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1.
Nano Lett ; 22(4): 1812-1817, 2022 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-34890208

RESUMO

Control of a single ionic charge state by altering the number of bound electrons has been considered as an ultimate testbed for atomic charge-induced interactions and manipulations, and such subject has been studied in artificially deposited objects on thin insulating layers. We demonstrate that an entire layer of controllable atomic charges on a periodic lattice can be obtained by cleaving metallic Co1/3NbS2, an intercalated transition metal dichalcogenide. We identified a metastable charge state of Co with a different valence and manipulated atomic charges to form a linear chain of the metastable charge state. Density functional theory investigation reveals that the charge state is stable due to a modified crystal field at the surface despite the coupling between NbS2 and Co via a1g orbitals. The idea can be generalized to other combinations of intercalants and base matrices, suggesting that they can be a new platform to explore single-atom-operational 2D electronics/spintronics.

2.
Angew Chem Int Ed Engl ; 60(30): 16500-16505, 2021 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-33904630

RESUMO

The Jahn-Teller (JT) theorem constitutes one of the most fundamental concepts in chemistry. In transition-element chemistry, the 3d4 and 3d9 configurations in octahedral complexes are particularly illustrative, where a distortion in local geometry is associated with a reduction of the electronic energy. However, there has been a lasting debate about the fact that the octahedra are found to exclusively elongate. In contrast, for Na9 Bi5 Os3 O24 , the octahedron around Os6+ (5d2 ) is heavily compressed, lifting the degeneracy of the t2g set of 5d orbitals such that in the sense of a JT compression a diamagnetic ground state results. This effect is not forced by structural constraints, the structure offers sufficient space for osmium to shift the apical oxygen atoms to a standard distance. The relevance of these findings is far reaching, since they provide new insights in the hierarchy of perturbations defining ground states of open shell electronic systems.

3.
Proc Natl Acad Sci U S A ; 115(40): 9945-9950, 2018 10 02.
Artigo em Inglês | MEDLINE | ID: mdl-30232258

RESUMO

Gold is a very inert element, which forms relatively few compounds. Among them is a unique material-mineral calaverite, [Formula: see text] Besides being the only compound in nature from which one can extract gold on an industrial scale, it is a rare example of a natural mineral with incommensurate crystal structure. Moreover, it is one of few systems based on Au, which become superconducting (at elevated pressure or doped by Pd and Pt). Using ab initio calculations we theoretically explain these unusual phenomena in the picture of negative charge-transfer energy and self-doping, with holes being largely in the Te [Formula: see text] bands. This scenario naturally explains incommensurate crystal structure of [Formula: see text], and it also suggests a possible mechanism of superconductivity. An ab initio evolutionary search for stable compounds in the Au-Te system confirms stability of [Formula: see text] and [Formula: see text] and leads to a prediction of an as yet unknown stable compound AuTe, which until now has not been synthesized.

4.
Chemphyschem ; 18(18): 2482-2486, 2017 Sep 20.
Artigo em Inglês | MEDLINE | ID: mdl-28726353

RESUMO

The copper salt of trifluoroacetic acid, Cu(CF3 COO)2 , offers a new platform to investigate the quantum ground states of low-dimensional magnets. In practice, it realizes the ideal case of a solid hosting essentially isolated magnetic monolayers. These entities are constituted by well-separated two-leg half-integer spin ladders organized in a zigzag fashion. The ladders are comprised of dimeric units of edge-sharing tetragonal pyramids coupled through carbon ions. The spin-gap state in this compound was revealed by static and dynamic magnetic measurements. No indications of long range magnetic ordering down to liquid helium temperature were obtained in specific heat measurements. First principles calculations allow estimation of the main exchange interaction parameters, J⊥ =176 K and J∥ =12 K, consistent with the weakly interacting dimers model.

5.
Curr Hypertens Rev ; 12(3): 203-214, 2016.
Artigo em Inglês | MEDLINE | ID: mdl-28034357

RESUMO

The article represents literature review and provides evidence for psychological stress to play essential role in the development of arterial hypertension. The pathogenesis of hypertension is complex with a significant diversity and variability of the mechanisms involved in individual patient. In this regard, the determination of specific pathogenic pathways underlying sustained blood pressure elevation in each patient would substantially individualize therapeutic approaches, and hence increase the effectiveness of treatment. Psychological stress is proposed as a significant factor contributing to the development of hypertension. Global urbanization, sedentary lifestyle, daily stress at workplace, lack of physical activity and social support lead to increased anxiety, uncertainty, and finally to chronic mental and emotional stress. This review provides information about alterations in neuroendocrine and immune systems as the main pathogenic pathways linking psychological stress and hypertension. Endothelial dysfunction is considered not only as a consequence but also a primary factor causing prohypertensive state. Moreover, physical inactivity is discussed as one of the plausible mechanisms playing a key role in the development of hypertension in modern lifestyle conditions. Particularly the loss of connection between psychosocial strain and physical activity may underlie the deleterious effect of stress on cardiovascular and metabolic health.


Assuntos
Hipertensão Essencial/etiologia , Estresse Psicológico/complicações , Ansiedade/psicologia , Hipertensão Essencial/psicologia , Humanos , Pré-Hipertensão/etiologia , Comportamento Sedentário , Apoio Social , Urbanização , Local de Trabalho/psicologia
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