cometadata/datacite-titles-descriptions-related-identifiers huggingface dataset:
DOI: 10.24435/materialscloud:3k-v7
title: Temperature-invariant crystal-glass heat conduction: from meteorites to refractories

description: The thermal conductivities of crystals and glasses vary strongly and with opposite trends upon heating, decreasing in crystals and increasing in glasses. Here, we show---with first-principles predictions based on the Wigner transport equation and thermoreflectance experiments---that the dominant transport mechanisms of crystals (particle-like propagation) and glasses (wave-like tunnelling) can coexist and compensate in materials with crystalline bond order and nearly glassy bond geometry. We demonstrate that ideal compensation emerges in silica tridymite, carved from a meteorite found in Steinbach (Germany) in 1724, and yields a 'Propagation-Tunneling-Invariant' (PTI) conductivity that is independent of temperature and intermediate between the opposite trends of α-quartz crystal and silica glass. We show how such PTI conductivity occurs in the quantum regime below the Debye temperature, and can largely persist at high temperatures in a geometrically amorphous tridymite phase found in refractory bricks fired for years in furnaces for steel smelting. Overall, we elucidate how disorder in the bond geometry determines the macroscopic conductivity, providing guidance to design materials for heat management, electronics, and phononics. We discuss implications to heat transfer in solids exposed to extreme temperature variations, ranging from planetary cooling to heating protocols to reduce the carbon footprint of industrial furnaces.

This record contains the atomic structures studied of α-quartz crystal, average (AV) tridymite, monoclinic (MC) meteoritic tridymite, Topologically Ordered and Geometrically Amorphous (TOGA) HP tridymite, and silica glass.
DOI: 10.24435/materialscloud:tr-d6
title: Temperature-invariant crystal-glass heat conduction: from meteorites to refractories

description: The thermal conductivities of crystals and glasses vary strongly and with opposite trends upon heating, decreasing in crystals and increasing in glasses. Here, we show---with first-principles predictions based on the Wigner transport equation and thermoreflectance experiments---that the dominant transport mechanisms of crystals (particle-like propagation) and glasses (wave-like tunnelling) can coexist and compensate in materials with crystalline bond order and nearly glassy bond geometry. We demonstrate that ideal compensation emerges in silica tridymite, carved from a meteorite found in Steinbach (Germany) in 1724, and yields a 'Propagation-Tunneling-Invariant' (PTI) conductivity that is independent of temperature and intermediate between the opposite trends of α-quartz crystal and silica glass. We show how such PTI conductivity occurs in the quantum regime below the Debye temperature, and can largely persist at high temperatures in a geometrically amorphous tridymite phase found in refractory bricks fired for years in furnaces for steel smelting. Overall, we elucidate how disorder in the bond geometry determines the macroscopic conductivity, providing guidance to design materials for heat management, electronics, and phononics. We discuss implications to heat transfer in solids exposed to extreme temperature variations, ranging from planetary cooling to heating protocols to reduce the carbon footprint of industrial furnaces.

This record contains the atomic structures studied of α-quartz crystal, average (AV) tridymite, monoclinic (MC) meteoritic tridymite, Topologically Ordered and Geometrically Amorphous (TOGA) HP tridymite, and silica glass.
DOI: 10.24435/materialscloud:8q-a1
title: Substrate-aware computational design of two-dimensional materials

description: Two-dimensional (2D) materials have attracted considerable attention due to their remarkable electronic, mechanical and optical properties, making them prime candidates for next-generation electronic and optoelectronic applications. Despite their widespread use in combination with substrates in practical applications, including the fabrication process and final device assembly, computational studies often neglect the effects of substrate interactions for simplicity. 
In this record, we provide the results of the computational study of the stable 2D molybdenum-sulfur (Mo-S) structures on a c-cut sapphire (Al₂O₃). In particular, we provide the results of the evolutionary search in the Mo-S / Al₂O₃ (0001) system, the machine learning interatomic potential (MLIP) used for local relaxation of the systems during the evolutionary search together with its training set, post-processing data on electronic and phonon band structures of the stable 2D Mo-S structures, and the predicted stability patterns from the perspective of CVD synthesis.
DOI: 10.24435/materialscloud:fc-jh
title: Substrate-aware computational design of two-dimensional materials

