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"639/638/298/917"
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Discovery of high-performance low-cost n-type Mg3Sb2-based thermoelectric materials with multi-valley conduction bands
by
Zhang, Jiawei
,
Pedersen, Steffen Hindborg
,
Hung, Le Thanh
in
639/301/299/2736
,
639/638/298/917
,
Heat conductivity
2017
Widespread application of thermoelectric devices for waste heat recovery requires low-cost high-performance materials. The currently available n-type thermoelectric materials are limited either by their low efficiencies or by being based on expensive, scarce or toxic elements. Here we report a low-cost n-type material, Te-doped Mg
3
Sb
1.5
Bi
0.5
, that exhibits a very high figure of merit
zT
ranging from 0.56 to 1.65 at 300−725 K. Using combined theoretical prediction and experimental validation, we show that the high thermoelectric performance originates from the significantly enhanced power factor because of the multi-valley band behaviour dominated by a unique near-edge conduction band with a sixfold valley degeneracy. This makes Te-doped Mg
3
Sb
1.5
Bi
0.5
a promising candidate for the low- and intermediate-temperature thermoelectric applications.
Zintl-phase thermoelectrics are predominantly p-type. Here, Zhang
et al
. use tellurium to n-dope Mg
3
Sb
1.5
Bi
0.5
and obtain thermoelectric figures of merit up to 1.6 at 700 K. Calculations show that these performances result from a conduction band with sixfold valley degeneracy.
Journal Article
Large, non-saturating magnetoresistance in WTe2
by
Schoop, Leslie M.
,
Flynn, Steven
,
Liang, Tian
in
639/301/119/997
,
639/638/298/917
,
639/766/119/997
2014
The magnetoresistance effect in WTe
2
, a layered semimetal, is extremely large: the electrical resistance can be changed by more than 13 million per cent at very high magnetic fields and low temperatures.
Titanic magnetoresistance in WTe
2
Apply a magnetic field to a magnetoresistive material and its electrical resistance changes — a technologically useful phenomenon that is harnessed, for example, in the data-reading sensors of hard drives. Mazhar Ali and colleagues have now identified a material (tungsten ditelluride or WTe
2
) in which the magnetoresistance effect is unusually large: the electrical resistance can be changed by more than 13 million per cent. Its remarkable magnetoresitance is evident at very high magnetic fields and at extremely low temperatures, so practical applications are not yet in prospect. But this finding suggests new directions in the study of magnetoresistivity that could ultimately lead to new uses of this effect.
Magnetoresistance is the change in a material’s electrical resistance in response to an applied magnetic field. Materials with large magnetoresistance have found use as magnetic sensors
1
, in magnetic memory
2
, and in hard drives
3
at room temperature, and their rarity has motivated many fundamental studies in materials physics at low temperatures
4
. Here we report the observation of an extremely large positive magnetoresistance at low temperatures in the non-magnetic layered transition-metal dichalcogenide WTe
2
: 452,700 per cent at 4.5 kelvins in a magnetic field of 14.7 teslas, and 13 million per cent at 0.53 kelvins in a magnetic field of 60 teslas. In contrast with other materials, there is no saturation of the magnetoresistance value even at very high applied fields. Determination of the origin and consequences of this effect, and the fabrication of thin films, nanostructures and devices based on the extremely large positive magnetoresistance of WTe
2
, will represent a significant new direction in the study of magnetoresistivity.
