Materials & Design 210 (2021) 110037

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Materials & Design

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Machine learning assisted empirical formula augmentation

Bin Xiong a, Xinpeng Zhao a, Yunfeng Hu a, Haiyou Huang a,b,⇑, Yang Liu c, Yanjing Su a,b,d
a
Institute for Advanced Materials and Technology, University of Science and Technology Beijing, Beijing 100083, China
b
Beijing Key Laboratory of Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China
c
Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
d
Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing 100083, China

h i g h l i g h t s g r a p h i c a l a b s t r a c t

We have proposed an augmentation

strategy for empirical formula based
on machine learning mothed.

A novel empirical formula of Ms as
the function of compositions was
fitted based on an augmented dataset
combined experimental data with
predicted data.

Compared with previous empirical
formula, the accuracy and robustness
of the novel empirical formula we
proposed was significantly improved
without additional experimental cost.

This strategy offers a recipe to build
empirical formula based on a small
experimental dataset.

a r t i c l e i n f o a b s t r a c t

Article history: Tuning the martensite transformation temperature through composition design has become an impor-
Received 27 May 2021 tant way to broaden the applicable temperature range of shape memory alloys (SMAs). The empirical for-
Revised 23 July 2021 mula based on traditional statistics is a key reference for composition design. Due to the lack of
Accepted 8 August 2021
experimental data, a large deviation may exist among the prediction results from the empirical formulas
Available online 10 August 2021
obtained by different data sources. In present work, we proposed an augmentation strategy of empirical
formula based on a machine learning method to build the relationship between martensite transforma-
Keywords:
tion start temperature (Ms) and compositions in Cu-Al-based SMA system. A series of ML models were
Shape memory alloy
Machine learning
established by physical and chemical features and a Gaussian radial basis kernel function support vector
Empirical formula machine (SVR.rbf) model was screened out based on mathematical and domain knowledge criteria. An
Transformation temperature augmented empirical formula of Ms as the function of compositions was fitted based on the abundant
Composition design augmented dataset combined experimental data with predicted data by the SVR.rbf model. Compared
with previous empirical formula fitted by small experimental dataset, the accuracy and robustness of
the augmented empirical formula was significantly improved without additional experimental cost.
This strategy offers a recipe to build empirical formula based on a small experimental dataset.
Ó 2021 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).

⇑ Corresponding author.
E-mail address: huanghy@mater.ustb.edu.cn (H. Huang).

