Efficient surface plasmon amplification in gain-assisted silver nanotubes and

associated dimers
HaiQun Yu, ShuMin Jiang, and DaJian Wu
Citation: Journal of Applied Physics 117, 153101 (2015); doi: 10.1063/1.4918310
View online: http://dx.doi.org/10.1063/1.4918310
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JOURNAL OF APPLIED PHYSICS 117, 153101 (2015)

Efficient surface plasmon amplification in gain-assisted silver nanotubes

and associated dimers
HaiQun Yu,1 ShuMin Jiang,1 and DaJian Wu2,a)
1

Faculty of Science, Jiangsu University, Zhenjiang 212013, China

Jiangsu Key Lab on Opto-Electronic Technology, School of Physics and Technology,
Nanjing Normal University, Nanjing 210023, China
2

(Received 14 January 2015; accepted 4 April 2015; published online 16 April 2015)
SPASER (surface plasmon amplification by stimulated emission of radiation) properties in active
SiO2Ag nanotubes and associated dimers have been investigated by using the scattering theory and
the finite element method. In the active Ag nanotube, as the gain coefficient of the core increases to
a critical value, a super-resonance occurs. The SPASER phenomenon also can be found in the active
Ag nanotube dimer. The strong couplings between two nanotubes lead to larger gain threshold for
the active Ag nanotube dimer compared with the active Ag nanotube. At the super-resonance, the
maximal surface enhanced Raman scattering factor at the hot spot in the active Ag nanotube dimer
can achieve about 8  1018, which is large enough for single molecule detection. Furthermore,
with increasing the separation between two Ag nanotubes, the gain threshold value for the superresonance of the active Ag nanotube dimer decreases, while the corresponding super-resonance
C 2015 AIP Publishing LLC.
wavelength increases first and then decreases. V
[http://dx.doi.org/10.1063/1.4918310]

I. INTRODUCTION

The optical properties of metallic nanostructures have

been intensively studied in recent decades and various metal
nanostructures with different shapes have been produced and
investigated.1 It is well known that the surface plasmon (SP)
responses in the metal nanostructures are strongly dependence on the detailed shape parameters.2,3 The specific optical
properties in different metallic nanostructures can lead to
many applications in functional materials,4 surface-enhanced
Raman spectroscopy (SERS),5 biological sensing,6
plasmonic lasers,7 etc. Among many novel plasmonic nanostructures, the metal dimer is a simple but important nanostructure.810 Above all, an enormous SERS response can be
found in metal nanoparticle dimers when the molecules were
trapped at the gap between two particles.11 By adjusting the
geometry parameters of the dimers, the near-field enhancement, resonance wavelength, scattering, and absorption all
will be changed effectively.12 For example, Huck et al.13
found that the near-field couplings in the gold nanoantennas
arranged in tip-to-tip configuration lead to strong near-field
enhancements in the infrared region. Ag nanoshell dimers
have been reported to be a dual-band photoluminescence
enhancer at the dipole and quadrupole modes of the SP
resonances.14 In the plasmonic split nanoring dimer, the coupling and interference of the dimer SP modes can induce the
multiple Fano-like resonances.15 In addition, Marinica
et al.16 found the strong nonlinear effects in a coupled metal
nanoparticle dimer.
Recently, surface plasmon amplification by stimulated
emission of radiation (SPASER) has received extensive
attention because of their potential applications in
a)

Author to whom correspondence should be addressed. Electronic mail:

wudajian@njnu.edu.cn

0021-8979/2015/117(15)/153101/5/$30.00

ultrasensing,17 scanning near-field optical microscopy,18 biomedical tests,19 and SP-enhanced photodetectors.20 The gain
materials near the metal surface couple with the plasmonic
structures and transfer energy to compensate the losses of
the SPs. Finally, it will lead to the enormous amplification of
the desired SP response.2125 In 2009, Noginov et al.26 first
demonstrated experimentally that a nanoparticle with a gold
core and dye-doped silica shell can realize a SPASER-based
nanolaser. Li et al.27 reported an efficient nanorod-based
SPASER with wavelength tunability and polarization sensitivity. A Fano resonance-based SPASER was found in a rod
and concentric square ring-disk nanostructure.28 We also
proposed a dual-frequency SPASER based on the gainassisted metallic nanomatryushkas.29 However, the SPASER
properties in metal nanotubes were seldom reported, especially in their dimers.
In this paper, we present a theoretical investigation for
the SPASER properties of the active Ag nanotubes and associated dimers. As the gain coefficient increases to the critical
values, the super-resonances can be found in the active Ag
nanotubes and the active Ag nanotube dimers. We focus on
the far- and near-field properties of the active Ag nanotube
dimers at the super-resonances. The influences of the dimer
gap on the gain threshold and super-resonance wavelength of
the active Ag nanotube dimer have been discussed in detail.
II. ACTIVE AG NANOTUBE AND ASSOCIATED DIMER

