arXiv subjects

J. A. Mundy

Publications and source records attributed to J. A. Mundy.

6 recordsLinked to original sources

arXiv2026

Contrasting Spin Excitations in Octahedral and Square-Planar n=8 Ruddlesden-Popper Nickelates

The discovery of superconductivity in reduced square-planar nickelates marked a major advance in identifying structural and electronic analogs to the high-$T_c$ cuprates. The more recent observation of superconductivity in parent Ruddlesden-Popper (RP) octahedral nickelates with a clear difference in electron count with respect to cuprates raises new questions about the nature of superconductivity across these related but distinct nickelate families. Here, we use Ni $L_3$-edge resonant inelastic x-ray scattering (RIXS) to probe the low-energy excitations in a representative compound of both families: the parent octahedral $n=8$ RP phase Nd$_9$Ni$_8$O$_{25}$ (p-RP), which is non-superconducting, and its reduced square-planar counterpart Nd$_9$Ni$_8$O$_{18}$ (r-RP), which exhibits superconducting correlations with a $T_c \approx 5$ K. The $n=8$ p-RP develops a spin-density-wave (SDW) ground state with ordering wave vector $q_{\mathrm{SDW}} = (1/4,\, 1/4)$, analogous to the bilayer RP, while the $n=8$ r-RP shows an elastic peak at $q^\star = (1/3,\, 0)$. Polarimetric RIXS shows that the p-RP exhibits low-energy spectra dominated by weakly dispersive paramagnons along the 0$\rightarrowπ$ and $π\!\rightarrow\! π$ directions, whereas the r-RP with superconducting correlations displays dispersionless magnetic excitations. Our results comprehensively map out the spin excitations and reveal fundamental differences in the ground state between these two distinct structural families.

cond-mat.str-el↗

arXiv2024

Electronic band structure of a superconducting nickelate probed by the Seebeck coefficient in the disordered limit

Superconducting nickelates are a new family of strongly correlated electron materials with a phase diagram closely resembling that of superconducting cuprates. While analogy with the cuprates is natural, very little is known about the metallic state of the nickelates, making these comparisons difficult. We probe the electronic dispersion of thin-film superconducting 5-layer ($n=5$) and metallic 3-layer ($n=3$) nickelates by measuring the Seebeck coefficient, $S$. We find a temperature-independent and negative $S/T$ for both $n=5$ and $n=3$ nickelates. These results are in stark contrast to the strongly temperature-dependent $S/T$ measured at similar electron filling in the cuprate La$_{1.36}$Nd$_{0.4}$Sr$_{0.24}$CuO$_4$. The electronic structure calculated from density functional theory can reproduce the temperature dependence, sign, and amplitude of $S/T$ in the nickelates using Boltzmann transport theory. This demonstrates that the electronic structure obtained from first-principles calculations provides a reliable description of the Fermiology of superconducting nickelates, and suggests that, despite indications of strong electronic correlations, there are well-defined quasiparticles in the metallic state. Finally, we explain the differences in the Seebeck coefficient between nickelates and cuprates as originating in strong dissimilarities in impurity concentrations. Our study demonstrates that the high elastic scattering limit of the Seebeck coefficient reflects only the underlying band structure of a metal, analogous to the high magnetic field limit of the Hall coefficient. This opens a new avenue for Seebeck measurements to probe the electronic band structures of relatively disordered quantum materials.

cond-mat.supr-con↗

arXiv2023

3D oxygen vacancy order and defect-property relations in multiferroic (LuFeO$_3$)$_9$/(LuFe$_2$O$_4$)$_1$ superlattices

