Singlet fission is a promising candidate to increase the efficiency of organic photovoltaic solar cells and the realization of molecular qubits for quantum applications at room temperature. The singlet fission (SF) process involves a two-step process initiated by the absorption of a single photon, creating a singlet excitation that is converted into a singlet-coupled pair of triplet states (TT) on a fast timescale.  A consequence of this predominantly two-electron transition is that SF is computationally and experimentally difficult to analyze which has made it difficult to elucidate key steps including: the role of charge transfer states, orientation effects, and structure of multiexciton delocalization. In this talk, I will discuss our group’s recently developed Tensor Product Selected Configuration Interaction (TPSCI) method which provides us with near-FCI accuracy and direct access to physically relevant quantities (e.g., charge-transfer character and multiexciton delocalization).  I will demonstrate how our method can be used to provide both accurate and qualitatively insightful results on <i>ab initio</i> models that reach beyond the simple dimer picture.

Rigorously coarse-grained electronic structure theory for understanding the excited state spin-processes in singlet fission

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