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Laser pulse control of exciton dynamics in the FMO complex: Polarization shaping versus effects of structural and energetic disorder

Brüggemann, Ben LU ; Pullerits, Tönu LU and May, V (2006) In Journal of Photochemistry and Photobiology, A: Chemistry 180(3). p.322-327
Abstract
Femtosecond laser pulse control of exciton dynamics in biological chromophore complexes is studied theoretically using the optimal control theory specified to open quantum systems. Based on the laser pulse induced formation of an excitonic wave packet the possibility to localize excitation energy at a certain chromophore within a photosynthetic antenna system (FMO complex of green bacteria) is investigated both for linearly polarized and polarization shaped pulses. Results are presented for an ensemble of N energetically disordered and randomly oriented FMO complexes. Here, the optimized control pulse represents a compromise with respect to the solution of the control task for any individual complex of the ensemble. For the case of an... (More)
Femtosecond laser pulse control of exciton dynamics in biological chromophore complexes is studied theoretically using the optimal control theory specified to open quantum systems. Based on the laser pulse induced formation of an excitonic wave packet the possibility to localize excitation energy at a certain chromophore within a photosynthetic antenna system (FMO complex of green bacteria) is investigated both for linearly polarized and polarization shaped pulses. Results are presented for an ensemble of N energetically disordered and randomly oriented FMO complexes. Here, the optimized control pulse represents a compromise with respect to the solution of the control task for any individual complex of the ensemble. For the case of an ensemble with N = 10 members the polarization shaped control pulse leads to a higher control yield compared with a linearly polarized pulse. This difference becomes considerably smaller for an ensemble with N = 120 members. The respective optimized pulses are used to drive excitation energy in a different ensemble with M >> N complexes to simulate the usual experimental condition in solution. For the case with N = 120, the relative control yield coincides with the resulting control yield "in solution", giving a slightly higher control yield for polarization shaped pulses. (c) 2006 Elsevier B.V. All rights reserved. (Less)
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publication status
published
subject
keywords
photosynthetic antenna system, FMO, exciton, polarization, control, optimal control
in
Journal of Photochemistry and Photobiology, A: Chemistry
volume
180
issue
3
pages
322 - 327
publisher
Elsevier
external identifiers
  • wos:000238669800014
  • scopus:33646936896
ISSN
1873-2666
DOI
10.1016/j.jphotochem.2006.02.026
language
English
LU publication?
yes
additional info
The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)
id
77e51f3f-1cf8-48e4-8e9c-69341ba81ecf (old id 404855)
date added to LUP
2016-04-01 15:19:14
date last changed
2021-10-10 04:13:57
@article{77e51f3f-1cf8-48e4-8e9c-69341ba81ecf,
  abstract     = {Femtosecond laser pulse control of exciton dynamics in biological chromophore complexes is studied theoretically using the optimal control theory specified to open quantum systems. Based on the laser pulse induced formation of an excitonic wave packet the possibility to localize excitation energy at a certain chromophore within a photosynthetic antenna system (FMO complex of green bacteria) is investigated both for linearly polarized and polarization shaped pulses. Results are presented for an ensemble of N energetically disordered and randomly oriented FMO complexes. Here, the optimized control pulse represents a compromise with respect to the solution of the control task for any individual complex of the ensemble. For the case of an ensemble with N = 10 members the polarization shaped control pulse leads to a higher control yield compared with a linearly polarized pulse. This difference becomes considerably smaller for an ensemble with N = 120 members. The respective optimized pulses are used to drive excitation energy in a different ensemble with M >> N complexes to simulate the usual experimental condition in solution. For the case with N = 120, the relative control yield coincides with the resulting control yield "in solution", giving a slightly higher control yield for polarization shaped pulses. (c) 2006 Elsevier B.V. All rights reserved.},
  author       = {Brüggemann, Ben and Pullerits, Tönu and May, V},
  issn         = {1873-2666},
  language     = {eng},
  number       = {3},
  pages        = {322--327},
  publisher    = {Elsevier},
  series       = {Journal of Photochemistry and Photobiology, A: Chemistry},
  title        = {Laser pulse control of exciton dynamics in the FMO complex: Polarization shaping versus effects of structural and energetic disorder},
  url          = {http://dx.doi.org/10.1016/j.jphotochem.2006.02.026},
  doi          = {10.1016/j.jphotochem.2006.02.026},
  volume       = {180},
  year         = {2006},
}