cometadata/datacite-titles-descriptions-related-identifiers huggingface dataset:
DOI: 10.24435/materialscloud:xx-pr
title: Computational synthesis of substrates by crystal cleavage

description: In order to identify novel substrate materials, we developed a high-throughput bond breaking algorithm. This algorithm takes a three-dimensional crystal as input, systematically breaks bonds, and checks if the bonding network has been reduced to two periodic directions. We apply this algorithm to Materials Project database and identify 4,693 symmetrically unique cleaved surfaces across 2,133 crystals. We then characterize the thermodynamic stability of these cleaved surfaces using the DFT software VASP, characterizing 3,991 surfaces as potential substrates with energy comparable to the experimentally used substrates (0001) AlN, ZnO, and CdS.

This repository contains the structure files, setting files, pseudopotential choices, bulk precursor structure and MaterialsProject ID, and thermodynamic data for the substrates considered in this work.
DOI: 10.24435/materialscloud:36-ww
title: Nonempirical semilocal density functionals for correcting the self-interaction of polaronic states

description: Through the use of the piecewise-linearity condition of the total energy, we correct the self-interaction for the study of polarons by constructing nonempirical functionals at the semilocal level of theory. We consider two functionals, the γDFT and the μDFT functionals, both of which are based on the addition of a weak local  potential to the semilocal Hamiltonian to enforce the piecewise-linearity condition. We show that the resulting polaron properties are in good agreement with reference hybrid functional calculations. This supports the use of semilocal functionals for calculating polaron properties.
DOI: 10.24435/materialscloud:2q-0b
title: Nonempirical semilocal density functionals for correcting the self-interaction of polaronic states

description: Through the use of the piecewise-linearity condition of the total energy, we correct the self-interaction for the study of polarons by constructing nonempirical functionals at the semilocal level of theory. We consider two functionals, the γDFT and the μDFT functionals, both of which are based on the addition of a weak local  potential to the semilocal Hamiltonian to enforce the piecewise-linearity condition. We show that the resulting polaron properties are in good agreement with reference hybrid functional calculations. This supports the use of semilocal functionals for calculating polaron properties.
DOI: 10.24435/materialscloud:yn-de
title: Diversifying databases of metal organic frameworks for high-throughput computational screening

description: By combining metal nodes and organic linkers, an  infinite number of metal organic frameworks (MOFs) can be designed in silico. When making new databases of such hypothetical MOFs, we need to assure that they not only contribute towards the growth of the count of structures but also add different chemistry to existing databases. In this work, we designed a database of ~20,000 hypothetical MOFs which are diverse in terms of their chemical design space—metal nodes, organic linkers, functional groups and pore geometries. Using Machine Learning techniques, we visualized and quantified the diversity of these structures. We then assessed the usefulness of diverse structures by evaluating their performance, using grand-canonical Monte Carlo simulations, in two important environmental applications---post combustion carbon capture and hydrogen storage. We find that many of these structures perform better than widely used benchmark materials such as Zeolite-13X (for post combustion carbon capture) and MOF-5 (for hydrogen storage).
DOI: 10.24435/materialscloud:90-4r
title: Diversifying databases of metal organic frameworks for high-throughput computational screening

description: By combining metal nodes and organic linkers, an  infinite number of metal organic frameworks (MOFs) can be designed in silico. When making new databases of such hypothetical MOFs, we need to assure that they not only contribute towards the growth of the count of structures but also add different chemistry to existing databases. In this work, we designed a database of ~20,000 hypothetical MOFs which are diverse in terms of their chemical design space—metal nodes, organic linkers, functional groups and pore geometries. Using Machine Learning techniques, we visualized and quantified the diversity of these structures. We then assessed the usefulness of diverse structures by evaluating their performance, using grand-canonical Monte Carlo simulations, in two important environmental applications---post combustion carbon capture and hydrogen storage. We find that many of these structures perform better than widely used benchmark materials such as Zeolite-13X (for post combustion carbon capture) and MOF-5 (for hydrogen storage).
DOI: 10.24435/materialscloud:r7-pc
title: Two-component density functional theory study of quantized muons in solids

description: The quantum effect of light nuclei in materials is usually considered as lattice vibration and zero-point motion (ZPM) from an ab initio perspective. Here we start from full-quantized particles and take the muon as an example, considering the two-body quantized system of the muon and the electrons within Two-Component Density Functional Theory, which can calculate the related two-body wave functions directly and automatically taking into account the quantum effect of the muon. This is an attempt to reveal the quantum effect of light nuclei in materials from a different respect. It is tested in some metallic systems (Fe-bcc, Co-fcc, Co-hcp) and some non-metallic systems (NaF, CaF₂, diamond), we finally find this fundamental method agrees better with experiments and shows good potential for further such study.
DOI: 10.24435/materialscloud:qn-04
title: Two-component density functional theory study of quantized muons in solids