Oxide heterostructures exhibit a vast variety of unique physical properties. Examples are unconventional superconductivity in layered nickelates and topological polar order in (PbTiO$_3$)$_n$/(SrTiO$_3$)$_n$ superlattices. Although it is clear that variations in oxygen content are crucial for the electronic correlation phenomena in oxides, it remains a major challenge to quantify their impact. Here, we measure the chemical composition in multiferroic (LuFeO$_3$)$_9$/(LuFe$_2$O$_4$)$_1$ superlattices, revealing a one-to-one correlation between the distribution of oxygen vacancies and the electric and magnetic properties. Using atom probe tomography, we observe oxygen vacancies arranging in a layered three-dimensional structure with a local density on the order of 10$^{14}$ cm$^{-2}$, congruent with the formula-unit-thick ferrimagnetic LuFe$_2$O$_4$ layers. The vacancy order is promoted by the locally reduced formation energy and plays a key role in stabilizing the ferroelectric domains and ferrimagnetism in the LuFeO$_3$ and LuFe$_2$O$_4$ layers, respectively. The results demonstrate the importance of oxygen vacancies for the room-temperature multiferroicity in this system and establish an approach for quantifying the oxygen defects with atomic-scale precision in 3D, giving new opportunities for deterministic defect-enabled property control in oxide heterostructures.

cond-mat.mtrl-sci↗

arXiv2017

Electron Accumulation and Emergent Magnetism in LaMnO3/SrTiO3 Heterostructures

Emergent phenomena at polar-nonpolar oxide interfaces have been studied intensely in pursuit of next-generation oxide electronics and spintronics. Here we report the disentanglement of critical thicknesses for electron reconstruction and the emergence of ferromagnetism in polar-mismatched LaMnO3/SrTiO3 (001) heterostructures. Using a combination of element-specific X-ray absorption spectroscopy and dichroism, and first-principles calculations, interfacial electron accumulation and ferromagnetism have been observed within the polar, antiferromagnetic insulator LaMnO3. Our results show that the critical thickness for the onset of electron accumulation is as thin as 2 unit cells (UC), significantly thinner than the observed critical thickness for ferromagnetism of 5 UC. The absence of ferromagnetism below 5 UC is likely induced by electron over-accumulation. In turn, by controlling the doping of the LaMnO3, we are able to neutralize the excessive electrons from the polar mismatch in ultrathin LaMnO3 films and thus enable ferromagnetism in films as thin as 3 UC, extending the limits of our ability to synthesize and tailor emergent phenomena at interfaces and demonstrating manipulation of the electronic and magnetic structures of materials at the shortest length scales.

cond-mat.mtrl-sci↗

arXiv2014

Epitaxial Growth of VO$_{2}$ by Periodic Annealing

We report the growth of ultrathin VO$_{2}$ films on rutile TiO$_{2}$ (001) substrates via reactive molecular-beam epitaxy. The films were formed by the cyclical deposition of amorphous vanadium and its subsequent oxidation and transformation to VO$_{2}$ via solid-phase epitaxy. Significant metal-insulator transitions were observed in films as thin as 2.3 nm, where a resistance change ΔR/R of 25 was measured. Low angle annular dark field scanning transmission electron microscopy was used in conjunction with electron energy loss spectroscopy to study the film/substrate interface and revealed the vanadium to be tetravalent and the titanium interdiffusion to be limited to 1.6 nm.

cond-mat.mtrl-sci↗

arXiv2013

LaAlO3 stoichiometry found key to electron liquid formation at LaAlO3/SrTiO3 interfaces

Emergent phenomena, including superconductivity and magnetism, found in the two-dimensional electron liquid (2-DEL) at the interface between the insulators LaAlO3 and SrTiO3 distinguish this rich system from conventional two-dimensional electron gases at compound semiconductor interfaces. The origin of this 2-DEL, however, is highly debated with focus on the role of defects in the SrTiO3 while the LaAlO3 has been assumed perfect. Our experiments and first principles calculations show that the cation stoichiometry of the nominal LaAlO3 layer is key to 2-DEL formation: only Al-rich LaAlO3 results in a 2-DEL. While extrinsic defects including oxygen deficiency are known to render LaAlO3/SrTiO3 samples conducting, our results show that in the absence of such extrinsic defects, an interface 2-DEL can form. Its origin is consistent with an intrinsic electronic reconstruction occurring to counteract a polarization catastrophe. This work provides a roadmap for identifying other interfaces where emergent behaviors await discovery.

cond-mat.mtrl-sci↗