arXiv subjects

Daniel G. Chica

Publications and source records attributed to Daniel G. Chica.

At least 19 recordsLinked to original sources

arXiv2026

Layer- and Field-Dependent Magnetic Order in 2D CrSBr Revealed by Pulsed Nanocalorimetry

Understanding the evolution of magnetic order in the two-dimensional limit remains a central challenge in van der Waals magnets, where thermodynamic measurements are constrained by the femtogram-scale mass of exfoliated flakes. Here, microsecond pulse-heating nanocalorimetry is used to measure the heat capacity and magnetic entropy of CrSBr flakes down to the monolayer limit. The measurements reveal the entropy landscape associated with magnetic ordering, uncovering a decreasing interlayer transition temperature toward the monolayer limit and an entropy-derived effective moment per layer that increases with thickness toward the expected spin-only scale. Thermodynamic anomalies capture a crossover from bulk-like interlayer antiferromagnetism to a regime dominated by intralayer ferromagnetic correlations. A pronounced layer-parity effect further emerges, with odd-layer samples displaying an additional high-temperature contribution associated with uncompensated magnetic layers. Under in-plane magnetic fields applied along the easy axis, antiferromagnetic order is progressively suppressed, allowing extraction of a thickness-dependent characteristic suppression field reflecting weakened interlayer exchange coupling. Entropy analysis further reveals an extended regime of magnetic fluctuations persisting well above the interlayer ordering transition. Together, these results establish nanocalorimetry as a powerful thermodynamic probe of low-dimensional magnetism, providing direct access to magnetic entropy, exchange interactions, and dimensional crossover in atomically thin van der Waals magnets.

cond-mat.mtrl-sci↗

arXiv2026

Antiferromagnetism-altered plasmon dynamics

The interaction between plasmons and magnons is a long-sought phenomenon with implications for fundamental physics and spintronics applications. In three-dimensional systems, this coupling is suppressed by the large mismatch in energy scales, but two-dimensional (2D) plasmons with gapless dispersion can overlap with magnons over a broad spectral range. Despite numerous theoretical predictions, experimental observation of magnon-plasmon interaction has remained elusive. In this work, we study a first-of-its-kind hybrid plasmon-magnon platform based on 2D materials. By deploying scattering-type scanning near-field optical microscopy (s-SNOM) with terahertz radiation, we image propagating plasmon wavepackets at a graphene/NiPS$_3$ interface and track their dynamics across the antiferromagnetic transition of NiPS$_3$. We observe a clear renormalization of the plasmon-polariton dispersion concurrent with the onset of antiferromagnetic order. With complementary Raman scattering and nano-terahertz spectroscopy, we unveil spectral weight redistribution and dielectric screening changes, potentially associated with the multi-magnon continuum, as the underlying mechanism. These results provide solid evidence of coupling between plasmon and antiferromagnetic order, marking a cornerstone for a potential platform for hybrid magnon-plasmon interactions in 2D materials, opening avenues for coherent spin-plasmon devices and tunable terahertz spintronic components.

cond-mat.str-el↗

arXiv2026

Observation of Coherent Ferron Emission and Propagation

Excitation of ordered quantum phases gives rise to collective modes and quasiparticles, as exemplified by spin waves and magnons emerging from magnetic order. Extending this paradigm to ferroelectric materials suggests the existence of polarization waves and their fundamental quanta, ferrons. Here, we report the generation and transport of polarization waves, i.e., coherent ferrons, in the van der Waals ferroelectric material NbOI2. Upon excitation by a short laser pulse, the polarization wave emits intense and narrow-band terahertz (THz) radiation at the ferroelectric transverse optical phonon frequency, modulates the ferroelectric order parameter, and propagates uniaxially along the polar axis at hypersonic velocities of ~105 m/s. These long-lived, uniaxial, and dipole-carrying polarization waves may find applications in narrow-band THz emission, ferronic information processing, and coherent electric control.

cond-mat.mtrl-sci↗

arXiv2026

Giant optical spin-orbit interactions in ferroelectric van der Waals waveguides

Optical spin-orbit interactions (SOI) link photonic spin to momentum, offering a route toward on-chip polarization control and beam steering. Nevertheless, achieving sufficient optical SOI and nonlinearities on sub-micrometer scales - a prerequisite for dense photonic integration - remains an outstanding challenge. Here, we show that highly birefringent van der Waals (vdW) waveguides provide an ideal, chip-compatible platform to address this limitation. We focus on the ferroelectric semiconductor NbOI2, which exhibits record optical nonlinearities and dielectric anisotropy. Using femtosecond optical microscopy, we image light propagation and harmonic conversion beyond the total internal reflection barrier over tens of micrometers in NbOI2 slab waveguides. We report giant optical spin-splitting through the optical spin Hall effect, which facilitates spatial separation of optical spin currents on sub-micrometer scales, in quantitative agreement with a microscopic light-matter interaction model. We further leverage optical spin-momentum locking to realize polarization-controlled waveguide steering. We generalize these observations across various vdW waveguides and empirically confirm a scaling law linking dielectric anisotropy to geometric spin-splitting. Our results establish highly anisotropic vdW waveguides as an ideal platform for densely integrated opto-spintronic technologies.

