RESEARCH ARTICLE | FEBRUARY 13 2024

Second harmonic generation for estimating state of charge

of lithium-ion batteries 
Hongbin Sun  ; Pradeep Ramuhalli ; Ruhul Amin ; Ilias Belharouak

Appl. Phys. Lett. 124, 073902 (2024)

https://doi.org/10.1063/5.0187829

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 Applied Physics Letters ARTICLE pubs.aip.org/aip/apl

Second harmonic generation for estimating state

of charge of lithium-ion batteries
Cite as: Appl. Phys. Lett. 124, 073902 (2024); doi: 10.1063/5.0187829
Submitted: 16 November 2023 . Accepted: 12 January 2024 .
Published Online: 13 February 2024

Hongbin Sun,a) Pradeep Ramuhalli, Ruhul Amin, and Ilias Belharouak

AFFILIATIONS
Oak Ridge National Laboratory, 1 Bethel Valley Road, Oak Ridge, Tennessee 37830, USA

a)
Author to whom correspondence should be addressed: sunh1@ornl.gov

ABSTRACT
This study applied the nonlinear ultrasonic method, second harmonic generation, to precisely estimate the state of charge (SoC) in lithium-
ion batteries. The second harmonic of the longitudinal wave is generated on a pouch cell battery at 5 MHz with a through-transmission setup.
The relative nonlinear parameter b0 is determined by analyzing the amplitudes at the fundamental and second harmonic frequencies. To
enhance the nonlinear parameter’s measurement accuracy, multiple excitation amplitudes are employed. Two separate charge/discharge tests
(four-cycle and eight-cycle) are conducted on the battery at a rate of C/10. The nonlinear parameter is measured periodically during the

25 February 2024 03:30:15

charge/discharge process, and temperature compensation is applied to the measurement. The correlation curves between the nonlinear
parameter and the actual SoC align well for the four-cycle and eight-cycle tests, and a robust linear relationship is observed for both correla-
tion curves. A linear model and a second-order polynomial model are applied to fit the correlation using all data points from both tests. The
two models are employed to validate the SoC prediction on a second battery by using a four-cycle test. The results indicate that both models
can predict the SoC with an accuracy of approximately 3%, whereas the polynomial model demonstrates smaller errors in the regions near
0% and 100% SoC. Therefore, the nonlinear parameter b0 , measured through the second harmonic generation, can effectively predict
lithium-ion battery SoC with an accuracy of less than 3%.
Published under an exclusive license by AIP Publishing. https://doi.org/10.1063/5.0187829

The lithium-ion battery (LIB) stands as a widely embraced energy
storage solution, making its presence felt across diverse industries and
in our daily routines. For the optimal performance and lifetime of
LIBs, a battery management system (BMS) is required to regulate their
operation. The state of charge (SoC) is one of the critical parameters
for battery management. Diverse methods have been implemented to
estimate SoC, including the discharge test method, the ampere-hour
integral (coulomb counting) method,1 the open-circuit voltage (OCV)
method,2 the battery model-based approach,3 and the neural network
model method.4 However, each method presents unique advantages
and challenges. The discharge test, while simple and reliable, proves
impractical for real-time SoC estimation due to its time-intensive
nature.5 The ampere-hour integral method’s precision is notably influ-
enced by the initial SoC and the battery operating states (SoC, temper-
ature, current, etc.). The OCV method, while simple, confronts
challenges with hysteresis during charge/discharge processes, particu-
larly affecting specific battery types (e.g., C/LiFePO4);6 additionally, it
mandates the battery to be in an equilibrium state for accurate real-
time SoC estimation. The battery model-based method (equivalent
circuit model and electrochemical model) does not require rest time
and is insensitive to the initial SoC value. However, the precision
and complexity of the battery model are very critical to the estima-
tion accuracy. The neural network model method, a data-driven
method, exhibits a versatile capability for real-time SoC estimation
across diverse battery types while demanding extensive training
using a substantial dataset. Recently, the acoustic/ultrasonic nonde-
structive evaluation (NDE) of LIBs has gathered increasing attention
on the estimation of SoC and state of health (SoH) as well as moni-
toring structural changes within LIBs.7–9 The ultrasonic NDE tech-
nique exhibits several advantages for SoC estimation in LIBs. It is a
nondestructive method that can provide rapid results through
open-circuit measurements, a feature especially advantageous for
inspecting second-life batteries. Its uncomplicated setup and high
repeatability further facilitate real-time monitoring of battery states.
Furthermore, the LIB operates as a composite material system com-
prising multiple layers of anodes and cathodes. The underlying prin-
ciple of ultrasonic NDE for LIBs lies in its ability to detect the
physical changes in the material properties and internal structure of
the battery. Therefore, this approach can offer a deeper and more
fundamental understanding of the battery’s condition than

