Dendritic Pattern Prediction
Dendritic Pattern Prediction
Energy and AI
journal homepage: www.sciencedirect.com/journal/energy-and-ai
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
A R T I C L E I N F O A B S T R A C T
Keywords: Electrodeposition in electrochemical cells is one of the leading causes of its performance deterioration. The
Electrodeposition prediction of electrodeposition growth demands a good understanding of the complex physics involved, which
Electrochemical cell can lead to the fabrication of a probabilistic mathematical model. As an alternative, a convolutional Long short-
Deep learning
term memory architecture-based image analysis approach is presented herein. This technique can predict the
Data-driven modelling
Convolutional long short-term memory
electrodeposition growth of the electrolytes, without prior detailed knowledge of the system. The captured
images of the electrodeposition from the experiments are used to train and test the model. A comparison between
the expected output image and predicted image on a pixel level, percentage mean squared error, absolute per
centage error, and pattern density of the electrodeposit are investigated to assess the model accuracy. The
randomness of the electrodeposition growth is outlined by investigating the fractal dimension and the interfacial
length of the electrodeposits. The trained model predictions show a significant promise between all the exper
imentally obtained relevant parameters with the predicted one. It is expected that this deep learning-based
approach for predicting random electrodeposition growth will be of immense help for designing and opti
mizing the relevant experimental scheme in near future without performing multiple experiments.
1. Introduction coating and modification of the surface properties of metal [1]. It is one
of the key processes used in various engineering [2] and scientific ap
Electrolytic deposition is one of the conventional processes for the plications [3]. The method involves the formation of solid metal deposits
* Corresponding authors.
E-mail addresses: [email protected] (H. Hu), [email protected] (M. Chakraborty).
https://doi.org/10.1016/j.egyai.2022.100203
from an ionic solution on the application of an external electric field [4]. complex output results from a set of unknown input data. Recently Attia
The electrodeposition technique is extensively studied for past decades et al [32]. have developed a machine learning methodology to predict a
to explore different morphological variations of the metallic deposits parameter space for maximizing battery cycle life, where they have
[5].The deposits produced by this process can produce a large variety of shown, how this methodology can reduce the optimization cost and time
fascinating shapes [6]. Among all, the tree-like, self-similar, repetitive for experiments by foretelling the final cycle life of the battery. Apart
branched structure observed during the electrodeposition [7], is known from that, Ng et al [33]. have provided a wide overview of machine
as dendritic growth. This is also one of the major concerns pertaining to learning algorithms to predict the state of charge (SOC) and state of
the generation of the consistent energy supply of an electrochemical cell. health (SOH) for the battery management system. Tu et al [34]. used an
This uncontrolled growth is highly undesirable in rechargeable batteries artificial neural network with a physics-based model to predict the state
involving metal anodes [8]. Lithium-ion batteries are extensively stud of lithium-ion batteries. Machine learning techniques are proved to be
ied as a means of energy storage in diverse electronic devices in the past very promising even for predicting the deposition thickness of ZnNi
decades [9]. Conventional Lithium-ion batteries have Lithium interca electroplating [35]. Electrodeposition is an integral part of a battery
lated transition metal oxide cathodes and graphite anodes. The charging (during the charging cycle). The morphological variation of the elec
phase involves the application of an external electric field, and the trodeposits during the charging cycle is completely random and un
Li-ions get transported to the graphite anode. Therefore, electrodepo predictable. Extensive research is still going on to capture the variety of
sition is the fundamental process to carry out the charging phase in a such outgrowing structures during the electrodeposition. This will help
rechargeable battery. Similarly, during discharge, the Li ions again in understanding the dynamic behavior of the deposited growth as well
travel from the graphite electrode to the cathode material. The con as the heterogeneity of the structural evolution [36]. The use of the
ventional graphite-based anode is replaced by Lithium metal due to its real-time experimental frames of growing electrodeposits to predict the
high specific capacity (3860 mAhg− 1). This resulted in a major opera dynamics of the deposition is inadequate. Forecasting the deposition
tional drawback due to the formation of metallic dendrites during the dynamics is tremendously advantageous for experimentalists working in
charging of metal anode-based batteries [10, 11]. These self-repeating the battery industries. For example, with a given set of initial data, the
growing metallic units may form a bridge connecting the two elec time at which the growing unit touches the other electrode to cause
trodes after several charging cycles, leading to a short circuit. Another short-circuit may be foreseen even without performing a trial. This can
factor is the formation of Solid Electrolyte Interface (SEI) [12], which is prevent unwanted damage to the entire circuit. However, a model
an electrically insulating layer that may form when the electrolyte capable of predicting metal electrodeposition is scant in literature. A
molecules come in contact with the lithium metal. SEI is capable of physical model depends upon a lot of measured parameters to predict
passing Li ions but incapable of conducting electricity. Thus, this insu electrolytic growth [11]. Several phase-field based theoretical simula
lating layer covers freshly deposited solid Lithium on the metal anode. tions [37] and mathematical models [38] are present in the literature.
