High-quality heteroepitaxial two-dimensional (2D) InSb layers are very difficult to realize because of the large lattice mismatch with other widespread semiconductor substrates. A way around this problem is to grow free-standing 2D InSb nanostructures on nanowire (NW) stems, thanks to the capability of NWs to efficiently relax elastic strain along the sidewalls when lattice-mismatched semiconductor systems are integrated. In this work, we optimize the morphology of free-standing 2D InSb nanoflags (NFs). In particular, robust NW stems, optimized growth parameters, and the use of reflection high-energy electron diffraction (RHEED) to precisely orient the substrate for preferential growth are implemented to increase the lateral size of the 2D InSb NFs. Transmission electron microscopy (TEM) analysis of these NFs reveals defect-free zinc blend crystal structure, stoichiometric composition, and relaxed lattice parameters. The resulting NFs are large enough to fabricate Hall-bar contacts with suitable length-to-width ratio enabling precise electrical characterization. An electron mobility of ∼29 500 cm2/(V s) is measured, which is the highest value reported for free-standing 2D InSb nanostructures in literature. We envision the use of 2D InSb NFs for fabrication of advanced quantum devices.
High-quality heteroepitaxial two-dimensional (2D) InSb layers are very difficult to realize because of the large lattice mismatch with other widespread semiconductor substrates. A way around this problem is to grow free-standing 2D InSb nanostructures on nanowire (NW) stems, thanks to the capability of NWs to efficiently relax elastic strain along the sidewalls when lattice-mismatched semiconductor systems are integrated. In this work, we optimize the morphology of free-standing 2D InSb nanoflags (NFs). In particular, robust NW stems, optimized growth parameters, and the use of reflection high-energy electron diffraction (RHEED) to precisely orient the substrate for preferential growth are implemented to increase the lateral size of the 2D InSb NFs. Transmission electron microscopy (TEM) analysis of these NFs reveals defect-free zinc blend crystal structure, stoichiometric composition, and relaxed lattice parameters. The resulting NFs are large enough to fabricate Hall-bar contacts with suitable length-to-width ratio enabling precise electrical characterization. An electron mobility of ∼29 500 cm2/(V s) is measured, which is the highest value reported for free-standing 2D InSb nanostructures in literature. We envision the use of 2D InSb NFs for fabrication of advanced quantum devices.
High-quality III–V
narrow band gap semiconductor materials
with strong spin–orbit coupling and large Landé g-factor
provide a promising platform for applications in the field of optoelectronics,
spintronics, and quantum computing. Indium antimonide (InSb) offers
a narrow band gap, high carrier mobility, and a small effective mass
and perfectly fits to this scope. In fact, it has attracted tremendous
attention in recent years, both theoretically[1,2] and
experimentally,[3−6] for the implementation of topological superconducting states supporting
Majorana zero modes (MZMs). In particular, high quality InSb nanowires
(NWs) have opened new research arenas in quantum transport, since
their geometry leads to carrier confinement and their electron energy
levels are electrostatically tunable. However, the challenge remains
as NW morphology does not provide enough flexibility to fabricate
multicontact Hall-bar devices. An alternative geometry that would
allow a high degree of freedom in device fabrication and give the
opportunity to explore new material properties is represented by two-dimensional
(2D) InSb nanostructures.Unfortunately, because of large lattice
mismatch between InSb and
other widespread semiconductor systems, the growth of high-quality
heteroepitaxial 2D InSb layers is complicated and demands stacks of
buffer layers. To counter this problem, one can grow free-standing
2D InSb nanostructures on NW stems, thanks to the limited size of
the heterointerface and the capability to efficiently relax elastic
strain along the sidewalls. Nevertheless, controlling the aspect ratio
of free-standing InSb nanostructures is challenging, due to the low
vapor pressure of Sb and the surfactant effect.[7] In general, the narrower growth window of III–Sb
in comparison to other III–Vs (III–P and III–As)
