Real space visualization of entangled excitonic states in charged molecular assemblies

Abstract

Entanglement of excitons holds great promise for the future of quantum computing, which would use individual molecular dyes as building blocks of their circuitry. Even though entangled excitonic eigenstates emerging in coupled molecular assemblies can be detected by far-field spectroscopies, access to the individual modes in real space will bring the much needed insight into the photophysics of these fascinating quantum phenomena. Here we combine tip-enhanced spectromicroscopy with atomic force microscopy to inspect delocalized single-exciton states of charged molecular assemblies engineered from individual perylenetetracarboxylic dianhydride molecules. Hyperspectral mapping of the eigenstates and comparison with calculated many-body optical transitions reveals a second low-lying excited state of the anion monomers and its role in the exciton entanglement within the assemblies. We also demonstrate control over the coupling by switching the assembly charge states. Our results reveal the possibility of tailoring excitonic properties of organic dye aggregates for advanced functionalities and establish the methodology to address them individually at the nanoscale.

References in corpus (8)

• Two-Dimensional Material Nanophotonics
• Single organic molecules for photonic quantum technologies
• Electrically-driven vibronic spectroscopy with sub-molecular resolution
• Energy funnelling within multichromophore architectures monitored with subnanometre resolution
• Charge carrier injection electroluminescence with CO functionalized tips on single molecular emitters
• Exciton-trion dynamics of a single molecule in a radio-frequency cavity
• Inter-layer charge transport controlled by exciton-trion coherent coupling
• Directly profiling the dark-state transition density via scanning tunneling microscope

Cited by in corpus (5)

• Topologically localized excitons in single graphene nanoribbons
• Many-body description of STM-induced fluorescence of charged molecules
• Fluorescent single-molecule STM probe
• Evidence of trion-libron coupling in chirally adsorbed single molecules
• Bipolar single-molecule electroluminescence and electrofluorochromism