Single-molecule strong coupling at room temperature in plasmonic nanocavities
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Supporting information
Accepted version
Author(s)
Type
Journal Article
Abstract
Emitters placed in an optical cavity experience an environment that changes their coupling to
light. In the weak-coupling regime light extraction is enhanced, but more profound effects
emerge in the single-molecule strong-coupling regime where mixed light-matter states
form1,2
. Individual two-level emitters in such cavities become non-linear for single photons,
forming key building blocks for quantum information systems as well as ultra-low power
switches and lasers3–6
. Such cavity quantum electrodynamics has until now been the preserve
of low temperatures and complex fabrication, severely compromising their use5,7,8
. Here, by
scaling the cavity volume below 40 nm3
and using host-guest chemistry to align 1-10
protectively-isolated methylene-blue molecules, we reach the strong-coupling regime at
room temperature and in ambient conditions. Dispersion curves from >50 plasmonic
nanocavities display characteristic anticrossings, with Rabi frequencies of 300 meV for 10
molecules decreasing to 90 meV for single molecules, matching quantitative models.
Statistical analysis of vibrational spectroscopy time-series and dark-field scattering spectra
provide evidence of single-molecule strong coupling. This dressing of molecules with light can
modify photochemistry, opening up the exploration of complex natural processes such as
photosynthesis9
and pathways towards manipulation of chemical bonds10
.
light. In the weak-coupling regime light extraction is enhanced, but more profound effects
emerge in the single-molecule strong-coupling regime where mixed light-matter states
form1,2
. Individual two-level emitters in such cavities become non-linear for single photons,
forming key building blocks for quantum information systems as well as ultra-low power
switches and lasers3–6
. Such cavity quantum electrodynamics has until now been the preserve
of low temperatures and complex fabrication, severely compromising their use5,7,8
. Here, by
scaling the cavity volume below 40 nm3
and using host-guest chemistry to align 1-10
protectively-isolated methylene-blue molecules, we reach the strong-coupling regime at
room temperature and in ambient conditions. Dispersion curves from >50 plasmonic
nanocavities display characteristic anticrossings, with Rabi frequencies of 300 meV for 10
molecules decreasing to 90 meV for single molecules, matching quantitative models.
Statistical analysis of vibrational spectroscopy time-series and dark-field scattering spectra
provide evidence of single-molecule strong coupling. This dressing of molecules with light can
modify photochemistry, opening up the exploration of complex natural processes such as
photosynthesis9
and pathways towards manipulation of chemical bonds10
.
Date Issued
2016-07-07
Date Acceptance
2016-04-01
Citation
Nature, 2016, 535 (7), pp.127-130
ISSN
0028-0836
Publisher
Nature Publishing Group
Start Page
127
End Page
130
Journal / Book Title
Nature
Volume
535
Issue
7
Sponsor
The Royal Society
European Office Of Aerospace Research & Developmen
Engineering & Physical Science Research Council (E
Engineering & Physical Science Research Council (E
Grant Number
IE151097
FA9550-14-1-0181
RG72590
EP/L027151/1
Subjects
Science & Technology
Multidisciplinary Sciences
Science & Technology - Other Topics
LIGHT
ENHANCEMENT
General Science & Technology
Publication Status
Published
Date Publish Online
2016-06-13