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Feizhou He

Publications and source records attributed to Feizhou He.

At least 19 recordsLinked to original sources

Discovery of an electronic crystal in a cuprate Mott insulator

Copper oxide high temperature superconductors universally exhibit multiple forms of electronically ordered phases that break the native translational symmetry of the CuO2 planes. The interplay between these orders and the superconducting ground state, as well as how they arise through doping a Mott insulator, is essential to decode the mechanisms of high-temperature superconductivity. Over the years, various forms of electronic liquid crystal phases including charge/spin stripes and incommensurate charge-density-waves (CDWs) were found to emerge out of a correlated metallic ground state in underdoped cuprates. Early theoretical studies also predicted the emergence of a Coulomb-frustrated 'charge crystal' phase in the very lightly-doped, insulating limit of the CuO2 planes. Here, we use resonant X-ray scattering, electron transport, and muon spin rotation measurements to fully resolve the electronic and magnetic ground state and search for signatures of charge order in very lightly hole-doped cuprates from the RBa2Cu3O7-d family (RBCO; R: Y or rare earth). X-ray scattering data from RBCO films reveal a breaking of translational symmetry more pervasive than was previously known, extending down to the Mott limit. The ordering vector of this charge crystal state is linearly connected to the charge-density-waves of underdoped RBCO, suggesting that the former phase is a precursor to the latter as hole doping is increased. Most importantly, the coexistence of charge and spin order in RBCO suggests that this electronic symmetry-breaking state is common to the CuO2 planes in the very lightly-doped regime. These findings bridge the gap between the Mott insulating state and the underdoped metallic state and underscore the prominent role of Coulomb-frustrated electronic phase separation among all cuprates.

cond-mat.str-el

Spin-orbit phase behaviors of Na2Co2TeO6 at low temperatures

We present a comprehensive study of single crystals of Na2Co2TeO6, a putative Kitaev honeycomb magnet, focusing on its low-temperature phase behaviors. A new thermal phase transition is identified at 31.0 K, below which the system develops a two-dimensional (2D) long-range magnetic order. This order precedes the well-known 3D order below 26.7 K, and is likely driven by strongly anisotropic interactions. Surprisingly, excitations from the 3D order do not support the order's commonly accepted "zigzag" nature, and are instead consistent with a "triple-q" description. The 3D order exerts a fundamental feedback on high-energy excitations that likely involve orbital degrees of freedom, and it remains highly frustrated until a much lower temperature is reached. These findings render Na2Co2TeO6 a spin-orbit entangled frustrated magnet that hosts very rich physics.

cond-mat.str-el

Strain induced stabilization of a static Jahn-Teller distortion in the O$^*$-phase of La$_{7/8}$Sr$_{1/8}$MnO$_3$

At room temperature, bulk La$_{7/8}$Sr$_{1/8}$MnO$_3$ is in the dynamic Jahn--Teller O$^*$ phase, but undergoes a transition to a static, magnetically ordered Jahn--Teller phase at lower temperatures. Here we study a $6$ unit cells thin film of this compound grown on SrTiO$_3$, resulting in small compressive strain due to a lattice mismatch of $\lesssim 0.2\%$. We combine X-ray absorption spectroscopy with multiplet ligand field theory to study the local electronic and magnetic properties of Mn in the film. We determine the Mn $d_{3z^2-r^2}$ orbital to be $0.13\;\text{eV}$ lower in energy than the $d_{x^2-y^2}$, which is a disproportionately large splitting given the small degree of compressive strain. We interpret this as resulting from the strain providing a preferential orientation for the MnO$_6$ octahedra, which are strongly susceptible to such a deformation in the vicinity of the phase transition. Hence, they collectively elongate along the $c$ axis into a static Jahn--Teller arrangement. Furthermore, we demonstrate the strongly covalent character of La$_{7/8}$Sr$_{1/8}$MnO$_3$, with a contribution of nearly $50\%$ of the one-ligand-hole configuration $d^{5} \underline{L}^1$ to the ground state wavefunction. Finally, we find the system to be in a high-spin configuration, with the projection of the local magnetic moment on the quantization axis being about $3.7\;μ_{\text{B}}/\text{Mn}$. We show, however, that the system is close to a high-spin--low-spin transition, which might be triggered by crystal field effects.

