arXiv subjects

Tian Cui

Publications and source records attributed to Tian Cui.

At least 37 records · Page 2Linked to original sources

arXiv2024

Bidirectional Optimization onto Thermoelectric Performance via Hydrostatic-Pressure in Chalcopyrite AgXTe2 (X=In, Ga)

Pressure tuning has emerged as a powerful strategy for manipulating the thermoelectric properties of materials by inducing structural and electronic modifications. Herein, we systematically investigate the transport properties and thermoelectric performance concerning lattice distortions induced by hydrostatic pressure in Ag-based chalcopyrite AgXTe2 (X=In, Ga). The findings reveal that the lattice distortion in AgXTe2 exhibits distinct behaviors under lattice compression, diverging from trends observed at ambient pressure. Importantly, the hydrostatic pressure breaks the phenomenally negative correlation between thermal conductivity and lattice distortion. Pressure-induced softening of low-frequency acoustic phonons broadens the low-energy phonon spectrum, enhancing interactions between acoustic and optical phonons. Such broadening substantially increases the number of available three-phonon scattering channels, resulting in a marked reduction in thermal conductivity. Meanwhile, we establish a macroscopic connection between metavalent bonding and anharmonicity, providing an indirect explanation for lattice anharmonicity through pressure-driven transferred charge. Additionally, the applied pressure achieves a notable net increase in the power factor despite the strong coupling of electrical transport parameters, which underscores the potential for bidirectional optimization of transport properties in AgXTe2. As a result, the maximum ZT value of AgInTe2 is nearly doubled, demonstrating that pressure modulation is a powerful strategy for enhancing thermoelectric performance. Our work not only establishes the link between pressure, lattice dynamics, and thermoelectric properties within chalcopyrite AgXTe2, but also inspires the exploration of pressure-related optimization strategies for conventional thermoelectric materials.

cond-mat.mtrl-sci↗

arXiv2024

Interstitial anionic electrons involved superconductivity and T-linear resistivity behavior in electride La3In

Electrides are unique materials because of the existence of interstitial anionic electrons (IAEs). Due to these loosely bound IAEs and their strong interaction with the framework of cations, electrides can host superconductivity with rather high Tc, especially under high pressure, as predicted in theory. However, the experimental observations of superconductivity in electrides are very rare, let alone the detailed studies on intrinsic properties of single crystals. Here, we report the superconducting and normal-state properties of electride La3In single crystals. La3In shows a type-II superconductivity with Tc ~ 9.4 K and a T-linear resistivity in a wide temperature range. Experimental measurements and theoretical calculations suggest that the relatively high Tc could be ascribed to the high density of states around the Fermi level caused by short flat bands along R-M direction and the strong electron-phonon coupling, partially derived from the IAEs. Meanwhile, the T-linear resistivity may reflect the significant electronic correlation effect in this material. These findings will shed light on understanding the role of IAEs in superconductivity and open a promising way to explore high-temperature superconductors in electrides.

cond-mat.supr-con↗

arXiv2024

Hierarchical Characterization of Thermoelectric Performance in Copper-Based Chalcogenide CsCu$_3$S$_2$: Unveiling the role of Anharmonic Lattice Dynamics

We explicitly consider both phonon energy shifts and broadening arising from both cubic and quartic anharmonicities, as well as diagonal/non-diagonal terms of heat flux operators in thermal conductivity. Our findings show that the strong anharmonicity of CsCu$_3$S$_2$ primarily arises from the presence of $p$-$d$ anti-bonding hybridization between Cu and S atoms, coupled with the random oscillations of Cs atoms. Notably, the competition between phonon hardening described by the loop diagram and softening induced by the bubble diagram significantly influences particle-like propagation, predominantly reflected in group velocity and energy-conservation rule. Additionally, the electrical transport properties are determined by employing the precise momentum relaxation-time approximation (MRTA). At high temperatures, the thermoelectric performance of $p$-type CsCu$_3$S$_2$ reaches its optimum theoretical value of 0.94 along the in-plane direction based on advanced phonon renormalization theory. In striking contrast, the harmonic approximation theory significantly overestimates the thermoelectric efficiency at the same temperatures, rendering it an impractical expectation. Conversely, the first-order renormalization approach leads to a serious underestimation of the thermoelectric properties due to the over-correction of phonon energy. Our study not only reveals the pivotal role of anharmonic lattice dynamics in accurately assessing thermoelectric properties but also underscores the potential thermoelectric applications for novel copper-based chalcogenides.

