
Title: Real-space visualization of excitonic states in single molecules
Abstract:
The ability to control the emission from single-molecule quantum emitters is an important step towards their implementation in optoelectronic technology. [1] Even though excitonic states in single molecules 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 I will show combined tip-enhanced spectromicroscopy with scanning tunneling and atomic force microscopies to inspect exciton states of molecular emitters engineered on surfaces. I will introduce electroluminescence from phthalocyanine-derived metal complexes on thin insulating layers. [2] Copper phthalocyanine (CuPc) emission can be reproducibly switched by atomic scale manipulations permitting precise positioning of the molecule on the NaCl ionic crystal lattice. I will show the modulation of electronic and optical bandgaps, and the exciton binding energy in CuPc by tens of meV and explain this effect by spatially-dependent Coulomb interaction occurring at the molecule-insulator interface. [3] Zinc phthalocyanine (ZnPc) shows emission from neutral and charged excitons (trions). I will present the intertwined exciton-trion dynamics combining radio frequency modulated scanning tunnelling luminescence with time-resolved single photon detection. [4] At last, PTCDA forms coupled molecular assemblies with entangled excitonic states. I will present hyperspectral mapping of the eigenstates and the comparison with calculated many-body optical transitions. [5]
These results reveal the possibility of tailoring excitonic properties of organic dye adsorbates for advanced functionalities and establish the methodology to address them individually at the nanoscale.
References
[1] K. Kuhnke et al., Chemical Reviews, 117 5174 (2017).
[2] J. Doležal et al., Nano Letters, 19, 8606 (2019).
[3] J. Doležal et al., ACS Nano, 14, 8931 (2020).
[4] J. Doležal et al. ACS Nano 15, 7694 (2021)
[5] J. Doležal et al. arXiv: 2110.00310v1 (2021)
Biography:
I am currently a Ramon y Cajal Fellow at the Institute for Material Science of Madrid (ICMM-CSIC), where I conduct my research on structural, electronic and optical characterization of low-dimensional carbon-materials. Previously I have been researcher of the ERC Synergy project Nanocosmos at the ICMM-CSIC and Humboldt Research Fellow in the Max Planck Institute for Solid State Research. I performed my PhD in the Center for Astrobiology (Spain) associated to NASA Astrobiology Institute. My investigations lie at the horizon where the fields of surface science, astrophysics and nanophotonics meet, yet I am further interested in any problem where carbon physics and chemistry dominate.