Electron-phonon Coupling Constant Research Articles

Electronic structure, lattice dynamics and superconductivity in Li2CuX and LiCu2X (X = Si, Ge and Sn) Heusler compounds

First-principles computational methods have been employed to explore the electronic, lattice dynamics, and superconducting properties of the intermetallic Heusler compounds Li2CuX and LiCu2X (X = Si, Ge, or Sn). The electronic structure calculations suggest that all of these compounds exhibit metallic properties. The dynamic stability of the compounds has been examined by computing the phonon dispersion spectra and phonon density of states. Six out of twelve phases are found to be dynamically stable. Additionally, the superconductivity of stable and metastable compounds has been investigated using the electron–phonon-mediated mechanism. In calculations, it turns out that, regular cubic full Heusler Fm-3m LiCu2Ge exhibited the highest superconducting critical temperature (Tc) of 2.0 K, with a calculated electron–phonon coupling constant (λ) of 0.58.

Superconductivity in LaO: a density functional theory study with local, semilocal, and nonlocal exchange-correlation functionals

We studied the dynamical, electronic, and superconducting properties of LaO using a local (PZ), a semilocal (PBE), and three nonlocal correlation functionals (rVV10, vdW-DF2, and vdW-DF3) of the density-functional theory. We concluded that the nonlocal correlations have a marginal effect on the electronic band energies near the Fermi surface. However, the corresponding shifts in the density of states are relatively significant. In contrast, the phonon energies get modified by larger amounts, particularly for optical phonons. These variations in energies of optical phonons do not get reflected to the same degree in electron-phonon coupling constant, λ, from different functionals as their contribution in λ is minor that ranges from 21% to 33%. Moreover, the imperative role of Kohn anomalies and Fermi surface nesting for the electron-phonon coupling is reconfirmed. We also highlighted the role of the matrix elements that surpasses, in certain parts of the Brillouin Zone, all other factors including the Fermi surface nesting. The nonlocal correlation functional, vdW-DF2, gives significantly different results than other nonlocal as well as local/semilocal functionals due to excessive low energy phonons and larger phonon linewidth.

Distinct ultrafast dynamics of bilayer and trilayer nickelate superconductors regarding the density-wave-like transitions

In addition to the pressurized high-temperature superconductivity, bilayer and trilayer nickelate superconductors Lan+1NinO3n+1 (n = 2 and 3) exhibit many intriguing properties at ambient pressure, such as orbital-dependent electronic correlation, non-Fermi liquid behavior, and density-wave transitions. Here, using ultrafast reflectivity measurement, we observe a drastic difference between the ultrafast dynamics of the bilayer and trilayer nickelates at ambient pressure. We observe a coherent phonon mode in La4Ni3O10 involving the collective vibration of La, Ni, and O atoms, which is absent in La3Ni2O7. Temperature-dependent relaxation time diverges near the density-wave transition temperature of La4Ni3O10, while it is inversely proportional to the temperature in La3Ni2O7 above ∼150 K, suggesting a dramatic difference in the density-wave states of the two compounds and a non-Fermi liquid behavior of La3Ni2O7. Moreover, we estimate the electron-phonon coupling constants to be 0.05–0.07 and 0.12–0.16 for La3Ni2O7 and La4Ni3O10, respectively, suggesting a relatively minor role of electron-phonon coupling in the electronic properties of Lan+1NinO3n+1. Our work not only sheds light on the relevant microscopic interaction but also establishes a foundation for further studying the interplay between superconductivity and density-wave transitions in nickelate superconductors.

Intercalating Architecture for the Design of Charge Density Wave in Metallic MA2Z4 Materials.