https://doi.org/10.1016/j.matdes.2021.110037
0264-1275/Ó 2021 The Authors. Published by Elsevier Ltd.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
B. Xiong, X. Zhao, Y. Hu et al.
1. Introduction
Concluding empirical law from experimental or calculational
data is an important method of scientific research [1]. The accuracy
and applicability of the empirical law is strongly dependent on the
quantity and quality of the data sample. In practical investigation,
we often face low-quality dataset such as insufficient data,
severely skewed distribution and low mergeable data due to col-
lecting from different experimentations with various processing
parameters. A formula fitted by these low-quality data will show
a low accuracy. Improving the quantity or quality of data sample
under a consistent experimental condition is a feasible way to
solve the problem, but it also means high experimental costs.
With the development of materials information, machine learn-
ing (ML) is emerging as a powerful tool for dealing with material
data problems [2]. In addition to dealing with big data, ML has
been successful in small data problems [3]. Data Augmentation is
an effective technique in ML which helps in adding value to base
dataset by adding the gathered information from various sources
to improve the quantity and the quality of data. Data Augmenta-
tion is one of the most important processes that makes the data
more informational.
Shape memory alloys (SMAs) is a kind of important functional
material that has been widely used in sensors, actuators, environ-
mental protection refrigeration and energy conversion equipment
due to its unique shape memory effect and superelasticity [4–7].
The martensitic transformation temperature that determines the
temperature window of SMAs in their applications, is one of the
most important material parameters in material design [8–10].
The martensitic transformation temperatures have strong com-
position sensitivity [11–17]. Therefore, it is a convenient way to
control the martensitic transformation temperatures by composi-
tion design, which also becomes an important way to broaden
the application temperature range of SMAs and to develop
ultralow-temperature or high-temperature SMAs. Consequently,
obtaining the relationship between the martensitic transformation
temperatures and the compositions of SMAs is a key premise to
accurate composition design.
Among lots of SMAs systems, the Ni-Ti-based SMAs are the
most practical systems because of their excellent superelasticity
and shape memory effect, good ductility and good fatigue resis-
tance [18]. Cu-based SMAs, especially Cu-Al-Mn SMAs, on the
other hand, are another promising system because they have high
superelasticity (>10%) [19], high isothermal entropy change (~20 J/
kgK), wide operation temperature window (>100 ℃) [20] as well
as are easy to manufacture and cheaper cost compared to Ni-Ti-
based SMAs. Moreover, Cu-Al-Mn SMAs also show a wide appliable
temperature window (4.2℃~450℃) [20] which can be adjusted by
composition design, which makes it very necessary to obtain an
accurate relationship between the transformation temperatures
and compositions for their industry application. Many researches
Table 1
Empirical formulas of martensitic transformation temperature as a function of composition of Cu-Al-Mn SMAs.
No. Formula Number of experimental data
1 Ms(℃) = 1045.1–18.6Al-72.5Mn(at.%) 7 hot extrusion and heat
2 Ms(℃) = 2023.9–75.9Al-46.8Mn(at.%) 12
3 Ms(℃) = 1616.9–42.1Al-78.0Mn(at.%) 7 as-cast
N1 Ms(℃) = 1292–40.62Al-55.86Mn(at.%) 71
N2 Ms(℃) = 1040–33.30Al-42.90Mn(at.%) 9143*
* Note: it is composed of 9072 prediction data + 71 experimental data.
2
Materials & Design 210 (2021) 110037
have concluded several empirical formulas from their respectively
experimental studies in TiNi-based and Cu-based SMAs. As a sam-
ple, the formulas of martensitic start transformation temperature
(Ms) as a function of the composition in Cu-Al-Mn SMAs [21–23]
were summarized in Table 1 and illustrated in Fig. 1. Fig. 1 indi-
cated that these empirical formulas obtained by different research-
ers show significant differences in the composition space.
In general, an accurate empirical formula needs to be fitted with
sufficient experimental data. However, due to the limitation of
experimental cost, the experimental data used by researchers for
formula fitting is often only a few to a dozen. Collecting more
experimental data from other researchers to increase the total
amount of data may be a simple and feasible solution. However,
the mergeability of the data from different researchers is often
hard to determine easily.
Compared to the traditional data fitting method, the ML model
can not only perform statistical fitting, but also build physically
meaningful relationships by mining hidden information beneath
the data, which is becoming an important and powerful tool for
material discovery and design, even building emerging materials
intelligence ecosystems [24–28].
In the present work, we proposed an empirical formula aug-
mentation strategy based on ML method, as schematically shown
in Fig. 2. Based on published literatures, an experimental dataset
including Ms and compositions (Ci) of Cu-Al-based SMAs was sum-
marized. Two novel empirical formulas were obtained in our work.
The empirical formula N1 was fitted directly based on the summa-