is due to the surfactant effect of Sb atoms, as the atoms tend to
segregate to the surface, thereby modifying the surface energy.[7,8] For this reason, it is essential to investigate the growth mechanisms
and the morphology of InSb free-standing nanostructures.Studies
on the synthesis and the characterization of free-standing
2D InSb nanostructures grown by catalyst-assisted molecular beam epitaxy
(MBE) and metal–organic vapor phase epitaxy (MOVPE) are present
in literature.[9−11] Pure zinc blende (ZB) InSb nanosheets were grown
by Ag-assisted MBE.[9] In refs (10 and 11), a twin plane boundary induced
the formation of 2D InSb nanosails/nanoflakes. Here, we have realized
single-crystal free-standing InSb nanoflags (NFs) via Au-assisted
chemical beam epitaxy (CBE).In our previous work, we reported
on the growth and morphology
control of InSb nanostructures such as nanocubes, nanowires, and nanoflags
on top of InAs NW stems.[12] Concerning the
2D shape, we found that the limitation in achieving InSb NFs larger
than 1 μm in length and 280 nm in width was the flexibility
of the thin untapered InAs NW stems. As the growth time of the asymmetric
InSb segment is increased, the InAs stem bends, leading to the loss
of the alignment with the precursor fluxes and consequently of the
InSb orientation. Therefore, the preferential growth direction vanishes,
and 3D-like InSb structures are obtained. A possible solution to avoid
this problem is to employ more robust stems as, for example, tapered
NWs to provide a more stable support for the InSb NFs. This will keep
them well aligned even after long growth durations. Tapered InAs NWs
are not so easy to obtain because of their wurtzite (WZ) crystal structure
that reduces the radial vapor–solid growth on the NW sidewalls.[13] Instead, it is known that ZB or mixed WZ/ZB
structures in NWs enhance the radial growth rate.[13] InP NWs grown by Au-assisted CBE on InP(111)B substrates
have a mixed WZ/ZB crystal structure and a tapered morphology.[14]Keeping this into account, here we present
the growth of InSb NFs
on tapered and robust InP NWs. By using this approach, we are able
to achieve (2.8 ± 0.2) μm long, (470 ± 80) nm wide,
and (105 ± 20) nm thick InSb NFs. Furthermore, we have employed
reflection high-energy electron diffraction (RHEED), in order to carefully
adjust the substrate orientation with respect to the precursor beam
fluxes, which minimizes the thickness of these NFs. Thanks to the
larger dimension of the InSb NFs that we have obtained, we were able
to realize Hall-bar contacts far enough to keep the standard length-to-width
ratio between longitudinal and transversal contacts, which avoided
the presence of mixed components in Hall-bar measurements and allowed
one to accurately investigate the electrical properties. We demonstrate
an electron Hall mobility of ∼29 500 cm2/(V
s) at 4.2 K, which to our knowledge is the highest value reported
so far for free-standing 2D InSb nanostructures.[9−11]
Experimental Details
The InP–InSb axial heterostructures
of the present study
were synthesized by CBE in a Riber Compact-21 system on InP(111)B
substrates via Au-assisted growth[15,16] following
a methodology very similar to that reported in ref (12). We used 30 nm Au colloids
dropcasted onto the bare substrate as seeds to catalyze the growth
and trimethylindium (TMIn), tert-butylphosphine (TBP),
and trimethylantimony (TMSb) as metal–organic (MO) precursors.The growth sequence of the InP–InSb heterostructures consists
of the growth of InP stems followed by the InSb segments. We grew
InP stems for 60 min at a growth temperature (TInP) of 400 °C using 0.6 and 1.2 Torr of TMIn and TBP
line pressures, respectively. Afterward, the substrate temperature
was ramped down by ΔT in the presence of TBP
flux only to the InSb growth temperature, TInSb = TInP + ΔT (ΔT is negative here). In order to initiate InSb growth, group
V flux was abruptly switched from TBP to TMSb. For the growth of the
InSb segment, we used TMIn line pressures in the 0.3–0.9 Torr
range and TMSb line pressures in the 0.8–2.4 Torr range, as
described in the following section. The growth temperatures were measured
with a pyrometer with overall accuracy of ±5 °C. At the
end of the growth, samples were cooled down to room temperature in
an ultrahigh vacuum (UHV) environment without group V precursor flux
