This paper assesses the accuracy of the ΔSCF method for computing low-lying HOMO→LUMO transitions in organic dye molecules. For a test set of vertical excitation energies of 16 chromophores, surprisingly similar accuracy is observed for time-dependent density functional theory and for ΔSCF density functional theory. In light of this performance, we reconsider the ad hoc ΔSCF prescription and demonstrate that it formally obtains the exact stationary density within the adiabatic approximation, partially justifying its use. The relative merits and future prospects of ΔSCF for simulating individual excited states are discussed.
Download full-text PDF |
Source |
|---|---|
| http://dx.doi.org/10.1063/1.3530801 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Deletion of metal transporter Zip14 reduces major histocompatibility complex II expression in murine small intestinal epithelial cells.
Proc Natl Acad Sci U S A
January 2025
Center for Nutritional Sciences, Food Science and Human Nutrition Department, College of Agricultural and Life Sciences, University of Florida, Gainesville, FL 32611.
Documented worldwide, impaired immunity is a cardinal signature resulting from loss of dietary zinc, an essential micronutrient. A steady supply of zinc to meet cellular requirements is regulated by an array of zinc transporters. Deletion of the transporter Zip14 (Slc39a14) in mice produced intestinal inflammation.
View Article and Find Full Text PDFA hybrid meta on-top functional for multiconfiguration pair-density functional theory.
Proc Natl Acad Sci U S A
January 2025
Department of Chemistry, Chemical Theory Center, University of Minnesota, Minneapolis, MN 55455-0431.
Multiconfiguration pair-density functional theory (MC-PDFT) was proposed a decade ago, but it is still in the early stage of density functional development. MC-PDFT uses functionals that are called on-top functionals; they depend on the density and the on-top pair density. Most MC-PDFT calculations to date have been unoptimized translations of generalized gradient approximations (GGAs) of Kohn-Sham density functional theory (KS-DFT).
View Article and Find Full Text PDFClimate change could amplify weak synchrony in large marine ecosystems.
Proc Natl Acad Sci U S A
January 2025
Department of Ecology and Evolutionary Biology, University of Kansas, Lawrence, KS 66045.
Climate change is increasing the frequency of large-scale, extreme environmental events and flattening environmental gradients. Whether such changes will cause spatially synchronous, large-scale population declines depends on mechanisms that limit metapopulation synchrony, thereby promoting rescue effects and stability. Using long-term data and empirical dynamic models, we quantified spatial heterogeneity in density dependence, spatial heterogeneity in environmental responses, and environmental gradients to assess their role in inhibiting synchrony across 36 marine fish and invertebrate species.
View Article and Find Full Text PDFAdvancing the Mechanosensitivity of Atropisomeric Diarylethene Mechanophores through a Lever-Arm Effect.
J Am Chem Soc
January 2025
Department of Chemistry, BioInspired Institute, Syracuse University, Syracuse, New York 13244, United States.
Understanding structure-mechanical activity relationships (SMARs) in polymer mechanochemistry is essential for the rational design of mechanophores with desired properties, yet SMARs in noncovalent mechanical transformations remain relatively underexplored. In this study, we designed a subset of diarylethene mechanophores based on a lever-arm hypothesis and systematically investigated their mechanical activity toward a noncovalent-yet-chemical conversion of atropisomer stereochemistry. Results from Density functional theory (DFT) calculations, single-molecule force spectroscopy (SMFS) measurements, and ultrasonication experiments collectively support the lever-arm hypothesis and confirm the exceptional sensitivity of chemo-mechanical coupling in these atropisomers.
View Article and Find Full Text PDFDual-Anion-Rich Polymer Electrolytes for High-Voltage Solid-State Lithium Metal Batteries.
ACS Nano
January 2025
Department of Physics, JC STEM Lab of Energy and Materials Physics, City University of Hong Kong, Hong Kong 999077, P. R. China.
Solid polymer electrolytes (SPEs) are promising candidates for lithium metal batteries (LMBs) owing to their safety features and compatibility with lithium metal anodes. However, the inferior ionic conductivity and electrochemical stability of SPEs hinder their application in high-voltage solid-state LMBs (HVSSLMBs). Here, a strategy is proposed to develop a dual-anion-rich solvation structure by implementing ferroelectric barium titanate (BTO) nanoparticles (NPs) and dual lithium salts into poly(vinylidene fluoride) (PVDF)-based SPEs for HVSSLMBs.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!