IEEE TRANSACTIONS ON APPLIED SUPERCONDUCTIVITY, VOL. 32, NO.
4, JUNE 2022
Investigation of the Superconducting Ti/PdAu
Bilayer Films for Transition Edge Sensors
Xiaolong Xu, Mauro Rajteri , Jinjin Li , Shuo Zhang, Eugenio Monticone , Jian Chen, Carlo Pepe ,
Huifang Gao, Wei Li, Xu Li, Qi Li, Ying Gao, Zheng Liu, and Xueshen Wang
Abstract—High quality superconducting films are crucial for the
development of transition edge sensors (TESs) with high energy
resolution ability. Controlling the superconducting transition tem-
perature (Tc ) and the transition width (ΔTc ) of the films from
the superconducting to normal metal state is important for the
performance of TESs. We present a new kind of superconducting
Ti/PdAu bilayer film. The influence of Ti/PdAu thickness ratio on
Tc through the proximity effect is investigated. The Tc can be tuned
from 175 mK to 336 mK by setting the PdAu thickness to 60 nm
and varying the thickness of Ti from 50 nm to 70 nm. The minimum
ΔTc is ∼1 mK. The element distribution at the interface between
the Ti and PdAu layers has been analyzed by a high-resolution
transmission electron microscopy (HRTEM), energy-dispersive
spectrometer (EDS) and X-ray diffraction (XRD). Roughness, elec-
trical resistivity, and cryogenic properties are also shown. The
superconducting Ti/PdAu bilayer film shows a great promise as
a new material for TESs.
Index Terms—Proximity effect, superconductivity, Ti/PdAu,
transition-edge sensor.
I. INTRODUCTION
RANSITION Edge sensors (TESs) have been widely used
T as energy detectors for microwave [1], NIR-visible-UV
light [2], X-ray [3] and gamma-ray [4]. The key sensor unit is
often a superconducting thin film, such as Ti [5], W [6] and Hf
[7]. However, the tunable range of the transition temperature
(Tc ) by the thickness for a superconducting film based on single
Manuscript received September 28, 2021; revised December 8, 2021 and
February 5, 2022; accepted February 15, 2022. Date of publication February 24,
2022; date of current version May 16, 2022. This work was supported in part
by Young Scientists Fund of the National Natural Science Foundation of China
under Grants 61901432 and 61701470, in part by the Science and Technology
project of State Administration for Market Regulation, China, under Grants
2020MK153 and 2019MK112, and in part by the Fundamental Research Projects
in Basic Scientific Research at NIM under Grant AKYZD1903. (Corresponding
author: Jinjin Li.)
Xiaolong Xu, Jinjin Li, Jian Chen, Huifang Gao, Wei Li, Xu Li, Qi Li,
Ying Gao, Zheng Liu, and Xueshen Wang are with the National Institute of
Metrology (NIM), Beijing 100029, China (e-mail: xiaolong.xu@nim.ac.cn;
jinjinli@nim.ac.cn; chenjian@nim.ac.cn; gaohf@nim.ac.cn; liwei@nim.ac.
cn; li-xu@nim.ac.cn; liqi@nim.ac.cn; gaoying2018@nim.ac.cn; lzheng@
nim.ac.cn; wangxs@nim.ac.cn).
Mauro Rajteri and Eugenio Monticone are with the Istituto Nazionale di
Ricerca Metrologica (INRiM), 10135 Torino, Italy (e-mail: m.rajteri@inrim.it;
e.monticone@inrim.it).
Shuo Zhang is with Center for Transformative Science, ShanghaiTech Uni-
versity, Shanghai 201210, China (e-mail: shuozhang@shanghaitech.edu.cn).
Carlo Pepe is with Politecnico di Torino, 10129 Torino, Italy (e-mail:
carlo.pepe@polito.it).
Color versions of one or more figures in this article are available at
https://doi.org/10.1109/TASC.2022.3153233.
Digital Object Identifier 10.1109/TASC.2022.3153233
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2100404
material is limited. In our previous work, Tc of a 100 nm Ti film
was 550 mK [8], while other research groups reported that for
their Ti thin films, the Tc was from 360 mK to 500 mK [9]–[11].
