Article
Chemistry, Multidisciplinary
J. Patrick Zobel, Anna M. Wernbacher, Leticia Gonzalez
Summary: The mechanism of reverse intersystem crossing (rISC) in metal-based TADF emitters is still not clear, as the small singlet/triplet energy gaps necessary for thermal rISC in donor-acceptor systems with charge-transfer excited states have spin-orbit couplings that are too small for effective rISC. In this study, the first nonadiabatic dynamics simulation of rISC process in a carbene-copper(I)-carbazolyl TADF emitter is reported. Efficient rISC on a picosecond time scale is demonstrated, involving an intermediate higher-lying triplet state of metal-to-ligand charge transfer character ((MLCT)-M-3) that enables large spin-orbit couplings with the lowest singlet charge transfer state. The mechanism is completed in the S-1 state where the complex can return to a co-planar coordination geometry with high fluorescence efficiency.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Delin Kong, Feng Tian, Yingying Xu, Shaoqun Zhu, Zetong Yu, Lefeng Xiong, Peipei Li, Huiyun Wei, Xinhe Zheng, Mingzeng Peng
Summary: In addition to three-dimensional structures, polar semiconductor heterostructures are developing towards two-dimensional scale with mix-dimensional integration for novel properties and multifunctional applications. In this study, 2D Janus MoSSe and 3D wurtzite GaN polar semiconductors were stacked to form MoSSe/GaN polar heterostructures by polarity configurations. The polarity reversal of GaN in contact with Janus MoSSe and strain modulation were utilized to enhance the structural stability and tune the electronic energy band profiles of the heterostructures.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Tong Wu, Mingzi Sun, Bolong Huang
Summary: Current characterization techniques cannot unravel the detailed strain distributions on high-index facets, hindering the understanding of electroactivity origins. The lack of theoretical principles to quantify structural features on HIFs makes experimental efforts laborious, but exploring surface structural features and establishing a database of atomic strain distributions can promote efficient transition metal based electrocatalysts design and synthesis.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Multidisciplinary
Tony Stueker, Xiya Xia, Helmut Beckers, Sebastian Riedel
Summary: Pseudo-tetrahedral nitrido trifluorides equivalent to MF3 (M=Fe, Ru, Os) and square pyramidal nitrido tetrafluorides equivalent to MF4 (M=Ru, Os) were formed by reactions of free metal atoms with NF3 and isolated in solid neon at 5 K. Their IR spectra were analyzed with quantum-chemical calculations, revealing a high-spin (3)A(2) ground state for FeF3.
CHEMISTRY-A EUROPEAN JOURNAL
(2021)
Article
Chemistry, Physical
Soulef Jellali, Hela Habli
Summary: This paper focuses on the study of molecules such as francium dimer and a comparative spectroscopic investigation of cationic systems Fr-(Ca+, Sr+, Ba+). Computational methods are used to determine relevant parameters and the accuracy and reliability of the results are discussed. The findings provide insights for future laser cooling applications.
JOURNAL OF PHYSICAL CHEMISTRY A
(2022)
Article
Chemistry, Multidisciplinary
Di Yang, Chunyu Zhao, Ruqian Lian, Lin Yang, Yizhan Wang, Yu Gao, Xu Xiao, Yury Gogotsi, Xudong Wang, Gang Chen, Yingjin Wei
Summary: A method for achieving planar, dendrite-free Li metal growth on Ti3C2Tx MXene is reported, overcoming the barrier of irregular and nonplanar electrodeposition of Li. The prepared Li metal anode demonstrates stable cycling and high capacity retention, making it promising for application in Li metal batteries.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Masaki Fujikane, Shijo Nagao, Dariusz Chrobak, Toshiya Yokogawa, Roman Nowak
Summary: The research reveals that nanodeconfined GaN compressed along the M direction exhibits room-temperature plasticity, while the response along the C direction is quasi-brittle. First-principles bandgap calculations, nanomechanical tests, and ultrahigh-voltage transmission electron microscopy observations confirm the authenticity of the phenomenon. Molecular dynamics simulations demonstrate how this process occurs in C- and M-oriented GaN frustum, reflecting nanopillar crystals.
