LiHe is an extreme open-shell system. It is among the weakest bound systems known, and its mean interatomic distance extends dramatically into the classical forbidden region. Upon 1s → 2p excitation of He, interatomic Coulombic decay (ICD) takes place in which the electronically excited helium atom relaxes and transfers its excess energy to ionize the neighboring lithium atom. A substantial part of the decay is found to be to the dissociation continuum producing Li and He atoms. The distribution of the kinetic energy released by the ICD products is found to be highly oscillatory. Its analysis reveals that quantum phase shifts between the decaying states and the dissociating final states are controlling this ICD reaction. The semiclassical reflection principle, which commonly explains ICD reactions, fails. The process is expected to be amenable to experiment.
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http://dx.doi.org/10.1021/acs.jpclett.0c01974 | DOI Listing |
J Chem Phys
December 2024
Computational Science Research Center, Korea Institute of Science and Technology (KIST), Seoul 02792, Republic of Korea.
Graph neural network interatomic potentials (GNN-IPs) are gaining significant attention due to their capability of learning from large datasets. Specifically, universal interatomic potentials based on GNN, usually trained with crystalline geometries, often exhibit remarkable extrapolative behavior toward untrained domains, such as surfaces and amorphous configurations. However, the origin of this extrapolation capability is not well understood.
View Article and Find Full Text PDFRep Prog Phys
November 2024
Department of Physics and Astronomy, Aarhus University, 8000 Aarhus, C, Denmark.
J Chem Phys
November 2024
Sorbonne Université, CNRS, Laboratoire de Chimie Physique Matière et Rayonnement, UMR 7614, F-75005 Paris, France.
Via the interatomic Coulombic electron capture (ICEC) process, an electron can be captured by an atom or a molecule, while the binding and excess energy is transferred, via a long-range Coulomb interaction, to a neighboring atom or molecule. The transferred energy can be used to ionize or electronically excite the neighboring species. When the two species are asymptotically far apart, an analytical formula for the ICEC cross sections can be derived.
View Article and Find Full Text PDFNature
October 2024
State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Sciences, Beijing, China.
Softening of the transverse optical (TO) phonon, which could trigger ferroelectric phase transition, can usually be achieved by enhancing the long-range Coulomb interaction over the short-range bonding force, for example, by increasing the Born effective charges. However, it suffers from depolarization effects as the induced ferroelectricity is suppressed on size reduction of the host materials towards high-density nanoscale electronics. Here, we present an alternative route to drive the TO phonon softening by showing that the abnormal soft TO phonon in rocksalt-structured ultrawide-bandgap BeO (ref.
View Article and Find Full Text PDFJ Am Chem Soc
November 2024
Department of Molecular Engineering, Graduate School of Engineering, Kyoto University, Kyoto-shi, Kyoto 615-8510, Japan.
Molecules that contain bonds whose length significantly deviates from the average are of interest in the context of understanding the nature and limits of the chemical bonds. However, it is difficult to disentangle the individual contributions of the multiple factors that give rise to such bond-length deviations as reports on such molecules remain scarce. In the present study, we have succeeded in synthesizing hexafluorodihalocubanes of the type CFX () (X = Cl (), Br (), I ()), which represent a new series of molecules with unusual C(sp)-halogen bonds.
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