A common method to tune the Tc in a wider range is exploiting
the proximity effect which occurs at the interface between a
superconducting and a normal metal film [12]. Several kinds
of bilayer films have been used in TESs, such as Mo/Cu [13],
Mo/Au [14], Ti/Au [15], Ti/Al [16], Ir/Au [17] and so on. For
UV-Vis-NIR TESs the Tc typically ranges between ∼100 mK
and 500 mK [9], [11], [14], [16].
In this paper, we show some results on a new superconducting
Ti/PdAu bilayer film for TESs. PdAu is an alloy easily made in
different ratios [18], and remains in the normal state even when
the temperature is at millikelvin level [19]. Pd has a narrower lat-
tice spacing than Au, which can block the diffusion of Au atoms
to the Ti layer via the pinning effect [20]. We expect that the
Ti/PdAu bilayer film will show a better long-term stability than
Ti/Au. Moreover, as the resistivity of PdAu is much higher than
Au, Ti/PdAu bilayer will show a larger resistance than Ti/Au,
which allows sensors with smaller rise time and higher saturation
energy possibility[21]. The Tc is tuned by the thickness ratio of
Ti and PdAu layers. The nanoscale morphology and structure of
the interface between the two layers, and the electrical properties
are characterized.
II. EXPERIMENTAL DETAILS
A. Deposition of Ti/PdAu Thin Films
The superconducting Ti/PdAu bilayer films are deposited on
a silicon substrate in a magnetron sputtering system with a base
pressure of ∼10−6 Pa. A Ti target (99.995 at. %) and a PdAu
target with a mass ratio of 35 (Pd, 99.99 at. %): 65 (Au, 99.95 at.
%) are used as sources. The substrate is kept at 20°C during the
deposition process using a water-cooling system and rotated at 5
rpm to improve the uniformity of the film. The sputter pressure
is 0.1 Pa and the sputtering power is 200 W for both Ti and
PdAu targets. The PdAu film is deposited immediately after the
deposition of the Ti film to avoid the contamination of Ti film.
The thickness of the PdAu (dPdAu ) film is kept to 60 nm and the
dTi is changed from 50 nm to 70 nm.
B. Characterization of Ti/PdAu Thin Films
Focused ion beam milling is used to expose the cross section
of the bilayer film with a dual beam SEM/FIB system. In order to
2100404
Fig. 1. (a) Element distribution at the cross-section of the Ti (55nm)/PdAu
(60nm) bilayer film on a silicon substrate, with protective Pt films coated.
(b) Crystalline structure distribution at the interface.
protect the bilayer structure, two layers of Pt are prepared by an
electron beam and an ion beam deposition process, respectively.
Then the cross-section is characterized by a high-resolution
transmission electron microscope (HRTEM) and energy disper-
sive X-ray spectroscopy (EDS) to obtain element information
in each layer. X-ray diffraction (XRD) pattern of the films
are recorded on a Panalytical X’Pert PRO MRD diffractometer
using Cu λKα radiation (λ = 1.541874 Å) with the incidence
angle fixed at 0.5°. The 2θ range is from 10° to 90° with a
scanning step of 0.05°.
The surface roughness Rq (root mean square roughness) of
thin films is measured using a Veeco Dimension Icon system.
The data are acquired by scanning 2 µm × 2 µm area with 256
lines of resolution. The resistivity is mapped at room temper-
ature with a CDE Resmap 178 system based on the van der
Pauw method. Cryogenic performance of the films such as the
Tc and ΔTc is measured in a HPD adiabatic demagnetization
refrigerator (ADR) with an excitation current of 316 nA.
III. RESULTS AND DISCUSSION
A. Morphology of the Ti/PdAu Films
Fig. 1 shows the TEM image of the cross-section of a Ti
(55 nm) /PdAu (60 nm) bilayer film. Fig. 1(a) shows the clear
multi-layer Pt/PdAu/Ti/Si interface structure as marked with
different colors. The Pt protection layers are deposited before
the FIB milling process. There is no oxidized Ti layer between
the PdAu/Ti layers. The Ti films is uniform, Ti-PdAu interface
appears much smoother than the PdAu-Pt interface.
