Vous êtes sur la page 1sur 7

Home Search Collections Journals About Contact us My IOPscience

Enhanced light scattering of the forbidden longitudinal optical phonon mode studied by micro-

Raman spectroscopy on single InN nanowires

This article has been downloaded from IOPscience. Please scroll down to see the full text article.

2010 Nanotechnology 21 315702

(http://iopscience.iop.org/0957-4484/21/31/315702)

View the table of contents for this issue, or go to the journal homepage for more

Download details:
IP Address: 194.57.171.11
The article was downloaded on 14/10/2011 at 12:55

Please note that terms and conditions apply.


IOP PUBLISHING NANOTECHNOLOGY
Nanotechnology 21 (2010) 315702 (6pp) doi:10.1088/0957-4484/21/31/315702

Enhanced light scattering of the forbidden


longitudinal optical phonon mode studied
by micro-Raman spectroscopy on single
InN nanowires
E O Schafer-Nolte1,2, T Stoica1,3 , T Gotschke1 , F A Limbach1 ,
E Sutter2, P Sutter2, D Grutzmacher1 and R Calarco1
1
Institute of Bio- and Nanosystems (IBN-1) and JARA-FIT Julich-Aachen Research Alliance,
Forschungszentrum Julich, D-52425 Julich, Germany
2
Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973,
USA

E-mail: t.stoica@fz-juelich.de

Received 24 March 2010, in final form 28 May 2010


Published 15 July 2010
Online at stacks.iop.org/Nano/21/315702

Abstract
In the literature, there are controversies on the interpretation of the appearance in InN Raman
spectra of a strong scattering peak in the energy region of the unscreened longitudinal optical
(LO) phonons, although a shift caused by the phononplasmon interaction is expected for the
high conductance observed in this material. Most measurements on light scattering are
performed on ensembles of InN nanowires (NWs). However, it is important to investigate the
behavior of individual nanowires and here we report on micro-Raman measurements on single
nanowires. When changing the polarization direction of the incident light from parallel to
perpendicular to the wire, the expected reduction of the Raman scattering was observed for
transversal optical (TO) and E2 phonon scattering modes, while a strong symmetry-forbidden
LO mode was observed independently on the laser polarization direction. Single Mg- and
Si-doped crystalline InN nanowires were also investigated. Magnesium doping results in a
sharpening of the Raman peaks, while silicon doping leads to an asymmetric broadening of the
LO peak. The results can be explained based on the influence of the high electron concentration
with a strong contribution of the surface accumulation layer and the associated internal electric
field.
(Some figures in this article are in colour only in the electronic version)

1. Introduction can be covered, which makes the material ideally applicable in


solar cells [46] and solid state lighting [7, 8]. Furthermore,
InN is a very intriguing material due to its physical properties the small electron effective mass, the large mobility and the
as well as the variety of promising applications. Its high peak and saturation velocity are promising for high
direct bandgap of 0.64 eV makes it an ideal candidate for speed device applications [9, 10]. The unusual band bending
optoelectronic applications in the near-infrared region [1]. and the electron accumulation at the surface of InN can be
InN-based quantum well structures are reported to emit at the exploited for chemical sensing and field effect devices [11, 12].
technologically important wavelength of 1.55 m suitable for However, a major drawback of III-nitrides is the difficult
fiber optics communication [2]. Also terahertz emission by fabrication of high quality crystalline films due to lattice
InN has been demonstrated [3]. By appropriate alloying with mismatch with heterosubstrates. In this respect, nanowires
GaN an extended energy range including the visible spectrum (NWs) represent a preferred alternative to thin films, due to
their single nanocrystal morphology and enhanced ability for
3 Author to whom any correspondence should be addressed.
lateral elastic relaxation.