in order to prevent the accumulation of Sb on the heterostructure
sidewalls.In this work, we first demonstrate the optimization
of InSb NWs
on InP NW stems. From the knowledge of the effect of the growth parameters
we progress toward InSb NF growth. The growth procedures of both InSb
NWs and NFs are discussed in detail later in the text.The InP
NW stems and InSb NWs were grown rotating the substrate
at 5 rotations per minute (rpm) for the whole growth time. Conversely,
there was no sample rotation during the growth of the InSb NFs, and
the orientation was carefully adjusted before starting their growth
with the help of the RHEED pattern. Indeed, by stopping the rotation,
we trigger asymmetric growth, which is crucial to achieve the NF morphology.[12] The alignment protocol is illustrated in Figure . InP NWs grown on
InP(111)B have a hexagonal cross section with six equivalent {112}
sidewalls, as visible from the SEM image (45°-tilted and top-view)
of a representative NW (Figure a). Panel b shows a schematic view of the InP NW inside the
growth chamber (top- and side-view) with respect to the RHEED beam
(red arrow). Before initiating the InSb NF growth, the ⟨110⟩
direction was identified using the RHEED pattern as illustrated in Figure c. Indeed, this is
the direction at which we can see the overlap of the WZ and ZB reciprocal
lattices on the RHEED screen.[17] The substrate
was then rotated by 30° to obtain an alignment with the precursor
beam that maximizes the InSb NF elongation, as described in Results and Discussion, and the InSb NF growth was
initiated.
Figure 1
(a) A 45°-tilted and top view (inset) SEM images of an InP
NW stem (scale bar: 100 nm). (b) Top view (inset) and side view representation
of the alignment procedure of InP NWs with their corresponding RHEED
pattern along the ⟨110⟩ direction (red arrow). (c) RHEED
pattern of mixed WZ/ZB InP NWs in ⟨110⟩ direction.
(a) A 45°-tilted and top view (inset) SEM images of an InP
NW stem (scale bar: 100 nm). (b) Top view (inset) and side view representation
of the alignment procedure of InP NWs with their corresponding RHEED
pattern along the ⟨110⟩ direction (red arrow). (c) RHEED
pattern of mixed WZ/ZB InP NWs in ⟨110⟩ direction.The morphological characterization of the grown
heterostructures
was performed by acquiring field emission scanning electron microscopy
(SEM) images with a Zeiss Merlin SEM operating at an accelerating
voltage of 5 keV. Characterization of crystal structure and chemical
composition of mechanically detached NFs were carried out by transmission
electron microscopy (TEM) in a JEOL JEM-2200FS operated at 200 keV,
equipped with an in-column Ω-filter and Oxford X-ray energy
dispersive spectrometer (EDS/EDX). Imaging was performed in high-resolution
(HR) TEM mode combined with zero-loss energy filtering and by high-angle
annular dark-field in scanning mode (HAADF-STEM).To fabricate
the devices, the as-grown InSb NFs were dry transferred
on a prepatterned p-type Si(111) substrate, which serves as a global
back gate. A 285 nm thick SiO2 layer covers the Si substrate.
During the mechanical transfer, the InSb NFs are detached from the
InP NW stems, so that well isolated InSb NFs were found lying randomly
distributed on the substrate. Then the position of selected InSb NFs
was determined relative to predefined alignment markers using SEM
images. Considering the thickness and the edge geometry of the InSb
NFs, electrodes were patterned on a 400 nm thick layer of AR-P 679.04
resist with standard electron-beam lithography (EBL). Prior to metal
deposition, the samples were chemically etched for 1 min in a 1:9
(NH4)2S DI water-diluted
solution at 40 °C, to remove the native oxide layer from the
exposed NF areas and then rinsed for 30 s in H2O. Next,
a 10/190 nm Ti/Au film was deposited using thermal evaporation, followed
by lift off. All low-temperature magneto-transport data that we present
in this paper are from one single device, but we obtained consistent
data from three other devices.
Results and Discussion
InSb NWs
We first
studied the effect of InSb growth
temperature on the final shape of the InP–InSb heterostructured
NWs. Figure shows
SEM images of three samples grown at different ΔT. For all samples, the growth of the InP NW stems was followed by
InSb growth for 30 min using 0.6 Torr of TMIn and 1.2 Torr of TMSb
with sample rotation at 5 rpm for the whole growth duration.