We present a novel approach to induce charge density waves (CDWs) in metallic MA2Z4 materials, resembling the behavior observed in transition metal dichalcogenides (TMDCs). This method leverages the intercalating architecture to maintain the same crystal field and Fermi surface topologies. Our investigation reveals that CDW instability in these materials arises from electron-phonon coupling (EPC) between the d band and longitudinal acoustic (LA) phonons, mirroring TMDC's behavior. By combining α-MA2Z4 with 1H-MX2 materials in a predictive CDW phase diagram using critical EPC constants, we demonstrate the feasibility of extending CDW across material families with comparable crystal fields and reveal the crucial role in CDW instability of the competition between ionic charge transfer and electron correlation. We further uncover a strain-induced Mott transition in β2-NbGe2N4 monolayer featuring star-of-David patterns. This work highlights the potential of intercalating architecture to engineer CDW materials, expanding our understanding of CDW instability and correlation physics.

Anharmonic and quantum effects in Pm3̄ AlM(M = Hf, Zr)H6 under high pressure: A first-principles study.

First-principles calculations were employed to investigate the impact of quantum ionic fluctuations and lattice anharmonicity on the crystal structure and superconductivity of Pm3̄ AlM(M = Hf, Zr)H6 at pressures of 0.3-21.2GPa (AlHfH6) and 4.7-39.5GPa (AlZrH6) within the stochastic self-consistent harmonic approximation. A correction is predicted for the crystal lattice parameters, phonon spectra, and superconducting critical temperatures, previously estimated without considering ionic fluctuations on the crystal structure and assuming the harmonic approximation for lattice dynamics. The findings suggest that quantum ionic fluctuations have a significant impact on the crystal lattice parameters, phonon spectra, and superconducting critical temperatures. Based on our anharmonic phonon spectra, the structures will be dynamically stable at 0.3GPa for AlHfH6 and 6.2GPa for AlZrH6, ∼6 and 7GPa lower than pressures given by the harmonic approximation, respectively. Due to the anharmonic correction of their frequencies, the electron-phonon coupling constants (λ) are suppressed by 28% at 11GPa for AlHfH6 and 22% at 30GPa for AlZrH6, respectively. The decrease in λ causes Tc to be overestimated by ∼12K at 11GPa for AlHfH6 and 30GPa for AlZrH6. Even if the anharmonic and quantum effects are not as strong as those of Pm3̄n-AlH3, our results also indicate that metal hydrides with hydrogen atoms in interstitial sites are subject to anharmonic effects. Our results will inevitably stimulate future high-pressure experiments on synthesis, structural, and conductivity measurements.

Differentiating contribution of electron–phonon coupling to the thermal boundary conductance of metal–metal–dielectric systems

Electron–phonon coupling thermal resistance in metals is a key factor affecting the thermal boundary conductance (TBC) of metal–metal–dielectric systems. However, quantitatively differentiating the contribution of electron–phonon coupling to TBC is still a challenge, as various thermal resistances are coupled in a complicated manner at the metal–metal–dielectric interface. Herein, we propose a two-step strategy to study electron–phonon coupling. We first decouple the phonon–phonon thermal conductance (TBCp-p) between metallic interlayer and dielectric from the metal–metal–dielectric interface by experimentally characterizing the TBCp-p of a single metallic interlayer deposited dielectric with the transient thermoreflectance technique; Combining metal–metal–dielectric TBC measurement and a thermal circuit model with measured TBCp-p as input, the contribution of electron–phonon coupling to TBC of the metal–metal–dielectric system is differentiated quantitatively. For the Au–Ni–GaN system, the contribution of electron–phonon coupling thermal resistance in the Ni interlayer (Re−ph,Ni) is substantially higher at lower Ni interlayer thickness, reaching 35% at ∼1 nm Ni. The electron–phonon coupling constant of Ni (gNi) was fitted in the range of 6.4 × 1016–36 × 1016 W/m3K. The above results were also verified in the Au–Ni–SiC system. This study will promote a deeper understanding of the thermal transport in the metal–metal–dielectric system and provide an insightful indication for the manipulation of TBC in this system.

Symmetry-Shaped Singularities in High-Temperature Superconductor H3S.

