Exciton relaxation and polaron formation in LH2 at low temperature

被引:64
作者
Polivka, T [1 ]
Pullerits, T [1 ]
Herek, JL [1 ]
Sundström, V [1 ]
机构
[1] Univ Lund, S-22100 Lund, Sweden
来源
JOURNAL OF PHYSICAL CHEMISTRY B | 2000年 / 104卷 / 05期
关键词
D O I
10.1021/jp9915984
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Excited state dynamics of antenna complexes in an LH2-only mutant of the purple bacterium Rb, sphaeroides have been investigated by means of two-color femtosecond spectroscopy combined with computer simulations. Measurements of transient absorption spectra revealed a new spectral band in the stimulated emission region around 880 nm at 6 K. To simulate this new dynamic feature that appears within the first 2 ps after light absorption. we have used a simplified polaron model via a decoupled red pigment within the B850 ring. Comparison of simulations and experiment suggests the following kinetic scheme: (1) initial ultrafast (similar to 100 fs) dynamics correspond to exciton relaxation to the lowest exciton state; (2) mixing of the lowest exciton state with charge-transfer states results in a relaxation to these states in about 600 fs; (3) picosecond dielectric relaxation in the charge-transfer states corresponding to polaron formation follows.
引用
收藏
页码:1088 / 1096
页数:9
相关论文
共 42 条
[1]   Calculations of spectroscopic properties of the LH2 bacteriochlorophyll - Protein antenna complex from Rhodopseudomonas acidophila [J].
Alden, RG ;
Johnson, E ;
Nagarajan, V ;
Parson, WW ;
Law, CJ ;
Cogdell, RG .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (23) :4667-4680
[2]   PROPERTIES OF THE EXCITED-SINGLET STATES OF BACTERIOCHLOROPHYLL-A AND BACTERIOPHEOPHYTIN-A IN POLAR-SOLVENTS [J].
BECKER, M ;
NAGARAJAN, V ;
PARSON, WW .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1991, 113 (18) :6840-6848
[3]   Characterization of the light-harvesting antennas of photosynthetic purple bacteria by stark spectroscopy .2. LH2 complexes: Influence of the protein environment [J].
Beekman, LMP ;
Frese, RN ;
Fowler, GJS ;
Picorel, R ;
Cogdell, RJ ;
vanStokkum, IHM ;
Hunter, CN ;
vanGrondelle, R .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (37) :7293-7301
[4]   Excitons in photosynthetic purple bacteria: Wavelike motion or incoherent hopping? [J].
Chachisvilis, M ;
Kuhn, O ;
Pullerits, T ;
Sundstrom, V .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (37) :7275-7283
[5]   VIBRATIONAL DYNAMICS IN THE LIGHT-HARVESTING COMPLEXES OF THE PHOTOSYNTHETIC BACTERIUM RHODOBACTER-SPHAEROIDES [J].
CHACHISVILIS, M ;
PULLERITS, T ;
JONES, MR ;
HUNTER, CN ;
SUNDSTROM, V .
CHEMICAL PHYSICS LETTERS, 1994, 224 (3-4) :345-351
[6]  
CHACHISVILIS M, 1996, THESIS LUND U SWEDEN, pCH5
[7]   Electronic excitations in aggregates of bacteriochlorophylls [J].
Cory, MG ;
Zerner, MC ;
Xu, XC ;
Shulten, K .
JOURNAL OF PHYSICAL CHEMISTRY B, 1998, 102 (39) :7640-7650
[8]   Exciton delocalization in the antenna of purple bacteria: Exciton spectrum calculations using X-ray data and experimental site inhomogeneity [J].
Dracheva, TV ;
Novoderezhkin, VI ;
Razjivin, AP .
FEBS LETTERS, 1996, 387 (01) :81-84
[9]  
DVAYDOV AS, 1971, THEORY MOL EXCITONS
[10]   FRENKEL EXCITONS IN A VIBRATING MOLECULAR CRYSTAL [J].
FISCHER, S ;
RICE, SA .
JOURNAL OF CHEMICAL PHYSICS, 1970, 52 (04) :2089-&