Computational Materials Science 161 (2019) 143–150

Contents lists available at ScienceDirect

Computational Materials Science

journal homepage: www.elsevier.com/locate/commatsci

Accelerating materials science with high-throughput computations and T

machine learning
Shyue Ping Ong
Materials Virtual Lab, Department of NanoEngineering, University of California San Diego, 9500 Gilman Dr, Mail Code 0448, La Jolla, CA 92093-0448, United States

ARTICLE INFO ABSTRACT

Keywords: With unprecedented amounts of materials data generated from experiments as well as high-throughput density
Machine learning functional theory calculations, machine learning techniques has the potential to greatly accelerate materials
High-throughput discovery and design. Here, we review our efforts in the Materials Virtual Lab to integrate software automation,
Materials discovery data generation and curation and machine learning to (i) design and optimize technological materials for energy
Materials design
storage, energy efficiency and high-temperature alloys; (ii) develop scalable quantum-accurate models, and (iii)
Multi-scale models
enhance the speed and accuracy in interpreting characterization spectra.

1. Introduction human performance in a variety of tasks, from playing board games

Computational methods are today an important complement to
experiments in the study and design of materials. Computational
techniques provide the means to precisely control the simulation con-
ditions (e.g., modification of a single parameter or set of parameters),
something which is difficult to truly achieve under experimental con-
ditions. Such controlled “virtual experiments” can often lead to fun-
damental insights on the factors determining a particular material
property or set of material properties, enabling rational materials de-
sign. Among computational techniques, first principles electronic
structure methods, which start from the basic laws of physics with
minimal assumptions, are particularly useful due to their chemical
agnosticity.
In the recent decade, electronic structure codes have matured and
computing power has advanced to a degree that first principles calcu-
lations, especially those based on more cost-effective approximations
such as Kohn-Sham density functional theory (DFT) [1,2], can be re-
liably automated [3–5] for high-throughput property prediction across
vast number of materials. High-throughput DFT calculations have been
used in successful materials design efforts for applications as varied as
alkali-ion batteries [6–8], catalysts [9], topological insulators [10], and
organic semiconductors [11], and led to the development of large, high-
quality open databases of computed materials properties such as the
Materials Project [12], Open Quantum Materials Database [13] and the
AFLOW repository [14]. This explosion in the quantity of computed
materials data has also begun to fuel interest in the application of
machine learning to accelerate the study and design of materials. Ma-
chine learning (ML) has emerged as a means to mimic, or even surpass,
such as chess and Go [15] to interpretation of medical images [16] to
autonomous driving. It should be noted that most large computed
materials databases (and the ML models on which they are based) are
still constructed using the Perdew-Berke-Ernzerhof (PBE) [17] gen-
eralized gradient approximation (GGA) functional for reasons of com-
putational efficiency, which has well-known failures in certain patho-
logical systems, such as those where strong electron correlation and van
der Waals interactions play a significant role [18–21]. Nevertheless,
this is a limitation that we believe will be gradually addressed by
methodological advances, for example, such as the SCAN functional
[22], in the future.
In the Materials Virtual Lab, we leverage on our core expertise in
software automation [3–5], data generation and curation [23–27], and
machine learning in three ways: (i) to optimize existing materials or
discover new technological materials, (ii) to develop models to access
beyond-DFT scales at near-DFT accuracy, and (iii) to accelerate and
enhance the accuracy of materials characterization.
2. Materials optimization and discovery
2.1. Rechargeable alkali-ion batteries
As rechargeable alkali-ion batteries move beyond consumer elec-
tronic applications into large-scale applications such as transportation
and grid storage, there is an urgent need for novel materials and battery
architectures that not only deliver higher gravimetric and volumetric
densities, but are also safer. To this end, our research efforts on this
front are focused on two parallel efforts: (i) solid electrolytes for safer,

E-mail address: ongsp@eng.ucsd.edu.