rized experimental dataset, which was in contrast to the aug-
mented empirical formula N2. Along the other way, a ML
surrogate model Ms = f (pi) was built by the use of physical and
chemical features (pi) of the elements as this is known to be closely
related to the transformation temperature. It should be noted that
during the ML model selection process, both the mathematical and
physical (domain-knowledge) criteria were employed to optimize
the best model. Consequently, the optimum ML model was applied
to generate amount of predicted data, which could augment the
experimental data to product an augmented dataset. Then, the
empirical formula N2 was fitted by using the augmented dataset.
At last, the robustness of the empirical formulas was also
discussed.
2. Experimental dataset
The experimental dataset was built based on the SMAs dataset
from MGEData platform [29]. Our dataset used in this work only
selected experimental data from literatures and our group. Consid-
ering the martensitic transformation temperatures of SMAs is not
only affected by the composition content, but also by processing
technology, heat treatment conditions, and aging treatment signif-
icantly [30–36]. Therefore, during experimental data collecting, the
processing status and condition were attention to mark on the
Sample state Range of compositions Ref.
Al: 16.7 ~ 19.3 at.% [21]
treatment @850℃ Mn:11.1 ~ 12.3 at.%
as-cast Al: 21.3 ~ 22.5 at.% [22]
Mn:5.1 ~ 7.5 at.%
Al: 17.1 ~ 18.1 at.% [23]
Mn:11.4 ~ 13.3 at.%
as-cast Al: 16.39～28.30 This work
Mn: 0～11.90
—— Al: 16.39～28.30 This work
Mn: 0～11.90
B. Xiong, X. Zhao, Y. Hu et al.
Fig. 1. Fitting surface diagram of three empirical formulas in component space.
labels of the data. In the process of data screening and cleaning, we
fixed the processing conditions of the data source to the cast sam-
ples that have not been rolled or drawn because we must avoid the
dimensional disaster caused by the variability of processing
parameters. Additionally, the data with the same component hav-
ing different Ms due to suffering different heat treatment processes
are also not selected into our dataset. After the data screening, we
tried to minimize the influence of the processing on the martensite
transformation temperature to ensure that the intrinsic relation-
ship between the martensite transformation temperature and the
composition can be found out. In the end, a total of 71 data from
13 literatures are selected to build the experimental dataset.
3. Machine learning models
Several well-known machine learning models including least
absolute shrinkage and selection operator (Lasso), linear regression
(Lin), polynomial regression (Poly), gradient boosting regression
(GBR), random forest (RF), ridge regression (Ridge) and Gaussian
radial basis kernel function support vector machine (SVR.rbf) were
employed to produce machine learning models.
Fig. 2. A schematic of the empirical formula fitting strategies based on experimental data directly (Route I) and augmented data assisted by ML method.
3
Materials & Design 210 (2021) 110037
The root mean square error (RMSE) score obtained by the leave-
one-out method was used to evaluate the model according to Eq.
(1)
rffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
1 Xm  2
RMSE ¼ yi  ybi ð1Þ
m i1
where m is the number of the data, yi is the true value and ybi the
predicted value. There was 71 data in our experimental dataset.
According to the leave-one-out method, there would be 71 division
methods, and 71 RMSE scores would be obtained after machine
model training. The average value of these 71 RMSE scores was
used to balance the training effect of the model. The leave-one-
out method can obtain as much effective information as possible
from limited data, so that samples can be learned from multiple
aspects and avoid falling into local extremes.
In the process of model training, the Grid Search method was
used to optimize the hyperparameters. After partitioning the data
using the K-CV method, use the partitioned training set to train
the model and use the test set for testing to obtain the model score
under the set of hyperparameters. Train the model and test for
each set of hyperparameters in turn, and finally compare each
set of hyperparameter combination scores, and output the set of
hyperparameters with the best score as the best parameter.
We adopted a combined grid search strategy of coarse adjust-
ment in a large range and fine adjustment in a small range to find
the best parameters, and the model evaluation also returns the
RMSE of the training set and the test set after the ten-fold cross-
validation scoring for model evaluation. The corresponding search
range and step length were determined according to the hyperpa-
rameter characteristics of different machine learning models.
4. Results and discussion
4.1. Empirical formula N1
As shown in Fig. 1, the existing empirical formulas from differ-
ent researchers show significant numerical deviation in the com-
position space, but all of them were linearly fitted, which implied
that a linear relationship between martensitic transformation tem-
peratures and the content of alloying element. This empirical
domain knowledge was also supported by lots of researches in
B. Xiong, X. Zhao, Y. Hu et al. Materials & Design 210 (2021) 110037

