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LETTER | APRIL 11 2023

Effect of substrate rotation speed on AlGaN nanowire deep


ultraviolet light-emitting diodes by molecular beam epitaxy

Mohammad Fazel Vafadar ; Rezoana Bente Arif ; Qihua Zhang ; Songrui Zhao 

Journal of Vacuum Science & Technology B 41, 030601 (2023)


https://doi.org/10.1116/6.0002494

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LETTER avs.scitation.org/journal/jvb

Effect of substrate rotation speed on AlGaN


nanowire deep ultraviolet light-emitting diodes by
molecular beam epitaxy
Cite as: J. Vac. Sci. Technol. B 41, 030601 (2023); doi: 10.1116/6.0002494
Submitted: 16 January 2023 · Accepted: 15 March 2023 · View Online Export Citation CrossMark
Published Online: 11 April 2023

Mohammad Fazel Vafadar, Rezoana Bente Arif, Qihua Zhang, and Songrui Zhaoa)

AFFILIATIONS

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Department of Electrical and Computer Engineering, McGill University, 3480 University Street, Montreal,
Quebec H3A 0E9, Canada

a)
Author to whom correspondence should be addressed: songrui.zhao@mcgil.ca

ABSTRACT
Aluminum gallium nitride (AlGaN) nanowires by molecular beam epitaxy (MBE) have become an emerging platform for semiconductor
deep ultraviolet (UV) light-emitting diodes (LEDs). Despite of the progress, much less attention has been paid to the effect of substrate rota-
tion speed on the device performance. Herein, we investigate the effect of the substrate rotation speed on the nanowire height and diameter
uniformity, as well as the electrical and optical performance of MBE-grown AlGaN nanowire deep UV LED structures with low and high
substrate rotation speeds. It is found that by increasing the substrate rotation speed from 4 revolutions per minute (rpm) to 15 rpm, the stat-
istical variation of the nanowire height and diameter is reduced significantly. Increasing the substrate rotation speed also improves the
device electrical performance, with a factor of 4 reduction on the device series resistance. This improved electrical performance further
transfers to the improved optical performance. The underlying mechanisms for these improvements are also discussed.

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I. INTRODUCTION investigated.14–21 Compared to planar structures, AlGaN NWs offer


Deep UV light sources including LEDs and lasers have several advantages. Due to the effective lateral stress relaxation,
nearly defect-free AlGaN NWs can be grown on various substrates
become demanding due to their wide range of applications includ-
including silicon (Si), metal, graphene, and so on.22,23 More impor-
ing food sterilization, wastewater treatment, air purification, photo-
tantly, AlGaN NWs are promising to significantly improve p-type
ionization, medical care, and so on. In this context, semiconductor
conduction due to the drastic enhancement of magnesium
AlGaN deep UV light sources have been intensively studied in the
(Mg)-dopants incorporation in NW structures.24–26 In addition,
past few years due to their excellent physical, chemical, and owing to the multiple scattering effect and the large
mechanical properties, such as ultrawide, direct, and tunable band surface-to-volume ratio in NW structures, the emitted light can
gap energies, that can allow light emission down to close to escape relatively easily compared to planar structures, in particular,
200 nm.1–13 Moreover, they are environment-friendly due to the for TM polarized light.27–29 Several studies have shown, both exper-
use of nonhazardous chemicals. Nevertheless, despite of intensive imentally and theoretically, the advantages of utilizing AlGaN NW
efforts in the development of AlGaN-based planar deep UV LEDs structures in deep UV LEDs and lasers, such as the demonstration
and lasers, a number of critical challenges have remained, such as of electrically injected deep UV lasing down to 239 nm, which is
large threading dislocation and defect densities in the AlGaN epi- still challenging for planar structures.30–32
taxial layer, poor p-type doping, low light extraction efficiency due Plasma-assisted (PA) MBE is one of the major driving tech-
to light polarization, and local heating under high current injection, niques for AlGaN NW deep UV light-emitting device development,
e.g., Refs. 1, 2, 6, 7, 10, and 13. such as UV lasers aforementioned. In general, by properly control-
In recent years, as an alternative route to semiconductor deep ling the growth parameters, such as the substrate temperature, the
UV LEDs and lasers, AlGaN nanowires (NWs) have been nitrogen (N) flow rate, and metal (Ga and Al) fluxes, highly dense

