A5058042607- Advanced Chemical Physics Studies
- Catalysis and Oxidation Reactions
- Catalytic Processes in Materials Science
- Machine Learning in Materials Science
- Molecular Junctions and Nanostructures
- Photochemistry and Electron Transfer Studies
- Computational Drug Discovery Methods
- Crystal Structures and Properties
- Crystallization and Solubility Studies
- Inorganic Chemistry and Materials
- Topic Modeling
- Advanced Data Processing Techniques
- Analytical Chemistry and Sensors
- Scientific Computing and Data Management
- Spectroscopy and Quantum Chemical Studies
- Boron and Carbon Nanomaterials Research
- Chemistry and Chemical Engineering
- X-ray Diffraction in Crystallography
- Lanthanide and Transition Metal Complexes
- Axial and Atropisomeric Chirality Synthesis
- Synthesis and Biological Activity
- Electron and X-Ray Spectroscopy Techniques
- Quantum-Dot Cellular Automata
- Advanced Synthetic Organic Chemistry
- Organoboron and organosilicon chemistry
Argonne National Laboratory
2023-2025
University of California, Merced
2016-2022
University of California System
2019
This contribution presents a comprehensive extension of the QM9 dataset (originally at 133 K molecules) with calculation G4MP2 enthalpies for 9,841 molecules, featuring up to nine heavy atoms. We present QM9-LOHC, (de)hydrogenation 10,373 reactions, including minimum 5.5% weight hydrogen storage capacity in line Department Energy standards Liquid Organic Hydrogen Carriers (LOHC). By utilizing accurate quantum chemical method we expand database and explore new avenues exploration technologies...
ConspectusLanthanide (Ln) oxide clusters and molecular systems provide a bottom-up look at the electronic structures of bulk materials because close parallels in patterns Ln 4fN subshell occupancy between Ln2O3 size limits. At same time, these molecules offer challenge to theory community find appropriate robust treatments for across series. Anion photoelectron (PE) spectroscopy provides powerful experimental tool studying systems, mapping energies ground low-lying excited states neutral...
A compact orbital representation of ionization processes is described utilizing the difference calculated one-particle density matrices. Natural analysis involving this matrix simplifies interpretation electronic detachment and allows differentiation between one-electron transitions shake-up/shake-off transitions, in which are accompanied by excitation a second electron into virtual space.
The Socratic method, grounded in iterative questioning and critical dialogue, offers a compelling framework for leveraging large language models (LLMs) to advance scientific reasoning discovery chemistry materials science. In this paper, we explore how principles can be integrated into prompt engineering enhance model performance by fostering hypothesis refinement, conceptual clarity, problem-solving computational experimental chemistry. By aligning with chain-of-thought techniques,...
The Socratic method, grounded in iterative questioning and critical dialogue, offers a compelling framework for leveraging large language models (LLMs) to advance scientific reasoning discovery chemistry materials science. In this paper, we explore how principles can be integrated into prompt engineering enhance model performance by fostering hypothesis refinement, conceptual clarity, problem-solving computational experimental chemistry. By aligning with chain-of-thought techniques,...
Electrochemical transformations of metal ions in aqueous media are challenging to model accurately due the dynamic solvation structure surrounding at different charge states.
The electronic and molecular structure of the CeB6 unit has been probed by anion PE spectroscopy DFT calculations to gain insight into structural relaxation on edge corner sites this ionic material. While boron in bulk lanthanide hexaboride materials assumes octahedral B63– units, monomer a less compact delocalize charge. Two competitive structures were identified for neutral species, which include boat-like planar or near-planar teardrop structure. Ce adopts different orbital occupancies...
We present a comprehensive, in silico -based discovery approach to identifying novel liquid organic hydrogen carrier (LOHC) candidates using cheminformatics methods and quantum chemical calculations.
Photoelectron spectra of Gd2O2– obtained with photon energies ranging from 2.033 to 3.495 eV exhibit numerous close-lying neutral states photon-energy-dependent relative intensities. Transitions these states, which fall within the electron binding energy window 0.9 and 1.6 eV, are attributed one- or two-electron transitions ground low-lying excited states. An additional, similar manifold electronic is observed in an 2.1–2.8 cannot be assigned any simple one-electron transitions. This study...
Readily prepared cis-β-(α′,α′-dimethyl)-4′-methindolylstyrenes undergo acid-catalyzed intramolecular hydroindolation to afford tetrahydrobenzo[cd]indoles. Our experimental and computational investigations suggest that dispersive interactions between the indole styrene preorganize substrates such 6-membered ring formation is preferred, apparently via concerted protonation C–C bond formation. When dispersion attenuated (by a substituent or heteroatom), regioselectivity erodes competing...
