论文标题
线性分子聚集体中激子和电荷转移态之间耦合的光学签名
Optical Signatures of the Coupling between Excitons and Charge Transfer States in Linear Molecular Aggregates
论文作者
论文摘要
电荷转移（CT）由于对分子结构的实验控制增加，导致在例如光伏和氢生产中应用的实验控制，因此具有连续的兴趣。在本文中，我们使用散射矩阵技术研究了CT状态对线性分子聚集体吸收光谱的影响，该技术使我们能够处理任意大型系统。提出的理论对于激子和CT状态的强和弱混合都很好，弥合了先前使用的方法之间仅适用于这些限制之一的差距。在实验光谱中，均匀的线宽通常太大而无法单独解决所有光学允许的过渡，从而在弱偶联和强偶联方向上产生了特征性的两峰吸收光谱。使用散射矩阵技术，我们详细研究了自由状态和约束状态的贡献。我们得出的结论是，高频峰的偏度可以用作识别激子-CT状态耦合强度的新方法。
Charge Transfer (CT) has enjoyed continuous interest due to increasing experimental control over molecular structure leading to applications in, for example, photovoltaics and hydrogen production. In this paper, we investigate the effect of CT states on the absorption spectrum of linear molecular aggregates using a scattering matrix technique that allows us to deal with arbitrarily large systems. The presented theory performs well for both strong and weak mixing of exciton and CT states, bridging the gap between previously employed methods which are applicable in only one of these limits. In experimental spectra the homogeneous linewidth is often too large to resolve all optically allowed transitions individually, resulting in a characteristic two-peak absorption spectrum in both the weak- and strong-coupling regime. Using the scattering matrix technique we examine the contributions of free and bound states in detail. We conclude that the skewness of the high-frequency peak may be used as a new way to identify the exciton-CT-state coupling strength.