https://doi.org/10.1016/j.commatsci.2019.01.013
Received 27 October 2018; Received in revised form 10 January 2019; Accepted 10 January 2019
0927-0256/ © 2019 Elsevier B.V. All rights reserved.
S.P. Ong
more energy dense all-solid-state alkali-ion batteries; and (ii) multi-
electron cathodes for high-capacity batteries.
2.1.1. All-solid-state batteries
There has been a surge in interest in all-solid-state rechargeable
alkali-ion batteries (SSABs) in recent years [28–32]. By replacing
flammable organic solvent electrolytes with nonflammable solid elec-
trolytes (SE), SSABs have the potential to be safer and to provide gains
in system-level energy densities through stacking or enabling new
electrode chemistries (e.g., high-voltage cathodes and alkali metal an-
odes. To be an effective SE, a material has to have extremely high ionic
conductivities (> 0.1 mS/cm), i.e., be a superionic conductor, and
exhibit good chemical and mechanical compatibility with the elec-
trodes. In the Materials Virtual Lab, we have sought to simultaneously
address all these requirements using DFT computations [26,33–42].
Using nudged elastic band [43] calculations coupled with a bond per-
colation model, we have proposed rational composition optimization
strategies for the lithium-rich anti-perovskite [44] family of superionic
conductors [33]. We have also used ab initio molecular dynamics
(AIMD) simulations to propose cation and anion doping strategies for
Na3PS4 [34,35], a highly promising SE for all-solid-state Na-ion bat-
teries [31]. These works have led to the successful development of Cl-
doped Na3PS4 with experimentally-measured room temperature ionic
conductivity exceeding 1 mS/cm, and stable cycling demonstrated over
more than 10 cycles in a TiS2/Cl-Na3PS4/Na cell [35]. On a broader
level, our work has provided insights into the crucial role of defects and
alkali concentration play in optimizing ionic conductivity [33–38], and
the intrinsic mechanical properties [26] and electrochemical stability
[35–38] of various classes of superionic conductors.
Besides bulk ionic conductivity, a critical bottleneck to the practical
application of SSABs is the high resistance and poor stability of elec-
trode/solid electrolyte interface. Using various thermodynamic ap-
proximations with DFT calculations, we have shown that the formation
of energetically favored PO34 through an exchange reaction is the main
cause of instability between layered oxide cathodes and thiophosphate
(a)
Fig. 1. Reaction energies and volume changes for (a) discharged electrode/solid electrolyte pairs and (b) potential buffer layer materials and active materials, in all-
solid-state sodium-ion batteries. Reproduced with permission from Ref. [41].
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Computational Materials Science 161 (2019) 143–150
solid electrolytes (see Fig. 1) [41]. We have also identified several
binary oxides (Sc2O3, SiO2, TiO2, ZrO2 and HfO2) to be chemically inert
with respect to electrodes and SEs and therefore are potential candidate
buffer layers in addition to the commonly used Al2O3 [41]. Finally, we
have demonstrated that AIMD simulations of an explicit electrode/SE
interface model predict that the oxidation of S2− to form SxOy may be
kinetically preferred over the formation of PO34 , in contrast to the
thermodynamic predictions [41]. This hierarchy of models provide a
spectrum of computational approaches to study interfacial stability, and
provide much-needed guidance for the future development of practical
SSABs.
2.1.2. Multi-electron cathodes
Cathodes in commercial lithium-ion batteries today operate on the
basis of a single redox per transition metal on average. For example,
LiCoO2 and LiFePO4 operate on the Co3+/4+ and Fe2+/3+ redox cou-
ples, respectively. To achieve higher capacities, one approach is to
develop multi-electron cathodes that can reversibly cycle more than
one electron per transition metal [45]. A particularly promising family
of multi-electron cathodes are the vandayl phosphates with formula
VOPO4. Utilizing the V3+/4+/5+ couple, VOPO4 has high theoretical
capacities of 308 mAh/g [46] and relatively high voltages due to the
inductive effect of the PO4 polyanion [47]. Through a highly colla-
borative effort integrating DFT calculations, in operando characteriza-
tion and electrochemical measurements, we have provided crucial in-
sights into the thermodynamics, phase evolution and kinetics of the
polymorphs of VOPO4 upon lithiation [48–51]. We have successfully
identified the structures of the intermediate phases -Li1.5VOPO4 and
-Li1.75VOPO4, and showed that nanosizing and carbon coating are
critical to achieving good electrochemical performance due to the poor
electronic conductivity and 1D diffusion topology of -LixVOPO4 [48].
More recently, we have performed a comprehensive DFT study of the
, and -I polymorphs of VOPO4, which suggested the phase may
yield superior kinetics for Li diffusion, but only the layered -I phase is
predicted to have sufficiently low migration barriers for Na [49].
(b)
S.P. Ong Computational Materials Science 161 (2019) 143–150