cond-mat.str-el

Sudden collapse of magnetic order in oxygen deficient nickelate films

Oxygen vacancies play a crucial role in the control of the electronic, magnetic, ionic, and transport properties of functional oxide perovskites. Rare earth nickelates (RENiO$_{3-x}$) have emerged over the years as a rich platform to study the interplay between the lattice, the electronic structure, and ordered magnetism. In this study, we investigate the evolution of the electronic and magnetic structure in thin films of RENiO$_{3-x}$, using a combination of X-ray absorption spectroscopy and imaging, resonant X-ray scattering, and extended multiplet ligand field theory modeling. We find that oxygen vacancies modify the electronic configuration within the Ni-O orbital manifolds, leading to a dramatic evolution of long-range electronic transport pathways despite the absence of nanoscale phase separation. Remarkably, magnetism is robust to substantial levels of carrier doping, and only a moderate weakening of the $(1/4, 1/4, 1/4)_{pc}$ antiferromagnetic order parameter is observed, whereas the magnetic transition temperature is largely unchanged. Only at a certain point long-range magnetism is abruptly erased without an accompanying structural transition. We propose the progressive disruption of the 3D magnetic superexchange pathways upon introduction of point defects as the mechanism behind the sudden collapse of magnetic order in oxygen-deficient nickelates. Our work demonstrates that, unlike most other oxides, ordered magnetism in RENiO$_{3-x}$ is mostly insensitive to carrier doping. The sudden collapse of ordered magnetism upon oxygen removal may provide a new mechanism for solid-state magneto-ionic switching and new applications in antiferromagnetic spintronics.

cond-mat.str-el

Doping-dependent phonon anomaly and charge-order phenomena in the HgBa$_{2}$CuO$_{4+δ}$ and HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$

Using resonant X-ray diffraction and Raman spectroscopy, we study charge correlations and lattice dynamics in two model cuprates, HgBa$_{2}$CuO$_{4+δ}$ and HgBa$_{2}$CaCu$_{2}$O$_{6+δ}$. We observe a maximum of the characteristic charge order temperature around the same hole concentration ($p \approx 0.09$) in both compounds, and concomitant pronounced anomalies in the lattice dynamics that involve the motion of atoms in and/or adjacent to the CuO$_2$ layers. These anomalies are already present at room temperature, and therefore precede the formation of the static charge correlations, and we attribute them to an instability of the CuO$_2$ layers. Our finding implies that the charge order in the cuprates is an emergent phenomenon, driven by a fundamental variation in both lattice and electronic properties as a function of doping.

cond-mat.supr-con

Epitaxial Growth of Perovskite SrBiO$_3$ Film on SrTiO$_3$ by Oxide Molecular Beam Epitaxy

Hole-doped perovskite bismuthates such as Ba$_{1-x}$K$_x$BiO$_3$ and Sr$_{1-x}$K$_x$BiO$_3$ are well-known bismuth-based oxide high-transition-temperature superconductors. Reported thin bismuthate films show relatively low quality, likely due to their large lattice mismatch with the substrate and a low sticking coefficient of Bi at high temperatures. Here, we report the successful epitaxial thin film growth of the parent compound strontium bismuthate SrBiO$_3$ on SrO-terminated SrTiO$_3$ (001) substrates by molecular beam epitaxy. Two different growth methods, high-temperature co-deposition or recrystallization cycles of low-temperature deposition plus high-temperature annealing, are developed to improve the epitaxial growth. SrBiO$_3$ has a pseudocubic lattice constant $\sim$4.25 Å, an $\sim$8.8\% lattice mismatch on SrTiO$_3$ substrate, leading to a large strain in the first few unit cells. Films thicker than 6 unit cells prepared by both methods are fully relaxed to bulk lattice constant and have similar quality. Compared to high-temperature co-deposition, the recrystallization method can produce higher quality 1-6 unit cell films that are coherently or partially strained. Photoemission experiments reveal the bonding and antibonding states close to the Fermi level due to Bi and O hybridization, in good agreement with density functional theory calculations. This work provides general guidance to the synthesis of high-quality perovskite bismuthate films.

cond-mat.supr-con

Evolution of charge order topology across a magnetic phase transition in cuprate superconductors

