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1.
Nat Commun ; 15(1): 5348, 2024 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-38914556

RESUMO

Quantum fluctuations in low-dimensional systems and near quantum phase transitions have significant influences on material properties. Yet, it is difficult to experimentally gauge the strength and importance of quantum fluctuations. Here we provide a resonant inelastic x-ray scattering study of magnon excitations in Mott insulating cuprates. From the thin film of SrCuO2, single- and bi-magnon dispersions are derived. Using an effective Heisenberg Hamiltonian generated from the Hubbard model, we show that the single-magnon dispersion is only described satisfactorily when including significant quantum corrections stemming from magnon-magnon interactions. Comparative results on La2CuO4 indicate that quantum fluctuations are much stronger in SrCuO2 suggesting closer proximity to a magnetic quantum critical point. Monte Carlo calculations reveal that other magnetic orders may compete with the antiferromagnetic Néel order as the ground state. Our results indicate that SrCuO2-due to strong quantum fluctuations-is a unique starting point for the exploration of novel magnetic ground states.

2.
J Phys Condens Matter ; 36(31)2024 May 09.
Artigo em Inglês | MEDLINE | ID: mdl-38657622

RESUMO

It has been suggested that Ba3In2O6might be a high-Tcsuperconductor. Experimental investigation of the properties of Ba3In2O6was long inhibited by its instability in air. Recently epitaxial Ba3In2O6with a protective capping layer was demonstrated, which finally allows its electronic characterization. The optical bandgap of Ba3In2O6is determined to be 2.99 eV in-the (001) plane and 2.83 eV along thec-axis direction by spectroscopic ellipsometry. First-principles calculations were carried out, yielding a result in good agreement with the experimental value. Various dopants were explored to induce (super-)conductivity in this otherwise insulating material. NeitherA- norB-site doping proved successful. The underlying reason is predominately the formation of oxygen interstitials as revealed by scanning transmission electron microscopy and first-principles calculations. Additional efforts to induce superconductivity were investigated, including surface alkali doping, optical pumping, and hydrogen reduction. To probe liquid-ion gating, Ba3In2O6was successfully grown epitaxially on an epitaxial SrRuO3bottom electrode. So far none of these efforts induced superconductivity in Ba3In2O6,leaving the answer to the initial question of whether Ba3In2O6is a high-Tcsuperconductor to be 'no' thus far.

4.
Nat Mater ; 23(4): 486-491, 2024 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-38278983

RESUMO

A hallmark of many unconventional superconductors is the presence of many-body interactions that give rise to broken-symmetry states intertwined with superconductivity. Recent resonant soft X-ray scattering experiments report commensurate 3a0 charge density wave order in infinite-layer nickelates, which has important implications regarding the universal interplay between charge order and superconductivity in both cuprates and nickelates. Here we present X-ray scattering and spectroscopy measurements on a series of NdNiO2+x samples, which reveal that the signatures of charge density wave order are absent in fully reduced, single-phase NdNiO2. The 3a0 superlattice peak instead originates from a partially reduced impurity phase where excess apical oxygens form ordered rows with three-unit-cell periodicity. The absence of any observable charge density wave order in NdNiO2 highlights a crucial difference between the phase diagrams of cuprate and nickelate superconductors.

5.
Phys Rev Lett ; 129(4): 047001, 2022 Jul 22.
Artigo em Inglês | MEDLINE | ID: mdl-35938998

RESUMO

We use resonant inelastic x-ray scattering to probe the propagation of plasmons in the electron-doped cuprate superconductor Sr_{0.9}La_{0.1}CuO_{2}. We detect a plasmon gap of ∼120 meV at the two-dimensional Brillouin zone center, indicating that low-energy plasmons in Sr_{0.9}La_{0.1}CuO_{2} are not strictly acoustic. The plasmon dispersion, including the gap, is accurately captured by layered t-J-V model calculations. A similar analysis performed on recent resonant inelastic x-ray scattering data from other cuprates suggests that the plasmon gap is generic and its size is related to the magnitude of the interlayer hopping t_{z}. Our work signifies the three dimensionality of the charge dynamics in layered cuprates and provides a new method to determine t_{z}.