0957-4484/10/315702+06$30.00 1 2010 IOP Publishing Ltd Printed in the UK & the USA
Nanotechnology 21 (2010) 315702 E O Schafer-Nolte et al

Raman spectroscopy, widely used in the study of not of the symmetry-allowed A1 (LO) in those experiments
semiconductors, yields information about lattice properties was explained by strong scattering of the excitation light
such as crystal structure and quality, as well as electronic inside the NW ensemble of the as-grown samples. In
properties like carrier concentration and mobility. It has the contrast, in their study on InN films Cusco et al attributed the
advantages of being non-destructive and contactless and does unscreened LO peak to surface-field-induced scattering in the
not require any special sample preparation. The first-order accumulation layer [17]. To summarize, different mechanisms
phonon Raman scattering for InN follows the selection rules and models have been proposed for the interpretation of the
corresponding to its wurtzite structure [13]. For back scattering LO and PLP peaks. Raman spectroscopy of single NWs
geometry, if the excitation laser light propagates along the c in a controlled scattering geometry, avoiding multiple light
axis, the allowed scattering modes are the non-polar mode E2 scattering in NW ensembles and fluctuations from wire to wire
and the longitudinal phonon A1 (LO), while for the incident as well as along a wire, can contribute to resolve controversies
light perpendicular to the c axis, only the E2 and the transversal in the interpretation of Raman scattering in InN. Raman
optical phonons A1 (TO) and E1 (TO) are allowed. The LO measurements on individual NWs may also offer information
mode can be in polar semiconductors strongly coupled to the about the light interaction with the electronic and phononic
plasmonic system of the free carriers, resulting in a low-energy systems in single InN nanowire devices.
branch PLP (at energy smaller than the TO) and a high- In this paper we present Raman measurements on undoped
energy branch PLP+ (at energy higher than the LO mode). and Mg-doped, as well as Si-doped single nanowires. Taking
The Raman shift of these coupled modes increases with the advantage of the well-defined scattering geometry and the
plasma frequency and can be used to determine the density high spatial resolution, the presented data provide relevant
and mobility of the free carriers. Raman studies on InN information about both the light scattering mechanism and
nanowires reported so far showed a simultaneous occurrence the physical properties of InN nanowires. To the best of our
of a strong peak in the region of the expected uncoupled knowledge, this is a first report on single InN nanowire Raman
longitudinal optical A1 (LO) and E1 (LO) modes and of the measurements.
broad low-energy branch of the LO phononplasmon coupled
mode (PLP ) close to A1 (TO) [14, 15]. 2. Experimental details
The detailed analysis of the PLP lineshape in InN and
the spatial location of the electrons are still controversial. InN nanowires are grown catalyst-free by plasma-assisted
Some papers attribute the scattering mechanism, from molecular beam epitaxy under N-rich conditions on Si(111)
which originates the Raman peak close to A1 (TO), not substrates, as already reported by various groups [1923].
to the low branch phononplasmon coupled mode PLP , Details of the growth mechanism as well as the structural,
but to an impurity-induced one or due to charge-density morphological, optical and electrical properties of undoped
fluctuations [16]. Cusco et al have clearly found for high nanowires have been discussed elsewhere [19, 2429]. The
mobility InN films with electron concentrations in the range obtained nanowires have a diameter between 80 and 120 nm
of 2 1018 2 1019 cm3 that PLP scattering arises from and a length of up to 2 m. Nominal p- and n-type
coupling to the bulk-electron plasmons and can be explained doping is achieved by supplying Mg and Si during growth,
by the standard dielectric model based on dipole-allowed respectively. The dopant fluxes in this paper are given in beam
deformation potential and electro-optic mechanism [17]. In equivalent pressure (BEP). To investigate single nanowires,
contrast, for InN NWs, the PLP peak was attributed not to the they were removed from the growth substrate and spread on
wire bulk but to the spontaneous accumulation of electrons on a graphite substrate (highly ordered pyrolytic graphite) by a
the lateral surfaces of the NWs [14]. The high-energy branch dry transfer method. Raman scattering measurements have
of the LO phononplasmon coupled PLP+ mode has not been been carried out using a WITec alpha 300 microscopy system.
detected in InN NWs nor in compact layers. The absence of a For measurements on nanowire ensembles a 20 (NA 0.4)
clear PLP+ scattering in Raman spectra in spite of a detected microscope objective was used to focus the laser beam and
PLP was explained by a rapid broadening of PLP+ due to to collect the scattered light. Laser radiation with 532 and
high carrier density and the associated fluctuations [17]. It 633 nm wavelength with a power of about 5 mW was employed
is worth noting that at high electron concentrations the PLP as an excitation source. The scattered light was analyzed in
behaves more phonon-like, while the PLP+ has a dominant a 1800 mm1 grating spectrometer with a spectral resolution
plasmon character and therefore is more sensitive to the carrier of about 1 cm1 . Single scan was used for acquisition of
distribution. Another explanation given in the literature for Raman spectra of NW ensembles, with an integration time of 1
the absence of the PLP+ is based on the unscreening, and and 2 h for 532 and 633 nm laser wavelengths, respectively.
consequently de-coupling, of the polar LO phonons in the For Raman studies on single nanowires a 100 (NA 0.9)
case of highly damped plasmons, while an LO-phonon-like microscope objective was used to focus the 532 nm laser
structure occurs as an interaction of the polar phonons with beam to a spot size of about 300 nm. To avoid strong laser
electronhole pairs [18]. But the origin of the unscreened heating, the laser power was reduced to 0.5 mW. The scattered
LO peak in InN is controversial as well. For InN ensemble light was analyzed using a 600 mm1 spectrometer grating
nanowires, the LO peak was attributed to E1 (LO) scattering with a spectral resolution of about 3 cm1 . The sample was
in the NW core with low carrier concentration [14, 15]. The scanned relative to the laser beam by a piezoelectrical stage
observation of the symmetry-forbidden E1 (LO) mode and to obtain spatially resolved intensity maps. Since the Raman