Article
Chemistry, Multidisciplinary
Lede Xian, Ammon Fischer, Martin Claassen, Jin Zhang, Angel Rubio, Dante M. Kennes
Summary: Twisting adjacent layers of van der Waals materials can create flat two-dimensional electronic bands, and this concept can be extended to three spatial dimensions. By applying this approach to various two-dimensional materials like graphitic systems, boron nitride, and WSe2, interesting three-dimensional phases such as quantum magnets and unconventional superconducting states can be induced and controlled.
Article
Chemistry, Physical
Juan J. J. Aucar, Alejandro F. F. Maldonado, Juan I. I. Melo
Summary: In this work, relativistic corrections to the electric field gradient (EFG) are presented, including spin-dependent corrections for the first time. The results show that these new corrections significantly improve the performance of the existing method and are in close agreement with calculations at the four-component Dirac-Hartree-Fock (4c-DHF) level. The accuracy of the EFG values obtained with this new method allows for the analysis of the electronic origin of relativistic effects using well-known nonrelativistic operators.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Jing Shang, Congxin Xia, Chun Tang, Chun Li, Yandong Ma, Yuantong Gu, Liangzhi Kou
Summary: The bending deformation of AgBiP2Se6 monolayers can manipulate the polarization direction and domain size, significantly improving the ferroelectric stability. This mechano-ferroelectric coupling represents a new mechanism for stabilization and polarization flip in 2D ferroelectrics, with potential applications in next-generation non-volatile storage devices.
NANOSCALE HORIZONS
(2021)
Article
Chemistry, Physical
Jacek Piechota, Stanislaw Krukowski, Petro Sadovyi, Bohdan Sadovyi, Sylwester Porowski, Izabella Grzegory
Summary: The study investigated the dissolution of molecular nitrogen in liquid gallium and iron through ab initio calculations and experiments, revealing fundamental differences in N bonding between the two solvents. It was found that the nitrogen solubility in iron is much higher than in gallium, indicating that liquid iron may be a prospective solvent for gallium nitride crystallization from metallic solutions.
Article
Chemistry, Applied
Thibault Pariat, Pauline M. Verite, Denis Jacquemin, Julien Massue, Gilles Ulrich
Summary: A dual-emissive fluorophore, HBBODipic, with an Excited-State Intramolecular Proton Transfer (ESIPT) process has been described. It has been used for generating panchromatic white-emission and ratiometric detection of substrates.
Article
Chemistry, Physical
Valentina Migliorati, Giuseppe Fazio, Simone Pollastri, Alessandra Gentili, Pierpaolo Tomai, Francesco Tavani, Paola D'Angelo
Summary: This study utilizes a synergic approach combining XANES, EXAFS spectroscopies, and QM calculations to investigate the solvation properties of HgCl2 and HgO in DESs. The experimental results show that Hg2+ forms a tetrahedral complex with four chloride ions in DESs, indicating strong interactions between Cl- anions and Hg2+.
JOURNAL OF MOLECULAR LIQUIDS
(2021)
Article
Chemistry, Multidisciplinary
Dayton J. Vogel, Jessica M. Rimsza, Tina M. Nenoff
Summary: Reactive gas formation in pores of metal-organic frameworks (MOFs) is known to cause framework destruction, understanding these mechanisms are key to future durability design. This study used AIMD simulations for the first time to predict competitive adsorption of mixed acid gases in RE-DOBDC MOFs and identified spontaneous formation of HONO as a result of deprotonation of the MOF organic linker. This study provides a novel mechanism for HONO formation in MOFs and offers a methodology for predicting future gas interactions in new nanoporous materials.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Physics, Applied
Shukai Yao, Babak Anasori, Alejandro Strachan
Summary: 2D rare-earth metal carbides (MXenes) with novel electronic and magnetic properties and potential as scalable 2D magnets were investigated. The effect of the U parameter on the stability and magnetism of different termination sites was studied. It was found that Mo2NdC2O2 and Mo2NdC2(OH)(2) exhibited magnetic properties regardless of termination and Hubbard U value.
JOURNAL OF APPLIED PHYSICS
(2022)