description: The quantum effect of light nuclei in materials is usually considered as lattice vibration and zero-point motion (ZPM) from an ab initio perspective. Here we start from full-quantized particles and take the muon as an example, considering the two-body quantized system of the muon and the electrons within Two-Component Density Functional Theory, which can calculate the related two-body wave functions directly and automatically taking into account the quantum effect of the muon. This is an attempt to reveal the quantum effect of light nuclei in materials from a different respect. It is tested in some metallic systems (Fe-bcc, Co-fcc, Co-hcp) and some non-metallic systems (NaF, CaF₂, diamond), we finally find this fundamental method agrees better with experiments and shows good potential for further such study.
DOI: 10.24435/materialscloud:br-jf
title: Dynamics of the charge transfer to solvent process in aqueous iodide

description: Charge-transfer-to-solvent states in aqueous halides are ideal systems for studying the electron-transfer dynamics to the solvent involving a complex interplay between electronic excitation and solvent polarization. Despite extensive experimental investigations, a full picture of the charge-transfer-to-solvent dynamics has remained elusive. Here, we visualise the intricate interplay between the dynamics of the electron and the solvent polarization occurring in this process. Through the combined use of ab initio molecular dynamics and machine learning methods, we investigate the structure, dynamics and free energy as the excited electron evolves through the charge-transfer-to-solvent process, which we characterize as a sequence of states denoted charge-transfer-to-solvent, contact-pair, solvent-separated, and hydrated electron states, depending on the distance between the iodine and the excited electron. Our assignment of the charge-transfer-to-solvent states is supported by the good agreement between calculated and measured vertical binding energies. Our results reveal the charge transfer process in terms of the underlying atomic processes and mechanisms.
DOI: 10.24435/materialscloud:nf-vk
title: Dynamics of the charge transfer to solvent process in aqueous iodide

description: Charge-transfer-to-solvent states in aqueous halides are ideal systems for studying the electron-transfer dynamics to the solvent involving a complex interplay between electronic excitation and solvent polarization. Despite extensive experimental investigations, a full picture of the charge-transfer-to-solvent dynamics has remained elusive. Here, we visualise the intricate interplay between the dynamics of the electron and the solvent polarization occurring in this process. Through the combined use of ab initio molecular dynamics and machine learning methods, we investigate the structure, dynamics and free energy as the excited electron evolves through the charge-transfer-to-solvent process, which we characterize as a sequence of states denoted charge-transfer-to-solvent, contact-pair, solvent-separated, and hydrated electron states, depending on the distance between the iodine and the excited electron. Our assignment of the charge-transfer-to-solvent states is supported by the good agreement between calculated and measured vertical binding energies. Our results reveal the charge transfer process in terms of the underlying atomic processes and mechanisms.
DOI: 10.24435/materialscloud:rd-wm
title: Perturbative spin-orbit couplings for the simulation of extended framework materials

description: A comprehensive description of photo-chemical processes in materials, comprising spin-forbidden processes such as intersystem crossing and phosphorescence, implies to take into account spin-orbit coupling. We present an efficient implementation of a perturbative spin-orbit coupling correction for the Tamm-Dancoff approximation of linear-response time-dependent density functional theory within a mixed Gaussian and plane waves framework relying on spin-orbit coupling corrected pseudopotentials. The implementation is validated for a benchmark set of small aromatic molecules, with mean errors in excitation energies and spin-orbit coupling matrix elements being in the range of 0.1 - 0.6 eV and 1.0 to 13.8 cm⁻¹ in comparison to density functional theory and density functional theory multi-reference configuration interaction reference results. Computational timings are given for a bismuth-containing metal-organic framework. 
The data in this record are supplementary data to the manuscript linked below.
DOI: 10.24435/materialscloud:1b-aa
title: One dimensional edge localized YSR states in CrCl₃ on NbSe₂

description: Magnet/superconductor hybrid systems have been put forward as a platform for realizing topological superconductivity. We investigated the heterostructure of ferromagnetic monolayer CrCl₃ and superconducting NbSe₂. Using low-temperature scanning tunneling microscopy, we observe topologically trivial Yu-Shiba-Rusinov (YSR) states localized at the edge of CrCl₃ islands. DFT simulations reveal that the Cr atoms at the edge have an enhanced d-orbital DOS close to the Fermi energy. This leads to an exchange coupling between these atoms and the substrate that rationalizes the edge-localization of the YSR states.

