cometadata/datacite-titles-descriptions-related-identifiers huggingface dataset:
DOI: 10.24435/materialscloud:xk-xk
title: Interface polarization in heterovalent core/shell nanocrystals

description: The potential profile and the energy level offset of core/shell heterostructured nanocrystals (h-NCs) determine the photophysical properties and the charge transport characteristics of h-NC solids. However, limited material choices for heavy metal-free III-V/II-VI h-NCs pose challenges in comprehensive control of the potential profile. Herein, we present an approach to such control by steering dipole densities at the interface of III-V/II-VI h-NCs. The controllable heterovalency at the interface is responsible for interfacial dipole densities that result in the vacuum-level shift, providing an additional knob for the control of optical and electrical characteristics of h-NCs. The synthesis of h-NCs with atomic precision allows us to correlate interfacial dipole moments with the nanocrystals' photochemical stability and optoelectronic performance.

The description was referred to the abstract of the original paper. All numerical data of the main figures in the articles are included in this data repository.
In particular, each tab of the data file indicates each panel in the main figures.
Please refer to the main research article.
DOI: 10.24435/materialscloud:j9-fc
title: Interface polarization in heterovalent core/shell nanocrystals

description: The potential profile and the energy level offset of core/shell heterostructured nanocrystals (h-NCs) determine the photophysical properties and the charge transport characteristics of h-NC solids. However, limited material choices for heavy metal-free III-V/II-VI h-NCs pose challenges in comprehensive control of the potential profile. Herein, we present an approach to such control by steering dipole densities at the interface of III-V/II-VI h-NCs. The controllable heterovalency at the interface is responsible for interfacial dipole densities that result in the vacuum-level shift, providing an additional knob for the control of optical and electrical characteristics of h-NCs. The synthesis of h-NCs with atomic precision allows us to correlate interfacial dipole moments with the nanocrystals' photochemical stability and optoelectronic performance.

The description was referred to the abstract of the original paper. All numerical data of the main figures in the articles are included in this data repository.
In particular, each tab of the data file indicates each panel in the main figures.
Please refer to the main research article.
DOI: 10.24435/materialscloud:gs-fc
title: Electronic structure and magnetism of pristine and Fe-doped α-MnO₂ from density-functional theory with extended Hubbard functionals

description: We present a first-principles investigation of the structural, electronic, and magnetic properties of the pristine and Fe-doped α-MnO₂ using density-functional theory with extended Hubbard functionals. The onsite U and intersite V Hubbard parameters are determined from first principles and self-consistently using density-functional perturbation theory in the basis of Löwdin-orthogonalized atomic orbitals. Among the ferromagnetic and four types of antiferromagnetic (AFM) orderings for the pristine α-MnO₂ we find the C2-AFM spin configuration to be the most energetically favorable, in agreement with the experimentally observed AFM state. The computed lattice parameters, magnetic moments, and band gaps are overall in good agreement with the experimental ones when both the onsite and intersite Hubbard corrections are included. For the Fe-doped α-MnO₂ two types of doping are considered: Fe insertion in the 2 × 2 tunnels and partial substitution of Fe for Mn. The calculated formation energies show that Fe insertion is energetically favorable, in agreement with experiments. We find that both types of doping preserve the C2 AFM spin configuration of the host lattice. The oxidation state of Fe is found to be 2+ and 4+ in the case of the interstitial and substitutional doping, respectively, while the oxidation state of Mn is 4+ in both cases. This work opens a door for accurate studies of other Mn oxides and complex transition-metal compounds when the localization of 3d electrons occurs in the presence of strong covalent interactions with ligands.
DOI: 10.24435/materialscloud:r5-gx
title: A new dataset of 175k stable and metastable materials calculated with the PBEsol and SCAN functionals

description: In the past decade we have witnessed the appearance of large databases of calculated material properties. These are most often obtained with the Perdew-Burke-Ernzerhof (PBE) functional of density-functional theory, a well established and reliable technique that is by now the standard in materials science. However, there have been recent theoretical developments that allow for an increased accuracy in the calculations. Here, we present a dataset of calculations for 175k solid-state materials obtained with two improved functionals: PBE for solids (that yields consistently better geometries than the PBE) and SCAN (probably the best all-around functional at the moment). Our results provide an accurate overview of the landscape of stable (and nearly stable) materials, and as such can be used for more reliable predictions of novel compounds. They can also be used for training machine learning models, or even for the comparison and benchmark of PBE, PBE for solids, and SCAN.
DOI: 10.24435/materialscloud:br-33
title: Critical step in the HCl oxidation reaction over single-crystalline CeO2−x(111): Peroxo-induced site change of strongly adsorbed surface chlorine