Charge order is now accepted as an integral constituent of cuprate high-temperature superconductors, one that is intimately related to other instabilities in the phase diagram including antiferromagnetism and superconductivity. Unlike nesting-induced Peierls-like density waves, the charge correlations in the CuO2 planes have been predicted to display a rich momentum space topology depending on the detailed fermiology of the system. However, to date charge order has only been observed along the high-symmetry Cu-O bond directions. Here, using resonant soft X-ray scattering, we investigate the evolution of the full momentum space topology of charge correlations in Ln2CuO4 (Ln=Nd, Pr) as a function of intrinsic electron doping. We report that, upon electron doping the parent Mott insulator, charge correlations first emerge in a hitherto-unobserved form, with full (Cinf) rotational symmetry in momentum-space. At higher doping levels, the orientation of charge correlations is sharply locked to the Cu-O bond high-symmetry directions, restoring a more conventional bidirectional charge order with enhanced correlation lengths. Through charge susceptibility calculations, we closely reproduce the drastic evolution in the topology of charge correlations across an antiferromagnetic quantum phase transition, highlighting the interplay between spin and charge degrees of freedom in electron-doped cuprates. Finally, using the established link between charge correlations and the underlying fermiology, we propose a revised phase diagram of Ln2CuO4 with a superconducting region extending toward the Mott limit.

cond-mat.str-el

Complex magnetic order in nickelate slabs

Magnetic ordering phenomena have a profound influence on the macroscopic properties of correlated-electron materials, but their realistic prediction remains a formidable challenge. An archetypical example is the ternary nickel oxide system RNiO3 (R = rare earth), where the period-four magnetic order with proposals of collinear and non-collinear structures and the amplitude of magnetic moments on different Ni sublattices have been subjects of debate for decades. Here we introduce an elementary model system - NdNiO3 slabs embedded in a non-magnetic NdGaO3 matrix - and use polarized resonant x-ray scattering (RXS) to show that both collinear and non-collinear magnetic structures can be realized, depending on the slab thickness. The crossover between both spin structures is correctly predicted by density functional theory and can be qualitatively understood in a low-energy spin model. We further demonstrate that the amplitude ratio of magnetic moments in neighboring NiO6 octahedra can be accurately determined by RXS in combination with a correlated double cluster model. Targeted synthesis of model systems with controlled thickness and synergistic application of polarized RXS and ab-initio theory thus provide new perspectives for research on complex magnetism, in analogy to two-dimensional materials created by exfoliation.

cond-mat.str-el

Intertwined Spin and Orbital Density Waves in MnP Uncovered by Resonant Soft X-ray Scattering

Unconventional superconductors are often characterized by numerous competing and even intertwined orders in their phase diagrams. In particular, the electronic nematic phases, which spontaneously break rotational symmetry and often simultaneously involve spin, charge and/or orbital orders, appear conspicuously in both the cuprate and iron-based superconductors. The fluctuations associated with these phases may provide the exotic pairing glue that underlies their high-temperature superconductivity. Helimagnet MnP, the first Mn-based superconductor under pressure, lacks high rotational symmetry. However our resonant soft X-ray scattering (RSXS) experiment discovers novel helical orbital density wave (ODW) orders in this three-dimensional, low-symmetry system, and reveals intertwined ordering phenomena in unprecedented detail. In particular, a ODW forms with half the period of the spin order and fully develops slightly above the spin ordering temperature, their domains develop simultaneously, yet the spin order domains are larger than those of the ODW, and they cooperatively produce another ODW with 1/3 the period of the spin order. These observations provide a comprehensive picture of the intricate interplay between spin and orbital orders in correlated materials, and they suggest that nematic-like physics ubiquitously exists beyond two-dimensional and high-symmetry systems, and the superconducting mechanism of MnP is likely analogous to those of cuprate and iron-based superconductors.

cond-mat.supr-con

Chemical and valence reconstruction at the surface of SmB6 revealed with resonant soft x-ray reflectometry

Samarium hexaboride (SmB$_6$), a Kondo insulator with mixed valence, has recently attracted much attention as a possible host for correlated topological surface states. Here, we use a combination of x-ray absorption and reflectometry techniques, backed up with a theoretical model for the resonant $M_{4,5}$ absorption edge of Sm and photoemission data, to establish laterally averaged chemical and valence depth profiles at the surface of SmB$_6$. We show that upon cleaving, the highly polar (001) surface of SmB$_6$ undergoes substantial chemical and valence reconstruction, resulting in boron termination and a Sm$^{3+}$ dominated sub-surface region. Whereas at room temperature, the reconstruction occurs on a time scale of less than two hours, it takes about 24 hours below 50 K. The boron termination is eventually established, irrespective of the initial termination. Our findings reconcile earlier depth resolved photoemission and scanning tunneling spectroscopy studies performed at different temperatures and are important for better control of polarity and, as a consequence, surface states in this system.