Sometimes, a dendrite can break down at its weaker neck. As a result of Most of the models deal with the physics involved and also include
that, as soon as the Li atoms at the cross-section of the neck are exposed various variables which make the prediction uncertain. Generally, these
to the electrolyte molecules, they get covered with the SEI layer. Thus an models deal with the physics involved behind this random uncontrolled
insulated dendritic structure (‘dead Lithium’) is formed [13], which is growth. Unlike physical models, a machine learning model can work
no longer a part of the electrode surface [14]. This insulated broken part with simple input like images, which is highly advantageous in pre
is known as Columbic loss [15]. The ‘dead Lithium’ accumulated over dicting the dynamics of a rapidly changing system like self-driving cars
the electrode surface and may cause extra resistance for any incoming [39]. For example, XGB algorithm [35] is observed to predict electro
Li-ion to participate in the electrodeposition process. This may lead to deposition thickness with a high correlation coefficient. Herein, the
heat generation and even thermal run away[16]. In this context, it is application of the machine learning concept has been shown using
worth paying attention to the other metal anodes like Cu [17], Na [18], real-time experimental frames of growing electrodeposits. It is to be
Zn [19], Ag [20], and Mg [21], which also can procedure dendritic noted that most of the metal anodes (Li, Na, Mg, etc.) used in the battery
deposition in the charging cycle. Investigation of copper electrodeposits industry are highly reactive, and cannot be handled at room temperature
are observed to become the pivot for decades. Schilardi et al [17]. without an inert atmosphere [18,21,40]. As the objective is to predict
investigated the in situ evolution of the growing interface of copper, and the deposition dynamics by image-based ML techniques, a safer metal
the results are validated with the Edward-Wilkinson equation [22]. electrode has been chosen so that a pool of real-time images can be
Schneideret al [23]. investigated the growth front behavior of copper captured easily with clarity. Therefore, to mimic the real scenario, a
electrodeposition using liquid cell TEM by image analysis technique. model Copper-Copper symmetric electrochemical cell has been
Several other experimental studies have also been performed to observe employed due to its availability and ease of handling. Investigation of
the morphological variation of copper electrodeposits at different copper electrodeposits are observed to become the pivot for decades.
overpotentials [24]. It is observed that mostly video microscopy [25] Schilardi et al [17]. investigated the in situ evolution of the growing
and post-experiment image analysis [26,27] are used to determine the interface of copper, and the results are validated with the
nature of the deposition growth pattern [28]. As a result of that, Edward-Wilkinson equation [22]. Schneideret al [23]. investigated the
monitoring of the deposition dynamics is strictly limited to the experi growth front behavior of copper electrodeposition by analysing images
mental time scale and other complex instrument availability. However, obtained from liquid cell transmission electron microscopy (TEM) .
detailed investigations of the effect and the dynamics of the electrode Several other experimental studies have also been performed to observe
position growth beyond the experimental duration are challenging and the morphological variation of copper electrodeposits at different
limited in the literature. Machine Learning (ML) techniques can be overpotentials [24].