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IEEE TRANSACTIONS ON APPLIED SUPERCONDUCTIVITY, VOL. 32, NO. 4, JUNE 2022
TABLE I
PROPERTY SUMMARY EVALUATED IN THIS ARTICLE
Fig. 1(b) shows the crystalline structure distribution at the
interface between the Ti and PdAu layers. The upper gray area
corresponds to the cubic Ti (110) plane with a lattice spacing
of 2.34 Å, and the bottom deep dark area shows the cubic Pd
(111) plane with a lattice spacing of 2.25 Å and the cubic
Au (111) plane with a lattice spacing of 2.35 Å. The lattice
spacing of Ti (110) plane and Au (111) planes are very close,
which may be responsible for the instability of Ti/Au TESs.
The similar crystalline structure will induce the diffusion of
Au and Ti atoms. Pd atoms at the interface will decrease the
atom diffusion process by separating the Au and Ti atoms and
blocking the Au atom via the pinning effect [20]. The interface
between the superconducting Ti layer and the normal metal
PdAu layer plays an important role in the modulation of the
Tc due to the Usadel theory [22]. The interval time between
the deposition of PdAu and Ti is critical because Ti is easily
oxidated. The interface quality affects the critical temperature
and transition sharpness [23]. The thin Ti oxidation layer will
affect the proximity effect at the interface between the PdAu
and Ti layers making the critical temperature unpredictable. So,
based on our experimental results, the interval time should be
<10 s. It worth to notice that the area at intermediate layer in
Fig. 1(b) (marked with dashed oval) is Au phase with lattice
distortion, probably due to the interface, stress, and Ti doping
during deposition with such a short interval time.
The Rq of the films with 60 nm of PdAu and different thick-
nesses of Ti films (NIM-1 to NIM-4) are shown in Table I. As
shown, all the bilayer films show a similar roughness <1 nm,
which is equivalent or better than peer report of other kinds of
superconducting films for TES [13], [24]. The smooth surface
indicates the sputter factors are set at the suitable values. The Rq
is mainly due to the PdAu layer as shown in Fig. 1(a) considering
the smaller fluctuation in the surface of the Ti layer.
B. Structure and Phase
Fig. 2 shows the X-ray diffraction (XRD) pattern of a typical
Ti/PdAu film. Two intense preferential peaks of PdAu alloy
(Palladium, JCPDS card # 46-1043 and Gold, JCPDS card
# 04-0784) are clearly present at 2θ = 39.52° and 66.82°,
which correspond to the PdAu alloy crystal plane (111) and
(220). There are two weak signals at 2θ = 45.73° and 80.26°
which correspond to the PdAu alloy (200) and (311) planes,
respectively. Ti (211) planes (Titanium, JCPDS card # 44-1288)
shows a shoulder peak at 2θ = 69.48°, and another Ti (110) plane
should appear at 2θ = 38.48°, but it is unfortunately submerged
in the high-intensity signal of PdAu (111) plane. But there is
XU et al.: INVESTIGATION OF THE SUPERCONDUCTING Ti/PdAu BILAYER FILMS FOR TRANSITION EDGE SENSORS
Fig. 2. XRD pattern of a typical Ti/PdAu bilayer thin film.
Fig. 3. Thickness of Ti/PdAu bilayer thin film vs. effective resistivity.
clear evidence that Ti (110) plane exists as shown in Fig. 1(b).
Considering that PdAu alloy has a heavy density and can easily
scatter the X-ray, the weak XRD pattern signal of the Ti film is
predictable. The XRD is used to obtain macro-scale elementary
information of the sample.
C. Electrical Property
The resistivity of the films is strongly correlated with the
thickness ratio dTi /dPdAu as shown in Fig. 3 and Table I. The
dPdAu is fixed as 60 nm and the dTi is changed from 70 nm to
50 nm, named as NIM-1 to NIM-4 The effective resistivity ρeff
of the bilayer film is defined as R × (dPdAu + dTi ), where R is
the sheet resistance. The bilayer film could be considered as an
integrated structure, and the ρeff could exclude the thickness
effect of the single film. The resistivities of pure PdAu and
Ti films are 297 nΩm and 681 nΩm at room temperature,
respectively. As shown in Fig. 3, the ρeff increases with the ratio
dTi /dPdAu . NIM-1 shows the highest ρeff as 403 nΩm, and
NIM-4 shows the lowest one as 373 nΩm. The ρeff increases
towards to that of a pure Ti film as the dTi increases. The Ti/PdAu
bilayer film could keep relative high resistivity as a single film
of Ti.
