Duration of an intense laser pulse can determine the breakage of multiple chemical bonds.
Control over the breakage of a certain chemical bond in a molecule by an ultrashort laser pulse has been considered for decades. With the availability of intense non-resonant laser fields it became possible to pre-determine femtosecond to picosecond molecular bond breakage dynamics by controlled distortions of the electronic molecular system on sub-femtosecond time scales using field-sensitive processes such as strong-field ionization or excitation. So far, all successful demonstrations in this area considered only fragmentation reactions, where only one bond is broken and the molecule is split into merely two moieties. Here, using ethylene (C2H4) as an example, we experimentally investigate whether complex fragmentation reactions that involve the breakage of more than one chemical bond can be influenced by parameters of an ultrashort intense laser pulse. We show that the dynamics of removing three electrons by strong-field ionization determines the ratio of fragmentation of the molecular trication into two respectively three moieties. We observe a relative increase of two-body fragmentations with the laser pulse duration by almost an order of magnitude. Supported by quantum chemical simulations we explain our experimental results by the interplay between the dynamics of electron removal and nuclear motion.
Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, A-1040 Vienna, Austria, EU.
Xinhua
X
Xie
1] Laser Technology Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan [2] RIKEN Center for Advanced Photonics, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan [3] Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan.
Erik
E
Lötstedt
Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, A-1040 Vienna, Austria, EU.
Stefan
S
Roither
Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, A-1040 Vienna, Austria, EU.
Markus
M
Schöffler
Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, A-1040 Vienna, Austria, EU.
Daniil
D
Kartashov
1] Laser Technology Laboratory, RIKEN, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan [2] RIKEN Center for Advanced Photonics, 2-1 Hirosawa, Wako, Saitama 351-0198, Japan.
Katsumi
K
Midorikawa
Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, A-1040 Vienna, Austria, EU.
Andrius
A
Baltuška
Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan.
Kaoru
K
Yamanouchi
Photonics Institute, Vienna University of Technology, Gusshausstrasse 27, A-1040 Vienna, Austria, EU.
Markus
M
Kitzler