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Giant Rabi splitting in metal/semiconductor
nanohybrids
J. Bellessa, C. Symonds, J.C. Plenet, A. Lemaitre, K. Vinck, D. Felbacq
Laboratoire de Physique de la Matière Condensée et Nanostructure, Lyon, FranceLaboratoire de Photonique et Nanostructures, Marcoussis, FranceGroupement d’Etude des Semiconducteurs, Montpellier, France
• Properties of surface plasmons• Description of surface plasmons• Plasmons in strong coupling
• Hybridisation localised plasmon/exciton• Localised plasmon in nanodisks• Nanodisks with organic semiconductor
• Particularities of the hybrid states• Inhomogeneous broadenings• Geometrical effects
• Conclusion
Outline
Surface plasmon
• Interface metal / dielectric material
• Damping in the metal
Dielectric
Metal
100nm
20nm
2D 0D nanoparticules1D plasmon guide
W. L. Barnes et al., Nature, 418, 306 (2002)
Properties of surface plasmons
Properties of surface plasmons
Delocalised plasmon in strong coupling
D.E. Gomez et al. Nano Lett. 10 274 (2010)
Strong interaction between plasmons and :
• Aggregated dyes
• Laser dyes such as Rhodamine 6G
• Semiconductor nanocrystals arrays : CdSe dots under a thin silver film
Rabi splitting of 112 meV
T.K. Hakala et al. PRL 103 053602 (2009)
J. Bellessa, C. Bonnand, J.C. Plenet, J. Mugnier., PRL 93, 36404 (2004)
Weak coupling : Luminescence enhancement with nanoantennas
Plasmon in strong coupling
J. Dintinger et al. Phys. Rev. B 71, 035424 (2005)
Plasmons in nanoshells
N. T. Fofang et al. Nanoletters 8 10 3481 (2008)
GOLD
Y. Sugawara et al. PRL 97, 266808 (2006)
Metallic nanostructures
Holes and voids in metallic structures
Properties of surface plasmons
Localised plasmons
• Discrete Plasmon resonance
• Distance between the disks 200nm• Low inhomogeneous broadening
300nm
Hybridisation localised plasmon/exciton
100 120 140 1600
2
4
6
8
10
12
14
16
Num
ber
of p
artic
les
Size (nm)
Ag Nanodisks control of the environment and size
Bare plasmon resonances
Transmission of nanodisks
Plasmon resonances
energy : size dependant
linewidth 150meV
No plasmon overlapping
100 120 140 160 180 200 2201.61.71.81.92.02.12.22.32.42.5
Tra
nsm
issi
on
Nanodisk diameter (nm)
143 nm121 nm
111 nm
1.7 1.8 1.9 2.0 2.1 2.2 2.3 2.4 2.5 2.6 2.7 2.80.0
0.2
0.4
0.6
0.8
1.0
(b)
Energy (eV)
Ene
rgy
(eV
)
(a)
50 100
20
40
60
80
100
120
Hybridisation localised plasmon/exciton
Nanodisks with TDBC
Three transmission dips
TDBC absorption
two size dependant dips
Uncoupled regions Bare TDBC
1.7 1.8 1.9 2.0 2.1 2.2 2.3 2.4 2.5 2.60.0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
1.0
Ab
sorp
tion
(a
. u
.)T
ran
smis
sio
n
Energy (eV)
121 nm143 nm
111 nm
1.7 1.8 1.9 2.0 2.1 2.2 2.3 2.4 2.5 2.6
(b)
(a)
Hybridisation localised plasmon/exciton
Nanodisks covered with a TDBC layer
Two levels model
• Formation of localised plasmon/ exciton mixed states
excexc
plpl
iE
ikEH
2/
2/)(
Eplasmon Eexcitonħ
1.8
2.0
2.2
2.4
LMSBare exciton
Nanoparticle diameter (nm)
LMS
(a)
E (
eV)
(b)
Bare plasmon
100 120 140 160 180 20040
60
80
100
120
140
160
180
200
UMS
UMS
Line
wid
th (
meV
)
Hybridisation localised plasmon/exciton
Formation of polaritons• Rabi splitting depends on TDBC thickness
• FDTD simulations• Rabi energy 450meV
20% of the transition energy
100 120 140 160 180 200 220
1.6
1.7
1.8
1.9
2.0
2.1
2.2
2.3
2.4
2.5
En
erg
y (e
V)
Nanodisk diameter (nm)
(b)
Nanodisk diameter (nm)
450meV
1 TDBC layer 2 TDBC layers
100 120 140 160 180 200 220
1.6
1.7
1.8
1.9
2.0
2.1
2.2
2.3
2.4
2.5
En
erg
y (e
V)
Hybridisation localised plasmon/exciton
J. Bellesa et al. Phys. Rev. B 80, 33303 (2009)
Homogeneous and inhomogeneous broadenings
• In microcavities
• In nanoparticles
Particularities of the hybrid states
N
N N
photon Excitons
?N. F. Fofang et al. Nanolett. 2008, 8 (10), 3481
Strong couplingERabi<inhomogène
plasmonsexciton
Distance between disks
Large modification of the bare plasmons
Diffractive effects
Rabi energy roughly unchanged
1500 2000 2500
0.3
0.6
0.9
Energie (meV)
250nm 185nm 235nm 210nm
Particularities of the hybrid states