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Monica Ciomaga Hatnean

Publications and source records attributed to Monica Ciomaga Hatnean.

At least 19 recordsLinked to original sources

Coherent spin waves in a maximal entropy phase

In solids, disorder is conventionally regarded as detrimental to coherence. It typically localizes and dampens collective excitations, as exemplified by Anderson localization or the broadening of magnetic modes in systems lacking long-range order. While high-entropy materials are specifically designed to harness disorder and stabilize homogeneous mixed-phase structures that can display unique properties, this same disorder is nonetheless expected to preclude the formation of coherent magnetic excitations. To test the limits of this picture, we selected the antiferromagnetic system YBaCuFeO5, as it features two distinct transition metal atoms with significantly different magnetic moments, rendering its spin dynamics exceptionally sensitive to local atomic ordering. Combining resonant inelastic x-ray scattering and linear spin wave theory, we reveal a surprising paradox: YBaCuFeO5 exhibits an unexpected, entropy-driven mixed phase, in which disorder, rather than reducing the lifetime of the collective excitations, favors coherence. In this mixed phase, the spin waves remain dispersive, markedly distinct from those expected for an ordered ground state, and exhibit well-defined acoustic and optical branches separated by a large optical gap. These results demonstrate that in entropy-stabilized magnets, disorder can favor coherent collective modes previously thought to be exclusive to low-entropy systems.

cond-mat.str-el↗

Hierarchical quasiparticle dynamics in antiferromagnets revealed by time- and momentum-resolved X-ray scattering

Energy flows among coupled subsystems are essential for ultrafast dynamics and high-speed technologies. In magnetic materials, spin fluctuations -- magnons -- mediate these flows in ultrafast magnetism. Yet momentum-resolved access to low-energy magnons governing the microscopic dynamics has been lacking. Using time-resolved resonant diffuse scattering alongside complementary time-resolved X-ray techniques and quantum-kinetic simulations, we unveil the hierarchical energy pathways among correlated systems in the photoexcited antiferromagnet CuO. Above-bandgap excitation triggers near-instantaneous spin disorder, generating non-thermal magnons throughout reciprocal space within femtoseconds. Real-time momentum-resolved tracking reveals picosecond magnon quasi-thermalization, followed by nanosecond recovery via momentum-selective magnon-phonon scattering. The quasiparticle dispersion mismatch creates recovery bottlenecks that control non-equilibrium lifetimes. This microscopic framework transcends phenomenological models and generalizes across materials, establishing design principles for ultrafast control of material properties.

cond-mat.str-el↗

An inelastic neutron scattering study of the magnetic field dependence of the quantum dipolar garnet: Yb$_3$Ga$_5$O$_{12}$

The garnet compound Yb$_3$Ga$_5$O$_{12}$ is a fascinating material that is considered highly suitable for low-temperature refrigeration, via the magnetocaloric effect, in addition to enabling the exploration of quantum states with long-range dipolar interactions. It has previously been theorized that the magnetocaloric effect can be enhanced, in Yb$_3$Ga$_5$O$_{12}$ , via magnetic soft mode excitations which in the hyperkagome structure would be derived from an emergent magnetic structure formed from nanosized 10-spin loops. We study the magnetic field dependence of bands of magnetic soft mode excitations in the effective spin $S = 1/2$ hyperkagome compound Yb$_3$Ga$_5$O$_{12}$ using single crystal inelastic neutron scattering. We probe the magnetically short ranged ordered state, in which we determine magnetic nanoscale structures coexisting with a fluctuating state, and the magnetically saturated state. We determine that Yb$_3$Ga$_5$O$_{12}$ can be described as a quantum dipolar magnet with perturbative weak near-neighbor and inter-hyperkagome exchange interaction. The magnetic excitations, under the application of a magnetic field, reveal highly robust soft modes with distinctive signatures of the quantum nature of the Yb3+ spins. Our results enhance our understanding of soft modes in topological frustrated magnets that drive both the unusual physics of quantum dipolar systems and future refrigerant material design.