Furthermore, other VOPO4 derived from bigger alkali cations, e.g.,
KVOPO4, may also yield low migration barriers for Na+ and high
achievable capacities and energy densities [52].
2.2. Phosphors for next-generation solid-state lighting
Phosphor-converted white-light-emitting diodes (pc-WLEDs) are an
energy efficient and environmentally friendly next generation lighting
technology [53,54]. For white light for general illumination, the key
performance metrics are high quantum efficiency, resistance to thermal
quenching, and high color quality, i.e., a low color-correlated tem-
perature (CCT) of <3000 K and a high color-rendering index (CRI) of >
85. Even today, commercial WLEDs such as those based on blue LED
chips with a yellow-emitting phosphor (Y3Al5O12:Ce3+)) have poor CRI
<80 and high CCT >5000 K, and many contain phosphors with rare
earths or expensive elements in large quantities. There is therefore a
critical need to find new earth-abundant phosphors as well as to further
optimize the performance of existing phosphors.
In the Materials Virtual Lab, our focus has been primarily on
phosphors utilizing Eu2+ and Ce3+ activators. One of our major
achievements has been the discovery of the Sr2LiAlO4 phosphor host
(see Fig. 2) [55]. Sr2LiAlO4, the first known quaternary crystal in the Sr-
Li-Al-O system, was identified to be a thermodynamically and dyna-
mically stable crystal by a machine-learned structure prediction algo-
rithm [56] and DFT screening effort, guided by statistical analysis of
known phosphors in the Inorganic Crystal Structure Database (ICSD)
[57]. Experimental collaborators have successfully synthesized
Sr2LiAlO4 and confirmed that the Eu2+- and Ce3+-activated phosphors
exhibit broad emissions at 512 nm (green-yellow) and
max
434 nm (blue), respectively, with excellent thermal quenching
max

Fig. 2. (a) Frequency at which each element appears in compounds having the word “phosphor” in the publication title in the 2017 version of ICSD. (b) DFT 0 K SrO-
Li2O-Al2O3 phase diagram. Blue circles, known stable phases in the Materials Project database [12]; red square, new stable quaternary phase, Sr2LiAlO4. (c) Unit cell
and Sr local environment (in Å) of the Sr2LiAlO4 crystal. (d, e) Measured excitation and emission spectra of (d) Sr2LiAlO4:0.005Eu2+ and (e) Sr2LiAlO4:0.005Ce3+
phosphors. Colors are indicated under the emission spectra for easy reference. Reproduced with permission from Ref. [55].

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S.P. Ong Computational Materials Science 161 (2019) 143–150