2
Nanotechnology 21 (2010) 315702 E O Schafer-Nolte et al

signal of a single InN nanowire is very weak, the wire was A1(TO) E1(TO) E2H A1(LO) E1(LO)
imaged by mapping the intensity of the elastically scattered
light (Rayleigh peak at 0 cm1 ). It was observed that this 2.5
*
intensity is strongly enhanced when the wire is in the laser
focus. Therefore a good contrast between the nanowire and 2.0
the graphite substrate could be achieved in a relative short

Intensity (a.u.)
acquisition time (about 15 min for a complete map). After 1.5
localizing the nanowire, the laser spot was positioned on the 200"nm
200 nm
wire and a single spectrum with an integration time of 1 h was
1.0 633 nm
recorded.

0.5
3. Results and discussion 532 nm
0.0
Raman spectra of undoped InN nanowire ensembles are shown
400 450 500 550 600 650
in figure 1. The samples are measured as-grown, i.e. with Raman shift (1/cm)
nanowires still attached to the silicon substrate on which they
were grown. Therefore a strong Raman peak from the silicon Figure 1. Raman spectra of undoped InN nanowire ensembles
substrate can be seen at 520 cm1 . Since the nanowires are for 532 and 633 nm excitation wavelengths. The spectra are
normalized to the EH2 peak intensity and shifted for clarity. Black
oriented nearly parallel to the incident laser beam, the nominal dotted lines show Raman mode frequencies reported in the
scattering configuration is z(, )z . Selection rules predict literature [13]. The asterisk marks the Raman signal of the silicon
only the occurrence of EH 2 and A1 (LO) for this geometry. E2
H
substrate. Inset is an SEM image of the as-grown NW sample.
1
is clearly pronounced at 487 cm with an FWHM of about
8 cm1 , while the assignment of the strong peak close to
the position of the LO modes is questionable, as discussed and light trapping in NW ensembles, and thus more intense
above. For 532 nm excitation wavelength, the peak occurs heating, can be expected, even though the same incident
close to the reported A1 (LO) frequency at 586 cm1 , for power of the laser beam was used. However, changing the
633 nm wavelength it is shifted closer to the frequency of laser power within the measurement range used, no significant
E1 (LO) at 593 cm1 . The nanowire morphology, which allows change of the peak position was observed. A similar redshift
that most of the light enters through and scatters from the with photon energy was reported for InN films in [30] and
lateral side of the nanowire, could explain the observation of explained by the difference of the light penetration depth at
the symmetry-forbidden E1 (LO) [14, 15], as well as the weak different wavelengths in the presence of an accumulation layer
occurrence of E1 (TO) (476 cm1 ). However, the peculiarity with a very non-uniform distribution of the free carriers. To
of the LO mode in InN NWs, i.e. its symmetry-forbidden fully understand these phenomena related to the wavelength
occurrence with high intensity, is clearly shown by single NW approaching a resonance condition in InN nanowires, further
measurements, as we discuss in the following. The intensity theoretical and experimental efforts would be necessary.
of the LO mode is strongly depending on the laser wavelength: The origin of the broad feature at 440 cm1 in the spectra
