Giant Purcell Broadening and Lamb Shift for DNA-Assembled Near-Infrared Quantum Emitters
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.
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BibTeX
@article{verlekar2026giant,
title = {{Giant Purcell Broadening and Lamb Shift for DNA-Assembled Near-Infrared Quantum Emitters}},
author = {Sachin Verlekar and Maria Sanz-Paz and Mario Zapata-Herrera and Mauricio Pilo-Pais and Karol Kołątaj and Ruben Esteban and Javier Aizpurua and Guillermo Acuna and Christophe Galland},
journal = {ACS Nano},
year = {2026},
month = oct,
doi = {10.1021/acsnano.4c09829},
eprint = {2407.19513},
archivePrefix = {arXiv},
url = {https://hal.science/hal-05824713v1},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Giant Purcell Broadening and Lamb Shift for DNA-Assembled Near-Infrared Quantum Emitters
AU - Sachin Verlekar
AU - Maria Sanz-Paz
AU - Mario Zapata-Herrera
AU - Mauricio Pilo-Pais
AU - Karol Kołątaj
AU - Ruben Esteban
AU - Javier Aizpurua
AU - Guillermo Acuna
AU - Christophe Galland
PY - 2026
DA - 2026/10/26
JO - ACS Nano
DO - 10.1021/acsnano.4c09829
UR - https://hal.science/hal-05824713v1
AB - 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.
SN - 1936-0851
SN - 1936-086X
ER -