J. Vac. Sci. Technol. B 41(3) May/Jun 2023; doi: 10.1116/6.0002494 41, 030601-1
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LETTER avs.scitation.org/journal/jvb

and relatively uniform AlGaN NWs can be formed without any surface reconstruction. Two substrate rotation speeds were used,
substrate patterning. As such, although the substrate patterning can 4 rpm for sample A and 15 rpm for sample B. The scanning elec-
lead to highly uniform AlGaN NWs, it is still meaningful to opti- tron microscopy (SEM) images were taken at a 45° tilting angle
mize growth conditions for self-organized AlGaN NWs due to the using a field-emission SEM.
low substrate preparation cost.33–36 Standard photolithography and metallization processes were
Compared to parameters such as the substrate temperature used for fabricating the electrically injected devices, in which a con-
and metal fluxes, much less attention has been paid to the substrate ventional Ni/Au thin metal bilayer was used as the p-contact to the
rotation speed during the growth of AlGaN NWs, e.g., Refs. 37–39. NW top surface. The device size was determined by the p-contact
Therefore, to further improve the device performance of AlGaN size, which varied from 0.3 × 0.3 to 1 × 1 mm2. Colloidal silver
NW deep UV LEDs, elucidating the effect of substrate rotation is paste was used as the n-contact to the backside of the n-Si sub-
necessary. In this study, we investigate the effect of the substrate strate. Current–voltage (I–V) characteristics of the devices were
rotation speed on the nanowire height and diameter uniformity of measured under continuous-wave biasing conditions, and the elec-
AlGaN NWs and further the electrical and optical performance of troluminescence (EL) spectra of the fabricated devices were col-
AlGaN NW deep UV LEDs. It is found that the height and diame- lected from the device top surface at room temperature using an
ter variations of AlGaN NWs are drastically reduced using a rela- optical fiber and analyzed through a deep UV spectrometer.
tively high substrate rotation speed (15 rpm) compared to using a

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low substrate rotation speed (4 rpm). The electrical and optical per- III. RESULTS AND DISCUSSION
formances of AlGaN NW deep UV LEDs are also improved. This
study will further help the development of AlGaN NW-based semi- Figures 1(b) and 1(c) show SEM images of AlGaN NWs
conductor deep UV LEDs and lasers. grown with the substrate rotation speed of 4 (sample A) and
15 rpm (sample B), respectively, with the inset showing high mag-
nification SEM images. It is seen that, by increasing the substrate
II. EXPERIMENT rotation speed, the NW top-surface morphology improves. In spe-
Experimentally, the device structures were grown on n-Si cific, the coalescence in sample B is reduced compared to sample
(111) substrates by PA-MBE (model: Veeco GENxplor) in N-rich A. The inset also suggests a more significant variation of the nano-
conditions. Figure 1(a) shows the schematic of the layer-by-layer wire height and diameter in sample A compared to sample B.
structure of an individual NW that constitutes the large area To further investigate the nanowire height and diameter varia-
AlGaN NW deep UV LEDs, including an n-GaN seed layer, fol- tion comparing the two samples, statistics based on the SEM
lowed by p–i–n AlGaN homojunction, and a very thin p-GaN images was carried out. Figure 2(a) shows the results for the NW
contact layer. As the purpose is to evaluate the effect of substrate diameter. It seen that, for sample A, the NW diameter varies from
rotation speed, simple p–i–n AlGaN homojunction structures were 40 to 80 nm, with a statistical average of 56.4 nm and a standard
used. The growth parameters included a nitrogen flow rate of deviation of 9.2 nm; for sample B, the NW diameter varies in a
0.9 SCCM, a substrate temperature of 725 °C for the n-GaN layer, much smaller range of 45–65 nm, with a statistical average of
845 °C for the AlGaN homojunction, and 750 °C for the p-GaN 54.1 nm and a standard deviation of 4.9 nm. These statistical values
contact layer, as well as a Ga flux of 4 × 10−8 Torr and an Al flux of clearly indicate an improved NW diameter uniformity by using a
2 × 10−8 Torr. The substrate temperature was calibrated by Si (111) higher substrate rotation speed. Figure 2(b) shows the statistics of

