Evidence of exciton-libron coupling in chirally adsorbed single molecules
Doležal, Jiří (Charles University. Faculty of Mathematics and Physics)
Canola, Sofia (Czech Academy of Sciences. Institute of Physics)
Hapala, Prokop (Czech Academy of Sciences. Institute of Physics)
de Campos Ferreira, Rodrigo Cezar (Czech Academy of Sciences. Institute of Physics)
Merino, Pablo (Institut Català de Nanociència i Nanotecnologia)
Švec, Martin (Czech Academy of Sciences. Institute of Organic Chemistry and Biochemistry)

Fecha:	2022
Resumen:	Interplay between motion of nuclei and excitations has an important role in molecular photophysics of natural and artificial structures. Here we provide a detailed analysis of coupling between quantized librational modes (librons) and charged excited states (trions) on single phthalocyanine dyes adsorbed on a surface. By means of tip-induced electroluminescence performed with a scanning probe microscope, we identify libronic signatures in spectra of chirally adsorbed phthalocyanines and find that these signatures are absent from spectra of symmetrically adsorbed species. We create a model of the libronic coupling based on the Franck-Condon principle to simulate the spectral features. Experimentally measured librational spectra match very well the theoretically calculated librational eigenenergies and peak intensities (Franck-Condon factors). Moreover, the comparison reveals an unexpected depopulation channel for the zero libron of the excited state that can be effectively controlled by tuning the size of the nanocavity. Our results showcase the possibility of characterizing the dynamics of molecules by their low-energy molecular modes using µeV-resolved tip-enhanced spectroscopy. Vibronic coupling in molecules plays an essential role in photophysics. Here, the authors observe optical fingerprints of the coupling between librational states and charged excited states in a single phthalocyanine molecule chirally absorbed on a surface.
Ayudas:	Ministerio de Ciencia e Innovación EUR2021-122006 Ministerio de Ciencia e Innovación PID2021-125309OA-I00 Ministerio de Ciencia e Innovación RYC2020-029800-I
Derechos:	Aquest document està subjecte a una llicència d'ús Creative Commons. Es permet la reproducció total o parcial, la distribució, la comunicació pública de l'obra i la creació d'obres derivades, fins i tot amb finalitats comercials, sempre i quan es reconegui l'autoria de l'obra original.
Lengua:	Anglès
Documento:	Article ; recerca ; Versió publicada
Materia:	Surfaces, interfaces and thin films ; Single photons and quantum effects ; Chemical physics
Publicado en:	Nature communications, Vol. 13 (2022) , art. 6008, ISSN 2041-1723

DOI: 10.1038/s41467-022-33653-7
PMID: 36224183

8 p, 1.3 MB

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Documentos de investigación > Documentos de los grupos de investigación de la UAB > Centros y grupos de investigación (producción científica) > Ciencias > Institut Català de Nanociència i Nanotecnologia (ICN2)
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