Figure 2
InP–InSb
heterostructured NWs at different ΔT. 45°-titled
SEM images of NWs obtained at (a) ΔT = −50
°C, (b) −40 °C, and (c)
−30 °C (scale of all panels is the same as in a). Insets
represent respective high-magnification top view SEM images of one
representative NW with red arrow indicating the ⟨110⟩
substrate direction (inset scale bars: 50 nm). The aspect ratio, L/W, of the InSb NWs is denoted for each
ΔT at the bottom of the corresponding SEM image.
InP–InSb
heterostructured NWs at different ΔT. 45°-titled
SEM images of NWs obtained at (a) ΔT = −50
°C, (b) −40 °C, and (c)
−30 °C (scale of all panels is the same as in a). Insets
represent respective high-magnification top view SEM images of one
representative NW with red arrow indicating the ⟨110⟩
substrate direction (inset scale bars: 50 nm). The aspect ratio, L/W, of the InSb NWs is denoted for each
ΔT at the bottom of the corresponding SEM image.The aspect ratio, that is, length/width (L/W) of the InSb segments, is reported
at the bottom of each
panel. Larger values of ΔT, corresponding to
lower InSb growth temperatures, enhance the InSb radial growth rate
(larger diameter) and lower the axial growth rate, all together decreasing L/W. Increasing the temperature above ΔT = −30 °C leads instead to InSb desorption,
as in fact the InSb sublimation temperature is known to be around
400 °C.[18] Therefore, ΔT = −30 °C is the optimal InSb growth temperature
to obtain high aspect ratio InSb NWs on top of InP NW stems. The insets
in each panel of Figure show top view SEM images of an individual InP–InSb heterostructured
NW with hexagonal cross section of the upper InSb segment comprising
of six equivalent {110} oriented sidewalls.To evaluate other
growth parameters affecting the growth and the
morphology of the InP–InSb heterostructured NWs, we grew the
InSb segments at different TMIn/TMSb line pressure ratios.Figure illustrates
the morphology of the InP–InSb heterostructured NWs, obtained
as a function of TMIn and TMSb line pressure employed for the InSb
segment growth. The x- and y-axes
denote TMSb and TMIn line pressures, respectively. All samples are
grown at the optimal growth temperature of ΔT = −30 °C. We find that the yield (i.e., the ratio between
straight InSb nanostructures and total number of InP–InSb heterostructures,
counting all straight, kinked, and non-nucleating InSb) and the heterostructure
morphology strongly depend on the precursor line pressures. The InSb
segments are grown in two configurations: constant TMIn and varying
TMSb, or constant TMSb but varying TMIn line pressure. For the series
with constant TMIn line pressure (0.6 Torr) we grew three samples
with TMSb line pressure of (a) 0.8, (b) 1.2, and (c) 2.4 Torr. We
found that increasing Sb flux increases the aspect ratio of the NWs.
The yield is 4% for both the samples grown at lower (TMSb = 0.8 Torr)
and at higher (TMSb = 2.4 Torr) Sb flux. Instead, the yield is much
higher (around 86%) for TMSb line pressure of 1.2 Torr.
Figure 3
Yield and morphology
map of InP–InSb heterostructured NWs
as a function of the TMIn and TMSb line pressures. The InSb segments
are grown in two configurations: constant TMIn and constant TMSb line
pressure. (a–c) The 45°-tilted SEM images of InSb segments
for constant TMIn line pressure of 0.6 Torr and TMSb line pressure
of (a) 0.8, (b) 1.2, and (c) 2.4 Torr. (d,e) The 45°-tilted SEM
images of InSb segments for constant TMSb line pressure of 1.2 Torr
and TMIn line pressure of (d) 0.3 and (e) 0.9 Torr. All images have
the same scale indicated in (a).