Journal Article
Highly efficient luminescence from space-confined charge-transfer emitters
by
Liao, Liang-Sheng
,
Qu, Yang-Kun
,
Auras, Florian
in
639/624/1020/1091
,
639/638/298/917
,
Biomaterials
2020
Charge-transfer (CT) complexes, formed by electron transfer from a donor to an acceptor, play a crucial role in organic semiconductors. Excited-state CT complexes, termed exciplexes, harness both singlet and triplet excitons for light emission, and are thus useful for organic light-emitting diodes (OLEDs). However, present exciplex emitters often suffer from low photoluminescence quantum efficiencies (PLQEs), due to limited control over the relative orientation, electronic coupling and non-radiative recombination channels of the donor and acceptor subunits. Here, we use a rigid linker to control the spacing and relative orientation of the donor and acceptor subunits, as demonstrated with a series of intramolecular exciplex emitters based on 10-phenyl-9,10-dihydroacridine and 2,4,6-triphenyl-1,3,5-triazine. Sky-blue OLEDs employing one of these emitters achieve an external quantum efficiency (EQE) of 27.4% at 67 cd m
−2
with only minor efficiency roll-off (EQE = 24.4%) at a higher luminous intensity of 1,000 cd m
−2
. As a control experiment, devices using chemically and structurally related but less rigid emitters reach substantially lower EQEs. These design rules are transferrable to other donor/acceptor combinations, which will allow further tuning of emission colour and other key optoelectronic properties.
The use of rigid linkers to control the relative position and interaction of donor and acceptor units in exciplex emitters leads to the realization of organic light-emitting devices with enhanced external quantum efficiency.
Journal Article
High-performance thermoelectrics and challenges for practical devices
2022
Thermoelectric materials can be potentially employed in solid-state devices that harvest waste heat and convert it to electrical power, thereby improving the efficiency of fuel utilization. The spectacular increases in the efficiencies of these materials achieved over the past decade have raised expectations regarding the use of thermoelectric generators in various energy saving and energy management applications, especially at mid to high temperature (400–900 °C). However, several important issues that prevent successful thermoelectric generator commercialization remain unresolved, in good part because of the lack of a research roadmap.
Thermoelectric materials can generate energy from a heat differential. This Review provides an overview of mid- to high-temperature thermoelectrics, their application in modules, and the issues that need to be addressed to enable commercial implementation of state-of-the-art materials.
Journal Article
Reducing the efficiency–stability–cost gap of organic photovoltaics with highly efficient and stable small molecule acceptor ternary solar cells
by
Durrant, James R.
,
Abdelsamie, Maged
,
Holliday, Sarah
in
140/125
,
639/301/299/946
,
639/638/298/917
2017
Technological deployment of organic photovoltaic modules requires improvements in device light-conversion efficiency and stability while keeping material costs low. Here we demonstrate highly efficient and stable solar cells using a ternary approach, wherein two non-fullerene acceptors are combined with both a scalable and affordable donor polymer, poly(3-hexylthiophene) (P3HT), and a high-efficiency, low-bandgap polymer in a single-layer bulk-heterojunction device. The addition of a strongly absorbing small molecule acceptor into a P3HT-based non-fullerene blend increases the device efficiency up to 7.7 ± 0.1% without any solvent additives. The improvement is assigned to changes in microstructure that reduce charge recombination and increase the photovoltage, and to improved light harvesting across the visible region. The stability of P3HT-based devices in ambient conditions is also significantly improved relative to polymer:fullerene devices. Combined with a low-bandgap donor polymer (PBDTTT-EFT, also known as PCE10), the two mixed acceptors also lead to solar cells with 11.0 ± 0.4% efficiency and a high open-circuit voltage of 1.03 ± 0.01 V.
Ternary organic blends using two non-fullerene acceptors are shown to improve the efficiency and stability of low-cost solar cells based on P3HT and of high-performance photovoltaic devices based on low-bandgap donor polymers.