by changing the excitation wavelength from 532 to 633 nm, of figure 1 might be due to the PLP mode. On the other hand,
the intensity of LO relative to EH 2 is roughly tripled. This an assignment to the symmetry-forbidden A1 (TO) seems to be
result is in agreement with the one reported by Kuball et al reasonable due to the unusual light propagation in the nanowire
for InN thin films [30]. A similar increase of the LO intensity sample. The second-order spectrum of silicon also has a peak
for longer excitation wavelength was also observed in Si-and in this spectral range [32], which complicates the evaluation
Mg-doped nanowire ensembles studied in this work. Such of this mode. We can conclude that the Raman spectra of
a strong increase is hardly explicable by distinct penetration our as-grown samples are consistent with those reported in the
depths. Moreover, the internal scattering of the excitation literature for InN NWs.
light should be stronger for shorter wavelength and increases Typical results for undoped single nanowires are shown in
the contribution of E1 (LO) to the LO peak [15]. This is figure 2. Raman spectra and the related Rayleigh peak intensity
in contradiction to the experimental data in figure 1. The maps are presented for two wires with different orientations
most probable explanation is therefore a resonance effect at relative to the laser polarization direction. The polarization
a critical point of the electronic structure which enhances of the incident light is depicted by the arrow in the bottom
scattering of polar modes by the Frohlich mechanism, as was left corner of the map. The scattering geometry in these
suggested in [30] and observed in other materials such as, experiments can be described by a combination of x(y, )x
for example, in GaAs [31]. By decreasing the excitation and x(z, )x , while the contribution of the particular scattering
wavelength, a redshift of the Raman peaks can also be seen in processes depends on the orientation of the nanowire. The
figure 1. This was constantly observed for undoped and doped spectra in figure 2 are measured in different parts of the same
samples. Moreover, the energetic distance between EH 2 and LO wire. The labels A and B in the maps denote the particular
peaks is increased for longer excitation wavelengths. A local origin of the spectra. The relative intensity of these peaks
heating induced by laser beam could explain a redshift of the varies from spectrum to spectrum and in some cases its position
Raman peaks. For shorter wavelengths, stronger absorption does not correspond very well with the literature values. The

3
Nanotechnology 21 (2010) 315702 E O Schafer-Nolte et al

A1(TO) E1(TO) E2H A1(LO) E1(LO) expressed in the spectra of wire 2. The reduction of the EH 2
scattering in wires with parallel orientation to the polarization
of the excitation light is a proof that the wires vertical axis is
wire 1
1500
parallel to the crystallographic c direction, as also shown by
HRTEM analysis [24]. The A1 (TO) mode exhibits a contrary
A
A trend, i.e. it is strongly pronounced in the spectra of wire 2 and
has a rather low intensity for wire 1.
1000
B
B The NW shape influences the light penetration into
the wire. If the NW diameter is much smaller than the
laser wavelength, the electromagnetic field inside the wire,
500
B and consequently the expected Raman scattering modes, are
Intensity (a.u.)

