Journal of Magnetism and Magnetic Materials 563 (2022) 169892

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Journal of Magnetism and Magnetic Materials

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

Anomalous Nernst thermopile made of a single element iron

Ting-Wei Weng a, 1, Tsao-Chi Chuang a, 1, Danru Qu b, c, *, Ssu-Yen Huang a, c, *
a
Department of Physics, National Taiwan University, Taipei 106, Taiwan
b
Center for Condensed Matter Sciences, National Taiwan University, Taipei 106, Taiwan
c
Center of Atomic Initiative for New Materials, National Taiwan University, Taipei 106, Taiwan

A B S T R A C T

Anomalous Nernst thermopiles that utilize spin–orbit coupling in magnetic materials are beneficial for energy harvesting. Under an out-of-plane temperature
gradient, the thermopiles can generate sizable and scalable thermoelectric voltages due to the anomalous Nernst effect (ANE). In this work, we show that a ther-
mopile made of only one element, Iron (Fe), can generate a significant spin-dependent thermoelectric signal. We find that by varying the thickness of Fe, the
anomalous Nernst signal changes sign and becomes exceptionally large in the thinner-thickness region. As a result, the anomalous Nernst thermopile consisting of
only Fe exhibits a sizable thermoelectric signal. Moreover, the plateau behavior in the thermopile owing to the sequential flipping of magnetic moments demonstrates
that the ANE could serve as a sensitive tool to detect magnetic switching. The multi-level ANE signals further indicate the anomalous Nernst thermopiles can be
utilized as the ANE valve for logic gates. These results provide an essential guide for energy harvesting and spin-dependent electrothermal sensor using magnetic
materials.

Spin caloritronics studies the interaction among charge, spin, and
heat. Intensive studies have been focused on the spin Seebeck effect
(SSE) and the anomalous Nernst effect (ANE), where heat currents
generate spin and spin-polarized currents in magnets longitudinally and
transversely, respectively [1]. The SSE is often observed in magnetic
insulator, and an attached metallic layer with sizable spin–orbit
coupling converts the spin current to a transverse charge current via the
inverse spin Hall effect (ISHE) [2]. The ANE is often observed in con-
ducting magnetic materials, including metals, semiconductors, and to-
pological semimetals and it is caused by the spin–orbit scattering of
unbalanced electrons with up and down spins [3]. The thermoelectric
voltages generated from the SSE/ISHE or the ANE are typically in the
order of microvolt, which are too small for practical applications.
Therefore, boosting the thermoelectric signal is of crucial importance for
efficient thermal energy harvesting from heat and is one of the strongest
driving forces for spin caloritronic research.
One approach for large heat to charge conversion is to search for
magnetic materials with large anomalous Nernst coefficient. In the ANE,
the thermoelectric signal (E), the external magnetic field (H), and the
temperature gradient (∇T) are mutually orthogonal to each other, as
shown in Fig. 1(a). The ANE signal can be described by.
EANE = − Sxy m × ∇T
where Sxy is the anomalous Nernst coefficient, also known as the
transverse Seebeck coefficient, and m is the unit vector of the magnetic
moment. According to Eq. (1), the thermoelectric voltage is directly
proportional to the Sxy . In order to obtain a large ANE signal, intensive
studies have been devoted to searching for materials with large Sxy ,
including the topologically nontrivial quantum materials, for example,
Mn3Sn [4], Co2MnGa [5], Fe3Ga [6], YbMnBi2 [7], etc., which have
band touching points in their band structures, and have Sxy of a few
microvolts per kelvin at room temperature.
To further boost the thermoelectric voltage, fabrication of anoma-
lous Nernst thermopile is crucial. In the anomalous Nernst thermopile,
as shown in Fig. 1(b), strips made of magnets with opposite signs in Sxy
are located alternatively and parallelly with each other while connected
in series. The anomalous Nernst thermopile is scalable; the total thermal
voltage is a sum of the ANE voltages of all the strips. By further reducing
the width and increasing the total effective length of the strips, the
anomalous Nernst thermopile can reach a high heat flux sensitivity
comparable to or even exceed some of the commercial Seebeck-type
thermopiles [1,8]. It is worth pointing out that since the anomalous
Nernst thermopile is made of thin films, it could be extremely flexible
compared to the Seebeck-type thermopiles. Moreover, for the anoma-
lous Nernst thermopile, the applied temperature difference (ΔT) and the
detected voltage (V) are in the transverse direction, which in principle
(1)
allows arbitrarily large voltage when the strip length is increased. In
contrast, for the Seebeck-type device, ΔT and V are in the same direction,