6.
Phys Rev Lett ; 128(11): 114801, 2022 Mar 18.
Artigo em Inglês | MEDLINE | ID: mdl-35363005

RESUMO

The properties of photoemission electron sources determine the ultimate performance of a wide class of electron accelerators and photon detectors. To date, all high-efficiency visible-light photocathode materials are either polycrystalline or exhibit intrinsic surface disorder, both of which limit emitted electron beam brightness. In this Letter, we demonstrate the synthesis of epitaxial thin films of Cs_{3}Sb on 3C-SiC (001) using molecular-beam epitaxy. Films as thin as 4 nm have quantum efficiencies exceeding 2% at 532 nm. We also find that epitaxial films have an order of magnitude larger quantum efficiency at 650 nm than comparable polycrystalline films on Si. Additionally, these films permit angle-resolved photoemission spectroscopy measurements of the electronic structure, which are found to be in good agreement with theory. Epitaxial films open the door to dramatic brightness enhancements via increased efficiency near threshold, reduced surface disorder, and the possibility of engineering new photoemission functionality at the level of single atomic layers.

7.
Nat Commun ; 12(1): 2757, 2021 May 12.
Artigo em Inglês | MEDLINE | ID: mdl-33980848

RESUMO

Magnetostrictive materials transduce magnetic and mechanical energies and when combined with piezoelectric elements, evoke magnetoelectric transduction for high-sensitivity magnetic field sensors and energy-efficient beyond-CMOS technologies. The dearth of ductile, rare-earth-free materials with high magnetostrictive coefficients motivates the discovery of superior materials. Fe1-xGax alloys are amongst the highest performing rare-earth-free magnetostrictive materials; however, magnetostriction becomes sharply suppressed beyond x = 19% due to the formation of a parasitic ordered intermetallic phase. Here, we harness epitaxy to extend the stability of the BCC Fe1-xGax alloy to gallium compositions as high as x = 30% and in so doing dramatically boost the magnetostriction by as much as 10x relative to the bulk and 2x larger than canonical rare-earth based magnetostrictors. A Fe1-xGax - [Pb(Mg1/3Nb2/3)O3]0.7-[PbTiO3]0.3 (PMN-PT) composite magnetoelectric shows robust 90° electrical switching of magnetic anisotropy and a converse magnetoelectric coefficient of 2.0 × 10-5 s m-1. When optimally scaled, this high coefficient implies stable switching at ~80 aJ per bit.

8.
Nat Commun ; 12(1): 59, 2021 Jan 04.
Artigo em Inglês | MEDLINE | ID: mdl-33397949

RESUMO

Superconductivity is among the most fascinating and well-studied quantum states of matter. Despite over 100 years of research, a detailed understanding of how features of the normal-state electronic structure determine superconducting properties has remained elusive. For instance, the ability to deterministically enhance the superconducting transition temperature by design, rather than by serendipity, has been a long sought-after goal in condensed matter physics and materials science, but achieving this objective may require new tools, techniques and approaches. Here, we report the transmutation of a normal metal into a superconductor through the application of epitaxial strain. We demonstrate that synthesizing RuO2 thin films on (110)-oriented TiO2 substrates enhances the density of states near the Fermi level, which stabilizes superconductivity under strain, and suggests that a promising strategy to create new transition-metal superconductors is to apply judiciously chosen anisotropic strains that redistribute carriers within the low-energy manifold of d orbitals.

