journal article·2020-07-28Open access

Mechano-Optical Switching of a Single Molecule with Doublet Emission

Jiří Doležal, Pingo Mutombo, Dana Nachtigallová, Pavel Jelínek, Pablo Merino, Martin Švec

ACS Nano· Volume 14· Issue 7

Abstract

The ability to control the emission from single-molecule quantum emitters is an important step toward their implementation in optoelectronic technology. Phthalocyanine and derived metal complexes on thin insulating layers studied by scanning tunneling microscope-induced luminescence (STML) offer an excellent playground for tuning their excitonic and electronic states by Coulomb interaction and to showcase their high environmental sensitivity. Copper phthalocyanine (CuPc) has an open-shell electronic structure, and its lowest-energy exciton is a doublet, which brings interesting prospects in its application for optospintronic devices. Here, we demonstrate that the excitonic state of a single CuPc molecule can be reproducibly switched by atomic-scale manipulations permitting precise positioning of the molecule on the NaCl ionic crystal lattice. Using a combination of STML, AFM, and ab initio calculations, we show the modulation of electronic and optical bandgaps and the exciton binding energy in CuPc by tens of meV. We explain this effect by spatially dependent Coulomb interaction occurring at the molecule–insulator interface, which tunes the local dielectric environment of the emitter.
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Research context

OpenAlex topics: Molecular Junctions and Nanostructures · Mechanical and Optical Resonators · Quantum and electron transport phenomena

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Institute of Physics, Czech Academy of Sciences, Cukrovarnická 10/112, CZ16200 Praha 6, Czech Republic

Faculty of Mathematics and Physics, Charles University, Ke Karlovu 3, CZ12116 Praha 2, Czech Republic

Department of Petrochemistry and Refining, University of Kinshasa, Kinshasa, Democratic Republic of Congo

Institute of Organic Chemistry and Biochemistry of the Czech Academy of Sciences, Flemingovo náměstí 542/2, CZ16000 Praha, Czech Republic

Regional Centre of Advanced Technologies and Materials, Šlechtitelů 27, CZ78371 Olomouc, Czech Republic

Instituto de Ciencia de Materiales de Madrid, CSIC, Sor Juana Inés de la Cruz 3, E28049 Madrid, Spain

Instituto de Física Fundamental, CSIC, Serrano 121, E28006 Madrid, Spain

Funding

Comunidad de Madrid · Ministerio de Econom?a y Competitividad · Grantov? Agentura Cesk? Republiky · FP7 Ideas: European Research Council · Grantov? Agentura, Univerzita Karlova · Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences

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