49 Works

The geometric blueprint of perovskites

Feliciano Giustino & Marina R. Filip
Perovskite minerals form an essential component of the Earth’s mantle, and synthetic crystals are ubiquitous in electronics, photonics, and energy technology. The extraordinary chemical diversity of these crystals raises the question of how many and which perovskites are yet to be discovered. Here we show that the “no-rattling” principle postulated by Goldschmidt in 1926, describing the geometric conditions under which a perovskite can form, is much more effective than previously thought and allows us to...

Emergence of hidden phases of methylammonium lead-iodide (CH3NH3PbI) upon compression

Stefan Goedecker, Daniele Tomerini, José A. Flores-Livas, Ursula Rothlisberger, Ariadni Boziki & Maximilian Amsler
We perform a thorough structural search with the minima hopping method (MHM) to explore low-energy structures of methylammonium lead iodide. By combining the MHM with a forcefield, we efficiently screen vast portions of the configurational space with large simulation cells containing up to 96 atoms. Our search reveals two structures of methylammonium iodide perovskite (MAPI) that are substantially lower in energy than the well-studied experimentally observed low-temperature orthorhombic phase. The data set containing approximately ~180,000...

Barcodes for nanoporous materials

Senja D. Barthel, Berend Smit, Paweł Dłotko, Yongjin Lee, Kathryn Hess & S. Mohamad Moosavi
In most applications of nanoporous materials the pore structure is as important as the chemical composition as a determinant of performance. For example, one can alter performance in applications like carbon capture or methane storage by orders of magnitude by only modifying the pore structure. For these applications it is therefore important to identify the optimal pore geometry and use this information to find similar materials. However, the mathematical language and tools to identify materials...

In Silico Design of 2D and 3D Covalent Organic Frameworks for Methane Storage Applications

Aliaksandr V. Yakutovich, Leopold Talirz, Berend Smit, Rueih-Sheng Fu, Maciej Haranczyk & Rocio Mercado
Here we present 69,840 covalent organic frameworks (COFs) assembled in silico from a set of 666 distinct organic linkers into 2D-layered and 3D configurations. We investigate the feasibility of using these frameworks for methane storage by using grand-canonical Monte Carlo (GCMC) simulations to calculate their deliverable capacities (DCs). From these calculations, we predict that the best structure in the database is linker91_C_linker91_C_tbd, a structure composed of carbon-carbon bonded triazine linkers in the tbd topology. This...

Isobaric-Isothermal Monte Carlo Simulations of Bulk Liquid Water from MP2 and RPA Theory (MC Trajectories Data Download)

Mauro Del Ben, Joost VandeVondele & Juerg Hutter
Methods based on the second order Møller–Plesset perturbation theory (MP2) and the Random Phase Approximation (RPA) have emerged as practicable and reliable approaches to improve the accuracy of density functional approximations for first principle atomistic simulations. Such approaches are in fact capable to account ab-initio for non-local dynamical electron correlation effects, which play a fundamental role, for example, in the description of non-bonded interactions. To assess the performance of MP2 and RPA for real applications,...

Improving the Mechanical Stability of Metal-Organic Frameworks Using Chemical Caryatids

Berend Smit, Lev Sarkisov, Seyed Mohamad Moosavi & Peter G. Boyd
Metal-organic frameworks (MOFs) have emerged as versatile materials for applications ranging from gas separation and storage, catalysis, and sensing. The attractive feature of MOFs is that by changing the ligand and/or metal, they can be chemically tuned to perform optimally for a given application. In most, if not all, of these applications one also needs a material that has a sufficient mechanical stability, but our understanding of how changes in the chemical structure influence mechanical...

The Influence of Intrinsic Framework Flexibility on Adsorption in Nanoporous Materials (Data Download)

Berend Smit, Maciej Haranczyk, Ben Slater, Sanliang Ling, Matthew Witman, Sudi Jawahery & Peter G. Boyd
Project Abstract: For applications of metal-organic frameworks (MOFs) such as gas storage and separation, flexibility is often seen as a parameter that can tune material performance. In this work we aim to determine the optimal flexibility for the shape selective separation of similarly sized molecules (e.g., Xe/Kr mixtures). To obtain systematic insight into how the flexibility impacts this type of separation we develop a simple analytical model that predicts a material's Henry regime adsorption and...