This dataset contains the first-principles calculations performed on a nanoribbon of CrCl₃ on NbSe₂ and the associated notebooks used to generate figures from this data.
DOI: 10.24435/materialscloud:zs-q9
title: Perturbative spin-orbit couplings for the simulation of extended framework materials

description: A comprehensive description of photo-chemical processes in materials, comprising spin-forbidden processes such as intersystem crossing and phosphorescence, implies to take into account spin-orbit coupling. We present an efficient implementation of a perturbative spin-orbit coupling correction for the Tamm-Dancoff approximation of linear-response time-dependent density functional theory within a mixed Gaussian and plane waves framework relying on spin-orbit coupling corrected pseudopotentials. The implementation is validated for a benchmark set of small aromatic molecules, with mean errors in excitation energies and spin-orbit coupling matrix elements being in the range of 0.1 - 0.6 eV and 1.0 to 13.8 cm⁻¹ in comparison to density functional theory and density functional theory multi-reference configuration interaction reference results. Computational timings are given for a bismuth-containing metal-organic framework. 
The data in this record are supplementary data to the manuscript linked below.
DOI: 10.24435/materialscloud:aa-2q
title: One dimensional edge localized YSR states in CrCl₃ on NbSe₂

description: Magnet/superconductor hybrid systems have been put forward as a platform for realizing topological superconductivity. We investigated the heterostructure of ferromagnetic monolayer CrCl₃ and superconducting NbSe₂. Using low-temperature scanning tunneling microscopy, we observe topologically trivial Yu-Shiba-Rusinov (YSR) states localized at the edge of CrCl₃ islands. DFT simulations reveal that the Cr atoms at the edge have an enhanced d-orbital DOS close to the Fermi energy. This leads to an exchange coupling between these atoms and the substrate that rationalizes the edge-localization of the YSR states.

This dataset contains the first-principles calculations performed on a nanoribbon of CrCl₃ on NbSe₂ and the associated notebooks used to generate figures from this data.
DOI: 10.24435/materialscloud:j2-h8
title: Data and analyses for first proton-coupled electron transfer of water oxidation at the BiVO₄-water interface

description: This entry provides original trajectories of on-the-fly probability enhanced sampling (OPES) and of molecular dynamics simulations and images of nudged-elastic band (NEB) calculation. Jupyter notebooks are provided for a NEB profile, NEB collective variables, free energy surface of the OPES simulations, hole transfer of the OPES simulations, proton transfer mechanisms of of the OPES simulations, water density profiles of MD simulations, radial distribution functions of MD simulations, reweight of Bi-O bonds of OPES simulations, coordination numbers of surface Bi atoms and hydrogen-bond analysis of proton transfer.
DOI: 10.24435/materialscloud:wq-w4
title: Data and analyses for first proton-coupled electron transfer of water oxidation at the BiVO₄-water interface

description: This entry provides original trajectories of on-the-fly probability enhanced sampling (OPES) and of molecular dynamics simulations and images of nudged-elastic band (NEB) calculation. Jupyter notebooks are provided for a NEB profile, NEB collective variables, free energy surface of the OPES simulations, hole transfer of the OPES simulations, proton transfer mechanisms of of the OPES simulations, water density profiles of MD simulations, radial distribution functions of MD simulations, reweight of Bi-O bonds of OPES simulations, coordination numbers of surface Bi atoms and hydrogen-bond analysis of proton transfer.
DOI: 10.60686/t-fsd3616
title: FSD3616 Finnish Student Health and Well-being Survey 2021
DOI: 10.24435/materialscloud:x8-7y
title: Tunable topological phases in nanographene-based spin-½ alternating-exchange Heisenberg chains

description: Unlocking the potential of topological order within many-body spin systems has long been a central pursuit in the realm of quantum materials. Despite extensive efforts, the quest for a versatile platform enabling site-selective spin manipulation, essential for tuning and probing diverse topological phases, has persisted. Here, we utilize on-surface synthesis to construct spin-1/2 alternating-exchange Heisenberg (AH) chains with antiferromagnetic couplings J1 and J2 by covalently linking Clar's goblets -- nanographenes each hosting two antiferromagnetically-coupled unpaired electrons. In a recent work, utilizing scanning tunneling microscopy, we exert atomic-scale control over the spin chain lengths, parities and exchange-coupling terminations, and probe their magnetic response by means of inelastic tunneling spectroscopy. Our investigation confirms the gapped nature of bulk excitations in the chains, known as triplons. Besides, the triplon dispersion relation is successfully extracted from the spatial variation of tunneling spectral amplitudes. Furthermore, depending on the parity and termination of chains, we observe varying numbers of in-gap S=1/2 edge spins, enabling the determination of the degeneracy of distinct topological ground states in the thermodynamic limit-either 1, 2, or 4. By monitoring interactions between these edge spins, we identify the exponential decay of spin correlations. Our experimental findings, corroborated by theoretical calculations, present a phase-controlled many-body platform, opening promising avenues toward the development of spin-based quantum devices. The record contains data and codes that support the results discussed in the manuscript.
DOI: 10.24435/materialscloud:fk-jg
title: Device-to-materials pathway for electron traps detection in amorphous GeSe-based selectors

