title: Coherent Control of Bond Making.
abstract: We demonstrate coherent control of bond making, a milestone on the way to coherent control of photoinduced bimolecular chemical reactions. In strong-field multiphoton femtosecond photoassociation experiments, we find the yield of detected magnesium dimer molecules to be enhanced for positively chirped pulses and suppressed for negatively chirped pulses. Our ab initio model shows that control is achieved by purification combined with chirp-dependent Raman transitions. Experimental closed-loop phase optimization using a learning algorithm yields an improved pulse that utilizes vibrational coherent dynamics in addition to chirp-dependent Raman transitions. Our results show that coherent control of binary photoreactions is feasible even under thermal conditions.
authors.affiliation: The Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel.
authors.forename: Liat
authors.initials: L
authors.lastname: Levin
authors.affiliation: Theoretische Physik, Universität Kassel, Heinrich-Plett-Straße 40, 34132 Kassel, Germany.
authors.forename: Wojciech
authors.initials: W
authors.lastname: Skomorowski
authors.affiliation: The Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel.
authors.forename: Leonid
authors.initials: L
authors.lastname: Rybak
authors.affiliation: Fritz Haber Research Centre and The Department of Physical Chemistry, Hebrew University, Jerusalem 91904, Israel.
authors.forename: Ronnie
authors.initials: R
authors.lastname: Kosloff
authors.affiliation: Theoretische Physik, Universität Kassel, Heinrich-Plett-Straße 40, 34132 Kassel, Germany.
authors.forename: Christiane P
authors.initials: CP
authors.lastname: Koch
authors.affiliation: The Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel.
authors.forename: Zohar
authors.initials: Z
authors.lastname: Amitay