cond-mat.str-el

Orbital order and fluctuations in the two-leg ladder materials BaFe$_2X_3$ ($X$ = S and Se) and CsFe$_2$Se$_3$

The electronic structure of BaFe$_2X_3$ ($X$ = S and Se) and CsFe$_2$Se$_3$ in which two-leg ladders are formed by the Fe sites are studied by means of x-ray absorption and resonant inelastic x-ray scattering spectroscopy. The x-ray absorption spectra at the Fe L edges for BaFe$_2X_3$ exhibit two components, indicating that itinerant and localized Fe 3$d$ sites coexist. Substantial x-ray linear dichroism (XLD) is observed in polarization dependent spectra, indicating the existence of orbital order or fluctuation in the Fe-ladder even above the Néel temperature $T_N$. Direct exchange interaction along the legs of the Fe-ladder stabilizes the orbital and antiferromagnetic orders in BaFe$_2$S$_3$, while the ferromagnetic molecular orbitals are realized between the rungs in CsFe$_2$Se$_3$.

cond-mat.supr-con

Quasiparticle interference of heavy fermions in resonant X-ray scattering

Resonant X-ray scattering (RXS) has recently become an increasingly important tool for the study of ordering phenomena in correlated electron systems. Yet, the interpretation of the RXS experiments remains theoretically challenging due to the complexity of the RXS cross-section. Central to this debate is the recent proposal that impurity-induced Friedel oscillations, akin to quasiparticle interference signals observed with the scanning tunneling microscope (STM), can lead to scattering peaks in the RXS experiments. The possibility that quasiparticle properties can be probed in RXS measurements opens up a new avenue to study the bulk band structure of materials with the orbital and element selectivity provided by RXS. Here, we test these ideas by combining RXS and STM measurements of the heavy fermion compound CeMIn$_5$ (M = Co, Rh). Temperature and doping dependent RXS measurements at the Ce-M$_4$ edge show a broad scattering enhancement that correlates with the appearance of heavy f-electron bands in these compounds. The scattering enhancement is consistent with the measured quasiparticle interference signal in the STM measurements, indicating that quasiparticle interference can be probed through the momentum distribution of RXS signals. Overall, our experiments demonstrate new opportunities for studies of correlated electronic systems using the RXS technique.

cond-mat.str-el

Charge ordering in the electron-doped superconductor Nd2-xCexCuO4

In cuprate high-temperature superconductors, an antiferromagnetic Mott insulating state can be destabilized toward unconventional superconductivity by either hole- or electron-doping. In addition to these two electronic phases there is now a copious amount of evidence that supports the presence of a charge ordering (CO) instability competing with superconductivity inside the pseudogap state of the hole-doped (p-type) cuprates, but so far there has been no evidence of a similar CO in their electron-doped (n-type) counterparts. Here we report resonant x-ray scattering (RXS) measurements which demonstrate the presence of charge ordering in the n-type cuprate Nd2-xCexCuO4 near optimal doping. Remarkably we find that the CO in Nd2-xCexCuO4 occurs with similar periodicity, and along the same direction, as the CO in p-type cuprates. However, in contrast to the latter, the CO onset in Nd2-xCexCuO4 is higher than the pseudogap temperature, and is actually in the same temperature range where antiferromagnetic fluctuations are first detected -- thereby showing that CO and antiferromagnetic fluctuations are likely coupled in n-type cuprates. Overall our discovery uncovers a missing piece of the cuprate phase diagram and opens a parallel path to the study of CO and its relationship to other phenomena, such as antiferromagnetism (AF) and high-temperature superconductivity.

cond-mat.supr-con

Strain-Induced Spin States in Atomically Ordered Cobaltites

Epitaxial strain imposed in complex oxide thin films by heteroepitaxy is recognized as a powerful tool for identifying new properties and exploring the vast potential of materials performance. A particular example is LaCoO3, a zero spin, nonmagnetic material in the bulk, whose strong ferromagnetism in a thin film remains enigmatic despite a decade of intense research. Here, we use scanning transmission electron microscopy complemented by X-ray and optical spectroscopy to study LaCoO3 epitaxial thin films under different strain states. We observed an unconventional strain relaxation behavior resulting in stripe-like, lattice modulated patterns, which did not involve uncontrolled misfit dislocations or other defects. The modulation entails the formation of ferromagnetically ordered sheets comprising intermediate or high spin Co3+, thus offering an unambiguous description for the exotic magnetism found in epitaxially strained LaCoO3 films. This observation provides a novel route to tailoring the electronic and magnetic properties of functional oxide heterostructures.