Boronyl (B≡O) ligands have garnered much attention as isoelectronic and isolobal analogues of CO CN-, yet successful efforts in synthesizing metal boronyl complexes remain scarce. Anion photoelectron (PE) spectroscopy density functional theory calculations were employed to investigate two small CeO2B x- ( x = 2, 3) generated from laser ablation a mixed Ce/B pressed powder target. The spectra reveal markedly different bonding upon incorporation an additional B atom. Most interestingly,...
Evidence of strong photoelectron-valence electron (PEVE) interactions has been observed in the anion photoelectron (PE) spectra several lanthanide suboxide clusters, which are exceptionally complex from an electronic structure standpoint and strongly correlated systems. The PE spectrum Gd2O-, should have relatively simple because its half-filled 4f subshell, exhibits numerous transitions. affinity determined is 0.26 eV. intensities transitions to excited states increase relative lower-energy...
Predicting the synthesizability of a new molecule remains an unsolved challenge that chemists have long tackled with heuristic approaches. Here, we report method for predicting using simple, yet accurate thermochemical descriptor. We introduce E_min, energy difference between and its lowest constitutional isomer, as predictor is accurate, physically meaningful, first-principles based. apply E_min to 134,000 molecules in QM9 dataset find when used alone reduces incorrect predictions...
Predicting the synthesizability of a new molecule remains an unsolved challenge that chemists have long tackled with heuristic approaches. Here, we report method for predicting using simple yet accurate thermochemical descriptor. We introduce Emin, energy difference between and its lowest constitutional isomer, as predictor is accurate, physically meaningful, first-principles based. apply Emin to 134,000 molecules in QM9 data set find when used alone reduces incorrect predictions...
Here, we present the outcomes from second Large Language Model (LLM) Hackathon for Applications in Materials Science and Chemistry, which engaged participants across global hybrid locations, resulting 34 team submissions. The submissions spanned seven key application areas demonstrated diverse utility of LLMs applications (1) molecular material property prediction; (2) design; (3) automation novel interfaces; (4) scientific communication education; (5) research data management automation;...
The calculation of photoionization cross sections can play a key role in spectral assignments using modeling and simulation. In this work, we provide formal relationships between pole strengths, which are proportional to the section, terms related natural ionization orbital model for ΔSCF calculations. A set numerical calculations developed models is carried out. Pole strength values computed two approaches demonstrate excellent agreement with an electron propagator theory model.
Molecular electronic devices require precise control over the flow of current in single molecules. However, electron transport properties molecules critically depend on dynamic molecular conformations nanoscale junctions. Here, we report a unique strategy for controlling conductance using shape-persistent ladder Chemically diverse, charged molecules, synthesized via one-pot multicomponent ladderization strategy, show (dlog(G/G0)/dx ≈ -0.1 nm-1) that is nearly independent junction...
Lanthanide hydroxides are key species in a variety of catalytic processes and the preparation corresponding oxides. This work explores fundamental structure bonding simplest lanthanide hydroxide, LnOH (Ln = La-Lu), using density functional theory calculations. Interestingly, calculations predict that all structures this series will be linear. Furthermore, these results indicate valence electron configuration σ2π4 for compounds, suggesting lanthanide-hydroxide bond is best characterized as...
Readily prepared <i>cis</i>-<i>β</i>-(<i>α</i>’,<i>α</i>’-dimethyl)-4’-methindolylstyrenes undergo Brønsted acid-catalyzed intramolecular hydroarylation to afford a variety of 3-aryl-5,5-dimethyl-1,3,4,5-tetrahydrobenzo[<i>cd</i>]indoles. Our experimental and computational investigations suggest that dispersive interactions between the indole styrene preorganize substrates such 6-membered ring formation occurs via concerted step....
The calculation of photoionization cross-sections can play a key role in spectral assignments using modeling and simulation. In this work, we provide formal relationships between pole strengths, which are proportional to the cross-section, terms related Natural Ionization Orbital model for Delta-SCF calculations. A set numerical calculations developed models is carried out. Pole strength values computed two approaches demonstrate excellent agreement with an electron propagator theory model.
Lanthanide hydroxides are key species in a variety of catalytic processes and the preparation corresponding oxides. This work explores fundamental structure bonding simplest lanthanide hydroxide, LnOH (Ln=La-Lu), using density functional theory calculations. Interestingly, calculations predict that all structures this series will be linear. Furthermore, these results indicate valence electron configuration featuring an occupied sigma orbital two pi orbitals for compounds, suggesting...