Yield and morphology
map of InP–InSb heterostructured NWs
as a function of the TMIn and TMSb line pressures. The InSb segments
are grown in two configurations: constant TMIn and constant TMSb line
pressure. (a–c) The 45°-tilted SEM images of InSb segments
for constant TMIn line pressure of 0.6 Torr and TMSb line pressure
of (a) 0.8, (b) 1.2, and (c) 2.4 Torr. (d,e) The 45°-tilted SEM
images of InSb segments for constant TMSb line pressure of 1.2 Torr
and TMIn line pressure of (d) 0.3 and (e) 0.9 Torr. All images have
the same scale indicated in (a).Panels d and e of Figure show 45°-tilted SEM images of the InP–InSb
heterostructured NWs obtained at constant TMSb line pressure of 1.2
Torr and TMIn line pressure of 0.3 and 0.9 Torr, respectively. For
constant TMSb line pressure, the highest L/W is obtained for TMIn/TMSb = 0.6/1.2. The InSb growth yield
first increases from 31% to 86% by increasing the TMIn line pressure
from 0.3 to 0.6 Torr and then drops to 60% for 0.9 Torr of TMIn. On
the basis of the MO line pressure experiment, we found that the maximum
yield is obtained at TMIn/TMSb = (0.6/1.2) while the highest L/W of 15.9 is obtained at TMIn/TMSb= (0.6/2.4).
On the basis of these results, we can conclude that the best conditions,
at ΔT = −30 °C, to obtain both
high L/W and good yield for InSb
NWs are TMIn line pressure of 0.6 Torr and TMSb line pressure in the
range of 1.2–2.4 Torr.It is worth noting that some elongated
structures similar to flags
are occasionally observed in the samples. However, these are very
few (their occurrence is always <15%) and randomly oriented objects
among many NWs with symmetric cross section. It might be that these
asymmetric structures are formed due to partial shadowing of the beam
fluxes by neighboring NWs, or to some other local effects that we
did not study in detail.
InSb NFs
To grow free-standing InSb
NFs, we can exploit
our knowledge derived from the growth optimization of InSb NW on InP
stems (as discussed above) and from the asymmetric InSb growth and
its elongation via substrate orientation and higher Sb flux (from
previous work reported in ref (12)). InP NW stems were grown with sample rotation for 90 min
to provide more sturdy support, followed by InSb growth at ΔT = −30 °C without rotation with an abrupt switch
in group V flux from TBP to TMSb without variation in the TMIn flux.
The growth protocol employed for the growth of InSb NFs is schematically
shown in panel (a) of Figure . The initial InSb growth comprises of 0.6 Torr of TMIn and
2.3 Torr of TMSb to have a high Sb flux but still a good yield, and
then an additional 60 min of growth, linearly increasing the TMSb
line pressure from 2.3 to 2.6 Torr. Such Sb flux grading helps to
enhance the asymmetric growth, increasing the lateral dimensions of
the NFs, without compromising too much the yield of the InSb growth
on top of the InP NW stems that is known to drop if the growth starts
directly with higher Sb flux (see Figure ).
Figure 4
Growth and orientation protocol of InSb NFs.
(a) Schematics of
the growth protocol developed for obtaining InSb NFs. (b) Top-view
schematics of the precursor beams projection with respect to the InP–InSb
heterostructure cross section (bottom) and corresponding SEM images
after the first 30 min of InSb growth (top) in the two possible configurations:
configuration A with the Sb beam projection perpendicular to a {110}
plane, and configuration B with the Sb beam projection perpendicular
to a {112} plane. The scale bar is 100 nm. (c) Top view and (d) 45°-tilted
SEM image of the InSb NFs obtained in configuration B (scale bar:
1 μm). The InSb NFs which have (w/t) ≥ 4 are marked by yellow circles in panel c.
Growth and orientation protocol of InSb NFs.
(a) Schematics of
the growth protocol developed for obtaining InSb NFs. (b) Top-view
schematics of the precursor beams projection with respect to the InP–InSb
heterostructure cross section (bottom) and corresponding SEM images
after the first 30 min of InSb growth (top) in the two possible configurations:
configuration A with the Sb beam projection perpendicular to a {110}
plane, and configuration B with the Sb beam projection perpendicular
to a {112} plane. The scale bar is 100 nm. (c) Top view and (d) 45°-tilted
SEM image of the InSb NFs obtained in configuration B (scale bar:
1 μm). The InSb NFs which have (w/t) ≥ 4 are marked by yellow circles in panel c.As mentioned in the experimental details, before initiating
the
growth of InSb NFs the substrate rotation was stopped, and the orientation
of the NWs was carefully adjusted with the help of the RHEED pattern.
