Nonexponentialities in the ultrafast electron-transfer dynamics in the system oxazine 1 in N,N-dimethylaniline

被引:61
作者
Engleitner, S [1 ]
Seel, M [1 ]
Zinth, W [1 ]
机构
[1] Univ Munich, Inst Med Opt, D-80538 Munich, Germany
关键词
D O I
10.1021/jp9843712
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
Transient absorption experiments with probing in the blue part of the spectrum (440-500 nm) are performed for the electron-transfer system oxazine 1 in N,N-dimethylaniline. The experiments with high time resolution of better than 20 fs show pronounced modulations due to high-frequency wave packet motion (600 cm(-1)) in the excited electronic state of the oxazine I molecule before electron transfer. Additionally, modulations due to wave packet motion in the product state of oxazine 1 after complete charge separation are observed. The absorption transients related to the electron transfer from N,N-dimethylaniline to oxazine 1 are clearly nonmonoexponential with time constants of 30 and 80 fs. This behavior points to a strong adiabaticity of the electron-transfer reaction with a high relevance of nuclear motions.
引用
收藏
页码:3013 / 3019
页数:7
相关论文
共 24 条
  • [1] EXCITATION TRANSFER IN THE CORE LIGHT-HARVESTING COMPLEX (LH-1) OF RHODOBACTER-SPHAEROIDES - AN ULTRAFAST FLUORESCENCE DEPOLARIZATION AND ANNIHILATION STUDY
    BRADFORTH, SE
    JIMENEZ, R
    VANMOURIK, F
    VANGRONDELLE, R
    FLEMING, GR
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (43) : 16179 - 16191
  • [2] THEORY OF ULTRAFAST NONADIABATIC EXCITED-STATE PROCESSES AND THEIR SPECTROSCOPIC DETECTION IN REAL TIME
    Domcke, Wolfgang
    Stock, Gerhard
    [J]. ADVANCES IN CHEMICAL PHYSICS <D>, 1997, 100 : 1 - 169
  • [3] EXPERIMENTAL-DETERMINATION OF THE DYNAMICS OF A MOLECULAR NUCLEAR WAVE-PACKET VIA THE SPECTRA OF SPONTANEOUS EMISSION
    DUNN, TJ
    SWEETSER, JN
    WALMSLEY, IA
    RADZEWICZ, C
    [J]. PHYSICAL REVIEW LETTERS, 1993, 70 (22) : 3388 - 3391
  • [4] COMPRESSION OF OPTICAL PULSES TO 6 FEMTOSECONDS BY USING CUBIC PHASE COMPENSATION
    FORK, RL
    CRUZ, CHB
    BECKER, PC
    SHANK, CV
    [J]. OPTICS LETTERS, 1987, 12 (07) : 483 - 485
  • [5] COHERENT EFFECTS IN PUMP PROBE SPECTROSCOPY OF EXCITONS
    JOFFRE, M
    HULIN, D
    MIGUS, A
    ANTONETTI, A
    LAGUILLAUME, CBA
    PEYGHAMBARIAN, N
    LINDBERG, M
    KOCH, SW
    [J]. OPTICS LETTERS, 1988, 13 (04) : 276 - 278
  • [6] SUBPICOSECOND TRANSIENT ABSORPTION STUDY OF INTERMOLECULAR ELECTRON-TRANSFER BETWEEN SOLUTE AND ELECTRON-DONATING SOLVENTS
    KANDORI, H
    KEMNITZ, K
    YOSHIHARA, K
    [J]. JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (20) : 8042 - 8048
  • [7] SUBPICOSECOND FLUORESCENCE DYNAMICS OF DYE MOLECULES
    MOKHTARI, A
    CHEBIRA, A
    CHESNOY, J
    [J]. JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS, 1990, 7 (08) : 1551 - 1557
  • [8] QUANTUM-MECHANICAL THEORY FOR 6-FS DYNAMIC ABSORPTION-SPECTROSCOPY AND ITS APPLICATION TO NILE BLUE
    POLLARD, WT
    FRAGNITO, HL
    BIGOT, JY
    SHANK, CV
    MATHIES, RA
    [J]. CHEMICAL PHYSICS LETTERS, 1990, 168 (3-4) : 239 - 245
  • [9] POLLARD WT, 1992, ANNU REV PHYS CHEM, V43, P497, DOI 10.1146/annurev.physchem.43.1.497
  • [10] FEMTOSECOND REAL-TIME OBSERVATION OF WAVE PACKET OSCILLATIONS (RESONANCE) IN DISSOCIATION REACTIONS
    ROSE, TS
    ROSKER, MJ
    ZEWAIL, AH
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1988, 88 (10) : 6672 - 6673