Photon-avalanche-like upconversion in

NdAl3(BO3)4 nanoparticles excited at 1064 nm

Cite as: Appl. Phys. Lett. 117, 151102 (2020); https://doi.org/10.1063/5.0024619
Submitted: 09 August 2020 . Accepted: 02 October 2020 . Published Online: 13 October 2020

Jefferson F. da Silva , Rodrigo F. da Silva, Emanuel P. Santos , Lauro J. Q. Maia, and André L. Moura

Appl. Phys. Lett. 117, 151102 (2020); https://doi.org/10.1063/5.0024619 117, 151102

© 2020 Author(s).
 Applied Physics Letters ARTICLE scitation.org/journal/apl

Photon-avalanche-like upconversion in
NdAl3(BO3)4 nanoparticles excited at 1064 nm
Cite as: Appl. Phys. Lett. 117, 151102 (2020); doi: 10.1063/5.0024619
Submitted: 9 August 2020 . Accepted: 2 October 2020 .
Published Online: 13 October 2020

Jefferson F. da Silva,1 Rodrigo F. da Silva,1 Emanuel P. Santos,1 Lauro J. Q. Maia,2 and Andre
 L. Moura1,3,a)

AFFILIATIONS
1
Grupo de Fısica da Mate  ria Condensada, Nu  cleo de Cie^ ncias Exatas–NCEx, Campus Arapiraca, Universidade Federal de Alagoas,
57309-005 Arapiraca, AL, Brazil
2
Instituto de Fısica, Universidade Federal de Goia  s, 74690-900 Goia ^ nia, GO, Brazil
3
Programa de Po  s-graduaça~ o em Fısica, Instituto de Fısica, Universidade Federal de Alagoas, 57072-900 Maceio
 , AL, Brazil

a)
Author to whom correspondence should be addressed: andre.moura@fis.ufal.br

ABSTRACT
We report efficient nonresonant ground-state excitation at 1064 nm of trivalent neodymium (Nd3þ) ions in stoichiometric neodymium
aluminum borate NdAl3(BO3)4 nanoparticles, which are crystalline and, besides the large content of Nd3þ ions, present excellent photolumi-
nescence properties. Upconversion (UC) emission was observed, and the energy pathways were identified starting from multi-phonon
assisted ground-state absorption (4I9/2 ! 4F3/2) and excited-state absorption (4I11/2 ! 4F3/2) with the population of the 4I11/2 level by thermal
coupling with the ground state. The excited state 4I11/2 is also populated by relaxations of the Nd3þ ions at upper-lying levels. Cross-
relaxation between two Nd3þ ions (4F3/2, 4I9/2) ! (4I15/2, 4I15/2) with subsequent phonon emission leads to two ions at the 4I11/2 level, with
every iteration triggering a photon-avalanche-like emission, which greatly enhances the efficiency of the UC emissions. Ladder thermal exci-
tation 4F3/2 ! (4F5/2, 2H9/2) ! (4F7/2, 4S3/2) ! 4F9/2 was achieved, and the ground-state relaxation from these levels provided emission at
880 nm, 810 nm, 750 nm, and 690 nm, respectively. Energy transfer UC (Auger) between Nd3þ ions at the 4F3/2 level allowed the population
of (2G3/2, 4G7/2) from which relaxations to the 4I9/2, 4I11/2, and 4I13/2 states provided emissions around 536 nm, 600 nm, and 660 nm, respec-
tively. Associated with the nonradiative relaxations, we observed the heating of the nanoparticles (22  C–240  C) with subsequent thermal
enhancement of the frequency UC emissions due to population redistribution between the coupled energy levels of the Nd3þ ions. The
present results have potential applications in super-resolution imaging and nanothermometry.
Published under license by AIP Publishing. https://doi.org/10.1063/5.0024619