strongly reduced for polarization perpendicular to the wire. For


A example, in undoped GaN thin NWs, the Raman scattering is
0
practically suppressed for perpendicular polarization [34]. In
wire 2
contrast, in Raman spectra of InN NWs, the crystal orientation
3000 selection rules dominate over the NW shape effect, as shown
B
B for TO and EH
A
A 2 phonon modes in figure 2. This result can
be related to the high electron concentration with a surface
2000 accumulation layer present in InN NWs, which influences
Raman scattering by changing the phenomena of the light
penetration into the wire, as well as the scattering process itself.
1000 B
The peculiarity of the Raman scattering in InN NWs
A
is also reflected in the LO phonon scattering modes. All
single NW spectra show a very intense LO peak close to
0
the E1 (LO) mode independent of the nanowire orientation,
300 350 400 450 500 550 600 650
although both E1 (LO) and A1 (LO) are forbidden in x(, )x
Raman shift (1/cm)
geometry. This result implies that the interpretation given
Figure 2. Raman spectra of undoped InN single nanowires for the in [14, 15] that the LO peak arises from the E1 (LO) mode
laser polarization quasi-perpendicular (wire 1) and parallel (wire 2) excited by light incident on lateral NW sides is questionable.
to the wire direction. Black dotted lines show Raman mode The intense excitation of the LO mode cannot be explained
frequencies reported in the literature [13]. The insets show the
related Rayleigh peak intensity maps. The scale bar is 500 nm,
only by deviations from the ideal scattering geometry in
arrows denote the polarization direction of the incident laser light. A the experimental set-up. The possible explanations of the
and B mark the locations where the related spectra were acquired. occurrence of the intense LO forbidden mode are discussed
The spectra are shifted on the vertical axis for clarity. at the end of the section based on published models and
simulations [16, 17].
fluctuation of the Raman spectra can be related to fluctuations The interaction between phonons and the electronic
of NW sizes, doping and local strain, as well as to fluctuations subsystem of the sample can be influenced by varying the
of the local thermal contact to the graphite substrate. The free carrier concentration. To this end, different samples with
length and diameter fluctuations of the investigated single NWs Mg and Si as dopants have been investigated. To study the
reflect the size fluctuation of the as-grown NWs, but also, effect of Mg doping, two nominally p-type doped samples are
during the preparation of single NW samples, breaking of grown with Mg fluxes of 1 109 mbar and 3 109 mbar,
NWs and additional internal strain fluctuations might occur. respectively.
Additionally, the relative low spectral resolution of about Two representative Raman spectra obtained on single
3 cm1 used for the acquisition of single NW spectra can nanowires of Mg-doped samples are presented in figure 3.
also affect the accuracy of the measurements. However, some As already observed for the undoped wires, the spectra are
interesting trends can be clearly seen and are discussed below. dominated by the forbidden LO mode. Both nanowires
The Raman spectra of wire 1, which is oriented nearly are oriented nearly parallel to the laser polarization and
perpendicular to the laser polarization direction, should reveal therefore show a strong A1 (TO), while E1 (TO) and EH 2 are
a major contribution of x(y, )x scattering processes, while less pronounced. No significant change correlated with the
for wire 2 a significant component of the electric field increase of the Mg fluxes can be found. However, compared
is oriented parallel to the wire axis and therefore should to the undoped nanowires, the spectra of the Mg-doped
cause predominantly scattering in the x(z, )x configuration. nanowires exhibit sharper peaks with smaller FWHMs. This
Selection rules for wurtzite crystals predict the occurrence could indicate that the crystal quality of the InN nanowires is
of A1 (TO), EH 2 and E1 (TO) phonon modes for x(y, ) x enhanced by the presence of magnesium during growth and
processes, while in x(z, )x geometry only A1 (TO) and the background doping which produces additional disorder is
E1 (TO) are allowed [13]. compensated.
Indeed, in agreement with the selection rules, wire 1 A small Raman peak can be observed close to 400 cm1 ,
shows a pronounced EH 2 phonon mode, while it is only weakly in some Raman spectra of single NWs. This is more frequently