other SMAs including Cu-based and Fe-based SMAs based on Table 2

experimental data and thermodynamical model [37–40]. The physical and chemical features used in ML modeling.

Followed above empirical domain knowledge, at first, we lin- Name Description Ref.
early fitted the 71 experimental data using the least square Cu The atomic percentage of Copper
method. The obtained linear formula N1 was shown in Eq.(2) Al The atomic percentage of Aluminum
Mn The atomic percentage of Manganese
Ms( C)=1292  40.62Al  55.86 Mn(at.%) ð2Þ Arc Clementi’s atomic radii [35]
En Pauling electronegativity [36]
In Fig. 3(a) and (b), the four empirical formulas were compared by Ven Valence electron numbers [37]
the deviation between prediction values and true values and RMSE, Mr Metallic radius [38]
respectively. In the deviation graph (Fig. 3(a)), the more concen- Dor Waber-Cromer’s pseudopotential radii [39]
trated the scattered point distribution is near the diagonal line, the Anum Atomic number
Mass Atomic mass
more consistent the predicted value and the experimental measure-
ment value are. However, the smaller RMSE is, the more accurate the
prediction is. It is obvious that formula N1 has more accuracy than
the previous three formulas due to using far more data. tics in SMAs, and provide a relatively simple physical basis or
In addition, according to the distribution of scattered points, the structure–property relationship of phase transition temperature
forecast trend of the empirical formula in the component space can [21]. All of them have been tabulated in Table 2. The features
also be understood. The scattered points of the empirical formula except for the atomic percentage of Cu, Al, and Mn were also called
N1 obtained based on the as-cast data set are concentrated on both initial features.
sides of the diagonal. Except for individual data, the prediction The objects of our experimental dataset are shape memory
effect of Ms value in the range of 150 ~ 200℃ is better, and the alloys, not single elements. The unique mapping relationship
predicted value of Ms in the range of 200 ~ 350℃ is about 70℃ between the component space and the compound feature is con-
lower than the actual measured value. The scattered points of structed by the following five calculation formulas, including: X1
the previous three formulas are mostly distributed on the lower was calculated based on the linear mixing rule; X2 was calculated
right side of the diagonal, indicating that the predicted values based on the reciprocal mixing rule; CX was obtained based on
given by the three formulas tend to be higher than the true values. the ratio of each feature X1 to the atomic number of each alloy;
XD and Xd were the deviation and discrepancy, respectively. In each
calculation formula, f Cu , f Al and f Mn represent the atomic percent-
4.2. Empirical formula N2
age. X Cu , X Al and X Mn represent the corresponding features of each
In the above strategy, it is obvious that data augmentation can element, and Z Cu , Z Al and Z Mn represent the atomic number of each
significantly improve the accuracy of empirical formula. Can we element.
break through the limitations of experimental data and further
X 1 ¼ f Cu X Cu þ f A lX Al þ f Mn X Mn ð3Þ
improve the usability of the formula? Therefore, we employ
machine learning model based on physical and chemical descrip-  1
tors that are also related to the transformation temperatures of X 2 ¼ f Cu =X Cu þ f Al =X Al þ f Mn =X Mn ð4Þ
SMAs.
In previous researches, Frenzel et al.[41] indicated that the geo-
f Cu X Cu þ f A lX Al þ f Mn X Mn
metric change during phase transition and the inherent instability CX ¼ ð5Þ
of the parent phase are two key factors to control the phase tran- f Cu Z Cu þ f A lZ Al þ f Mn Z Mn
sition temperature, and the latter is related to the electronic struc- rffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
 2  2  2
ture. Sampath et al. [31] evidenced that the addition of alloying
XD f Cu X Cu  X 1 þ f Al X Al  X 1 þ f Mn X Mn  X 1 ð6Þ
elements (aluminum, iron, zinc, silicon) would reduce the EV/a
ratio, thereby reducing the Ms. Therefore, the features we used vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
u !2 !2 !2ffi
include: Clementi’s atomic radii (Arc) [42], Pauling electronegativ- u X Cu X Al X Mn
ity (En) [43], metal radius (Mr) [44], valence electron number (Ven)
t
X d f cu 1  þ f Al 1  þ f Mn 1  ð7Þ
X1 X1 X1
[45], and Waber-Cromer pseudopotential radius (Dor) [46]. These
features represent the electronic, bonding and radius characteris-

Fig. 3. The predicted values as a function of the experimental values (a) and RMSE (b) comparison of four empirical formulas fitted by experimental data.

