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In topological magnetic materials, the topology of the electronic wave function is strongly coupled to the structure of the magnetic order. In general, ferromagnetic Weyl semimetals generate a strong anomalous Hall conductivity (AHC) due to a large Berry curvature that scales with their magnetization. In contrast, a comparatively small AHC is observed in noncollinear antiferromagnets. We investigated HoAgGe, an antiferromagnetic (AFM) Kagome spin-ice compound, which crystallizes in a hexagonal ZrNiAl-type structure in which Ho atoms are arranged in a distorted Kagome lattice, forming an intermetallic Kagome spin-ice state in the ab-plane. It exhibits a large topological Hall resistivity of ~1.6 µΩ-cm at 2.0 K in a field of ~3 T owing to the noncoplanar structure. Interestingly, a total AHC of 2,800 Ω-1 is observed at ~45 K, i.e., 4 TN, which is quite unusual and goes beyond the normal expectation considering HoAgGe as an AFM Kagome spin-ice compound with a TN of ~11 K. We demonstrate further that the AHC below TN results from the nonvanishing Berry curvature generated by the formation of Weyl points under the influence of the external magnetic field, while the skew scattering led by Kagome spins dominates above the TN. These results offer a unique opportunity to study frustration in AFM Kagome lattice compounds. [ABSTRACT FROM AUTHOR]

Weyl semimetal is a unique topological phase with topologically protected band crossings in the bulk and robust surface states called Fermi arcs. Weyl nodes always appear in pairs with opposite chiralities, and they need to have either time‐reversal or inversion symmetry broken. When the time‐reversal symmetry is broken the minimum number of Weyl points (WPs) is two. If these WPs are located at the Fermi level, they form an ideal Weyl semimetal (WSM). In this study, intrinsic ferromagnetic (FM) EuCd2As2 are grown, predicted to be an ideal WSM and studied its electronic structure by angle‐resolved photoemission spectroscopy, and scanning tunneling microscopy which agrees closely with the first principles calculations. Moreover, anomalous Hall conductivity and Nernst effect are observed, resulting from the non‐zero Berry curvature, and the topological Hall effect arising from changes in the band structure caused by spin canting produced by magnetic fields. These findings can help realize several exotic quantum phenomena in inorganic topological materials that are otherwise difficult to assess because of the presence of multiple pairs of Weyl nodes. [ABSTRACT FROM AUTHOR]

Mechanical stirring of bulk Te in N‐methyl‐2‐pyrrolidone (NMP) solution at room temperature resulted in the formation of free‐standing few‐layer (∼1.2–2.8 nm) crystalline ultrathin nanosheets of tellurene with a large lateral thickness (∼1–1.6 μm) as confirmed by atomic force microscopy (AFM). High‐resolution transmission electron microscopy (HRTEM) confirms the presence of α‐ and β‐phases of tellurene. First‐principle density functional theoretical (DFT) based electronic structure calculations demonstrate the indirect band gap of bi‐layer β‐tellurene. The band gap decreases with increasing number of layers in the tellurene nanosheet. [ABSTRACT FROM AUTHOR]

Orthorhombic GeSe is a promising thermoelectric material. However, large band gap and strong covalent bonding result in a low thermoelectric figure of merit, zT≈0.2. Here, we demonstrate a maximum zT≈1.35 at 627 K in p‐type polycrystalline rhombohedral (GeSe)0.9(AgBiTe2)0.1 , which is the highest value reported among GeSe based materials. The rhombohedral phase is stable in ambient conditions for x=0.8–0.29 in (GeSe)1−x(AgBiTe2)x. The structural transformation accompanies change from covalent bonding in orthorhombic GeSe to metavalent bonding in rhombohedral (GeSe)1−x(AgBiTe2)x. (GeSe)0.9(AgBiTe2)0.1 has closely lying primary and secondary valence bands (within 0.25–0.30 eV), which results in high power factor 12.8 μW cm−1 K−2 at 627 K. It also exhibits intrinsically low lattice thermal conductivity (0.38 Wm−1 K−1 at 578 K). Theoretical phonon dispersion calculations reveal vicinity of a ferroelectric instability, with large anomalous Born effective charges and high optical dielectric constant, which, in concurrence with high effective coordination number, low band gap and moderate electrical conductivity, corroborate metavalent bonding in (GeSe)0.9(AgBiTe2)0.1. We confirmed the presence of low energy phonon modes and local ferroelectric domains using heat capacity measurement (3–30 K) and switching spectroscopy in piezoresponse force microscopy, respectively. [ABSTRACT FROM AUTHOR]

