Giant Purcell Broadening and Lamb Shift for DNA-Assembled Near-Infrared Quantum Emitters
Source abstract
Abstract
Controlling the light emitted by individual molecules is instrumental to a number of advanced nanotechnologies ranging from super-resolution bioimaging and molecular sensing to quantum nanophotonics. Molecular emission can be tailored by modifying the local photonic environment, for example, by precisely placing a single molecule inside a plasmonic nanocavity with the help of DNA origami. Here, using this scalable approach, we show that commercial fluorophores may experience giant Purcell factors and Lamb shifts, reaching values on par with those recently reported in scanning tip experiments. Engineering of plasmonic modes enables cavity-mediated fluorescence far detuned from the zero-phonon-line (ZPL)─at detunings that are up to 2 orders of magnitude larger than the fluorescence line width of the bare emitter and reach into the near-infrared. Our results point toward a regime where the emission line width can become dominated by the excited-state lifetime, as required for indistinguishable photon emission, bearing relevance to the development of nanoscale, ultrafast quantum light sources and to the quest toward single-molecule cavity QED. In the future, this approach may also allow the design of efficient quantum emitters at infrared wavelengths, where standard organic sources have a reduced performance.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Plasmonic and Surface Plasmon Research · Advanced biosensing and bioanalysis techniques · Gold and Silver Nanoparticles Synthesis and Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, Switzerland
Department of Physics, University of Fribourg, 1700 Fribourg, Switzerland
Centro de Física de Materiales CFM-MPC, 20018 Donostia-San Sebastián, Spain
Donostia International Physics Center (DIPC), 20018 Donostia-San Sebastián, Spain
Ikerbasque, Basque Foundation for Science, 48013 Bilbao, Spain
Dept. of Electricity and Electronics, University of the Basque Country (UPV/EHU), 48940 Leioa, Spain
Center of Quantum Science and Engineering, Swiss Federal Institute of Technology Lausanne (EPFL), 1015 Lausanne, Switzerland
Funding
National Center of Competence in Research Bio-Inspired Materials, University of Fribourg · Ministerio de Ciencia, Innovaci?n y Universidades · Schweizerischer Nationalfonds zur F?rderung der Wissenschaftlichen Forschung · European Regional Development Fund · Eusko Jaurlaritza · Hezkuntza, Hizkuntza Politika Eta Kultura Saila, Eusko Jaurlaritza · NextGenerationEU · H2020 European Research Council
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