Superatomic-Charge-Density-Wave in Cluster-Assembled Au6Te12Se8 Superconductors

Xu, Chen; Ge, Fei; Song, Yanpeng; Ying, Tianping; Huang, Dajian; Pan, Bingying; Yang, Dongliang; Yang, Xiaofan; Chen, Keyu; Zhan, Xinhui; Wang, Junjie; Zhang, Qinghua; Li, Yanchun; Gu, Lin; Gou, Huiyang; Chen, Xin; Li, Shiyan; Cheng, Jinguang; Liu, Xiaobing; Hosono, Hideo; Guo, Jiangang; Chen, Xiaolong

doi:10.1021/jacs.2c09499

Cited by 8 publications

(7 citation statements)

References 37 publications

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“…The phase diagram of superconducting and CDW states for Bi 2 Rh 3 Se 2 against pressure is shown in Figure , suggesting the existence of exotic physical nature hidden in this material. In addition, the phase diagram is consistent with those reported for various materials with both the superconducting and CDW states. − …”

Section: Resultssupporting

confidence: 85%

“…In addition, the application of pressure to Ba 1– x Cs x Ti 2 Sb 2 O suppressed the CDW state to support the superconducting transition . Moreover, many reports on the suppression of CDW-ordered state and the simultaneous enhancement of T c through the application of pressure have been published. − From these results, we assumed that the T c increased via the suppression of the CDW state by applying pressure.…”

Section: Resultsmentioning

confidence: 98%

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Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi₂Rh₃Se₂

et al. 2023

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The structural and superconducting properties of a Bi-based compound, Bi2Rh3Se2, are investigated over a wide pressure range. Bi2Rh3Se2 is a superconductor with a superconducting transition temperature, T c, of 0.7 K. This compound is in a charge-density-wave (CDW) state below 240 K, which implies the coexistence of superconducting and CDW states at low temperatures. Here, the superconducting properties of Bi2Rh3Se2 are studied from the perspective of the temperature dependence of electrical resistance (R) at high pressures (p’s). The pressure dependence of T c of Bi2Rh3Se2 shows a slow increase in T c at 0–15.5 GPa, and the T c slowly decreases with pressure above 15.5 GPa, which is markedly different from that of normal superconductors because the value of T c should simply decrease owing to the decrease in density of states (DOS) on the Fermi level, N(εF), driven by a simple shrinkage of the lattice under pressure. To ascertain the origin of such a dome-like T c–p behavior, the crystal structure of Bi2Rh3Se2 was explored over a wide pressure range of 0–20 GPa on the basis of powder X-ray diffraction; no structural phase transitions or simple shrinkage of the lattice was observed. This result implies that the increase in T c against pressure cannot simply be explained from a structural point of view. In other words, a direct relation between superconductivity and crystal structure was not found. On the other hand, the CDW transition became ambiguous at pressures higher than 3.8 GPa, suggesting that the T c had been suppressed by the CDW transition in a low pressure range. Thus, the findings suggest that for Bi2Rh3Se2, T c is enhanced through the suppression of CDW transition, which may be reasonable because the CDW-ordered state restrains the charge fluctuation to weaken the electron–phonon coupling and opens the gap to decrease the density of states on the Fermi level. The obtained dome-like T c–p behavior indicates the possibility of Bi2Rh3Se2 being an exotic superconductor.

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Section: Resultssupporting

confidence: 85%

Section: Resultsmentioning

confidence: 98%

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi₂Rh₃Se₂

et al. 2023

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“…It bears some resemblance to the Pd 6 Cl 12 clusters present in β-PdCl 2 , in which square planar PdCl 4 units form cubes with bridging chloride ligands on the edges of the cube and no atoms on the corners . Additionally, the cube-shaped superatoms that comprise Au 6 Te 12 Se 8 , are nearly identical to the Pd 6 Se 20 clusters, although the Au phase has six additional electrons per cluster.…”

Section: Resultsmentioning

confidence: 99%

Diselenide Dianion’s Dual Powers: PdSe₂Polymorph Control and Pd₃Se₁₀Superatomic Crystal Creation

Irvine,

Hoefer,

Moser

et al. 2023

Chem. Mater.

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There is a diverse family of palladium selenide compounds, including semiconducting orthorhombic PdSe2 (O-PdSe2) and monoclinic PdSe2 (M-PdSe2), which are unusual among transition-metal dichalcogenides as they are composed of diselenide dianions Se2 2–. Thus far, the solution syntheses of materials with Se–Se bonds typically require the in situ reduction of Se precursors. Here, we explore the use of electrochemically precise reactions between Na2Se2 and a Pd2+ source, Na2PdCl4, as a solution-phase route to selectively form different PdSe2 polymorphs in the absence of surfactants. By altering the reactant molar ratios and time, we map out a synthetic phase space diagram that shows how to create a wide variety of palladium selenide phases. With increasing Se2 2–/Pd2+ molar ratios, regions are identified where Pd17Se15, M-PdSe2, and O-PdSe2 exist as the dominant or exclusive thermodynamic product. Additionally, we discover Pd3Se10, a superatomic crystal composed of Pd6Se20 cube-shaped clusters held together by van der Waals forces, which forms as a kinetic product under short reaction times. In total, the use of the diselenide dianion precursor allows for the selective solution-phase synthesis of M-PdSe2 or O-PdSe2, as well as the discovery of a previously unreported palladium selenide phase.