resistance of >88% intensity at 150°C and excellent CRI exceeding 90 in
a prototype WLED. This is a rare example of the successful discovery of
a technological material from computational prediction to experimental
confirmation to device fabrication. We have also developed an elec-
tronic structure descriptor for emission bandwidth and identified po-
tential narrow-band red phosphors, which are of great interest for im-
proving CRI [58].
Using DFT calculations, we have provided insights into the struc-
ture-composition-photoluminescent property relationships in
-SiAlON:Eu2+ [59], one of the most promising narrow-band green
phosphors for high-power light-emitting diodes and liquid crystal dis-
play back-lighting with wide color gamut. We showed that reducing
oxygen content is a pathway to reduce red shifting and achieving nar-
rower band emissions, predictions which have independently been
confirmed by experiments [60].
2.3. Molybdenum and its alloys
Mo and its alloys are known for their high stiffness, low coefficient
of thermal expansion and the ability to maintain excellent mechanical
properties under extreme temperatures [61]. This makes them well
suited for use in harsh environments such as those found in aerospace
engineering, defense applications and nuclear power plants. However,
their wider applicability is limited by their intrinsic brittleness due to
their fragile grain boundaries (GBs) under room temperature [62,63].
Introducing dopants and secondary “getter” phases are common ap-
proaches to address these limitations.
We have performed a large-scale DFT study of 29 metallic dopants
in the 5 (310) tilt and 5 (100) twist Mo GBs [64]. We have demon-
strated that segregation preference between different GBs was due to
the strain effect of the dopants and segregation site. The smaller seg-
regation site of the twist GB will better facilitate segregation of smaller
dopants. We also demonstrated that previous empirical continuum
models such as the McLean [65] and Miedema [66] do not account for
the effects of intermetallic compound formation between the dopants
and host material. Furthermore, Ta, W, Re and Os were predicted to
strengthen the 5(310) tilt Mo GB while dopants such as Bi acted as GB
embrittlers, which is in agreement with previous experimental ob-
servations [67]. Using multilinear regression, we have successfully
modelled the GB strengthening energy as a function of the dopant strain
and cohesive energy.
Most practical applications of Mo involves the use of its inter-
metallic compounds such as MoSi2, which has a melting temperature up
to 2030 °C and excellent oxidation resistance [68]. Despite its out-
standing refractory properties, MoSi2 is brittle at intermediate tem-
peratures (400–600 °C) due to the oxygen short-circuit diffusion at the
GB [68,69]. Alloying with Zr has been shown to improve the ductility of
Mo-based host materials [70–73]. Through the use of GB and interfacial
models, we have shown using DFT calculations that the most effective
strengthening mechanism of Zr in MoSi2 is as “getter” nanoparticles
[74]. While Zr dopants somewhat mitigate the embrittling effect of
oxygen interstitials, a Zr secondary phase nanoparticle has a strong
affinity for parasitic oxygen (see Fig. 3(a)). This getter effect sig-
nificantly increases the work of separation of the GB. Based on these
findings, we have also developed a simple and effective screening ap-
proach to identify other potential getter materials for MoSi2(Fig. 3(b))

Fig. 3. (a) The relationship between the position of interstitial oxygen and relative energy. The energy of Oint in bulk-like MoSi2 is set as a zero reference. (b) Two
descriptors: silicate formation energy and oxygen exchange reaction energy, are used to assess the viability of 55 elements as getter materials. The regions are labeled
as follows: I: oxygen exchange reaction favored and silicate formation energy is lower than Zr; II: oxygen exchange reaction favored and silicate formation energy is
higher than Zr; III: oxygen exchange reaction not favored but silicate formation energy is negative. Reproduced with permission from [74].

