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1.
Phys Rev Lett ; 119(18): 187401, 2017 Nov 03.
Artículo en Inglés | MEDLINE | ID: mdl-29219545

RESUMEN

ZrSiS exhibits a frequency-independent interband conductivity σ(ω)=const(ω)≡σ_{flat} in a broad range from 250 to 2500 cm^{-1} (30-300 meV). This makes ZrSiS similar to (quasi-)two-dimensional Dirac electron systems, such as graphite and graphene. We assign the flat optical conductivity to the transitions between quasi-two-dimensional Dirac bands near the Fermi level. In contrast to graphene, σ_{flat} is not universal but related to the length of the nodal line in the reciprocal space, k_{0}. Because of spin-orbit coupling, the discussed Dirac bands in ZrSiS possess a small gap Δ, for which we determine an upper bound max(Δ)=30 meV from our optical measurements. At low temperatures the momentum-relaxation rate collapses, and the characteristic length scale of momentum relaxation is of the order of microns below 50 K.

2.
Energy Environ Sci ; 16(4): 1520-1530, 2023 Apr 12.
Artículo en Inglés | MEDLINE | ID: mdl-37063253

RESUMEN

Solar batteries capable of harvesting sunlight and storing solar energy present an attractive vista to transition our energy infrastructure into a sustainable future. Here we present an integrated, fully earth-abundant solar battery based on a bifunctional (light absorbing and charge storing) carbon nitride (K-PHI) photoanode, combined with organic hole transfer and storage materials. An internal ladder-type hole transfer cascade via a transport layer is used to selectively shuttle the photogenerated holes to the PEDOT:PSS cathode. This concept differs from previous designs such as light-assisted battery schemes or photocapacitors and allows charging with light during both electrical charge and discharge, thus substantially increasing the energy output of the cell. Compared to battery operation in the dark, light-assisted (dis)charging increases charge output by 243%, thereby increasing the electric coulombic efficiency from 68.3% in the dark to 231%, leading to energy improvements of 94.1% under illumination. This concept opens new vistas towards compact, highly integrated devices based on multifunctional, carbon-based electrodes and separators, and paves the way to a new generation of earth-abundant solar batteries.

3.
Nat Commun ; 12(1): 4512, 2021 Jul 23.
Artículo en Inglés | MEDLINE | ID: mdl-34301938

RESUMEN

α-RuCl3 is a major candidate for the realization of the Kitaev quantum spin liquid, but its zigzag antiferromagnetic order at low temperatures indicates deviations from the Kitaev model. We have quantified the spin Hamiltonian of α-RuCl3 by a resonant inelastic x-ray scattering study at the Ru L3 absorption edge. In the paramagnetic state, the quasi-elastic intensity of magnetic excitations has a broad maximum around the zone center without any local maxima at the zigzag magnetic Bragg wavevectors. This finding implies that the zigzag order is fragile and readily destabilized by competing ferromagnetic correlations. The classical ground state of the experimentally determined Hamiltonian is actually ferromagnetic. The zigzag state is stabilized by quantum fluctuations, leaving ferromagnetism - along with the Kitaev spin liquid - as energetically proximate metastable states. The three closely competing states and their collective excitations hold the key to the theoretical understanding of the unusual properties of α-RuCl3 in magnetic fields.

4.
Nanoscale Horiz ; 3(4): 383-390, 2018 Jul 01.
Artículo en Inglés | MEDLINE | ID: mdl-32254125

RESUMEN

The porous nature and structural diversity of metal-organic frameworks (MOFs) provide a versatile platform for specific and selective sorption behavior. When integrated as functional layers into photonic crystals (PCs), loading of the porous network with organic solvent vapors translates into an optical response, allowing analyte discrimination according to the specific host-guest interactions and, hence, framework affinity to the analytes. However, the optical response of PCs is critically influenced by the overall PC architecture, leading to batch-to-batch variations, thus rendering unequivocal analyte assignment challenging. To circumvent these problems, we have developed a straightforward and mild "post-assembly" modification strategy to impart differences in chemical selectivity to the MOF layers whilst keeping the overall PC backbone constant. To this end, one-dimensional photonic crystal (1D PC) sensors based on CAU-1 and TiO2 layers were fabricated to obtain a generic platform for post-assembly modification, targeting either the secondary building unit (SBU) or the linker unit of the as-assembled MOF nanoparticle layers. The optical response to solvent vapor exposure was investigated with the pristine CAU-1 based sensor as well as its modifications, showing enhanced analyte selectivity for the post-modified systems.

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