Orthorhombic GeSe is a promising thermoelectric material. However, large band gap and strong covalent bonding result in a low thermoelectric figure of merit, zT≈0.2. Here, we demonstrate a maximum zT≈1.35 at 627 K in p‐type polycrystalline rhombohedral (GeSe)0.9(AgBiTe2)0.1 , which is the highest value reported among GeSe based materials. The rhombohedral phase is stable in ambient conditions for x=0.8–0.29 in (GeSe)1−x(AgBiTe2)x. The structural transformation accompanies change from covalent bonding in orthorhombic GeSe to metavalent bonding in rhombohedral (GeSe)1−x(AgBiTe2)x. (GeSe)0.9(AgBiTe2)0.1 has closely lying primary and secondary valence bands (within 0.25–0.30 eV), which results in high power factor 12.8 μW cm−1 K−2 at 627 K. It also exhibits intrinsically low lattice thermal conductivity (0.38 Wm−1 K−1 at 578 K). Theoretical phonon dispersion calculations reveal vicinity of a ferroelectric instability, with large anomalous Born effective charges and high optical dielectric constant, which, in concurrence with high effective coordination number, low band gap and moderate electrical conductivity, corroborate metavalent bonding in (GeSe)0.9(AgBiTe2)0.1. We confirmed the presence of low energy phonon modes and local ferroelectric domains using heat capacity measurement (3–30 K) and switching spectroscopy in piezoresponse force microscopy, respectively. [ABSTRACT FROM AUTHOR]

High thermoelectric performance is generally achieved through either electronic structure modulations or phonon scattering enhancements, which often counteract each other. A leap in performance requires innovative strategies that simultaneously optimize electronic and phonon transports. We demonstrate high thermoelectric performance with a near room-temperature figure of merit, ZT ~ 1.5, and a maximum ZT ~ 2.6 at 573 kelvin, by optimizing atomic disorder in cadmium-doped polycrystalline silver antimony telluride (AgSbTe2). Cadmium doping in AgSbTe2 enhances cationic ordering, which simultaneously improves electronic properties by tuning disorder-induced localization of electronic states and reduces lattice thermal conductivity through spontaneous formation of nanoscale (~2 to 4 nanometers) superstructures and coupling of soft vibrations localized within ~1 nanometer around cadmium sites with local strain modulation. The strategy is applicable to most other thermoelectric materials that exhibit inherent atomic disorder. [ABSTRACT FROM AUTHOR]

The discovery of topological insulators with unique metallic surface states has added a new dimension in the field of electronics and spintronics. Following the initial breakthrough, the topologically non-trivial materials have been extended to various categories namely weak topological insulator, topological crystalline insulator, Dirac semimetal and Weyl semimetal. Interestingly, most of the topological materials are also good candidates for thermoelectric energy conversion because both demand similar material features such as heavy constituent elements, narrow band gap, and high spin-orbit coupling. Heavy metal chalcogenides satisfy these criteria and present a nice platform for exploring both thermoelectrics and topological insulation. Here, we present a brief overview of both topological materials and thermoelectrics with examples based on heavy metal chalcogenides from the perception of a solid-state chemist. Last part of this review deals with the major challenges at the intersection of these two fields and possible solutions to establish the strong correlation between topological and thermoelectric materials. Image 1 • Topological and thermoelectric materials demand heavy constituent elements, narrow bandgap and strong spin-orbit coupling. • Overview of both topological material and thermoelectrics based on heavy metal chalcogenides is discussed. • Thermoelectric properties of various topological materials such as TI, WTI, TCI and WSM are discussed. [ABSTRACT FROM AUTHOR]