Appl. Phys. Lett. 124, 073902 (2024); doi: 10.1063/5.0187829 124, 073902-1
Published under an exclusive license by AIP Publishing
 Applied Physics Letters
traditional electrochemistry methods for an enhanced determina-
tion of SoC, SoH, and battery failure.
During a LIB’s charge and discharge cycles, the mechanical prop-
erties, such as modulus, density, and Poisson’s ratio, undergo changes
as part of the delithiation and lithiation processes. In ultrasonic testing,
the stress wave generated from the ultrasonic transmitter propagates
through the thickness of the battery and carries information about the
material properties and even the changes in the internal structure.
Correlations could be established between the battery’s SoC or SoH and
the various wave features. Among these, time of flight (TOF) is a prom-
inent parameter that signifies the time it takes for a wave to travel
between the transmitter and receiver, typically across the battery’s
thickness.7,10 The signal amplitude,9,11 wave attenuation,12,13 and wave
velocity13,14 are also utilized as crucial indicators. In practice, these fea-
tures are often combined to enhance the accuracy of the SoC estimate.
However, to effectively estimate SoC, it is desirable to have an ultrasonic
wave feature that exhibits a linear relationship with the SoC.
Unfortunately, many studies have shown that TOF and signal ampli-
tude do not exhibit a perfect linear relationship with battery SoC, par-
ticularly in the SoC range below 20%. Moreover, these studies have
found hysteresis behavior during the charge and discharge pro-
cesses.7,13,15 This behavior implies that the same SoC may yield signifi-
cantly different wave feature values during battery charging and
discharging. These nonlinear behaviors contribute to a substantial mar-
gin of error in the battery’s SoC estimation.
These methods, employing various ultrasonic wave features, fall
under the category of linear acoustic/ultrasonic techniques. These tech-
niques are based on the assumption that the relationship between
applied stress or strain and the resulting acoustic/ultrasonic response
adheres to proportionality and follows Hooke’s law. By contrast, non-
linear ultrasonic methods assume a nonlinear relationship, giving rise
to the generation of higher harmonics and other nonlinear effects
caused by the interaction between ultrasonic waves and the material.
Nonlinear ultrasonic methods offer enhanced sensitivity to microstruc-
tural changes and damage, making them a prevalent choice for micro-
structural characterization and damage assessment.16–19 Considering
that a LIB represents a composite system with high acoustic nonlinear-
ity that experiences noticeable microstructural changes throughout its
operation, nonlinear ultrasonic methods become pertinent approaches
to detect and monitor these physical transformations during battery
charge and discharge processes. Surprisingly, nonlinear ultrasonic
methods have seen limited use in diagnosing LIBs, with only one nota-
ble exception.20 The present study explores the application of a specific
nonlinear ultrasonic method—second harmonic generation (SHG)—
to facilitate NDE of LIBs, with the primary aim of achieving highly
accurate SoC estimation. The correlation between the nonlinear
parameter b0 and the battery SoC is built for SoC prediction.
Higher harmonic generation is a phenomenon that emerges
when an ultrasonic waveform undergoes distortion caused by the non-
linear reactions within the material. Consequently, it gives rise to
higher harmonic waves. SHG represents a prominent technique within
the higher harmonic generation family; it is extensively employed to
characterize materials and to assess damage. The foundational princi-
ple of SHG involves the transmission of an ultrasonic wave possessing
a fundamental frequency, denoted as x, through a nonlinear material.
This interaction converts a portion of the energy into a second-order
harmonic wave with a frequency of 2x.21,22
Appl. Phys. Lett. 124, 073902 (2024); doi: 10.1063/5.0187829
Published under an exclusive license by AIP Publishing
ARTICLE pubs.aip.org/aip/apl
Considering 1D wave propagation in an isotropic solid,
 
