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Claudio Mazzoli

Publications and source records attributed to Claudio Mazzoli.

18 recordsLinked to original sources

Excitations across the equilibrium and photoinduced `hidden' states of magnetoresistive manganites

"Hidden" phases, generated using ultrafast laser pulses (few hundred femtoseconds), with properties distinct from thermodynamic equilibrium, are appealing for technologies because they can be long-lived, with lifetimes of hours or weeks, and reversible with temperature sweeping or extra pulses. In this regard, La$_{2/3}$Ca$_{1/3}$MnO$_3$ (LCMO) stands out due to its tunability through epitaxial strain, which can drive the bulk ferromagnetic metal (FMM) into an antiferromagnetic insulator (AFI), and its susceptibility to photo-induced transitions. Indeed, AFI LCMO displays a long-lived photo-induced transition into a putative 'hidden' phase whose exact nature and excitations are still largely unknown. Here, we combine ultrafast photo-excitation in the near infrared with in situ transport, x-ray absorption (XAS), and Resonant Inelastic X-ray Scattering (RIXS) to investigate the excitations (polarons, phonons, and orbital) of the photo-excited phase of LCMO and contrast them with the thermodynamic phases achieved through strain and temperature. In the thermodynamic regime, we establish the correlation between polarons and transport, placing them in the 'strong coupling' regime of the Holstein model. Upon photo-excitation of LCMO-AFI, we uncover a long-lived phase characterized by the softening of the polaron excitations, the partial suppression of the Jahn-Teller distortion, and nearly unchanged phonons, showing the emergence of a photo-excited state absent in the equilibrium phase diagram. Finally, by varying temperature, epitaxial strain, and photo-excitation fluence, we construct a polaron phase diagram and identify the key spectroscopic signatures of each phase. Our laser-RIXS approach establishes a versatile platform for exploring photo-induced 'hidden' phases in quantum materials in non-stroboscopic conditions.

cond-mat.str-el

Manipulation of the orbital angular momentum of soft x-ray beams by consecutive diffractive optics

Production and manipulation of orbital angular momentum (OAM) of coherent soft x-ray beams is demonstrated utilizing consecutive diffractive optics. OAM addition is observed upon passing the beam through consecutive fork gratings. The OAM of the beam was found to be decoupled from its spin angular momentum (SAM). Practical implementation of angular momentum control by consecutive devices in the x-ray regime opens new experimental opportunities, such as direct measurement of OAM beams without resorting to phase sensitive techniques, including holography. OAM analyzers utilizing fork gratings can be used to characterize the beams produced by synchrotron and free electron lasers sources; they can also be used in scattering experiments.

physics.optics

Structural origin of resonant diffraction in RuO$_2$

We report Ru L$_3$-edge resonant X-ray diffraction studies on single crystal and (001) epitaxial films of RuO$_2$. We investigate the distinct $\mathbf{Q} = (100)$ and $(001)$ reflections as a function of incident energy, azimuthal angle, and temperature. The results show that the observed resonant diffraction in RuO$_2$ is fully consistent with a resonant charge anisotropy signal of structural origin permitted by the parent (non-magnetic) rutile $P4_2/mnm$ space group. These results significantly constrain the magnetic contribution to the resonant diffraction signal and indicate the unlikely existence of $\mathbf{k} = 0$ antiferromagnetic order in RuO$_2$.

cond-mat.str-el

Time-dependent correlations of the Edwards-Anderson order parameter above the spin-glass transition

In 1975 Edwards and Anderson introduced a new paradigm that interacting quenched systems, such as a spin-glass, have a phase transition in which long time memory of spatial patterns is realized without spatial correlations. We show here that the information about the time-dependent correlations above the spin-glass transition are embedded in the four spin correlations of the intensity of speckle pattern. This encodes the spin-orientation memory and can be measured by the technique of resonant magnetic x-ray photon correlation spectroscopy (RM- XPCS). We have implemented this method to observe and accurately characterize the critical slowing down of the spin orientation fluctuations in the classic metallic spin glass alloy $Cu_{1-x}{Mn}_x$ over time scales of ${2}$ sec. to $2 \times 10^{\mathbf{4}}$ secs. Remarkably the divergence of the correlation time as a function of temperature is consistent with the Vogel-Vulcher law, universally used to characterize the viscous relaxation time in structural glasses. Our method also opens the way for studying phase transitions in systems such as spin ices, quantum spin liquids, the structural glass transition, as well as possibly provide new perspectives on the multifarious problems in which spin-glass concepts have found applications.

cond-mat.dis-nn

Photon correlation spectroscopy with heterodyne mixing based on soft-x-ray magnetic circular dichroism