FIG. 1. (a) Schematic of an individual AlGaN NW. (b) and (c) Tilted-view SEM images of the AlGaN NWs grown under the same growth parameters, except the difference
in the substrate rotation speed, with (b) of 4 rpm (sample A) and (c) of 15 rpm (sample B). The inset highlights the top-surface morphology difference, with a more severe
coalescence on the top in sample A (the arrows exemplify a few coalescences) compared to sample B.

J. Vac. Sci. Technol. B 41(3) May/Jun 2023; doi: 10.1116/6.0002494 41, 030601-2
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FIG. 2. (a) and (b) Statistics of the NW diameter and height for samples A and B, respectively.

the NW height. It is seen that for sample A, the NW height is in deep UV emitting AlGaN NWs have been shown at a low substrate
the range of 150–250 nm with a statistical average of 201.6 nm and rotation speed.44,45 Using a high substrate rotation speed helps the
a standard deviation of 30.7 nm; for sample B, the NW height only scenarios in which the III/N ratio or the temperature is not opti-
varies from 170 to 215 nm with a statistical average of 197.2 nm mized, and an additional knob for a better uniformity is needed. A
and a standard deviation of 10.3 nm. These statistical values clearly high substrate rotation speed essentially relaxes the requirements of
suggest an improved NW height uniformity as well with using a other parameters to obtain highly uniform AlGaN NWs.
higher substrate rotation speed. We have next compared the electrical performance of AlGaN
Previous studies on the epitaxy of III–V epilayers have clearly NW deep UV LEDs. Figure 3 shows the I–V characteristics for
shown the critical role of substrate rotation speed on the epilayer
uniformity. Given the flux profile for a fixed source position, a flux
gradient exists over the wafer; as such, certain substrate rotation
speed criteria should be satisfied in order to minimize the thickness
variation.40 Moreover, for the nanowire growth, additional effect due
to the substrate rotation exists. This was reported by Foxon et al.41 It
is found that in the growth of GaN nanowires with sources not in
the normal direction with respect to the substrate (like ours),
although atoms (N and Ga) can arrive at a given point on the top
surface of nanowires simultaneously, they do not arrive at a given
location on the sidewall at the same time due to different source
locations and the substrate rotation. As such, the growth on the side-
wall is mimicking metal-modulated epitaxy (MME); and in this case,
the lateral growth rate is dependent on the rotation speed and more
uniform nanowires can be obtained by using substrate rotation.
Separate studies further show that the lateral growth rate strongly
affects the nanowire uniformity through the lateral growth enhanced
shadow effect.42 As such, higher substrate rotation leads to a more
uniform nanowire formation. This model can also explain our case.
It is also noted that, in the growth of indium gallium nitride
(InGaN) NWs, holding the substrate steady leads to nanosheets
rather than NWs.43
Nonetheless, it is worth mentioning that, to obtain relatively FIG. 3. I–V characteristic for samples A and B. Dashed lines are guide for eyes
uniform self-organized AlGaN NWs, using a high substrate rota- for the series resistance estimation. The device size is 1 × 1 mm2.
tion speed might not be necessary. For example, relatively uniform