The Ag nanotube comprises a dielectric core with radius

r1 and an Ag shell with radius r2. The schematic of the Ag
nanotube dimer is shown in Fig. 1. The Ag nanotube dimer
is illuminated by an incident electric field with K vector normal to the axis of dimer and electric vector parallel to the
axis of dimer. Throughout the paper, r1 and r2 are set as 40
and 50 nm, respectively. The other values of r1 and r2 of

117, 153101-1

C 2015 AIP Publishing LLC

V

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Yu, Jiang, and Wu

FIG. 1. Schematic diagram of the Ag nanotube dimer.

course can be used for this model. However, the influences

of the structure parameters of the Ag nanotube on the SP
amplifications are not the main part of this work. We focus
on the effects of the couplings between two Ag nanotubes on
the SPASER properties of the active Ag nanotube dimers.
Thus, we only study one kind of Ag nanotube. The dielectric
functions of the core and shell are e1 and e2, respectively.
The separation between two nanotubes is defined as D and C
point is the midpoint in the dimer gap. A Drude model is
adopted for the complex dielectric function of the Ag shell.29
The gain materials such as dye molecules,26 rare-earth ions,
and semiconductor quantumdots21 can be doped into silica
core to realize the active nanotubes and associated dimers.
For simplicity, a complex refractive index of the doped SiO2
core is set as n  ik. The real part n represents the refractive
index of SiO2 (n 1.43) and gain coefficient k is related to
the amount of optical gain induced by external pumping.30
The embedding medium is assumed as air with e3 1. The
incident light interacting with a infinite active Ag nanotube
can be described by the scattering theory.31 The scattering
and absorption spectra of the nanotubes are shown by using
the scattering efficiency Qsca and absorption efficiency Qabs.
For the Ag nanotube dimer, using scattering theory
directly to deal with the near- and far-field properties is

J. Appl. Phys. 117, 153101 (2015)

difficult and complex. Thus, the finite element method (FEM)

is used to study the near and far-field optical properties of the
passive and active Ag nanotube dimers. The FEM has been
proved to be a flexible and efficient numerical tool to analyze
the inhomogeneous and complex structures. The FEM has the
advantage of defining the material interfaces accurately and
can use an unstructured adaptive mesh to improve the high
numerical resolution wherever necessary. Therefore, the
FEM has been widely used in the researches of the optical
properties of the metallic nanostructures.32,33 Our 2D-FEM
model consists of an Ag nanotube dimer, the embedding medium, and a perfectly matched layer (PML). The cylindrical
PML around the Ag nanotube dimer acts as an absorber of
the scattered fields. The plan wave for excitation is defined
through the background field with the polarization parallel to
the axis of the dimer. The scatterer and embedding medium
are meshed with free triangular elements and the PML
domain is meshed with quadrilateral elements by mapping.
III. RESULTS AND DISCUSSION

Firstly, we investigate the optical properties of a single

Ag nanotube. Figure 2 shows the absorption and scattering
spectra of the Ag nanotubes with different gain coefficients.
It is found that the scattering and absorption of the Ag nanotube can be adjusted by changing the gain coefficient of the
core. In Fig. 2(a), as k 0, a strong peak appears at about
632 nm, which is due to the dipole plasmon resonance in the
passive Ag nanotube. The line width of the scattering peak is
about 80 nm and the corresponding quality factor is about 8.
The quality factor Q is evaluated from Q k/Dk, where k
and Dk are the central emission wavelength and the full
width at half maximum, respectively.34 As the gain coefficient k increases to 0.0715, the absorption at the SP
resonance wavelength becomes zero, while the Qsca-value
increases to 8.5, as shown in Fig. 2(b). At this point, the SP
losses in the Ag nanotube are compensated by gain media. In

FIG. 2. Scattering and absorption spectra of the active Ag nanotubes with

gain coefficient k of (a) 0, (b) 0.0715,
(c) 0.1753, and (d) 0.1816.