Trivalent lanthanide (Ln3þ) ions possess the capability to absorb
and emit radiation in a broad spectral range covering the ultra-violet
(UV), visible, and infrared regions.1 Because of that, the Ln3þ ions are
used in several applications due to their peculiar electronic structures.2
One interesting mechanism to excite Ln3þ ions is the photon ava-
lanche (PA) that takes place when the excitation wavelength is not res-
onant with ground-state absorption (GSA) transitions, but is resonant
with an excited-state absorption (ESA) transition. In such conditions,
the GSA cross section (rGSA) is much lower than the ESA cross section
(rESA), i.e., rGSA  rESA.3–5 A small population at the lower level of
the ESA transition (intermediate level) is promoted to an upper energy
level by ESA, and the ions in this upper excited state can transfer the
stored energy to neighboring ones by cross-relaxation (CR), promot-
ing a large number of ions to the intermediate level. Afterward, these
ions can absorb excitation photons again and be promoted to more
energetic levels, restarting the chain of events and establishing an
avalanche mechanism (PA). In this way, the small absorption of the
material to the excitation wavelength would increase by several orders
of magnitude and, consequently, the output luminescence due to the
relaxations of ions at the more energetic level to lower lying ones.
Among the Ln3þ ions, the photoluminescence properties of
neodymium (Nd3þ) ions have been extensively studied due to their
rich energy level structure. For example, Nd3þ ions can be excited to
emit radiation over the ultra-violet, visible, and infrared spectral
ranges. They also present several thermally coupled energy levels and
can exchange stored energy with neighboring ions of the same or dif-
ferent species. Excitation pathways of single-, double-, and triply
doped materials with Nd3þ ions can be by upconversion (UC) and
downconversion mechanisms, with temperature-dependent absorp-
tion cross sections, cross-relaxation mechanisms, ESA, and thermal
coupling of the energy levels. PA in Nd3þ-based materials has been
demonstrated in bulk materials (YLiF4,6,7 LaCl3,8,9 and CeCl310) at low

