Vibronic exciton theory of singlet fission. II. Two-dimensional spectroscopic detection of the correlated triplet pair state

Abstract

Singlet fission, the molecular process through which photons are effectively converted into pairs of lower energy triplet excitons, holds promise as a means of boosting photovoltaic device efficiencies. In the preceding article of this series, we formulated a vibronic theory of singlet fission, inspired by previous experimental and theoretical studies suggesting that vibronic coupling plays an important role in fission dynamics. Here, we extend our model in order to simulate two-dimensional electronic spectra, through which the theory is further validated based on a comparison to recent measurements on pentacene crystals. Moreover, by means of such spectral simulations, we provide new insights into the nature of the correlated triplet pair state, the first product intermediate in the fission process. In particular, we address a disagreement in the literature regarding the identification, energies, and transition dipole moments of its optical transitions towards higher-lying triplet states.

References in corpus (2)

• Morphology Effectively Controls Singlet-Triplet Exciton Relaxation and Charge Transport in Organic Semiconductors
• Vibronic exciton theory of singlet fission. I. Linear absorption and the anatomy of the correlated triplet pair state

Cited by in corpus (8)

• Time-dependent Density Matrix Renormalization Group Quantum Dynamics for Realistic Chemical Systems
• Vibronic exciton theory of singlet fission. I. Linear absorption and the anatomy of the correlated triplet pair state
• Vibronic exciton theory of singlet fission. III. How vibronic coupling and thermodynamics promote rapid triplet generation in pentacene crystals
• Origins of singlet fission in solid pentacene from an ab initio Green's-function approach
• Quantum Beats of a Multiexciton State in Rubrene Single Crystals
• Effect of off-diagonal exciton-phonon coupling on intramolecular singlet fission
• Beating maps of singlet fission: Full-quantum simulation of coherent two-dimensional electronic spectroscopy in organic aggregates
• Vibronic Resonance Along Effective Modes Mediates Selective Energy Transfer in Excitonically Coupled Aggregates