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2100404
Fig. 4. The Tc of the Ti/PdAu bilayer thin films.
D. Cryogenic Property
The Tc and ΔTc of the measured films are shown in Fig. 4. The
PdAu film has suppressed the Tc of the Ti films via the proximity
effect. The Tc of PdAu/Ti bilayer decreases with the dTi . The
Tc of NIM-1, with the largest dTi /dPdAu ratio, is 335.6 mK,
showing a weakest proximity effect among 4 samples; inversely,
the Tc of NIM-4 is 175.3 mK with more intense proximity effect.
The ΔTc ranges from 0.9 mK to 4.7 mK. The theoretical energy
resolution (ΔE) and effective response time (τ eff ) of a TES, is
given by the following equations [25]:
 
4kTc2 C n/2
ΔE = 2.35 (1)
α
τth
τef f ∝ (2)
1 + αn
∂ log R
α= (3)
∂ log T
where k is the Boltzmann constant, Tc is the transition temper-
ature, C is the heat capacity of TES, α is the thermal sensitivity
of superconducting thin film, n is an exponent factor of thermal
conductance, τ th is thermal time constant, respectively.
With narrow ΔTc and higher value of resistance, the transition
zone has a sharp and linear edge, which represent higher thermal
sensitivity α and current sensitivity. With these properties our
TES has the potential to obtain improved ΔE and smaller τ eff .
IV. CONCLUSION
In this paper we have presented a new kind of Ti/PdAu
superconducting bilayer films suitable for the development of
TESs. The Tc of the films could be tuned between 336-175 mK
as the dTi /dPdAu decreases. The resistivity keeps as large as Ti
film, in the meanwhile the Tc and ΔTc are lowered, which will
be beneficial to improve the energy resolution of single photon
detection.
ACKNOWLEDGMENT
The author would like to thank Mrs Q. Zhong at NIM for
helpful discussion.
2100404 IEEE TRANSACTIONS ON APPLIED SUPERCONDUCTIVITY, VOL. 32, NO. 4, JUNE 2022
REFERENCES
[1] W. Zhang, W. Miao, K. M. Zhou, X. H. Guo, J. Q. Zhong, and S. C. Shi,
High Sensitive THz Superconducting Hot Electron Bolometer Mixers and
Transition Edge Sensors, Bellingham, WA, USA: SPIE, 2016.
[2] E. Taralli et al., “Reduced active area in transition-edge sensors for
visible-NIR photon detection: A comparison of experimental data and
two-fluid model,” IEEE Trans. Appl. Supercond., vol. 25, no. 3, Jun. 2015,
Art. no. 2200304.
[3] F. T. Jaeckel et al., “Energy calibration of high-resolution X-Ray TES mi-
crocalorimeters with 3 eV optical photons,” IEEE Trans. Appl. Supercond.,
vol. 29, no. 5, May 2019, Art. no. 2100104.
[4] F. T. Jaeckel, L. N. Le, K. W. Martin, and S. T. P. Boyd, “Development of a
precision scanning optical pulser for low-temperature particle detectors,”
IEEE Trans. Appl. Supercond., vol. 23, no. 3, Jun. 2013, Art. no. 1301005.
[5] K. Hattori, S. Inoue, R. Kobayashi, K. Niwa, T. Numata, and D. Fukuda,
“Optical transition-edge sensors: Dependence of system detection ef-
ficiency on wavelength,” IEEE Trans. Instrum. Meas., vol. 68, no. 6,
pp. 2253–2259, Jun. 2019.
[6] A. J. Miller, A. E. Lita, B. Calkins, I. Vayshenker, S. M. Gruber, and S. W.
Nam, “Compact cryogenic self-aligning fiber-to-detector coupling with
losses below one percent,” Opt. Exp., vol. 19, no. 10, 2011, Art. no. 9102.
[7] A. E. Lita, B. Calkins, L. A. Pellochoud, A. J. Miller, and S. Nam,
“High-efficiency photon-number-resolving detectors based on hafnium
transition-edge sensors,” in Proc. AIP Conf., 2009, pp. 351–354.
[8] X. Xu et al., “Investigation of superconducting titanium films for transition
edge sensors,” in Proc. Conf. Precis. Electromagn. Meas., 2020, pp. 1–2.