Appl. Phys. Lett. 117, 151102 (2020); doi: 10.1063/5.0024619 117, 151102-1
Published under license by AIP Publishing
 Applied Physics Letters
temperature under visible excitation, as well as in nanoparticles
(LiLaNdP4O12,11 NdVO4,12,13 and CeVO412) at room temperature
under near infrared excitation (800 nm). Although Nd3þ ions have a
strong radiative transition at around 1060 nm, these ions present very
low GSA at this wavelength. However, this wavelength is resonant
with the 4I11/2 ! 4F3/2 ESA transition, fulfilling one of the PA require-
ments. There is only one report on PA in Nd3þ-doped materials under
excitation around 1060 nm,14 in which the authors investigated the PA
in NaYF4, Y2O3, YGdO3, YAlO3, Y3Al5O12, LiLaP4O12, and Gd2O3
nanoparticles, demonstrating an intense emission around 880 nm
(Nd3þ transition 4F3/2 ! 4I9/2).14
A current trend involving Ln3þ ions is the investigation of photo-
luminescence properties of Nd3þ-doped nanoparticles obtained
through different synthesis routes.15–19 One interesting material is
neodymium-aluminum-borate NdAl3(BO3)4, which is obtained by
replacing the yttrium ions by Nd3þ in the YAl3(BO3)4 crystalline
structure.20–24 In principle, the large amount of Nd3þ ions in this
structure may favor quenching mechanisms, deleterious thermal
effects, and crystalline structure modification. However, NdAl3(BO3)4
presents excellent linear and nonlinear optical properties, an anoma-
lously high quantum efficiency (0.30, 4F3/2 level),24 and allows the laser
(and random laser) operation,23,25–28 including those with self-
frequency conversions.29,30
Here, we investigate an unconventional excitation route of the
Nd3þ ions at 1064 nm using NdAl3(BO3)4 nanoparticles. At this wave-
length, there is no resonant GSA, and the energy mismatch to the clos-
est resonant ground-state transition (4I9/2 ! 4F3/2) is large
(1850 cm1). Also, the resonant ESA transition 4I11/2 ! 4F3/2 occurs
with low probability at room temperature due to the large energy gap
(1870 cm1) between 4I11/2 and the ground state. We demonstrate
the feasibility of the excitation through phonon annihilation in order
to compensate the energy mismatches. Energy transfer between Nd3þ
(4F3/2, 4I9/2) doubles the number of ions at the 4I11/2 level, with every
iteration succeeding a photon-avalanche-like mechanism that allows
efficient population of the Nd3þ ions to the 4F3/2 level through the res-
onant ESA transition 4I11/2 ! 4F3/2. The involved relaxation pathways
of Nd3þ via multi-phonon generation increased the nanoparticle tem-
perature, which provided the population redistribution of the Nd3þ
energy levels. The output photoluminescence consists of several wave-
lengths (visible and near infrared) whose energy pathways were
identified.
The synthesis procedure of the NdAl3(BO3)4 nanoparticles was
performed by the polymeric precursor method as described in the
supplementary material. The morphological and structural characteri-
zation studies were performed in a previous publication.29 It suffices to
mention that the nanoparticles have a crystalline structure of the
monoclinic cell with the C2/c space group. The particle size distribu-
tion is broad, with its peak at 80 nm.29 The largest phonon energy is
1360 cm1,31,32 and the density of Nd3þ ions is 5  1021 ions/cm3. The
diffuse reflectance spectrum of the nanoparticle powder was obtained
using an UV/Vis/near-infrared (NIR) spectrophotometer using BaSO4
powder as the reference. In the photoluminescence experiments, the
excitation source was provided by a Nd:YAG laser operating at
1064 nm in the continuous wave (cw) regime and excitation powers
(Pexc) up to 2.0 W. The laser light was focused onto the powder, which
was gently pressed in a sample holder. The excited area at the powder
surface was 0.06 mm2. A pair of lenses was used to collect and focus
Appl. Phys. Lett. 117, 151102 (2020); doi: 10.1063/5.0024619
Published under license by AIP Publishing
ARTICLE scitation.org/journal/apl
the generated light onto a multimode optical fiber coupled to a spec-
trometer. The spectrometer was equipped with a charge-coupled
device (ccd) allowing real-time spectral measurements from 330 nm to
1180 nm with a 2.0-nm resolution. The ccd integration time was fixed
at 50 ms, allowing consecutive spectrum acquisition every 50 ms. A
short-pass optical filter was used to reject the elastically scattered exci-
tation laser light. Simultaneous to the spectral measurements, the tem-
perature nanoparticle temperature was monitored using a thermal
camera (detection range of 20 to 650  C, accuracy of 1  C), allowing
the correlation between the spectrum and the temperature of the
nanoparticles. The procedure is detailed in the supplementary
material. Radiative transitions from the Nd3þ ions within the wave-
length range operation of the thermal camera (7.5–13 lm) are not
expected.
The absorbance of the NdAl3(BO3)4 nanoparticle powder can be
inferred from the diffuse reflectance spectrum [Fig. 1(a)], in which the
valleys correspond to Nd3þ absorption transitions from the ground
state (4I9/2) to the indicated energy levels. It can also be observed that
no resonant GSA occurs at the excitation wavelength (1064 nm),
represented by the vertical arrow. In spite of that, exciting the nano-
particles at this wavelength generated temperature-dependent, up-
converted, near-infrared, and visible emission bands centered at
880 nm, 810 nm, 750 nm, 690 nm, 660 nm, 600 nm, and 536 nm
[Fig. 1(b), Pexc ¼ 1.8 W], associated with Nd3þ ion electronic transi-
tions between their 4f states. The emission at around 1064 nm in
Fig. 1(b) is due to the excitation laser, which was not filtered
completely. A photograph of the nanoparticle powder at 240  C is dis-
played in the inset of Fig. 1(b). The intense yellowish emission could
be seen by the naked eye, even at room illumination.
Based on Refs. 22 and 23, we present the simplified energy level
diagram of the Nd3þ ions in the NdAl3(BO3)4 nanoparticles (Fig. 2),
in which the energy pathways involved in the UC emissions of
Fig. 1(b) are described. First, there is nonresonant GSA of the
