Searching low-energy conformers of neutral and protonated di-, tri-, and tetra-glycine using first-principles accuracy assisted by the use of neural network potentials.

In the last ten years, combinations of state-of-the-art gas-phase spectroscopies and quantum chemistry calculations have suggested several intuitive trends in the structure of small polypeptides that may not hold true. For example, the preference for the cis form of the peptide bond and multiple protonated sites was proposed by comparing experimental spectra with low-energy minima obtained from limited structural sampling using various density functional theory methods. For understanding the structures of polypeptides, extensive sampling of their configurational space with high-accuracy computational methods is required. In this work, we demonstrated the use of deep-learning neural network potential (DL-NNP) to assist in exploring the structure and energy landscape of di-, tri-, and tetra-glycine with the accuracy of high-level quantum chemistry methods, and low-energy conformers of small polypeptides can be efficiently located. We hope that the structures of these polypeptides we found and our preliminary analysis will stimulate further experimental investigations.

The electronic structures and magnetic properties of mixed-valence Fe-based metal-organic VNU-15 frameworks: a theoretical study from linear response DFT+U calculations.

The crystal symmetries, electronic structures, and magnetic properties of metal-organic VNU-15 frameworks (VNU = Vietnam National University) were investigated using density functional calculations (DFT) with an on-site Coulomb repulsion approximation, U eff, of 4.30 eV, determined via the linear response method. Two different orientations of dimethylammonium (DMA+) cations in VNU-15 were investigated. Antiferromagnetic configurations were predicted to be the ground states, with Fe ions in high-spin states for both phases. Furthermore, VNU-15 had intrinsic semiconductor electronic behavior with a small band gap of about 1.20 eV. The change in the orientation of DMA+ led to changes in the dispersion of the band structure, the band gap, and the Fe contributions to the valence band and conduction band. A fascinating feature was found involving exchange of oxidation numbers between two adjacent Fe atoms in the two phases. Our results revealed that VNU-15 has strong oxidation activity and predicted the important role of an anisotropic effect on the hole and electron effective masses. The findings presented that the electronic and magnetic properties could be controlled via hydrogen bonds and proved VNU-15 to be a prospective material for photocatalytic applications.