High-throughput computational screening of nanoporous adsorbents for CO 2 capture from natural gas

Efrem Braun, Sondre Schnell, Wouter Thijssen, Jihan Kim, Li-Chiang Lin, Alexander F. Zurhelle, Joshua A. Thompson & Berend Smit
With the growth of natural gas as an energy source, upgrading CO2-contaminated supplies has become increasingly important. Here we develop a single metric that captures how well an adsorbent performs the separation of CH4 and CO2, and we then use this metric to computationally screen tens of thousands of all-silica zeolites. We show that the most important predictors of separation performance are the CO2 heat of adsorption (Qst, CO2) and the CO2 saturation loading capacity....

Adatom-Induced Local Melting

Francesca Baletto, Ngoc Linh Nguyen & Nicola Marzari
We introduce and discuss the phenomenon of adatom-induced surface local melting, using extensive first-principles molecular dynamics simulations of Al(100) taken as a paradigmatic case of a non-premelting surface that nevertheless displays facile adatom diffusion with single and multiple exchange pathways. Here, a single adatom deposited on the surface is sufficient to nucleate a localized and diffusing liquid-like region that remains confined to the surface layer, but with an area that increases with temperature; in the...

Hidden Beneath the Surface: Origin of the Observed Enantioselective Adsorption on PdGa(111)

Alexandre Tkatchenko, Aliaksandr V. Yakutovich, Carlo A. Pignedoli, Johannes Hoja & Daniele Passerone
We provide the input files to reproduce the data presented in the work:
Hidden Beneath the Surface: Origin of the Observed Enantioselective Adsorption on PdGa(111)
The files are subdivided in directories named after the figures/table of the manuscript
A. V. Yakutovich, J. Hoja, D. Passerone, Alexandre Tkatchenko, C. A. Pignedoli
J. Am. Chem. Soc., 140, 1401-1408 (2018) DOI: 10.1021/jacs.7b10980
In the work, we unravel the origin of the recently observed...

Accurate Characterization of the Pore Volume in Microporous Crystalline Materials (Data Download)

Senja Barthel, Berend Smit, Daniele Ongari, Matthew Witman, Peter G. Boyd & Maciej Haranczyk
Project Abstract: Pore volume is one of the main properties for the characterization of microporous crystals. It is experimentally measurable and it can also be obtained from the refined unit cell by a number of computational techniques. In this work we assess the accuracy and the discrepancies between the different computational methods which are commonly used for this purpose, i.e, geometric, helium and probe center pore volume, by studying a database of more than 5000...

In Silico Design of 2D and 3D Covalent Organic Frameworks for Methane Storage Applications

Rocio Mercado, Berend Smit, Aliaksandr V. Yakutovich, Maciej Haranczyk, Leopold Talirz & Rueih-Sheng Fu
Here we present 69,840 covalent organic frameworks (COFs) assembled in silico from a set of 666 distinct organic linkers into 2D-layered and 3D configurations. We investigate the feasibility of using these frameworks for methane storage by using grand-canonical Monte Carlo (GCMC) simulations to calculate their deliverable capacities (DCs). From these calculations, we predict that the best structure in the database is linker91_C_linker91_C_tbd, a structure composed of carbon-carbon bonded triazine linkers in the tbd topology. This...

Symmetry-Adapted Machine Learning for Tensorial Properties of Atomistic Systems

Michele Ceriotti, Andrea Grisafi, David M. Wilkins & Gabor Csányi
Here we present 1,000 structures each of a water monomer, water dimer, Zundel cation and bulk water used to train tensorial machine-learning models in Phys. Rev. Lett. 120, 036002 (2018). The archive entry contains files in extended-XYZ format including the structures and several tensorial properties: for the monomer, dimer and Zundel cation, the dipole moment, polarizability and first hyperpolarizability are included, and for bulk water the dipole moment, polarizability and dielectric tensor are given.

