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From weak to strong coupling of quantum emitters in metallic nano-slit Bragg cavities. Ronen Rapaport. Acknowledgments. Graduate Students: Nitzan Livneh Moshe Harats Itamar Rosenberg Ilai Schwartz. Collaborations: Adiel Zimran, Uri Banin – Chemistry, Hebrew Univ. - PowerPoint PPT Presentation
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From weak to strong coupling of quantum emitters in metallic nano-slit
Bragg cavitiesRonen Rapaport
The nanophotonics and quantum fluids group
AcknowledgmentsAcknowledgmentsGraduate Students:Nitzan LivnehMoshe HaratsItamar RosenbergIlai Schwartz
Collaborations:Adiel Zimran, Uri Banin – Chemistry, Hebrew Univ.Ayelet Strauss, Shira Yochelis, Yossi Paltiel – Applied Physics Hebrew Univ. Loren Pfeiffer – EE, Princeton UniversityGang Chen – Bell Labs
Support: -EU FP7 Marie Currie-ISF (F.I.R.S.T) -Wolfson Family Charitable Trust-Edmond Safra Foundation
The nanophotonics and quantum fluids group
OutlineOutline• Extraordinary transmission (EOT) in nanoslit arrays
• EOT in nanoslit array exposed – Bragg Cavity Model
• Two level system in a cavity – the weak and strong coupling limits
• 3 Examples of control and manipulations of light-matter coupling:
1. WCL – linear: the Purcell effect and controlled directional emission of quantum dots
2. WCL – nonlinear: enhancement of optical nonlinearities: Two photon absorption induced fluorescence
3. SCL : Strong exciton-Bragg cavity mode coupling: Bragg polaritons
The nanophotonics and quantum fluids group
Resonant Extraordinary Transmission – output light intensity (at resonant wavelengths) larger than the geometrical ratio of open to opaque areas
Iout ()/Iin()>(open area)/(total area)
Extraordinary Transmission (EOT) in Extraordinary Transmission (EOT) in subwavelength metal Hole/slit arrayssubwavelength metal Hole/slit arrays
Channeling of energy through the subwavelength openings!
The nanophotonics and quantum fluids group
EOT in nanoslit arrays: Possible mechanisms EOT in nanoslit arrays: Possible mechanisms
sin2sin kkx
TM
EOT
EOT of more than 5
Full numerical EM simulations: give full account◦No clear physical picture.
EH
TM
The nanophotonics and quantum fluids group
EOT in nanoslit arrays: Possible mechanisms EOT in nanoslit arrays: Possible mechanisms
SPP modes
TM
EH
TM sin2sin kkx
Unit cell near field
Surface Plasmon Polaritons (SPPs)
The nanophotonics and quantum fluids group
EOT in nanoslit arrays: Possible mechanisms EOT in nanoslit arrays: Possible mechanisms
SPP modes
TM
EH
TM sin2sin kkx
• Slit-Cavity resonances
The nanophotonics and quantum fluids group
EOT in nanoslit arrays: Possible mechanisms EOT in nanoslit arrays: Possible mechanisms
SPP modes
TE
• EOT in TE with a thin dielectric layer• No propagating (or standing) modes in subwavelength slits• No SPP in TE polarization•Waveguide modes
E HTE
The nanophotonics and quantum fluids group
Bragg Cavity Model for EOTBragg Cavity Model for EOT
• Fabry-Perot Cavity: high resonant transmission with very highly reflective mirrors
Standing optical modes constructive forward interference High transmission
The nanophotonics and quantum fluids group
Bragg Cavity Model for EOTBragg Cavity Model for EOT
[( ) ] ˆ( )prop
x zi k gm x k zmj
m
H r H e y
• Inside the slit array: periodic Bragg (Bloch) modesfor g > k, there are modes with m ≠ 0
dg 2
• Outside the slit array: For g > k, only the mode with m = 0 is propagating
We can have Standing m ≠ 0 Bragg waves in the structure!