@ 2 u1 2 @ u1
2
@u1
¼ c 1 þ b ; (1)
@t 2 @X12 X1
where u1 is the displacement, t is the time, and c is the longitudinal
wave velocity. b is the nonlinearity parameter and X1 is the coordinate.
The solution to this equation can be given by considering a time-
harmonic plane wave A1 cosðkX1  xtÞ,
1
u1 ¼  bk2 A21 X1 þ A1 cosðkX1  xtÞ
8
1
þ bk2 A21 X1 cos½2ðkX1  xtÞ
8
¼ A0 þ A1 cosðkX1  xtÞ þ A2 cos½2ðkX1  xtÞ; (2)
where A1 and A2 represent the absolute amplitudes of the funda-
mental harmonic and second harmonic, respectively, in the fre-
quency spectral. x is the wave propagation distance, and k is the
wave number. The nonlinear parameter b can be calculated using
these two amplitudes:
8A2
b¼ : (3)
A21 xk
However, the solution in Eq. (3) only applies to the longitudinal wave.
For the Raleigh wave, a different solution of b is used.16 Furthermore,
the amplitudes of the fundamental and second harmonics are absolute
25 February 2024 03:30:15
displacements, which are challenging to measure. Absolute displace-
ment could be measured either using piezoelectric contact transducers
with careful reciprocity-based calibration procedure23,24 or by using a
laser vibrometer.25 In current practice, the relative nonlinear parameter
b0 is used based on relative amplitudes of fundamental (A01 ) and sec-
ond harmonic (A02 ) as below for longitudinal modes:
A02
b0 ¼ : (4)
A02
1
The LIB cells used in this study were fabricated at the US
Department of Energy’s Oak Ridge National Laboratory (ORNL)
Battery Manufacturing Facility (BMF). These cells were engineered
with specific battery chemistry, featuring a LiNi0.6Mn0.2Co0.2O2
(NMC622) cathode, graphite carbon anode, and Gen-2 electrolyte
packaged with aluminum laminate. The cathode was NMC622 (90%/
5% polyvinylidene fluoride [PVDF]/5% carbon black) with a total
thickness of 122 lm with double-sided coating. The anode was graph-
ite (Superior SLC1520T 92%/6% PVDF/2% carbon black) with a total
thickness of 115 lm. The cathode and anode were both calendared to
35% porosity. The negative/positive ratio was set at 1.1. More details
about the battery’s electrochemical properties and performance can be
found in previous work.13 The choice of chemistry was influenced by
several essential factors. First, it closely mirrors the chemistry com-
monly used in electric vehicle batteries. Second, it enables the consis-
tent production of batteries that have uniform properties and material
characteristics throughout the cell. Third, the chemistry exhibits pre-
dictable changes in both chemical and physical properties during
repeated charge/discharge cycles. Additionally, it aligns with the practi-
cal application of cycling within the standard cell voltage range of 2.5–
4.5 V, taking into account practical SoC and discharge considerations.
The pouch cell had 27 layers: 14 cathode layers and 13 anode layers.
124, 073902-2
 Applied Physics Letters
FIG. 1. Schematic diagram of the second harmonic generation test on a lithium-ion
battery.
The total thickness of the cell was about 4.4 mm, including the separa-
tor and pouch materials, and the total capacity was around 2.6 Ah.
Building upon the work established in the prior study,13 the oper-
ational frequency was determined to be 2.5 MHz, with the second har-
monic frequency at 5 MHz. This work employed longitudinal
transducers of 2.25 MHz (Olympus C106) and 5 MHz (Olympus
C110). The test setup for the SHG is depicted in Fig. 1. Ritec SNAP
5000 was used to excite the ultrasonic transmitter at 2.5 MHz with an
eight-cycle sinusoidal tone burst. The resulting ultrasonic wave propa-
gated through the thickness of the battery and was captured by the
receiver. The ultrasonic receiver converted the ultrasonic wave
Appl. Phys. Lett. 124, 073902 (2024); doi: 10.1063/5.0187829
Published under an exclusive license by AIP Publishing
ARTICLE pubs.aip.org/aip/apl
(vibration) to an electrical signal (voltage). The received signal was