The realization of n‐type Ge chalcogenides is elusive owing to intrinsic Ge vacancies that make them p‐type semiconductors. GeSe crystallizes into a layered orthorhombic structure similar to SnSe at ambient conditions. The high‐symmetry cubic phase of GeSe is predicted to be stabilized by applying 7 GPa external pressure or by enhancing the entropy by increasing to temperature to 920 K. Stabilization of the n‐type cubic phase of GeSe at ambient conditions was achieved by alloying with AgBiSe2 (30–50 mol %), enhancing the entropy through solid solution mixing. The interplay of positive and negative chemical pressure anomalously changes the band gap of GeSe with increasing the AgBiSe2 concentration. The band gap of n‐type cubic (GeSe)1−x(AgBiSe2)x (0.30≤x≤0.50) has a value in the 0.3–0.4 eV range, which is significantly lower than orthorhombic GeSe (1.1 eV). Cubic (GeSe)1−x(AgBiSe2)x exhibits an ultralow lattice thermal conductivity (κL≈0.43 W m−1 K−1) in the 300–723 K range. The low κL is attributed to significant phonon scattering by entropy‐driven enhanced solid‐solution point defects. [ABSTRACT FROM AUTHOR]

The realization of n‐type Ge chalcogenides is elusive owing to intrinsic Ge vacancies that make them p‐type semiconductors. GeSe crystallizes into a layered orthorhombic structure similar to SnSe at ambient conditions. The high‐symmetry cubic phase of GeSe is predicted to be stabilized by applying 7 GPa external pressure or by enhancing the entropy by increasing to temperature to 920 K. Stabilization of the n‐type cubic phase of GeSe at ambient conditions was achieved by alloying with AgBiSe2 (30–50 mol %), enhancing the entropy through solid solution mixing. The interplay of positive and negative chemical pressure anomalously changes the band gap of GeSe with increasing the AgBiSe2 concentration. The band gap of n‐type cubic (GeSe)1−x(AgBiSe2)x (0.30≤x≤0.50) has a value in the 0.3–0.4 eV range, which is significantly lower than orthorhombic GeSe (1.1 eV). Cubic (GeSe)1−x(AgBiSe2)x exhibits an ultralow lattice thermal conductivity (κL≈0.43 W m−1 K−1) in the 300–723 K range. The low κL is attributed to significant phonon scattering by entropy‐driven enhanced solid‐solution point defects. n‐Type cubic GeSe has been stabilized at ambient conditions by entropy‐driven formation of a solid solution with AgBiSe2. It demonstrated promising thermoelectric properties with ultralow thermal conductivity. Upon increasing the AgBiSe2 concentration in GeSe, the band gap of the system changes anomalously. [ABSTRACT FROM AUTHOR]

Lead chalcogenides and their alloys belong at the heart of thermoelectrics due to their large thermoelectric figure of merit (zT). However, recent research has shown a limitation in the use of lead (Pb)-based materials due to their toxicity and efforts have been made to produce non-toxic analogues of lead chalcogenides. Tin chalcogenides have been predicted to be promising for this purpose due to their unique electronic structure and phonon dispersion properties. Here, we discuss the journey of tin chalcogenides in the field of thermoelectrics and topological materials with the main emphasis on the bonding, crystal structures, electronic band structures, phonon dispersion and thermoelectric properties. The thermal transport properties of tin chalcogenides are explained based on lattice dynamics, where resonant bonding and local structural distortion play an important role in creating lattice anharmonicity, thereby lowering the lattice thermal conductivity. Since thermoelectric and topological materials, especially topological insulators and topological crystalline insulators, share similar material features, such as a narrow band gap, heavy constituent elements and significant spin–orbit coupling, we have discussed the thermoelectric properties of several topological tin chalcogenides from a chemistry perspective. This feature article serves as a useful reference for researchers who strive to improve the properties of tin chalcogenides and advance the field of thermoelectric and topological materials. [ABSTRACT FROM AUTHOR]

