arXiv subjects

Riccardo Comin

Publications and source records attributed to Riccardo Comin.

At least 73 records · Page 4Linked to original sources

arXiv2021

Maskless off-axis X-ray Holography

Off-axis X-ray holography is a lensless imaging technique that allows unambiguous retrieval of an object's exit-wave function with high fidelity. It has been used with great success to study nanoscale phenomena and spatio-temporal dynamics in solids, with sensitivity to the phase component of electronic and magnetic textures. However, the method requires patterning a nanostructured holography mask directly onto the sample. This invasive fabrication process is labor-intensive and defines a fixed field of view, limiting the range of applicable samples and diminishing the signal-to-noise ratio at high-resolution. In this work, we propose using wavefront-shaping X-ray diffractive optics to create a spatially structured probe with full control of its phase at the sample plane, obviating the need for a holography mask. We demonstrate in silico that the method can image nanoscale structures and magnetic textures. The proposed holography route can image extended regions of interest, enabling the investigation of a broad range of physical phenomena at the nanoscale including magnetism and electronic phase coexistence in quantum materials. We further envisage applications in phase-contrast imaging of other weakly absorbing objects in the realm of soft and biological matter research.

physics.optics↗

arXiv2021

Ferromagnetic helical nodal line and Kane-Mele spin-orbit coupling in kagome metal Fe3Sn2

The two-dimensional kagome lattice hosts Dirac fermions at its Brillouin zone corners K and K', analogous to the honeycomb lattice. In the density functional theory electronic structure of ferromagnetic kagome metal Fe$_3$Sn$_2$, without spin-orbit coupling we identify two energetically split helical nodal lines winding along $z$ in the vicinity of K and K' resulting from the trigonal stacking of the kagome layers. We find that hopping across A-A stacking introduces a layer splitting in energy while that across A-B stacking controls the momentum space amplitude of the helical nodal lines. The effect of spin-orbit coupling is found to resemble that of a Kane-Mele term, where the nodal lines can either be fully gapped to quasi-two-dimensional massive Dirac fermions, or remain gapless at discrete Weyl points depending on the ferromagnetic moment orientation. Aside from numerically establishing Fe$_3$Sn$_2$ as a model Dirac kagome metal, our results provide insights into materials design of topological phases from the lattice point of view, where paradigmatic low dimensional lattice models often find realizations in crystalline materials with three-dimensional stacking.

cond-mat.mtrl-sci↗

arXiv2020

Single-frame far-field diffractive imaging with randomized illumination

We introduce a single-frame diffractive imaging method called randomized probe imaging (RPI). In RPI, a sample is illuminated by a structured probe field containing speckles smaller than the sample's typical feature size. Quantitative amplitude and phase images are then reconstructed from the resulting far-field diffraction pattern. The experimental geometry of RPI is straightforward to implement, requires no near-field optics, and is applicable to extended samples. When the resulting data are analyzed with a complimentary algorithm, reliable reconstructions which are robust to missing data are achieved. To realize these benefits, a resolution limit associated with the numerical aperture of the probe-forming optics is imposed. RPI therefore offers an attractive modality for quantitative X-ray phase imaging when temporal resolution and reliability are critical but spatial resolution in the tens of nanometers is sufficient. We discuss the method, introduce a reconstruction algorithm, and present two proof-of-concept experiments: one using visible light, and one using soft X-rays.

physics.optics↗

arXiv2020

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↗

arXiv2020

Multi-orbital charge density wave excitations and concomitant phonon anomalies in Bi$_2$Sr$_2$LaCuO$_{6+δ}$

Charge density waves (CDWs) are ubiquitous in under-doped cuprate superconductors. As a modulation of the valence electron density, CDWs in hole-doped cuprates possess both Cu-3d and O-2p orbital character owing to the strong hybridization of these orbitals near the Fermi level. Here, we investigate under-doped Bi$_2$Sr$_{1.4}$La$_{0.6}$CuO$_{6+δ}$ using resonant inelastic X-ray scattering (RIXS) and find that a short-range CDW exists at both Cu and O sublattices in the copper-oxide (CuO2) planes with a comparable periodicity and correlation length. Furthermore, we uncover bond-stretching and bond-buckling phonon anomalies concomitant to the CDWs. Comparing to slightly over-doped Bi$_2$Sr$_{1.8}$La$_{0.2}$CuO$_{6+δ}$, where neither CDWs nor phonon anomalies appear, we highlight that a sharp intensity anomaly is induced in the proximity of the CDW wavevector (QCDW) for the bond-buckling phonon, in concert with the diffused intensity enhancement of the bond-stretching phonon at wavevectors much greater than QCDW. Our results provide a comprehensive picture of the quasi-static CDWs, their dispersive excitations, and associated electron-phonon anomalies, which are key for understanding the competing electronic instabilities in cuprates.