utilized to confront this problem and that may revolutionize electro In this study, the real-time frames of electrodeposition on the copper
chemical science [29]. electrode are recorded using a video microscope at 250 frames/s. With
Machine learning is a branch of artificial intelligence (AI), that al the given set of initial data obtained from two different experiments, a
lows a data-driven prediction even without the requirement of the single model is proposed, that can successfully predict the deposition
physical insights of the process [30,31]. Electrodeposition is a complex dynamics for different concentration ranges. It must be stated here that
process that depends on many system variables. To model such complex the choice of the metal electrode has significant effect on the electro
processes, machine learning tools along with process physics are proven deposition mechanism [41]. For instance, a specific metal electrode has
to be helpful. Deep learning and AI-based machine learning methods are unique electrode-electrolyte interaction, self-diffusion barrier [42], and
capable of fitting high-dimensional data or system variables in a mechanical properties of the SEI, which affect the deposition charac
generalized model. The model can be used later for the prediction of teristics [43]. The proposed model herein solely operates with the
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Fig. 1. Schematic representation of the electrochemical cell modified and reprinted from Dhara et al [44]. Two copper wires serve as electrodes. On the application
of voltage, the deposition of metallic copper takes place on the negative electrode. The schematic portrayal of the dendritic electrodeposits is also presented.
Figure not to scale.
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previous study [44], a comparatively uniform deposition was observed 0 to255. These images are normalized and the final pixel value is set in
at a higher electrolyte concentration as compared to the branched the range of 0 to1. Further binary segmentation is performed so that the
dendritic structure at a lower one. Hence, the two representative elec pixel values are either 0 or 1. The normalization and segmentation steps
trolyte concentrations (0.025 M and 0.1 M) are prepared herein to ensure fast training time. For a given sequence of images, vectors are
observe different morphological variations of the electrodeposition generated from the pixel value of images. After the data preprocessing
growth. After inserting the wires in the electrolyte solution, the cuvette step, an appropriate model for sequence learning has to be selected. An
is sealed with parafilm. A potential difference of 6 V is applied to the LSTM-based model is generated with assigned weight to the model. The
electrodes. The entire setup is placed in line with the camera to capture model is then trained and the binary cross entropy loss is monitored.
real-time images of metallic growth. During the training, the model weight is changed to optimize the loss
With the increase in the electrolyte concentration, the nature of the function. In the subsequent iterations, when the loss is reduced, the
dendritic growth changes from highly fractal to dense agglomerated weight is saved. If the weight remains constant through a few predefined
clusters [45]. The growing micro-structures consist of several morpho numbers of iterations, or if a maximum number of iterations is reached,
logical variations, such as dendritic, cauliflower-like, mossy, etc. How the training is stopped.
ever, all of them are lumped considering the randomness, and hereafter The current model consists of 4 stacked convolutional LSTM [51]
termed as dendritic growth. The observation window in the experiments (convLSTM) followed by a batch normalization [52] layer. The model
is kept fixed such that the growing deposits do not cross the vertical parameters like filters and kernel size are adjusted by monitoring the
frame dimension (240 pixels) with time. A set of 5566 images for 0.1 M loss and optimizing the computational cost. Processed image vectors of
and 5905 images for 0.025 M electrolyte concentration is obtained from dimension 100 × 80 × 128 × 1 are fed as input to the model. The input is
the experiments. A sample sequence of the images is presented in Fig. 2a. followed by a 2D–convolutional LSTM layer. Contrary to a normal
All the captured images have a dimension of 640 × 240 px. To reduce LSTM, a convLSTM uses convolutional transform in recurrent and input
the computational cost, all the images are converted (Fig. 2b) to binary transition, which facilitates feature extraction from the images and
images using the Chan-Vese segmentation algorithm [46]. training on 2D image data [53]. A schematic representation of the model
To inspect the presence of redundant and repetitive images in the architecture is depicted in Fig. 4.