cond-mat.mtrl-sci

Direct evidence for the suppression of charge stripes in epitaxial La$_{1.67}$Sr$_{0.33}$NiO$_4$ thin films

We have successfully grown epitaxial La$_{1.67}$Sr$_{0.33}$NiO$_4$ films with a small crystalline mosaic using pulsed laser deposition. With synchrotron radiation, the x-ray diffraction peaks associated with charge stripes have been successfully observed for relatively thick films. Anomalies due to the charge-ordering transition have been examined using four-point probe resistivity measurements. X-ray scattering provides direct evidence for suppression of the stripe phase in thin samples; the phase disappears for film thicknesses $\leqslant$ 2600 ~Å. The suppression appears to be a result of shrinking the stripe phase domains. This may reflect the stripe phase progressing from nematic to isotropic.

cond-mat.str-el

Lattice Relaxation in Epitaxial BaTiO$_3$ Thin Films

We have investigated the out-of-plane lattice relaxation related to the ferroelectric transitions in epitaxial BaTiO$_3$ (BTO) films using synchrotron X-ray diffraction. Under either compressive strain or tensile strain, there is evidence for two structural phase transitions as a function of temperature. The transition temperature $T_C$ is a strong function of strain, which can be as much as 100 K above the corresponding $T_C$ in bulk. Under compressive strain, the tetragonality of BTO unit cell implies that the polarization of the first ferroelectric phase is out-of-plane, while under tensile strain, the polarization is in-plane. The transitions at lower temperature may correspond to the $aa\to r$ or $c\to r$ transitions, following the notations by Pertsev \textit{et al}. The orientations of the domains are consistent with theoretical predictions.

cond-mat.mtrl-sci

Strain phase diagram and domain orientation in SrTiO$_3$ thin films

SrTiO$_3$ thin films were used as a model system to study the effects of strain and epitaxial constraint on structural phase transitions of perovskite films. The basic phenomena revealed will apply to a variety of important structural transitions including the ferroelectric transition. Highly strained SrTiO$_3$ films were grown on different substrates, providing both compressive and tensile strain. The measured strain-temperature phase diagram is qualitatively consistent with theory, however the increase in the phase transition temperature is much larger than predicted. Due to the epitaxial strain and substrate clamping, the SrTiO$_3$ lattice is tetragonal at all temperatures. The phase transitions involve only changes in internal symmetry. The low temperature phase under tensile strain has a unique structure with orthorhombic $Cmcm$ space group but a tetragonal lattice, an interesting consequence of epitaxial constraint.

cond-mat.other

Structural phase transitions in epitaxial perovskite films

Three different film systems have been systematically investigated to understand the effects of strain and substrate constraint on the phase transitions of perovskite films. In SrTiO$_3$ films, the phase transition temperature T$_C$ was determined by monitoring the superlattice peaks associated with rotations of TiO$_6$ octahedra. It is found that T$_C$ depends on both SrTiO$_3$ film thickness and SrRuO$_3$ buffer layer thickness. However, lattice parameter measurements showed no sign of the phase transitions, indicating that the tetragonality of the SrTiO$_3$ unit cells was no longer a good order parameter. This signals a change in the nature of this phase transition, the internal degree of freedom is decoupled from the external degree of freedom. The phase transitions occur even without lattice relaxation through domain formation. In NdNiO$_3$ thin films, it is found that the in-plane lattice parameters were clamped by the substrate, while out-of-plane lattice constant varied to accommodate the volume change across the phase transition. This shows that substrate constraint is an important parameter for epitaxial film systems, and is responsible for the suppression of external structural change in SrTiO$_3$ and NdNiO$_3$ films. However, in SrRuO$_3$ films we observed domain formation at elevated temperature through x-ray reciprocal space mapping. This indicated that internal strain energy within films also played an important role, and may dominate in some film systems. The final strain states within epitaxial films were the result of competition between multiple mechanisms and may not be described by a single parameter.

cond-mat.other