TY - JOUR
T1 - Photoinduced ultrafast dynamics of Ru(dcbpy)2(NCS)2-sensitized nanocrystalline TiO2 films
T2 - The influence of sample preparation and experimental conditions
AU - Kallioinen, Jani
AU - Benkö, Gabor
AU - Myllyperkiö, Pasi
AU - Khriachtchev, Leonid
AU - Skårman, Björn
AU - Wallenberg, Reine
AU - Tuomikoski, Markus
AU - Korppi-Tommola, Jouko
AU - Sundström, Villy
AU - Yartsev, Arkady P.
PY - 2004
Y1 - 2004
N2 - In most of the previous ultrafast electron injection studies of Ru(dcbpy)2(NCS)2-sensitized nanocrystalline TiO2 films, experimental conditions and sample preparation have been different from study to study and no studies of how the differences affect the observed dynamics have been reported. In the present paper, we have investigated the influence of such modifications. Pump photon density, environment of the sensitized film (solvent and air), and parameters of the film preparation (crystallinity and quality of the film) were varied in a systematic way and the obtained dynamics were compared to that of a well-defined reference sample: Ru(dcbpy)2(NCS)2−TiO2 in acetonitrile. In some cases, the induced changes in the dynamics were uncorrelated to the electron injection process. High pump photon density (not in the linear response region) and exposure of the sensitized film to air altered the picosecond-time-scale kinetics considerably, and the changes were attributed mostly to degradation of the dye. In other cases, changes in the measured kinetics were related to the electron injection processes: reducing the firing temperature of the nanocrystalline film or making the film via electron beam evaporation (EBE) resulted in a decrease of the overall crystallinity of the film, and the electron injection slowed. In the sensitized EBE films, in addition to an increased contribution of triplet excited-state electron injection, a new electron transfer (ET) process with a time constant of 200 fs was observed.
AB - In most of the previous ultrafast electron injection studies of Ru(dcbpy)2(NCS)2-sensitized nanocrystalline TiO2 films, experimental conditions and sample preparation have been different from study to study and no studies of how the differences affect the observed dynamics have been reported. In the present paper, we have investigated the influence of such modifications. Pump photon density, environment of the sensitized film (solvent and air), and parameters of the film preparation (crystallinity and quality of the film) were varied in a systematic way and the obtained dynamics were compared to that of a well-defined reference sample: Ru(dcbpy)2(NCS)2−TiO2 in acetonitrile. In some cases, the induced changes in the dynamics were uncorrelated to the electron injection process. High pump photon density (not in the linear response region) and exposure of the sensitized film to air altered the picosecond-time-scale kinetics considerably, and the changes were attributed mostly to degradation of the dye. In other cases, changes in the measured kinetics were related to the electron injection processes: reducing the firing temperature of the nanocrystalline film or making the film via electron beam evaporation (EBE) resulted in a decrease of the overall crystallinity of the film, and the electron injection slowed. In the sensitized EBE films, in addition to an increased contribution of triplet excited-state electron injection, a new electron transfer (ET) process with a time constant of 200 fs was observed.
KW - dye-sensitized solar cell
KW - solar cells
KW - solar energy
KW - electron injection
KW - electron transfer
U2 - 10.1021/jp037265v
DO - 10.1021/jp037265v
M3 - Article
SN - 1520-6106
VL - 108
SP - 6365
EP - 6373
JO - The Journal of Physical Chemistry B
JF - The Journal of Physical Chemistry B
IS - 20
ER -