Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 106, Issue 27, Pages 10896-10900Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0904589106
Keywords
coherent control; photoisomerization; ultrafast science
Categories
Funding
- National Science Foundation [CHE 0718219, PHY 0649578]
- FOCUS Center at the University of Michigan
- Division Of Physics
- Direct For Mathematical & Physical Scien [0969322] Funding Source: National Science Foundation
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A learning algorithm was used to manipulate optical pulse shapes and optimize retinal isomerization in bacteriorhodopsin, for excitation levels up to 1.8 x 10(16) photons per square centimeter. Below 1/3 the maximum excitation level, the yield was not sensitive to pulse shape. Above this level the learning algorithm found that a Fourier-transform-limited (TL) pulse maximized the 13-cis population. For this optimal pulse the yield increases linearly with intensity well beyond the saturation of the first excited state. To understand these results we performed systematic searches varying the chirp and energy of the pump pulses while monitoring the isomerization yield. The results are interpreted including the influence of 1-photon and multiphoton transitions. The population dynamics in each intermediate conformation and the final branching ratio between the all-trans and 13-cis isomers are modified by changes in the pulse energy and duration.
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