CaltechAUTHORS
  A Caltech Library Service

Dark Structures in Molecular Radiationless Transitions Determined by Ultrafast Diffraction

Srinivasan, Ramesh and Feenstra, Jonathan S. and Park, Sang Tae and Xu, Shoujun and Zewail, Ahmed H. (2005) Dark Structures in Molecular Radiationless Transitions Determined by Ultrafast Diffraction. Science, 307 (5709). pp. 558-563. ISSN 0036-8075. http://resolver.caltech.edu/CaltechAUTHORS:20141114-123532852

[img]
Preview
PDF - Supplemental Material
See Usage Policy.

114Kb

Use this Persistent URL to link to this item: http://resolver.caltech.edu/CaltechAUTHORS:20141114-123532852

Abstract

The intermediate structures formed through radiationless transitions are termed “dark” because their existence is inferred indirectly from radiative transitions. We used ultrafast electron diffraction to directly determine these transient structures on both ground-state and excited-state potential energy surfaces of several aromatic molecules. The resolution in space and time (0.01 angstrom and 1 picosecond) enables differentiation between competing nonradiative pathways of bond breaking, vibronic coupling, and spin transition. For the systems reported here, the results reveal unexpected dynamical behavior. The observed ring opening of the structure depends on molecular substituents. This, together with the parallel bifurcation into physical and chemical channels, redefines structural dynamics of the energy landscape in radiationless processes.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1126/science.1107291DOIArticle
http://www.sciencemag.org/content/307/5709/558PublisherArticle
http://www.sciencemag.org/content/307/5709/558/suppl/DC1PublisherSupporting Online Material
Additional Information:© 2005 American Association for the Advancement of Science. Received 9 November 2004; accepted 21 December 2004; Published online 6 January 2005. Supported by NSF and the U.S. Air Force Office of Scientific Research.
Funders:
Funding AgencyGrant Number
NSFUNSPECIFIED
Air Force Office of Scientific Research (AFOSR)UNSPECIFIED
Record Number:CaltechAUTHORS:20141114-123532852
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20141114-123532852
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:51779
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:14 Nov 2014 21:53
Last Modified:19 Feb 2015 19:42

Repository Staff Only: item control page