description: The catalytic oxidation of HCl by molecular oxygen (Deacon process) over ceria allows the recovery of molecular chlorine from omnipresent HCl waste produced in various industrial processes. In previous density functional theory (DFT) model calculations by Amrute et al. [J. Catal. 2012, 286, 287–297.], it was proposed that the most critical reaction step in this process is the displacement of tightly bound chlorine at a vacant oxygen position on the CeO2(111) surface (Clvac) toward a less strongly bound cerium on-top (Cltop) position. This step is highly endothermic by more than 2 eV. On the basis of a dedicated model study, namely the re-oxidation of a chlorinated single crystalline Clvac-CeO2−x(111)-(√3 × √3)R30° surface structure, we provide in-situ synchrotron-based spectroscopic data (high-resolution core level spectroscopy (HRCLS) and X-ray adsorption near edge structure (XANES)) for this oxygen-induced de-chlorination process. Combined with theoretical evidence from DFT calculations, the Clvac → Cltop displacement reaction is predicted to be induced by an adsorbed peroxo species (O22-), making the displacement step concerted and exothermic by only 0.6 eV with an activation barrier of only 1.04 eV. The peroxo species is shown to be important for the re-oxidation of Clvac-CeO2−x(111) and is considered essential for understanding the function of ceria in oxidation catalysis.
DOI: 10.24435/materialscloud:dq-1c
title: Critical step in the HCl oxidation reaction over single-crystalline CeO2−x(111): Peroxo-induced site change of strongly adsorbed surface chlorine

description: The catalytic oxidation of HCl by molecular oxygen (Deacon process) over ceria allows the recovery of molecular chlorine from omnipresent HCl waste produced in various industrial processes. In previous density functional theory (DFT) model calculations by Amrute et al. [J. Catal. 2012, 286, 287–297.], it was proposed that the most critical reaction step in this process is the displacement of tightly bound chlorine at a vacant oxygen position on the CeO2(111) surface (Clvac) toward a less strongly bound cerium on-top (Cltop) position. This step is highly endothermic by more than 2 eV. On the basis of a dedicated model study, namely the re-oxidation of a chlorinated single crystalline Clvac-CeO2−x(111)-(√3 × √3)R30° surface structure, we provide in-situ synchrotron-based spectroscopic data (high-resolution core level spectroscopy (HRCLS) and X-ray adsorption near edge structure (XANES)) for this oxygen-induced de-chlorination process. Combined with theoretical evidence from DFT calculations, the Clvac → Cltop displacement reaction is predicted to be induced by an adsorbed peroxo species (O22-), making the displacement step concerted and exothermic by only 0.6 eV with an activation barrier of only 1.04 eV. The peroxo species is shown to be important for the re-oxidation of Clvac-CeO2−x(111) and is considered essential for understanding the function of ceria in oxidation catalysis.
DOI: 10.24435/materialscloud:8n-bm
title: Pivotal role of intersite Hubbard interactions in Fe-doped α-MnO₂

description: We present a first-principles investigation of the structural, electronic, and magnetic properties of the pristine and Fe-doped α-MnO₂ using density-functional theory with extended Hubbard functionals. The onsite U and intersite V Hubbard parameters are determined from first principles and self-consistently using density-functional perturbation theory in the basis of Löwdin-orthogonalized atomic orbitals. First, we analyze the pristine α-MnO₂ and show that the C2-AFM spin configuration is the most energetically favorable, in agreement with the experimentally observed antiferromagnetic state. For the Fe-doped α-MnO₂ two types of doping are considered: Fe insertion in the 2 × 2 tunnels and partial substitution of Fe for Mn. The calculated formation energies show that the experimentally observed Fe insertion is energetically favorable only when intersite Hubbard interactions are taken into account. Moreover, we find that both types of doping preserve the C2-AFM spin configuration of the host lattice only when Hubbard V corrections are included. The oxidation state of Fe is found to be +2 and +4 in the case of the interstitial and substitutional doping, respectively, while the oxidation state of Mn is +4 in both cases. This work opens a door for accurate studies of other Mn oxides and complex transition-metal compounds when the localization of 3d electrons occurs in the presence of strong covalent interactions with ligands.
DOI: 10.24435/materialscloud:cx-2m
title: Pivotal role of intersite Hubbard interactions in Fe-doped α-MnO₂