Constructive interference with m=0 mode EOT
I. Schwarz et al., preprint arXiv 1011.3713
The nanophotonics and quantum fluids group
Bragg Cavity Model for EOTBragg Cavity Model for EOT
12 232 2 2 2propzk w l Are phases accumelated
upon collision with the boundaryij
Mapping to FP (waveguide) physics: Analytic condition for standing Bragg modes
2 2( )propz
eff
k gn
k
The nanophotonics and quantum fluids group
Bragg Cavity Model for EOTBragg Cavity Model for EOT
TE TM
Very good agreement with full numerical calculations.
I. Schwarz et al., preprint arXiv 1011.3713
The nanophotonics and quantum fluids group
Bragg CavitiesBragg Cavities
• “one mirror” cavities
• easily integrated with various active/passive media
• small mode volume
• easily controllable Q-factor
The nanophotonics and quantum fluids group
At resonance, the relative strength of the Two Level
System (TLS) - cavity interaction is determined by:
•the photon decay rate of the cavity κ,•the TLS non-resonant decay rate γ,•the TLS–photon coupling parameter g0.
TLS in a cavity – weak and strong coupling TLS in a cavity – weak and strong coupling
The nanophotonics and quantum fluids group
At resonance, the relative strength of the Two level
System (TLS) - cavity interaction is determined by:
•the photon decay rate of the cavity κ,•the TLS non-resonant decay rate γ,•the TLS–photon coupling parameter g0.
Weak coupling: g0<<max(κ,γ)
The emission of the photon by the TLS is an irreversible process.
Resonant enhancement of spontaneous emission rate into cavity modes.
Purcell effect
TLS in a cavity – weak and strong coupling TLS in a cavity – weak and strong coupling
The nanophotonics and quantum fluids group
At resonance, the relative strength of the Two level
System (TLS) - cavity interaction is determined by:
•the photon decay rate of the cavity κ,•the TLS non-resonant decay rate γ,•the TLS–photon coupling parameter g0.
Strong coupling: g0>>max(κ,γ)
The emission of a photon is a reversible process.
Vacuum Rabi splitting
TLS in a cavity – weak and strong coupling TLS in a cavity – weak and strong coupling
The nanophotonics and quantum fluids group
At resonance, the relative strength of the Two level
System (TLS) - cavity interaction is determined by:
•the photon decay rate of the cavity κ,•the TLS non-resonant decay rate γ,•the TLS–photon coupling parameter g0.
Strong coupling for excitons in planar microcavities – exciton-polaritons
See J. Kasprzak, et al., Nature, 443 (2006) 409-414.
“Dynamical” Exciton – polariton BEC in a microcavity
TLS in a cavity – weak and strong coupling TLS in a cavity – weak and strong coupling
The nanophotonics and quantum fluids group
1. Weak coupling of Quantum dots to Bragg1. Weak coupling of Quantum dots to Braggcavity modes – directional emissioncavity modes – directional emissionNanocrystal quantum dots - NQDsNanocrystal quantum dots - NQDsNanometric light source:◦Essentially a TLS◦Tunable emission wavelength◦High quantum efficiency
Possible applications:◦Photodetectors◦Solar cells◦Lasing medium◦Single Photon sources
ShellCore
Type I
ShellCore
Type I
Lumo
Homo
Lumo
Homo
InAs/CdSe type I
The nanophotonics and quantum fluids group N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
samplessamples
Reference sample – quantum dots on a glass substrate
Quantum dots in a polymer layer on the nano-slit array
Quantum dot self-assembled monolayer on the nano-slit array
N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
Angular emission spectrum - ReferenceAngular emission spectrum - Reference
0 10 201
1.1
1.2
1.3
1.4
Emission angle
Wav
elen
gth
[m
]
0
0.5
1TE
No angular dependence – as expected
N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
Angular emission spectrum – Nanoslit arrayAngular emission spectrum – Nanoslit array
0 10 201
1.1
1.2
1.3
1.4
Emission angle
Wav
elen
gth
[m
]
0
0.5
1TE
0 10 201
1.1
1.2
1.3
1.4
Emission angle
Wav
elen
gth
[m
]
0
0.5
1TE
0 10 201
1.1
1.2
1.3
1.4
Emission Angle
Wav
elen
gth
[m
]0
5
10
15TE emission
Strong angular dependence, directional emission (follow EOT disp.)