then digitized by the oscilloscope (Tektronix MS044) and stored in the
computer for further analysis. To acquire data for determining the
nonlinear parameter, multiple ultrasonic signals were collected under
five different excitation amplitudes from 160 to 480 V, in 80 V incre-
ments. The battery cell was charged and discharged using a potentio-
stat (Biologic, SP-200) with a C/10 rate from 3.0 to 4.2 V, maintaining
a constant current of 240 mA. Throughout the charge/discharge cycle,
the nonlinear parameter was assessed at 15 min intervals.
A time-domain signal collected with an excitation amplitude of
160 V is shown in Fig. 2(a). First, the time-domain signal was win-
dowed from 9 to 16 ls and then transferred to the frequency domain
[Fig. 2(b)] using a fast Fourier transform. In the frequency spectrum,
the amplitude A01 at 2.5 MHz and the amplitude A02 at the second har-
monic frequency of 5 MHz were extracted. In Fig. 2(c), the data points
of (A02 0
1 ; A2 ) for five different excitation amplitudes were fitted using a
linear relationship. The slope of the fitted curve represents the nonlin-
ear parameter b0 .
The battery was first charged and discharged for four cycles at a
rate of C/10. Before the test, the battery experienced about 40 cycles of
charge/discharge from the beginning of life for other tests. The nonlin-
ear parameter b0 was measured every 15 min. The SoC history and the
b0 history over the four charge/discharge cycles are presented in Fig. 3.
During the charge process, the nonlinear parameter b0 progressively
25 February 2024 03:30:15
FIG. 2. Measurement of the nonlinear
parameter b0 from second harmonic gen-
eration: (a) time-domain signal, (b) fre-
quency spectrum, and (c) A02 vs A021 for
fitting b0 .
124, 073902-3
 Applied Physics Letters
FIG. 3. (a) SoC history for a four-cycle charge/discharge and (b) corresponding
nonlinear parameter b0 measured.
increased [blue curve in Fig. 3(b)], escalating as the SoC advanced
from 0% to 100%. Conversely, in the discharge phase, b0 decreased
with the SoC’s return to 0%. During charge, lithium ions are driven
from the cathode to the anode. This migration causes structural
changes in the electrodes, including expansion of the anode and con-
traction of the cathode. These mechanical changes can introduce non-
linearities in the acoustic response of the battery materials. Meanwhile,
the cathode materials often undergo phase transformations, and these
transformations can cause abrupt changes in the material’s mechanical
properties and increase the acoustic nonlinearity. The expansion and
contraction of the electrodes because of lithium insertion and extrac-
tion create significant stress and strain on the battery materials, also
causing nonlinear effects. The ultrasonic wave can also be influenced
by interactions between the electrodes and the electrolyte. The chang-
ing chemical and mechanical interactions between these components
during charge can contribute to nonlinear acoustic effects. In sum-
mary, the increase/decrease in acoustic nonlinearity during the charge/
discharge process of a LIB is a result of complex physical and chemical
changes within the battery materials. The measured nonlinear parame-
ter b0 serves as a clear indicator of these changes in acoustic nonlinear-
ity throughout the charge and discharge processes. This study revealed
that the nonlinear parameter b0 was also sensitive to temperature
change. Therefore, the temperature sensitivity of b0 was measured at
different SoC percentages in the temperature range of 20–30  C. The
sensitive coefficient was estimated to be around 0:25  106 = C. The
corrected b0 (red curve) with a temperature compensation on the origi-
nal data (blue curve) is shown in Fig. 3(b).
The correlation between the SoC and the measured nonlinear
parameter b0 is illustrated in Fig. 4 (depicted by the blue curve). The
