title: Multidirectional Angular Electronic Flux during Adiabatic Attosecond Charge Migration in Excited Benzene.
abstract: Recently, adiabatic attosecond charge migration (AACM) has been monitored and simulated for the first time, with application to the oriented iodoacetylene cation where AACM starts from the initial superposition of the ground state (φ0) and an electronic excited state (φ1). Here, we develop the theory for electronic fluxes during AACM in ring-shaped molecules, with application to oriented benzene prepared in the superposition of the ground and first excited singlet states. The initial state and its time evolution are analogous to coherent tunneling where φ0 and φ1 have different meanings; however, they denote the wave functions of the lowest tunneling doublet. This analogy suggests to transfer the theory of electronic fluxes during coherent tunneling to AACM, with suitable modifications which account for (i) the different time scales and (ii) the different electronic states, and which make use of (iii) the preparation of the initial state for AACM by a linearly polarized laser pulse. Application to benzene yields the multidirectional angular electronic flux with a pincer-motion type pattern during AACM: this unequivocal result confirms a previous working hypothesis. Moreover, the theory of AACM allows quantification of the electronic flux; that is, the maximum number of electrons (out of 42) which flow concertedly during AACM in benzene is 6 × 0.08 = 0.48.
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.
authors.forename: Gunter
authors.initials: G
authors.lastname: Hermann
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.
authors.forename: ChunMei
authors.initials: C
authors.lastname: Liu
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.|State Key Laboratory of Quantum Optics and Quantum Optics Devices, Institute of Laser Spectroscopy, Shanxi University , Taiyuan 030006, China.|Collaborative Innovation Center of Extreme Optics, Shanxi University , Taiyuan 030006, China.
authors.forename: Jörn
authors.initials: J
authors.lastname: Manz
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.
authors.forename: Beate
authors.initials: B
authors.lastname: Paulus
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.
authors.forename: Jhon Fredy
authors.initials: JF
authors.lastname: Pérez-Torres
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.
authors.forename: Vincent
authors.initials: V
authors.lastname: Pohl
authors.affiliation: Freie Universität Berlin , Institut für Chemie und Biochemie, Takustrasse 3, 14195 Berlin, Germany.
authors.forename: Jean Christophe
authors.initials: JC
authors.lastname: Tremblay