A5066200150- Machine Learning in Materials Science
- Advanced Chemical Physics Studies
- X-ray Diffraction in Crystallography
- Crystallization and Solubility Studies
- Geological and Geochemical Analysis
- earthquake and tectonic studies
- Spectroscopy and Quantum Chemical Studies
- High-pressure geophysics and materials
- Catalysis and Oxidation Reactions
- Zeolite Catalysis and Synthesis
- Advanced NMR Techniques and Applications
- Computational Drug Discovery Methods
- Granular flow and fluidized beds
- Catalytic Processes in Materials Science
- Metal-Organic Frameworks: Synthesis and Applications
- Advanced Research in Systems and Signal Processing
- Solidification and crystal growth phenomena
- Theoretical and Computational Physics
- Catalytic C–H Functionalization Methods
- History and advancements in chemistry
- Radical Photochemical Reactions
- Chemistry and Chemical Engineering
- Nuclear Materials and Properties
- Complex Systems and Dynamics
- Target Tracking and Data Fusion in Sensor Networks
University of Chicago
2021-2025
University of California, Berkeley
2024-2025
NSWC Corona Division
2024
Naval Surface Warfare Center
2024
University of Kansas
2021
University of California, Los Angeles
2021
University of Minnesota
2009-2020
Texas A&M University
2019
Pennsylvania State University
2011-2012
University of Vermont
2007
The developments of the open-source OpenMolcas chemistry software environment since spring 2020 are described, with a focus on novel functionalities accessible in stable branch package or via interfaces other packages. These span wide range topics computational and presented thematic sections: electronic structure theory, spectroscopy simulations, analytic gradients molecular optimizations, ab initio dynamics, new features. This report offers an overview chemical phenomena processes can...
Predicting and understanding the chemical bond is one of major challenges computational quantum chemistry. Kohn-Sham density functional theory (KS-DFT) most common method, but approximate functionals may not be able to describe systems where multiple electronic configurations are equally important. Multiconfigurational wave functions, on other hand, can provide a detailed structures bonds such systems. In complete active space self-consistent field (CASSCF) performs full configuration...
The past decade has seen a great increase in the application of high-throughput computation to variety important problems chemistry. However, one area which been resistant approach is multireference wave function methods, large part due technicalities setting up these calculations and particular not always intuitive challenge active space selection. As we look toward future applying all areas chemistry, it prepare methods for large-scale automation. Here, propose ranked-orbital select spaces...
In organic reactivity studies, quantum chemical calculations play a pivotal role as the foundation of understanding and machine learning model development. While prevalent black-box methods like density functional theory (DFT) coupled-cluster (e.g., CCSD(T)) have significantly advanced our reactivity, they frequently fall short in describing multiconfigurational transition states intermediates. Achieving more accurate description necessitates use multireference methods. However, these not...
The localized active space self-consistent field method factorizes a complete wave function into an antisymmetrized product of fragments. Correlation between fragments is then reintroduced through state interaction (LASSI), in which the Hamiltonian diagonalized model LAS states. However, optimal procedure for defining and LASSI unknown. We here present automated framework to explore systematically convergent sets spaces, we call LASSI[r, q]. This requires user select only r, number electron...
Torsion experiments on partially molten aggregates of olivine þ chromite 4 vol. % mid-ocean ridge basalt provide new insights into the interactions between deformation and melt segregation. When samples are sheared, segregates distinct melt-rich bands oriented � 208 antithetic to macroscopic shear plane. In one series experiments, were deformed at similar strain rates (or stresses) a range finite strains explore evolution bands. another effect rate stress) band spacing microstructure. We...
Faulting and brittle deformation of mantle rocks occurs in many tectonic settings such as oceanic transform faults, detachment subduction zones, continental rifts. However, few data exist that directly explore the frictional properties peridotite rocks. Improved constraints on is important for a more complete understanding rheological lithosphere. Furthermore, our comparatively detailed plastic olivine allows us to possible role thermally activated intracrystalline mechanisms macroscopically...
Photonic materials with positionally ordered structure can interact strongly light to produce brilliant structural colors. Here, we found that the nonperiodic nematic liquid crystals of nanoplates also display color only significant orientational order. Owing loose stacking nanodiscs, such colloidal dispersion is able reflect a broad-spectrum wavelength, which reflection be further enhanced by adding carbon nanoparticles reduce background scattering. Upon addition electrolytes, vivid colors...
