ترغب بنشر مسار تعليمي؟ اضغط هنا

Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores

117   0   0.0 ( 0 )
 نشر من قبل Claudio Castelnovo
 تاريخ النشر 2015
  مجال البحث فيزياء
والبحث باللغة English




اسأل ChatGPT حول البحث

The idea of magnetic monopoles in spin ice has enjoyed much success at intermediate temperatures, but at low temperatures a description in terms of monopole dynamics alone is insufficient. Recently, numerical simulations were used to argue that magnetic impurities account for this discrepancy by introducing a magnetic equivalent of residual resistance in the system. Here we propose that oxygen deficiency is the leading cause of magnetic impurities in as-grown samples, and we determine the defect structure and magnetism in Y2Ti2O(7-delta) using diffuse neutron scattering and magnetization measurements. These defects are eliminated by oxygen annealing. The introduction of oxygen vacancies causes Ti4+ to transform to magnetic Ti3+ with quenched orbital magnetism, but the concentration is anomalously low. In the spin-ice material Dy2Ti2O7 we find that the same oxygen-vacancy defects suppress moments on neighbouring rare-earth sites, and that these magnetic distortions dramatically slow down the long-time monopole dynamics at sub-Kelvin temperatures.



قيم البحث

اقرأ أيضاً

Bodies in relative motion separated by a gap of a few nanometers can experience a tiny friction force. This non-contact dissipation can have various origins and can be successfully measured by a sensitive pendulum atomic force microscope tip oscillat ing laterally above the surface. Here, we report on the observation of dissipation peaks at selected voltage-dependent tip-surface distances for oxygen-deficient strontium titanate (SrTiO_3) surface at low temperatures (T = 5K). The observed dissipation peaks are attributed to tip-induced charge and spin state transitions in quantum-dot-like entities formed by single oxygen vacancies (and clusters thereof, possibly through a collective mechanism) at the SrTiO_3 surface, which in view of technological and fundamental research relevance of the material opens important avenues for further studies and applications.
Oxygen vacancies play a crucial role in the control of the electronic, magnetic, ionic, and transport properties of functional oxide perovskites. Rare earth nickelates (RENiO$_{3-x}$) have emerged over the years as a rich platform to study the interp lay between the lattice, the electronic structure, and ordered magnetism. In this study, we investigate the evolution of the electronic and magnetic structure in thin films of RENiO$_{3-x}$, using a combination of X-ray absorption spectroscopy and imaging, resonant X-ray scattering, and extended multiplet ligand field theory modeling. We find that oxygen vacancies modify the electronic configuration within the Ni-O orbital manifolds, leading to a dramatic evolution of long-range electronic transport pathways despite the absence of nanoscale phase separation. Remarkably, magnetism is robust to substantial levels of carrier doping, and only a moderate weakening of the $(1/4, 1/4, 1/4)_{pc}$ antiferromagnetic order parameter is observed, whereas the magnetic transition temperature is largely unchanged. Only at a certain point long-range magnetism is abruptly erased without an accompanying structural transition. We propose the progressive disruption of the 3D magnetic superexchange pathways upon introduction of point defects as the mechanism behind the sudden collapse of magnetic order in oxygen-deficient nickelates. Our work demonstrates that, unlike most other oxides, ordered magnetism in RENiO$_{3-x}$ is mostly insensitive to carrier doping. The sudden collapse of ordered magnetism upon oxygen removal may provide a new mechanism for solid-state magneto-ionic switching and new applications in antiferromagnetic spintronics.
SrTiO$_3$ (STO) is the substrate of choice to grow oxide thin-films and oxide heterojunctions, which can form quasi-two-dimensional electronic phases that exhibit a wealth of phenomena, and, thus, a workhorse in the emerging field of metal-oxide elec tronics. Hence, it is of great importance to know the exact character of the STO surface itself under various oxygen environments. Using density functional theory within the spin generalized gradient approximation we have investigated the structural, electronic and magnetic properties of the oxygen-deficient STO surface. We find that the surface oxygen vacancies order in periodic arrays giving rise to surface magnetic moments and a quasi two-dimensional electron gas in the occupied Ti 3-d orbitals. The surface confinement, the oxygen-vacancy ordering, and the octahedra distortions give rise to spin-polarized $t_{2g}$ dispersive sub-bands; their energy split near the Brillouin zone center acts as an effective Zeeman term, which, when we turn on a Rashba interaction, produces bands with momentum-spin correlations similar to those recently discovered on oxygen deficient STO surface.
While defects such as oxygen vacancies in correlated materials can modify their electronic properties dramatically, understanding the microscopic origin of electronic correlations in materials with defects has been elusive. Lanthanum nickelate with o xygen vacancies, LaNiO$_{3-x}$, exhibits the metal-to-insulator transition as the oxygen vacancy level $x$ increases from the stoichiometric LaNiO$_3$. In particular, LaNiO$_{2.5}$ exhibits a paramagnetic insulating phase, also stabilizing an antiferromagnetic state below $T_Nsimeq152$K. Here, we study the electronic structure and energetics of LaNiO$_{3-x}$ using first-principles. We find that LaNiO$_{2.5}$ stabilizes a vacancy-ordered structure with an insulating ground state and the nature of the insulating phase is a site-selective paramagnetic Mott state as obtained using density functional theory plus dynamical mean field theory (DFT+DMFT). The Ni octahedron site develops a Mott insulating state with strong correlations as the Ni $e_g$ orbital is half-filled while the Ni square-planar site with apical oxygen vacancies becomes a band insulator. Our oxygen vacancy results can not be explained by the pure change of the Ni oxidation state alone within the rigid band shift approximation. Our DFT+DMFT density of states explains that the peak splitting of unoccupied states in LaNiO$_{3-x}$ measured by the experimental X-ray absorption spectra originates from two nonequivalent Ni ions in the vacancy-ordered structure.
Defects in semiconductors can exhibit multiple charge states, which can be used for charge storage applications. Here we consider such charge storage in a series of oxygen deficient phases of TiO$_2$, known as Magneli phases. These Ti$_n$O$_{2n-1}$ M agneli phases present well-defined crystalline structures, i. e., their deviation from stoichiometry is accommodated by changes in space group as opposed to point defects. We show that these phases exhibit intermediate bands with the same electronic quadruple donor transitions akin to interstitial Ti defect levels in TiO$_2$-rutile. Thus, the Magneli phases behave as if they contained a very large pseudo-defect density: $frac{1}{2}$ per formula unit Ti$_n$O$_{2n-1}$. Depending on the Fermi Energy the whole material will become charged. These crystals are natural charge storage materials with a storage capacity that rivals the best known supercapacitors.
التعليقات
جاري جلب التعليقات جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
mircosoft-partner

هل ترغب بارسال اشعارات عن اخر التحديثات في شمرا-اكاديميا