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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) CoCr2O4 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 â¼1000. 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. These results collectively indicate the realization of a proximate quantum spin liquid state on the synthetic lattice.
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We report on the emergent magnetic state of (111)-oriented CoCr2O4 ultrathin films sandwiched between Al2O3 spacer layers in a quantum confined geometry. At the two-dimensional crossover, polarized neutron reflectometry reveals an anomalous enhancement of the total magnetization compared to the bulk value. Synchrotron X-ray magnetic circular dichroism measurements demonstrate the appearance of a long-range ferromagnetic ordering of spins on both Co and Cr sublattices. Brillouin function analyses and ab-initio density functional theory calculations further corroborate that the observed phenomena are due to the strongly altered magnetic frustration invoked by quantum confinement effects, manifested by the onset of a Yafet-Kittel-type ordering as the magnetic ground state in the ultrathin limit, which is unattainable in the bulk.
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Artificial complex-oxide heterostructures containing ultrathin buried layers grown along the pseudocubic [111] direction have been predicted to host a plethora of exotic quantum states arising from the graphene-like lattice geometry and the interplay between strong electronic correlations and band topology. To date, however, electronic-structural investigations of such atomic layers remain an immense challenge due to the shortcomings of conventional surface-sensitive probes with typical information depths of a few angstroms. Here, we use a combination of bulk-sensitive soft X-ray angle-resolved photoelectron spectroscopy (SX-ARPES), hard X-ray photoelectron spectroscopy (HAXPES), and state-of-the-art first-principles calculations to demonstrate a direct and robust method for extracting momentum-resolved and angle-integrated valence-band electronic structure of an ultrathin buckled graphene-like layer of NdNiO3 confined between two 4-unit cell-thick layers of insulating LaAlO3. The momentum-resolved dispersion of the buried Ni d states near the Fermi level obtained via SX-ARPES is in excellent agreement with the first-principles calculations and establishes the realization of an antiferro-orbital order in this artificial lattice. The HAXPES measurements reveal the presence of a valence-band bandgap of 265 meV. Our findings open a promising avenue for designing and investigating quantum states of matter with exotic order and topology in a few buried layers.
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One of the central challenges in condensed matter physics is to comprehend systems that have strong disorder and strong interactions. In the strongly localized regime, their subtle competition leads to glassy electron dynamics which ceases to exist well before the insulator-to-metal transition is approached as a function of doping. Here, we report on the discovery of glassy electron dynamics deep inside the good metal regime of an electron-doped quantum paraelectric system: KTaO3. We reveal that upon excitation of electrons from defect states to the conduction band, the excess injected carriers in the conduction band relax in a stretched exponential manner with a large relaxation time, and the system evinces simple aging phenomena-a telltale sign of glassy dynamics. Most significantly, we observe a critical slowing down of carrier dynamics below 35 K, concomitant with the onset of quantum paraelectricity in the undoped KTaO3. Our combined investigation using second harmonic generation technique, density functional theory and phenomenological modeling demonstrates quantum fluctuation-stabilized soft polar modes as the impetus for the glassy behavior. This study addresses one of the most fundamental questions regarding the potential promotion of glassiness by quantum fluctuations and opens a route for exploring glassy dynamics of electrons in a well-delocalized regime.
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A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phase via a topotactic reaction with a strongly reducing agent such as CaH2. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La1-xXxNiO2 / SrTiO3 (X = Ca and Sr) and Nd6Ni5O12 / NdGaO3 films, along with non-superconducting NdNiO2 / SrTiO3 and (Nd,Sr)NiO2 / SrTiO3. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that extensive hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates.
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Dynamic hysteresis, viz., delay in switching of a bistable system on account of the finite sweep rate of the drive, has been extensively studied in dynamical and thermodynamic systems. Dynamic hysteresis results from slowing of the response around a saddle-node bifurcation. As a consequence, the hysteresis area increases with the sweep rate. Mean-field theory, relevant for noise-free situations, predicts power-law scaling with the area scaling exponent of 2/3. We have experimentally investigated the dynamic hysteresis for a thermally driven metal-insulator transition in a high-quality NdNiO_{3} thin film and found the scaling exponent to be about 1/3, far less than the mean-field value. To understand this, we have numerically studied Langevin dynamics of the order parameter and found that noise, which can be thought to parallel finite temperature effects, influences the character of dynamic hysteresis by systematically lowering the dynamical exponent to as small as 0.2. The power-law scaling character, on the other hand, is unaffected in the range of chosen parameters. This work rationalizes the ubiquitous power-law scaling of the dynamic hysteresis as well as the wide variation in the scaling exponent between 0.66 and 0.2 observed in different systems over the last 30 years.
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Transition metal oxides are complex electronic systems that exhibit a multitude of collective phenomena. Two archetypal examples are VO2 and NdNiO3 , which undergo a metal-insulator phase transition (MIT), the origin of which is still under debate. Here this study reports the discovery of a memory effect in both systems, manifested through an increase of resistance at a specific temperature, which is set by reversing the temperature ramp from heating to cooling during the MIT. The characteristics of this ramp-reversal memory effect do not coincide with any previously reported history or memory effects in manganites, electron-glass or magnetic systems. From a broad range of experimental features, supported by theoretical modelling, it is found that the main ingredients for the effect to arise are the spatial phase separation of metallic and insulating regions during the MIT and the coupling of lattice strain to the local transition temperature of the phase transition. We conclude that the emergent memory effect originates from phase boundaries at the reversal temperature leaving "scars" in the underlying lattice structure, giving rise to a local increase in the transition temperature. The universality and robustness of the effect shed new light on the MIT in complex oxides.
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An unusual magnetoresistance (MR) behavior in Sr(2)FeMoO(6), recently termed as spin-valve-type MR (SVMR), presents several anomalies that are little understood so far. The formation of a magnetically distorted skin layer around every soft, ferromagnetic grain seems to be the reason behind such an unprecedented tunneling MR (TMR) response. However, initially it appeared that Sr(2)FeMoO(6) is an exclusive TMR material showing an unusual SVMR effect, while other well-known magnetoresistive compounds do not exhibit such behavior. Instead, in this present work, we show that SVMR is a generic feature of the extremely important class of the metallic, ferromagnetic double perovskite family as a whole. Our detailed magnetic study also offers a serious correction to our previous SVMR model, where the strong exchange coupling between the ferromagnetic core and the magnetically frustrated skin of each grain, generating the famous 'exchange bias' effect and consequently the 'valve' for SVMR, needs to be considered.