J. Vac. Sci. Technol. B 41(3) May/Jun 2023; doi: 10.1116/6.0002494 41, 030601-3
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FIG. 4. (a) EL emission spectra of samples A and B under an injection current of 40 mA. (b) Light intensity vs the injection current for samples A and B.

samples A and B, with the main figure showing the linear scale and clearly manifests the improvement on the light intensity with using
the inset showing the semilogarithmic scale. It is seen that sample a high substrate rotation speed. Lastly, it is worth mentioning that
B has improved I–V characteristics compared to sample A, includ- these I–V and EL improvements are measured at a wafer scale.
ing (1) the leakage current of sample B is reduced roughly by one
order of magnitude at −8 V compared to sample A and (2) the
IV. SUMMARY AND CONCLUSIONS
forward current (at 10 V) of sample B is also increased by more
than twice in comparison to sample A. This leads to more than In conclusion, we have reported the effect of the substrate
one order of magnitude improvement on the rectification ratio at rotation speed on the nanowire height and diameter uniformity, as
±8 V. The series resistance for both samples is further estimated by well as the electrical and optical performance of AlGaN NW deep
the slope near 10 V, which gives 447.6 Ω for sample A and 115.7 Ω UV LED structures. SEM studies, combining NW statistics, suggest
for sample B. an improved NW height and diameter uniformity, when a high
Two possible reasons could largely account for this improved substrate rotation speed is used. The improved nanowire uniformity
electrical performance. First, it could be related to a more uniform can be explained by the reduced MME effect for the nanowire
Mg doping. It is known from previous studies that high Mg doping lateral growth. Device electrical performance is further compared,
could be harmful for p-type conduction due to doping induced and a factor of 4 reduction in the device series resistance and one
defects; as such, if no rotation, Mg concentration could be high order of magnitude improvement on the rectification ratio
locally (this has been shown in previous studies, e.g., Ref. 43), (at ±8 V) are also obtained by using a high substrate rotation speed,
reducing p-type conductivity. Second, the improvement could be largely due to the improved p-type conduction in the p-AlGaN
through a reduced coalescence. With higher rotation speed, nano- layer. This electrical performance enhancement further transfers to
wires are more uniform (as explained earlier), and coalescence the improved light intensity of AlGaN NW deep UV LEDs. This
could be reduced (SEM images do suggest coalescence is less in the work represents the first report on the effect of the substrate rota-
higher rpm sample, although coalescence is still present, due to a tion speed on the properties of AlGaN NW deep UV LED struc-
high nanowire density). As most of the defects in Mg-doped tures and will help the further development of AlGaN NW-based
III-nitrides are detrimental to p-type doping, reducing coalescence, semiconductor deep UV LEDs and lasers.
thus, could improve p-type conduction.
The enhanced electrical performance further transfers to the ACKNOWLEDGMENTS
improved light output power. Figure 4(a) shows the EL emission
spectra for samples A and B under an injection current of 40 mA. This work is supported by Natural Sciences and Engineering
It is seen that both samples emit light around 240 nm, shown by Research Council of Canada (NSERC) and Fonds de Recherche du
the dominant EL emission peak. Moreover, the light intensity of Quebec—Nature et Technologies (FRQNT). The authors would
sample B is higher than sample A. It is also noted that, in addition also like to acknowledge CMC Microsystems for the provision of
to the main EL emission peak, another EL emission peak with a products and services that facilitated this research.
wavelength in the range of 280–300 nm is also observed, which
could be due to the light emission from the p-AlGaN region, i.e., AUTHOR DECLARATIONS
optical transitions related to the deep levels in high Al content
AlGaN alloys.46–48 Figure 4(b) further shows the light intensity as a Conflict of Interest
function of the injection current for samples A and B, which The authors have no conflicts to disclose.