N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
Directional emission with divergence of 3.4o
20 fold emission enhancement to this angle
Photon emission rate:
The interaction with the structure is in the single quantum-dot (photon?) level
Second order correlation measurements g(2) on the way
0 5 10 150
5
10
15
20
QD emission angleN
orm
. int
ensi
ty [a
.u]
nanoslit array samplereference sample
3.4o
0 10 201
1.1
1.2
1.3
1.4
Emission Angle
Wav
elen
gth
[m
]
0
5
10
15
N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
Physical explanation – Purcell effectPhysical explanation – Purcell effect
Purcell effect: The emission rate of a dipole in a cavity into a cavity mode is enhanced.
Our structure acts as a Bragg cavity with an eigenmode at 0o → stronger emission to 0o
Near field in 0o (structure mode) Near field in 15o
The nanophotonics and quantum fluids group
Physical explanation – Purcell effectPhysical explanation – Purcell effectThe dipole emission rate into a cavity mode is given by
-2 0 2 4 6 8 10 12 140
5
10
15
20
QD emission angle
Nor
m. i
nten
sity
[a.u
]
nanoslit array samplereference samplepurcell factor
3.4o
Experimental values:
Numerical model:
Despite a low Q factor, the nanoslit array significantly enhances the emission to 0o due to a Small modal volume
N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
Angular emission spectrum – QD monolayerAngular emission spectrum – QD monolayer
N. Livneh et al., Nano Letters(2011)
The nanophotonics and quantum fluids group
Towards directional emission of a single Towards directional emission of a single QD - QD -
The nanophotonics and quantum fluids group
2. enhancement of optical nonlinearities: 2. enhancement of optical nonlinearities: Two photon absorption induced fluorescenceTwo photon absorption induced fluorescence
Experimental configuration Excitation and Nanocrystal Quantum Dots Photoluminescence
Two photon upconversion process
M. Harats et al., Optics Express (2011)
The nanophotonics and quantum fluids group
Two photon absorption induced fluorescenceTwo photon absorption induced fluorescence
( )
(2) 2 2UC e hI N I I
- the intensity enhancement factor in the nanoslit array
Using the resonant enhancement of EM fields in the nanoslit array results with
The induced upconversion is:
(2)I I I
Glass substrate
Polymer layer
Al Al Al Al Ald a
H
h
M. Harats et al., Optics Express (2011)
QD absorption:
The nanophotonics and quantum fluids group
TPA and induced upconverted fluorescence in semiconductor NQDs in TE polarization in metallic nanoslit arrays with a maximal enhancement of ~400
Two photon absorption induced fluorescenceTwo photon absorption induced fluorescence
M. Harats et al., Optics Express (2011)
The nanophotonics and quantum fluids group
3. Strong exciton-Bragg cavity mode coupling: 3. Strong exciton-Bragg cavity mode coupling: Bragg exciton-polaritons in GaAs QW’sBragg exciton-polaritons in GaAs QW’s
The signature of strong coupling: vacuum Rabi splitting (avoided crossing)
Second order bragg resonance
The nanophotonics and quantum fluids group
TM
Calculated angular absorption spectrum –Calculated angular absorption spectrum – no excitonsno excitons
The nanophotonics and quantum fluids group
Angular absorption spectrum – with excitonsAngular absorption spectrum – with excitons
Clear vacuum RabiSplitting (~4meV).Clear avoided crossings
TM
The nanophotonics and quantum fluids group
Angular absorption spectrum – TEAngular absorption spectrum – TE
TE
TE
The nanophotonics and quantum fluids group
Thank youThank you
Experimental results - wavelength dependence
Using Dynamical Diffraction(1), near-field intensities are extracted. An averaged unit cell enhancement is calculated by:
(1) M. M. J. Treacy, Phys. Rev. B, 66(19):195105, Nov 2002.
( )unit cell
calcPFCB
unit cell
I r d r
d r
What’s happening in the wavelengths noted by the red circles?
2
Analysis
As we used a pulse with a spectral width ( ), the enhancement per wavelength is taken into account:
( )P
( ) ( )( )
( )calc
avg
P d
P d
This is good agreement between the experimental and theoretical
results