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“…They can be regarded as "molecular fragments" of the polymeric inorganic chalcogenides. These clusters were found in complexes or superstructures of proteins containing flexible organic ligands 35−37 and some recently discovered superatomic compounds, 38,39 with few examples of three-dimensional (3-D) extended inorganic compounds. 40 To achieve the "rigidness in softness" model, we used soft Bi chalcogen motifs to connect the newly found [Pt 6 Q 12 ] 12− clusters, and successfully obtained a series of new compounds Pt 3 Bi 4 Q 9 (Q = S, Se).…”

Section: ■ Introductionmentioning

confidence: 99%

“…They can be regarded as “molecular fragments” of the polymeric inorganic chalcogenides. These clusters were found in complexes or superstructures of proteins containing flexible organic ligands − and some recently discovered superatomic compounds, , with few examples of three-dimensional (3-D) extended inorganic compounds …”

Section: Introductionmentioning

confidence: 99%

Ultralow Thermal Conductivity of a Chalcogenide System Pt₃Bi₄Q₉ (Q = S, Se) Driven by the Hierarchy of Rigid [Pt₆Q₁₂]^12– Clusters Embedded in Soft Bi-Q Sublattice

Wang,

Liang,

Zhang

et al. 2024

J. Am. Chem. Soc.

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Knowledge of structure–property relationships in solids with intrinsic low thermal conductivity is crucial for fields such as thermoelectrics, thermal barrier coatings, and refractories. Herein, we propose a new “rigidness in softness” structural scheme for intrinsic low lattice thermal conductivity (κL), which embeds rigid clusters into the soft matrix to induce large lattice anharmonicity, and accordingly discover a new series of chalcogenides Pt3Bi4Q9 (Q = S, Se). Pt3Bi4S9–x Se x (x = 3, 6) achieved an intrinsic ultralow κL down to 0.39 W/(m K) at 773 K, which is considerably low among the Bi chalcogenide thermoelectric materials. Pt3Bi4Q9 contains the rigid cubic [Pt6Q12]12– clusters embedded in the soft Bi-Q sublattice, involving multiple bonding interactions and vibration hierarchy. The hierarchical structure yields a large lattice anharmonicity with high Grüneisen parameters (γ) 1.97 of Pt3Bi4Q9, as verified by the effective scatter of low-lying optical phonons toward heat-carrying acoustic phonons. Consequently, the rigid-soft coupling significantly inhibits heat propagation, exhibiting low acoustic phonon frequencies (∼25 cm–1) and Debye temperatures (ΘD = 170.4 K) in Pt3Bi4Se9. Owing to the suppressed κL and considerable power factor (PF), the ZT value of Pt3Bi4S6Se3 can reach 0.56 at 773 K without heavy carrier doping, which is competitive among the pristine Bi chalcogenides. Theoretical calculations predicted a large potential for performance improvement via proper doping, indicating the great potential of this structure type for promising thermoelectric materials.

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Superatomic-Charge-Density-Wave in Cluster-Assembled Au₆Te₁₂Se₈ Superconductors

Cited by 8 publications

References 37 publications

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi₂Rh₃Se₂

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi₂Rh₃Se₂

Diselenide Dianion’s Dual Powers: PdSe₂Polymorph Control and Pd₃Se₁₀Superatomic Crystal Creation

Ultralow Thermal Conductivity of a Chalcogenide System Pt₃Bi₄Q₉ (Q = S, Se) Driven by the Hierarchy of Rigid [Pt₆Q₁₂]^12– Clusters Embedded in Soft Bi-Q Sublattice

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Superatomic-Charge-Density-Wave in Cluster-Assembled Au6Te12Se8 Superconductors

Cited by 8 publications

References 37 publications

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi2Rh3Se2

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi2Rh3Se2

Diselenide Dianion’s Dual Powers: PdSe2Polymorph Control and Pd3Se10Superatomic Crystal Creation

Ultralow Thermal Conductivity of a Chalcogenide System Pt3Bi4Q9 (Q = S, Se) Driven by the Hierarchy of Rigid [Pt6Q12]12– Clusters Embedded in Soft Bi-Q Sublattice

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Superatomic-Charge-Density-Wave in Cluster-Assembled Au₆Te₁₂Se₈ Superconductors

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi₂Rh₃Se₂

Pressure Dependence of Superconductivity in a Charge-Density-Wave Superconductor Bi₂Rh₃Se₂

Diselenide Dianion’s Dual Powers: PdSe₂Polymorph Control and Pd₃Se₁₀Superatomic Crystal Creation

Ultralow Thermal Conductivity of a Chalcogenide System Pt₃Bi₄Q₉ (Q = S, Se) Driven by the Hierarchy of Rigid [Pt₆Q₁₂]^12– Clusters Embedded in Soft Bi-Q Sublattice