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Yu, Jiang, and Wu

Fig. 2(c), as k-value increases to the critical point of

kc 0.1753, a super-resonance occurs in the active Ag nanotube at about 620.7 nm. The peak value of Qsca significantly
increases to about 4.04  107, which is about 1.3  107 times
the value for the passive Ag nanotube. Meanwhile, the peak
value of Qabs decreases dramatically to a minimum
4.04  107. The line width of the SP peak reduces to about
0.5 nm and the extinction efficiency Qext Qsca Qabs
reaches zero. It is well known that the SP amplification arises
from the interactions among the gain medium, Ag nanotube,
and incident light. As the gain coefficient reaches the critical
value, the light amplification and dissipation of the system
keep a dynamic balance and the net amplification of the
SPASER becomes zero.23 Then, a stable SPASER is established. Under this condition, the quality factor of the SP
resonance is greatly increased (about 1240) and hence the
strength of the SP resonance is significantly enhanced. With
further increasing the gain coefficient, the strengths of the
scattering and absorption peaks decrease rapidly and the
super-resonance disappears.30 In Fig. 2(d), for k 0.1816,
the peak values of Qsca and Qabs reduce to 2440 and 2574,
respectively, and the line width of the scattering peak
increases to about 3 nm. In this case, the absorbed energy
outnumbers the losses, leading to a negative Qext.
We further investigate the SPASER properties of the
active Ag nanotube dimer. Figure 3(a) shows the scattering
and absorption spectra of the passive Ag nanotube dimer
(k 0). Here, D-value is fixed at 5 nm. A strong peak appears
at about 721.5 nm. The plasmon resonance of the Ag nanotube dimer exhibits an apparent red shift compared with the
Ag nanotube. According to the plasmon hybridization theory,
when the incident polarization is parallel to the dimer axis,
the couplings between the SP resonances in two Ag nanotubes
lead to a bonding mode (low energy) and an antibonding
mode (high energy).35 Thus, the dipole peak of the bonding
mode of the Ag nanotube dimer will show a red shift. In Fig.
3(b), as k-value increases to 0.1386, the Qsca of the dipole

J. Appl. Phys. 117, 153101 (2015)

peak of the bonding mode increases to about 13 while the corresponding Qabs-value tends to zero. When k-value increases
to the critical point of kc 0.5715, a super-resonance occurs
in the active Ag nanotube dimer. At this super-resonance, the
Qsca-value can reach about 6.87  107, which is larger than
that of the active Ag nanotube. The line width of the scattering peak becomes extremely narrow of about 0.1 nm and the
corresponding quality reaches about 6318. We also note that
the gain threshold of the active Ag nanotube dimer is larger
than that of the active Ag nanotube. The gain threshold of the
active plasmonic nanostructures depends on the dissipation in
the metal and the radiation of electromagnetic waves.36 The
plasmonic nanostructure with lower radiation and metallic
losses means a smaller gain threshold. In the Ag nanotube
dimer, the strong coupling between two Ag nanotubes results
in a considerable enhancement of the near-fields. Therefore,
the metallic losses due to the electric field penetration into
metal layer could be high and hence the large threshold value
for the active Ag nanotube dimer.26,37,38 In addition, it is
found that the super-resonance wavelength of the active Ag
nanotube dimer shows a blue shift from 721.5 nm to
631.8 nm. With increasing the gain coefficient k, the real part
of the dielectric constant of the doped silica core [(n  k)2]
decreases. The decreased dielectric constant of the inner core
will increase the number of the induced charges on the internal surface of the Ag nanotube.39 Then, the strength of the
collective oscillation of the induced electrons is enhanced and
hence the increased resonance energies of the SP modes.
Therefore, the resonance energies of both bonding and antibonding modes in the Ag nanotube dimer will be increased
and hence the super-resonance wavelength shows a blue shift.
In addition, for k 0.5715, the energy transferred from gain
media to the bonding mode is more than that to the antibonding mode. Thus, the antibonding mode peak (Qsca  3000) is
much weaker than the bonding mode peak. In Fig. 3(d), the
super-resonance is disrupted when k-value further increases
to 0.5991.

FIG. 3. Scattering and absorption spectra of the active Ag nanotube dimers

with gain coefficient k of (a) 0, (b)
0.1386, (c) 0.5715, and (d) 0.5991.

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Figures 4(a) and 4(b) show the electric field distributions