The superconducting critical temperature of H3S ranks among the highest measured, at 203 K. This impressive value stems from a singularity in the electronic density-of-states, induced by a flat-band region that consists of saddle points. The peak sits right at the Fermi level, so that it gives rise to a giant electron-phonon coupling constant. In this work, we show how atomic orbital interactions and space group symmetry work in concert to shape the singularity. The body-centered cubic Brillouin Zone offers a unique 2D hypersurface in reciprocal space: fully connecting squares with two different high-symmetry points at the corners, Γ and H, and a third one in the center, N. Orbital mixing leads to the collapse of fully connected 1D saddle point lines around the square centers, due to a symmetry-enforced s-p energy inversion between Γ and H. The saddle-point states are invariably nonbonding, which explains the unconventionally weak response of the superconductor's critical temperature to pressure. Although H3S appears to be a unique case, the theory shows how it is possible to engineer flat bands and singularities in 3D lattices through symmetry considerations.

TTEP: A code for efficient calculation of the thermal transport from constant electron-phonon coupling approximation

A Fortran code named TTEP (Thermal Transport from constant Electron-Phonon coupling approximation) is presented in this work. Within the framework of first-principles calculation, this code utilizes the deformation potential approximation to replace the electron–phonon (EP) coupling matrix element in the phonon scattering due to EP interaction. By adopting this approximation, our method achieves a balance between computational efficiency and accuracy, enabling the exploration of the thermal transport from EP interaction with much reduced computational consumption. One of the key features of TTEP is its versatility in handling a broad range of carrier concentration, including both hole and electron doping. We also extend the applicability of TTEP to actual doping case and capture EP effect over a wide temperature range. Other scattering mechanisms, such as grain boundary scattering and phonon–phonon interaction, have been included in the calculation of lattice thermal conductivity through the Matthiessen’s rule. Several test cases are presented in this work to demonstrate the above features.

Strong electron-phonon coupling and multigap superconductivity in 2H/1T Janus MoSLi monolayer.

Two-dimensional (2D) Janus transition metal dichalcogenides MXY manifest novel physical properties owing to the breaking of out-of-plane mirror symmetry. Recently, the 2H phase of MoSH has been demonstrated to possess intrinsic superconductivity, whereas the 1T phase exhibits a charge density waves state. In this paper, we have systematically studied the stability and electron-phonon interaction characteristics of MoSLi. Our results have shown that both the 2H and 1T phases of MoSLi are stable, as indicated by the phonon spectrum and the abinitio molecular dynamics. However, the 1T phase exhibits an electron-phonon coupling constant that is twice as large as that of the 2H phase. In contrast to MoSH, the 1T phase of MoSLi exhibits intrinsic superconductivity. By employing the abinitio anisotropic Migdal-Eliashberg formalism, we have revealed the two-gap superconducting nature of 1T-MoSLi, with a transition temperature (Tc) of 14.8K. The detailed analysis indicates that the superconductivity in 1T-MoSLi primarily originates from the interplay between the vibration of the phonon modes in the low-frequency region and the dz2 orbital. These findings provide a fresh perspective on superconductivity within Janus structures.

Impacts of hot electron diffusion, electron–phonon coupling, and surface atoms on metal surface dynamics revealed by reflection ultrafast electron diffraction

Metals exhibit nonequilibrium electron and lattice subsystems at transient times following femtosecond laser excitation. In the past four decades, various optical spectroscopy and time-resolved diffraction methods have been used to study electron–phonon coupling and the effects of underlying dynamical processes. Here, we take advantage of the surface specificity of reflection ultrafast electron diffraction (UED) to examine the structural dynamics of photoexcited metal surfaces, which are apparently slower in recovery than predicted by thermal diffusion from the profile of absorbed energy. Fast diffusion of hot electrons is found to critically reduce surface excitation and affect the temporal dependence of the increased atomic motions on not only the ultrashort but also sub-nanosecond times. Whereas the two-temperature model with the accepted physical constants of platinum can reproduce the observed surface lattice dynamics, gold is found to exhibit appreciably larger-than-expected dynamic vibrational amplitudes of surface atoms while keeping the commonly used electron–phonon coupling constant. Such surface behavioral difference at transient times can be understood in the context of the different strengths of binding to surface atoms for the two metals. In addition, with the quantitative agreements between diffraction and theoretical results, we provide convincing evidence that surface structural dynamics can be reliably obtained by reflection UED even in the presence of laser-induced transient electric fields.