cond-mat.mtrl-sci↗

arXiv2024

The Critical Metallization of Hydrogen in Pressurized LaBeH8 Hydride

Behaviours of hydrogen, such as fluidity and metallicity, are crucial for our understanding of planetary interiors and the emerging field of high-temperature superconducting hydrides. These behaviours were discovered in complex phase diagrams of hydrogen and hydrides, however, the transition mechanism of behaviours driven by temperature, pressure and chemical compression remain unclear, particularly in the processes of metallization. Until now, a comprehensive theoretical framework to quantify atomization and metallization of hydrogen in phase diagram of hydrides has been lacking. In this study, we address this gap by combining molecular dynamics and electronic structure analysis to propose a theoretical framework, which clarify the content and properties of atomic hydrogen under various temperature and pressure conditions and chemical compression exerted by non-hydrogen elements in hydrides. Applying this framework to the superconducting hydride LaBeH8, we identify three general hydrogen orderings within its phase diagram: molecular, sublattice and warm hydrogens. During the phase transition from molecule to sublattice, hydrogen exhibits different properties from three general hydrogen orderings, such as fast superionicity, metallicity and unusual atomic content response to temperature. These abnormal behaviours were defined as the critical metallization of hydrogen, which not only suggests a potential synthesis route for the metastable phase but also provides valuable insights into the complex synthetic products of superconducting hydrides.

cond-mat.mtrl-sci↗

arXiv2024

Electronic Correlations and Hund's Rule Coupling in Trilayer Nickelate La4Ni3O10

Trilayer Ruddlesden-Popper phase La4Ni3O10 has been observed with Tc of about 30 K at high pressure in recent experiment, which further expanded the family of nickelate superconductors. In this study, we explored the effects of electronic correlations in La4Ni3O10 using density function theory plus dynamical mean-field theory at ambient and high pressures. Our derived spectral functions and Fermi surface of ambient pressure phase are nicely consistent with the experimental results by angle-resolved photoemission spectroscopy, which emphasized the importance of electronic correlations in La4Ni3O10. We also found the electronic correlations in pressured La4Ni3O10 are both orbital-dependent and layer-dependent due to the presence of Hund's rule coupling. There is a competition between the Hund's rule coupling and the crystal-field splitting, and therefore the Ni-O layers with weaker crystal-field splitting energy would have stronger electronic correlations.

cond-mat.str-el↗

arXiv2024

Modulation of the Octahedral Structure and Potential Superconductivity of La$_3$Ni$_2$O$_7$ through Strain Engineering

The recent transport measurement of La$_3$Ni$_2$O$_7$ uncover a "right-triangle" shape of the superconducting dome in the pressure-temperature (P-T) phase diagram. Motivated by this, we perform theoretical first-principles studies of La$_3$Ni$_2$O$_7$ with the pressure ranging from 0 to 100 GPa. Notably, we reveal a pressure dependence of the Ni-$d_{z^2}$ electron density at the Fermi energy ($n_z^{EF}$) that highly coincides with such shape. On this basis, we further explore the electronic structure under uniaxial stress. By tracking the stress response of $n_z^{EF}$, we propose that superconductivity can be achieved by applying only about 2 GPa of compression along the c axis. The idea is further exemplified from the perspectives of lattice distortion, band structure, Fermi surface and superconducting phase coherence. We also discuss the possible charge modulation under the stress and provide an insight to the relation between n_z^EF and the superconducting Tc in La$_3$Ni$_2$O$_7$ system. Our study provides a helpful guide to the future experiment.

cond-mat.supr-con↗

arXiv2024

High-temperature Superconductivity in Perovskite Hydride below 10 GPa

Hydrogen and hydrides materials have long been considered promising materials for high-temperature superconductivity. But the extreme pressures required for the metallization of hydrogen-based superconductors limit their applications. Here, we have designed a series of high-temperature perovskite hydrides that can be stable within 10 GPa. Our research covered 182 ternary systems and ultimately determined that 9 compounds were stable within 20 GPa, of which 5 exhibited superconducting transition temperatures exceeding 120 K within 10 GPa. Excitingly, KGaH3 and CsInH3 are thermodynamically stable at 50 GPa. Among these perovskite hydrides, alkali metals are responsible for providing a fixed amount of charge and maintaining structural stability, while the cubic framework formed by IIIA group elements and hydrogen is crucial for high-temperature superconductivity. This work will inspire further experimental exploration and take an important step in the exploration of low-pressure stable high-temperature superconductors.