Orientation choices are illustrated in panel b of Figure : the InP NW (represented in
green) exhibits a hexagonal cross section with six equivalent {112}
sidewalls. The InSb segments (shown in blue) still have a hexagonal
cross section but with six equivalent {110} sidewalls. A schematic
top view of InP–InSb heterostructures is shown for two orientations:
configuration A and B. In configuration A, the Sb beam flux projection
is perpendicular to a {110} sidewall of the InSb NWs, while in configuration
B, the Sb beam projection is perpendicular to a {112} InP NW sidewall.
We found that the growth in configuration A leads to thicker InSb
NFs, while the growth in configuration B results in thinner NFs for
the same growth time. This is explained by considering that the growth
of the InSb segment involves two growth mechanisms that simultaneously
occur: the vapour-liquid-solid (VLS) axial growth on top of the NW
stem and the vapour-solid (VS) radial growth that is enhanced by high
Sb flux.[12] If the sample was rotated, the
radial growth would be uniform on the six {110} facets, and we would
obtain InSb nanowires with symmetric cross section, showing six sidewalls
equivalent in width. Conversely, when we stop the sample rotation
and align the substrate in configuration B, there are only two {110}
facets facing the Sb injector, that is, reached by direct impingement,
so the growth rate on these two facets will be higher compared to
the other four sidewalls, and we obtain thinner flags. On the other
hand, when the sample is oriented in configuration A, only the three
backside InSb facets (opposite to the Sb beam) are totally screened
from Sb impingement, while the sidewall perpendicular to the Sb beam
projection will receive the direct beam, and the two adjacent inclined
facets will be reached by the beam at grazing incidence. So, the NFs
will be larger and less elongated. Therefore, once we found the ⟨110⟩
direction with the help of the RHEED pattern at the end of the InP
NWs growth (as shown in Figure ), we rotated the substrate by 30° (i.e., to configuration
B) and started the InSb growth.Panels c and d of Figure show top view and 45°-tilted
SEM images of a sample
grown in configuration B. The yield of the NFs, that is, nanostructures
showing a width-to-thickness ratio (w/t) ≥ 4 (marked with yellow circles in panel c) is 40%, and
they have average length, width, and thickness of (2.8 ± 0.2)
μm, (470 ± 80) nm, and (105 ± 20) nm, respectively.
With the appropriate parameters (growth temperature and precursor
fluxes), robust InP stems, and precise substrate orientation, we could
grow the InSb NFs for longer time, obtaining larger InSb NFs with
similar thickness, compared with the InSb NFs obtained on InAs NW
stems[12] (see also Supporting Information Section S1), which are suitable for making electronic
devices, as demonstrated later. In addition, we speculate that similar
morphologies might be achieved by adopting this directional growth
approach for other materials if they show a consistent radial growth
together with the axial elongation.To determine the crystal
quality of the NFs, their structure was
analyzed by TEM (Figure ). A STEM-HAADF overview of a single InSb NF with a short segment
of its InP stem and the catalyst particle at the tip is shown in Figure a. The corresponding
HRTEM images acquired at the three NF corners (purple-, green-, and
yellow-framed panels) show the defect-free InSbzinc blende lattice.
The lattice spacing and the interplanar angles (see also the Fast
Fourier Transform in Figure b) match those of relaxed zinc blendeInSb (JCPDS card 6-208).
The analysis of the NFs faceting confirms the indexing observed in
our previously grown samples described in detail in ref (12). The major flat facets
are of the type (101̅) and (1̅01), bordered by sides parallel
to three pairs of directions: [1̅01̅] (dashed arrows),
[1̅2̅1̅] (dotted arrows), and [1̅1̅1̅]
(solid arrows, aligned with the growth axis).
Figure 5
(a) STEM-HAADF image
and corresponding HRTEM images acquired at
the NF corners in [101̅] zone axis; (b) indexed FFT of the HRTEM
image framed in yellow in panel (a). (c,d) HRTEM images acquired at
NF tip and base, respectively. The inset to (d) shows the FFT obtained
by color mixing the FFTs of a small square region in InP (blue color)
and InSb (red).