Many magnetic equilibrium states and phase transitions are characterized by fluctuations. Such magnetic fluctuation can in principle be detected with scattering-based x-ray photon correlation spectroscopy (XPCS). However, in the established approach of XPCS, the magnetic scattering signal is quadratic in the magnetic scattering cross section, which results not only in often prohibitively small signals but also in a fundamental inability to detect negative correlations (anticorrelations). Here, we propose to exploit the possibility of heterodyne mixing of the magnetic signal with static charge scattering to reconstruct the first-order (linear) magnetic correlation function. We show that the first-order magnetic scattering signal reconstructed from heterodyne scattering now directly represents the underlying magnetization texture. Moreover, we suggest a practical implementation based on an absorption mask rigidly connected to the sample, which not only produces a static charge scattering signal but also eliminates the problem of drift-induced artificial decay of the correlation functions. Our method thereby significantly broadens the range of scientific questions accessible by magnetic x-ray photon correlation spectroscopy.

cond-mat.mtrl-sci

Site-specific electronic and magnetic excitations of the skyrmion material Cu$_2$OSeO$_3$

The manifestation of skyrmions in the Mott-insulator Cu$_2$OSeO$_3$ originates from a delicate balance between magnetic and electronic energy scales. As a result of these intertwined couplings, the two symmetry-inequivalent magnetic ions, Cu-I and Cu-II, bond into a spin S=1 entangled tetrahedron. However, conceptualizing the unconventional properties of this material and the energy of the competing interactions is a challenging task due the complexity of this system. Here we combine X-ray Absorption Spectroscopy and Resonant Inelastic X-ray Scattering to uncover the electronic and magnetic excitations of Cu$_2$OSeO$_3$ with site-specificity. We quantify the energies of the 3d crystal-field splitting for both Cu-I and Cu-II, fundamental to optimize model Hamiltonians. Additionally, we unveil a site-specific magnetic mode, indicating that individual spin character is preserved within the entangled-tetrahedron picture. Our results thus provide experimental constraint for validating theories that describe the interactions of Cu$_2$OSeO$_3$, highlighting the site-selective capabilities of resonant spectroscopies

cond-mat.str-el

Switchable X-ray Orbital Angular Momentum from an Artificial Spin Ice

Artificial spin ices (ASI) have been widely investigated as magnetic metamaterials with exotic properties governed by their geometries. In parallel, interest in X-ray photon orbital angular momentum (OAM) has been rapidly growing. Here we show that a square ASI with a programmed topological defect, a double edge dislocation, imparts OAM to scattered X-rays. Unlike single dislocations, a double dislocation does not introduce magnetic frustration, and the ASI equilibrates to its antiferromagnetic (AF) ground state. The topological charge of the defect differs with respect to the structural and magnetic order; thus, X-ray diffraction from the ASI produces photons with even and odd OAM quantum numbers at the structural and AF Bragg conditions, respectively. The magnetic transitions of the ASI allow the AF OAM beams to be switched on and off by modest variations of temperature and applied magnetic field. These results demonstrate ASIs can serve as metasurfaces for reconfigurable X-ray optics that could enable selective probes of electronic and magnetic properties.

cond-mat.mes-hall

Spatially correlated incommensurate lattice modulations in an atomically thin high-temperature Bi_{2.1}Sr_{1.9}CaCu_{2.0}O_{8+δ} superconductors

Strong variations in superconducting critical temperatures in different families of the cuprate perovskites, even with similar hole doping in their copper-oxygen planes, suggest the importance of lattice modulation effects. The one-dimensional incommensurate lattice modulation (ILM) of Bi_2Sr_2CaCu_2O_{8+y}, with the average atomic positions perturbed beyond the unit cell, offers an ideal test ground for studying the interplay between superconductivity and the long-range incommensurate lattice fluctuations. Here we report Scanning nano X-ray Diffraction (SnXRD) imaging of incommensurate lattice modulations in Bi_{2.1}Sr_{1.9}CaCu_{2.0}O_{8+δ} Van der Waals heterostructures of thicknesses down to two-unit cells. Using SnXRD, we probe that the long-range and short-range incommensurate lattice modulations in bulk sample surface with spatial resolution below 100 nm. We find that puddle-like domains of ILM of size uniformly evolving with dimensionality. In the 2-unit cell thin sample, it is observed that the wavevectors of the long- and short-range orders become anti-correlated with emerging spatial patterns having a directional gradient. The emerging patterns, originated by tiny tuning of lattice strain, induce static mesoscopic charge density waves. Our findings thus demonstrate that the strain can be used to tune and control the electromagnetic properties of two-dimensional high-temperature superconductors.

cond-mat.mtrl-sci

Evidence for the Alternating Next-Nearest Neighbor model in the dynamic behavior of a frustrated antiferromagnet