Abstract: Crystalline solids with intrinsically low lattice thermal conductivity (κL) are crucial to realizing high‐performance thermoelectric (TE) materials. Herein, we show an ultralow κL of 0.35 Wm−1 K−1 in AgCuTe, which has a remarkable TE figure‐of‐merit, zT of 1.6 at 670 K when alloyed with 10 mol % Se. First‐principles DFT calculation reveals several soft phonon modes in its room‐temperature hexagonal phase, which are also evident from low‐temperature heat‐capacity measurement. These phonon modes, dominated by Ag vibrations, soften further with temperature giving a dynamic cation disorder and driving the superionic transition. Intrinsic factors cause an ultralow κL in the room‐temperature hexagonal phase, while the dynamic disorder of Ag/Cu cations leads to reduced phonon frequencies and mean free paths in the high‐temperature rocksalt phase. Despite the cation disorder at elevated temperatures, the crystalline conduits of the rigid anion sublattice give a high power factor. [ABSTRACT FROM AUTHOR]

Abstract: Crystalline solids with intrinsically low lattice thermal conductivity (κL) are crucial to realizing high‐performance thermoelectric (TE) materials. Herein, we show an ultralow κL of 0.35 Wm−1 K−1 in AgCuTe, which has a remarkable TE figure‐of‐merit, zT of 1.6 at 670 K when alloyed with 10 mol % Se. First‐principles DFT calculation reveals several soft phonon modes in its room‐temperature hexagonal phase, which are also evident from low‐temperature heat‐capacity measurement. These phonon modes, dominated by Ag vibrations, soften further with temperature giving a dynamic cation disorder and driving the superionic transition. Intrinsic factors cause an ultralow κL in the room‐temperature hexagonal phase, while the dynamic disorder of Ag/Cu cations leads to reduced phonon frequencies and mean free paths in the high‐temperature rocksalt phase. Despite the cation disorder at elevated temperatures, the crystalline conduits of the rigid anion sublattice give a high power factor. [ABSTRACT FROM AUTHOR]

Waste heat sources are generally diffused and provide a range of temperatures rather than a particular temperature. Thus, thermoelectric waste heat to electricity conversion requires a high average thermoelectric figure of merit ( ZTavg) of materials over the entire working temperature along with a high peak thermoelectric figure of merit ( ZTmax). Herein an ultrahigh ZTavg of 1.4 for (GeTe)80(AgSbSe2)20 [TAGSSe-80, T=tellurium, A=antimony, G=germanium, S=silver, Se=selenium] is reported in the temperature range of 300-700 K, which is one of the highest values measured amongst the state-of-the-art Pb-free polycrystalline thermoelectric materials. Moreover, TAGSSe-80 exhibits a high ZTmax of 1.9 at 660 K, which is reversible and reproducible with respect to several heating-cooling cycles. The high thermoelectric performance of TAGSSe- x is attributed to extremely low lattice thermal conductivity ( κlat), which mainly arises due to extensive phonon scattering by hierarchical nano/meso-structures in the TAGSSe- x matrix. Addition of AgSbSe2 in GeTe results in κlat of ≈0.4 W mK−1 in the 300-700 K range, approaching to the theoretical minimum limit of lattice thermal conductivity ( κmin) of GeTe. Additionally, (GeTe)80(AgSbSe2)20 exhibits a higher Vickers microhardness (mechanical stability) value of ≈209 kgf mm−2 compared to the other state-of-the-art metal chalcogenides, making it an important material for thermoelectrics. [ABSTRACT FROM AUTHOR]

