Bright Frenkel excitons in molecular crystals: a survey

We computed the optical properties of a large set of molecular crystals (∼2200 structures) composed of molecules whose lowest excited states are strongly coupled and generate wide excitonic bands. Such bands are classified in terms of their dimensionality (1-, 2-, and 3-dimensional), the position of the optically allowed state in relation with the excitonic density of states, and the presence of Davydov splitting. The survey confirms that one-dimensional aggregates are rare in molecular crystals highlighting the need to go beyond the simple low-dimensional models. Furthermore, this large set of data is used to search for technologically interesting and less common properties. For instance, we considered the largest excitonic bandwidth that is achievable within known molecular crystals and identified materials with strong super-radiant states. Finally, we explored the possibility that strong excitonic coupling can be used to generate emissive states in the near-infrared region in materials formed by molecules with bright visible absorption and we could identify the maximum allowable red shift in this material class. These insights with the associated searchable database provide practical guidelines for designing materials with interesting optical properties.