9.
Phys Rev Lett ; 125(21): 217401, 2020 Nov 20.
Artigo em Inglês | MEDLINE | ID: mdl-33274990

RESUMO

SrRuO_{3}, a ferromagnet with an approximately 160 K Curie temperature, exhibits a T^{2}-dependent dc resistivity below ≈30 K. Nevertheless, previous optical studies in the infrared and terahertz range show non-Drude dynamics at low temperatures, which seem to contradict Fermi-liquid predictions. In this work, we measure the low-frequency THz range response of thin films with residual resistivity ratios, ρ_{300K}/ρ_{4K}≈74. At temperatures below 30 K, we find both a sharp zero frequency mode which has a width narrower than k_{B}T/ℏ as well as a broader zero frequency Lorentzian that has at least an order of magnitude larger scattering. Both features have temperature dependences consistent with a Fermi liquid with the wider feature explicitly showing a T^{2} scaling. Above 30 K, there is a crossover to a regime described by a single Drude peak that we believe arises from strong interband electron-electron scattering. Such two channel Drude transport sheds light on reports of the violation of Matthiessen's rule and extreme sensitivity to disorder in metallic ruthenates.

10.
Nat Commun ; 11(1): 2597, 2020 May 22.
Artigo em Inglês | MEDLINE | ID: mdl-32444617

RESUMO

The evolution of Sr2IrO4 upon carrier doping has been a subject of intense interest, due to its similarities to the parent cuprates, yet the intrinsic behaviour of Sr2IrO4 upon hole doping remains enigmatic. Here, we synthesize and investigate hole-doped Sr2-xKxIrO4 utilizing a combination of reactive oxide molecular-beam epitaxy, substitutional diffusion and in-situ angle-resolved photoemission spectroscopy. Upon hole doping, we observe the formation of a coherent, two-band Fermi surface, consisting of both hole pockets centred at (π, 0) and electron pockets centred at (π/2, π/2). In particular, the strong similarities between the Fermi surface topology and quasiparticle band structure of hole- and electron-doped Sr2IrO4 are striking given the different internal structure of doped electrons versus holes.

11.
Sci Rep ; 9(1): 19158, 2019 Dec 16.
Artigo em Inglês | MEDLINE | ID: mdl-31844071

RESUMO

Strain-coupled magnetoelectric (ME) phenomena in piezoelectric/ferromagnetic thin-film bilayers are a promising paradigm for sensors and information storage devices, where strain manipulates the magnetization of the ferromagnetic film. In-plane magnetization rotation with an electric field across the film thickness has been challenging due to the large reduction of in-plane piezoelectric strain by substrate clamping, and in two-terminal devices, the requirement of anisotropic in-plane strain. Here we show that these limitations can be overcome by designing the piezoelectric strain tensor using the boundary interaction between biased and unbiased piezoelectric. We fabricated 500 nm thick, (001) oriented [Pb(Mg1/3Nb2/3)O3]0.7-[PbTiO3]0.3 (PMN-PT) unclamped piezoelectric membranes with ferromagnetic Ni overlayers. Guided by analytical and numerical continuum elastic calculations, we designed and fabricated two-terminal devices exhibiting electric field-driven Ni magnetization rotation. We develop a method that can apply designed strain patterns to many other materials systems to control properties such as superconductivity, band topology, conductivity, and optical response.

12.
J Phys Condens Matter ; 31(44): 445601, 2019 Nov 06.
Artigo em Inglês | MEDLINE | ID: mdl-31295728

RESUMO

We have studied the low temperature electrical transport properties of La x Sr1-x CuO2 thin films grown by oxide molecular beam epitaxy on (1 1 0) GdScO3 and TbScO3 substrates. The transmission electron microscopy measurements and the x-ray diffraction analysis confirmed the epitaxy of the obtained films and the study of their normal state transport properties, removing the ambiguity regarding the truly conducting layer, allowed to highlight the presence of a robust hidden Fermi liquid charge transport in the low temperature properties of infinite layer electron doped cuprate superconductors. These results are in agreement with recent observations performed in other p  and n doped cuprate materials and point toward a general description of the superconducting and normal state properties in these compounds.

