Singlet fission spin dynamics from molecular structure: A modular computational pipeline

Area of Science:

• Quantum chemistry and condensed matter physics
• Photophysics and materials science

Background:

• Singlet fission (SF) is crucial for solar energy and quantum information technologies.
• SF relies on spin dynamics influenced by spin-spin exchange interactions.
• Previous models lacked realistic material-specific fluctuations.

Purpose of the Study:

• To develop a computational pipeline for calculating SF spin dynamics.
• To model realistic fluctuations informed by material structure.
• To interpret measured spin dynamics and constrain geometric fluctuations.

Main Methods:

• Modular computational pipeline integrating electronic structure calculations.
• Molecular dynamics simulations to capture nuclear geometry changes.
• Numerical models for simulating spin dynamics.

Main Results:

• The pipeline successfully models SF spin dynamics.
• It links electronic, nuclear, and spin degrees of freedom.
• Results provide constraints on geometric fluctuations consistent with experimental data.

Conclusions:

• The developed pipeline offers a robust approach to studying SF.
• It enables a deeper understanding of the role of material properties in SF.
• This work facilitates the rational design of materials for SF applications.