4
Nanotechnology 21 (2010) 315702 E O Schafer-Nolte et al

A1(TO) E1(TO) E2H A1(LO) E1(LO) A1(TO) E1(TO) E2H A1(LO) E1(LO)

-9 -9
Mg BEP =3 10 mbar Si BEP=5 .8 10 mbar
1500
500
1000
Intensity (a.u.)

500

Intensity (a.u.)
0 0
-9 -9
1500 Mg BEP =1 10 mbar Si BEP=1 10 mbar

1000
500

500

0 0
350 400 450 500 550 600 650 350 400 450 500 550 600 650
Raman shift (1/cm) Raman shift (1/cm)

Figure 3. Raman spectra of Mg-doped InN nanowires with different Figure 4. Raman spectra of Si-doped InN nanowires with different
doping levels, acquired from the center of the wire. Black dotted doping levels, acquired from the center of the wire. Black dotted
lines show Raman mode frequencies reported in the literature [13]. lines show Raman mode frequencies reported in the literature [13].
The insets show the related Rayleigh peak intensity maps. The scale The insets show the related Rayleigh peak intensity maps. The scale
bar is 500 nm, arrows denote the polarization direction of the bar is 500 nm, arrows denote the polarization direction of the
incident laser light. incident laser light.

highly doped wires reveal a fine structure of the asymmetric


observed for Mg-doped NWs than for undoped ones, and is
LO band in the range of 480580 cm1 , which consists of
systematically detected at higher energy in Raman spectra
nearly equidistant peaks with a periodicity of about 20 cm1
of NW ensembles (figure 1). If this peak is not related to 2.5 meV. The origin of this fine structure is currently unknown
specific defects in InN, a possible assignment is the low-energy to us. It might be, for example, related to electron transitions
branch PLP of the LO phononplasmon coupled mode. The on localized states.
energy position of this peak is slightly decreased by Mg doping As can be seen in the presented results, Raman spectra
and increased by low Si doping (results not shown here), of single NWs show in many respects similar features as
supporting its PLP assignment. An electron concentration InN nanowire ensembles. The investigation of single wires
value of 46 1018 cm3 can be evaluated from the PLP shows fluctuations between wires from the same sample. We
peak position of about 400 cm1 (see, for example, [13] and a observed variations in the LO lineshape for wires from the
more complex fit in [17]). lightly Si-doped sample, indicating fluctuations in the carrier
The effect of silicon doping on the Raman spectra of InN concentration from wire to wire. Additionally the speculation
NWs can be seen in figure 4. Two n-type doped samples grown about the propagation direction of the excitation light in the
with Si fluxes of 1 109 and 5.8 109 mbar are studied. as-grown nanowire sample due to scattering on different wires
The spectra of highly Si-doped NWs show sharp peaks at EH 2 for explaining the LO peak [14, 15] can be circumvented by
and A1 (TO) frequencies. single undoped NW investigations. As shown in this paper, a
The sharpness of the EH 2 peak proves a high crystal strong LO scattering mode was observed in single NW spectra,
quality in spite of high doping. The most interesting feature independent of the relative direction of the incident light
of the spectra in figure 4 is the LO phonon mode, which polarization, although these modes are symmetry-forbidden.
exhibits a strong low-energy tail. Its intensity clearly increases The observed reduction of the Raman scattering of
with Si doping. A similar asymmetric lineshape has been A1 (TO) and EH 2 modes for polarization of the incident light
observed in InN thin films with carrier concentrations n > perpendicular to the InN wire is a common result of the light
1020 cm3 [18, 33]. Thakur et al explained this feature interaction with nanowires. However, the Raman phonon
by the activation of the silent BH 1 mode due to disorder, scattering remains of significant intensity for all polarization
which practically covers in highly doped InN the scattering directions. This is in contrast with results on GaN NWs, for
of LO phonons in interaction with electronhole pairs [18]. which we have found that Raman phonon scattering is almost
Demangeot et al calculated theoretical LO lineshapes for suppressed for perpendicular polarization [34]. As shown in
different light scattering processes and found a similar the literature for InN films [16, 17] a more complex explanation
asymmetric broadening for LO scattering by the forbidden in which the selection rules are disregarded is necessary.
Frohlich mechanism in combination with wavevector non- The multiple possible light scattering processes induced by
conservation [16]. Additionally, the Raman spectra of the the high electron concentration with a strong contribution