We have calculated state-averaged complete-active-space self-consistent-field (SA-CASSCF), multiconfiguration pair-density functional theory (MC-PDFT), hybrid MC-PDFT (HMC-PDFT), and
We have screened an array of 23 metals deposited onto the metal–organic framework (MOF) NU-1000 for propyne dimerization to hexadienes. By a first-of-its-kind study utilizing data-driven algorithms and high-throughput experimentation (HTE) in MOF catalysis, yields on Cu-deposited were improved from 0.4 24.4%. Characterization best-performing catalysts reveal conversion hexadiene be due formation large Cu nanoparticles, which is further supported by reaction mechanisms calculated with density...
Exhumed sections of the middle and lower crust in western New Zealand reveal how deformation was partitioned within a thermally rheologically evolving crustal column during Cretaceous continental extension. Structural data, P ‐ T determinations, U‐Pb geochronology from central Fiordland Paparoa Range Westland show that extension initiated by ∼114 Ma as period arc‐related magmatism waned. Initially, localized into areas were weakened heat magma. However, these hot, weak zones ephemeral....
We introduce multiconfiguration data-driven functional methods (MC-DDFMs), a group of which aim to correct the total or classical energy qualitatively accurate multiconfigurational wave function using machine-learned some featurization such as its density, on-top both. On data set carbene singlet–triplet splittings, we show that MC-DDFMs are able achieve near-benchmark performance on systems not used for training with robust degree active-space independence. Beyond demonstrating density and...
Excited states of transition metal complexes are generally strongly correlated due to the near-degeneracy d orbitals. Consequently, electronic structure calculations such species often necessitate multireference approaches. However, widespread use methods is hindered active space selection problem, which has historically required system-specific chemical knowledge and a trial-and-error approach. Here, we address this issue with an automated method combining approximate pair coefficient (APC)...
Qualitative and quantitative orbital properties such as bonding/antibonding character, localization, energies are critical to how chemists understand reactivity, catalysis, excited-state behavior. Despite this, representations of orbitals in deep learning models have been very underdeveloped relative molecular geometries Hamiltonians. Here, we apply state-of-the-art equivariant architectures the task assigning global labels orbitals, namely characterizations, given coefficients from...
The number of materials that ``bridge the gap'' between single molecules and extended solids, such as metal-organic frameworks organic semiconductors, has been increasing. Consequently, there is a growing need for modeling approaches effectively integrate real-space molecular perspective employed by computational chemists reciprocal-space dispersive physicists. Here, we propose localized active space (LAS) approach promising method to successfully bridge this gap. LAS extends concept from...
In this article the recent developments of open-source OpenMolcas chemistry software environment, since spring 2020, are described, with main focus on novel functionalities that accessible in stable branch package and/or via interfaces other packages. These community span a wide range topics computational chemistry, and presented thematic sections associated electronic structure theory, spectroscopy simulations, analytic gradients molecular optimizations, ab initio dynamics, new features....
The selection of an adequate set active orbitals for modeling strongly correlated electronic states is difficult to automate because it highly dependent on the and molecule interest. Although many approaches have shown some success, no single approach has worked well in all cases. In light this, we present "discrete variational selection" (DVS) space selection, which one generates multiple trial wave functions from a diverse systematically constructed spaces then selects between these...
[1] We present results from experiments designed to investigate the interactions between stress-driven melt segregation and reaction-enhanced infiltration, two mechanisms that have previously been studied independently of each other. A source (with a fraction below rheologically critical fraction) in which basaltic is either orthopyroxene-saturated or orthopyroxene-undersaturated was coupled with nominally melt-free olivine + orthopyroxene sink cylindrical configurations deformed torsion. As...
Chiral monoprotected aminoethyl amine (MPAAM) ligands were recently reported to facilitate enantioselective Pd-catalyzed arylation of strong cyclopropane C(sp3)–H bonds. Herein, we describe detailed experimental and theoretical investigations into the influence MPAAM ligands, L1 L2, as well a thioether (MPAThio) ligand, L3, on reaction kinetics, product enantioselectivity, turnover number. We show an unusual negative nonlinear effect in ligand enantiopurity rate ee that has not been shown...
To investigate the coupling between stress-driven melt segregation and reaction-driven infiltration, we performed static annealing torsional deformation experiments on couples constructed from a melt-rich basaltic source melt-poor olivine + orthopyroxene chromite basalt sink. In this study (the second of two companion papers), is almost completely molten with ϕ = 0.8–0.9, well above rheologically critical fraction. We deformed geometries source/sink either as core or outer ring cylinder. Our...
The number of materials that "bridge the gap" between single molecules and extended solids, such as metal-organic frameworks organic semiconductors, has been increasing. Consequently, there is a growing need for modeling approaches effectively integrate real-space molecular perspective employed by computational chemists reciprocal-space dispersive physicists. Here, we propose localized active space (LAS) approach promising method to successfully bridge this gap. LAS extends concept from...