High-resolution vibronic spectroscopy of a single molecule embedded in a crystal

• DOI: 10.1063/5.0081297
• Publication Date: 2022-02-11T17:35:56Z
• Authors: Johannes Zirkelbach; Masoud Mirzaei; Irena Deperasińska; Boleslaw Kozankie...; Burak Gurlek; Alexey Shkarin; Tobias Utikal; Stephan Götzinger; Vahid Sandoghdar
• Keywords: Vibrational energy relaxation; Vibronic spectroscopy

Vibrational levels of the electronic ground states in dye molecules have not been previously explored at a high resolution solid matrices. We present new spectroscopic measurements on single polycyclic aromatic dibenzoterrylene embedded an organic crystal made para-dichlorobenzene. To do this, we use narrow-band continuous-wave lasers and combine spectroscopy methods based fluorescence excitation stimulated emission depletion to assess individual vibrational linewidths state ∼30 MHz dictated by linewidth excited state. In this fashion, identify several exceptionally narrow vibronic with down values around 2 GHz. Additionally, sample distribution wavenumbers, relaxation rates, Franck-Condon factors, both for handful molecules. discuss various noteworthy experimental findings compare them outcome density functional theory calculations. The highly detailed spectra obtained our work pave way studying nanoscopic local environment approach also provides improved understanding mechanisms state, which may help create long-lived applications quantum technology.