cond-mat.str-el↗

arXiv2020

Topological flat bands in frustrated kagome lattice CoSn

Electronic flat bands in momentum space, arising from strong localization of electrons in real space, are an ideal stage to realize strong correlation phenomena. In certain lattices with built-in geometrical frustration, electronic confinement and flat bands can naturally arise from the destructive interference of electronic hopping pathways. Such lattice-borne flat bands are often endowed with nontrivial topology if combined with spin-orbit coupling, while their experimental realization in condensed matter system has been elusive so far. Here, we report the direct observation of topological flat bands in the vicinity of the Fermi level in frustrated kagome system CoSn, using angle-resolved photoemission spectroscopy and band structure calculations. The flat band manifests itself as a dispersionless electronic excitation along the G-M high symmetry direction, with an order of magnitude lower bandwidth (below 150 meV) compared to the Dirac bands originating from the same orbitals. The frustration-driven nature of the flat band is directly confirmed by the real-space chiral d-orbital texture of the corresponding effective Wannier wave functions. Spin-orbit coupling opens a large gap of 80 meV at the quadratic band touching point between the Dirac and flat bands, endowing a nonzero Z2 topological invariant to the flat band in the two-dimensional Brillouin zone. Our observation of lattice-driven topological flat band opens a promising route to engineer novel emergent phases of matter at the crossroad between strong correlation physics and electronic topology.

cond-mat.str-el↗

arXiv2019

Evidence for a pressure-induced phase transition of few-layer graphene to 2D diamond

We unveil the diamondization mechanism of few-layer graphene compressed in the presence of water, providing robust evidence for the pressure-induced formation of 2D diamond. High-pressure Raman spectroscopy provides evidence of a phase transition occurring in the range of 4-7 GPa for 5-layer graphene and graphite. The pressure-induced phase is partially transparent and indents the silicon substrate. Our combined theoretical and experimental results indicate a gradual top-bottom diamondization mechanism, consistent with the formation of diamondene, a 2D ferromagnetic semiconductor. High-pressure x-ray diffraction on graphene indicates the formation of hexagonal diamond, consistent with the bulk limit of eclipsed-conformed diamondene.

cond-mat.mtrl-sci↗

arXiv2019

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↗

arXiv2019

Temperature-independent thermal radiation

Thermal emission is the process by which all objects at non-zero temperatures emit light, and is well-described by the classic Planck, Kirchhoff, and Stefan-Boltzmann laws. For most solids, the thermally emitted power increases monotonically with temperature in a one-to-one relationship that enables applications such as infrared imaging and non-contact thermometry. Here, we demonstrate ultrathin thermal emitters that violate this one-to-one relationship via the use of samarium nickel oxide (SmNiO3), a strongly correlated quantum material that undergoes a fully reversible, temperature-driven solid-state phase transition. The smooth and hysteresis-free nature of this unique insulator-to-metal (IMT) phase transition allows us to engineer the temperature dependence of emissivity to precisely cancel out the intrinsic blackbody profile described by the Stefan-Boltzmann law, for both heating and cooling. Our design results in temperature-independent thermally emitted power within the long-wave atmospheric transparency window (wavelengths of 8 - 14 um), across a broad temperature range of ~30 °C, centered around ~120 °C. The ability to decouple temperature and thermal emission opens a new gateway for controlling the visibility of objects to infrared cameras and, more broadly, new opportunities for quantum materials in controlling heat transfer.

