Tuning Electronic Correlation with Pressure

Strongly correlated electron systems display some of the most exotic ground states in condensed matter. In this thesis high pressure is used to tune the degree of electron correlations in systems of current interest. Their electronic and structural properties were investigated at high pressure using x-ray spectroscopy and scattering as well as transport techniques in a diamond anvil cell. The interplay between short- and long-range structural order, one-dimensional charge ordering, and superconductivity was studied in La1.875Ba0.125CuO4. At ambient pressure, this material displays charge ordering at the onset of a low temperature structural phase transition, resulting in strong suppression of superconductivity. The electronic ordering is shown here to be tightly coupled to short-range, rather than long-range, structural order. It is argued that persistence of charge order on a very short length scale is responsible for the marginal enhancement of superconductivity under pressure, being evidence of competing electronic correlations. The lanthanides Gd and Tb display an atomic-like partially filled 4f level at ambient pressure. Here, extreme pressure was used in an attempt to delocalize these 4f states. Instability in Tb\u27s 4f8 level emerges through 4f-conduction band hybridization, triggering a Kondo effect in the Y(Tb) alloy. In contrast, the half-filled 4f7 level in Gd remains stable to at least 120 GPa. Tb appears to become a strongly correlated Kondo lattice at high pressure, the properties of which are of great interest. Alkali metals display unexpected properties at high pressure which are suggested to be due to enhanced electronic correlation of the once nearly-free conduction electrons. In this thesis, the mechanisms leading to the low symmetry phases observed at high pressure in K, Rb, and Cs were investigated. These phases are suggested to develop from the pressure-induced localization of the conduction band, which triggers a Peierls-like distortion. Furthermore, stripe-like charge ordering is theoretically observed in Cs at high pressure, in close resemblance to La1.875Ba0.125CuO4, including proximity of charge order to superconductivity

Inverted orbital polarization in strained correlated oxide films

Manipulating the orbital occupation of valence electrons via epitaxial strain in an effort to induce new functional properties requires considerations of how changes in the local bonding environment affect the band structure at the Fermi level. Using synchrotron radiation to measure the x-ray linear dichroism of epitaxially strained films of the correlated oxide CaFeO3, we demonstrate that the orbital polarization of the Fe valence electrons is opposite from conventional understanding. Although the energetic ordering of the Fe 3d orbitals is confirmed by multiplet ligand field theory analysis to be consistent with previously reported strain-induced behavior, we find that the nominally higher energy orbital is more populated than the lower. We ascribe this inverted orbital polarization to an anisotropic bandwidth response to strain in a compound with nearly filled bands. These findings provide an important counterexample to the traditional understanding of strain-induced orbital polarization and reveal a new method to engineer otherwise unachievable orbital occupations in correlated oxides

Spontaneous orbital polarization in the nematic phase of FeSe

The origin of nematicity in FeSe remains a critical outstanding question towards understanding unconventional superconductivity in proximity to nematic order. To understand what drives the nematicity, it is essential to determine which electronic degree of freedom admits a spontaneous order parameter independent from the structural distortion. Here, we use X-ray linear dichroism at the Fe K pre-edge to measure the anisotropy of the 3d orbital occupation as a function of in situ applied stress and temperature across the nematic transition. Along with X-ray diffraction to precisely quantify the strain state, we reveal a lattice-independent, spontaneously-ordered orbital polarization within the nematic phase, as well as an orbital polarizability that diverges as the transition is approached from above. These results provide strong evidence that spontaneous orbital polarization serves as the primary order parameter of the nematic phase.Comment: Main: 22 pages, 4 figures. Supp: 32 pages, 18 figure

Machine learning spectral indicators of topology

Topological materials discovery has emerged as an important frontier in condensed matter physics. Recent theoretical approaches based on symmetry indicators and topological quantum chemistry have been used to identify thousands of candidate topological materials, yet experimental determination of materials' topology often poses significant technical challenges. X-ray absorption spectroscopy (XAS) is a widely-used materials characterization technique sensitive to atoms' local symmetry and chemical environment; thus, it may encode signatures of materials' topology, though indirectly. In this work, we show that XAS can potentially uncover materials' topology when augmented by machine learning. By labelling computed X-ray absorption near-edge structure (XANES) spectra of over 16,000 inorganic materials with their topological class, we establish a machine learning-based classifier of topology with XANES spectral inputs. Our classifier correctly predicts 81% of topological and 80% of trivial cases, and can achieve 90% and higher accuracy for materials containing certain elements. Given the simplicity of the XAS setup and its compatibility with multimodal sample environments, the proposed machine learning-empowered XAS topological indicator has the potential to discover broader categories of topological materials, such as non-cleavable compounds and amorphous materials. It can also inform a variety of field-driven phenomena in situ, such as magnetic field-driven topological phase transitions.Comment: 14 pages, 3 main figures and 5 supplementary figures. Feedback most welcom

First demonstration of tuning between the Kitaev and Ising limits in a honeycomb lattice

