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Jerzy T. Sadowski

Publications and source records attributed to Jerzy T. Sadowski.

At least 19 recordsLinked to original sources

Direct Evidence for Robust Bulk Band Gap Across the Charge Density Wave Transition in TiSe2

The mechanism driving the charge density wave (CDW) transition in TiSe2 has been debated for decades, with proposals ranging from an excitonic insulator to a lattice-driven instability. A central question remains whether the transition involves an opening or enhancement of the bulk band gap. Using high-resolution angle-resolved photoemission spectroscopy, we directly track the temperature evolution of the bulk band edges across the CDW transition at TCDW = 200 K. Contrary to the expectation of a gap-opening transition, we find that the size of the fundamental band gap remains constant from the high-temperature normal phase down to 160 K. While the CDW induces clear band-folding signatures and spectral weight redistribution, the underlying band extrema are unperturbed. These results demonstrate that TiSe2 does not undergo a temperature-driven electronic gap opening. Instead, they support a scenario where the transition is governed by a lattice symmetry-breaking reconstruction that folds, but does not gap, the electronic structure of a pre-existing band insulator.

cond-mat.str-el

Proximity-induced charge transfer, strain and magnetic exchange in graphene/CrSBr heterostructure

Stacking van der Waals materials provides a powerful route to engineer emergent electronic and magnetic behaviors through proximity-driven interactions. The graphene/CrSBr heterostructure has emerged as a compelling platform in this frontier, exhibiting exotic macroscopic responses-- including uniaxial surface-plasmon-polariton propagation and an unconventional quantum Hall effect-- indicative of strong interfacial electronic and magnetic coupling. However, a microscopic electronic landscape governing these phenomena has remained elusive. Here, we provide a comprehensive spectroscopic characterization of the graphene/CrSBr interface using a combination of angle-resolved photoemission spectroscopy (ARPES), low-energy electron microscopy (LEEM), and density functional theory. We resolve a massive redistribution of interfacial charge that concurrently hole dopes graphene and populates the quasi-one-dimensional spin-polarized conduction band of CrSBr, resulting insulator-to-metal transition in the interfacial CrSBr layer. Furthermore, electronic structure of CrSBr exhibits strong momentum-dependent renormalization distinct from conventional charge doping, and theoretical modeling supported by Raman spectroscopy points to additional interfacial compressive strain. In addition, ARPES reveals a splitting-like feature in the graphene Dirac cone consistent with spin degeneracy lifting, providing possible evidence of magnetic proximity coupling. These findings provide crucial microscopic insight into the system's optical and transport responses and establish graphene/CrSBr as a versatile platform for charge-transfer control, strain-driven band engineering, magnetic-proximity coupling, and directionally confined excitations for next-generation spintronic and nanophotonic devices.

cond-mat.str-el

Magnetic metamaterials by ion-implantation

We present a method for the additive fabrication of planar magnetic nanoarrays with minimal surface roughness. Synthesis is accomplished by combining electron-beam lithography, used to generate nanometric patterned masks, with ion implantation in thin films. By implanting $^{56}$Fe$^{+}$ ions, we are able to introduce magnetic functionality in a controlled manner into continuous Pd thin films, achieving 3D spatial resolution down to a few tens of nanometers. Our results demonstrate the application of this technique in fabricating square artificial spin ice lattices, which exhibit well-defined magnetization textures and interactions among the patterned magnetic elements.

cond-mat.mtrl-sci

Evolution of the Fermi surface of 1T-VSe$_2$ across a structural phase transition

The electronic origin of the structural transition in 1T-VSe$_2$ is re-evaluated through an extensive angle-resolved photoemission spectroscopy experiment. The components of the band structure, missing in previous reports, are revealed. Earlier observations, shown to be temperature independent and therefore not correlated with the phase transition, are explained in terms of the increased complexity of the band structure close to the Fermi level. Only the overall size of the Fermi surface is found to be positively correlated with the phase transition at 110 K. These observations, quite distant from the charge density wave scenario commonly considered for 1T-VSe$_2$, bring fresh perspectives toward the correct description of structural transitions in dichalcogenides materials.