Predicting Product Distribution of Propene Dimerization in Nanoporous Materials (Data Download)

Berend Smit & Yifei Michelle Liu
Project abstract: In this work, a theoretical framework is developed to explain and predict changes in the product distribution of the propene dimerization reaction, which yields a mixture of C6 olefin isomers, resulting from the use of different porous materials as catalysts. The MOF-74 class of materials has shown promise in catalyzing the dimerization of propene with high selectivity for valuable linear olefin products. We show that experimentally observed changes in the product distribution can...

Gaussian Approximation Potentials for iron from extended first-principles database (Data Download)

Nicola Marzari, Daniele Dragoni, Tom Daff & Gabor Csanyi
Interatomic potentials are often necessary to describe complex realistic systems that would be too costly to study from first-principles. Commonly, interatomic potentials are designed using functional forms driven by physical intuition and fitted to experimental or computational data. The moderate flexibility of these functional forms limits their ability to be systematically improved by increasing the fitting datasets; on the other hand, their qualitative description of the essential physical interactions ensures a modicum degree of transferability....

Synthesis of Metal-Organic Frameworks: capturing chemical intuition

Seyed Mohamad Moosavi, Arunraj Chidambaram, Berend Smit, Leopold Talirz, Kyriakos C. Stylianou & Maciej Haranczyk
We report a methodology using machine learning to capture chemical intuition from a set of (partially) failed attempts to synthesize a metal organic framework. We define chemical intuition as the collection of unwritten guidelines used by synthetic chemists to find the right synthesis conditions. As (partially) failed experiments usually remain unreported, we have reconstructed a typical track of failed experiments in a successful search for finding the optimal synthesis conditions that yields HKUST-1 with the...

Capturing chemical intuition in synthesis of metal-organic frameworks

Arunraj Chidambaram, Leopold Talirz, Kyriakos C. Stylianou, Berend Smit, Maciej Haranczyk & Seyed Mohamad Moosavi
We report a methodology using machine learning to capture chemical intuition from a set of (partially) failed attempts to synthesize a metal organic framework. We define chemical intuition as the collection of unwritten guidelines used by synthetic chemists to find the right synthesis conditions. As (partially) failed experiments usually remain unreported, we have reconstructed a typical track of failed experiments in a successful search for finding the optimal synthesis conditions that yields HKUST-1 with the...

High-throughput computational screening of nanoporous adsorbents for CO 2 capture from natural gas

Li-Chiang Lin, Sondre Schnell, Efrem Braun, Wouter Thijssen, Berend Smit, Jihan Kim, Joshua A. Thompson & Alexander F. Zurhelle
With the growth of natural gas as an energy source, upgrading CO2-contaminated supplies has become increasingly important. Here we develop a single metric that captures how well an adsorbent performs the separation of CH4 and CO2, and we then use this metric to computationally screen tens of thousands of all-silica zeolites. We show that the most important predictors of separation performance are the CO2 heat of adsorption (Qst, CO2) and the CO2 saturation loading capacity....

Generating carbon schwarzites via zeolite-templating

Rocio Mercado, Davide M. Proserpio, Igor A. Baburin, Berend Smit, Yongjin Lee, Seyed Mohamad Moosavi, Senja Barthel & Efrem Braun
Zeolite-templated carbons (ZTCs) comprise a relatively recent material class synthesized via the chemical vapor deposition of a carbon-containing precursor on a zeolite template, followed by the removal of the template. We have developed a theoretical framework to generate a ZTC model from any given zeolite structure, which we show can successfully predict the structure of known ZTCs. We use our method to generate a library of ZTCs from all known zeolites, to establish criteria for...

