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  4. Giant Purcell Broadening and Lamb Shift for DNA-Assembled Near-Infrared Quantum Emitters
 
research article

Giant Purcell Broadening and Lamb Shift for DNA-Assembled Near-Infrared Quantum Emitters

Verlekar, Sachin  
•
Sanz-Paz, Maria
•
Zapata-Herrera, Mario
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2025
ACS Nano

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.

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Type
research article
DOI
10.1021/acsnano.4c09829
Scopus ID

2-s2.0-85214805210

Author(s)
Verlekar, Sachin  

École Polytechnique Fédérale de Lausanne

Sanz-Paz, Maria

University of Fribourg

Zapata-Herrera, Mario

CSIC-UPV/EHU - Centro de Física de Materiales (CFM)

Pilo-Pais, Mauricio

University of Fribourg

Kołątaj, Karol

University of Fribourg

Esteban, Ruben

CSIC-UPV/EHU - Centro de Física de Materiales (CFM)

Aizpurua, Javier

Donostia International Physics Center

Acuna, Guillermo P.

University of Fribourg

Galland, Christophe  

École Polytechnique Fédérale de Lausanne

Date Issued

2025

Published in
ACS Nano
Subjects

DNA origami

•

Lamb shift

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plasmonic nanocavities

•

Purcell effect

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single photon sources

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single-molecule fluorescence spectroscopy

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
LASPE  
Available on Infoscience
January 25, 2025
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/244461
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