cond-mat.mtrl-sci

Twisted MoSe2 Homobilayer Behaving as a Heterobilayer

Heterostructures (HSs) formed by the transition-metal dichalcogenides (TMDCs) materials have shown great promise in next-generation optoelectronic and photonic applications. An artificially twisted HS, allows us to manipulate the optical, and electronic properties. With this work, we introduce the understanding of the complex energy transfer (ET) process governed by the dipolar interaction in a twisted molybdenum diselenide (MoSe2) homobilayer without any charge-blocking interlayer. We fabricated an unconventional homobilayer (i.e., HS) with a large twist angle by combining the chemical vapor deposition (CVD) and mechanical exfoliation (Exf.) techniques to fully exploit the lattice parameters mismatch and indirect/direct (CVD/Exf.) bandgap nature. This effectively weaken the charge transfer (CT) process and allows the ET process to take over the carrier recombination channels. We utilize a series of optical and electron spectroscopy techniques complementing by the density functional theory calculations, to describe a massive photoluminescence enhancement from the HS area due to an efficient ET process. Our results show that the electronically decoupled MoSe2 homobilayer is coupled by the ET process, mimicking a 'true' heterobilayer nature.

cond-mat.mes-hall

Direct evidence of low work function on SrVO$_3$ cathode using thermionic electron emission microscopy and high-field ultraviolet photoemission spectroscopy

Perovskite SrVO$_3$ has recently been proposed as a novel electron emission cathode material. Density functional theory (DFT) calculations suggest multiple low work function surfaces and recent experimental efforts have consistently demonstrated effective work functions of ~2.7 eV for polycrystalline samples, both results suggesting, but not directly confirming, some fraction of even lower work function surface is present. In this work, thermionic electron emission microscopy (ThEEM) and high-field ultraviolet photoemission spectroscopy are used to study the local work function distribution and measure the work function of a partially-oriented-(110)-SrVO$_3$ perovskite oxide cathode surface. Our results show direct evidence of low work function patches of about 2.1 eV on the cathode surface, with corresponding onset of observable thermionic emission at 750 $^o$C. We hypothesize that, in our ThEEM experiments, the high applied electric field suppresses the patch field effect, enabling the direct measurement of local work functions. This measured work function of 2.1 eV is comparable to the previous DFT-calculated work function value of the SrVO-terminated (110) SrVO$_3$ surface (2.3 eV) and SrO terminated (100) surface (1.9 eV). The measured 2.1 eV value is also much lower than the work function for the (001) LaB$_6$ single crystal cathode (~2.7 eV) and comparable to the effective work function of B-type dispenser cathodes (~2.1 eV). If SrVO$_3$ thermionic emitters can be engineered to access domains of this low 2.1 eV work function, they have potential to significantly improve thermionic emitter-based technologies.

cond-mat.mtrl-sci

Hydrogen-induced tunable remanent polarization in a perovskite nickelate

Materials with field-tunable polarization are of broad interest to condensed matter sciences and solid-state device technologies. Here, using hydrogen (H) donor doping, we modify the room temperature metallic phase of a perovskite nickelate NdNiO3 into an insulating phase with both metastable dipolar polarization and space-charge polarization. We then demonstrate transient negative differential capacitance in thin film capacitors. The space-charge polarization caused by long-range movement and trapping of protons dominates when the electric field exceeds the threshold value. First-principles calculations suggest the polarization originates from the polar structure created by H doping. We find that polarization decays within ~1 second which is an interesting temporal regime for neuromorphic computing hardware design, and we implement the transient characteristics in a neural network to demonstrate unsupervised learning. These discoveries open new avenues for designing novel ferroelectric materials and electrets using light-ion doping.

cond-mat.str-el

Phonon-Mediated Quasiparticle Lifetime Renormalizations in Few-Layer Hexagonal Boron Nitride

Understanding the collective behavior of the quasiparticles in solid-state systems underpins the field of non-volatile electronics, including the opportunity to control many-body effects for well-desired physical phenomena and their applications. Hexagonal boron nitride (hBN) is a wide energy bandgap semiconductor, showing immense potential as a platform for low-dimensional device heterostructures. It is an inert dielectric used for gated devices, having a negligible orbital hybridization when placed in contact with other systems. Despite its inertness, we discover a large electron mass enhancement in few-layer hBN affecting the lifetime of the $π$-band states. We show that the renormalization is phonon-mediated and consistent with both single- and multiple-phonon scattering events. Our findings thus unveil a so-far unknown many-body state in a wide-bandgap insulator, having important implications for devices using hBN as one of their building blocks.