Recent observations of novel spin-orbit coupled states have generated tremendous interest in $4d/5d$ transition metal systems. A prime example is the $J_{\text{eff}}=\frac{1}{2}$ state in iridate materials and $\alpha$-RuCl$_{3}$ that drives Kitaev interactions. Here, by tuning the competition between spin-orbit interaction ($\lambda_{\text{SOC}}$) and trigonal crystal field splitting ($\Delta_\text{T}$), we restructure the spin-orbital wave functions into a novel $\mu=\frac{1}{2}$ state that drives Ising interactions. This is done via a topochemical reaction that converts Li$_{2}$RhO$_{3}$ to Ag$_{3}$LiRh$_{2}$O$_{6}$, leading to an enhanced trigonal distortion and a diminished spin-orbit coupling in the latter compound. Using perturbation theory, we present an explicit expression for the new $\mu=\frac{1}{2}$ state in the limit $\Delta_\text{T}\gg \lambda_{\text{SOC}}$ realized in Ag$_{3}$LiRh$_{2}$O$_{6}$, different from the conventional $J_\text{eff}=\frac{1}{2}$ state in the limit $\lambda_{\text{SOC}}\gg \Delta_\text{T}$ realized in Li$_{2}$RhO$_{3}$. The change of ground state is followed by a dramatic change of magnetism from a 6 K spin-glass in Li$_{2}$RhO$_{3}$ to a 94 K antiferromagnet in Ag$_{3}$LiRh$_{2}$O$_{6}$. These results open a pathway for tuning materials between the two limits and creating a rich magnetic phase diagram.Comment: 22 pages, 4 figure

Strain-Switchable Field-Induced Superconductivity

Field-induced superconductivity is a rare phenomenon where an applied magnetic field enhances or induces superconductivity. This fascinating effect arises from a complex interplay between magnetism and superconductivity, and it offers the tantalizing technological possibility of an infinite magnetoresistance superconducting spin valve. Here, we demonstrate field-induced superconductivity at a record-high temperature of T=9K in two samples of the ferromagnetic superconductor Eu(Fe$_{0.88}$Co$_{0.12}$)$_{2}$As$_{2}$. We combine tunable uniaxial stress and applied magnetic field to shift the temperature range of the zero-resistance state between 4K and 10K. We use x-ray diffraction and spectroscopy measurements under stress and field to demonstrate that stress tuning of the nematic order and field tuning of the ferromagnetism act as independent tuning knobs of the superconductivity. Finally, DFT calculations and analysis of the Eu dipole field reveal the electromagnetic mechanism of the field-induced superconductivity.Comment: Main text: 15 pages, 5 figures; Supplement: 15 pages, 10 supplementary figure

Pressure-induced charge orders and their postulated coupling to magnetism in hexagonal multiferroic LuFe\u3csub\u3e2\u3c/sub\u3eO\u3csub\u3e4\u3c/sub\u3e

Hexagonal LuFe2O4 is a promising charge order (CO) driven multiferroic material with high charge and spin-ordering temperatures. The coexisting charge and spin orders on Fe3+/Fe2+ sites result in magnetoelectric behaviors, but the coupling mechanism between the charge and spin orders remains elusive. Here, by tuning external pressure, we reveal three charge-ordered phases with suggested correlation to magnetic orders in LuFe2O4: (i) a centrosymmetric incommensurate three-dimensional CO with ferrimagnetism, (ii) a non-centrosymmetric incommensurate quasi-two-dimensional CO with ferrimagnetism, and (iii) a centrosymmetric commensurate CO with antiferromagnetism. Experimental in situ single-crystal X-ray diffraction and X-ray magnetic circular dichroism measurements combined with density functional theory calculations suggest that the charge density redistribution caused by pressure-induced compression in the frustrated double-layer [Fe2O4] cluster is responsible for the correlated spin-charge phase transitions. The pressure-enhanced effective Coulomb interactions among Fe-Fe bonds drive the frustrated (1/3, 1/3) CO to a less frustrated (1/4, 1/4) CO, which induces the ferrimagnetic to antiferromagnetic transition. Our results not only elucidate the coupling mechanism among charge, spin, and lattice degrees of freedom in LuFe2O4, but also provide a new way to tune the spin-charge orders in a highly controlled manner

Quasi-2D anomalous Hall Mott insulator of topologically engineered Jeff =1/2 electrons

We investigate an experimental toy-model system of a pseudospin-half square-lattice Hubbard Hamiltonian in [(SrIrO3)1/(CaTiO3)1] to include both nontrivial complex hopping and moderate electronic correlation. While the former induces electronic Berry phases as anticipated from the weak-coupling limit, the later stabilizes an antiferromagnetic (AFM) Mott insulator ground state in analogous to the strong-coupling limit. Their combined results in the real system are found to be an anomalous Hall effect with a non-monotonic temperature dependence due to the self-competition of the electron-hole pairing in the Mott state, and an exceptionally large Ising anisotropy that is captured as a giant magnon gap beyond the superexchange approach. The unusual phenomena highlight the rich interplay of electronic topology and electronic correlation in the intermediate-coupling regime that is largely unexplored and challenging in theoretical modelling.Comment: Accepted by Phys. Rev.