sequence, the overall black pixel is calculated for each image. Images of To keep the vector dimensions uniform after the convolution oper
similar nature, where the consecutive frame is indistinguishable with no ation, the padding is kept the same throughout the model. Padding in
significant change in the electrodeposition pattern are removed. This serts a zero in the output vector so that the dimension is consistent with
ensures the model learns the electrodeposition growth pattern and not the input vector. The convLSTM uses tanh as the default activation
the experimental anomaly. The images obtained from the experiments function, which can take large inputs and outputs values in the range of
from both concentrations of electrolytes are used to train the model. [-1,1]. All LSTM units have 40 filters, with a 3 × 3 kernel size. The kernel
All the images are sorted and the image dimension is reduced to 80 × is responsible for extracting the feature map from the image vector. The
128 pixels to decrease the computational cost and speed up the training stride and dropout values are kept as default to avoid the down-sampling
process. The images are stacked and the input and output image vectors of the feature map. Each convLSTM is followed by a batch normalization
of the same dimension are generated. The output vector represents the layer, which helps to deal with the problem of “internal covariate shift”
next sequence of images for a given input image vector. The input and during the training. The batch normalization layer standardizes the
output vectors are shuffled and divided randomly into a train-test set in layer input and helps the model converge faster. The model has a 3D
the ratio of 80:20. convolution layer attached at the end, which extracts important infor
mation from the output of convLSTM layers. The 2D convolution layer
performs a spatial convolution operation using a 2D kernal resulting in a
2.2. Model architecture 2D output, in contrast to a 3D convolution layer, which uses a 3D
cuboidal kernal and produces a 3D output. Using a 3D convolution layer
In the current study, the aim is to understand the future growth on a sequence of 2D images, the temporal feature variation in the input is
image sequence given the current growth pattern. The electrodeposition also captured. The 3D convolution layer is more suitable to extract
growth problem can be fit into the many to many sequence prediction spatiotemporal features from data [54] as it can perform convolution
categories. Recurrent neural networks (RNN) are well known for operations in 3D. Sigmoid activation is used in the 3D convolution layer,
sequence prediction and used for machine translation [47], speech and an output image vector having a pixel value between [0,1] is
recognition [48], time-series forecasting [49], protein structure pre obtained.
diction [50], etc. Basic RNN has an inherent problem of vanishing and The model uses binary cross-entropy loss as a performance matrix
exploding gradient, making it incompatible for training on a large (Supporting Information S2 (Figure S2) as it is easy to compare the
dataset. A special type of RNN such as gated recurrent unit (GRU) and predicted pixel value with an actual pixel value of the binary image. The
long short-term memory (LSTM) provide the solution to extreme model is optimized using the ‘adadelta’ optimizer [55]. Three different
gradient problems by leveraging the information flow control using a callback methods, namely ‘ModelCheckpoint’, ‘TimeHistory’, and ‘Ear
gating mechanism. LSTM has a ‘forget’, ‘input’, and ‘output’ gate lyStopping’ are defined for the model. The ‘ModelCheckpoint’ is used to
structure which decides the important information to be carried in the save the best model weight. The ‘EarlyStopping’ is used with patience
network. value 7. Early Stopping can stop training the model if the performance
Fig. 3 represents the overall process, from collecting the experi matrix shows no improvement for a certain number of epochs. The
mental images to model training. The study starts by capturing experi TimeHistory callback records the history object and determines the time
mental images of electrodeposition growth on copper electrodes. The for each epoch. The model is fitted with a validation split of 0.05 for 50
images are grayscale and have a pixel intensity value in the range of
Fig. 2. (a) Real-time images of the growing electrodeposit for 0.025 M electrolyte concentration (b) Binary images obtained after Chan-Vese segmentation.
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Fig. 3. Flowsheet of convolutional LSTM-based model training prepared using the experimentally obtained image dataset and used for the prediction of the elec
trodeposition growth.
epochs on the bridges 2 GPU partition. A schematic of the entire algo difference of the pixel intensity value as presented in Eq. (1) where, Aij
rithm is presented in Fig. 5 for an improved understanding. and Bij represent pixel values at coordinate i, j in the compared images of
A and B. Black pixel and white pixel values have gray values of 0 and
3. Results and discussion 255.
( ) ( ) (∑ i=P ∑j=Q
)
100 1
Once the model is prepared, it is then trained on the electrodeposi %MSE = × × 2 2
Aij − Bij (1)
65025 P×Q
tion growth image dataset obtained for 0.025 M and 0.1 M electrolytic i=0 j=0
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Fig. 4. Model architecture of the convolutional LSTM (a) with corresponding input-output vector size across the different layers of the model (b) with layers
including the number of filters, kernel size, padding, and activation function details.
