在PCDTBT中激发形成,放松和衰变
Natalie Banerji1, Sarah Cowan, Mario Leclerc
1Center for Polymers and Organic Solids, University of California at Santa Barbara, Santa Barbara, California 93106-5090, USA.
Journal of the American Chemical Society
|November 20, 2010
概括
像PCDTBT这样的原始合聚合物在皮秒钟内形成激子. 这些刺激子迁移和放松,这一过程比PCDTBT:富勒烯混合物中的电荷转移要慢得多,这表明了超快电荷分离的替代机制.
科学领域:
- 有机电子学有机电子学
- 结合聚合物的光物理学
背景情况:
- 结合聚合物是有机电子产品的关键材料.
- 了解初级激发动态对于设备的效率至关重要.
研究的目的:
- 调查原始PCDTBT中激发的时间演变.
- 在薄膜和溶液中比较放松动态.
- 澄清光诱导电荷分离的机制.
主要方法:
- 5秒分辨率的光上转换光谱学.
- 在PCDTBT薄膜和溶液上的测量.
- 偏振敏感和波长依赖的研究.
主要成果:
- 移动充电的光生成,然后在100 fs以内进行自我定位.
- 在<1 ps. 中形成结合的单点刺激子.
- 刺激迁移和构造性放松发生在500 fs到几十个皮秒的时间内.
结论:
- 在PCDTBT中,刺激子的形成和迁移比PCDTBT:富勒烯混合物中的电荷转移要慢.
- 挑战了电荷分离之前的激子扩散模型.
- 提出了在激电定位之前进行超快电荷分离的替代机制.
相关概念视频
Thermal and Photochemical Electrocyclic Reactions: Overview
Electrocyclic reactions are reversible reactions. They involve an intramolecular cyclization or ring-opening of a conjugated polyene. Shown below are two examples of electrocyclic reactions. In the first reaction, the formation of the cyclic product is favored. In contrast, in the second reaction, ring-opening is favored due to the high ring strain associated with cyclobutene formation.
Photochemical Electrocyclic Reactions: Stereochemistry
The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
Selection Rules: Photochemical Activation
Selection Rules: Photochemical Activation
Deactivation Processes: Jablonski Diagram
Luminescence, the emission of light by a substance that has absorbed energy, is a process that involves the interaction of molecules with light. The energy-level diagram, or Jablonski diagram, is a graphical representation of these interactions, illustrating the various states and transitions a molecule can undergo. In a typical Jablonski diagram, the lowest horizontal line represents the ground-state energy of the molecule, which is usually a singlet state. This state represents the energies...
Atomic Nuclei: Types of Nuclear Relaxation
Nuclear relaxation restores the equilibrium population imbalance and can occur via spin–lattice or spin–spin mechanisms, which are first-order exponential decay processes.
In spin–lattice or longitudinal relaxation, the excited spins exchange energy with the surrounding lattice as they return to the lower energy level. Among several mechanisms that contribute to spin–lattice relaxation, magnetic dipolar interactions are significant. Here, the excited nucleus transfers energy to a nearby...
In spin–lattice or longitudinal relaxation, the excited spins exchange energy with the surrounding lattice as they return to the lower energy level. Among several mechanisms that contribute to spin–lattice relaxation, magnetic dipolar interactions are significant. Here, the excited nucleus transfers energy to a nearby...
Thermal Electrocyclic Reactions: Stereochemistry
The stereochemistry of electrocyclic reactions is strongly influenced by the orbital symmetry of the polyene HOMO. Under thermal conditions, the reaction proceeds via the ground-state HOMO.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.
Selection Rules: Thermal Activation
Conjugated systems containing an even number of π-electron pairs undergo a conrotatory ring closure. For example, thermal electrocyclization of (2E,4E)-2,4-hexadiene, a conjugated diene containing two π-electron pairs, gives trans-3,4-dimethylcyclobutene.
Carrier Generation and Recombination
Carrier generation is the process by which electron-hole pairs (EHPs) are created within the semiconductor. In direct-bandgap semiconductors, such as gallium arsenide (GaAs), this occurs efficiently when energy absorption prompts valence electrons to leap into the conduction band, leaving behind holes.
This process is given by the generation rate G and is efficient due to the conservation of momentum between the valence band maximum and conduction band minimum.
Indirect generation involves an...
This process is given by the generation rate G and is efficient due to the conservation of momentum between the valence band maximum and conduction band minimum.
Indirect generation involves an...


