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Title: How Shaped Light Discriminates Nearly Identical Biochromophores

Journal Article · · Physical Review Letters
 [1];  [2];  [1];  [3]; ;  [4]
  1. Department of Chemistry, Humboldt-Universitaet zu Berlin, Brook-Taylor-Str. 2, 12489 Berlin (Germany)
  2. Department of Physics, Freie Universitaet Berlin, Arnimallee 14, 14195 Berlin (Germany)
  3. GAP, University of Geneva, 20 rue de l'Ecole de Medecine, CH 1211 Geneva 4 (Switzerland)
  4. Department of Chemistry, Princeton University, Princeton, New Jersey 08544 (United States)

We present a general mechanism for successful discrimination of spectroscopically indistinguishable biochromophores by shaped light. For this purpose we use nonadiabatic dynamics in excited electronic states in the frame of the field-induced surface hopping method driven by the experimentally shaped laser fields. Our findings show that optimal laser fields drive low-frequency vibrational modes localized in the side chains of two biochromophores, thus selecting the parts of their potential energy surfaces characterized by different transition dipole moments leading to different ionization probabilities. The presented mechanism leads to selective fluorescence depletion which serves as a discrimination signal. Our findings offer a promising perspective for using optimally shaped laser pulses in bioanalytical applications by increasing the selectivity beyond the current capability.

OSTI ID:
21470957
Journal Information:
Physical Review Letters, Vol. 105, Issue 7; Other Information: DOI: 10.1103/PhysRevLett.105.073003; (c) 2010 American Institute of Physics; ISSN 0031-9007
Country of Publication:
United States
Language:
English