physics.optics↗

arXiv2019

Dirac fermions and flat bands in the ideal kagome metal FeSn

The kagome lattice based on 3d transition metals is a versatile platform for novel topological phases hosting symmetry-protected electronic excitations and exotic magnetic ground states. However, the paradigmatic states of the idealized two-dimensional (2D) kagome lattice - Dirac fermions and topological flat bands - have not been simultaneously observed, partly owing to the complex stacking structure of the kagome compounds studied to date. Here, we take the approach of examining FeSn, an antiferromagnetic single-layer kagome metal with spatially-decoupled kagome planes. Using polarization- and termination-dependent angle-resolved photoemission spectroscopy (ARPES), we detect the momentum-space signatures of coexisting flat bands and Dirac fermions in the vicinity of the Fermi energy. Intriguingly, when complemented with bulk-sensitive de Haas-van Alphen (dHvA) measurements, our data reveal an even richer electronic structure that exhibits robust surface Dirac fermions on specific crystalline terminations. Through band structure calculations and matrix element simulations, we demonstrate that the bulk Dirac bands arise from in-plane localized Fe-3d orbitals under kagome symmetry, while the surface state realizes a rare example of fully spin-polarized 2D Dirac fermions when combined with spin-layer locking in FeSn. These results highlight FeSn as a prototypical host for the emergent excitations of the kagome lattice. The prospect to harness these excitations for novel topological phases and spintronic devices is a frontier of great promise at the confluence of topology, magnetism, and strongly-correlated electron physics.

cond-mat.str-el↗

arXiv2019

An XMCD study of magnetism and valence state in iron-substituted strontium titanate

Room temperature ferromagnetism was characterized for thin films of SrTi$_{0.6}$Fe$_{0.4}$O$_{3-δ}$ grown by pulsed laser deposition on SrTiO$_{3}$ and Si substrates under different oxygen pressures and after annealing under oxygen and vacuum conditions. X-ray magnetic circular dichroism demonstrated that the magnetization originated from Fe$^{2+}$ cations, whereas Fe$^{3+}$ and Ti$^{4+}$ did not contribute. Films with the highest magnetic moment (0.8 μB per Fe) had the highest measured Fe$^{2+}$:Fe${^3+}$ ratio of 0.1 corresponding to the largest concentration of oxygen vacancies (δ = 0.19). Post-growth annealing treatments under oxidizing and reducing conditions demonstrated quenching and partial recovery of magnetism respectively, and a change in Fe valence states. The study elucidates the microscopic origin of magnetism in highly Fe-substituted SrTi$_{1-x}$Fe$_x$O$_{3-δ}$ perovskite oxides and demonstrates that the magnetic moment, which correlates with the relative content of Fe$^{2+}$ and Fe$^{3+}$, can be controlled via the oxygen content, either during growth or by post-growth annealing.

cond-mat.mtrl-sci↗

arXiv2019

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↗

arXiv2019

Giant enhancement of interlayer exchange in an ultrathin 2D magnet

Following the recent isolation of monolayer CrI3, there has been a surge of new two-dimensional van der Waals magnetic materials, whose incorporation in van der Waals heterostructures offers a new platform for spintronics, proximity magnetism, and quantum spin liquids. A primary question in this burgeoning field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies on CrI3 have shown a different magnetic ground state for ultrathin exfoliated films but the origin is not yet understood. Here, we use electron tunneling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order, finding a ten-fold enhancement in the interlayer exchange compared to bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveal that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low temperature stacking order and, we hypothesize, increased interlayer exchange. Our study provides new insight into the connection between stacking order and interlayer interactions in novel two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets, such as RuCl3.