description: We present a first-principles investigation of the structural, electronic, and magnetic properties of the pristine and Fe-doped α-MnO₂ using density-functional theory with extended Hubbard functionals. The onsite U and intersite V Hubbard parameters are determined from first principles and self-consistently using density-functional perturbation theory in the basis of Löwdin-orthogonalized atomic orbitals. First, we analyze the pristine α-MnO₂ and show that the C2-AFM spin configuration is the most energetically favorable, in agreement with the experimentally observed antiferromagnetic state. For the Fe-doped α-MnO₂ two types of doping are considered: Fe insertion in the 2 × 2 tunnels and partial substitution of Fe for Mn. The calculated formation energies show that the experimentally observed Fe insertion is energetically favorable only when intersite Hubbard interactions are taken into account. Moreover, we find that both types of doping preserve the C2-AFM spin configuration of the host lattice only when Hubbard V corrections are included. The oxidation state of Fe is found to be +2 and +4 in the case of the interstitial and substitutional doping, respectively, while the oxidation state of Mn is +4 in both cases. This work opens a door for accurate studies of other Mn oxides and complex transition-metal compounds when the localization of 3d electrons occurs in the presence of strong covalent interactions with ligands.
DOI: 10.24435/materialscloud:gh-wt
title: The mapped gaussian process (MGP) force-field of Cu-Zn surface alloy

description: The mapped gaussian process (MGP) force-field used to elucidate the surface alloying of Cu-Zn. The force-field is made based on first-principles data by using machine-learning technique called Gaussian Process as implemented in FLARE package (https://github.com/mir-group/flare). Active and on-the-fly learning were employed to build the database efficiently. The simulation reveals atomistic details of the alloying process, i.e., the incorporation of deposited Zn adatoms to the Cu substrate. The surface alloying is found to start at upper and lower terraces near the step edge, which emphasize the role of steps and kinks in the alloying. The incorporation of Zn at the middle terrace was found at the later stage of the simulation.
DOI: 10.24435/materialscloud:fn-j7
title: The mapped gaussian process (MGP) force-field of Cu-Zn surface alloy

description: The mapped gaussian process (MGP) force-field used to elucidate the surface alloying of Cu-Zn. The force-field is made based on first-principles data by using machine-learning technique called Gaussian Process as implemented in FLARE package (https://github.com/mir-group/flare). Active and on-the-fly learning were employed to build the database efficiently. The simulation reveals atomistic details of the alloying process, i.e., the incorporation of deposited Zn adatoms to the Cu substrate. The surface alloying is found to start at upper and lower terraces near the step edge, which emphasize the role of steps and kinks in the alloying. The incorporation of Zn at the middle terrace was found at the later stage of the simulation.
DOI: 10.24435/materialscloud:er-mz
title: The impact of valley profile on the mobility and Kerr rotation of transition metal dichalcogenides

description: The transport and optical properties of semiconducting transition metal dichalcogenides around room temperature are dictated by electron-phonon scattering mechanisms within a complex, spin-textured and multi-valley electronic landscape. The relative positions of the valleys are critical, yet they are sensitive to external parameters and very difficult to determine directly. We propose a first-principles model as a function of valley positions to calculate carrier mobility and Kerr rotation angles, and apply it to MoS₂, WS₂, MoSe₂, and WSe₂. The model brings valuable insights, as well as quantitative predictions of macroscopic properties for a wide range of carrier density. The doping-dependant mobility displays a characteristic peak, the height depending on the position of the valleys. In parallel, the Kerr rotation signal is enhanced when same spin-valleys are aligned, and quenched when opposite spin-valleys are populated. We provide guidelines to optimize and correlate these quantities with respect to experimental parameters, as well as the theoretical support for in situ characterization of the valley positions. 
The dataset contains the necessary data, a jupyter notebook, a supporting python library, and a small app with a simple user interface to reproduce the results.
DOI: 10.24435/materialscloud:9m-en
title: BELLO: A post-processing tool for the local-order analysis of disordered systems

description: The characterization of the atomic structure of disordered systems, such as amorphous, glasses and (bio)molecule in solution, is a fundamental step for most theoretical investigations. The properties of short- and medium-range local order structures are responsible for the electronic, optical and transport properties of these systems. Here, we present the BELLO open source code, a post-processing script-tool created for the automatic analysis and extraction of structural characteristics of disordered and amorphous systems. BELLO is agnostic to the code that generated single configurations or trajectories, it provides an intuitive access through a graphical user interface (GUI), and it requires minimal computational resources. Its capabilities include the calculation of the order parameter , the folded structure identification, and statistical analysis tools such as atomic coordination number and pair/angle-distribution functions. The working principles of the code are described and tested on ab initio molecular dynamics trajectories of amorphous chalcogenides.