cond-mat.supr-con↗

arXiv2024

Structures and Superconductivity of Hydrogen and Hydrides under Extreme Pressure

Metallic hydrogen, existing in remarkably extreme environments, was predicted to exhibit long-sought room-temperature superconductivity. Although the superconductivity of metallic hydrogen has not been confirmed experimentally, superconductivity of hydrogen in hydrides was recently discovered with remarkably high critical temperature as theoretically predicted. In recent years, theoretical simulations have become a new paradigm for material science, especially exploration of material at extreme pressure. As the typical high-pressure material, metallic hydrogen has been providing a fertile playground for advanced simulations for long time. Simulations not only provide the substitute of experiments for hydrogen at high-pressure, but also encouraged the discovery of almost all the experimentally discovered superconducting hydrides with the record high superconducting transition temperature. This work reviews recent progress in hydrogen and hydrides under extreme pressure, focusing on phase diagram, structures and the long-sought goal of high-temperature superconductivity. In the end, we highlight structural features of hydrides for realization of hydrogen-driven superconducting hydrides near ambient pressure.

cond-mat.supr-con↗

arXiv2024

Prediction of Room-Temperature Superconductivity in Quasi-atomic H2-Type Hydrides at High Pressure

Achieving superconductivity at room temperature (RT) is a holy grail in physics. Recent discoveries on high-Tc superconductivity in binary hydrides H3S and LaH10 at high pressure have directed the search for RT superconductors to compress hydrides with conventional electron-phonon mechanisms. Here, we predict an exceptional family of superhydrides under high pressures, MH12 (M = Mg, Sc, Zr, Hf, Lu), all exhibiting RT superconductivity with calculated Tcs ranging from 313 to 398 K. In contrast to H3S and LaH10, the hydrogen sublattice in MH12 is arranged as quasi-atomic H2 units. This unique configuration is closely associated with high Tc, attributed to the high electronic density of states derived from H2 antibonding states at the Fermi level and the strong electron-phonon coupling related to the bending vibration of H2 and H-M-H. Notably, MgH12 and ScH12 remain dynamically stable even at pressure below 100 GPa. Our findings offer crucial insights into achieving RT superconductivity and pave the way for innovative directions in experimental research.

cond-mat.supr-con↗

arXiv2024

Ultra-low glassy thermal conductivity and controllable, promising thermoelectric properties in crystalline o-CsCu5S3

We thoroughly investigate the microscopic mechanisms of the thermal transport in orthorhombic \textit{o}-CsCu$_5$S$_3$ by integrating the first-principles-based self-consistent phonon calculations (SCP) with the linearized Wigner transport equation (LWTE). Our methodology takes into account contributions to phonon energy shifts and phonon scattering rates from both three- and four-phonon processes. Additionally, it incorporates the off-diagonal terms of heat flux operators to calculate the total thermal conductivity. The predicted $κ_\mathrm{L}$ with an extremely weak temperature dependence following $\sim T^{-0.33}$, in good agreement with experimental values along with the parallel to the Bridgman growth direction. Such nonstandard temperature dependence of $κ_\mathrm{L}$ can be traced back to the dual particlelike-wavelike behavior exhibited by thermal phonons. Specifically, the coexistence of the stochastic oscillation of Cs atoms and metavalent bonding among interlayer Cu-S atoms limits the particle-like phonon propagation and enhances the wave-like tunneling of phonons. Simultaneously, the electrical transport properties are determined by employing a precise momentum relaxation-time approximation (MRTA) within the framework of the linearized Boltzmann transport equation (LBTE). By properly adjusting the carrier concentration, excellent thermoelectric performance is achieved, with a maximum thermoelectric conversion efficiency of 18.4$\%$ observed at 800 K in \textit{p}-type \textit{o}-CsCu$_5$S$_3$.} Our work not only elucidates the anomalous thermal transport behavior in the copper-based chalcogenide \textit{o}-CsCu$_5$S$_3$ but also provides insights for manipulating its thermal and electronic properties for potential thermoelectric applications.

cond-mat.mtrl-sci↗

arXiv2024

Large negative magnetoresistance and pseudogap phase in superconducting A15-type La$_4$H$_{23}$