Journal Article
A sodium-ion sulfide solid electrolyte with unprecedented conductivity at room temperature
2019
Solid electrolytes are key materials to enable solid-state rechargeable batteries, a promising technology that could address the safety and energy density issues. Here, we report a sulfide sodium-ion conductor, Na
2.88
Sb
0.88
W
0.12
S
4
, with conductivity superior to that of the benchmark electrolyte, Li
10
GeP
2
S
12
. Partial substitution of antimony in Na
3
SbS
4
with tungsten introduces sodium vacancies and tetragonal to cubic phase transition, giving rise to the highest room-temperature conductivity of 32 mS cm
−1
for a sintered body, Na
2.88
Sb
0.88
W
0.12
S
4
. Moreover, this sulfide possesses additional advantages including stability against humid atmosphere and densification at much lower sintering temperatures than those (>1000 °C) of typical oxide sodium-ion conductors. The discovery of the fast sodium-ion conductors boosts the ongoing research for solid-state rechargeable battery technology with high safety, cost-effectiveness, large energy and power densities.
Solid-state rechargeable batteries using solid electrolytes instead of liquid ones could address the safety and energy density issues. Here the authors report a Na-ion solid electrolyte Na
2.88
Sb
0.88
W
0.12
S
4
which exhibits record high ionic conductivity of 32 mS/cm at room temperature.
Journal Article
Ligand-engineered bandgap stability in mixed-halide perovskite LEDs
2021
Lead halide perovskites are promising semiconductors for light-emitting applications because they exhibit bright, bandgap-tunable luminescence with high colour purity
1
,
2
. Photoluminescence quantum yields close to unity have been achieved for perovskite nanocrystals across a broad range of emission colours, and light-emitting diodes with external quantum efficiencies exceeding 20 per cent—approaching those of commercial organic light-emitting diodes—have been demonstrated in both the infrared and the green emission channels
1
,
3
,
4
. However, owing to the formation of lower-bandgap iodide-rich domains, efficient and colour-stable red electroluminescence from mixed-halide perovskites has not yet been realized
5
,
6
. Here we report the treatment of mixed-halide perovskite nanocrystals with multidentate ligands to suppress halide segregation under electroluminescent operation. We demonstrate colour-stable, red emission centred at 620 nanometres, with an electroluminescence external quantum efficiency of 20.3 per cent. We show that a key function of the ligand treatment is to ‘clean’ the nanocrystal surface through the removal of lead atoms. Density functional theory calculations reveal that the binding between the ligands and the nanocrystal surface suppresses the formation of iodine Frenkel defects, which in turn inhibits halide segregation. Our work exemplifies how the functionality of metal halide perovskites is extremely sensitive to the nature of the (nano)crystalline surface and presents a route through which to control the formation and migration of surface defects. This is critical to achieve bandgap stability for light emission and could also have a broader impact on other optoelectronic applications—such as photovoltaics—for which bandgap stability is required.
The binding of multidentate ligands to the surface of lead halide perovskite nanocrystals suppresses the formation of surface defects that result in halide segregation, yielding materials with efficient and colour-stable red emission.
Journal Article
Compositional engineering of perovskite materials for high-performance solar cells
by
Seo, Jangwon
,
Kim, Young Chan
,
Seok, Sang Il
in
639/301/299/946
,
639/624/1075/524
,
639/638/298/917
2015
Inorganic–organic lead halide perovskite could be efficient when used as the light-harvesting component of solar cells; here incorporation of methylammonium lead bromide into formamidinium lead iodide stabilizes the perovskite and improves the power conversion efficiency of the solar cell up to 17.9 per cent.
High-performance perovskites solar cells
Inorganic–organic lead halide perovskites are currently attracting considerable interest for solar-cell applications. Most of the best performing perovskite solar cells to date have made use of methylammonium-based perovskites; formamidinium-based perovskites have also shown promise, but are not as stable. Now Nam Joong Jeon and colleagues show that the formamidinium-based perovskites can be stabilized by the addition of some methylammonium-based perovskite, and that solar cells incorporating the resulting compositionally tuned materials can reach new heights of efficiency.
