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2.
Nat Commun ; 14(1): 8261, 2023 Dec 13.
Artigo em Inglês | MEDLINE | ID: mdl-38086835

RESUMO

Exciton polaritons are quasiparticles of photons coupled strongly to bound electron-hole pairs, manifesting as an anti-crossing light dispersion near an exciton resonance. Highly anisotropic semiconductors with opposite-signed permittivities along different crystal axes are predicted to host exotic modes inside the anti-crossing called hyperbolic exciton polaritons (HEPs), which confine light subdiffractionally with enhanced density of states. Here, we show observational evidence of steady-state HEPs in the van der Waals magnet chromium sulfide bromide (CrSBr) using a cryogenic near-infrared near-field microscope. At low temperatures, in the magnetically-ordered state, anisotropic exciton resonances sharpen, driving the permittivity negative along one crystal axis and enabling HEP propagation. We characterize HEP momentum and losses in CrSBr, also demonstrating coupling to excitonic sidebands and enhancement by magnetic order: which boosts exciton spectral weight via wavefunction delocalization. Our findings open new pathways to nanoscale manipulation of excitons and light, including routes to magnetic, nonlocal, and quantum polaritonics.

3.
Nat Commun ; 14(1): 5565, 2023 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-37689731

RESUMO

Many strongly correlated transition metal insulators are colored, even though they have band gaps much larger than the highest energy photons from the visible light. An adequate explanation for the color requires a theoretical approach able to compute subgap excitons in periodic crystals, reliably and without free parameters-a formidable challenge. The literature often fails to disentangle two important factors: what makes excitons form and what makes them optically bright. We pick two archetypal cases as examples: NiO with green color and MnF2 with pink color, and employ two kinds of ab initio many body Green's function theories; the first, a perturbative theory based on low-order extensions of the GW approximation, is able to explain the color in NiO, while the same theory is unable to explain why MnF2 is pink. We show its color originates from higher order spin-flip transitions that modify the optical response, which is contained in dynamical mean-field theory (DMFT). We show that symmetry lowering mechanisms may determine how 'bright' these excitons are, but they are not fundamental to their existence.

4.
ACS Nano ; 16(10): 16713-16723, 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36174128

RESUMO

Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. We pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

5.
Phys Rev Lett ; 124(23): 237001, 2020 Jun 12.
Artigo em Inglês | MEDLINE | ID: mdl-32603152

RESUMO

Recent observations of selective emergence (suppression) of superconductivity in the uncollapsed (collapsed) tetragonal phase of LaFe_{2}As_{2} has rekindled interest in understanding what features of the band structure control the superconducting T_{c}. We show that the proximity of the narrow Fe-d_{xy} state to the Fermi energy emerges as the primary factor. In the uncollapsed phase this state is at the Fermi energy, and is most strongly correlated and a source of enhanced scattering in both single and two particle channels. The resulting intense and broad low energy spin fluctuations suppress magnetic ordering and simultaneously provide glue for Cooper pair formation. In the collapsed tetragonal phase, the d_{xy} state is driven far below the Fermi energy, which suppresses the low-energy scattering and blocks superconductivity. A similar source of broad spin excitation appears in uncollapsed and collapsed phases of CaFe_{2}As_{2}. This suggests controlling coherence provides a way to engineer T_{c} in unconventional superconductors primarily mediated through spin fluctuations.

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