cond-mat.str-el↗

Impact of disorder in Nd-based pyrochlore magnets

We study the stability of the antiferromagnetic all-in--all-out state observed in dipolar-octupolar pyrochlores that have neodymium as the magnetic species. Different types of disorder are considered, either affecting the immediate environment of the Nd$^{3+}$ ion, or substituting it with a non-magnetic ion. Starting from the well studied Nd$_2$Zr$_2$O$_7$ compound, Ti substitution on the Zr site and dilution on the Nd magnetic site with La substitution are investigated. The recently discovered entropy stabilized compound NdMox, which exhibits a high degree of disorder on the non magnetic site is also studied. Using a range of experimental techniques, especially very low-temperature magnetization and neutron scattering, we show that the all-in--all-out state is very robust and withstands substitutional disorder up to large rates. From these measurements, we estimate the Hamiltonian parameters and discuss their evolution in the framework of the phase diagram of dipolar-octupolar pyrochlore magnets.

cond-mat.str-el↗

Electrical transport signatures of metallic surface state formation in the strongly-correlated insulator FeSb2

We present local and nonlocal electrical transport measurements of the correlated insulator FeSb$_2$. By employing wiring configurations that delineate between bulk- and surface-dominated conduction, we reveal the formation of a metallic surface state in FeSb$_2$ for temperatures $\lessapprox 5$~K. This result is corroborated by an angular rotation study of this material's magnetotransport, which also shows signatures of the transition from bulk- to surface-dominated conduction over the same temperature interval as the local/nonlocal transport divergence. Notable similarities with the topological Kondo insulator candidate SmB$_6$ are discussed.

cond-mat.str-el↗

Charge doping into spin minority states mediates doubling of $T_\mathrm{C}$ in ferromagnetic CrGeTe$_3$

The recent discovery of the persistence of long-range magnetic order when van der Waals layered magnets are thinned towards the monolayer limit has provided a tunable platform for the engineering of novel magnetic structures and devices. Here, we study the evolution of the electronic structure of CrGeTe$_3$ as a function of electron doping in the surface layer. From angle-resolved photoemission spectroscopy, we observe spectroscopic fingerprints that this electron doping drives a marked increase in $T_\mathrm{C}$, reaching values more than double that of the undoped material, in agreement with recent studies using electrostatic gating. Together with density functional theory calculations and Monte Carlo simulations, we show that, surprisingly, the increased $T_\mathrm{C}$ is mediated by the population of spin-minority Cr $t_{2g}$ states, forming a half-metallic 2D electron gas at the surface. We show how this promotes a novel variant of double exchange, and unlocks a significant influence of the Ge -- which was previously thought to be electronically inert in this system -- in mediating Cr-Cr exchange.

cond-mat.mtrl-sci↗

Covalency, correlations, and inter-layer interactions governing the magnetic and electronic structure of Mn$_3$Si$_2$Te$_6$

Mn$_3$Si$_2$Te$_6$ is a rare example of a layered ferrimagnet. It has recently been shown to host a colossal angular magnetoresistance as the spin orientation is rotated from the in- to out-of-plane direction, proposed to be underpinned by a topological nodal-line degeneracy in its electronic structure. Nonetheless, the origins of its ferrimagnetic structure remain controversial, while its experimental electronic structure, and the role of correlations in shaping this, are little explored to date. Here, we combine x-ray and photoemission-based spectroscopies with first-principles calculations, to probe the elemental-selective electronic structure and magnetic order in Mn$_3$Si$_2$Te$_6$. Through these, we identify a marked Mn-Te hybridisation, which weakens the electronic correlations and enhances the magnetic anisotropy. We demonstrate how this strengthens the magnetic frustration in Mn$_3$Si$_2$Te$_6$, which is key to stabilising its ferrimagnetic order, and find a crucial role of both exchange interactions extending beyond nearest-neighbours and anti-symmetric exchange in dictating its ordering temperature. Together, our results demonstrate a powerful methodology of using experimental electronic structure probes to constrain the parameter space for first-principles calculations of magnetic materials, and through this approach, reveal a pivotal role played by covalency in stabilising the ferrimagnetic order in Mn$_3$Si$_2$Te$_6$.