Superconductivity in breathing kagome-structured C14 Laves phase XOs2(X = Zr, Hf)

Recently, the emergence of superconductivity in kagome metals has generated significant interest due to its interaction with flat bands and topological electronic states, which exhibit a range of unusual quantum characteristics. This study thoroughly investigates largely unexplored breathing kagome structure C14 Laves phase compounds XOs2 (X = Zr, Hf) by XRD, electrical transport, magnetization, and specific heat measurements. Our analyses confirm the presence of the MgZn2-type structure in ZrOs2 and HfOs2 compounds, exhibiting type-II superconductivity with critical temperature ( TC ) values of 2.90(3) K and 2.69(6) K, respectively. Furthermore, specific heat measurements and electron–phonon coupling constants for both compounds indicate weakly coupled fully gapped superconductivity.

Anomalous superconductivity in Li/F modified two-dimensional molybdenene

Anomalous superconductivity in Li/F modified two-dimensional molybdenene

Superconductivity in monolayer Janus titanium-sulfur hydride (TiSH) at ambient pressure

Janus two dimensional (2D) materials are new and novel materials. As they break out-of-plane symmetry, they possess several fascinating properties which can be applied in catalytic reactions and opto-electronics. Recent synthesis of MoSH and the prediction of phonon-mediated superconductivity have opened a new way to investigate the properties of hydrogenated Janus materials (Novoselov et al 2004 Science 306 666–9; Mehta et al 2023 Solid State Commun. 375 115347; Naik et al 2023 Comput. Theor. Chem. 1228 114278). In this work, we performed the density functional theory calculations to demonstrate that titanium sulfur hydride (TiSH) is dynamically stable and becomes phonon-mediated superconductor with the superconducting critical temperature, Tc = 9.24 K with the corresponding value of electron–phonon coupling constant, λ = 0.71, in the weak interaction limits, under ambient conditions. Eliashberg spectral function α2F(ω) was well converged for dense grid of q1 × q2 × q3 = 12 × 12 × 1 and nk1 × nk2 × nk3 = 140 × 140 × 1. The effect of smearing broadening was also considered for determining well converged value of Tc and λ. Figure (b) shows that after smearing broadening of 0.02 Ry, λ shows convergent values, and subsequent changes are as low as less that 5% of the peak value. Overall, our findings predicted a new member in the 2D Janus hydride family with possible applications in 2D nanomaterials and superconducting devices applications.

High-throughput discovery of metal oxides with high thermoelectric performance via interpretable feature engineering on small data

In this work, we have proposed a data-driven screening framework combining the interpretable machine learning with high-throughput calculations to identify a series of metal oxides that exhibit both high-temperature tolerance and high power factors. Aiming at the problem of weak generalization ability of small data with power factors at high temperatures, we employ symbolic regression for feature creation which enhances the robustness of the model while preserving the physical meaning of features. 33 candidate metal oxides are finally targeted for high-temperature thermoelectric applications from a pool of 48,694 compounds in the Materials Project database. The Boltzmann transport theory is utilized to perform electrical transport properties calculations at 1,000 K. The relaxation time is approximated by employing constant electron-phonon coupling based on the deformation potential theory. Considering band degeneracy, the electron group velocity is obtained using the momentum matrix element method, yielding 28 materials with power factors greater than 50 μWcm−1K−2. The high-throughput framework we proposed is instrumental in the selection of metal oxides for high-temperature thermoelectric applications. Furthermore, our data-driven analysis and transport calculation suggest that metal oxides rich in elements such as cerium (Ce), tin (Sn), and lead (Pb) tend to exhibit high power factors at high temperatures.

