Orbital reconstruction in nonpolar tetravalent transition-metal oxide layers

A promising route to tailoring the electronic properties of quantum materials and devices rests on the idea of orbital engineering in multilayered oxide heterostructures. Here we show that the interplay of interlayer charge imbalance and ligand distortions provides a knob for tuning the sequence of electronic levels even in intrinsically stacked oxides. We resolve in this regard the $d$-level structure of layered Sr$_2$IrO$_4$ by electron spin resonance. While canonical ligand-field theory predicts $g_{\parallel}$-factors $\!<\!2$ for positive tetragonal distortions as present in Sr$_2$IrO$_4$, the experiment indicates $g_{\parallel}\!>\!2$. This implies that the iridium $d$ levels are inverted with respect to their normal ordering. State-of-the-art electronic-structure calculations confirm the level switching in Sr$_2$IrO$_4$, whereas we find them in Ba$_2$IrO$_4$ to be instead normally ordered. Given the nonpolar character of the metal-oxygen layers, our findings highlight the tetravalent transition-metal 214 oxides as ideal platforms to explore $d$-orbital reconstruction in the context of oxide electronics

Rolled-up self-assembly of compact magnetic inductors, transformers and resonators

Three-dimensional self-assembly of lithographically patterned ultrathin films opens a path to manufacture microelectronic architectures with functionalities and integration schemes not accessible by conventional two-dimensional technologies. Among other microelectronic components, inductances, transformers, antennas and resonators often rely on three-dimensional configurations and interactions with electromagnetic fields requiring exponential fabrication efforts when downscaled to the micrometer range. Here, the controlled self-assembly of functional structures is demonstrated. By rolling-up ultrathin films into cylindrically shaped microelectronic devices we realized electromagnetic resonators, inductive and mutually coupled coils. Electrical performance of these devices is improved purely by transformation of a planar into a cylindrical geometry. This is accompanied by an overall downscaling of the device footprint area by more than 50 times. Application of compact self-assembled microstructures has significant impact on electronics, reducing size, fabrication efforts, and offering a wealth of new features in devices by 3D shaping.Comment: 19 pages, 3 figures, 6 supplementary figure

Rolled‐Up Self‐Assembly of Compact Magnetic Inductors, Transformers, and Resonators

3D self-assembly of lithographically patterned ultrathin films opens a path to manufacture microelectronic architectures with functionalities and integration schemes not accessible by conventional 2D technologies. Among other microelectronic components, inductances, transformers, antennas, and resonators often rely on 3D configurations and interactions with electromagnetic fields requiring exponential fabrication efforts when downscaled to the micrometer range. Here, the controlled self-assembly of functional structures is demonstrated. By rolling up ultrathin films into cylindrically shaped microelectronic devices, electromagnetic resonators, inductive and mutually coupled coils are realized. Electrical performance of these devices is improved purely by transformation of a planar into a cylindrical geometry. This is accompanied by an overall downscaling of the device footprint area by more than 50 times. Application of compact self-assembled microstructures has significant impact on electronics, reducing size, fabrication efforts, and offering a wealth of new features in devices by 3D shaping

Phononic-magnetic dichotomy of the thermal Hall effect in the Kitaev material Na2 Co2 TeO6

The quest for a half-quantized thermal Hall effect of a Kitaev system represents an important tool to probe topological edge currents of emergent Majorana fermions. Pertinent experimental findings for α-RuCl3 are, however, strongly debated, and it has been argued that the thermal Hall signal stems from phonons or magnons rather than from Majorana fermions. Here, we investigate the thermal Hall effect of the Kitaev candidate material Na2Co2TeO6, and we show that the measured signal emerges from at least two components, phonons and magnetic excitations. This dichotomy results from our discovery that the longitudinal and transversal heat conductivities share clear phononic signatures, while the transversal signal changes sign upon entering the low-temperature, magnetically ordered phase. Our results demonstrate that uncovering a genuinely quantized magnetic thermal Hall effect in Kitaev topological quantum spin liquids such as α-RuCl3 and Na2Co2TeO6 requires disentangling phonon vs magnetic contributions, including potentially fractionalized excitations such as the expected Majorana fermions

Magnetic resonance study of rare-earth titanates

We present a nuclear magnetic resonance (NMR) and electron spin resonance (ESR) study of rare-earth titanates derived from the spin-1/2 Mott insulator YTiO$_3$. Measurements of single-crystalline samples of (Y,Ca,La)TiO$_3$ in a wide range of isovalent substitution (La) and hole doping (Ca) reveal several unusual features in the paramagnetic state of these materials. $^{89}$Y NMR demonstrates a clear discrepancy between the static and dynamic local magnetic susceptibilities, with deviations from Curie-Weiss behavior far above the Curie temperature $T_C$. No significant changes are observed close to $T_C$, but a suppression of fluctuations is detected in the NMR spin-lattice relaxation time at temperatures of about $3\times T_C$. Additionally, the nuclear spin-spin relaxation rate shows an unusual peak in dependence on temperature for all samples. ESR of the unpaired Ti electron shows broad resonance lines at all temperatures and substitution/doping levels, which we find to be caused by short electronic spin-lattice relaxation times. We model the relaxation as an Orbach process that involves a low-lying electronic excited state, which enables the determination of the excited-state gap from the temperature dependence of the ESR linewidths. We ascribe the small gap to Jahn-Teller splitting of the two lower Ti $t_{2g}$ orbitals. The value of the gap closely follows $T_C$ and is consistent with the temperatures at which deviations from Curie-Weiss fluctuations are observed in NMR. These results provide insight into the interplay between orbital and spin degrees of freedom in rare-earth titanates and indicate that full orbital degeneracy lifting is associated with ferromagnetic order

Probing the magnetic superexchange couplings between terminal CuII ions in heterotrinuclear bis(oxamidato) type complexes

The reaction of one equivalent of [n-Bu4N]2[Ni(opboR2)] with two equivalents of [Cu(pmdta)(X)2] afforded the heterotrinuclear CuIINiIICuII containing bis(oxamidato) type complexes [Cu2Ni(opboR2)(pmdta)2]X2 (R = Me, X = NO3– (1); R = Et, X = ClO4– (2); R = n-Pr, X = NO3– (3); opboR2 = o-phenylenebis(NR-substituted oxamidato); pmdta = N,N,N’,N”,N”-pentamethyldiethylenetriamine). The identities of the heterotrinuclear complexes 1–3 were established by IR spectroscopy, elemental analysis and single-crystal X-ray diffraction studies, which revealed the cationic complex fragments [Cu2Ni(opboR2)(pmdta)2]2+ as not involved in any further intermolecular interactions. As a consequence thereof, the complexes 1–3 possess terminal paramagnetic [Cu(pmdta)]2+ fragments separated by [NiII(opboR2)]2– bridging units representing diamagnetic SNi = 0 states. The magnetic field dependence of the magnetization M(H) of 1–3 at T = 1.8 K has been determined and is shown to be highly reproducible with the Brillouin function for an ideal paramagnetic spin = 1/2 system, verifying experimentally that no magnetic superexchange couplings exists between the terminal paramagnetic [Cu(pmdta)]2+ fragments. Susceptibility measurements versus temperature of 1–3 between 1.8–300 K were performed to reinforce the statement of the absence of magnetic superexchange couplings in these three heterotrinuclear complexes