Selective Excitation of Atomic-Scale Dynamics by Coherent Exciton

Letter pubs.acs.org/JPCL

Selective Excitation of Atomic-Scale Dynamics by Coherent Exciton Motion in the Non-Born−Oppenheimer Regime Zhaogang Nie,† Run Long,‡,§ Jialin Li,† Yi Ying Zheng,† Oleg V. Prezhdo,*,‡ and Zhi-Heng Loh*,† †

Division of Chemistry and Biological Chemistry, and Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, Singapore 631371, Singapore ‡ Department of Chemistry, University of Rochester, RC Box 270216, Rochester, New York 14627, United States § School of Physics, Complex Adaptive Systems Laboratory, University College Dublin, Belfield, Dublin 4, Ireland S Supporting Information *

ABSTRACT: Time-domain investigations of the nonadiabatic coupling between electronic and vibrational degrees of freedom have focused primarily on the formation of electronic superpositions induced by atomic motion. The effect of electronic nonstationary-state dynamics on atomic motion remains unexplored. Here, phasecoherent excitation of the two lowest electronic transitions in semiconducting singlewalled carbon nanotubes by broadband