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Coherent Control of Bond Making

Liat Levin1, Wojciech Skomorowski2, Leonid Rybak1, Ronnie Kosloff3, Christiane P. Koch2, and Zohar Amitay1

  • 1The Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel
  • 2Theoretische Physik, Universität Kassel, Heinrich-Plett-Straße 40, 34132 Kassel, Germany
  • 3Fritz Haber Research Centre and The Department of Physical Chemistry, Hebrew University, Jerusalem 91904, Israel

Phys. Rev. Lett. 114, 233003 – Published 10 June, 2015

DOI: https://doi.org/10.1103/PhysRevLett.114.233003

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.

Synopsis

On-Demand Chemical Bond Formation

Published 10 June, 2015

A tailored laser pulse controls the formation of a molecular bond between two atoms.

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