FIG. 1. NdAl3(BO3)4 nanoparticle optical characterization. (a) Room-temperature
diffusive reflectance. The indicated levels are the ending states of the ground-state
absorption transitions of Nd3þ ions. The up-arrow indicates the excitation wave-
length (kexc ¼ 1064 nm) used in the photoluminescence experiments. (b)
Photoluminescence spectrum under cw excitation at kexc when Pexc ¼ 1.8 W for dif-
ferent temperatures. The Nd3þ transitions are indicated along each band. The right
inset shows a photograph of the powder at T ¼ 240  C.
117, 151102-2
 Applied Physics Letters
FIG. 2. Simplified energy-level diagram of the NdAl3(BO3)4 nanoparticles. The verti-
cal arrows indicate the possible energy pathways in the nanoparticle excitation.
Thermal excitations are represented by wavy arrows. The acronyms NR, CR, and
ETU stand for nonradiative relaxations, cross-relaxations, and energy transfer
upconversion, respectively.
excitation photons, which occurs with the annihilation of phonons
from the crystalline lattice to compensate the energy mismatching
(1850 cm1) with the 4I9/2 ! 4F3/2 transition. Also, thermal coupling
of the 4I11/2 level with the ground state (DE 1870 cm1) allows the
resonant ESA 4I11/2 ! 4F3/2. Due to the relatively large energy gap in
both cases, the associated transition rates are very low at room temper-
ature. In spite of that, once excited, the Nd3þ ions at 4F3/2 can relax to
lower-lying levels, and the ground-state relaxation transition 4F3/2 !
4
I9/2 generates the emission around 880 nm. In addition, the Nd3þ
ions at 4F3/2 can be further excited to the (4F5/2, 2H9/2) levels by pho-
non anihilation,33–35 and by means of a ladder excitation mechanism
to the (4F7/2, 4S3/2) levels, their ground-state relaxations generate emis-
sions at 810 nm and 750 nm, respectively. Similar thermal coupling
under ESA at 1060 nm (4I11/2 ! 4F3/2) was recently reported in
LaPO4:Nd3þ nanoparticles.36 Here, we observed additional ladder
thermal excitations that populate 4F9/2 and upper-lying levels. The
ground-state relaxation 4F9/2 ! 4I9/2 generates the emission around
690 nm. On the other hand, the emissions at 536 nm, 600 nm, and
660 nm are obtained by the Nd3þ excitation to the (2G3/2, 4G7/2) levels,
which can occur by (1) energy transfer upconversion (ETU) between
two Nd3þ ions at 4F3/2, where one of them relaxes to 4I13/2 and the
other is promoted to the (2G3/2, 4G7/2) levels. Other possibility of pop-
ulating the (2G3/2, 4G7/2) levels is by (2) ESA of excitation radiation
(ESAER) of Nd3þ ions at the 4F3/2 level. However, the ETU is domi-
nant over ESAER in highly doped crystals.37 Also, previous works on
the NdAl3(BO3)4 crystal24,38 showed that the ETU is the dominant
mechanism and the emissions at 536 nm, 600 nm, and 660 nm are
assigned to the relaxations from (2G3/2, 4G7/2) to the 4I9/2, 4I11/2, and
4
I13/2 levels, respectively. Thermal coupling contributions from lower-
lying energy levels also contribute to populating the (2G3/2, 4G7/2)
levels. At high temperatures and long ccd exposure times, a blue emis-
sion near 480 nm was detected (Fig. S1), which is associated with the
thermal excitation (2G3/2, 4G7/2) ! (2G9/2, 4G11/2) followed by the
radiative transition (2G9/2, 4G11/2) ! 4I9/2. It is worth mentioning that
a previous study investigated Ga10Ge25S65 glasses doped with Nd3þ
Appl. Phys. Lett. 117, 151102 (2020); doi: 10.1063/5.0024619
Published under license by AIP Publishing
ARTICLE scitation.org/journal/apl
ions under pulsed (7 ns) excitation at 1064 nm.39 The observed emis-
sions at 535 nm, 600 nm, and 670 nm were attributed to the relaxation
transitions 4G7/2 ! 4I9/2, (4G7/2 ! 4I11/2; 4G5/2 ! 4I9/2), and (4G7/2 !
4
I13/2; 4G5/2 ! 4I11/2), respectively, obtained via two-photon absorp-
tion (TPA) from I9/2 to 4G7/2, and a single-photon absorption to 4F3/2
followed by ETU between the Nd3þ ions. Here, we also carried out
experiments under pulsed excitation, with the laser operating in the
Q-switched and mode-locked regimes. Since the results were qualita-
tively equivalent to those under cw excitation (Fig. S2), TPA as the
leading excitation mechanism was ruled out.
Generally, in photoluminescence experiments, the input–output
power dependence (Pin–Pout) is given by Pout ¼ A(Pin)n, with A being
the proportionality constant and n the number of excitation photons
required for each absorption transition. However, for the 880 nm
emission, n varied with Pexc (from 0.6 to 3.7, Fig. 3) presenting a
threshold power (Pth 1.1 W), from which the output intensity
changed its behavior attaining a threefold enhancement. n 1 for Pexc
< Pth agrees with the proposed energy pathway in which one excita-
tion photon is required to populate the 4F3/2 level. The output intensity
saturated for Pexc >1.5 W, and the input–output curve displayed an S-
shape that is characteristic of PA, which is associated with the resonant
ESA 4I11/2 ! 4F3/2.14 The PA is triggered by a small population of
the 4I11/2 level by the thermal coupling with the ground state
(DE 1870 cm1) and several relaxation pathways of the Nd3þ ions at
the 4F3/2 level. The radiative and multi-phonon Nd3þ relaxations from
4
F3/2 to lower-lying levels (4I11/2, 4I13/2, and 4I15/2) increase the popula-
tion at 4I11/2, establishing an energy loop.40 Cross-relaxations from
Nd3þ ions at 4F3/2 to nonexcited neighboring ones (favored by the
high amount of Nd3þ ions) double the number of ions at 4I15/2, i.e.,
(4F3/2, 4I9/2) ! (4I15/2, 4I15/2), and the subsequent multi-phonon relax-
ations (favored by the high phonon energy) contribute to double the
population at the 4I11/2 level after every iteration.14 This leads to a
strong population increase at the 4F3/2 level via resonant ESA. In this
FIG. 3. Input–output power dependencies for the up-converted emissions at
880 nm and 810 nm (on the log –log scale). A threshold excitation power (Pth) of
1.1 W is well-defined, evidencing the photon-avalanche-like. The curves were
obtained from linear fitting of the data, and the corresponding slopes are indicated.
The excitation of the nanoparticles caused light-to-heat conversion, and the steady-
state temperature is represented (the curve is a guide to the eye).