(a) STEM-HAADF image
and corresponding HRTEM images acquired at
the NF corners in [101̅] zone axis; (b) indexed FFT of the HRTEM
image framed in yellow in panel (a). (c,d) HRTEM images acquired at
NF tip and base, respectively. The inset to (d) shows the FFT obtained
by color mixing the FFTs of a small square region in InP (blue color)
and InSb (red).At the NF tip, a sharp interface
between InSb and the metal alloy
seed particle is observed (Figure c). EDX spectroscopy performed in STEM spot mode on
several NFs allowed us to identify the metal alloy components as Au
and In and to quantify an atom gold content of 34 ± 2%, consistent
with AuIn2.At the NF base, both an axial and a radial
growth of InSb on InP
is observed, as shown in Figure d and in Figure S2. As clearly
seen in these HRTEM images, the InP crystal structure is highly defected
with a mixed WZ/ZB stacking. Indeed, the energetic differences for
hexagonal or cubic stacking sequences in the ⟨111⟩ direction
are very small.[19] As a consequence, stacking
faults easily occur in InP NWs vertically grown on (111)B substrates,
resulting in NWs with alternating WZ/ZB segments.[14] The radially grown InSb, which was observed to be either
asymmetric or symmetric around the InP stem, as shown in Figure S2 from panels a–c, also appears
defected, showing several stacking faults and twins in its ZB lattice
along the stem length. On the contrary, the axially grown InSb shows
such a defected structure only in its initial layers, but after the
first 10 nm the stacking becomes regular and a perfect ZB structure
is recovered. After that, only a twin is observed occasionally within
the first 50 nm (as shown in Figure S2a,c). FFT analysis performed on the axial InSb close to the InP interface
(Figure d, indicated
in red with respect to the blue InP) shows that it reaches a complete
relaxation. EDX maps (as shown in Figure S2) confirm the purity (50 at% each for indium and antimony) and homogeneity
of InSb.To investigate the electronic properties of the InSb
NFs, we performed
low-temperature (4.2 K) magnetoresistance measurements on Hall-bar
devices. A SEM image of a representative Hall-bar device is shown
in Figure a. Figure b shows current–voltage
(ISD–VSD) curves of the source-drain (S-D) channel at 4.2 K as a function
of back gate voltage VBG. The linear ISD–VSD curves
together with the low resistance values indicate the presence of good
Ohmic contacts between the InSb NFs and the metal contacts, and the
absence of a Schottky barrier. Increasing the back gate voltage, the
source-drain resistance RSD = VSD/ISD decreases
from 25 kΩ for VBG = 10 V to 2.7
kΩ for VBG = 50 V. In a measurement
under constant AC voltage bias of 1 mV at 4.2 K, the variation of
the injected current as a function of back gate voltage was measured
and is shown in Figure c. A voltage bias is necessary here since in the depletion region
(negative gate voltages), the sample is insulating and a constant
current could not flow. In other words, in the range of back gate
voltages that we explored, we did not observe ambipolar behavior.
The longitudinal voltage drop V is measured
simultaneously in a four-probe configuration. We performed back gate
sweeps for both V contact
combinations [(1–2) and (3–4)], and both showed consistent
results. From these data, the four-probe field-effect mobility is
calculated to be about 28 000 cm2/(V s) (for details,
see Figure S3). The charge carrier modulation
shows an increasing conductance with increasingly positive back gate
voltage, consistent with an n-type behavior of the InSb NFs and in
agreement with the data shown in Figure b.
Figure 6
(a) SEM image of an InSb NF Hall-bar device
with corresponding
numbers for Hall-bar contacts. (b) Two-probe ISD–VSD curves as a function
of back gate voltage VBG. (c) Source-drain
current versus back gate voltage, measured under 1 mV constant AC
voltage bias. All measurements are performed at a temperature of 4.2
K.