* Corresponding authors.
E-mail addresses: danru@ntu.edu.tw (D. Qu), syhuang@phys.ntu.edu.tw (S.-Y. Huang).
1
These authors contributed equally to this work.

https://doi.org/10.1016/j.jmmm.2022.169892
Received 14 June 2022; Received in revised form 19 August 2022; Accepted 26 August 2022
Available online 6 September 2022
0304-8853/© 2022 Elsevier B.V. All rights reserved.
T.-W. Weng et al.
thus V is fixed for a fixed ΔT regardless of the lateral dimensions of the
device [1].
In the anomalous Nernst thermopiles, two different materials are
usually used since opposite signs in Sxy are required for the head-to-tail
series connection. In this work, we show the Sxy can be different and
even changes sign for one single element magnet Fe with different
thicknesses. Most importantly, we find the anomalous Nernst voltage
increases drastically at lower thickness region indicating the modifica-
tion of the band structure of ultrathin Fe. This observation eventually
leads to the thermopile consisting of only Fe. The fabrication process for
the anomalous Nernst thermopile could be exceedingly simplified with
only one element required. The single-element thermopile is not only
scientifically interesting but also technologically exciting.
The magnetic films studied in this work are deposited on 16-mm
wide, 16-mm long, and 0.5-mm thick Si substrates by DC magnetron
sputtering under an argon pressure of 10 millitorr in a chamber with a
base pressure of 10-7 Torr. The anomalous Nernst thermopiles are
fabricated by sequential photolithography processes. The thicknesses of
the thin films are determined by atomic force microscopy, and the
magnetization is measured by vibrating sample magnetometer (VSM).
During the ANE measurement, the sample is sandwiched between a
silicone sheet and a Cu heat sink. The silicone sheet is directly contacted
with a resistance heater and has an area size of about 1 cm2. A constant
heat power of 5.3 W is applied throughout our study. From COMSOL
simulation, an effective heat flux ϕq = 3.6 × 104 W/m2 , which considers
the different sizes between the substrate and the heating silicone sheet,
is maintained throughout our measurement.
We first show the ANE for Py (Ni80Fe20) and Fe thin films on Si
substrate. For an in-plane magnetic field along the x-axis and an out-of-
plane temperature gradient/heat flux along the z-axis, we obtain sizable
anomalous Nernst voltages for Py and Fe thin films with various thick-
nesses ranging from a few nanometers to 100 nm along the y-axis. The
ANE signals for the 30-nm thick Py (blue), 30-nm thick Fe (green), and
3-nm thick Fe (red) are shown in Fig. 1 (c). In all cases, the square-like
hysteresis loops are presented, which resemble their magnetization
loops. The difference in the width of the loops is caused by the different
coercivity of the ferromagnetic films. The ANE for the 30-nm thick Py
Fig. 1. Schematic illustration for (a) the ANE measurement (b) the anomalous Nernst thermopile, where H, E, and ∇T are magnetic field, electric field, and tem-
perature gradient, respectively. (c) The field-dependent ANE voltages for the 30-nm-thick Py (blue), 30-nm-thick Fe (green), and 3-nm-thick Fe (red). (d) Thickness-
dependent ANE signals for Py (blue) and Fe (red).
2
Journal of Magnetism and Magnetic Materials 563 (2022) 169892
and 30-nm thick Fe is about 3.7 μV and –1.5 μV at the saturation field of
60 Oe, respectively. Surprisingly, the ANE for 3-nm thick Fe is about +
7.4 μV, which not only changes the sign but also becomes 5 times larger
than that for the 30-nm thick Fe. The results for other thicknesses,
ranging from a few nm to 100 nm are shown in Fig. 1(d). For Py thin
films, the ANE voltage is about 3.7 μV in the thicker-film region (>9 nm)
and decreases to nearly zero with decreasing thicknesses below 9 nm. In
sharp contrast, the ANE for Fe is about –1 μV in the thicker-film region
(>9 nm) and decreases to zero when the thickness reaches 6 nm. For
even thinner film (less than 6 nm), the ANE signal surprisingly becomes
positive and drastically increases in magnitude. According to Eq. (1), the
ANE signal is proportional to the transverse Seebeck coefficient Sxy ,
which is expressed as Sxy = ρ(αxy − Sxx σxy ), here ρ is resistivity, αxy =
π 2 k2B T ∂σxy π 2 k2B T ∂σ
3e ( ∂E )EF is the transverse thermal conductivity, Sxx = 3eσ (∂E)EF is the
Seebeck coefficient, and σ xy is the transverse conductivity. As shown in
our previous work [3], we have utilized the Sxy and αxy derived from the
Mott relation to investigate the scaling relation of the ANE. We show
that the enhancement in thin films is primarily caused by the intrinsic
and side-jump mechanisms.
We have also performed the X-ray diffraction (XRD) study to inves-