cond-mat.mtrl-sci↗

Direct measurement of a remnant Fermi surface in SmB6

The quest to understand the nature of the electronic state in SmB6 has been challenging, perplexing and surprising researchers for over half a century. In the theoretically predicted topological Kondo insulator SmB6, the nature of the bulk electronic structure is not characterised unambiguously by quantum oscillations due to contrary interpretations. One simple definition of an electrical insulator is a material that lacks a Fermi surface and here we report the results of our investigation into its existence in SmB6 by Compton scattering. Compton scattering measures occupied electron momentum states, is bulk sensitive due to the high energy of the incoming photons and is also an ultra-fast probe of the correlated many-body electron wavefunction. Remarkably, direct evidence for a three-dimensional remnant Fermi surface is observed. However, a further dichotomy is raised in that the full occupancy expected of a conventional metal is not reproduced. Our observation of a remnant Fermi surface using a momentum-resolved probe provides significant new evidence that the paradigm of a bulk insulator is not robust for SmB6.

cond-mat.str-el↗

Intrinsic one-dimensional conducting channels in the Kondo insulator SmB6

Since its discovery as a Kondo insulator 50 years ago, SmB6 recently received a revival of interest due to detection of unexpected quantum oscillations in the insulating state, discovery of disorder-immune bulk transport, and proposals of correlation-driven topological physics. While recent transport results attribute the anomalous low temperature conduction to two-dimensional surface states, important alternatives, such as conduction channel residing in one-dimensional dislocation lines, have not been adequately explored. Here we study SmB6 with scanning microwave impedance microscopy and uncover evidence for conducting one-dimensional states terminating at surface step edges. These states remain conducting up to room temperature, indicating unusual robustness against scattering and an unconventional origin. Our results bring to light a heretofore undetected conduction route in SmB6 that contributes to the low temperature transport. The unique scenario of intrinsic one-dimensional conducting channels in a highly insulating correlated bulk offers a one-dimensional platform that may host exotic physics.

cond-mat.str-el↗

Impedance Spectroscopy of SmB$_6$ single crystals

We report results from an in--plane and out--of--plane impedance study on SmB$_6$ single crystals, performed at low temperatures and over a wide frequency range. A universal equivalent circuit describes the dielectric behavior of this system across the transition, from surface to bulk dominated electrical conduction between 2 and 10 K. We identify the resistive, capacitive, and inductive contributions to the impedance. The equivalent inductance, obtained from fits to experimental data, drops drastically as the bulk starts to control electrical conduction upon increasing temperature. SmB$_6$ single crystals also show current--controlled negative differential resistance at low temperatures, which is brought about by Joule heating. This feature, in addition to inductive and capacitive contributions to the impedance, can give rise to the self--sustained voltage oscillations observed below 5 K (Stern {\it et al.}, Phys. Rev. Lett. {\bf 116}, 166603 (2016)).

cond-mat.str-el↗

Emergent magnetic behaviour in the frustrated Yb$_3$Ga$_5$O$_{12}$ garnet

We report neutron scattering, magnetic susceptibility and Monte Carlo theoretical analysis to verify the short range nature of the magnetic structure and spin-spin correlations in a Yb$_3$Ga$_5$O$_{12}$ single crystal. The quantum spin state of Yb$^{3+}$ in Yb$_3$Ga$_5$O$_{12}$ is verified. The quantum spins organise into a short ranged emergent director state for T $<$ 0.4 K derived from anisotropy and near neighbour exchange. We derive the magnitude of the near neighbour exchange interactions $0.6\; {\rm K} < J_1 < 0.7\; {\rm K}, J_2 = 0.12$~K and the magnitude of the dipolar exchange interaction, $D$, in the range $0.18 < D < 0.21$ K. Certain aspects of the broad experimental dataset can be modelled using a $J_1D$ model with ferromagnetic near neighbour spin-spin correlations while other aspects of the data can be accurately reproduced using a $J_1J_2D$ model with antiferromagnetic near neighbour spin-spin correlation. As such, although we do not quantify all the relevant exchange interactions we nevertheless provide a strong basis for the understanding of the complex Hamiltonian required to fully describe the magnetic state of Yb$_3$Ga$_5$O$_{12}$.