(a) SEM image of an InSb NF Hall-bar device
with corresponding
numbers for Hall-bar contacts. (b) Two-probe ISD–VSD curves as a function
of back gate voltage VBG. (c) Source-drain
current versus back gate voltage, measured under 1 mV constant AC
voltage bias. All measurements are performed at a temperature of 4.2
K.In addition to field-effect measurements,
we performed a series
of Hall-effect measurements using a constant AC current bias of 100
nA at 4.2 K. Since these measurements were performed in current bias,
they start at a back gate voltage of 15 V at which the channel is
already well open. Figure a shows the resulting Hall-voltage curves as a function of
magnetic field for different back-gate voltages VBG. The
corresponding charge-carrier densities and Hall-mobilities for various
back-gate voltages are shown in Figure b (for details, see Figure S4). Hall mobility increases with increasing back-gate voltage and
shows a maximum of about 29 500 cm2/(V s) at VBG = 25 V, with a corresponding electron density
of 8.5 × 1011 cm–2. For even higher
carrier concentrations, mobility slightly drops again due to additional
carrier scattering induced by Coulomb interactions. Hence, Hall mobility
is in good agreement with the four-probe field effect mobility, and
higher than in previous studies,[9−11] which reported at most 20 000
cm2/(V s). We attribute this higher mobility to the fact
that our flags are slightly thicker (100 nm) than the flakes reported
previously that ranged from 50 to 80 nm, which reduces the contribution
of surface- and interface-scattering. Figure b also shows that charge-carrier density
increases with increasing back-gate voltage, as expected. Furthermore,
we estimated the electron mean free path λe, using
λe = (ℏμ/e)(2πn)1/2, ref (20), with ℏ
the reduced Planck’s constant and n the 2D
electron density from the Hall measurements (cf. Figure b). As shown in Figure c, λe reaches
values of ∼500 nm for VBG ≥
25 V, which compares favorably with literature.[10,11,21]
Figure 7
(a) Hall measurements on InSb NFs: V as a function of magnetic field B
for different
back gate voltages VBG at 4.2 K. (b) Mobility
and charge carrier density obtained from the Hall measurements shown
in (a). (c) Elastic mean free path λe as a function
of back gate voltage VBG.
(a) Hall measurements on InSb NFs: V as a function of magnetic field B
for different
back gate voltages VBG at 4.2 K. (b) Mobility
and charge carrier density obtained from the Hall measurements shown
in (a). (c) Elastic mean free path λe as a function
of back gate voltage VBG.
Conclusions
In conclusion, we have realized free-standing
2D InSb NFs on InP
NW stems exhibiting the highest electron mobility compared to other
similar 2D InSb nanostructures reported in literature. This was possible
by carefully choosing a robust supportive stem, tapered InP NWs, by
optimizing the growth parameters leading to the growth of InSb NWs
with high yield and high aspect ratio, and by aligning the samples
in the direction that maximizes the NF elongation keeping the NF thickness
at a minimum. This strategy allowed us to obtain InSb NFs of (2.8
± 0.2) μm length, (470 ± 80) nm width, and (105 ±
20) nm thickness with defect-free ZB crystal structure, stoichiometric
composition, and relaxed lattice parameters. We strongly believe that
these NFs can serve for realization of exotic bound states at the
semiconductor interface with superconductors, paving the way for the
development of topological quantum computation technologies.
Authors: María de la Mata; Renaud Leturcq; Sébastien R Plissard; Chloé Rolland; César Magén; Jordi Arbiol; Philippe Caroff Journal: Nano Lett Date: 2016-01-11 Impact factor: 11.189
Authors: Sasa Gazibegovic; Ghada Badawy; Thijs L J Buckers; Philipp Leubner; Jie Shen; Folkert K de Vries; Sebastian Koelling; Leo P Kouwenhoven; Marcel A Verheijen; Erik P A M Bakkers Journal: Adv Mater Date: 2019-02-19 Impact factor: 30.849
Authors: Önder Gül; Hao Zhang; Jouri D S Bommer; Michiel W A de Moor; Diana Car; Sébastien R Plissard; Erik P A M Bakkers; Attila Geresdi; Kenji Watanabe; Takashi Taniguchi; Leo P Kouwenhoven Journal: Nat Nanotechnol Date: 2018-01-15 Impact factor: 39.213
Authors: S Battiato; S Wu; V Zannier; A Bertoni; G Goldoni; A Li; S Xiao; X D Han; F Beltram; L Sorba; X Xu; F Rossella Journal: Nanotechnology Date: 2019-01-11 Impact factor: 3.874