X-ray photon correlation spectroscopy (XPCS) enables us to study dynamics of antiferromagnets. Using coherent soft X-ray diffraction, we resonantly probe Mn and Co Bragg peaks in the frustrated magnetic chain compound Lu2CoMnO6 significantly below the Neel temperature. Bragg peaks of incommensurate order slide towards commensurate 'up up down down' order with decreasing temperature. Antiferromagnetic inhomogeneities produce speckle within the Bragg peaks, whose dynamics are probed by XPCS and compared to the classic Axial Next-Nearest Neighbor Interaction model of frustration. The data supports a novel model prediction: with decreasing temperature the dynamics become faster.

cond-mat.str-el

Direct measurement of temporal correlations above the spin-glass transition by coherent resonant magnetic x-ray spectroscopy

In the 1970s a new paradigm was introduced that interacting quenched systems, such as a spin-glass, have a phase transition in which long time memory of spatial patterns is realized without spatial correlations. The principal methods to study the spin-glass transition, besides some elaborate and elegant theoretical constructions, have been numerical computer simulations and neutron spin echo measurements . We show here that the dynamical correlations of the spin-glass transition are embedded in measurements of the four-spin correlations at very long times. This information is directly available in the temporal correlations of the intensity, which encode the spin-orientation memory, obtained by the technique of resonant magnetic x-ray photon correlation spectroscopy (RM- XPCS). We have implemented this method to observe and accurately characterize the critical slowing down of the spin orientation fluctuations in the classic metallic spin glass alloy Cu(Mn) over time scales of 1 to 1000 secs. Our method opens the way for studying phase transitions in systems such as spin ices, and quantum spin liquids, as well as the structural glass transition.

cond-mat.str-el

Scale-invariant magnetic textures in the strongly correlated oxide NdNiO$_3$

Strongly correlated quantum solids are characterized by an inherently granular electronic fabric, with spatial patterns that can span multiple length scales in proximity to a critical point. Here, we used a resonant magnetic X-ray scattering nanoprobe with sub-100 nm spatial resolution to directly visualize the texture of antiferromagnetic domains in NdNiO$_3$. Surprisingly, our measurements revealed a highly textured magnetic fabric, which is shown to be robust and nonvolatile even after thermal erasure across its ordering ($T_{N\acute{e}el}$) temperature. The scale-free distribution of antiferromagnetic domains and its non-integral dimensionality point to a hitherto-unobserved magnetic fractal geometry in this system. These scale-invariant textures directly reflect the continuous nature of the magnetic transition and the proximity of this system to a critical point. The present study not only exposes the near-critical behavior in rare earth nickelates but also underscores the potential for novel X-ray scattering nanoprobes to image the multiscale signatures of criticality near a critical point.

cond-mat.str-el

Distinct fingerprints of charge density waves and electronic standing waves in ZrTe$_3$

Experimental signatures of charge density waves (CDW) in high-temperature superconductors have evoked much recent interest, yet an alternative interpretation has been theoretically raised based on electronic standing waves resulting from quasiparticles scattering off impurities or defects, also known as Friedel oscillations (FO). Indeed the two phenomena are similar and related, posing a challenge to their experimental differentiation. Here we report a resonant X-ray diffraction study of ZrTe$_3$, a model CDW material. Near the CDW transition, we observe two independent diffraction signatures that arise concomitantly, only to become clearly separated in momentum while developing very different correlation lengths in the well-ordered state. Anomalously slow dynamics of mesoscopic ordered nanoregions are further found near the transition temperature, in spite of the expected strong thermal fluctuations. These observations reveal that a spatially-modulated CDW phase emerges out of a uniform electronic fluid via a process that is promoted by self-amplifying FO, and identify a viable experimental route to distinguish CDW and FO.

cond-mat.str-el

Perovskite Quantum Organismoids

A central characteristic of living beings is the ability to learn from and respond to their environment leading to habit formation and decision making1-3. This behavior, known as habituation, is universal among forms of life with a central nervous system, and interestingly observed even in single cellular organisms that do not possess a brain4-5. Here, we report the discovery of habituation based plasticity utilizing a perovskite quantum system by dynamical modulation of electron localization via reversible dopant incorporation. Microscopic mechanisms and pathways that enable this organismic collective charge-lattice interaction are elucidated by a combination of first-principles theory, synchrotron investigations, ab-initio dynamical simulations and in-situ environmental breathing studies. We implement a new learning algorithm inspired from the conductance relaxation behavior of perovskites that naturally incorporates habituation and demonstrate "learning to forget": a key feature of animal and human brains6. Most surprisingly, our results show that incorporating this elementary skill in learning dramatically boosts the capability of artificial cognitive systems.

cond-mat.mtrl-sci

Crystallographic investigation of Au nanoparticles embedded in a SrTiO$_3$ thin film for plasmonics applications by means of synchrotron radiation