Topological crystalline insulator (TCI), Pb0.6Sn0.4Te, exhibits metallic surface states protected by crystal mirror symmetry with negligibly small band gap. Enhancement of its thermoelectric performances needs tuning of its electronic structure particularly through engineering of its band gap. While physical perturbations tune the electronic structure of TCI by breaking of the crystal mirror symmetry, chemical means such as doping have been more attractive recently as they result in better thermoelectric performance in TCIs. Here, we demonstrate that K doping in TCI, Pb0.6Sn0.4Te, breaks the crystal mirror symmetry locally and widens electronic band gap, which is confirmed by direct electronic absorption spectroscopy and electronic structure calculations. K doping in Pb0.6Sn0.4Te increases p-type carrier concentration and suppresses the bipolar conduction via widening a band gap, which collectively boosts the thermoelectric figure of merit (ZT) to 1 at 708K. [ABSTRACT FROM AUTHOR]

Classical magnetoresistance generally follows the quadratic dependence of the magnetic field at lower field and finally saturates when field is larger. Here, we report the large positive non-saturating linear magnetoresistance in topological crystalline insulator, Pb 0.6 Sn 0.4 Te, at different temperatures between 3 K and 300 K in magnetic field up to 9 T. Magnetoresistance value as high as ∼200% was achieved at 3 K at magnetic field of 9 T. Linear magnetoresistance observed in Pb 0.6 Sn 0.4 Te is mainly governed by the spatial fluctuation carrier mobility due to distortions in the current paths in inhomogeneous conductor. [ABSTRACT FROM AUTHOR]

Topological crystalline insulators (TCIs) are a new quantum state of matter in which linearly dispersed metallic surface states are protected by crystal mirror symmetry. Owing to its vanishingly small bulk band gap, a TCI like Pb0.6Sn0.4Te has poor thermoelectric properties. Breaking of crystal symmetry can widen the band gap of TCI. While breaking of mirror symmetry in a TCI has been mostly explored by various physical perturbation techniques, chemical doping, which may also alter the electronic structure of TCI by perturbing the local mirror symmetry, has not yet been explored. Herein, we demonstrate that Na doping in Pb0.6Sn0.4Te locally breaks the crystal symmetry and opens up a bulk electronic band gap, which is confirmed by direct electronic absorption spectroscopy and electronic structure calculations. Na doping in Pb0.6Sna4Te increases p-type carrier concentration and suppresses the bipolar conduction (by widening the band gap), which collectively gives rise to a promising zTof1 at 856 Kfor Pb0.58Sn0.40Na0.02Te. Breaking of crystal symmetry by chemical doping widens the bulk band gap in TCI, which uncovers a route to improve TCI for thermoelectric applications. [ABSTRACT FROM AUTHOR]

Topological crystalline insulators (TCIs) are a new quantum state of matter in which linearly dispersed metallic surface states are protected by crystal mirror symmetry. Owing to its vanishingly small bulk band gap, a TCI like Pb0.6Sn0.4Te has poor thermoelectric properties. Breaking of crystal symmetry can widen the band gap of TCI. While breaking of mirror symmetry in a TCI has been mostly explored by various physical perturbation techniques, chemical doping, which may also alter the electronic structure of TCI by perturbing the local mirror symmetry, has not yet been explored. Herein, we demonstrate that Na doping in Pb0.6Sn0.4Te locally breaks the crystal symmetry and opens up a bulk electronic band gap, which is confirmed by direct electronic absorption spectroscopy and electronic structure calculations. Na doping in Pb0.6Sn0.4Te increases p-type carrier concentration and suppresses the bipolar conduction (by widening the band gap), which collectively gives rise to a promising zT of 1 at 856 K for Pb0.58Sn0.40Na0.02Te. Breaking of crystal symmetry by chemical doping widens the bulk band gap in TCI, which uncovers a route to improve TCI for thermoelectric applications. [ABSTRACT FROM AUTHOR]