tigate the crystalline structure of our thin films. We confirmed the body
centered cubic structure for the 180-nm thick Fe films. However, for thin
Fe films less than 6 nm, we could not capture any XRD peaks, possibly
due to the limitation of our instrument. Therefore, we could not exclude
the possibility that for very thin Fe, its crystalline structure changes to
face centered cubic structure or amorphous structure. This awaits
further experimental studies.
Next, by head-to-tail series connection of strips with opposite ANE
signals, the same as connecting batteries in series, we fabricate two types
of thermopiles based on Py and Fe, and Fe only. The alternatively ar-
ranged and laterally connected thermopile is assembled as portrayed in
Fig. 2(a) and 2(b). Each component is named after the shapes, which are
“I” and “Z”, and there are 10 and 9 of them, respectively. Each strip in
the thermopile has a width of 200 μm, a length of 5 mm, and they are
separated by 480 μm. As shown in the upper panel of Fig. 2(c), the
thermopile of Py(30)-Fe(30) which consists of 30-nm-thick Py and 30-
T.-W. Weng et al.
Fig. 2. Schematic illustration of (a) the Py(30)-Fe(30) and (b) the Fe(3)-Fe(30) thermopiles. The blue, green and red strips represent Py(30), Fe(30), and Fe(3),
respectively. Field-dependent ANE (upper panel) and magnetization (lower panel) for (c) the Py(30)-Fe(30) and (d) the Fe(3)-Fe(30) thermopiles. The blue, green and
red arrows represent the direction of Py(30), Fe(30), and Fe(3) magnetic moments, respectively.
nm-thick Fe exhibits a thermal voltage of 21.9 μV at the saturation field
of 50 Oe. By further replacing Py with the 5-nm-thick Fe, as shown in the
upper panel of Fig. 2(d), the thermopile of Fe(5)-Fe(30) reaches a
significantly larger thermal voltage up to 122.3 μV, nearly-six times
larger than that of Py(30)-Fe(30). Since the voltage generated by the
anomalous Nernst thermopile is directly proportional to the effective
total length of the wires, by further reducing the width in the nanometer
scale and accommodating 1000 times more the anomalous Nernst pairs
on the same substrate, we would expect a thermal voltage up to 100 mV.
To verify that the ANE voltage is independent of the width, we study
the ANE in two types of 30-nm thick Py films with significant differences
in width, 200 μm and 30 mm (30,000 μm), respectively, while keeping
the same length of 5 mm. There are six individual 200-μm-wide strips on
one substrate and one uniform 30-mm-wide film on another substrate
with six different pairs of positions for Nernst measurement, as shown in
the inset of Fig. 3(a). Note that the dimension of the substrates are the
same, which is 5 mm by 30 mm, in order to keep the same heat flux. As a
3
Journal of Magnetism and Magnetic Materials 563 (2022) 169892
result, the ANE signals obtained in all samples are essentially the same
about 2 μV, as shown in Fig. 3(a), demonstrating their independence of
width. These results also indicate under the same heat flux, for thin films
of the same thickness, the ANE voltages are comparable with each other.
We further confirm the linear dependence of the ANE signals on the
effective total length of the thermopile strips. We connect several 30-
nm-thick, 5-mm-long, and 200-μm-wide Py strips (blue) in series with
30-nm-thick Cr strips (grey) of the same lateral dimensions, as shown in
the inset of Fig. 3(b). Since Cr produces no ANE signal, the voltage V we
obtained under in-plane magnetic field H and out-of-plane temperature
gradient ∇T solely comes from the Py signals. Furthermore, by
measuring different numbers of pairs of the Py-Cr strips, the ANE voltage
shows a linear dependence on the effective total length of the Py strips,
as shown in Fig. 3(b), demonstrating the scalability of the thermopile.
These results again indicate that by reducing the strip width and
increasing the effective total length while keeping the exact lateral di-
mensions of the device, an anomalous Nernst thermopile with large
Fig. 3. (a) The width dependence of the ANE signals.
The blue and red dots represent ANE signals of Py
with 200 μm and 30 mm in width, and they corre-
spond to upper and lower insets, respectively. The
insets are schematic illustration of the ANE measure-
ments. The 200-μm-wide sample has six individual
strips while the 30-mm-wide sample has six different
pairs of positions for the Nernst measurements. The
substrates maintain the same size in both cases to
keep the same heat flux. (b) The length dependence of
ANE signal in the Py(30)-Cr(30) thermopile. Inset is
schematic drawing of the Py(30)-Cr(30) thermopile,
where the blue and grey strips represent Py and Cr,
respectively.
T.-W. Weng et al. Journal of Magnetism and Magnetic Materials 563 (2022) 169892