Self-organized monocrystalline Au nanoparticles with potential applications in plasmonics are grown in a SrTiO$_3$ matrix by a novel two-step deposition process. The crystalline preferred orientation of these Au nanoparticles is investigated by synchrotron hard x-ray diffraction. Nanoparticles preferentially align with the (111) direction along the substrate normal (001), whereas two in-plane orientations are found with $[110]_{SrTiO_3} \: || \: [110]_{Au}$ and $[100]_{SrTiO_3} \: || \: [110]_{Au}$. Additionally, a smaller diffraction signal from nanoparticles with the (001) direction parallel to the substrate normal (001) is observed; once again, two in-plane orientations are found, with $[100]_{SrTiO_3} \: || \: [100]_{Au}$ and $[100]_{SrTiO_3} \: || \: [110]_{Au}$. The populations of the two in-plane orientations are found to depend on the thickness of the gold film deposited in the first step of the growth.

cond-mat.mes-hall

On the role of intrinsic disorder in the structural phase transition of magnetoelectric EuTiO3

Up to now the crystallographic structure of the magnetoelectric perovskite EuTiO3 was considered to remain cubic down to low temperature. Here we present high resolution synchrotron X-ray powder diffraction data showing the existence of a structural phase transition, from cubic Pm-3m to tetragonal I4/mcm, involving TiO6 octahedra tilting, in analogy to the case of SrTiO3. The temperature evolution of the tilting angle indicates a second-order phase transition with an estimated Tc=235K. This critical temperature is well below the recent anomaly reported by specific heat measurement at TA\sim282K. By performing atomic pair distribution function analysis on diffraction data we provide evidence of a mismatch between the local (short-range) and the average crystallographic structures in this material. Below the estimated Tc, the average model symmetry is fully compatible with the local environment distortion but the former is characterized by a reduced value of the tilting angle compared to the latter. At T=240K data show the presence of local octahedra tilting identical to the low temperature one, while the average crystallographic structure remains cubic. On this basis, we propose intrinsic lattice disorder to be of fundamental importance in the understanding of EuTiO3 properties.

cond-mat.str-el

Synthesis and Characterization of Single Crystal Samples of Spin-$1/2$ Kagome Lattice Antiferromagnets in the Zn-Paratacamite Family Zn$_{x}$Cu$_{4-x}$(OH)$_{6}$Cl$_{2}$

The Zn-paratacamite family, Zn$_{x}$Cu$_{4-x}$(OH)$_{6}$Cl$_{2}$ for $x \, \geq$ 0.33, is an ideal system for studying spin-1/2 frustrated magnetism in the form of antiferromagnetic Cu$^{2+}$ kagome planes. Here we report a new synthesis method by which high quality millimeter-sized single crystals of Zn-paratacamite have been produced. These crystals have been characterized by metal analysis, x-ray diffraction, neutron diffraction, and thermodynamic measurements. The $x$ = 1 member of the series displays a magnetic susceptibility that is slightly anisotropic at high temperatures with $χ_{c} \, > \, χ_{ab}$. Neutron and synchrotron x-ray diffraction experiments confirm the quality of these $x$ = 1 single crystals and indicate no obvious structural transition down to temperatures of T=2 K.

cond-mat.str-el

Charge and orbital ordering in Fe and Mn perovskite oxides far from half- doping by resonant x- ray scattering

The emergence of superlattice periodicities at metal to insulator transitions in hole doped perovskite oxides responds to a rearrangement of the local atomic structure, and electron and spin density distribution. Originally, the ionic model based on a checkerboard- type atomic distribution served to describe the low temperature charge and orbital ordered (COO) phases arising in half- doped manganites. In the last years, the exploitation of resonant x- ray scattering (RXS) capabilities has shown the need to revisit these concepts and improve the picture. Yet, we have realised that COO is a more common phenomenon than expected that can be observed in a wide range of doping levels. Here we compare the experimental data recently collected by RXS on La_0.4Sr_1.6MnO_4 (x=0.60) and La(Pr)_1/3Sr_2/3FeO_3 (x=0.67). The first shows a COO phase similar to that found in the x=0.5 sample but angular peak positions vs. T denotes the incommensurability of superlattice reflections. Meanwhile, the analysis of the commensurate CO phase in the studied ferrite underlines the role of the structural changes also involving La(Sr) and O atoms.

cond-mat.str-el

EuFe_2As_2 magnetic structure determination

Magnetic resonant X ray scattering experiments have been performed on a single crystal of EuFe_2As_2 at the Eu L_3 absorption edge. This has permitted us to determine for the first time the orientation of Eu magnetic moments in the antiferromagnetic ordered phase below T_N=19 K as parallel to the a-axis. In addition, non-resonant magnetic X ray measurements indicate that Fe magnetic moments align along the same direction in the spin density wave phase (T<T_S~190 K). Temperature dependences indicate that the onset of the Eu AFM phase barely affects the Fe magnetic sublattice.

cond-mat.str-el