Two-dimensional (2D) borocarbonitrides (BCN) are of interest since their electrical and optical properties can be tuned for renewable energy applications. Although there have been theoretical studies, experimental studies of the thermal transport and thermoelectric properties of BCN nanosheets have not yet been explored. We have synthesized few-layer BCN nanosheets of different compositions, and characterized them by Raman spectroscopy, X-ray photoelectron spectroscopy and transmission electron microscopy (TEM). They exhibit p -type semiconducting thermoelectric transport properties in 300–573 ​K range. More interestingly, the BCN nanosheets exhibit low thermal conductivity (0.58–1.86 ​W/mK) unlike boron nitride (h-BN) and graphene over the temperature range of 300–573 ​K. The low thermal conductivity of BCN nanosheets arises due to significant phonon scattering by the different length scale hierarchical nano/meso architectures such as bonding heterogeneity (e.g. C–B, C–N and B–N), point defects related C/B/N disorder, nanodomains of BN/carbon and grain boundaries. Image 1 BCN nanosheets exhibit low thermal conductivity due to the significant phonon scattering from the different length scale hierarchical nano/meso architectures such as bonding heterogeneity, point defects (C/B/N disorder), disordered BN/carbon nanodomains and grain boundaries. • Few-layer BCN nanosheets have been synthesized via solid state reaction employing urea method. • Low thermal conductivity (0.58–1.86 ​W/mK) in the temperature range of 300–573 ​K was achieved for BCN nanosheets. • The low thermal conductivity in BCN nanosheets arises due to significant phonon scattering by hierarchical architectures. [ABSTRACT FROM AUTHOR]

Heusler compounds belong to a large family of materials and exhibit numerous physical phenomena with promising applications, particularly ferromagnetic Weyl semimetals for their use in spintronics and memory devices. Here, anomalous Hall transport is reported in the room‐temperature ferromagnets NiMnSb (half‐metal with a Curie temperature (TC) of 660 K) and PtMnSb (pseudo half‐metal with a TC of 560 K). They exhibit 4 µB/f.u. magnetic moments and non‐trivial topological states. Moreover, NiMnSb and PtMnSb are the first half‐Heusler ferromagnets to be reported as Weyl semimetals, and they exhibit anomalous Hall conductivity (AHC) due to the extended tail of the Berry curvature in these systems. The experimentally measured AHC values at 2 K are 1.8 × 102 Ω−1 cm−1 for NiMnSb and 2.2 × 103 Ω−1 cm−1 for PtMnSb. The comparatively large value between them can be explained in terms of the spin‐orbit coupling strength. The combined approach of using ab initio calculations and a simple model shows that the Weyl nodes located far from the Fermi energy act as the driving mechanism for the intrinsic AHC. This contribution of topological features at higher energies can be generalized. [ABSTRACT FROM AUTHOR]

Ge1-xSbxTe (x = 0-0.1) is prepared from the elements (evacuated quartz tubes, 1223 K, 6 h). [ABSTRACT FROM AUTHOR]

Discovery of exotic phases of matter from the topologically non-trivial systems not only makes the research on topological materials more interesting but also enriches our understanding of the fascinating physics of such materials. Pb0.6Sn0.4Te was recently shown to be a topological crystalline insulator. Here, we show that by forming a mesoscopic point-contact using a normal non-superconducting elemental metal on the surface of Pb0.6Sn0.4Te, a superconducting phase is created locally in a confined region under the point-contact. This happens when the bulk of the sample remains to be nonsuperconducting, and the superconducting phase emerges as a nano-droplet under the point-contact. The superconducting phase shows a high transition temperature Tc that varies for different pointcontacts and falls in a range between 3.7K and 6.5 K. Therefore, this Letter presents the discovery of a superconducting phase on the surface of a topological crystalline insulator, and the discovery is expected to shed light on the mechanism of induced superconductivity in topologically non-trivial systems in general. [ABSTRACT FROM AUTHOR]

