We revisit the use of Meta-Generalized Gradient Approximations (mGGAs) in time-dependent density functional theory, reviewing conceptual questions and solving the generalized Kohn-Sham equations by real-time propagation. After discussing the technical aspects of using mGGAs in combination with pseudopotentials and comparing real-space and basis set results, we focus on investigating the importance of the current-density based gauge invariance correction. For the two modern mGGAs that we investigate in this work, TASK and r2SCAN, we observe that for some systems, the current density correction leads to negligible changes, but for others, it changes excitation energies by up to 40% and more than 0.8 eV. In the cases that we study, the agreement with the reference data is improved by the current density correction.

Download full-text PDF

Source
http://dx.doi.org/10.1063/5.0167972DOI Listing

Publication Analysis

Top Keywords

current density
12
density correction
12
meta-generalized gradient
8
gradient approximations
8
generalized kohn-sham
8
approximations time
4
time dependent
4
dependent generalized
4
kohn-sham theory
4
theory current
4

Similar Publications

Efficient harvesting of triplet excitons multiple fast TTA up-conversion and high-lying reverse intersystem crossing channels for efficient blue fluorescent organic light-emitting diodes.

Chem Sci

January 2025

Institute of Polymer Optoelectronic Materials and Devices, Guangdong Basic Research Center of Excellence for Energy & Information Polymer Materials, Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials, Guangdong Provincial Key Laboratory of Luminescence from Molecular Aggregates, State Key Laboratory of Luminescent Materials and Devices, South China University of Technology Guangzhou 510640 China

The efficient harvesting of triplet excitons is key to realizing high efficiency blue fluorescent organic light-emitting diodes (OLEDs). Triplet-triplet annihilation (TTA) up-conversion is one of the effective triplet-harvesting strategies. However, during the TTA up-conversion process, a high current density is necessary due to the competitive non-radiative triplet losses.

View Article and Find Full Text PDF

This perspective work examines the current advancements in integrated CO capture and electrochemical conversion technologies, comparing the emerging methods of (1) electrochemical reactive capture (eRCC) though amine- and (bi)carbonate-mediated processes and (2) direct (flue gas) adsorptive capture and conversion (ACC) with the conventional approach of sequential carbon capture and conversion (SCCC). We initially identified and discussed a range of cell-level technological bottlenecks inherent to eRCC and ACC including, but not limited to, mass transport limitations of reactive species, limitation of dimerization, impurity effects, inadequate generation of CO to sustain industrially relevant current densities, and catalyst instabilities with respect to some eRCC electrolytes, amongst others. We followed this with stepwise perspectives on whether these are considered intrinsic challenges of the technologies - otherwise recommendations were disclosed where appropriate.

View Article and Find Full Text PDF

Ligand-induced changes in the electrocatalytic activity of atomically precise Au nanoclusters.

Chem Sci

January 2025

School of Chemistry and Chemical Engineering, Chongqing Key Laboratory of Chemical Theory and Mechanism, Chongqing University Chongqing 401331 China

Atomically precise gold nanoclusters have shown great promise as model electrocatalysts in pivotal electrocatalytic processes such as the hydrogen evolution reaction (HER) and carbon dioxide reduction reaction (CORR). Although the influence of ligands on the electronic properties of these nanoclusters is well acknowledged, the ligand effects on their electrocatalytic performances have been rarely explored. Herein, using [Au(SR)] nanoclusters as a prototype model, we demonstrated the importance of ligand hydrophilicity hydrophobicity in modulating the interface dynamics and electrocatalytic performance.

View Article and Find Full Text PDF

In confluent cell monolayers, patterns of cell forces and motion are systematically altered near topological defects in cell shape. In turn, defects have been proposed to alter cell density, extrusion, and invasion, but it remains unclear how the defects form and how they affect cell forces and motion. Here, we studied +1/2 defects, and, in contrast to prior studies, we observed both tail-to-head and head-to-tail defect motion occurring at the same time in the same cell monolayer.

View Article and Find Full Text PDF

NbO(OH) has emerged as a highly attractive photocatalyst based on its chemical stability, energetic band positions, and large active lattice sites. Compared to other various photocatalytic semiconductors, it can be synthesized easily. This study presents a systematic analysis of pristine and doped NbO(OH) based on recent developments in related research.

View Article and Find Full Text PDF

Want 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!