[9] C. Portesi, E. Taralli, L. Lolli, M. Rajteri, and E. Monticone, “Fabrication
and characterization of fast TESs with small area for single photon
counting,” IEEE Trans. Appl. Supercond., vol. 25, no. 3, Jun. 2015,
Art. no. 2101004M.
[10] J. A. Bonetti et al., “Characterization of antenna-coupled tes bolometers
for the spider experiment,” IEEE Trans. Appl. Supercond., vol. 19, no. 3,
pp. 520–523, Jun. 2009.
[11] D. Vaccaro et al., “Tuning the Tc of titanium thin films for transition-edge
sensors by annealing in argon,” J. Low Temp. Phys., vol. 193, no. 5/6,
pp. 1122–1128, 2018.
[12] J. E. Sadleir et al., “Proximity effects and nonequilibrium superconduc-
tivity in transition-edge sensors,” Phys. Rev. B - Condens. Matter Mater.
Phys., vol. 84, no. 18, pp. 1–9, 2011.
Authorized licensed use limited to: Universidad de Sonora. Downloaded on January 12,2024 at 21:40:58 UTC from IEEE Xplore. Restrictions apply.
[13] F. T. Jaeckel, K. L. Kripps, K. M. Morgan, S. Zhang, and D. McCammon,
“Fabrication of superconducting Mo/Cu bilayers using ion-beam-assisted
e-beam evaporation,” J. Low Temp. Phys., vol. 184, no. 3/4, pp. 647–653,
Aug. 2016.
[14] M. Parra-Borderias et al., “Characterization of a Mo/Au thermometer
for ATHENA,” IEEE Trans. Appl. Supercond., vol. 23, no. 3, Jun. 2013,
Art. no. 2300405.
[15] F. W. Carter et al., “Tuning SPT-3G transition-edge-sensor electrical
properties with a four-layer Ti–Au–Ti–Au thin-film stack,” J. Low Temp.
Phys., vol. 193, no. 5/6, pp. 695–702, 2018.
[16] L. Lolli, E. Taralli, C. Portesi, M. Rajteri, and E. Monticone, “Aluminum–
titanium bilayer for near-infrared transition edge sensors,” Sensors, vol. 16,
no. 7, Jun. 2016, Art. no. 953.
[17] R. Hennings-Yeomans et al., “Controlling Tc of iridium films using
interfacial proximity effects,” pp. 1–5, Nov. 2017, arXiv:1711.03648.
[18] B. N. Ganguly, “Superconductivity in palladium-noble metal-hydrogen
systems,” Zeitschrift für Phys. B Condens. Matter, vol. 22, no. 2,
pp. 127–132, Jun. 1975.
[19] D. D. Awschalom et al., “Low-noise modular microsusceptometer using
nearly quantum limited dc SQUIDs,” Appl. Phys. Lett., vol. 53, no. 21,
pp. 2108–2110, 1988.
[20] X. Wang, B. Tang, X. Huang, Y. Ma, and Z. Zhang, “High activity of novel
nanoporous Pd-Au catalyst for methanol electro-oxidation in alkaline
media,” J. Alloys Compounds, vol. 565, pp. 120–126, 2013.
[21] E. Taralli, C. Portesi, R. Rocci, M. Rajteri, and E. Monticone, “Investi-
gation of Ti/Pd bilayer for single photon detection,” IEEE Trans. Appl.
Supercond., vol. 19, no. 3, pp. 493–495, Jun. 2009.
[22] J. M. Martinis, G. C. Hilton, K. D. Irwin, and D. A. Wollman, “Calcu-
lation of Tc in a normal-superconductor bilayer using the microscopic-
based usadel theory,” Nucl. Instruments Methods Phys. Res. Sect. A
Accel. Spectrometers Detect. Assoc. Equip., vol. 444, no. 1, pp. 23–27,
2000.
[23] X. Xu et al., “Influence of the interface composition to the superconductiv-
ity of Ti/PdAu films,” Nanomaterials, vol. 11, no. 1, Dec. 2021, Art. no. 39.
[24] V. Yefremenko et al., “Impact of electrical contacts design and materials on
the stability of Ti superconducting transition shape,” J. Low Temp. Phys.,
vol. 193, no. 5/6, pp. 732–738, Dec. 2018.
[25] D. McCammon et al., Cryogenic Particle Detection, vol. 99. Berlin,
Germany: Springer, 2005.