Nanostructured YbAgCu
4
for Potentially Cryogenic Thermoelectric
Cooling
Machhindra Koirala,
†
Hui Wang,
†
Mani Pokharel,
‡
Yucheng Lan,
†
Chuanfei Guo,
†
Cyril Opeil,
‡
and Zhifeng Ren
†,
*
†
Department of Physics and TcSUH, University of Houston, Houston, Texas 77204, United States
‡
Department of Physics, Boston College, Chesnut Hill, Massachusetts 02467, United States
ABSTRACT: We have studied the thermoelectric properties
of nanostructured YbAgCu
4
materials. A high power factor of
∼131 μW cm
-1
K
-2
has been obtained at 22 K for
nanostructured samples prepared by ball milling the arc
melted ingot into nanopowder and hot pressing the nano-
powder. The implementation of nanostructuring method
decreased the thermal conductivity at 42 K by 30-50%
through boundary scattering comparing with the previously
reported value of polycrystalline YbAgCu
4
. A peak dimension-
less thermoelectric figure-of-merit, ZT, of 0.11 has been
achieved at 42 K, which may find potential applications for
cryogenic cooling below 77 K. The nanostructuring approach
can be extended to other heavy Fermion materials to achieve high power factor and low thermal conductivity and ultimately
higher ZT.
KEYWORDS: Thermoelectric, heavy Fermions, Kondo lattice, boundary scattering, YbAgCu
4
T
he ability of thermoelectric (TE) materials for converting
heat into electricity and vice versa is very important for
power generation
1,2
as well as solid-state cooling.
3
For the
aerospace program where the weight and size compatibility of
the devices is important, thermoelectric devices are more useful
for cryogenic application in comparison to other heavy cooling
devices. The power generation efficiency or coefficient of
performance of thermoelectric devices are determined by the
dimensionless figure of merit, ZT = [(S
2
σ)/κ]T, where S is the
Seebeck coefficient, σ is the electrical conductivity, κ is the
thermal conductivity, and T is the absolute temperature.
4-6
All
of these quantities are related to each other and changing one
affects the others, so increasing ZT is really challenging. In the
recent years, the development of new techniques for controlling
the material properties through nanostructuring,
7
modulation
doping,
8,9
resonant doping,
10,11
and band engineering near
Fermi level
12,13
have helped to enhance ZT significantly. The
rapid development of technologies enabled to increases ZT
above 1 for cooling applications at around room temperature
and power generation at high temperatures but at the low-
temperature (cryogenic) range, the existing ZT is far below the
application requirement.
For low-temperature thermoelectric materials, most of the
focus is toward narrow band gap semiconductors and Kondo
insulators. In different temperature ranges below room
temperature, there are many materials that are being
investigated. The well-known low-temperature thermoelectric
material is single crystal Bi
1-x
Sb
x
with ZT ∼ 0.5 at ∼150 K.
14
Encapsulating Ce in clathrate has enhanced ZT to 0.1 at 150
K.
15
Doping on extremely high mobility materials CuAgSe has
enhanced ZT to 0.1 at 100 K.
16
Doped FeSi have been reported
to have peak ZT of 0.12 at 120 K.
17
However, the operating
temperature for these materials is above 100 K, which is above
liquid nitrogen temperature, 77 K. For temperature below 77 K,
ZT is very low because the temperature T is very small.
The current trend for cryogenic thermoelectric materials
involves mostly Kondo insulators like FeSb
2
,
18-20
CrSb
2
,
21
and
some rare earth Kondo systems like YbAl
3
,
22
CeCu
6
,
23
Ce
0.5
La
0.5
Al
3
,
24
YbCuAl,
25
CeAl
3
,
25
CePd
3
,
26
and so forth.
Rare earth metallic heavy Fermions like YbAl
3
, CePd
3
26
have
been investigated to the temperature range of 150 K and a peak
ZT ∼ 0.23 have been reported for both n- and p-type. Our
focus in this work is to study materials having good ZT at
below 77 K. FeSb
2
was studied for its giant Seebeck coefficient
below 77 K by Bentein.
18
Much effort have been made on that
materials but the optimized ZT is not more than 0.026.
18-20,27
In phonon drag systems like FeSb
2
28
and CrSb
2
, it is very
difficult to decouple the electrical and phonon part and the
value of ZT remains low. There are some rare earth Kondo
systems with good power factor at temperature below 77 K, but
they have high thermal conductivity so the overall ZT is low.
Maintaining that high power factor and reducing thermal
conductivity is really challenging.
Received: April 17, 2014
Revised: July 17, 2014
Published: July 31, 2014
Letter
pubs.acs.org/NanoLett
© 2014 American Chemical Society 5016 dx.doi.org/10.1021/nl501436w | Nano Lett. 2014, 14, 5016-5020