J. Vac. Sci. Technol. B 41(3) May/Jun 2023; doi: 10.1116/6.0002494 41, 030601-4
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LETTER avs.scitation.org/journal/jvb

22
Author Contributions C. Zhao et al., Prog. Quantum Electron. 61, 1 (2018).
23
H. Sun and X. Li, Phys. Status Solidi A 216, 1800420 (2018).
Mohammad Fazel Vafadar: Data curation (lead); Formal analysis 24
N. H. Tran, B. H. Le, S. Zhao, and Z. Mi, Appl. Phys. Lett. 110, 032102
(lead). Rezoana Bente Arif: Data curation (supporting); Formal anal- (2017).
ysis (supporting). Qihua Zhang: Data curation (supporting). Songrui 25
Z. Fang, E. Robin, E. Rozas-Jiménez, A. Cros, F. Donatini, N. Mollard,
Zhao: Conceptualization (lead); Formal analysis (supporting). J. Pernot, and B. Daudin, Nano Lett. 15, 6794 (2015).
26
S. Zhao, B. H. Le, D. P. Liu, X. D. Liu, M. G. Kibria, T. Szkopek, H. Guo, and
DATA AVAILABILITY Z. Mi, Nano Lett. 13, 5509 (2013).
27
R. Lin, S. V. Galan, H. Sun, Y. Hu, M. S. Alias, B. Janjua, T. K. Ng, B. S. Ooi,
The data that support the findings of this study are available and X. Li, Photonics Res. 6, 457 (2018).
28
from the corresponding author upon reasonable request. J. Lu, M. F. Vafadar, and S. Zhao, J. Nanophotonics 15, 036002 (2021).
29
M. Djavid and Z. Mi, Appl. Phys. Lett. 108, 051102 (2016).
30
S. Zhao, X. Liu, Y. Wu, and Z. Mi, Appl. Phys. Lett. 109, 191106 (2016).
REFERENCES 31
K. H. Li, X. Liu, Q. Wang, S. Zhao, and Z. Mi, Nat. Nanotechnol. 10, 140
1
M. Kneissl, T.-Y. Seong, J. Han, and H. Amano, Nat. Photonics 13, 233 (2019). (2015).
2 32
H. Amano et al., J. Phys. D: Appl. Phys. 53, 503001 (2020). S. Zhao, X. Liu, S. Y. Woo, J. Kang, G. A. Botton, and Z. Mi, Appl. Phys. Lett.
3
Y. Taniyasu, M. Kasu, and T. Makimoto, Nature 441, 325 (2006). 107, 043101 (2015).
4 33
H. Yoshida, Y. Yamashita, M. Kuwabara, and H. Kan, Nat. Photonics 2, 551 X. Liu, B. H. Le, S. Y. Woo, S. Zhao, A. Pofelski, G. A. Botton, and Z. Mi, Opt.

Downloaded from http://pubs.aip.org/avs/jvb/article-pdf/doi/10.1116/6.0002494/16827133/030601_1_6.0002494.pdf