117, 151102-3
 Applied Physics Letters
scenario, the PA condition rGSA  rESA (<2  103, see the supple-
mentary material) is fulfilled, and the cross-relaxation between Nd3þ
ions is fundamental to the observation of the S-shape curve (Fig. S6).
However, usually in PA, the enhancement factor of the photolumines-
cence is high. Here, besides the depletion of the 4I9/2 and 4I11/2 popula-
tions, the saturation also has the contribution from the coupling of the
4
F3/2 level with upper-lying levels, as described ahead, which limited
the enhancement factor to 3. The emission at 810 nm demonstrated
the threshold behavior and S-shape curve due to the population
dependence between the corresponding emitting levels (4F5/4, 2H9/2)
with 4F3/2 and also the thermal coupling with upper-lying levels: n var-
ied from 0.8 to 8.9 at Pexc > Pth and saturated at Pexc >1.8 W. It is
worth mentioning that, according to the energy level diagram in Fig. 2,
the same power dependence would be expected for both 880 nm and
810 nm emissions. However, as described ahead, the excitation of the
nanoparticles was accompanied by light-to-heat conversion that
increased the nanoparticle temperature (a function of Pexc, Fig. 3).
Since the thermal excitation of Nd3þ ions from 4F3/2 to (4F5/2, 2H9/2)
levels is temperature-dependent, the power dependence of the corre-
sponding emissions is affected by both Pexc and temperature. Then, we
attribute the difference in the 880 nm and 810 nm emission behavior
to the intrinsic heating of the sample when Pexc is increased (see the
discussion about Fig. S9).
Associated with the nonradiative relaxations (NR) of Nd3þ ions,
we observed the light-to-heat conversion, which increased the nano-
particle temperature provoking population redistribution between
Nd3þ energy levels, as described in the following lines. Figures
4(a)–4(c) show the nanoparticle temperature, measured using a ther-
mal camera, as a function of the exposure time to the excitation beam
FIG. 4. Photoluminescence intensity at 880 nm and nanoparticle temperature as a
function of the exposure time to the excitation laser at the indicated power. The
temperature increase is associated with light-to-heat conversion due to nonradiative
relaxations of the Nd3þ ions.
Appl. Phys. Lett. 117, 151102 (2020); doi: 10.1063/5.0024619
Published under license by AIP Publishing
ARTICLE scitation.org/journal/apl
when Pexc equals 1.1 W, 1.5 W, and 1.8 W, respectively. The steady-
state temperature as a function of Pexc is given in Fig. 3. Similar results
were reported in NaYF4:Nd3þ nanoparticles under excitation at
795 nm, and the authors attributed the heating mainly to cross-
relaxations between Nd3þ ions.41 Here, large multi-phonon relaxation
rates are expected due to the high maximum phonon energy
(1360 cm1).24
The temporal evolution of the emission at 880 nm and the nano-
particle temperature presented behaviors depending on Pexc with rela-
tion to the PA threshold (Fig. 4). For Pexc close to Pth (1.1 W), the
time dependence of the output luminescence closely follows the tem-
perature [Figs. 4(a) and 4(b)]. We associated it with a looping mecha-
nism, where nonradiative relaxations increase the nanoparticle
temperature, which, in turn, increases the excitation light absorption
(nonresonant GSA and ESA transitions), resulting in more nonradia-
tive relaxations. Then, the evolution of the 880 nm emission presented
rise times on the order of a few seconds, much larger than that
expected for PA (10 ls; Fig. S7). For Pexc ¼ 1.8 W [Fig. 4(c)], the
emission achieved its maximum at 4 s followed by a slight decrease.
We associate it with the depletion of the 4I9/2 and 4I11/2 levels caused
by the PA as well as with the quenching of the Nd3þ 4F3/2 population
to upper-lying levels, whose couplings are temperature dependent
(Fig. S7). Because of the intrinsic thermal effects influencing the tem-
poral evolution of the Nd3þ level population, the input–output behav-
ior presented here is better described as photon-avalanche-like, in the
sense that the underlying physical mechanism is not purely explained
by PA.
The change of the nanoparticle temperature due to nonradiative
relaxations of Nd3þ provoked pronounced modifications in the photo-
luminescence spectra, as shown in Fig. 1(b) for Pexc ¼ 1.8 W. The fol-
lowing features were observed in the output spectra: (1) pronounced
enhancement of the UC emissions and (2) changes in the emission
line shape of the bands, accompanied by a blue shift with the tempera-
ture increase. The peak intensity of UC emission bands increased with
the temperature, presenting distinct dependencies (Fig. 5).
Enhancements of 440, 300, and 25 times were observed when the tem-
perature increased from 22  C to 240  C for the emissions at 750 nm,
810 nm, and 880 nm, respectively. At room temperature (spectra
obtained immediately after the initial excitation of the nanoparticles),
the emissions at 536 nm, 600 nm, 660 nm, and 690 nm were not
intense enough to be detected by our measurement system, but were
detected for temperatures above 80  C. Notice that the emissions at
690 nm, 750 nm, and 810 nm started to increase significantly at differ-
ent temperatures, which corroborate the ladder thermal excitation
mechanism. Also, the emissions at 536 nm, 600 nm, and 660 nm pre-
sented similar temperature dependencies that corroborate with their
association with transitions departing from the same energy level
(2G3/2, 4G7/2). We investigated the operation of a thermometer based
on the intensity ratio between the emissions at 810 nm and 880 nm
(Fig. S8). The relative thermal sensitivity was temperature-dependent
presenting a maximum value of 2.95%  C1 at 34  C, which is consid-
ered high for Ln3þ ions.42,43
In summary, we investigated an unconventional excitation of
Nd3þ ions at 1064 nm in NdAl3(BO3)4 nanoparticles, which is nonres-
onant with ground-state transitions. It provided intense upconversion
(UC) emissions, which were enhanced by a photon avalanche (PA)
mechanism. The PA starts with the population of the lower-lying
117, 151102-4
 Applied Physics Letters ARTICLE scitation.org/journal/apl