0.025 M electrolyte concentration. ratio [59] of the growing electrodeposits, which can be one of the other
physical properties of the electrodeposits is not considered herein. The
reason behind this is essentially the real-time 2D images captured from
3.2. Absolute percentage error the experiments. In the experimentally obtained 2D real-time images,
the number of pores captured (white pixels surrounded by black pixels)
After comparing the pixel level correlation between the experiment inside the intricate compact structures of growing deposits is likely to be
and predicted images, the percentage difference in the experimental and erroneous. As the images are 2D and a growing unit that is exactly rising
predicted image area is calculated. The area of any image is determined behind another dendritic unit, will block the visibility of the pores of the
by counting the black pixel of the image. The absolute percentage error structure at the front. To characterize this exceedingly random struc
metric represents the percentage dissimilarity between the area of the tural progression, the definition provided by Saab and Sultan [60] is
predicted and experimental image. Mathematically the absolute per followed to determine another parameter, hereafter termed Pattern
centage error is represented in Eq. (2) as, Density.
⃒ ⃒
⃒Areaexperimental − Areapredicted ⃒
Absolute percentage error = 100 × ⃒⃒ ⃒
⃒ (2)
Areaexperimental
3.3. Pattern density
Fig. 8 represents the variation of the absolute error (%) for different
concentrations of electrolyte with time. At the beginning of the experi Pattern Density is defined as the percentage area covered by the
ment, when the dendritic area is less due to limited deposition, a rela electrodeposits (number of the black pixel as the percentage of the total
tively higher absolute error percentage is observed for both the number of pixels of the image concerned). Therefore, the transient
electrolyte concentration. With the increase in the dendritic area as the variation of pattern density (%) depicts the kinetic evolution of the
experiment proceeds, the absolute error percentage declines. This growing front. Once the model is trained, it is used to predict the output
demonstrates that the model prediction becomes extremely precise as sequence made from the input sequence of all the experimental images.
the experiment progresses. The relatively less accurate prediction at the The predicted images can be compared with the next sequence of
very early stage of the experiment is may be attributed due to the smaller experimental images to get the accuracy of the model. Predicting the
electrodeposition area and higher growth rate. Overall, it is observed whole sequence helps to visualize the electrodeposition growth area
that the growth rate is higher during the initial phase [44], and the with time. The pixel area measures the similarity between two images
dynamic evolution of metal deposits is highly irregular. The mesopore based on an aggregated value. The detailed calculation of pattern
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Fig. 5. Algorithmic representation of the process from experimental images to predicted images for the prediction of near future electrodeposition growth using the
convolutional LSTM model.
Fig. 6. Image sequence of the electrodeposition (a) From experiment for 0.025 M electrolyte concentration; (b) model predicted image sequence with time for 0.025
M electrolyte concentration.
density is presented in Supporting Information S5. between the pattern density of the experimental and predicted images
Fig. 9(a) and 9(b) represent the percentage of experimental and for both 0.025 M and 0.1 M electrolyte concentrations is found to be less
predicted electrodeposition growth for different concentrations. than 1, as presented in Supporting Information S6 (Figure S3). The
Initially, the electrodeposition growth shows a rapid increase, and with average error in pattern density percentage prediction for 0.025 M and
time a gradually decreasing trend is observed. With the increase in the 0.1 M electrolytic concentration is found to be 2.3 and 1.3% respec
electrolytic concentration, the grain size of the deposit rises, and a tively. The pattern densities for predicted and experimental images for
transition from fractal to bulk shape crystal is observed [21]. Due to the both concentrations show a similar trend and are barely distinguishable.
large crystal size in 0.1 M electrolyte concentration, the growth appears This shows the capability of the model to perfectly learn the underlying
to be uniform and changes gradually as compared to the occurrence with recurrent relationship of temporal growth of dendrites with concentra
0.025 M electrolyte concentration. The root mean square error (RMSE) tion as a parameter. The pattern density shows a similar trait as found by
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Fig. 7. Percentage mean square error by comparing the images obtained from the experiments with the model predicted one, for (a) 0.025 M, and (b) 0.1 M
electrolyte concentration.
Fig. 8. Percentage absolute error by comparing the calculated area obtained from the experimentally obtained images with the model predicted one for (a) 0.025 M
electrolyte concentration; (b) 0.1 M electrolyte concentration. (BP: Number of black pixels, WP: Number of white pixels).
Fig. 9. Pattern density percentage obtained by comparing the black pixel percentage, for the electrolyte concentration of (a) 0.025 M and (b) 0.1 M.