cond-mat.mtrl-sci

Magneto-transport and magnetic textures in Ho/FeCoGd/β-W multilayers

The enhancement of interfacial Dzyaloshinskii-Moriya Interaction (DMI) in magnetic multilayers results in the stabilization of topological spin textures like chiral domain walls and skyrmions. Here we report on the evaluation of interface-driven magnetic interactions in a uniquely designed multilayer where each magnetic layer of two AFM coupled sublattices of 3d and 4f moments is sandwiched between the layers of β-tungsten and holmium whose spin Hall angles are large but opposite in sign. The atomic and magnetic periodicity of these multilayers is established by polarized neutron reflectivity measurements and the presence of a labyrinth domain spin texture of zero remanence with x-ray photoelectron microscopy. Measurements of the Hall resistivity (ρ_{xy}(T, H)) together with static magnetization (M(T,H)) over a broad range of temperature (T) and magnetic field (H) indicate impending compensation between 3d and 4f sublattices at T>350 K. These multilayers are characterized by a small (0.04 %) but positive magnetoresistance indicative of interface enhance scattering and a large (40 nΩ.m) and negative anomalous ρ_{xy}(T,H) which results from a parallel alignment of 4f moments with the external magnetic field. No distinct scaling is seen between ρ_{xy}(T,H), ρ_{xx}(T, H) and M(T,H) at temperatures above 200K where the magnetization develops out-of-plane anisotropy. The field scans of ρ_{xy} at T>200K show a distinct cusp in the vicinity of magnetic saturation. These Hall data have been analyzed in the framework of a model where a distinct topological contribution to ρ_{xy} rides over the anomalous Hall resistivities of the 3d and 4f magnetic sublattices. It is suggested that this apparent topological effect results from an interfacial DMI and dominates ρ_{xy}(T,H) in the temperature regime where the 3d and 4f lattices are nearly compensated.

cond-mat.mtrl-sci

Spectroscopic evidence of high temperature superconductivity in VSe2

High-resolution angle-resolved photoemission experiments reveal subtle modifications of the surface electronic structure of VSe2. Most remarkably, we show that superconductivity can be induced in VSe2 by the right selection of substrate and growth parameters. Evidence for the superconducting state comes from the simultaneous detection of spectral kink, quasiparticle peak, Fermi gap, and their evolution with the temperature. The observation of Bogoliubov-like back-bending bands at low temperatures, signaling electron-hole pairing, further supports the presence of superconductivity in this system. The photoemission experiment also provides evidence for a formation of a pseudogap state at high temperatures, characterized by the progressive quenching of the quasiparticle peak feature coexisting with a persistent gap at the Fermi level, a behavior reminiscent of high-Tc superconductors. We attributed the origin of superconductivity in these VSe2 films to a modified Fermi surface combined with the formation of van Hove singularity points with a binding energy corresponding to the chemical potential of the system. Although Tc cannot be accurately determined from photoemission data, observations based on the survival temperature of the quasiparticle peak suggest that Tc could be as high as 100 ? 5 K and substantially higher than previous reports for any transition metal dichalcogenides.

cond-mat.supr-con

Correlating surface stoichiometry and termination in SrTiO$_{3}$ films grown by hybrid molecular beam epitaxy

Hybrid oxide molecular beam epitaxy (hMBE), a thin-film deposition technique in which transition metal cations are delivered using a metal-organic precursor, has emerged as the state-of-the-art approach to the synthesis of electronic-grade complex oxide films with a stoichiometric growth window. However, numerous questions remain regarding the chemical mechanisms of the growth process and the surface properties of the resulting films. To examine these properties, thin film SrTiO$_{3}$ (STO) was prepared by hMBE using a titanium tetraisopropoxide (TTIP) precursor for Ti delivery and an elemental Sr source on annealed STO and Nb-doped STO substrates with varying TTIP:Sr flux ratios to examine the conditions for the reported stoichiometric growth window. The films were transferred in vacuo to an x-ray photoelectron spectroscopy system to study the surface elemental composition. Samples were examined using x-ray diffraction to compare our surface sensitive results with previously reported measurements of the bulk of the films in the literature. Ex situ studies by atomic force microscopy, scanning tunneling microscopy and low energy electron microscopy confirmed the presence of surface reconstructions and an Ehrlich-Schwoebel barrier consistent with an A-site SrO termination. We find that a surface exhibiting a mixture of SrO and TiO$_{2}$ termination, or a full SrO termination is necessary to obtain stoichiometric adsorption-controlled growth. These results indicate that surface Sr is necessary to maintain chemical equilibrium for stoichiometric growth during the hMBE process, which is important for the design of future interfacial systems using this technique.