voltage output can be achieved. Table 1

For a more illustrative view of the exceptional performance of the The thermoelectric coefficient Sϕxy determined from Eq. (2) for various thermo-
single-element thermopile made of Fe, we compare the heat to charge piles. For Pt/YIG-Nb/YIG, FePt-Cr, and CoFeB-IrMn, the heat flux ϕq = ∇T • κ
conversions in several SSE/ISHE and ANE materials. When making such are estimated using the reported temperature gradient ∇ T of 10 K/mm, 1 K/
comparisons, correctly determining the temperature difference across mm, 21500 K/mm, and the thermal conductivity of 7.4 W/Km (YIG), 30 W/Km
the film is crucial. The anomalous Nernst coefficient, Sxy, is commonly (MgO), and 10.3 W/Km (CoFeB)-8.4 W/Km (IrMn), respectively. For FeAl-Au, at
used for bulk materials, and it is estimated as the electromotive force 0 T Sϕxy = 2.4 μVcm/W, at 140 mT Sϕxy = 8 μVcm/W.
normalized by a temperature gradient across the bulk sample, as shown Materials V (μV) L (cm) ϕq (W/cm2) Sϕxy (μVcm/W)
in Eq. (1). However, it is extremely difficult to accurately determine the
Py-Fe (this work) 21.9 9.5 3.6 0.64
temperature gradient across a thin film since not only the thermal
Fe-Fe(this work) 122.3 9.5 3.6 3.57
conductivity of both thin film and substrate are different, but also the Pt/YIG-Nb/YIG [11] 126 9.7 7.4 1.76
thermal resistance between the heat sink, the film, and the substrate are FePt-Cr [12] 6.6 1.2 3 1.83
all nontrivial. Moreover, it has been shown that the thermal conductivity FeAl-Au [13] 50 ~ 170 50 0.42 2.4 ~ 8
of thin films differs from that of bulk [9]. The complexity of accurate Mn3Sn [8] 254 192 0.97 1.36
CoFeB-IrMn [14] 10 0.013 20,900 0.0368
experimental determination of the temperature gradient across the thin
films places a barrier to the essential quantitative comparison of Sxy
among different materials.
Instead, we can quantitatively compare the heat to charge conver-
sion in various thin films through the heat flux method. The heat flux ϕq
is the heat power per area. It can be nicely controlled by supplying a
constant heat power and maintaining the same lateral dimensions of the
device. One of the prominent advantages of the heat flux method is that
the contributions from the bulk substrate and the interface to the tem-
perature profile can be ignored, since by keeping the same ϕq , the ∇T is
the same for a thin film of the same thermal conductivity κ, according to.
ϕq = ∇T • κ (2)