description: The choice of the ideal material employed in selector devices is a tough task both from the theoretical and experimental side, especially due to the lack of a synergistic approach between techniques able to correlate specific material properties with device characteristics. Using a material-to-device multiscale technique, a reliable protocol for an efficient characterization of the active traps in amorphous GeSe chalcogenide is proposed. The resulting trap maps trace back the specific features of materials responsible for the measured findings, and connect them to an atomistic description of the sample. The metrological approach can be straightforwardly extended to other materials and devices, which is very beneficial for an efficient material-device codesign and the optimization of novel technologies.
DOI: 10.24435/materialscloud:qw-vr
title: Tunable topological phases in nanographene-based spin-½ alternating-exchange Heisenberg chains

description: Unlocking the potential of topological order within many-body spin systems has long been a central pursuit in the realm of quantum materials. Despite extensive efforts, the quest for a versatile platform enabling site-selective spin manipulation, essential for tuning and probing diverse topological phases, has persisted. Here, we utilize on-surface synthesis to construct spin-1/2 alternating-exchange Heisenberg (AH) chains with antiferromagnetic couplings J1 and J2 by covalently linking Clar's goblets -- nanographenes each hosting two antiferromagnetically-coupled unpaired electrons. In a recent work, utilizing scanning tunneling microscopy, we exert atomic-scale control over the spin chain lengths, parities and exchange-coupling terminations, and probe their magnetic response by means of inelastic tunneling spectroscopy. Our investigation confirms the gapped nature of bulk excitations in the chains, known as triplons. Besides, the triplon dispersion relation is successfully extracted from the spatial variation of tunneling spectral amplitudes. Furthermore, depending on the parity and termination of chains, we observe varying numbers of in-gap S=1/2 edge spins, enabling the determination of the degeneracy of distinct topological ground states in the thermodynamic limit-either 1, 2, or 4. By monitoring interactions between these edge spins, we identify the exponential decay of spin correlations. Our experimental findings, corroborated by theoretical calculations, present a phase-controlled many-body platform, opening promising avenues toward the development of spin-based quantum devices. The record contains data and codes that support the results discussed in the manuscript.
DOI: 10.24435/materialscloud:aa-2w
title: Data-driven discovery of organic electronic materials enabled by hybrid top-down/bottom-up design

description: The high-throughput molecular exploration and screening of organic electronic materials often starts with either a 'top-down' mining of existing repositories, or the 'bottom-up' assembly of fragments based on predetermined rules and known synthetic templates. In both instances, the datasets used are often produced on a case-by-case basis, and require the high-quality computation of electronic properties and extensive user input: curation in the top-down approach, and the construction of a fragment library and introduction of rules for linking them in the bottom-up approach. Both approaches are time-consuming and require significant computational resources. Here, we generate a top-down set named FORMED consisting of 117K synthesized molecules containing their optimized structures, associated electronic and topological properties and chemical composition, and use these structures as a vast library of molecular building blocks for bottom-up fragment-based materials design. A tool is developed to automate the coupling of these building block units based on their available Csp2-H bonds, thus providing a fundamental link between the two philosophies of dataset construction. Statistical models are trained on this dataset and a subset of the resulting hybrid top-down/bottom-up compounds (selected dimers), which enable on-the-fly prediction of key ground state (frontier molecular orbital gaps) and excited state (S1 and T1 energies) properties from molecular geometries with high accuracy across all known p-block organic compound space.
With access to ab initio-quality optical properties in hand, it is possible to apply this bottom-up pipeline using existing compounds as molecular building blocks to any materials design campaign. To illustrate this, we construct and screen over a million molecular candidates (predicted dimers) for efficient intramolecular singlet fission, the leading candidates of which provide insight into the structural features that may promote this multiexciton-generating process.
DOI: 10.24435/materialscloud:ht-m2
title: Device-to-materials pathway for electron traps detection in amorphous GeSe-based selectors

description: The choice of the ideal material employed in selector devices is a tough task both from the theoretical and experimental side, especially due to the lack of a synergistic approach between techniques able to correlate specific material properties with device characteristics. Using a material-to-device multiscale technique, a reliable protocol for an efficient characterization of the active traps in amorphous GeSe chalcogenide is proposed. The resulting trap maps trace back the specific features of materials responsible for the measured findings, and connect them to an atomistic description of the sample. The metrological approach can be straightforwardly extended to other materials and devices, which is very beneficial for an efficient material-device codesign and the optimization of novel technologies.