Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 106, Issue 19, Pages 7714-7717Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0901833106
Keywords
coherent control; quantum-control spectroscopy; solvation dynamics
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Funding
- Stichting voor Fundamenteel Onderzoek der Materie (FOM)
- Nederlandse organisatie voor Wetenschappelijk Onderzoek (NWO)
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Coherent control holds the promise of becoming a powerful spectroscopic tool for the study of complex molecular systems. Achieving control requires coherence in the quantum system under study. In the condensed phase, coherence is typically lost rapidly because of fluctuating interactions between the solvated molecule and its surrounding environment. We investigate the degree of attainable control on a dye molecule when the fluctuations of its environment are systematically varied. A single successful learning curve for optimizing stimulated emission from the dye in solution is reapplied for a range of solvents with varying viscosity, revealing a striking trend that is correlated directly with the dephasing time. Our results provide clear evidence that the environment limits the leverage of control on the molecular system. This insight can be used to enhance the yield of control experiments greatly.
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