in the passive and active Ag nanotube dimers, respectively.
Here, D-value is fixed at 5 nm. In Fig. 4(a), the calculation
wavelength is fixed at the resonance wavelength of 721.5 nm
and k 0. In this passive Ag nanotube dimer, the strong field
enhancements occur in the gap between two Ag nanotubes.
When the incident polarization is parallel to the dimer axis,
the dipole resonance modes of the two Ag nanotubes are
aligned and coupled, and hence, the significant field
enhancements generate in the junction between two nanotubes.40 Meanwhile, the electric fields are suppressed elsewhere because of the coupling effect. The maximal
enhancement (18) of the electric field is found at C point in
the junction of the Ag nanotube dimer. In Fig. 4(b), the calculation wavelength is fixed at the super-resonance wavelength of 631.8 nm and the gain coefficient k is set as 0.5715.
It is obviously that the distribution of the electric fields of
the active Ag nanotube dimer at the super-resonance is similar to that in the passive Ag nanotube dimer. The SPASER
will not change the distribution of the electric fields.
However, The maximal electric field enhancement in the
active Ag nanotube dimer can reach about 5.37  104, which
is about 3  103 times that in the passive Ag nanotube dimer.
The enormous electric field enhancements in the active Ag
nanotube dimer also benefit by the energy transferred from
gain media. Figure 5 shows the log plot (base 10) of SERS
enhancement factor (G jE/E0j4) at C point in the active Ag
nanotube dimer versus gain coefficient k. With increasing
the gain coefficient k, the SERS G factor increases at first
and then decreases. At the critical point of kc 0.5715, the
maximal G factor can reach about 8  1018, which is high
enough for the single molecule detection. Nie et al.41 have
demonstrated experimentally that the SERS G factor of
10141015 in the metal nanoparticle aggregates is sufficient
for single-molecule detection. Li et al.30 also reported that
the active cubic gold nanobox can generate an extremely
high SERS G factor on the order of 10161017. They believed
that the single-molecule detection can be readily achieved by
using this cubic gold nanobox. In the active Ag nanotube
dimer, the maximal G factor of about 8  1018 is larger than
those reported in previous reports. Thus, we think that the
active Ag nanotube dimer can be well used for SERS.

FIG. 4. Electric field distributions of (a) the passive Ag nanotube dimer at

the resonance wavelength of 721.5 nm and (b) the active Ag nanotube dimer
at the super-resonance wavelength of 631.8 nm (k 0.5715).

J. Appl. Phys. 117, 153101 (2015)

FIG. 5. Log plot (base 10) of the maximal SERS G factor of the active Ag
nanotube dimer as a function of k-value.

Finally, we investigate the influences of the dimer gap

on the gain threshold and super-resonance wavelength of the
active Ag nanotube dimer. Figure 6(a) shows the dependence
of the gain threshold of the active Ag nanotube dimer on
D-value. It is found with increasing D-value that the gain
threshold value of the active Ag nanotube dimer decreases.
The increased D-value means the reduced coupling between
two Ag nanotubes, which reduces the electric fields in the
gap of the dimer. The reduced localized electric fields indicate the decrease of the metallic loss and hence the decrease
of the gain threshold.38 Figure 6(b) represents the variation
of the corresponding super-resonance wavelength of the
active Ag nanotube dimer with D-values. With increasing
D-value, the super-resonance wavelength of the active Ag
nanotube dimer increases first from 600.7 nm at D 2 nm to
631.8 nm at D 5 nm and then decreases to 624.1 nm at
D 25 nm. The increased D-value decreases the coupling
strength between two Ag nanotubes and hence the bonding
mode in the Ag nanotube dimer shows a blue shift.

FIG. 6. (a) Gain threshold value and (b) super-resonance wavelength of the
active Ag nanotube dimer as a function of the D-value.

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Yu, Jiang, and Wu

Meanwhile, the decrease of the gain threshold leads to the

increased real part of e1-value, which causes a red shift of
the bonding mode in the Ag nanotube dimer. As D < 5 nm,
the influence of the decreased coupling strength between two
Ag nanotubes on the resonance wavelength is weaker than
that from the decreased kc-value. The increase of the superresonance wavelength occurs. On the contrary, as D > 5 nm,
the super-resonance wavelength of the active Ag nanotube
dimer decreases.
IV. CONCLUSIONS

We have investigated the SPASER properties of the

active Ag nanotubes and associated dimers by means of the
scattering theory and the 2D-FEM. As the gain coefficient k
increases to the critical values, the super-resonances can be
found in the active Ag nanotubes and the associated dimers.
The gain threshold value of the active Ag nanotube dimer is
larger than that for the Ag nanotube because of the strong
coupling between two nanotubes. In the active Ag nanotube
dimer, the maximal SERS G factor at the hot spot can
reach about 8  1018, which is sufficient for single molecule
detection. We have further found that, with increasing the
separation between two nanotubes, gain threshold for the
super-resonance in the active Ag nanotube dimer decreases.
Meanwhile, the corresponding super-resonance wavelength
increases first and then decreases, which can be described as
the competition between the decrease of the coupling
strength and the increased electric constant of the core.
ACKNOWLEDGMENTS

This work was supported by the National Natural

Science Foundation of China under Grant No. 11174113,
Qing Lan Project of Jiangsu Province, Senior Talent
Foundation of Nanjing Normal University under Grant No.
2014102XGQ0189, Hundred Talents Program of Nanjing
Normal University, and Postgraduate Scientific Research
and Innovation Project of Jiangsu University under Grant
No. KYXX_0037.
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