5
Nanotechnology 21 (2010) 315702 E O Schafer-Nolte et al

of the accumulation layer at the wire surfaces can influence [3] Wilke I, Ascabazubi R and Schaff H L W 2008 Appl. Phys.
the Raman spectra via electronphonon interaction and by Lett. 93 221113
changing the light propagation path inside NWs. In [16] it is [4] Wu J, Walukiewicz W, Yu K, Shan W J A III, Haller E,
Lu H and Schaff W 2003 J. Appl. Phys. 94 6477
shown by modeling that, for high electron concentration and [5] Hamazaouni H, Bouazzi A and Rezig B 2005 Sol. Energy
strong Landau damping, the scattering on density fluctuations Mater. Sol. Cells 87 595
can dominate in the visible spectrum over Frohlich and [6] Hsu L and Walukiewicz W 2008 J. Appl. Phys. 104 024507
other mechanisms. A strong electric field in the surface [7] Xu T, Nikiforov A, France R, Williams C T A and
accumulation layer can also induce an enhancement, especially Moustakas T 2007 Phys. Stat. Sol. a 204 2098
[8] Soh C, Liu W, Teng J, Chow S, Ang S and Chua S 2008 Appl.
of the forbidden modes, as suggested in [17]. Indeed, the Phys. Lett. 92 261909
observation of a strong symmetry-forbidden LO scattering in [9] Bhuiyan A, Hashimoto A and Yamamoto A 2003 J. Appl. Phys.
our single NW Raman experiments might deliver additional 94 5
evidence of the formation of a surface accumulation layer [10] Kong Y, Zheng Y, Zhou C, Deng Y, Shen B, Gu S, Zhang R,
Han P, Jiang R and Shi Y 2005 Solid State Electron.
on non-polar surfaces of InN NWs, already suggested by
49 199
photoluminescence and electric transport experiments [24, 25]. [11] Lu H, Schaff W and Eastman L 2004 J. Appl. Phys. 96 3577
[12] Lu Y-S, Ho C-L, Yeh J, Lin H and Gwo S 2008 Appl. Phys.
4. Conclusions Lett. 92 212102
[13] Harima H 2002 J. Phys.: Condens. Matter 14 R967
[14] Lazc S, Gallardo E, Calleja J, Agullo-Rueda F, Grandal J,
In conclusion, Raman studies on single InN nanowires showed Sanchez-Garcia M, Calleja E, Luna E and Trampert A 2007
a strong polarization dependence of A1 (TO) and EH 2 phonon Phys. Rev. B 76 205319
modes in agreement with selection rules. Moreover, the [15] Segura-Ruiz J, Garro N, Cantarero A, Denker C,
occurrence of an intense symmetry-forbidden LO mode was Malindretos J and Rizzi A 2009 Phys. Rev. B 79 115305
[16] Demangeot F, Pinquier C, Frandon J, Gaio M, Briot O,
observed for single wires. A similar LO mode was also
Maleyre B, Ruffenbach S and Gil B 2005 Phys. Rev. B
found in the Raman spectra of as-grown nanowire ensembles. 71 104305
The observed strong excitation wavelength dependence of this [17] Cusco R, Ibanez J, Alarcon-Llado E, Artus L, Yamaguchi T and
mode is pointing to a resonance with electronic transitions, Nanishi Y 2009 Phys. Rev. B 79 155210
as suggested in the literature. The intensity enhancement at [18] Thakur J, Haddad D, Naik V, Naik R, Auner G, Lu H and
