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

Abstract

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

References in corpus (11)

• A Single-Atom Quantum Memory
• Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence
• Single ion-qubit exceeding one hour coherence time
• Coherent properties of single rare-earth spin qubits
• Electrically-driven vibronic spectroscopy with sub-molecular resolution
• Single-molecule vacuum Rabi splitting: four-wave mixing and optical switching at the single-photon level
• Time-Domain Measurement of Spontaneous Vibrational Decay of Magnetically Trapped NH
• Coherent coupling of single molecules to on-chip ring resonators
• Realization of two Fourier-limited solid-state single-photon sources
• Engineering long-lived vibrational states for an organic molecule
• Partial cloaking of a gold particle by a single molecule

Cited by in corpus (7)

• Superradiant and subradiant states in lifetime-limited organic molecules through laser-induced tuning
• Small but large: Single organic molecules as hybrid platforms for quantum technologies
• Spectral splitting of a stimulated Raman transition in a single molecule
• Addressing the correlation of Stokes-shifted photons emitted from two quantum emitters
• Accurate Machine Learning Interatomic Potentials for Polyacene Molecular Crystals: Application to Single Molecule Host-Guest Systems
• Organic molecules as single-photon sources
• Nonlinear opto-vibronics in molecular systems