Exciton-trion dynamics of a single molecule in a radio-frequency cavity

Abstract

Charged optical excitations (trions) generated by charge carrier injection are crucial for emerging optoelectronic technologies as they can be produced and manipulated by electric fields. Trions and neutral excitons can be efficiently induced in single molecules by means of tip-enhanced spectromicroscopic techniques. However, little is known of the exciton-trion dynamics at single molecule level as this requires methods permitting simultaneous sub-nanometer and sub-nanosecond characterization. Here, we investigate exciton-trion dynamics by phase fluorometry, combining radio-frequency modulated scanning tunnelling luminescence with time-resolved single photon detection. We generate excitons and trions in single Zinc Phthalocyanine (ZnPc) molecules on NaCl/Ag(111), determine their dynamics and trace the evolution of the system in the picosecond range with atomic resolution. In addition, we explore dependence of effective lifetimes on bias voltage and propose a conversion of neutral excitons into trions via charge capture as the primary mechanism of trion formation.

References in corpus (2)

• Optical Quantum Computing
• Charge carrier injection electroluminescence with CO functionalized tips on single molecular emitters

Cited by in corpus (8)

• Tip-induced excitonic luminescence nanoscopy of an atomically-resolved van der Waals heterostructure
• Internal Stark effect of single-molecule fluorescence
• Many-body description of STM-induced fluorescence of charged molecules
• Real space visualization of entangled excitonic states in charged molecular assemblies
• Single-molecule time-resolved spectroscopy in a tunable STM nanocavity
• Evidence of trion-libron coupling in chirally adsorbed single molecules
• Bipolar single-molecule electroluminescence and electrofluorochromism
• Selectively addressing plasmonic modes and excitonic states in a nanocavity hosting a quantum emitter