 and PID2019-106732GB-I00, and the Madrid Regional Government through the program Proyectos Sinergicos de I + D (Grant Y2018/NMT-5028 FULMATEN-CM). FM acknowledges support from the 'Severo Ochoa' Programme for Centres of Excellence in R&D (SEV-2016-0686) and the 'Maria de Maeztu' Programme for Units of Excellence in R&D (CEX2018-000805-M). All calculations were performed at the Mare Nostrum Supercomputer of the Red Espanola de Supercomputacion (BSC-RES) and the Centro de Computacion Cientifica de la Universidad Autonoma de Madrid (CCC-UAM). MV and OK acknowledge the support from the Deutsche Forschungsgeminschaft (KO 4920/1-1). This work was performed in the Max Born Institut (Berlin) in the kHz Laboratory and received financial support from LaserLab Europe through the MBI002239 project.

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Femtosecond XUV- IR induced photodynamics in the methyl iodide cation

Publicated to:NEW JOURNAL OF PHYSICS. 23 (7): 73023- - 2021-07-01 23(7), DOI: 10.1088/1367-2630/ac0c9b

Authors: Murillo-Sanchez, Marta L.; Reitsma, Geert; Poullain, Sonia Marggi; Fernandez-Milan, Pedro; Gonzalez-Vazquez, Jesus; de Nalda, Rebeca; Martin, Fernando; Vrakking, Marc J. J.; Kornilov, Oleg; Banares, Luis;

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Abstract

The time-resolved photodynamics of the methyl iodide cation (CH3I+) are investigated by means of femtosecond XUV-IR pump-probe spectroscopy. A time-delay-compensated XUV monochromator is employed to isolate a specific harmonic, the 9th harmonic of the fundamental 800 nm (13.95 eV, 88.89 nm), which is used as a pump pulse to prepare the cation in several electronic states. A time-delayed IR probe pulse is used to probe the dissociative dynamics on the first excited (A) over tilde (2)A(1) state potential energy surface. Photoelectrons and photofragment ions-CH3+ and I+- are detected by velocity map imaging. The experimental results are complemented with high level ab initio calculations for the potential energy curves of the electronic states of CH3I+ as well as with full dimension on-the-fly trajectory calculations on the first electronically excited state (A) over tilde (2)A(1), considering the presence of the IR pulse. The CH3+ and I+ pump-probe transients reflect the role of the IR pulse in controlling the photodynamics of CH3I+ in the (A) over tilde (2)A(1) state, mainly through the coupling to the ground state (X) over tilde E-2(3/2,1/2) and to the excited (B) over tilde E-2 state manifold. Oscillatory features are observed and attributed to a vibrational wave packet prepared in the (A) over tilde (2)A(1) state. The IR probe pulse induces a coupling between electronic states leading to a slow depletion of CH3+ fragments after the cation is transferred to the ground (X) over tilde E-2(3/2,1/2) states and an enhancement of I+ fragments by absorption of IR photons yielding dissociative photoionization.

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