High pressure plays a crucial role in the field of superconductivity. Compressed hydride superconductors are leaders in the race for a material that can conduct electricity without resistance at high or even room temperature. In the present work, we have discovered new lanthanum superhydride, cubic A15-type La$_4$H$_{23}$, with lower stabilization pressure compared to the reported $\textit{fcc}$ LaH$_{10}$. Superconducting La$_4$H$_{23}$ was obtained by laser heating of LaH$_3$ with ammonia borane at about 120 GPa. Transport measurements reveal the maximum critical temperature $\textit{T}$$_{C}$(onset) = 105 K and the critical field $\textit{H}$$_{C2}$(0) = 32 T at 118 GPa, as evidenced by the sharp drop of electrical resistance and the displacement of superconducting transitions in applied magnetic fields. Moreover, we provide evidence for unconventional transport associated with a pseudogap phase in La$_4$H$_{23}$ using pulsed magnetic fields up to 68 T. A large negative magnetoresistance in the non-superconducting state below 40 K, quasi $\textit{T}$-linear electrical resistance, and a sign-change of its temperature dependence mark the emergence of pseudogap in this hydride. Discovered lanthanum hydride is a new member of the A15 family of superconductors with $\textit{T}$$_C$ exceeding the boiling point of liquid nitrogen.

cond-mat.supr-con↗

arXiv2023

Double Dome and Reemergence of Superconductivity in Pristine 6R-TaS2 under Pressure

Investigating the implications of interlayer coupling on superconductivity is essential for comprehending the intrinsic mechanisms of high temperature superconductors. Van der Waals heterojunctions have attracted extensive research due to their exotic interlayer coupling. Here, we present a natural heterojunction superconductor of 6R-TaS2 that demonstrates a double-dome of superconductivity, in addition to, the reemergence of superconducting under high pressures. Our first principles calculation shows that the first dome of superconductivity in 6R-TaS2 can be attributed to changes in interlayer coupling and charge transfer. The second superconducting dome and the reemergence of superconductivity can be ascribed to changes in the density of states resulting from Fermi surface reconstruction, in which the DOS of T-layer and S p-orbitals play a crucial role. We have reported the first observation in TMDs that non-metallic atoms playing a dominant role in the reemergence of superconducting and the influence of two Lifshitz transitions on superconducting properties.

cond-mat.supr-con↗

arXiv2023

High temperature superconductivity of quaternary hydrides XM3Be4H32 (X, M = Ca, Sr, Ba, Y, La, Ac, Th) under moderate pressure

The compressed hydrogen-rich compounds have received extensive attention as promising candidates for room temperature superconductivity, however, the high pressure required to stabilize such materials hinders their wide practical application. In order to search for potential superconducting hydrides that are stable at low pressures, we have investigated the crystal structures and properties of quaternary hydrides, XM3Be4H32 (X, M = Ca, Sr, Ba, Y, La, Ac, Th) based on the first-principles calculations. We identified nine dynamically stable compounds at moderate pressure of 20 GPa. Strikingly, their superconducting transition temperatures are much higher than that of liquid nitrogen, especially CaTh3Be4H32 (124 K at 5 GPa), ThLa3Be4H32(134 K at 10 GPa), LaAc3Be4H32 (135 K at 20 GPa) and AcLa3Be4H32 (153 K at 20 GPa) exhibit outstanding superconductivity at mild pressures. Metal atoms acting as pre-compressors donate abundant electrons to hydrogen, weakening the H-H covalent bond and thus facilitating the metallization of the hydrogen sublattice. At the same time, the appropriate combination of metal elements with different ionic radius and electronegativity can effectively tune the electronic structure near the Fermi level and improve the superconductivity. These findings fully reveal the great promise of hosting high-temperature superconductivity of quaternary hydrides at moderate pressures and will further promote related exploration.

cond-mat.supr-con↗

arXiv2023

Imaging the Meissner effect and flux trapping in a hydride superconductor at megabar pressures using a nanoscale quantum sensor

By directly altering microscopic interactions, pressure provides a powerful tuning knob for the exploration of condensed phases and geophysical phenomena. The megabar regime represents an exciting frontier, where recent discoveries include novel high-temperature superconductors, as well as structural and valence phase transitions. However, at such high pressures, many conventional measurement techniques fail. Here, we demonstrate the ability to perform local magnetometry inside of a diamond anvil cell with sub-micron spatial resolution at megabar pressures. Our approach utilizes a shallow layer of Nitrogen-Vacancy (NV) color centers implanted directly within the anvil; crucially, we choose a crystal cut compatible with the intrinsic symmetries of the NV center to enable functionality at megabar pressures. We apply our technique to characterize a recently discovered hydride superconductor, CeH$_9$. By performing simultaneous magnetometry and electrical transport measurements, we observe the dual signatures of superconductivity: local diamagnetism characteristic of the Meissner effect and a sharp drop of the resistance to near zero. By locally mapping the Meissner effect and flux trapping, we directly image the geometry of superconducting regions, revealing significant inhomogeneities at the micron scale. Our work brings quantum sensing to the megabar frontier and enables the closed loop optimization of superhydride materials synthesis.

