Simulation of pump–probe spectroscopy of a highly-charged diatomic molecule: Role of intermediate charged states and electronic and vibrational excitation in the multiple ionization of Cl2 and strong-field spectroscopy of Cl23+

Abstract

Collisional energy transfer probabilities of highly excited molecules from kinetically controlled selective ionization (KCSI). I. The KCSI technique: Experimental approach for the determination of P(E ′ ,E) in the quasicontinuous energy range A subpicosecond pump-probe laser study of ionization and geminate charge recombination kinetics in alkane liquids This paper is a theoretical study of the effect of a pulsed ir laser on a neutral Cl 2 molecule, leading to the creation of highly-charged molecular ions. We also develop a new quantum-mechanical model for the ionization of diatomic molecules in the tunneling regime. We consider the effects of the pump pulse duration and also the wavelength of the probe laser on the trication Cl 2 3ϩ which is metastable, and consider how an experiment could be performed which would lead to the observation of its vibrational spectrum. The treatment considers nuclear wave packet dynamics which begin with vertical ionization from neutral Cl 2 to Cl 2 2ϩ , includes dynamics arising from the intermediate charged state Cl 2 2ϩ , and electronic excitation and dissociation from the trication Cl 2 3ϩ . The dynamical simulations of a pump-probe experiment show modulated signals which can be Fourier-transformed to yield vibrational spectra. The quality of the modulated signal changes dramatically at an intermediate ͑relative to the vibrational period͒ pump pulse duration ͑at ca. 50 fs͒. Analysis of this effect shows how to maximize the probability of observing a simple vibrational spectrum for a highly charged diatomic created in a laser field.

Interplay of strong chemical bonds and the repulsive Coulomb force in the metastable states of triply ionized homonuclear molecules: A theoretical study of N23+and O23Imamura1, Hatsui2 2012Phys. Rev. A3000View full textAdd to dashboardCite

“…However, several have been examined theoretically and experimentally [6][7][8][9][10][11][12][13]. The experimentally observed species are as follows: diatomic halogens [5,6], SF 3+ [8], B 2 3+ [9], Mo 2 3+ [10], Se 2 3+ [11], Te 2 3+ [11], and LaF 3+ [11]. Except for the SF 3+ , these were reported by using mass spectrometry.…”