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dendritic peak height calculation, using molecular simulation [61]. It dimension is considered herein to further comprehend the fluctuations
must be stated here that though pattern density successfully determines of the electrodeposits. Fractal dimension is a commonly used method to
the 2D deposition area of a specific frame, the characterization of the represent torturous surfaces [64].
surface undulation over the time experimental span (Fig. 2, from flat
interface to extremely irregular topology) is unresolved. Therefore, to
explore it, the transient variation of the length of the growing interface is 3.5. Fractal dimension
calculated and hereafter indexed as the interfacial length.
The fractal dimension is based on the idea that the detail of a pattern
varies when the scale of measurement changes. The fractal dimension
3.4. Interfacial length can be understood as the space-filling capacity of any pattern. Hence, it
is important to understand the electrodeposition growth [65].
The electrodeposition results in uneven growth in random directions. Geometrically, fractals are irregular complex structures that may have
The interfacial length can be defined as the overall length of the repeating substructures. Fractal dimension (D) is used to characterize
enclosure surrounding the electrodeposit growth interface (see Sup the complexity of a fractal, where complexity depends upon surface
porting Information S7 (Figure S4) for details). To calculate the inter detail and scale of measurement. In a fractal having N self-similar
facial length, images obtained from the experiments are binary shapes, and a scaling factor of ε, the fractal dimension D is defined
segmented using a threshold value of 127 using the OpenCV (cv2) and presented in Eq. (3) as,
threshold function. This resulted in a conversion of the grayscale image
logN
to a binary image. All the contour hierarchies in the image are found logNε = − D = (3)
log ε
using the findContour function using chain approx as a parameter [62].
FindContours function detects the change in image color and marks the Various approaches like the Richardson method [66] and the
point as a contour point. Chain approx is a way to store the coordinates box-counting method [67] are used to calculate the fractal dimension.
of the endpoints among all contour points which are in a straight line. The box-counting method is used to find the fractal dimension of com
The perimeter of the contour is found using the arcLength [63] function plex shapes and is currently employed in this study. In the box-counting
in OpenCV. The arcLength function takes the points which are given out method, 2 grids of different scales are used and the number of grid boxes
by the findContour function and calculate the distance between containing the image is counted [68]. For the grid counting method
consecutive contour points as the sum of the square of the coordinates of using 2 scales εa and εb, the fractal dimension is presented in Eq. (4) and
the points. defined as [68]
An interfacial length variation of the electrodeposits with time, is
logNa − logNb
presented in Fig. 10. For 0.1 M electrolyte concentration (Fig. 10(b)), the − D= (4)
logεa − logεb
interface length increases continuously and reached a maximum value
with time. It is observed that for 0.025 M electrolyte concentration Where Na and Nb are the numbers of the box containing the image.
(Fig. 10(a)), the interfacial length increases with time, and then reaches Fig. 11(a) depicts the fractal dimension for the experimental and
a peak near 5.5 s. This peak represents maximum random electrodepo predicted images obtained for the electrodeposition growth at 0.025 M
sition growth. From the figures in Fig. 10, it is clear that the deposition electrolyte concentration. The fractal dimension calculated from the
results in tree-like structures which are responsible for high interfacial images increases and reaches a maximum before starts declining, which
length. With time, the tree-like structure merges, resulting in a decrease suggests that the electrodeposition rises and has a highly irregular
in the interfacial length as can be observed from the experimental and structure during the electrochemical reaction. The fractal dimension
predicted images in the inset. The average RMSE between the experi shows an irregular trend after 10 s, which may be attributed to the
mental and predicted images are found to be 44.4 and 30.3 for 0.025 M inconsistent electrodeposition growth. Fig. 11(b) presents the fractal
and 0.1 M electrolyte concentrations respectively. A more detailed dy dimension for the electrodeposition growth at 0.1 M electrolyte con
namic analysis of the RMSE is presented in Supporting Information S7 centration. Initially, it shows an overall rising trend followed by a minor
(Figure S5). The average error in the prediction of interfacial lengths is change as the experiment progresses. This suggests that the electrode
observed to be 10.7 and 9.2% for 0.025 M and 0.1 M electrolytic con position growth in 0.1 M concentration is more consistent as compared
centration respectively. Though the interfacial length perfectly de to 0.025 M concentration. The model predicts the fractal dimension with
scribes the interface fluctuations, another parameter namely the fractal a 2.9% and 4.3% average deviation from the experimentally obtained
Fig. 10. Relative comparison of the length obtained from the experiments and the model prediction by calculating the length of the total interface of the elec
trodeposits for (a) 0.025 M electrolyte concentration and (b) 0.1 M electrolyte concentration.
