Spectroscopic analysis demonstrates photon bunching to determine intersystem crossing rates in single pentacene molecules, highlighting a powerful probe for condensed matter dynamics.
Key Points
To develop a unified correlation model combining coherent and incoherent electronic transitions, and measure intersystem crossing rates in single trapped molecules.
Formulated a theoretical framework modeling photon antibunching from coherent Rabi oscillations and photon bunching from incoherent level transitions.
Conducted single-molecule fluorescence correlation measurements on pentacene molecules embedded in a low-temperature para-terphenyl crystal matrix.
Demonstrated prominent photon bunching, allowing direct extraction of individual molecular intersystem crossing rates between excited singlet and triplet states.
Observed molecular-level rate variations relative to bulk literature values, which correspond to local molecular distortions caused by crystal lattice defects.