description: Two-dimensional (2D) materials have attracted considerable attention due to their remarkable electronic, mechanical and optical properties, making them prime candidates for next-generation electronic and optoelectronic applications. Despite their widespread use in combination with substrates in practical applications, including the fabrication process and final device assembly, computational studies often neglect the effects of substrate interactions for simplicity. 
In this record, we provide the results of the computational study of the stable 2D molybdenum-sulfur (Mo-S) structures on a c-cut sapphire (Al₂O₃). In particular, we provide the results of the evolutionary search in the Mo-S / Al₂O₃ (0001) system, the machine learning interatomic potential (MLIP) used for local relaxation of the systems during the evolutionary search together with its training set, post-processing data on electronic and phonon band structures of the stable 2D Mo-S structures, and the predicted stability patterns from the perspective of CVD synthesis.
DOI: 10.24435/materialscloud:v3-sc
title: First-principles electron-phonon interactions and polarons in the parent cuprate La₂CuO₄

description: Understanding electronic interactions in high-temperature superconductors is an outstanding challenge. In the widely studied cuprate materials, experimental evidence points to strong electron-phonon (e-ph) coupling and broad photoemission spectra. Yet, the microscopic origin of this behavior is not fully understood. Here we study e-ph interactions and polarons in a prototypical parent (undoped) cuprate, La₂CuO₄ (LCO), by means of first-principles calculations. Leveraging parameter-free Hubbard-corrected density functional theory, we obtain a ground state with band gap and Cu magnetic moment in nearly exact agreement with experiments. This enables a quantitative characterization of e-ph interactions. Our calculations reveal two classes of longitudinal optical (LO) phonons with strong e-ph coupling to hole states. These modes consist of Cu-O plane bond-stretching and bond-bending as well as vibrations of apical O atoms. The hole spectral functions, obtained with a cumulant method that can capture strong e-ph coupling, exhibit broad quasiparticle peaks with a small spectral weight (Z≈0.25) and pronounced LO-phonon sidebands characteristic of polaron effects. Our calculations predict features observed in photoemission spectra, including a 40-meV peak in the e-ph coupling distribution function not explained by existing models. These results show that the universal strong e-ph coupling found experimentally in lanthanum cuprates is an intrinsic feature of the parent compound, and elucidates its microscopic origin.
DOI: 10.24435/materialscloud:8g-rk
title: Dislocation-grain boundary interaction dataset for FCC Cu

description: Dislocation-grain boundary play a major role in the strength and ductility of structural materials. An understanding of governing parameters such as grain boundary local atomic structures on the outcome of this interaction can accelerate new alloy design strategies that tailors materials' microstructures. Previous studies have focused only on the subset of minimum-energy grain boundary structures. We present a comprehensive database of dislocation-grain boundary interaction for edge, screw, and 60o mixed dislocation with 449 < 110 > and < 112 > symmetric tilt grain boundary in FCC Cu consisting of 67 minimum-energy grain boundary structures and 389 metastable ones. The dataset contains the outcomes for 5593 unique interactions with a particular dislocation type, grain boundary structure, and applied shear stress.
DOI: 10.24435/materialscloud:r0-g5
title: First-principles electron-phonon interactions and polarons in the parent cuprate La₂CuO₄