intensity ratio of the emissions at 810 nm and 880 nm; and explanation
about the distinct power dependencies of the emissions at 880 nm and
810 nm.
AUTHORS’ CONTRIBUTIONS
J.F.d.S. and A.L.M. conceived this project. J.F.d.S. performed the
experimental measurements. L.J.Q.M. synthesized the nanoparticles.
All the authors discussed the experimental results, implemented the
rate equation model, and wrote this manuscript.

We acknowledge the financial support from the Brazilian

agencies: Fundaç~ao de Amparo a Pesquisa do Estado de Alagoas
(FAPEAL); Coordenaç~ao de Aperfeiçoamento de Pessoal de Nivel
Superior (CAPES)–Finance Code 001, Fundaç~ao de Amparo a
Pesquisa do Estado de Goias (FAPEG), Financiadora de Estudos e
Projetos (FINEP), Conselho Nacional de Desenvolvimento
Cientıfico e Tecnologico (CNPq) through the Grant No. 427606/
2016–0; scholarships in Research Productivity 2 under Nos.
303990/2019–8 and 305277/2017–0; and National Institute of
Photonics (INCT de Fot^onica). E.P.S. and R.F.d.S. thank CNPq for
their Scientific Initiation scholarship. We also thank J. G. B.
Cavalcante, M. A. Nascimento, and Professor C. Jacinto (also for
helpful discussion), Professor M. V. D. Vermelho, and Professor A.
S. Gouveia-Neto for the technical support. We thank F. G. Rego-
Filho for proofreading this manuscript.
DATA AVAILABILITY
The data that support the findings of this study are available
from the corresponding author upon reasonable request.

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Appl. Phys. Lett. 117, 151102 (2020); doi: 10.1063/5.0024619 117, 151102-6
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