13.
Nature ; 568(7752): 368-372, 2019 04.
Artigo em Inglês | MEDLINE | ID: mdl-30996320

RESUMO

Complex topological configurations are fertile ground for exploring emergent phenomena and exotic phases in condensed-matter physics. For example, the recent discovery of polarization vortices and their associated complex-phase coexistence and response under applied electric fields in superlattices of (PbTiO3)n/(SrTiO3)n suggests the presence of a complex, multi-dimensional system capable of interesting physical responses, such as chirality, negative capacitance and large piezo-electric responses1-3. Here, by varying epitaxial constraints, we discover room-temperature polar-skyrmion bubbles in a lead titanate layer confined by strontium titanate layers, which are imaged by atomic-resolution scanning transmission electron microscopy. Phase-field modelling and second-principles calculations reveal that the polar-skyrmion bubbles have a skyrmion number of +1, and resonant soft-X-ray diffraction experiments show circular dichroism, confirming chirality. Such nanometre-scale polar-skyrmion bubbles are the electric analogues of magnetic skyrmions, and could contribute to the advancement of ferroelectrics towards functionalities incorporating emergent chirality and electrically controllable negative capacitance.

14.
Nat Commun ; 9(1): 2965, 2018 07 27.
Artigo em Inglês | MEDLINE | ID: mdl-30054461

RESUMO

Creating oxide interfaces with precise chemical specificity at the atomic layer level is desired for the engineering of quantum phases and electronic applications, but highly challenging, owing partially to the lack of in situ tools to monitor the chemical composition and completeness of the surface layer during growth. Here we report the in situ observation of atomic layer-by-layer inner potential variations by analysing the Kikuchi lines during epitaxial growth of strontium titanate, providing a powerful real-time technique to monitor and control the chemical composition during growth. A model combining the effects of mean inner potential and step edge density (roughness) reveals the underlying mechanism of the complex and previously not well-understood reflection high-energy electron diffraction oscillations observed in the shuttered growth of oxide films. General rules are proposed to guide the synthesis of atomically and chemically sharp oxide interfaces, opening up vast opportunities for the exploration of intriguing quantum phenomena at oxide interfaces.

15.
Sci Rep ; 7(1): 15460, 2017 11 13.
Artigo em Inglês | MEDLINE | ID: mdl-29133957

RESUMO

The ability to control a magnetic phase with an electric field is of great current interest for a variety of low power electronics in which the magnetic state is used either for information storage or logic operations. Over the past several years, there has been a considerable amount of research on pathways to control the direction of magnetization with an electric field. More recently, an alternative pathway involving the change of the magnetic state (ferromagnet to antiferromagnet) has been proposed. In this paper, we demonstrate electric field control of the Anomalous Hall Transport in a metamagnetic FeRh thin film, accompanying an antiferromagnet (AFM) to ferromagnet (FM) phase transition. This approach provides us with a pathway to "hide" or "reveal" a given ferromagnetic region at zero magnetic field. By converting the AFM phase into the FM phase, the stray field, and hence sensitivity to external fields, is decreased or eliminated. Using detailed structural analyses of FeRh films of varying crystalline quality and chemical order, we relate the direct nanoscale origins of this memory effect to site disorder as well as variations of the net magnetic anisotropy of FM nuclei. Our work opens pathways toward a new generation of antiferromagnetic - ferromagnetic interactions for spintronics.

16.
Nat Mater ; 16(6): 622-627, 2017 06.
Artigo em Inglês | MEDLINE | ID: mdl-28319611

RESUMO

Ferroelectric domain walls hold great promise as functional two-dimensional materials because of their unusual electronic properties. Particularly intriguing are the so-called charged walls where a polarity mismatch causes local, diverging electrostatic potentials requiring charge compensation and hence a change in the electronic structure. These walls can exhibit significantly enhanced conductivity and serve as a circuit path. The development of all-domain-wall devices, however, also requires walls with controllable output to emulate electronic nano-components such as diodes and transistors. Here we demonstrate electric-field control of the electronic transport at ferroelectric domain walls. We reversibly switch from resistive to conductive behaviour at charged walls in semiconducting ErMnO3. We relate the transition to the formation-and eventual activation-of an inversion layer that acts as the channel for the charge transport. The findings provide new insight into the domain-wall physics in ferroelectrics and foreshadow the possibility to design elementary digital devices for all-domain-wall circuitry.