description: Understanding electronic interactions in high-temperature superconductors is an outstanding challenge. In the widely studied cuprate materials, experimental evidence points to strong electron-phonon (e-ph) coupling and broad photoemission spectra. Yet, the microscopic origin of this behavior is not fully understood. Here we study e-ph interactions and polarons in a prototypical parent (undoped) cuprate, La₂CuO₄ (LCO), by means of first-principles calculations. Leveraging parameter-free Hubbard-corrected density functional theory, we obtain a ground state with band gap and Cu magnetic moment in nearly exact agreement with experiments. This enables a quantitative characterization of e-ph interactions. Our calculations reveal two classes of longitudinal optical (LO) phonons with strong e-ph coupling to hole states. These modes consist of Cu-O plane bond-stretching and bond-bending as well as vibrations of apical O atoms. The hole spectral functions, obtained with a cumulant method that can capture strong e-ph coupling, exhibit broad quasiparticle peaks with a small spectral weight (Z≈0.25) and pronounced LO-phonon sidebands characteristic of polaron effects. Our calculations predict features observed in photoemission spectra, including a 40-meV peak in the e-ph coupling distribution function not explained by existing models. These results show that the universal strong e-ph coupling found experimentally in lanthanum cuprates is an intrinsic feature of the parent compound, and elucidates its microscopic origin.
DOI: 10.24435/materialscloud:t4-kf
title: Simulation of the crystallization process of Ge₂Sb₂Te₅ nanoconfined in superlattice geometries for phase change memories

description: Phase change materials are the most promising candidates for the realization of artificial synapsis for neuromorphic computing. Different resistance levels corresponding to analogic values of the
synapsis conductance can be achieved by modulating the size of an amorphous region embedded in its crystalline matrix. Recently, it has been proposed that a superlattice made of alternating layers of the phase change compound Sb₂Te₃ and of the TiTe₂ confining material allows for a better control of multiple intermediate resistance states and for a lower drift with time of the electrical resistance of the amorphous phase. In this work, we consider to substitute Sb₂Te₃ with the Ge₂Sb₂Te₅ prototypical phase change compound that should feature better data retention. By exploiting molecular dynamics simulations with a machine learning interatomic potential, we have investigated the crystallization kinetics of Ge₂Sb₂Te₅ nanoconfined in geometries mimicking Ge₂Sb₂Te₅/TiTe₂ superlattices. It turns out that nanoconfinement induces a slight reduction in the crystal growth velocities with respect to the bulk, but also an enhancement of the nucleation rate due to heterogeneous nucleation. The results support the idea of investigating Ge₂Sb₂Te₅/TiTe₂ superlattices for applications in neuromorphic devices with improved data retention. The effect on the crystallization kinetics of the addition of van der Waals interaction to the interatomic potential is also discussed.
DOI: 10.24435/materialscloud:f0-bh
title: Simulation of the crystallization process of Ge₂Sb₂Te₅ nanoconfined in superlattice geometries for phase change memories

description: Phase change materials are the most promising candidates for the realization of artificial synapsis for neuromorphic computing. Different resistance levels corresponding to analogic values of the
synapsis conductance can be achieved by modulating the size of an amorphous region embedded in its crystalline matrix. Recently, it has been proposed that a superlattice made of alternating layers of the phase change compound Sb₂Te₃ and of the TiTe₂ confining material allows for a better control of multiple intermediate resistance states and for a lower drift with time of the electrical resistance of the amorphous phase. In this work, we consider to substitute Sb₂Te₃ with the Ge₂Sb₂Te₅ prototypical phase change compound that should feature better data retention. By exploiting molecular dynamics simulations with a machine learning interatomic potential, we have investigated the crystallization kinetics of Ge₂Sb₂Te₅ nanoconfined in geometries mimicking Ge₂Sb₂Te₅/TiTe₂ superlattices. It turns out that nanoconfinement induces a slight reduction in the crystal growth velocities with respect to the bulk, but also an enhancement of the nucleation rate due to heterogeneous nucleation. The results support the idea of investigating Ge₂Sb₂Te₅/TiTe₂ superlattices for applications in neuromorphic devices with improved data retention. The effect on the crystallization kinetics of the addition of van der Waals interaction to the interatomic potential is also discussed.
DOI: 10.24435/materialscloud:v0-gn
title: Stabilization of oxygen vacancy ordering and electrochemical-proton-insertion-and- extraction-induced large resistance modulation in strontium iron cobalt oxides Sr(Fe,Co)Oy

