Exciton delocalization in the B850 light-harvesting complex: Comparison of different measures

M. Dahlbom; T. Pullerits; S. Mukamel; V. Sundström

doi:10.1021/jp004496i

Exciton delocalization in the B850 light-harvesting complex: Comparison of different measures

M. Dahlbom, T. Pullerits, S. Mukamel, V. Sundström

Chemical Physics

University of Rochester

Research output: Contribution to journal › Article › peer-review

Abstract

A much debated topic in recent studies of ultrafast exciton dynamics in molecular aggregates has been the precise definition of the exciton coherence domain in the B850 aggregate of photosynthetic purple bacteria. In this work we compare several measures of exciton delocalization and their variation with temperature, inhomogeneous broadening, and time. We find that the exciton wave packet prepared by a 40 fs pulse is initially delocalized over a substantial portion of the ring and contracts to a significantly smaller size on the time scale of a few hundreds of femtoseconds. Steady-state absorption and time-dependent pump-probe spectra of the B850 aggregate are simulated and compare well with previously reported experimental data. The calculated thermalized exciton wave packet size is in good agreement with previous experimental and theoretical estimates.

Original language	English
Pages (from-to)	5515-5524
Number of pages	10
Journal	Journal of Physical Chemistry B
Volume	105
Issue number	23
DOIs	https://doi.org/10.1021/jp004496i
Publication status	Published - 2001 Jun 14

Subject classification (UKÄ)

Physical Chemistry (including Surface- and Colloid Chemistry)

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10.1021/jp004496i

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@article{3dfc206c914249908932154b80be88f0,

title = "Exciton delocalization in the B850 light-harvesting complex: Comparison of different measures",

abstract = "A much debated topic in recent studies of ultrafast exciton dynamics in molecular aggregates has been the precise definition of the exciton coherence domain in the B850 aggregate of photosynthetic purple bacteria. In this work we compare several measures of exciton delocalization and their variation with temperature, inhomogeneous broadening, and time. We find that the exciton wave packet prepared by a 40 fs pulse is initially delocalized over a substantial portion of the ring and contracts to a significantly smaller size on the time scale of a few hundreds of femtoseconds. Steady-state absorption and time-dependent pump-probe spectra of the B850 aggregate are simulated and compare well with previously reported experimental data. The calculated thermalized exciton wave packet size is in good agreement with previous experimental and theoretical estimates.",

author = "M. Dahlbom and T. Pullerits and S. Mukamel and V. Sundstr{\"o}m",

year = "2001",

month = jun,

day = "14",

doi = "10.1021/jp004496i",

language = "English",

volume = "105",

pages = "5515--5524",

journal = "Journal of Physical Chemistry B",

issn = "1089-5647",

publisher = "The American Chemical Society (ACS)",

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TY - JOUR

T1 - Exciton delocalization in the B850 light-harvesting complex

T2 - Comparison of different measures

AU - Dahlbom, M.

AU - Pullerits, T.

AU - Mukamel, S.

AU - Sundström, V.

PY - 2001/6/14

Y1 - 2001/6/14

N2 - A much debated topic in recent studies of ultrafast exciton dynamics in molecular aggregates has been the precise definition of the exciton coherence domain in the B850 aggregate of photosynthetic purple bacteria. In this work we compare several measures of exciton delocalization and their variation with temperature, inhomogeneous broadening, and time. We find that the exciton wave packet prepared by a 40 fs pulse is initially delocalized over a substantial portion of the ring and contracts to a significantly smaller size on the time scale of a few hundreds of femtoseconds. Steady-state absorption and time-dependent pump-probe spectra of the B850 aggregate are simulated and compare well with previously reported experimental data. The calculated thermalized exciton wave packet size is in good agreement with previous experimental and theoretical estimates.

AB - A much debated topic in recent studies of ultrafast exciton dynamics in molecular aggregates has been the precise definition of the exciton coherence domain in the B850 aggregate of photosynthetic purple bacteria. In this work we compare several measures of exciton delocalization and their variation with temperature, inhomogeneous broadening, and time. We find that the exciton wave packet prepared by a 40 fs pulse is initially delocalized over a substantial portion of the ring and contracts to a significantly smaller size on the time scale of a few hundreds of femtoseconds. Steady-state absorption and time-dependent pump-probe spectra of the B850 aggregate are simulated and compare well with previously reported experimental data. The calculated thermalized exciton wave packet size is in good agreement with previous experimental and theoretical estimates.

UR - https://www.scopus.com/pages/publications/0035859428

U2 - 10.1021/jp004496i

DO - 10.1021/jp004496i

M3 - Article

AN - SCOPUS:0035859428

SN - 1089-5647

VL - 105

SP - 5515

EP - 5524

JO - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

IS - 23

ER -

Exciton delocalization in the B850 light-harvesting complex: Comparison of different measures

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