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Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins

Authors :
Jean-Pierre Wolf
Jonathan Roslund
Véronique Boutou
Matthias Roth
François Courvoisier
Laurent Guyon
Herschel Rabitz
Department of Chemistry
Princeton University
Laboratoire de Spectrométrie Ionique et Moléculaire (LASIM)
Université Claude Bernard Lyon 1 (UCBL)
Université de Lyon-Université de Lyon-Centre National de la Recherche Scientifique (CNRS)
Group of Applied Physics [Geneva] (GAP)
University of Geneva [Switzerland]
Source :
Journal of Chemical Physics, Journal of Chemical Physics, American Institute of Physics, 2011, 134 (3), pp.034511. ⟨10.1063/1.3518751⟩, Journal of Chemical Physics, Vol. 134, No 3 (2011) P. 034511
Publication Year :
2011
Publisher :
HAL CCSD, 2011.

Abstract

Fundamental molecular selectivity limits are probed by exploiting laser-controlled quantum interferences for the creation of distinct spectral signatures in two flavin molecules, erstwhile nearly indistinguishable via steady-state methods. Optimal dynamic discrimination (ODD) uses optimally shaped laser fields to transiently amplify minute molecular variations that would otherwise go unnoticed with linear absorption and fluorescence techniques. ODD is experimentally demonstrated by combining an optimally shaped UV pump pulse with a time-delayed, fluorescence-depleting IR pulse for discrimination amongst riboflavin and flavin mononucleotide in aqueous solution, which are structurally and spectroscopically very similar. Closed-loop, adaptive pulse shaping discovers a set of UV pulses that induce disparate responses from the two flavins and allows for concomitant flavin discrimination of ∼16σ. Additionally, attainment of ODD permits quantitative, analytical detection of the individual constituents in a flavin mixture. The successful implementation of ODD on quantum systems of such high complexity bodes well for the future development of the field and the use of ODD techniques in a variety of demanding practical applications.

Details

Language :
English
ISSN :
00219606 and 10897690
Database :
OpenAIRE
Journal :
Journal of Chemical Physics, Journal of Chemical Physics, American Institute of Physics, 2011, 134 (3), pp.034511. ⟨10.1063/1.3518751⟩, Journal of Chemical Physics, Vol. 134, No 3 (2011) P. 034511
Accession number :
edsair.doi.dedup.....3a1568100f07bfaeda4d5fbaefff6630
Full Text :
https://doi.org/10.1063/1.3518751⟩