Our recent work has shown that with the same heat flux, the
anomalous Nernst voltages are the same for the same 5-nm-thick Ni thin
films on Si and MgO substrates with different thermal conductivities
[10]. We thus propose to use a thermoelectric coefficient, Sϕxy , to study
the heat to charge conversion of the spin-caloritronic effects with
transverse geometries, e.g., SSE, ANE, etc. This thermoelectric coeffi-
cient is defined as.
ϕ
Sxy ≡ E/ϕq (3)

where the thermoelectric motive force E is normalized by the heat

flux ϕq instead of the temperature gradient. Here, E = V/L, with V
being the thermal voltages and L as the total effective length of the
thermopile. Noted that here we compare the thermoelectric voltages
generated for thin films under the same ϕq instead of the same ∇T,
where the two quantities can be converted by κ through Eq. (2).
For the Py(30)-Fe(30) thermopile, with the total effective length of
0.095 m, under a heat flux of ϕq = 3.6 × 104 W/m2 , the generated
voltage is 21.9 μV. Thus Sϕxy = 0.64 μVcm/W. For the Fe(3)-Fe(30)
thermopile, with the same lateral dimension and heat flux, the ther-
mal voltage is 122.3 μV, which results in a Sϕxy = 3.57 μVcm/W almost 6
Fig. 4. Comparison for the thermoelectric coefficient Sϕxy , which is the trans-
verse electromotive force averaged by heat flux, for various thermopiles. For
visibility, data of CoFeB(8)/IrMn are multiplied by a factor of 10. For FeAl-Au,
we plot the Sϕxy = 2.4 μVcm/W obtained at 0 T.
Mn3Sn thermopiles. The CoFeB(8)/IrMn thermopile has the CoFeB,
pinned by different degrees of exchange bias from IrMn [14]. Its thermal
voltage is a combination of both ANE and ISHE/SSE. However, since it is
extremely difficult to determine the temperature gradient across a thin
film experimentally, a COMSOL simulation is used. Based on the simu-
lation, we estimated a large ϕq for this study, according to Eq. (2), which