4
B. Xiong, X. Zhao, Y. Hu et al.
The physical features were calculated by the above five calcula-
tion formulas, and the three composition features were combined
to obtain the feature pool with a total of 37 descriptors.
The candidate feature (pi) is the input of the property (Ms)
required by the machine learning model to predict, that is, Ms = f
(pi). For a given target attribute Ms, there will be a corresponding
combination of pi to ensure that the trained machine learning
model has better performance. When faced with a comprehensive
coverage of pi, through feature selection, ‘‘excellent” features are
selected from the candidate features to achieve the effect of reduc-
ing dimensionality and improving model performance. Due to the
small number of features, we chose a simpler feature selection
route.
At the first step, a correlation analysis was employed to perform
feature selection to reduce the computation time and improve
model robustness by removing the redundant features. Fig. 4 indi-
cates the Pearson correlation coefficient map between different
features. Those with a correlation coefficient>0.95 were considered
as highly correlated. After the analysis of Pearson’s correlation
coefficient, a total of 9 features including En, Dor, Mass, Arc-2,
En-D, Mass-D, Mr-D, Mr-d and Mass-d were screened and listed
in Table 3.
Then, the RMSE scores of each feature subset were compared by
the method of feature exhaustion and the one with the highest
score was used for model training. All machine learning models
performed feature exhaustion evaluation and the results are
shown in Fig. 5.
Fig. 5 shows the deviation between the predicted values and
experimental values and the RMSE scores of the seven machine
learning models. Among them, the SVR.rbf model has the best per-
formance, with a test RMSE of 53.
In the process of feature exhaustion, we found that the RMSE
scores of lots of feature subsets are similar. Considering the exper-
imental data are imperfect and possible overfitting problem, only
relying on mathematical criterion may not be enough. In the previ-
ous review and discussion, we have concluded an important
domain knowledge that is a linear relationship between marten-
sitic transformation temperatures and the content of alloying ele-
ments. Therefore, we can evaluate the SVR.rbf models using
combined criterion with mathematical and physical (domain
knowledge) criteria. In the Cu-Al-Mn system, the linear relation-
ship between martensitic transformation temperatures and the
Fig. 4. The Pearson correlation map of the 37 features.
5
Materials & Design 210 (2021) 110037
Table 3
Feature selection result based on Pearson correlation coefficient.
No. Feature name
1 En
2 Dor
3 Mass
4 Arc-2
5 En-D
6 Mass-D
7 Mr-D
8 Mr-d
9 Mass-d
content of alloying element means the Ms values should distribute
on a plane in the composition space. Therefore, we not only exam-
ine the RMSE scores of the exhaustive feature subsets, but also pay
attention to whether the model is more consistent with the ‘‘one
plane” criterion for the component spatial prediction data, which
is called ‘‘RMSE + one plane” criterion method.
In this criterion method, on the one hand, the average value of
the test set RMSE score of the exhaustive feature subsets using
leave-one-out method were called RMSE_math. On the other hand,
a SVR.rbf model built by a feature subset was used to predict the
pre-divided component space, and then linearly fit the prediction
data as a function of the Al and Mn atomic percentages. The RMSE
of the linear fitting to the prediction data was called RMSE_phys as
the evaluation indicator for ‘‘one plane” criterion. It should be
noted that all physical and chemical features (37 descriptors) were
used to train the SVR.rbf model in order to avoid the omission of
feature subset under the multiply criterion condition.
A virtual composition space was built according to composition
range of experimental data, that is Cu: 66.68 ~ 76.21, Al:
16.39 ~ 28.30, Mn: 0 ~ 11.90. The virtual composition space was
divided into 9143 alloy composition points, in which the Ms values
of 9072 alloy compositions were unknown. At first, the top 40
models according to RMSE_math criterion were selected and their
RMSE_math scores illustrated as the red curve in Fig. 6. And then,
the 40 models were evaluated by RMSE_phys criterion and their
RMSE_phys scores were marked green curve in Fig. 6.
Fig. 6 indicates that the RMSE_math scores of the first to fortieth
SVR.rbf models are in the range of 52 ~ 59, but the fluctuation of
the RMSE_phys scores are very significant. The maximum and
the minimum values are 89 and 27 respectively, which implies that
the various models with the similar mathematical scores may have
a significant deviation of the data distribution in the prediction
space. In order to clarify this issue, we use the 25th model and
the 26th model in Fig. 6 as examples. The 25th model with two fea-
tures (Dor, cVen) shows low scores both of RMSE_math (57) and
RMSE_phys (26). The RMSE_math score difference between the
25th model and the 26th model (cVen, En-2) is only 0.11 and they
also have one common feature (cVen), but the RMSE_phys score
difference between them is 62.75.
The distribution of Ms values predicted by the 25th and 26th
models. It can be seen in Fig. 7(a) the contour distribution is rela-
tively smooth, and Ms values show a monotonous change trend
with the variation of the Al and Mn contents. On the contrary,
the Ms values in Fig. 7(b) show two local low temperature areas,
which is not consistent with actual experience.
For the ML modeling, when the amount of training data is small
or there is large error in training data, several local optimal solu-
tions could be obtained. All of them may have excellent RMSE
scores, but do not necessarily mean the real physical lawn. There-
fore, the introduction of domain knowledge (physical) criterion can
effectively help us to screen out the ML model with physical
meaning.
B. Xiong, X. Zhao, Y. Hu et al. Materials & Design 210 (2021) 110037

Fig. 5. The predicted values as a function of the experimental values (a)-(g) evaluated by the leave-one-out method and the RMSE scores (h) for seven ML models.