(2008). Express 25, 30494 (2017).
5 34
H. Hirayama, N. Maeda, S. Fujikawa, S. Toyoda, and N. Kamata, Jpn. J. Appl. A. Bengoechea-Encabo et al., J. Cryst. Growth 325, 89 (2011).
35
Phys. 53, 100209 (2014). M. F. Vafadar and S. Zhao, ACS Appl. Nano Mater. 5, 16045 (2022).
6 36
D. Li, K. Jiang, X. Sun, and C. Guo, Adv. Opt. Photonics 10, 43 (2018). B. H. Le, S. Zhao, X. Liu, S. Y. Woo, G. A. Botton, and Z. Mi, Adv. Mater. 28,
7
T. D. Moustakas and R. Paiella, Rep. Prog. Phys. 80, 106501 (2017). 8446 (2016).
8 37
H. Sun et al., Adv. Funct. Mater. 29, 1905445 (2019). S. Fernández-Garrido, J. Grandal, E. Calleja, M. A. Sánchez-García, and
9
H. Yu, M. H. Memon, D. Wang, Z. Ren, H. Zhang, C. Huang, M. Tian, H. Sun, D. López-Romero, J. Appl. Phys. 106, 126102 (2009).
38
and S. Long, Opt. Lett. 46, 3271 (2021). J. K. Zettler, C. Hauswald, P. Corfdir, M. Musolino, L. Geelhaar, H. Riechert,
10
Y. Muramoto, M. Kimura, and S. Nouda, Semicond. Sci. Technol. 29, 084004 O. Brandt, and S. Fernández-Garrido, Cryst. Growth Des. 15, 4104
(2014). (2015).
11 39
Y. Zhang, S. Krishnamoorthy, F. Akyol, J. M. Johnson, A. A. Allerman, Y. Zhong, E. Berikaa, J. Lu, X. Yin, and S. Zhao, AIP Adv. 10, 025022
M. W. Moseley, A. M. Armstrong, J. Hwang, and S. Rajan, Appl. Phys. Lett. 111, (2020).
40
051104 (2017). Z. R. Wasilewski, in Molecular Beam Epitaxy, edited by M. Henini (Elsevier,
12
C. Liu, Y. K. Ooi, S. M. Islam, J. Verma, H. G. Xing, D. Jena, and J. Zhang, Oxford, 2013), pp. 631–655.
41
Appl. Phys. Lett. 110, 071103 (2017). C. T. Foxon, S. V. Novikov, J. L. Hall, R. P. Campion, D. Cherns, I. Griffiths,
13
M. H. Crawford, in Semiconductors and Semimetals, edited by Z. Mi and and S. Khongphetsak, J. Cryst. Growth 311, 3423 (2009).
42
C. Jagadish (Elsevier, New York, 2017), Vol. 96, pp. 3–44. N. V. Sibirev, M. Tchernycheva, M. A. Timofeeva, J.-C. Harmand,
14
S. Zhao et al., Sci. Rep. 5, 8332 (2015). G. E. Cirlin, and V. G. Dubrovskii, J. Appl. Phys. 111, 104317 (2012).
15 43
H. Parimoo, Q. Zhang, M. Vafadar, J. Sivasundarampillai, and S. Zhao, Appl. F. A. Chowdhury, M. L. Trudeau, H. Guo, and Z. Mi, Nat. Commun. 9, 1707
Phys. Lett. 120, 171108 (2022). (2018).
16 44
A. T. M. G. Sarwar, B. J. May, J. I. Deitz, T. J. Grassman, D. W. McComb, and S. Zhao et al., APL Mater. 4, 086115 (2016).
45
R. C. Myers, Appl. Phys. Lett. 107, 101103 (2015). S. Zhao, S. M. Sadaf, S. Vanka, Y. Wang, R. Rashid, and Z. Mi, Appl. Phys.
17
S. Zhao and Z. Mi, IEEE J. Quantum Electron. 54, 1 (2018). Lett. 109, 201106 (2016).
18 46
B. J. May, C. M. Selcu, A. T. M. G. Sarwar, and R. C. Myers, Appl. Phys. Lett. M. L. Nakarmi, N. Nepal, J. Y. Lin, and H. X. Jiang, Appl. Phys. Lett. 94,
112, 093107 (2018). 091903 (2009).
19 47
M. F. Vafadar and S. Zhao, J. Vac. Sci. Technol. B 40, 050602 (2022). K. B. Nam, M. L. Nakarmi, J. Y. Lin, and H. X. Jiang, Appl. Phys. Lett. 86,
20
S. Zhao, J. Lu, X. Hai, and X. Yin, Micromachines 11, 125 (2020). 222108 (2005).
21 48
A. T. M. G. Sarwar, B. J. May, M. F. Chisholm, G. J. Duscher, and R. C. Myers, N. Nepal, M. L. Nakarmi, J. Y. Lin, and H. X. Jiang, Appl. Phys. Lett. 89,
Nanoscale 8, 8024 (2016). 092107 (2006).

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