nonlinear parameter b0 demonstrates an almost linear relationship
with the battery’s SoC, and no obvious hysteresis is observed in the
correlation curves. To confirm the reliability of this association, an
additional eight-cycle charge/discharge test was initiated 34 h after the
end of the four-cycle test. The correlation between the SoC and the
nonlinear parameter b0 is presented in Fig. 4 (yellow curve). This curve
Appl. Phys. Lett. 124, 073902 (2024); doi: 10.1063/5.0187829
Published under an exclusive license by AIP Publishing
ARTICLE pubs.aip.org/aip/apl
FIG. 4. Correlation between the SoC and nonlinear parameter b0 for the four-cycle
and eight-cycle charge/discharge tests.
closely aligns with the correlation curve from the four-cycle test, dis-
playing a similar approximately linear relationship. This robust repeat-
ability indicates that the nonlinear parameter b0 maintains a consistent
linear relationship with the battery SoC across multiple test cycles.
The linear relationship was fitted using all the data points gath-
ered from both the four-cycle and eight-cycle tests. The fitted relation-
ship (magenta curve) can be expressed as b0 ¼ ð0:0208  SoC
þ 4:562Þ  106 with a high goodness of fit R2 ¼ 0:984 and small
root mean square error (RMSE). However, the data points falling below
25 February 2024 03:30:15
10% and exceeding 90% SoC did not align well with the linear curve, indi-
cating a suboptimal fit within these two regions. To enhance the fitting
accuracy in the low- and high-SoC ranges, a second-order polynomial
curve was employed (red curve). The improved curve can be represented
as b0 ¼ ð0:000 049  SoC2 þ 0:0159  SoC þ 4:643Þ  106 . This for-
mulation increases the R2 slightly and decreases the RMSE, enhancing the
curve’s suitability for describing the nonlinear parameter b0 across the
entire SoC range.
To assess the efficacy of SoC prediction using the nonlinear
parameter b0 , a third test was conducted on a second battery, which
underwent a four-cycle charge/discharge procedure. This second bat-
tery was manufactured from the same batch and had experienced simi-
lar charge/discharge cycles as the previous battery. The SoC of this
battery in the third four-cycle test was predicted by using the previ-
ously fitted linear and second-order polynomial relationships and the
real-time measurement of the nonlinear parameter b0 . The two real-
time SoC predictions are plotted in Fig. 5 along with the actual SoC
FIG. 5. Battery SoC prediction for a separate four-cycle test using linear fit and
second-order polynomial.
124, 073902-4
 Applied Physics Letters
measured by the potentiostat. The predicted SoC curves closely match
the actual SoC values, demonstrating the viability of employing the
nonlinear parameter b0 to predict SoC. When using the linear fit, the
mean absolute error (MAE) of the predicted SoC was 3.1% compared
with the actual SoC measured by the potentiostat, and the predicted R2
value was 0.981, indicating a high level of prediction accuracy.
However, a relatively larger prediction error, approximately 10%,
appeared as the battery neared 100%. Using the second-order polyno-
mial model, the MAE improved to 2.8%, and the R2 increased slightly
to 0.985. Most notably, the maximum absolute error in prediction near
100% SoC was reduced to 6%. Thus, the second-order polynomial
model appears to offer greater accuracy for SoC prediction than the
linear model, particularly in SoC regions near 0% and 100%. In con-
clusion, the proposed method employing the nonlinear parameter b0 ,
measured via SHG, effectively predicts LIB SoC with an accuracy of
less than 3%. Further improvements may be achieved by using nonlin-
ear models, particularly in SoC regions close to 0% and 100%.
In this work, a nonlinear ultrasonic method, SHG, was used to
estimate the SoC of LIBs. The nonlinear parameter b0 was measured
with the wave amplitudes at 2.5 and 5 MHz using a through-