cond-mat.supr-con↗

arXiv2023

Phase diagrams and superconductivity of ternary Ca-Al-H compounds under high pressure

The search for high-temperature superconductors in hydrides under high pressure has always been a research hotspot. Hydrogen-based superconductors offer an avenue to achieve the long-sought goal of superconductivity at room temperature. We systematically explore the high-pressure phase diagram, electronic properties, lattice dynamics and superconductivity of the ternary Ca-Al-H system using ab initio methods. We found two stable ternary hydrides at 50 GPa: Cmcm-CaAlH5 and Pnnm-CaAl2H8, which both are semiconductors. At 200 GPa, a new phase of P21/m-CaAlH5, P4/mmm-CaAlH7 and a metastable compound Immm-Ca2AlH12 were found. Furthermore, P4/mmm-CaAlH7 has obvious phonon softening of high frequency vibrations along the Z-A direction, point A and point X, which improves the strength of electron-phonon coupling. Therefore, a superconducting transition temperature Tc of 71 K is generated at 50 GPa. In addition, the thermodynamic metastable Immm-Ca2AlH12 exhibits a superconducting transition temperature of 118 K at 250 GPa. These results are very useful for the experimental searching of new high-Tc superconductors in ternary hydrides.

cond-mat.supr-con↗

arXiv2023

First-principles study on the superconductivity of N-doped fcc-LuH3

Recently, room-temperature superconductor has been claimed in a nitrogen-doped lutetium hydride at near-ambient pressure [Nature 615, 244 (2023)]. Using X-ray diffraction (XRD) and Raman spectra analysis, the authors believed that the superconducting properties can most probably be attributed to Fm-3m-LuH3δNε. Here, we systematic study the phase diagram of Lu-N-H at 1 GPa by using first-principle theory and find that there have no thermodynamically stable ternary compounds. Besides, we analyzed the dynamically stability and superconducting properties of N-doped Fm-3m-LuH3 using virtual crystal approximation (VCA) and supercell method. Our theoretical results show that the Tc of N-doped LuH3 cannot reach the level of room-temperature.

cond-mat.supr-con↗

arXiv2023

Thermodynamically stable room-temperature superconductors in Li-Na hydrides under high pressures

Room-temperature superconductivity has been a long-standing goal for scientific progress and human development. Thermodynamic stability is a prerequisite for material synthesis and application. Here, we perform a combination of high-throughput screening and structural search and uncover two thermodynamically stable room-temperature superconductors, Fd-3m-Li2NaH17 and Pm-3n-LiNa3H23, exhibiting extraordinary critical temperature of 340 K at 300 GPa and 310 K at 350 GPa, respectively. Li2NaH17 possesses the highest Tc among all the thermodynamically stable ternary hydrides hitherto found. The dominated H density of states at the Fermi level and the strong Fermi surface nesting are favorable for the emergence of room-temperature superconductivity. Their excellent superconducting properties help us understand the mechanism of room-temperature superconductivity and find new room-temperature superconductors. Interestingly, the structures of LiNa3H23 and Li2NaH17 equal to the identified type-I and II clathrate geometry. Our results provide a structural reference and theoretical guidance for later experimental structure determination and theoretical search for high temperature superconductors.

cond-mat.supr-con↗

arXiv2023

Superconducting phases of YH9 under pressure

Yttrium superhydrides has attracted much attention due to their multiple stoichiometries and excellent superconductivities under high pressure. Especially, YH9 have a Tc of 243 K, which is the second highest Tc among all binary hydrides. It exhibits a positive pressure dependence of Tc below 200 GPa, contrary to the results of theoretical prediction. In order to explore the origin of Tc at low pressure, we extensively investigated the crystal structure of YH9 at different pressure, and found a distorted cage structure with a symmetry of Pnma. This phase has the lowest enthalpy at pressure below 220 GPa, and its X-ray diffraction patterns is consistent with experimental data. Most importantly, the pressure dependence of Tc in phase Pnma is in line with the experimental results. Further calculations show the structural distortion strongly affect the lattice vibration and electron-phonon coupling, leads to the Pnma phase exhibiting a positive pressure dependence of Tc.

cond-mat.supr-con↗