Predictions of thorium super nitrides and superconductivity under pressure: Ab initio calculations

Thorium nitrides have been the topic of intense studies due to their prospective applications as advanced nuclear fuels. The phase diagram of the Th–N scheme, however, continues unknown at low temperatures and extremely high pressures. In this article, we examine the Th–N system's phase diagram up to 300 GPa from the first-principle approach using universal structure predictor: evolutionary Xtallography (USPEX) method. Apart from the experimentally observed phase (ThN, Th2N3, and Th3N4), there are several unique chemical stoichiometries, i.e., ThN3, ThN4, ThN6, ThN8, ThN10, and ThN12 are found to have stability fields on the Th–N phase diagram at pressure of 3.0, 32, 100, 42, 28, and 236 GPa along with previously predicted composition ThN2 at 3.5 GPa. The structural stability of the predicted compositions is further assessed by evaluating the elastic and dynamic stability. Out of all above mentioned compositions, ThN3 is possibly a metastable one at 0 GPa. Electronic structure calculations predict that all newly discovered compositions are metallic except ThN10, which is semi-metallic at high pressures. Further, we predict that ThN4 and ThN6 have high electron–phonon coupling constant of 1.874 and 0.894 with Tc around 21.22 and 25.02 K, respectively, at 100 GPa.

First-principles study of superconducting transition temperature of niobium and vanadium as a function of pressure

Ultra-high pressure has recently led to the observation of high Tc superconductors. The exploration of superconducting properties under high pressure conditions offers valuable insights into the fundamental mechanisms governing superconductivity and opens avenues for the synthesis of novel materials with enhanced superconducting properties. In this study, the superconducting transition temperature, Tc, for niobium and vanadium has been investigated to maximum pressures of 250.0 and 70.0 GPa, respectively. Density functional theory and density functional perturbation theory were used to undertake first-principles computations to investigate the variations of superconducting properties under pressure. For both the metals niobium (Nb) and vanadium (V), we observed that the density of states at the Fermi level decreased, while the overall phonon frequency generally increased with pressure. For Nb, we find that the electron–phonon coupling constant (λ) and the superconducting transition temperature (Tc) decrease steadily with pressure; however, for V, we find that λ and Tc decrease smoothly up to 26.0 GPa, and then gradually increase to 70.0 GPa pressure. The observed phonon spectrum nature for both Nb and V is in good agreement with the neutron scattering approach’s output.

Superconductivity in transition metal carbides, TaC and HfC: A density functional theory study with local, semilocal, and nonlocal exchange–correlation functionals

We studied electronic, dynamical, and superconducting properties of TaC and HfC using local, semilocal, and nonlocal exchange–correlation functionals in the density functional theory. It turns out that there is a slight shift of Fermi energy and the corresponding density of states with different functionals. However, the phonon frequencies of, especially, the optical modes for both TaC and HfC shift by moderately larger values. The most important differences are observed for the electron–phonon interactions where the electron–phonon coupling constant, λ≈0.9, calculated using the nonlocal correlation functionals, vdW-DF2 and vdW-DF3 for TaC, are in the closest agreement with the experimental results. Although the Kohn anomalies and Fermi surface nesting are critical for the electron–phonon coupling, a significant contribution to λ, for TaC, comes from the regions of the Brillouin zone where the matrix elements have a predominant role. Moreover, the optical modes give 20%–23% of λ for TaC and 50%–57% for HfC.