cond-mat.str-el↗

Bulk transport paths through defects in floating zone and Al flux grown SmB$_6$

We investigate the roles of disorder on low-temperature transport in SmB$_6$ crystals grown by both the Al flux and floating zone methods. We used the inverted resistance method with Corbino geometry to investigate whether low-temperature variations in the standard resistance plateau arises from a surface or a bulk channel in floating zone samples. The results show significant sample-dependent residual bulk conduction, in contrast to smaller amounts of residual bulk conduction previously observed in Al flux grown samples with Sm vacancies. We consider hopping in an activated impurity band as a possible source for the observed bulk conduction, but it is unlikely that the large residual bulk conduction seen in floating zone samples is solely due to Sm vacancies. We therefore propose that one-dimensional defects, or dislocations, contribute as well. Using chemical etching, we find evidence for dislocations in both flux and floating zone samples, with higher dislocation density in floating zone samples than in Al flux grown samples. In addition to the possibility of transport through one-dimensional dislocations, we also discuss our results in the context of recent theoretical models of SmB$_6$.

cond-mat.str-el↗

Characterizing oxygen atoms in perovskite and pyrochlore oxides using ADF-STEM at a resolution of a few tens of picometers

We present an aberration corrected scanning transmission electron microscopy (ac-STEM) analysis of the perovskite (LaFeO3) and pyrochlore (Yb2Ti2O7 and Pr2Zr2O7) oxides and demonstrate that both the shape and contrast of visible atomic columns in annular dark-field (ADF) images are sensitive to the presence of nearby atoms of low atomic number (e.g. oxygen). We show that point defects (e.g. oxygen vacancies), which are invisible - or difficult to observe due to limited sensitivity - in X-ray and neutron diffraction measurements, are the origin of the complex magnetic ground state of pyrochlore oxides. In addition, we present, for the first time, a method by which light atoms can be resolved in quantitative ADF-STEM images. Using this method, we resolved oxygen atoms in perovskite and pyrochlore oxides.

cond-mat.mtrl-sci↗

Optical floating zone crystal growth of rare-earth disilicates, $R\mathbf{_{2}}$Si$\mathbf{_{2}}$O$\mathbf{_{7}}$ ($R=$ Er, Ho, and Tm)

The wealth of structural phases seen in the rare-earth disilicate compounds promises an equally rich range of interesting magnetic properties. We report on the crystal growth by the optical floating zone method of members of the rare-earth disilicate family, $R_{2}$Si$_{2}$O$_{7}$ (with $R=$ Er, Ho, and Tm). Through a systematic study, we have optimised the growth conditions for Er$_{2}$Si$_{2}$O$_{7}$. We have grown, for the first time using the floating zone method, crystal boules of Ho$_{2}$Si$_{2}$O$_{7}$ and Tm$_{2}$Si$_{2}$O$_{7}$ compounds. We show that the difficulties encountered in the synthesis of polycrystalline and single crystal samples are due to the similar thermal stability ranges of different rare-earth silicate compounds in the temperature-composition phase diagrams of the $R$-Si-O systems. The addition of a small amount of SiO$_{2}$ excess allowed the amount of impurity phases present in the powder samples to be minimised. The phase composition analysis of the powder X-ray diffraction data collected on the as-grown boules revealed that they were of single phase, except in the case of thulium disilicate, which comprised of two phases. All growths resulted in multi-grain boules, from which sizable single crystals could be isolated. The optimum conditions used for the synthesis and crystal growth of polycrystalline and single crystal $R_{2}$Si$_{2}$O$_{7}$ materials are reported. Specific heat measurements of erbium and thulium disilicate compounds confirm an antiferromagnetic phase transition below $T_{\mathrm{N}}=$ 1.8 K for D-type Er$_{2}$Si$_{2}$O$_{7}$ and a Schottky anomaly centered around 3.5 K in C-type Tm$_{2}$Si$_{2}$O$_{7}$, suggesting the onset of short-range magnetic correlations. Magnetic susceptibility data of E-type Ho$_{2}$Si$_{2}$O$_{7}$ reveals an antiferromagnetic ordering of the Ho spins below $T_\mathrm{N}=$ 2.3 K.

