激子
光致发光
激光线宽
斯托克斯位移
材料科学
堆积
分子物理学
谱线
相干长度
运动变窄
化学
凝聚态物理
光学
物理
光电子学
发光
激光器
超导电性
有机化学
天文
作者
Frank C. Spano,Jenny Clark,Carlos Silva,Richard H. Friend
摘要
The photoluminescence (PL) spectral line shape of regioregular poly(3-hexylthiophene) thin films is analyzed using a model which treats the polymer pi-stacks as H-aggregates with exciton-vibrational coupling and spatially correlated site disorder. The Stokes shift, linewidth, and relative vibronic peak intensities in the low-temperature PL spectrum (T=10 K) are accurately reproduced, allowing the coherence function corresponding to the lowest energy (emitting) exciton to be determined from the ratio of the 0-0 to 0-1 peak intensities. The exciton migration length is determined from the N-dependent Stokes shift, where N is the number of segments comprising the stack. Based on the temperature dependence of the PL spectrum it is concluded that emission arises from a low concentration of aggregates which are more disordered than the dominant species responsible for absorption. The emissive aggregates are characterized by shorter average conjugation lengths and hence greater exciton bandwidths. The coherence length of the emitting exciton is estimated to be only three lattice spacings ( approximately 1.1 nm) along the pi-stacking direction. By contrast, the exciton migration length for incoherent hopping between coherent domains is estimated to be approximately 15 nm.
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