Thebinding and rotational properties of an excited-state intramolecularproton transfer (ESIPT) fluorophore, 2,2′-bipyridine-3,3′-diol,BP(OH)2has been investigated in alkyltrimethylammoniumbromide containing (CnTAB, n= 12, 14, and 16) micelles and alkyltrimethylammonium bromide/cholesterol(CnTAB (n= 14 and 16)/cholesterol)forming vesicles using fluorescence-based spectroscopy techniques.The formation of thermodynamically stable unilamellar self-assembliesof alkyltrimethylammonium bromide/cholesterol are characterized bydynamic light scattering (DLS) and transmission electron microscopy(TEM) measurements. Individually, aqueous solutions of all these alkyltrimethylammoniumbromide form micelles after certain surfactant concentration (criticalmicelle concentration, cmc) of surfactant, whereas cholesterol moleculesare insoluble in water. But with the variation of the cholesterol-to-surfactantmolar ratio (Q= [cholesterol]/[surfactant]), uniformdistribution of vesicular aggregates in aqueous solution can be obtained.The micelle-to-vesicle transition of surfactant solution upon additionof cholesterol also influences the steady state emission profile,fluorescence lifetime, and rotational dynamics of BP(OH)2molecule. The diketo tautomer of BP(OH)2molecule getsstabilized as the concentration of surfactant increases in aqueoussolution. Fluorescence lifetime and rotational time constant of theBP(OH)2molecule are also influenced by the variation ofalkyl chain length of surfactant molecule. The emission quantum yield(Φ) is also found to be sensitive with surfactant concentration,variation in chain length of surfactants, and it saturates after thecmc of surfactants. The rigid and restricted microenvironment of vesiclebilayer enhance the lifetime and also rotational relaxation of BP(OH)2significantly. The rotational behavior of BP(OH)2in surfactant/cholesterol self-assemblies is also explained by usinganalytical parameters related to time-resolved anisotropy followingtwo-step process and wobbling in a cone models. [ABSTRACT FROM AUTHOR]

A two‐step optimization strategy is used to improve the thermoelectric performance of SnTe via modulating the electronic structure and phonon transport. The electrical transport of self‐compensated SnTe (that is, Sn1.03Te) was first optimized by Ag doping, which resulted in an optimized carrier concentration. Subsequently, Mn doping in Sn1.03−xAgxTe resulted in highly converged valence bands, which improved the Seebeck coefficient. The energy gap between the light and heavy hole bands, i.e. ΔEv decreases to 0.10 eV in Sn0.83Ag0.03Mn0.17Te compared to the value of 0.35 eV in pristine SnTe. As a result, a high power factor of ca. 24.8 μW cm−1 K−2 at 816 K in Sn0.83Ag0.03Mn0.17Te was attained. The lattice thermal conductivity of Sn0.83Ag0.03Mn0.17Te reached to an ultralow value (ca. 0.3 W m−1 K−1) at 865 K, owing to the formation of Ag7Te4 nanoprecipitates in SnTe matrix. A high thermoelectric figure of merit (z T≈1.45 at 865 K) was obtained in Sn0.83Ag0.03Mn0.17Te. [ABSTRACT FROM AUTHOR]

A two‐step optimization strategy is used to improve the thermoelectric performance of SnTe via modulating the electronic structure and phonon transport. The electrical transport of self‐compensated SnTe (that is, Sn1.03Te) was first optimized by Ag doping, which resulted in an optimized carrier concentration. Subsequently, Mn doping in Sn1.03−xAgxTe resulted in highly converged valence bands, which improved the Seebeck coefficient. The energy gap between the light and heavy hole bands, i.e. ΔEv decreases to 0.10 eV in Sn0.83Ag0.03Mn0.17Te compared to the value of 0.35 eV in pristine SnTe. As a result, a high power factor of ca. 24.8 μW cm−1 K−2 at 816 K in Sn0.83Ag0.03Mn0.17Te was attained. The lattice thermal conductivity of Sn0.83Ag0.03Mn0.17Te reached to an ultralow value (ca. 0.3 W m−1 K−1) at 865 K, owing to the formation of Ag7Te4 nanoprecipitates in SnTe matrix. A high thermoelectric figure of merit (z T≈1.45 at 865 K) was obtained in Sn0.83Ag0.03Mn0.17Te. [ABSTRACT FROM AUTHOR]