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Chakhalian, Jak

Publications and source records attributed to Chakhalian, Jak.

Ultrafast Terahertz Field Control of the Emergent Magnetic and Electronic Interactions at Oxide Interfaces

Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of the next generation of energy-efficient devices. Here, it is demonstrated that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense, single-cycle THz electric-field pulses. A suite of advanced X-ray spectroscopic techniques is employed to measure a detailed magneto-optical profile and the thickness of the ferromagnetic interfacial layer. Then, a combination of time-resolved and temperature-dependent optical measurements is used to disentangle several correlated electronic and magnetic processes driven by ultrafast, high-field THz pulses. Sub-picosecond non-equilibrium Joule heating of the electronic system is observed, ultrafast demagnetization of the ferromagnetic interfacial layer, and slower dynamics indicative of a change in the magnetic state of the superlattice due to the transfer of spin-angular momentum to the lattice. These findings suggest a promising avenue for the efficient control of 2D ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.

X-ray spectroscopy and scattering↗

Chiral spin-liquid-like state in pyrochlore iridate thin films

The pyrochlore iridates have become ideal platforms to unravel fascinating correlated and topological phenomena that stem from the intricate interplay among strong spin-orbit coupling, electronic correlations, lattice with geometric frustration, and itinerancy of the 5d electrons. The all-in-all-out antiferromagnetic state, commonly considered as the magnetic ground state, can be dramatically altered in reduced dimensionality, leading to exotic or hidden quantum states inaccessible in bulk. Here, by means of magnetotransport, resonant elastic and inelastic x-ray scattering experiments, we discover an emergent quantum disordered state in (111) Y 2 Ir 2 O 7 thin films (thickness ≤30 nm) persisting down to 5 K, characterized by dispersionless magnetic excitations. The anomalous Hall effect observed below an onset temperature near 125 K corroborates the presence of chiral short-range spin configurations expressed in non-zero scalar spin chirality, breaking the macroscopic time-reversal symmetry. The origin of this chiral state is ascribed to the restoration of magnetic frustration on the pyrochlore lattice in lower dimensionality, where the competing exchange interactions together with enhanced quantum fluctuations suppress any long-range order and trigger spin-liquid-like behavior with degenerate ground-state manifold.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Topological Excitations in Pyrochlore Heterostructures

This research project focuses on developing innovative materials that demonstrate unique quantum properties, specifically within electron systems that exhibit complex interactions, known as "correlated electron systems." Unlike non-correlated materials, finding topological phases (special states of matter with protected properties that make them stable against defects) in these correlated systems is a significant challenge. The project aims to design synthetic templates of two-dimensional "Kagome lattice" structures, made from specific materials called iridates and osmates, to study and control these exotic quantum behaviors. To achieve this, the project employs a cutting-edge spectroscopic tools that allow precise analysis of artificial quantum materials in terms of both energy and momentum while they are being created, using a specialized laser-based process called laser Molecular Beam Epitaxy.

36 MATERIALS SCIENCE↗

Magnetic Weyl Semimetallic Phase in Thin Films of Eu 2 Ir 2 O 7

The interplay between electronic interactions and strong spin-orbit coupling is expected to create a plethora of fascinating correlated topological states of quantum matter. Of particular interest are magnetic Weyl semimetals originally proposed in the pyrochlore iridates, which are only expected to reveal their topological nature in thin film form. To date, however, direct experimental demonstrations of these exotic phases remain elusive, due to the lack of usable single crystals and the insufficient quality of available films. Here, in this study, we report on the discovery of signatures for the long-sought magnetic Weyl semimetallic phase in (111)-oriented Eu 2 Ir 2 O 7 high-quality epitaxial thin films. We observed an intrinsic anomalous Hall effect with colossal coercivity but vanishing net magnetization, which emerges right below the onset of a peculiar magnetic phase with all-in-all-out (AIAO) antiferromagnetic ordering. The anomalous Hall conductivity obtained experimentally is consistent with the theoretical prediction, likely arising from the nonzero Berry curvature emanated by Weyl node pairs near the Fermi level that act as sources and sinks of Berry flux, activated by broken cubic crystal symmetry at the top and bottom terminations of the thin film.