cond-mat.mtrl-sci

The Breakdown of Mott Physics at VO$_2$ Surfaces

Transition metal oxides such as vanadium dioxide (VO$_2$), niobium dioxide (NbO$_2$), and titanium sesquioxide (Ti$_2$O$_3$) are known to undergo a temperature-dependent metal-insulator transition (MIT) in conjunction with a structural transition within their bulk. However, it is not typically discussed how breaking crystal symmetry via surface termination affects the complicated MIT physics. Using synchrotron-based x-ray spectroscopy, low energy electron diffraction (LEED), low energy electron microscopy (LEEM), transmission electron microscopy (TEM), and several other experimental techniques, we show that suppression of the bulk structural transition is a common feature at VO$_2$ surfaces. Our density functional theory (DFT) calculations further suggest that this is due to inherent reconstructions necessary to stabilize the surface, which deviate the electronic structure away from the bulk d$^1$ configuration. Our findings have broader ramifications not only for the characterization of other "Mott-like" MITs, but also for any potential device applications of such materials.

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

Emergent of the flat band and superstructures in the VSe2 / Bi2Se3 system

Dispersionless flat bands are proposed to be a fundamental ingredient to achieve the various sought after quantum states of matter including high-temperature superconductivity1-4 and fractional quantum Hall effect5-6. Materials with such peculiar electronic states, however, are very rare and often exhibit very complex band structures. Here, we report on the emergence of a flat band with a possible insulating ground state in the sub-monolayer VSe2 / Bi2Se3 heterostructure by means of angle-resolved photoemission spectroscopy and scanning tunneling microscopy. The flat band is dispersionless along the kll and kz momenta, filling the entire Brillouin zone, and it exhibits a complex circular dichroism signal reversing the sign at several points of the Brillouin zone. These properties together with the presence of a Moiré patterns in VSe2 suggest that the flat band is not a trivial disorder or confinement effect and could even be topologically non-trivial. Another intriguing finding is that the flat band does not modify the Dirac cone of Bi2Se3 around the Dirac point. Furthermore, we found that the flat band and the Dirac surface states of Bi2Se3 have opposite energy shifts with electron doping. This opens a novel way of controlling the spin texture of photocurrents as well as the transport properties of the heterostructure. These features make this flat band remarkably distinguishable from previous findings and our methodology can be applied to other systems opening a promising pathway to realize strongly correlated quantum effects in topological materials.

cond-mat.mtrl-sci

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

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

Second derivative analysis and alternative data filters for multi-dimensional spectroscopies: a Fourier-space perspective

The second derivative image (SDI) method is widely applied to sharpen dispersive data features in multi-dimensional spectroscopies such as angle resolved photoemission spectroscopy (ARPES). Here, the SDI function is represented in Fourier space, where it has the form of a multi-band pass filter. The interplay of the SDI procedure with undesirable noise and background features in ARPES data sets is reviewed, and it is shown that final image quality can be improved by eliminating higher Fourier harmonics of the SDI filter. We then discuss extensions of SDI-like band pass filters to higher dimensional data sets, and how one can create even more effective filters with some a priori knowledge of the spectral features.

physics.data-an

Surface buckling of phosphorene materials: determination, origin and influence on electronic structure

The surface structure of phosphorene crystals materials is determined using surface sensitive dynamical micro-spot low energy electron diffraction (μLEED) analysis using a high spatial resolution low energy electron microscopy (LEEM) system. Samples of (\textit{i}) crystalline cleaved black phosphorus (BP) at 300 K and (\textit{ii}) exfoliated few-layer phosphorene (FLP) of about 10 nm thicknes, which were annealed at 573 K in vacuum were studied. In both samples, a significant surface buckling of 0.22 Å and 0.30 Å, respectively, is measured, which is one order of magnitude larger than previously reported. Using first principle calculations, the presence of surface vacancies is attributed not only to the surface buckling in BP and FLP, but also the previously reported intrinsic hole doping of phosphorene materials.

cond-mat.mtrl-sci