description: Promoting hydrogen (H) insertion into and extraction from metal oxides plays a crucial role in tuning their properties. In our recent work, we found that the oxygen vacancy ordering in Sr(Fe,Co)Oy (SFCO) thin films can be stabilized by increasing the Co content and revealed that this stabilization is key to promoting the H insertion into SFCO oxides. This archive provides the computational inputs and crystal structures to elucidate the energies of oxygen reduction and hydrogen insertion reactions for SFCO perovskite oxides.
DOI: 10.24435/materialscloud:6e-aj
title: Experimental and Theoretical Insights on Gas Trapping in MOFs: A Case Study with Noble Gases and MFU-4 Type MOFs

description: Isostructural metal-organic frameworks (MOFs), namely MFU-4 and MFU-4-Br, in which the pore apertures are defined by anionic side ligands (Cl− and Br−, respectively), were synthesized and loaded with noble gases. By selecting the type of side ligand, one can fine-tune the pore aperture size, allowing for precise regulation of the entry and release of gas guests. In this study, we conducted experiments to examine gas loading and release using krypton and xenon as model gases, and we complemented our findings with computational modeling. Remarkably, the loaded gas guests remained trapped inside the pores even after being exposed to air under ambient conditions for extended periods, in some cases for up to several weeks. Therefore, we focused on determining the energy barrier preventing gas release using both theoretical and experimental methods. The results were compared in relation to the types of hosts and guests, providing valuable insights into the gas trapping process in MOFs, as well as programmed gas release in air under ambient conditions. Furthermore, the crystal structure of MFU-4-Br was elucidated using the three-dimensional electron diffraction (3DED) technique, and the bulk purity of the sample was subsequently verified through Rietveld refinement. The data in this record are supplementary data to the manuscript with DOI 10.26434/chemrxiv-2024-vb8pj.
DOI: 10.24435/materialscloud:et-ww
title: Stabilization of oxygen vacancy ordering and electrochemical-proton-insertion-and- extraction-induced large resistance modulation in strontium iron cobalt oxides Sr(Fe,Co)Oy

description: Promoting hydrogen (H) insertion into and extraction from metal oxides plays a crucial role in tuning their properties. In our recent work, we found that the oxygen vacancy ordering in Sr(Fe,Co)Oy (SFCO) thin films can be stabilized by increasing the Co content and revealed that this stabilization is key to promoting the H insertion into SFCO oxides. This archive provides the computational inputs and crystal structures to elucidate the energies of oxygen reduction and hydrogen insertion reactions for SFCO perovskite oxides.
DOI: 10.24435/materialscloud:82-75
title: Experimental and Theoretical Insights on Gas Trapping in MOFs: A Case Study with Noble Gases and MFU-4 Type MOFs

description: Isostructural metal-organic frameworks (MOFs), namely MFU-4 and MFU-4-Br, in which the pore apertures are defined by anionic side ligands (Cl− and Br−, respectively), were synthesized and loaded with noble gases. By selecting the type of side ligand, one can fine-tune the pore aperture size, allowing for precise regulation of the entry and release of gas guests. In this study, we conducted experiments to examine gas loading and release using krypton and xenon as model gases, and we complemented our findings with computational modeling. Remarkably, the loaded gas guests remained trapped inside the pores even after being exposed to air under ambient conditions for extended periods, in some cases for up to several weeks. Therefore, we focused on determining the energy barrier preventing gas release using both theoretical and experimental methods. The results were compared in relation to the types of hosts and guests, providing valuable insights into the gas trapping process in MOFs, as well as programmed gas release in air under ambient conditions. Furthermore, the crystal structure of MFU-4-Br was elucidated using the three-dimensional electron diffraction (3DED) technique, and the bulk purity of the sample was subsequently verified through Rietveld refinement. The data in this record are supplementary data to the manuscript with DOI 10.26434/chemrxiv-2024-vb8pj.
DOI: 10.24435/materialscloud:e2-k7
title: Quasiparticle self-consistent GW with effective vertex corrections in the polarizability and the self-energy applied to MnO, FeO, CoO, and NiO