Schaff W 2005 Phys. Rev. B 71 115203
longer excitation wavelength, as well as the deviation from
[19] Stoica T, Meijers R, Calarco R, Richter T and Luth H 2006
the expected symmetry found in single NW Raman spectra, J. Cryst. Growth 290 241
indicates that the observed LO peak needs a more complex [20] Shen C-H, Chen H-Y, Lin H-W, Gwo S, Klochikhin A and
explanation in which the phonon interaction with the electronic Davydov V Y 2006 Appl. Phys. Lett. 88 253104
system including the surface accumulation layer is involved [21] Grandal J, Sanchez-Garca M, Calleja E, Luna E and
Trampert A 2007 Appl. Phys. Lett. 91 021902
and the symmetry selection rules are disregarded. The effect [22] Denker C, Malindretos J, Werner F, Limbach F, Schuhmann H,
of magnesium doping is a sharpening of the Raman peaks, Niermann T, Seibt M and Rizzi A 2008 Phys. Status Solidi c
which indicates a good crystalline quality and reduction of the 5 1706
background doping, while for silicon doping the LO phonon [23] Nishikawa S, Nakao Y, Naoi H, Araki T, Na H and
develops an asymmetric lineshape with a pronounced low- Nanishi Y 2007 J. Cryst. Growth 301 490
[24] Stoica T, Meijers R, Calarco R, Richter T, Sutter E and
energy tail. Luth H 2006 Nano Lett. 6 1541
[25] Richter T, Luth H, Schapers T, Meijers R, Jeganathan K,
Acknowledgments Estevez Hernandez S, Calarco R and Marso M 2009
Nanotechnology 20 405206
[26] Frielinghaus R, Estevez Hernandez S, Calarco R and
The authors gratefully acknowledge fruitful discussions and Schapers T 2009 Appl. Phys. Lett. 94 252107
suggestions by Professor H Luth. The authors thank also [27] Richter T, Blomers C, Luth H, Calarco R, Indlekofer M,
K H Deussen for technical support. This work was financially Marso M and Schapers T 2008 Nano Lett. 8 2834
supported by the German Ministry of Education and Research [28] Blomers C, Schapers T, Richter T, Calarco R, Luth H and
Marso M 2008 Phys. Rev. B 77 201301
project EPHQUAM and performed under the auspices of [29] Calarco R and Marso M 2007 Appl. Phys. A 87 499
the US Department of Energy under contract no. DE-AC02- [30] Kuball M, Pomeroy J, Wintrebert-Fouquet M, Butcher K, Lu H,
98CH1-886. Schaff W, Shubina T, Ivanov S, Vasson A and
Leymarie J 2005 Phys. Status Solidi a 202 763
[31] Trommer R and Cardona M 1978 Phys. Rev. B 17 1865
References [32] Temple P and Hathaway C 1973 Phys. Rev. B 7 8
[33] Kuball M, Pomeroy J, Wintrebert-Fouquet M, Butcher K,
[1] Wu J 2009 J. Appl. Phys. 106 011101 Lu H and Schaff W 2004 J. Cryst. Growth 269 59
[2] Che S B, Mizuno T, Wang X, Ishitani Y and Yoshikawa A 2007 [34] Schafer-Nolte E O, Stoica T, Gotschke T, Limbach E, Setter E,
J. Appl. Phys. 10(2) 083539 Setter P and Calarco R 2010 Appl. Phys. Lett. 96 091907

Vous aimerez peut-être aussi