Electronic structure of BaBiO3 and electron–phonon coupling in K-doped superconducting bismuthate—A first-principles study

The electronic structure of BaBiO3 and Ba1−xKxBiO3, where x = 0.375, 0.4, and 0.425 is investigated using the density functional theory (DFT) in the generalized gradient approximation (GGA). The charge-density-wave (CDW) nature of the host compound is suppressed via potassium doping at Ba-site, resulting in the emergence of a metallic state. A strong hybridization between Bi-6s and O-A1g orbitals is observed in the electronic states near the Fermi level, particularly enhanced in the collapsed BiO6 octahedra of the undoped compound. The K-doped systems show stronger spσ hybridization than that of the host compound. The self-doped holes condensate in the antibonding combination of Bi-s and O-A1g orbitals of both the doped systems and in the collapsed octahedra of the undoped system. The exploration of lattice dynamics and electron–phonon coupling in Ba1−xKxBiO3 systems, elucidate that mainly the phonons corresponding to the oxygen bond stretching vibrations contribute most to the total electron–phonon coupling. The GGA-calculated electron–phonon coupling constants (λ) across varying K-concentrations inadequately account for experimental Tcs. The inclusion of long-range interactions through the HSE06 hybrid exchange–correlation functional substantially augments both λ and Tc, closely mirroring experimental observations and underscoring the crucial role of nonlocal correlations in these systems.

Physical properties of newly synthesized noncentrosymmetric TaIr2B2 and NbIr2B2 superconductors: an extensive comparison of GGA and LDA functional investigations.

In recent years, noncentrosymmetric (NCS) structural compounds have received much attention from the scientific community in the exploration for the unconventional nature of superconductivity with exciting physical properties. This study uses the comprehensive generalized gradient approximation (GGA) and local density approximation (LDA) to gain insights into the physical properties of two recently synthesized Ir-based NCS superconductors, TaIr2B2 and NbIr2B2. The structural parameters, mechanical performance, electronic structure, Debye temperature, melting temperature, electronic specific heat, and electron-phonon coupling constant of TaIr2B2 and NbIr2B2 are explored and discussed in detail. Density functional theory (DFT) optimized structural parameters of both NCS phases agree well with experimental observation. Both GGA and LDA calculations show that the compounds are ductile, machinable, mechanically stable, and anisotropic in nature. The elastic moduli and hardness calculations reveal that TaIr2B2 is harder than NbIr2B2. The calculation of the melting temperature reveals that TaIr2B2 is more suitable for high temperature technology applications compared to NbIr2B2. Both GGA and LDA functionals reveal that the optical functions are very similar. Both compounds display a significant amount of reflectivity spectra over a wide range of photon energies. The GGA functional reveals a somewhat higher density of states value compared to that of LDA. The present calculated values of the electron-phonon coupling constant of both compounds are consistent with values previously reported from experimental studies.

Few‐Hydrogen Metal‐Bonded Perovskite Superconductor MgHCu3 with a Critical Temperature of 42 K under Atmospheric Pressure

AbstractSince the prediction of multi‐hydrogen high‐temperature superconductor by Ashcroft in 2004, many possible candidates have been proposed, e.g., LaH10 showing the highest superconducting transition temperature (Tc) around 250–260 K at 170‐200 GPa hitherto. However, this pressure is too large to be taken into practical use. To address this challenge, it proposes a few‐hydrogen metal‐bonded perovskite superconductor, MgHCu3, by combining a novel design idea with first‐principles calculations. Different from multi‐hydrogen hydrides, whose high Tc relies on extreme pressure, the metallic bond in few‐hydrogen superconductor MgHCu3 improves the structural stability and ductility at atmospheric pressure. Here, the small amount of hydrogen is found to be vital for Tc. After the incorporation of hydrogen, the electron–phonon coupling constant of MgHCu3 is increased to 0.83, which is larger than that of the well‐known MgB2. Moreover, the anisotropy of MgHCu3 also plays an important role in enhancing Tc. Based on the Migdal‐Eliashberg theory, it predicts that the phonon‐mediated metal‐bonded perovskite MgHCu3 is a superconductor with Tc of 42 K. The first predicted ternary metal‐bonded perovskite, MgHCu3, enriches the family of perovskite and will promote further investigation on few‐hydrogen superconductors under atmospheric pressure.