cond-mat.mes-hall↗

arXiv2018

de Haas-van Alphen effect of correlated Dirac states in kagome metal Fe3Sn2

The field of topological electronic materials has seen rapid growth in recent years, in particular with the increasing number of weakly interacting systems predicted and observed to host topologically non-trivial bands. Given the broad appearance of topology in such systems, it is expected that correlated electronic systems should also be capable of hosting topologically non-trivial states. Interest in correlated platforms is heightened by the prospect that collective behavior therein may give rise to new types of topological states and phenomena not possible in non-interacting systems. However, to date only a limited number of correlated topological materials have been definitively reported due to both the challenge in calculation of their electronic properties and the experimental complexity of correlation effects imposed on the topological aspects of their electronic structure. Here, we report a de Haas-van Alphen (dHvA) study of the recently discovered kagome metal Fe$_3$Sn$_2$ mapping the massive Dirac states strongly coupled to the intrinsic ferromagnetic order. We observe a pair of quasi-two-dimensional Fermi surfaces arising from the massive Dirac states previously detected by spectroscopic probes and show that these band areas and effective masses are systematically modulated by the rotation of the ferromagnetic moment. Combined with measurements of Berry curvature induced Hall conductivity, we find that along with the Dirac fermion mass, velocity, and energy are suppressed with rotation of the moment towards the kagome plane. These observations demonstrate that strong coupling of magnetic order to electronic structure similar to that observed in elemental ferromagnets can be extended to topologically non-trivial electronic systems, suggesting pathways for connecting topological states to robust spintronic technologies.

cond-mat.str-el↗

arXiv2017

Massive Dirac fermions in a ferromagnetic kagome metal

The kagome lattice is a two-dimensional network of corner-sharing triangles known as a platform for exotic quantum magnetic states. Theoretical work has predicted that the kagome lattice may also host Dirac electronic states that could lead to topological and Chern insulating phases, but these have evaded experimental detection to date. Here we study the d-electron kagome metal Fe$_3$Sn$_2$ designed to support bulk massive Dirac fermions in the presence of ferromagnetic order. We observe a temperature independent intrinsic anomalous Hall conductivity persisting above room temperature suggestive of prominent Berry curvature from the time-reversal breaking electronic bands of the kagome plane. Using angle-resolved photoemission, we discover a pair of quasi-2D Dirac cones near the Fermi level with a 30 meV mass gap that accounts for the Berry curvature-induced Hall conductivity. We show this behavior is a consequence of the underlying symmetry properties of the bilayer kagome lattice in the ferromagnetic state with atomic spin-orbit coupling. This report provides the first evidence for a ferromagnetic kagome metal and an example of emergent topological electronic properties in a correlated electron system. This offers insight into recent discoveries of exotic electronic behavior in kagome lattice antiferromagnets and may provide a stepping stone toward lattice model realizations of fractional topological quantum states.

cond-mat.mtrl-sci↗

arXiv2017

Mottness at finite doping and charge-instabilities in cuprates

The intrinsic instability of underdoped copper oxides towards inhomogeneous states is one of the central puzzles of the physics of correlated materials. The influence of the Mott physics on the doping-temperature phase diagram of copper oxides represents a major issue that is subject of intense theoretical and experimental effort. Here, we investigate the ultrafast electron dynamics in prototypical single-layer Bi-based cuprates at the energy scale of the O-2p$\rightarrow$Cu-3d charge-transfer (CT) process. We demonstrate a clear evolution of the CT excitations from incoherent and localized, as in a Mott insulator, to coherent and delocalized, as in a conventional metal. This reorganization of the high-energy degrees of freedom occurs at the critical doping p$_{cr}\simeq$0.16 irrespective of the temperature, and it can be well described by dynamical mean field theory calculations. We argue that the onset of the low-temperature charge instabilities is the low-energy manifestation of the underlying Mottness that characterizes the p<p$_{cr}$ region of the phase diagram. This discovery sets a new framework for theories of charge order and low-temperature phases in underdoped copper oxides.

cond-mat.supr-con↗

arXiv2017

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↗

arXiv2016

Tracking local magnetic dynamics via high-energy charge excitations in a relativistic Mott insulator

We use time- and energy-resolved optical spectroscopy to investigate the coupling of electron-hole excitations to the magnetic environment in the relativistic Mott insulator Na$_2$IrO$_3$. We show that, on the picosecond timescale, the photoinjected electron-hole pairs delocalize on the hexagons of the Ir lattice via the formation of quasi-molecular orbital (QMO) excitations and the exchange of energy with the short-range-ordered zig-zag magnetic background. The possibility of mapping the magnetic dynamics, which is characterized by typical frequencies in the THz range, onto high-energy (1-2 eV) charge excitations provides a new platform to investigate, and possibly control, the dynamics of magnetic interactions in correlated materials with strong spin-orbit coupling, even in the presence of complex magnetic phases.

cond-mat.str-el↗