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Fig. 11. Relative comparison of the fractal dimension obtained from the experiments and the model predicted image sequences, for the electrolyte concentration of
(a) 0.025 M and (b) 0.1 M.
fractal dimension for 0.025 M and 0.1 M electrolyte concentration, architecture consisting of convolutional long short-term memory is
respectively. explored, which is capable of predicting the spatio-temporal variation of
It must be further noted that multiple parameters related to elec dendrites. The model is trained on two different datasets with varying
trodeposition are investigated by considering two different electrolyte concentrations. Various metrics like percentage MSE, pattern density,
concentrations (0.025 M and 0.1 M) only. The primary cause [69] of the interfacial length, and absolute percentage error are determined. During
growth of the electrodeposits is due to the combined effect of the testing, the mean squared error and the percentage absolute error are
electro-migration and diffusion on the reactant ions (in absence of found to be below 3% for all model predicted outcomes. A fast-growing
convection). The transport of ions towards the electrode surface be branched electrolytic deposition growth pattern is observed for 0.025 M
comes rate-limiting when the concentration of the ions (CCu2+ ,surface .) on electrolyte concentration compared to more uniform and slow growth in
the electrode surface falls to zero due to the high rate of the reaction. In the 0.1 M electrolyte concentration system. The model shows a high
that situation, the relative effect of electro-migration and diffusion of level of accuracy in predicting electrodeposition growth. The average
ions determines the morphology of the growing unit. If error for any selected parameter is found to be less than around 11
electro-migration predominates over diffusion, a sharp tip rises much percent, irrespective of the electrolytic concentration. Therefore, it is
longer forming dendrites instead of uniform deposition due to the high evident, after analyzing multiple matrix parameters, that the
field strength over that point. At a higher concentration of electrolyte ConvLSTM-based deep learning model is capable of predicting electro
solution, it is already established that comparatively lower growth ve deposition growth with reasonable accuracy. All the results indicate that
locity is obtained due to enhanced diffusive flux and inter-ionic inter the deep learning approach can be used as a remarkable tool and will be
action [44] as discussed earlier. Therefore, the difference in morphology certainly useful for electrodeposition studies in near future.
between the two aforementioned concentrations (0.025 M and 0.1 M) is
quite reasonable. However, the present objective specifically deals with Author contributions
electrodeposition prediction by analyzing real-time captured images.
The detailed mechanism behind the formation of dendrites is not R.K. and T.D. worked on data curation and data validation. R.K.
required to foresee the growth. It is also observed that the model is helped in the data visualization and further investigation. Idea
predicting the electrodeposition growth more accurately at a later stage conceptualization, methodology development, and project administra
of the experiment. Owing to the rapid growth rate and complex nature of tion, are done by H.H. and M.C. The model development and formal
the electrodeposition, the model lacks to predict an accurate outcome at analysis is performed by H.H. and R.K. Project supervision, funding, and
the early stage of the experiment. This shortcoming can be overcome by resource acquisition are managed by M.C. All authors contributed to
capturing more data points during the initial growth phase. The limi writing the original draft, editing and reviewing the manuscript.
tations of the high-speed image capturing capability set a restriction on
the frame rate of the captured images from the experiments. However, Declaration of Competing Interest
over time, the rate of electrodeposition growth decreases, and due to the
availability of sufficient data points for the same interval, the pre The authors declare that they have no known competing financial
dictions become significantly accurate . To further generalize the model, interests or personal relationships that could have appeared to influence
more experiments can be conducted by varying experimental conditions the work reported in this paper.
like the voltage, and inter-electrode gap, and the model can be trained
on a new set of images. This would lead to a more robust model. As the Data Availability
existing model is data-driven and has the capability of predicting an
accurate future electrodeposition growth, a similar concept can be used All the relevant have been uploaded with the manuscript.
for other experiments as well where a prediction of the future experi
mental outcome is required. However, the model has to be trained
accordingly to get an accurate result. Acknowledgement
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