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

Jonathan Roslund, Matthias Roth, Laurent Guyon, Véronique Boutou, Francois Courvoisier, Jean Pierre Wolf, Herschel Rabitz

Research output: Contribution to journalArticle

19 Scopus citations

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 ∼16. 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.

Original languageEnglish (US)
Article number034511
JournalJournal of Chemical Physics
Volume134
Issue number3
DOIs
StatePublished - Jan 21 2011

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Fingerprint Dive into the research topics of 'Resolution of strongly competitive product channels with optimal dynamic discrimination: Application to flavins'. Together they form a unique fingerprint.

  • Cite this