17.
J Phys Condens Matter ; 29(10): 105401, 2017 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-28075333

RESUMO

Magnetic resonance spectra of EuTiO3 in both bulk and thin film form were taken at temperatures from 3-350 K and microwave frequencies from 9.2-9.8 and 34 GHz. In the paramagnetic phase, magnetic resonance spectra are determined by magnetic dipole and exchange interactions between Eu2+ spins. In the film, a large contribution arises from the demagnetization field. From detailed analysis of the linewidth and its temperature dependence, the parameters of spin-spin interactions were determined: the exchange frequency is 10.5 GHz and the estimated critical exponent of the spin correlation length is ≈0.4. In the bulk samples, the spectra exhibited a distinct minimum in the linewidth at the Néel temperature, T N ≈ 5.5 K, while the resonance field practically does not change even on cooling below T N. This is indicative of a small magnetic anisotropy ~320 G in the antiferromagnetic phase. In the film, the magnetic resonance spectrum is split below T N into several components due to excitation of the magnetostatic modes, corresponding to a non-uniform precession of magnetization. Moreover, the film was observed to degrade over two years. This was manifested by an increase of defects and a change in the domain structure. The saturated magnetization in the film, estimated from the magnetic resonance spectrum, was about 900 emu cm-3 or 5.5 µ B/unit cell at T = 3.5 K.

18.
Phys Rev Lett ; 116(19): 197003, 2016 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-27232037

RESUMO

Here we demonstrate how the Fermi surface topology and quantum many-body interactions can be manipulated via epitaxial strain in the spin-triplet superconductor Sr_{2}RuO_{4} and its isoelectronic counterpart Ba_{2}RuO_{4} using oxide molecular beam epitaxy, in situ angle-resolved photoemission spectroscopy, and transport measurements. Near the topological transition of the γ Fermi surface sheet, we observe clear signatures of critical fluctuations, while the quasiparticle mass enhancement is found to increase rapidly and monotonically with increasing Ru-O bond distance. Our work demonstrates the possibilities for using epitaxial strain as a disorder-free means of manipulating emergent properties, many-body interactions, and potentially the superconductivity in correlated materials.

19.
Phys Rev Lett ; 116(2): 027602, 2016 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-26824566

RESUMO

We have directly measured the band gap renormalization associated with the Moss-Burstein shift in the perovskite transparent conducting oxide (TCO), La-doped BaSnO_{3}, using hard x-ray photoelectron spectroscopy. We determine that the band gap renormalization is almost entirely associated with the evolution of the conduction band. Our experimental results are supported by hybrid density functional theory supercell calculations. We determine that unlike conventional TCOs where interactions with the dopant orbitals are important, the band gap renormalization in La-BaSnO_{3} is driven purely by electrostatic interactions.

20.
Phys Rev Lett ; 115(9): 096405, 2015 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-26371669

RESUMO

We report the formation and observation of an electron liquid in Sr(2-x)La(x)TiO4, the quasi-two-dimensional counterpart of SrTiO3, through reactive molecular-beam epitaxy and in situ angle-resolved photoemission spectroscopy. The lowest lying states are found to be comprised of Ti 3d_{xy} orbitals, analogous to the LaAlO3/SrTiO3 interface and exhibit unusually broad features characterized by quantized energy levels and a reduced Luttinger volume. Using model calculations, we explain these characteristics through an interplay of disorder and electron-phonon coupling acting cooperatively at similar energy scales, which provides a possible mechanism for explaining the low free carrier concentrations observed at various oxide heterostructures such as the LaAlO3/SrTiO3 interface.

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