36 MATERIALS SCIENCE↗

Epitaxial stabilization of thin films of the frustrated Ge-based spinels

Frustrated magnets can host numerous exotic many-body quantum and topological phenomena. GeNi 2 O 4 is a three-dimensional S=1 frustrated magnet with an unusual two-stage transition to the two-dimensional antiferromagnetic ground state, while GeCu 2 O 4 is a high-pressure phase with a strongly tetragonally elongated spinel structure and magnetic lattice formed by S=1/2 CuO 2 linear chains with frustrated interchain exchange interactions and exotic magnetic behavior. Here, we report on the thin-film epitaxial stabilization of these two compounds. The developed growth mode, surface morphology, crystal structure, and copper valence state were characterized by in situ reflection high-energy electron diffraction, atomic force microscopy, x-ray reflectivity, x-ray diffraction, x-ray photoelectron spectroscopy, and resonant x-ray absorption spectroscopy. Our results pave an alternative route to the comprehensive investigation of the puzzling magnetic properties of these compounds and the exploration of emergent features driven by strain.

36 MATERIALS SCIENCE↗

Proximate Quantum Spin Liquid on Designer Lattice

Complementary to bulk synthesis, here we propose a designer lattice with extremely high magnetic frustration and demonstrate the possible realization of a quantum spin liquid state from both experiments and theoretical calculations. In an ultrathin (111) CoCr 2 O 4 slice composed of three triangular and one kagome cation planes, the absence of a spin ordering or freezing transition is demonstrated down to 0.03 K, in the presence of strong antiferromagnetic correlations in the energy scale of 30 K between Co and Cr sublattices, leading to the frustration factor of similar to 1000. Persisting spin fluctuations are observed at low temperatures via low-energy muon spin relaxation. Our calculations further demonstrate the emergence of highly degenerate magnetic ground states at the 0 K limit, due to the competition among multiply altered exchange interactions. Furthermore, these results collectively indicate the realization of a proximate quantum spin liquid state on the synthetic lattice.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Orientation-dependent stabilization of MgCr 2 O 4 spinel thin films

AB 2 O 4 normal spinels with a magnetic B site can host a variety of magnetic and orbital frustrations leading to spin-liquid phases and field-induced phase transitions. Here, we report the epitaxial growth of (111)-oriented MgCr 2 O 4 thin films. By characterizing the structural and electronic properties of films grown along the (001) and (111) directions, the influence of growth orientation has been studied. Despite distinctly different growth modes observed during deposition, the comprehensive characterization reveals no measurable disorder in the cation distribution nor multivalency issue for Cr ions in either orientation. Contrary to a naive expectation, the (111) stabilized films exhibit a smoother surface and a higher degree of crystallinity than (001)-oriented films. The preference in growth orientation is explained within the framework of heteroepitaxial stabilization in connection to a significantly lower (111) surface energy. Furthermore, these findings open broad opportunities in the fabrication of two-dimensional kagome-triangular heterostructures with emergent magnetic behavior inaccessible in bulk crystals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Strongly correlated and topological states in [111] grown transition metal oxide thin films and heterostructures

We highlight recent advances in the theory, materials fabrication, and experimental characterization of strongly correlated and topological states in [111] oriented transition metal oxide thin films and heterostructures, which are notoriously difficult to realize compared to their [001] oriented counterparts. We focus on two classes of complex oxides, with the chemical formulas ABO 3 and A 2 B 2 O 7 , where the B sites are occupied by an open-shell transition metal ion with a local moment and the A sites are typically a rare earth element. The [111] oriented quasi-two-dimensional lattices derived from these parent compound lattices can exhibit peculiar geometries and symmetries, namely, a buckled honeycomb lattice, as well as kagome and triangular lattices. These lattice motifs form the basis for emergent strongly correlated and topological states expressed in exotic magnetism, various forms of orbital ordering, topological insulators, topological semimetals, quantum anomalous Hall insulators, and quantum spin liquids. For transition metal ions with high atomic number, spin–orbit coupling plays a significant role and may give rise to additional topological features in the electronic band structure and in the spectrum of magnetic excitations. We conclude this perspective by articulating open challenges and opportunities in this actively developing field.

36 MATERIALS SCIENCE↗