146
S.P. Ong
which can be readily extended to other systems.
Our results have provided highly useful insights into the mechan-
isms behind the enhancement of mechanical properties of Mo and its
alloys due to atomic dopants and getter materials and will serve as a
guide towards the design and optimization of similar materials.
3. Beyond DFT scale, at near-DFT accuracy
A fundamental challenge in computational materials science is the
trade-off between scale (length and time), accuracy and transferability.
Today, empirical potentials can access reasonable length (> nm) and
time ( µ s) scales but are neither transferable across chemistries nor
especially accurate. Quantum mechanical calculations, such as those
based on DFT, are transferable and accurate but are too computation-
ally demanding for large systems and/or long time scales and/or large
chemical spaces. In the Materials Virtual Lab, we aim to address this
“scale challenge” by developing accurate potential models that scale
linearly with number of atoms, as well as property prediction models
that enable rapid screening across vast chemical spaces using machine
learning.
3.1. Quantum-accurate, linear scaling potentials
We have developed highly accurate Spectral Neighbor Analysis
Potential (SNAP) [75,76] models for various metals (Mo, Cu, Ni) and
alloys (Ni-Mo) [77,78]. The starting point is a robust description of the
local environments in a system of atoms that satisfies rigorous in-
variances under translation, rotation, and permutation of homonuclear
atoms and is unique and differentiable [79]. In the SNAP model, the
energies and forces are expressed as a linear function of the coefficients
of the bispectrum built from the four-dimensional spherical harmonic
expansion of the local 3D atomic density (see Bartók et al. [79] for
details). The simple formalism reduces the potential for over-fitting
compared to more complicated models and is expected to be more
generalizable. Using automated workflows developed using pymatgen
[3] and fireworks [4], we have generated accurate and consistent DFT
datasets for our systems of interest, which include elastically distorted
structures, vacancy structures, surfaces and grain boundaries, and
snapshots from AIMD simulations [77,78]. The models are then trained
to reproduce desired properties, e.g., elastic constants, with a feedback
look that optimizes model hyperparameters using a differential evolu-
tion global optimization scheme. We have developed an open-source
materials machine learning python package called veidt [80] that is
freely available to the research community. We have also published our
fitted SNAP models in a Github repo at https://github.com/
materialsvirtuallab/snap.
In general, the SNAP models for bcc Mo, fcc Ni, fcc Cu and Ni-Mo
binary systems significantly outperform current state-of-the-art em-
bedded atom method (EAM) and modified embedded atom method
(MEAM) empirical potentials. Not only are the mean absolute errors
(MAEs) lower for energy and force predictions, the SNAP models also
yield more accurate elastic constants, phonon dispersion curves,
equations of states, melting points and surface energies [77,78]. An
especially stark result can be seen in Fig. 4, where the Ni-Mo SNAP
model was used in a hybrid Monte-Carlo/Molecular Dynamics (MC/
MD) simulation of the Ni-Mo phase diagram. While the EAM potential
fails to achieve even qualitative agreement with the experimental phase
diagram, the SNAP model is able to reproduce the correct solubility
limits of Ni in Mo, the concave liquidus line and the almost-overlapping
liquidus and solidus lines at the Ni-rich portion of the phase diagram
near the melting point of Ni. We believe that such models, which are
about five orders of magnitude cheaper than DFT calculations and
linear scaling with respect to the number of atoms, will be an important
147
Computational Materials Science 161 (2019) 143–150
Fig. 4. High-temperature Ni-Mo phase diagram from experiments [81], CAL-
PHAD [82], SNAP, and EAM models. Reproduced with permission from Ref.
[77].
enabler to high accuracy studies of microstructure and other phe-
nomena requiring large-scale simulations over long-time scales.
3.2. Property prediction
Predicting stability is usually the first step in any materials dis-
covery, and the formation energy of a crystal is typically the metric by
which stability is determined. Though DFT calculations have proven to
be effective in estimating formation energies [83,84], they remain far
too computationally expensive to traverse large combinatorial chemical
spaces. It is therefore unsurprising that there have been substantial
efforts in the development of machine learning models to predict for-
mation energies [85–89].
In the Materials Virtual Lab, we have recently developed deep
neural network models [90] that are able to predict the DFT formation
energies of garnets and perovskites to within 7–34 meV/atom accuracy
(see Fig. 5), a substantial improvement over prior efforts [91]. To
overcome well-known limitations of DFT calculations in handling redox
reaction energies [92], we propose the formation energy from the
binary oxides as the appropriate target for a machine-learning model.
Starting from a chemically-intuitive hypothesis that a quantitative re-
lationship exists between the electronegativity and ionic radius of the
species on each symmetrically distinct site, we trained deep neural
networks to model that relationship using the DFT calculated formation
energies on thousands of unmixed and mixed garnets and perovskites.
We have shown that these models can be used to classify stable/un-
stable garnet and perovskite compositions with >80% accuracy. A
particularly important feature of our work is the extension of these
neural network models beyond simple garnets and perovskites to mixed
compositions with negligible increase in prediction error, which greatly
expands their applicability of the vast combinatorial chemical spaces
for discovery of novel technological materials. It is our belief that si-
milar approaches can be applied to develop accurate machine learning
models for prediction of other functional properties (e.g., band gap,
mechanical properties, etc.), potentially enabling multi-property opti-
mization of materials for a targeted technological application.
4. Accelerating and enhancing materials characterization
Finally, the Materials Virtual Lab aims to enhance the speed and
accuracy of materials characterization by combining automated com-
putations, experimental data curation and ML. Though similar ap-
proaches have been applied in the life sciences [16], the critical bot-
tleneck to the application of similar approaches in materials science is
S.P. Ong Computational Materials Science 161 (2019) 143–150

a b

c d

Fig. 5. Plot of neural network-predicted formation energy E fANN against DFT-calculated formation energy EfDFT for (a) unmixed garnets and (c) unmixed perovskites,
and mean absolute errors (MAEs) in Ef in training, validation, and test sets of all (b) garnet and (d) perovskite models. Mixing is carried out on the 24c (C-mixed), 16a
(A-mixed) and 24d (D-mixed) sites of the Ia3̄d C3A2D3O12 garnet crystal, and the 4c (A-mixed) and 4d (B-mixed) sites of the Pnma ABO3 perovskite crystal. The similar
MAEs for the mixed and unmixed models indicate that the former has learned the effect of orderings on Ef . Reproduced with permission from Ref. [91].

