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E-mail : fc.lin25@gmail.com
Abstract
Upon excitation gold nanorods exhibit localized surface plasmon resonance. The resonance wavelength of longitudinal modes scales with aspect ratio of the nanorods. When two rods are aligned headto-head, the longitudinal modes on each rod couple via the near field in the subwavelength gap. Such strong coupling results in two hybrid modes with different modal profiles and separated with an asymmetric energy splitting. Depending on the symmetry and frequency of the excitation, hybrid modes can be selectively excited. Therefore, nanorod dimers may function as nanoantennas with enhanced field in the gap or as high-Q plasmonic cavities depending on the coupling between two rods. Here, we theoretically investigate the coupling of longitudinal plamonic modes in asymmetric nanorod dimers. Gradually tuning the length of one rod and keeping the other, we have observed coupling behavior similar to adiabatic avoided curve crossing. The asymmetry of energy splitting is found to be different for dipole-dipole coupling and dipole-quadrupole coupling. Since the dark quadrupolar modes radiate less efficient than the dipolar modes, the far-field scattering spectrum may exhibit dip in contrast to peak. This makes it possible to engineer the resonance spectrum of nanorod dimers simply by linking rods with desired length. The result is insightful and provides a guideline for plasmonic enhanced spectrum engineering.
D
B A
2R
L2
L1
(b)
200 210 220 230 240 250 260 270 280 290 300
550
B
L2 L1 D = 10 nm D = 30 nm
Frequency (THz)
Frequency (THz)
500
500
450
450
400
400
10
200
220
240
260
280
300
Normalized intensity
Length of L2
(c)
(d)
500
Frequency (THz)
450
bonding
Energy level splitting (c) The color in figure (c) and (d) represent the same things in figure (b). All of which are extinction spectrum in addition to long rod(black dash line). (d) This is the
energy splitting of different gap length. In antibonding mode, we can see small intensity in the gap(black hollow square). On the contrary, there is stronger intensity in bonding mode (orange hollow square)
Single rod
z
y y x L 2R
In x-y plane 2R L x
1st bright mode
J i( material 0 ) E
(c)
2nd
16 14
bright mode
12
(a)
Asymmetrical excitation
Normalized
1.0
10
Normalized intensity
2nd
bright mode
0.8
0.6
k E
0.4
0.2
2
0.0
600
800
1000
1200
0 500 600
Wavelength (nm)
640
700
800
900
50 nm 60 nm 70 nm 80 nm 90 nm 100 nm 110 nm 120 nm 130 nm 140 nm 150 nm 160 nm 170 nm 180 nm 190 nm 200 nm 210 nm 220 nm 230 nm 240 nm 250 nm 260 nm 270 nm 280 nm 290 nm 300 nm
material r 0
n r r , r 1
material n 2 0
30
30
y position (nm)
y position (nm)
Z=0
Antibonding mode
1
-100 -50 0 50 100
-30
-30
-200
-100
100
Wavelength (nm)
L
30
x position (nm)
30 30
x position (nm)
30
(d)
1
y position (nm)
y position (nm)
y position (nm)
y position (nm)
Wavelength (nm)
(b)
symmetrical excitation
Normalized
1.0 0.8
900
800
-30
0.6
700
40
80
-30
-30 0 40 80
100
200
-30
40
80
x position (nm)
30
x position (nm)
x position (nm)
30
x position (nm)
0.4
0.2
600
640 nm
y position (nm)
50
100
150
200
250
300
Wavelength (nm)
Length of L (nm)
-1
0
y position (nm)
Dark mode & bright mode (a) While an asymmetrical excitation The ways of excitation The source of near field spectrum is a Gaussian wave. (a) Dark mode is
excited by asymmetrical illumination. There are three mode can be induced. (Asymmetrical excitation illuminates one side of structure.) (b) Symmetrical excitation must illuminate on the middle of structure or use the forward plane wave. There are only two mode can be induced. on various L of nanorods, we can find more modes with the different L. The red square is which we choose to couple bright mode and dark mode at wavelength of 640 nm. (b) Plot the peaks of 1st bright mode and 1st dark mode peak of various L. The screenshots are electron field distribution from FDTD simulation. We can observe simply that there are stronger field in two place of structure and three place of 1st bright mode and 1st dark
-30
-100
-50
50
100
Bonding mode
-30
-200
-100
100
x position (nm)
x position (nm)
Current density of antibonding and bonding mode The color chart is Jx value(xdirection current density) of x-y plane which get from middle of structure. The arrow chart is Jxy value
( Jxy Jx 2 Jy 2, we also calculate the angle. ) (Note : Current flow is positive charge to negative charge.) In the left side, the current flow of antibonding mode on both sides of the gap are opposite. The right side of the graph can also get the same results.
D B L2 A L1 2R
Frequency (THz)
Frequency (THz)
480
(b)
560
L2 L1 D = 10 nm D = 30 nm
THz
500
400
480
300
n = 1.0 n = 1.1 n = 1.2 n = 1.3 n = 1.4 n = 1.5 n = 1.6 n = 1.7 n = 1.8 n = 1.9 n = 2.0
400
500
Frequency (THz)
Frequency (THz)
300
Surrounding
200
y = a + b*x 0.99267 Intercept Slope Value Standard Error 693.66532 8.37531 -201.1019 5.46345
400
1.0
1.2
1.4
1.6
Index
400
400
200
200
1.0
1.2
1.4
1.6
1.8
2.0
Normalized intensity
When we change the surrounding index, the energy level different between antibonding and bonding is not change a lot. Therefore, we calculate only frequency shift per 1 index of antibonding mode. 201.1(THz)/index
500
50
100
150
Frequency (THz)
THz
Normalized intensity
Length of L2
500
Frequency (THz)
500
400
Equation y = a + b*x Adj. R-Square 0.99776
Surrounding
400
300
antibonding antibonding
Intercept Slope
(c)
500
(d)
Antibonding mode
400
1.0
1.1
1.2
Index
1.3
1.4
300 0 1 2 3 4 5
1.0
1.1
1.2
1.3
1.4
1.5
Normalized intensity
Frequency (THz)
When we change the surrounding index, the energy level different between antibonding and bonding is not also change a lot. Therefore, we calculate only frequency shift per 1 index of antibonding mode. 238.9 (THz)/index
450
Feedgap = 30nm
400
Result
A B
length of B length of A gap = 10 nm gap = 10 nm
Normalized
500
Energy level splitting (c) This is near field spectrum when R = 20 nm, L2 = L1 = 100 nm. Blue line is the background of
coupling. (When two rods far away, just like single rod) The black one and red one are the spectrum of D = 10 nm and 30 nm, respectively. (d) This is the energy splitting of different gap length. The antibonding mode is negative to negative(or positive to positive), so the electron field intensity is smaller in the gap.( black hollow square) On the contrary, the bonding mode is negative to positive, so that the electron field intensity is stronger than antibonding mode.
Bright mode
100 200 300
1. Dark mode is only induced by asymmetrical illumination. 2. The more smaller length of feedgap, the more stronger energy splitting. 3. When the modes of two gold rods at the same energy level, antibonding mode can only be asymmetrical exposure to stimulate 4. When the energy level in two rods are more close, we can observe clearly the phenomenon of avoided crossing behavior.
Frequency (THz)
0
1.8 2.0 1.5
0.0
0.2
0.4
0.6
0.8
1.0
1.2
1.4