Hefei National Laboratory for Physical Science at Microscale, and Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, People's Republic of China.
J Phys Chem A. 2009 Nov 19;113(46):12847-56. doi: 10.1021/jp904105p.
We present a theoretical study on the temperature-dependent absorption and photoluminescence spectroscopy of rubrene multichromophores by combining the time-dependent long-range-corrected density functional theory with the exciton model. The spectra of rubrene multichromophores up to heptamers are calculated, and the effects of exciton-phonon coupling and temperature on the photophysical properties of both H- and J-aggregated oligomers are addressed. It is found that the spectral behavior of rubrene aggregates is very much dependent on aggregation details. As the temperature increases, higher excitonic states become populated, and low-energy dark states in H-aggregated oligomers become observable gradually while the peak intensities near the 0-0 transition decrease for J-aggregated oligomers.
我们通过结合时变长程修正密度泛函理论和激子模型，对并五苯多发色团的温度相关吸收和光致发光光谱进行了理论研究。计算了并五苯多发色团高达七聚体的光谱，并研究了激子-声子耦合和温度对 H-和 J-聚集低聚物光物理性质的影响。结果表明，并五苯聚集体的光谱行为非常依赖于聚集细节。随着温度的升高，更高的激子态被占据，而 H-聚集低聚物中低能暗态逐渐变得可见，而 J-聚集低聚物中 0-0 跃迁附近的峰强度减小。