the lack of large, high-quality datasets for the training and development
of models.
We have simultaneously sought to address this data gap, as well as
push the frontiers in developing the application of machine learning
techniques in materials characterization. Using the Green’s function
approach [93,94], we have constructed the world’s largest reference
database of more than 500,000 computed K-edge X-ray absorption near
edge (XANES) spectra for more than 40,000 unique materials [24,25],
and are extending coverage to the extended fine structure (EXAFS) and
L-edges. We have also developed an Ensemble-Learned Spectra IdEn-
tification (ELSIE) algorithm (Fig. 6) that is able to match experimental
spectra with computed ones to identify the coordination environment
and oxidation state with 84% accuracy. These resources and tools
have been made publicly available via the Materials Project [12], and
have garnered substantial interest from users (>2000 spectra requests/
month) and industry.
We are building on these successful, albeit nascent efforts in several
ways. First, we are evaluating alternative approaches to XAS compu-
tations, such as the GW/Bethe-Saltpeter approach [95,96] implemented
in the OCEAN package [97,98], which may yield more accurate spectra,
especially for L edges. Beyond computed data, we are developing a data
platform for the automatic collection and curation of experimental
spectra through collaborations with the Advanced Light Source at
Berkeley Lab and Advanced Photon Source at Argonne National Lab.
We are developing ML models that can significantly outperform hu-
mans in terms of both speed and accuracy in the interpretation of
materials spectra and images (e.g., X-ray, neutron, electron). It is our
belief that such approaches will complement continued advances in
instrumentation, especially in in operando studies and artificial in-
telligence-guided design of experiments.
5. Conclusion
To conclude, we believe that machine learning will have a trans-
formative impact on the conduct of materials science, once critical is-
sues with regards to data quality and availability are addressed. In the
Materials Virtual Lab, we aim to address the data gap through high-
throughput DFT computations and experimental data curation, enabled
by the development of robust software frameworks for the automation
of simulations [3–5]. By machine learning large materials datasets, we
have developed models that allow us to better predict novel materials
and rapidly compute their properties, to access time/length scales and
chemical spaces beyond the current capabilities of DFT, and to out-
perform humans in the interpretation of characterization. It is our hope
that further developments in these areas will fuel an acceleration in the
study and discovery of materials for various technological applications.

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S.P. Ong Computational Materials Science 161 (2019) 143–150

(NSSEFF) under Office of Naval Research (ONR) Grant No. N00014-

15-1-0030 (doping in Mo and MoSi2);
Identify
Absorption Database • NSF Ceramics under Grant No. 1411192 (phosphors for solid-state
lighting);
Species • ONR Young Investigator Program (YIP) under Award N00014-16-1-
2621 (interfaces in all-solid-state batteries and SNAP models for Mo,
fcc metals and Ni-Mo alloys);
• NSF Data Infrastructure Building Blocks (DIBBS) under Award
Number 1640899 (X-ray absorption spectroscopy database and
matching algorithms).

Computation resources were provided by the Triton Shared

Computing Cluster (TSCC) at the University of California, San Diego,
the National Energy Research Scientific Computing Center (NERSC),
and the Extreme Science and Engineering Discovery Environment
(XSEDE) supported by National Science Foundation under Grant No.
Learner 1 Learner N ACI-1053575.
Peak Shifting / Peak Shifting /
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• NorthEast Center for Chemical Energy Storage (NECCES), an Energy

Frontier Research Center funded by the U.S. Department of Energy
(DOE), Office of Science, Basic Energy Sciences under Award #
DESC0012583 (multi-electron cathodes);
• National Science Foundation (NSF) Designing Materials to
Revolutionize and Engineer our Future (DMREF) program under
Grant No. 1436976 (solid-state electrolytes);
•
U.S. DOE, Office of Science, Basic Energy Sciences under Award
DESC0012118 (anti-perovskites);
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