Of the many materials and methodologies aimed at producing low-cost, efficient photovoltaic cells, inorganic–organic lead halide perovskite materials
1
,
2
,
3
,
4
,
5
,
6
,
7
,
8
,
9
,
10
,
11
,
12
,
13
,
14
,
15
,
16
,
17
appear particularly promising for next-generation solar devices owing to their high power conversion efficiency. The highest efficiencies reported for perovskite solar cells so far have been obtained mainly with methylammonium lead halide materials
1
,
2
,
3
,
4
,
5
,
6
,
7
,
8
,
9
,
10
. Here we combine the promising—owing to its comparatively narrow bandgap—but relatively unstable formamidinium lead iodide (FAPbI
3
) with methylammonium lead bromide (MAPbBr
3
) as the light-harvesting unit in a bilayer solar-cell architecture
13
. We investigated phase stability, morphology of the perovskite layer, hysteresis in current–voltage characteristics, and overall performance as a function of chemical composition. Our results show that incorporation of MAPbBr
3
into FAPbI
3
stabilizes the perovskite phase of FAPbI
3
and improves the power conversion efficiency of the solar cell to more than 18 per cent under a standard illumination of 100 milliwatts per square centimetre. These findings further emphasize the versatility and performance potential of inorganic–organic lead halide perovskite materials for photovoltaic applications.
Journal Article
Thermally conductive ultra-low-k dielectric layers based on two-dimensional covalent organic frameworks
by
Rahn, Matthew S.
,
McGaughey, Alan J. H.
,
Bartnof, Matthew
in
140/125
,
140/131
,
639/301/357/1018
2021
As the features of microprocessors are miniaturized, low-dielectric-constant (low-
k
) materials are necessary to limit electronic crosstalk, charge build-up, and signal propagation delay. However, all known low-
k
dielectrics exhibit low thermal conductivities, which complicate heat dissipation in high-power-density chips. Two-dimensional (2D) covalent organic frameworks (COFs) combine immense permanent porosities, which lead to low dielectric permittivities, and periodic layered structures, which grant relatively high thermal conductivities. However, conventional synthetic routes produce 2D COFs that are unsuitable for the evaluation of these properties and integration into devices. Here, we report the fabrication of high-quality COF thin films, which enable thermoreflectance and impedance spectroscopy measurements. These measurements reveal that 2D COFs have high thermal conductivities (1 W m
−1
K
−1
) with ultra-low dielectric permittivities (
k
= 1.6). These results show that oriented, layered 2D polymers are promising next-generation dielectric layers and that these molecularly precise materials offer tunable combinations of useful properties.
Low-
k
dielectric materials are essential to allow continued electronics miniaturization, but their low thermal conductivity limits performance. Here, two-dimensional covalent organic frameworks are shown to combine high thermal conductivity with a low dielectric constant.
Journal Article
Evidence for ion migration in hybrid perovskite solar cells with minimal hysteresis
by
O’Regan, Brian C.
,
Calado, Philip
,
Bryant, Daniel
in
639/301/1005/1007
,
639/301/299/946
,
639/638/298/917
2016
Ion migration has been proposed as a possible cause of photovoltaic current–voltage hysteresis in hybrid perovskite solar cells. A major objection to this hypothesis is that hysteresis can be reduced by changing the interfacial contact materials; however, this is unlikely to significantly influence the behaviour of mobile ionic charge within the perovskite phase. Here, we show that the primary effects of ion migration can be observed regardless of whether the contacts were changed to give devices with or without significant hysteresis. Transient optoelectronic measurements combined with device simulations indicate that electric-field screening, consistent with ion migration, is similar in both high and low hysteresis CH
3
NH
3
PbI
3
cells. Simulation of the photovoltage and photocurrent transients shows that hysteresis requires the combination of both mobile ionic charge and recombination near the perovskite-contact interfaces. Passivating contact recombination results in higher photogenerated charge concentrations at forward bias which screen the ionic charge, reducing hysteresis.
Ion migration has been related to hysteresis in perovskite solar cells, but not all perovskite cells exhibit a hysteresis. Here, Calado
et al
. show that ion migration occurs regardless of hysteresis, but photogenerated carriers screen the effects of ionic charge for some solar cell architectures.
Journal Article