description: Through quasiparticle self-consistent GW, we investigate the electronic structure of the antiferromagnetic ground state of four transition-metal monoxides: MnO, FeO, CoO, and NiO. In addition to the random-phase approximation, we consider two different schemes incorporating effective vertex corrections. The first scheme includes in the polarizability a vertex function derived from the solution of the Bethe-Salpeter equation (BSE), whereas the second scheme includes in both the polarizability and self-energy a vertex function, which carries a long-range part satisfying the Ward identity and a short-range part derived from the adiabatic local density approximation. Our results include fundamental band gaps, macroscopic dielectric constants, and local magnetic moments, emphasizing the role of vertex corrections in the description of these key electronic properties. We provide quasiparticle band structures and projected densities of states allowing us to establish a connection with the Mott insulator picture and to highlight the overall good agreement with experimental photoemission spectra. The inclusion of the vertex in the self-energy preserves the overall shape of the band structures but generally produces larger rigid energy shifts for d bands than for sp bands. Through the solution of the Bethe-Salpeter equation, we determine excitonic effects and obtain dielectric response functions. Despite the experimental uncertainties, which appear sizable in the case of FeO, it is possible to discern a good general correspondence between the calculated and measured spectra, particularly for the absorption onsets and the peak positions. Furthermore, deep excitons are found to occur in the absorption spectra of FeO, CoO, and NiO, in qualitative agreement with the available characterization. Our work indicates that many-body perturbation theory including effective vertex corrections is able to provide a quantitatively accurate description of key electronic-structure features of transition-metal monoxides.
DOI: 10.24435/materialscloud:fx-nr
title: Quasiparticle self-consistent GW with effective vertex corrections in the polarizability and the self-energy applied to MnO, FeO, CoO, and NiO

description: Through quasiparticle self-consistent GW, we investigate the electronic structure of the antiferromagnetic ground state of four transition-metal monoxides: MnO, FeO, CoO, and NiO. In addition to the random-phase approximation, we consider two different schemes incorporating effective vertex corrections. The first scheme includes in the polarizability a vertex function derived from the solution of the Bethe-Salpeter equation (BSE), whereas the second scheme includes in both the polarizability and self-energy a vertex function, which carries a long-range part satisfying the Ward identity and a short-range part derived from the adiabatic local density approximation. Our results include fundamental band gaps, macroscopic dielectric constants, and local magnetic moments, emphasizing the role of vertex corrections in the description of these key electronic properties. We provide quasiparticle band structures and projected densities of states allowing us to establish a connection with the Mott insulator picture and to highlight the overall good agreement with experimental photoemission spectra. The inclusion of the vertex in the self-energy preserves the overall shape of the band structures but generally produces larger rigid energy shifts for d bands than for sp bands. Through the solution of the Bethe-Salpeter equation, we determine excitonic effects and obtain dielectric response functions. Despite the experimental uncertainties, which appear sizable in the case of FeO, it is possible to discern a good general correspondence between the calculated and measured spectra, particularly for the absorption onsets and the peak positions. Furthermore, deep excitons are found to occur in the absorption spectra of FeO, CoO, and NiO, in qualitative agreement with the available characterization. Our work indicates that many-body perturbation theory including effective vertex corrections is able to provide a quantitatively accurate description of key electronic-structure features of transition-metal monoxides.
DOI: 10.24435/materialscloud:sy-35
title: Dislocation-grain boundary interaction dataset for FCC Cu

description: Dislocation-grain boundary play a major role in the strength and ductility of structural materials. An understanding of governing parameters such as grain boundary local atomic structures on the outcome of this interaction can accelerate new alloy design strategies that tailors materials' microstructures. Previous studies have focused only on the subset of minimum-energy grain boundary structures. We present a comprehensive database of dislocation-grain boundary interaction for edge, screw, and 60o mixed dislocation with 587 < 110 > and < 112 > symmetric tilt grain boundary in FCC Cu consisting of 73 minimum-energy grain boundary structures and 514 metastable ones. The dataset contains the outcomes for 5234 unique interactions with a particular dislocation type, grain boundary structure, and applied shear stress.