6
B. Xiong, X. Zhao, Y. Hu et al.
Fig. 6. RMSE_math and RMSE_phys scores of the top 40 SVR.rbf models ranked by
RMSE_math.
Finally, a SVR.rbf model with two physical features of Dor and
cVen was trained and used to predict the Ms values in the virtual
composition space. An augmented linear empirical formula N2 of
Ms as the function of composition was fitted by the combined
dataset including predicted Ms values and experimental data, as
shown as follows
Ms( C)=1040-33.30Al  42.90Mn(at.%)
4.3. Generalization of empirical formula based on the ML model
The machine learning model based on physical features was
used to predict the composition space with unknown Ms value,
and an augmented dataset combined the predicted data and the
experimental data was linearly fitted to obtain empirical formula.
This strategy not only augments huge amounts of data to high-
cost experimental data to solve the problem of insufficient data,
but also combines physical features and domain knowledge so that
the resulting empirical formula contains more information of
physical characteristics.
Another advantage of ML model built on physical features is
good generalization ability. In other words, the ML model builds
a relationship between the target property and physical factors
Fig. 7. The distribution heat map of Ms values predicted by the 25th (a) and 26th (b) ML models in composition space.
Materials & Design 210 (2021) 110037
which touches the inherent mechanism of the property in this
material system. Therefore, the obtained ML model can break
through the limitation of formula fitting based on single statistical
method, such as the constraint of component space.
Taking this advantage, more experimental data from other Cu-
Al-based SMAs were supplements collected from 19 published lit-
eratures [31,47–65]. The supplementary experimental dataset
included 77 data from 16 alloys and involved a total of 16 ele-
ments. If we use these 148 data (71 data for Cu-Al-Mn SMAs and
77 data for other Cu-Al-based SMAs) to fit a formula or build a
composition feature-based ML model of Ms as the function of com-
positions, a serious dimensional disaster will occur due to a huge
ratio of the number of features and the amount of data. However,
the physical feature-based ML model allows to expand the number
of elements by increasing the dimensions of prediction compo-
nents space, rather than increasing the model feature variables.
Based on the ML model of Cu-Al-Mn alloys obtained above, the
77 supplementary experimental data was used to fit the coefficient
of each element in linear formula. The obtained empirical formula
for multicomponent Cu-Al-based SMAs is as follows:
Ms( C) = 1040  33.30Al  42.90Mn  107.73Cr
 190:26Ni  138:28Si  61:07Zn þ 240:87Ti  327:59Nb
 1349:83Be  167:1Mg  187:08Fe þ 119:3Vðat:%Þ
ð9Þ
It should be clarified that the coefficient fitting for each element
was conducted one by one. In addition, the multicomponent
empirical formula is available when the content of each alloy’s ele-
ð8Þ ment is less than 3.5at.%.
5. Summary
In present work, we have proposed an augmentation strategy
for empirical formula based on ML mothed. The implicit relation-
ship between the target property and physical and chemical
descriptors including those associated with the elements is estab-
lished through an ML algorithm. Based on the ML model, a huge
amount of data could be obtained via prediction of the target prop-
erty of unmeasured compositions in a virtue composition space.
The predicted data can significantly solve the small data issue
due to insufficient experimental data. We have demonstrated this
augmentation strategy on the Cu-Al-based SMAs. A novel empirical
formula (empirical formula N2) of Ms as the function of composi-
tions was fitted based on an augmented dataset combined experi-
7
B. Xiong, X. Zhao, Y. Hu et al.
mental data with predicted data. Compared with previous empiri-
cal formula fitted by small experimental dataset, the accuracy and
robustness of empirical formula N2 was significantly improved
without additional experimental cost. This framework can also
be extended to establishing empirical relationships in other mate-
rial systems, especially in emerging material systems, which often
face the similar difficulties of insufficient experimental data.
6. Data availability
The raw/processed data required to reproduce these findings
can be obtained by contacting the corresponding author.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgements
This research was funded by the Guangdong Province Key Area
R&D Program (Grant No. 2019B010940001), Guangdong Major
Project of Basic and Applied Basic Research (Grant No.
2019B030302011), the National Key Research and Development
Program of China (Grant No. 2018YFB0704300,
2020YFB0704504), and Scientific and Technological Innovation
Foundation of Shunde Graduate School, USTB (BK19BE030).
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