The code is also on the GitHub repository
https://github.com/behnood-dianat/BELLO
DOI: 10.24435/materialscloud:xm-jb
title: The impact of valley profile on the mobility and Kerr rotation of transition metal dichalcogenides

description: The transport and optical properties of semiconducting transition metal dichalcogenides around room temperature are dictated by electron-phonon scattering mechanisms within a complex, spin-textured and multi-valley electronic landscape. The relative positions of the valleys are critical, yet they are sensitive to external parameters and very difficult to determine directly. We propose a first-principles model as a function of valley positions to calculate carrier mobility and Kerr rotation angles, and apply it to MoS₂, WS₂, MoSe₂, and WSe₂. The model brings valuable insights, as well as quantitative predictions of macroscopic properties for a wide range of carrier density. The doping-dependant mobility displays a characteristic peak, the height depending on the position of the valleys. In parallel, the Kerr rotation signal is enhanced when same spin-valleys are aligned, and quenched when opposite spin-valleys are populated. We provide guidelines to optimize and correlate these quantities with respect to experimental parameters, as well as the theoretical support for in situ characterization of the valley positions. 
The dataset contains the necessary data, a jupyter notebook, a supporting python library, and a small app with a simple user interface to reproduce the results.
DOI: 10.24435/materialscloud:h2-x5
title: On-surface interchain coupling and skeletal rearrangement of indenofluorene polymers

description: On-surface synthesis serves as a powerful approach to construct π-conjugated carbon nanostructures that are not accessible by conventional wet chemistry. Nevertheless, this method has been limited by the types and numbers of available on-surface transformations. While the majority of successful cases exploit thermally triggered dehalogenative carbon–carbon coupling and cyclodehydrogenation, rearrangement of appropriate functional moieties has received limited research attention. In a recent work, we describe the unprecedented interchain coupling and thermally induced skeleton rearrangement  of (dihydro)indeno[2,1-b]fluorene (IF) polymers on an Au(111) surface under ultrahigh vacuum conditions, leading to different ladder polymers as well as fully fused graphene nanoribbon segments containing pentagonal and heptagonal rings. Au-coordinated nanoribbons are also observed. All structures are unambiguously characterized by high-resolution scanning probe microscopy. The results provide an avenue to fabricating a wider variety of π-conjugated polymers and carbon nanostructures comprising nonhexagonal rings as well as rarely explored organometallic nanoribbons. This record contains data of the calculations that support our results.
DOI: 10.24435/materialscloud:z4-yx
title: BELLO: A post-processing tool for the local-order analysis of disordered systems

description: The characterization of the atomic structure of disordered systems, such as amorphous, glasses and (bio)molecule in solution, is a fundamental step for most theoretical investigations. The properties of short- and medium-range local order structures are responsible for the electronic, optical and transport properties of these systems. Here, we present the BELLO open source code, a post-processing script-tool created for the automatic analysis and extraction of structural characteristics of disordered and amorphous systems. BELLO is agnostic to the code that generated single configurations or trajectories, it provides an intuitive access through a graphical user interface (GUI), and it requires minimal computational resources. Its capabilities include the calculation of the order parameter , the folded structure identification, and statistical analysis tools such as atomic coordination number and pair/angle-distribution functions. The working principles of the code are described and tested on ab initio molecular dynamics trajectories of amorphous chalcogenides.

The code is also on the GitHub repository
https://github.com/behnood-dianat/BELLO
DOI: 10.24435/materialscloud:jh-p0
title: On-surface interchain coupling and skeletal rearrangement of indenofluorene polymers

description: On-surface synthesis serves as a powerful approach to construct π-conjugated carbon nanostructures that are not accessible by conventional wet chemistry. Nevertheless, this method has been limited by the types and numbers of available on-surface transformations. While the majority of successful cases exploit thermally triggered dehalogenative carbon–carbon coupling and cyclodehydrogenation, rearrangement of appropriate functional moieties has received limited research attention. In a recent work, we describe the unprecedented interchain coupling and thermally induced skeleton rearrangement  of (dihydro)indeno[2,1-b]fluorene (IF) polymers on an Au(111) surface under ultrahigh vacuum conditions, leading to different ladder polymers as well as fully fused graphene nanoribbon segments containing pentagonal and heptagonal rings. Au-coordinated nanoribbons are also observed. All structures are unambiguously characterized by high-resolution scanning probe microscopy. The results provide an avenue to fabricating a wider variety of π-conjugated polymers and carbon nanostructures comprising nonhexagonal rings as well as rarely explored organometallic nanoribbons. This record contains data of the calculations that support our results.
DOI: 10.24435/materialscloud:p8-ey
title: Automatized discovery of polymer membranes with AI generative design and molecular dynamics simulations

description: Data sets and scripts for computational discovery of polymer membranes for carbon dioxide separation. The training data set with 1,169 homo-polymers provides carbon dioxide permeability, glass transition temperature and half decomposition temperature for each listed material. The output data set contains 784 optimized homo-polymer candidates generated by Inverse Design and Machine Learning techniques. The Jupyter notebook enables the use of the Polymer Property Prediction Engine as a service for generating the properties provided in the training data set.