cond-mat.mtrl-sci↗

Intrinsic bulk quantum oscillations in a bulk unconventional insulator SmB$_6$

The finding of bulk quantum oscillations in the bulk Kondo insulator SmB$_6$, which has been proposed to be a correlated topological insulator, proved a considerable surprise. The subsequent measurement of bulk quantum oscillations in other correlated insulators including YbB$_{12}$ have lent support to our discovery of a class of unconventional insulators that are host to bulk quantum oscillations, of which SmB$_6$ was the first example. Here we perform a series of experiments to examine evidence for the intrinsic character of bulk quantum oscillations in floating zone-grown single crystals of SmB$_6$ that have been the subject of our quantum oscillation studies thus far. We present results of experiments including chemical composition analysis, magnetisation, thermal conductivity, electrical transport, and heat capacity on floating zone-grown single crystals of SmB$_6$, and a series of quantum oscillation experiments as a function of magnetic field, temperature, and magnetic field-orientation on single crystals of floating-zone grown SmB$_6$, LaB$_6$, and elemental Aluminium. Results of these experimental studies establish the intrinsic origin of quantum oscillations from the bulk of pristine floating zone-grown single crystals of SmB$_6$. The origin of the underlying bulk Fermi surface that bears close similarity with the unhybridised Fermi surface in metallic hexaborides despite the bulk insulating character of SmB$_6$ is thus at the heart of a theoretical mystery.

cond-mat.str-el↗

Direct observation of the energy gain underpinning ferromagnetic superexchange in the electronic structure of CrGeTe$_3$

We investigate the temperature-dependent electronic structure of the van der Waals ferromagnet, CrGeTe$_3$. Using angle-resolved photoemission spectroscopy, we identify atomic- and orbital-specific band shifts upon cooling through ${T_\mathrm{C}}$. From these, together with x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we identify the states created by a covalent bond between the Te ${5p}$ and the Cr ${e_g}$ orbitals as the primary driver of the ferromagnetic ordering in this system, while it is the Cr ${t_{2g}}$ states that carry the majority of the spin moment. The ${t_{2g}}$ states furthermore exhibit a marked bandwidth increase and a remarkable lifetime enhancement upon entering the ordered phase, pointing to a delicate interplay between localized and itinerant states in this family of layered ferromagnets.

cond-mat.str-el↗

Definitive Surface Magnetotransport Study of SmB$_{6}$

After the theoretical prediction that SmB$_6$ is a topological Kondo insulator, there has been an explosion of studies on the SmB$_6$ surface. However, there is not yet an agreement on even the most basic quantities such as the surface carrier density and mobility. In this paper, we carefully revisit Corbino disk magnetotransport studies to find those surface transport parameters. We first show that subsurface cracks exist in the SmB$_6$ crystals, arising both from surface preparation and during the crystal growth. We provide evidence that these hidden subsurface cracks are additional conduction channels, and the large disagreement between earlier surface SmB$_6$ studies may originate from previous interpretations not taking this extra conduction path into account. We provide an update of a more reliable magnetotransport data than the previous one (Phys. Rev. B 92, 115110) and find that the orders-of-magnitude large disagreements in carrier density and mobility come from the surface preparation and the transport geometry rather than the intrinsic sample quality. From this magnetotransport study, we find an updated estimate of the carrier density and mobility of 2.71$\times$10$^{13}$ (1/cm$^2$) and 104.5 (cm$^{2}$/V$\cdot$sec), respectively. We compare our results with other studies of the SmB$_6$ surface. By this comparison, we provide insight into the disagreements and agreements of the previously reported angle-resolved photoemission spectroscopy, scanning tunneling microscopy, and magnetotorque quantum oscillations measurements.

cond-mat.mes-hall↗

Neutron scattering signatures of a quantum spin ice

Quantum spin ice is an appealing proposal of a quantum spin liquid - systems where the magnetic moments of the constituent electron spins evade classical long-range order to form an exotic state that is quantum entangled and coherent over macroscopic length scales. Such phases are at the edge of our current knowledge in condensed matter as they go beyond the established paradigm of symmetry-breaking order and associated excitations. Neutron scattering experiments on the pyrochlore material Pr$_2$Hf$_2$O$_7$ reveal signatures of a quantum spin ice state that were predicted by theory.

cond-mat.str-el↗