transmission test setup. This nonlinear parameter was continuously
monitored throughout multiple charge and discharge cycles. A robust
linear relationship was observed between the nonlinear parameter b0
and actual SoC. To model this relationship, both a linear and a
second-order polynomial model were employed, and the two fitted
models were applied to predict SoC in a second battery based on the
measured nonlinear parameter b0 history. The results indicated that
both models could predict SoC reasonably accurately, with an accuracy
of approximately 3%. The linear model exhibited larger prediction
errors when the SoC approached 0% and 100%, whereas the second-
order polynomial model demonstrated smaller errors in these specific
regions.
The SoC prediction was conducted under a relatively stable SoH
condition and a constant charge/discharge rate on two newly manufac-
tured batteries. However, battery degradation and charge/discharge
rates would also affect the nonlinearity measurement. Therefore, fur-
ther investigations are required to decouple the effects of both SoC and
SoH on the nonlinearity measurements, and to validate the proposed
method under different battery operating conditions and aging mecha-
nisms. In the experimental setup, the two transducers were com-
pressed to the battery using a C-clamp to keep a constant distance
because the measurement of the nonlinear parameter via SHG is
highly sensitive to this distance. To enable practical applications, a reli-
able coupling mechanism should be established to eliminate the influ-
ence of coupling variations. This mechanism could involve the
permanent installation or embedding of ultrasonic transducers within
the battery structure.
This work was partially supported by Titan Advanced Energy
Solutions and the National Renewable Energy Laboratory through
the U.S. Department of Energy Lithium-Ion Battery Recycling Prize.
Nitin Muralidharan and Kelsey Livingston are appreciated for their
work on experimental setup and battery fabrication. Ryan Meyer
and Georgios Polyzos are also acknowledged for their helpful
comments on the earlier draft of the manuscript.
This manuscript has been authored by UT-Battelle, LLC,
under contract DE-AC05-00OR22725 with the U.S. Department of
Appl. Phys. Lett. 124, 073902 (2024); doi: 10.1063/5.0187829
Published under an exclusive license by AIP Publishing
ARTICLE pubs.aip.org/aip/apl
Energy (DOE). The U.S. government retains and the publisher, by
accepting the article for publication, acknowledges that the U.S.
government retains a nonexclusive, paid-up, irrevocable, worldwide
license to publish or reproduce the published form of this
manuscript or allow others to do so, for U.S. government purposes.
DOE will provide public access to these results of federally
sponsored research in accordance with the DOE Public Access Plan
(http://energy.gov/downloads/doe-public-access-plan).
AUTHOR DECLARATIONS
Conflict of Interest
The authors have no conflicts to disclose.
Author Contributions
Hongbin Sun: Conceptualization (equal); Data curation (equal);
Formal analysis (equal); Funding acquisition (equal); Investigation
(equal); Methodology (equal); Validation (equal); Writing – original
draft (equal); Writing – review & editing (equal). Pradeep Ramuhalli:
Funding acquisition (equal); Methodology (equal); Project administra-
tion (equal); Supervision (equal); Writing – review & editing (equal).
Ruhul Amin: Conceptualization (equal); Investigation (equal);
Resources (equal); Software (equal); Writing – original draft (equal);
Writing – review & editing (equal). Ilias Belharouak: Funding acquisi-
tion (equal); Project administration (equal); Supervision (equal);
Writing – review & editing (equal).
25 February 2024 03:30:15
DATA AVAILABILITY
The data that support the findings of this study are available from
the corresponding author upon reasonable request.
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