times the Py(30)-Fe(30) thermopile. We also estimate the Sϕxy in ther-
mopile devices from other groups based on their reported results and
make a comparison with ours, as shown in Table 1 and Fig. 4. We esti-
mate the heat flux using Eq. (2) when only temperature gradient ∇T and
thermal conductivity κ are provided. Among these thermopiles, the Pt/
YIG-Nb/YIG is a thermopile composed of Pt and Nb with opposite spin
Hall angles grown on YIG, and the thermal voltage is generated as a
result of the combined ISHE/SSE in both materials [11]. The FePt(30)-Cr
thermopile has the thermal voltage originating from the in-plane
magnetized FePt [12]. For FePt with perpendicular magnetization,
since the temperature gradient is applied in-plane, it is hard to estimate
the heat flux for the thermopile wires, therefore, we could not make a
comparison for this case. The FeAl-Au thermopile generates significant
thermal voltages at a high magnetic field but reduces to about 4 times
smaller when the magnetic field is absent [13]. The Mn3Sn-Au ther-
mopile consists of the magnetic Weyl semimetal Mn3Sn and Au strips
[8]. Despite the negligible magnetization, sizable ANE is observed in the
results in a relatively small Sϕxy . The much larger ϕq compared with other
studies, as shown in Table 1, could be caused by the inaccurate deter-
mination of the temperature gradient from the simulation for Ref. [14].
These results again highlight the importance of the heat flux method
when making comparisons among different studies. It is worth to
mention that among these studies, the Fe(3)-Fe(30) thermopile reported
in this work exhibits the largest value of Sϕxy = 3.57 μVcm/W if we
exclude that of FeAl-Au which works at relatively high field of 130 mT.
Besides, we show that the ANE measurement can be a sensitive tool
to detect the magnetization states along the short edge of the strip. In the
magnetic hysteresis loop of Py(30)-Fe(30) measured by VSM, as shown
in the bottom of Fig. 2(c), the magnetization switching of the Py strips
(blue arrow) and Fe strips (green arrow) are narrow. By adapting the
ANE measurement, the Py switching “plateau” becomes broader. The
contrast is marked in yellow in Fig. 2(c) and 2(d). Note that the coer-
civity of Fe(3) is smaller than that of Fe(30). The difference in the
“plateau” width between the magnetization and ANE measurements

4
T.-W. Weng et al.
may be caused by the misalignment between the magnetic field and the
short edge of the thermopile strip, where the magnetization and ANE
measurements detect the magnetization parallel to the magnetic field
and the short edge of the strip, respectively.
Furthermore, this multi-step plateau behavior gives the ANE a po-
tential usage in logic gates, namely the ANE valve [15]. To manifest the
degree of contrast between different states, we define an anomalous
Nernst valve ratio (ANVR) as (V↑↑ − V↑↓ )/(V↑↑ + V↑↓ ), where V↑↑(↑↓) de-
notes the anomalous Nernst voltage of the thermopile with parallel
(antiparallel) magnetization configurations. The ANVR for the Py(30)-
Fe(30) thermopile is 20 %, and for Fe(3)-Fe(30), it is 10 %. These re-
sults demonstrate that the ANE could serve as an alternative approach to
detect the magnetic switching sensitively and can be potentially used as
the ANE valve for logic gates.
In summary, we demonstrate an anomalous Nernst thermopile con-
sisting of single-element Fe. We show its large heat-to-charge conversion
characterized by the thermoelectric coefficient Sϕxy , which is thermo-
electric motive force averaged by heat flux. Besides, we show that the
ANE could serve as an alternative approach to sensitively detect the
magnetic switching and potentially be used as the ANE valve for logic
gates. These results provide an essential guide for energy harvesting and
spin-dependent electrothermal sensor using magnetic materials.
Declaration of interests
Ssu-Yen Huang, Danru Qu reports financial support was provided by
Ministry of Science and Technology, Taiwan. Ssu-Yen Huang, Danru Qu
reports financial support was provided by Ministry of Education,
Taiwan.
CRediT authorship contribution statement
Ting-Wei Weng: Investigation, Data curation, Formal analysis,
Writing – original draft. Tsao-Chi Chuang: Investigation, Data curation,
Formal analysis, Writing – original draft. Danru Qu: Formal analysis,
Writing – review & editing. Ssu-Yen Huang: Conceptualization, Meth-
odology, Supervision.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Journal of Magnetism and Magnetic Materials 563 (2022) 169892
Data availability
Data will be made available on request.
Acknowledgments
The authors would like to thank Professor C. L. Chien for his
tremendous support and enlightening discussions on science and other
aspects for many years. Happy Birthday, Prof. Chien! This work was
supported by the Ministry of Science and Technology of Taiwan under
Grant No. MOST 110-2123-M-002-008, and No. MOST 110-2112-M-
002-047-MY3. This study was also partially supported by Center of
Atomic Initiative for New Materials (AI-MAT), National Taiwan Uni-
versity, under Grant No. 110 L9008 and 111 L9008 from the Featured
Areas Research Center Program within the framework of the Higher
Education Sprout Project by the Ministry of Education in Taiwan.
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