Machine learning meets volcano plots: Computational discovery of cross-coupling catalysts

O. Anatole Von Lilienfeld, Stefan Niklaus Heinen, Benjamin Meyer, Boodsarin Sawatlon & Clémence Corminboeuf
The application of modern machine learning to challenges in atomistic simulation is gaining attraction. We present new machine learning models that can predict the energy of the oxidative addition process between a transition metal complex and a substrate for C-C cross-coupling reaction. In turn, this quantity can be used as a descriptor to estimate the activity of homogeneous catalysts using molecular volcano plots. The versatility of this approach is illustrated for vast libraries of organometallic...

In Silico Design of 2D and 3D Covalent Organic Frameworks for Methane Storage Applications

Rocio Mercado, Aliaksandr V. Yakutovich, Rueih-Sheng Fu, Leopold Talirz, Berend Smit & Maciej Haranczyk
Here we present 69,840 covalent organic frameworks (COFs) assembled in silico from a set of 666 distinct organic linkers into 2D-layered and 3D configurations. We investigate the feasibility of using these frameworks for methane storage by using grand-canonical Monte Carlo (GCMC) simulations to calculate their deliverable capacities (DCs). From these calculations, we predict that the best structure in the database is linker91_C_linker91_C_tbd, a structure composed of carbon-carbon bonded triazine linkers in the tbd topology. This...

Data-driven design and synthesis of metal-organic frameworks for wet flue gas CO2 capture

Kyriakos C. Stylianou, Peter George Boyd, Arunraj Chidambaram, Thomas D. Daff, Pascal Schouwink, Seyed Mohamad Moosavi, Berend Smit, Andrzej Gładysiak, Richard Bounds, Jeffrey A. Reimer, Jorge A. R. Navarro & Tom K. Woo
In this entry is a database of 324,426 hypothetical Metal-Organic Frameworks (MOFs) that were used in a study to screen potential carbon dioxide scrubbers. Using a method to assemble these materials with topological blueprints, we only selected materials that could be accurately represented with the MEPO-QEq charge generation method. By ensuring that the electrostatic potential is accurately represented in these materials, screening for CO2 adsorption properties would result very few false positives/negatives. The atom-centered charges...

Evaluating charge equilibration methods to generate electrostatic fields in nanoporous materials

Daniele Ongari, Peter G. Boyd, Seda Keskin, Ozge Kadioglu, Berend Smit & Amber K. Mace
Charge equilibration (Qeq) methods can estimate the electrostatic potential of molecules and periodic frameworks by assigning point charges to each atom, using only a small fraction of the resources needed to compute density functional (DFT)-derived charges. This makes possible, for example, the computational screening of thousands of microporous structures to assess their performance for the adsorption of polar molecules. Recently, different variants of the original Qeq scheme were proposed to improve the quality of the...

DORI reveals the influence of non-covalent interactions on covalent bonding patterns in molecular crystals under pressure

Clémence Corminboeuf, Benoit Guillot, Senja Barthel, Benjamin Meyer, Berend Smit, Amber Mace & Laurent Vannay
The study of organic molecular crystals under high pressure provides fundamental insight into crystal packing distortions and reveals mechanisms of phase transitions and the crystallization of polymorphs. These solid state transformations can be monitored directly by analyzing electron charge densities that are experimentally obtained at high pressure. However, restricting the analysis to the featureless electron density does not reveal the chemical bonding nature and the existence of intermolecular interactions. This shortcoming can be resolved by...

Unified theory of thermal transport in crystals and disordered solids

Michele Simoncelli, Nicola Marzari & Francesco Mauri
Crystals and glasses exhibit fundamentally different heat conduction mechanisms: the periodicity of crystals allows for the excitation of propagating vibrational waves that carry heat, as first discussed by Peierls; in glasses, the lack of periodicity breaks Peierls' picture and heat is mainly carried by the coupling of vibrational modes, often described by a harmonic theory introduced by Allen and Feldman. Anharmonicity or disorder are thus the limiting factors for thermal conductivity in crystals or glasses;...

Registration Year

  • 2017
    7
  • 2018
    23
  • 2019
    19

Resource Types

  • Dataset
    49