cond-mat.mtrl-sci↗

arXiv2025

Tunable Narrowband Terahertz Radiation from van der Waals Ferroelectrics

The terahertz (THz) spectral range is central to high-speed communication, precision metrology, sensing technologies, and a range of fundamental scientific investigations. Achieving these capabilities in practical systems increasingly demands chip-scale integration of THz photonic components that are typically bulky. In this context, van der Waals (vdW) materials provide a unique platform for integrated nonlinear photonics in the visible and near-infrared regimes, and extending this framework into the THz domain would constitute a significant advance. Here, we report tunable, intense, and narrowband THz radiation from ferroelectric niobium oxyhalides. Through halogen substitution and alloying, we achieve continuous and precise control over the emission frequency from 3.1 to 5.8 THz. We show that the narrowband THz radiation is driven by phonons associated with the ferroelectric polarization. We further demonstrate dynamic and nonvolatile control of the polarity of the coherent THz wave with external electric field. This work demonstrates efficient narrowband THz emission from vdW ferroeletrics and provides microscopic insight into its origin, paving the way for on-chip THz technology for a broad range of applications.

physics.optics↗

arXiv2025

Lateral Exchange Bias for Néel-Vector Control in Atomically Thin Antiferromagnets

Atomically thin van der Waals (vdW) magnets have emerged as a fascinating platform for the exploration of novel physical phenomena arising from their reduced dimensionality and exceptional material properties. Their single-crystalline nature and ultimate miniaturization position them as leading candidates for next-generation spintronic applications. Antiferromagnetic (AF) vdW magnets are of particular interest, as they combine the advantages of vdW magnets with the functionality of AF spintronics, offering unique opportunities for ultrafast and robust spintronic devices. However, the lack of approaches to locally and deterministically manipulate their order parameter -- the Néel-vector -- remains a key limitation. Here, we introduce a fundamentally new paradigm in nanomagnetism, which we term lateral exchange bias (LEB), to achieve Néel vector control in bilayers of the vdW AF CrSBr. We exploit the single-crystalline registry formed by terraced CrSBr samples, where the bilayer Néel vector is controlled by LEB from neighboring, odd-layered flakes, whose nonzero magnetization we manipulate using magnetic fields. Using this control, we achieve nonvolatile manipulation of magnetic domains and domain walls (DWs) in AF CrSBr bilayers, establishing a powerful toolkit for controlling atomically thin AFs at the nanoscale. Our results challenge conventional views on exchange bias and provide a previously unexplored mechanism for achieving atomic-scale control of AFic order. Our findings pave the way for the development of advanced spintronic architectures and quantum technologies based on vdW magnets.

cond-mat.mtrl-sci↗

arXiv2025

Defect complexes in CrSBr revealed through electron microscopy and deep learning

Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and ab-initio calculations. We apply a custom-developed machine learning work flow to detect, classify and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab-initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are furthermore predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family.

cond-mat.mtrl-sci↗

arXiv2025

Spin-filter tunneling detection of antiferromagnetic resonance with electrically-tunable damping

Antiferromagnetic spintronics offers the potential for higher-frequency operations and improved insensitivity to magnetic fields compared to ferromagnetic spintronics. However, previous electrical techniques to detect antiferromagnetic dynamics have utilized large, millimeter-scale bulk crystals. Here we demonstrate direct electrical detection of antiferromagnetic resonance in structures on the few-micrometer scale using spin-filter tunneling in PtTe$_2$/bilayer CrSBr/graphite junctions in which the tunnel barrier is the van der Waals antiferromagnet CrSBr. This sample geometry allows not only efficient detection, but also electrical control of the antiferromagnetic resonance through spin-orbit torque from the PtTe$_2$ electrode. The ability to efficiently detect and control antiferromagnetic resonance enables detailed studies of the physics governing these high frequency dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Charge Density Wave and Ferromagnetism in Intercalated CrSBr

In materials with one-dimensional electronic bands, electron-electron interactions can produce intriguing quantum phenomena, including spin-charge separation and charge density waves (CDW). Most of these systems, however, are non-magnetic, motivating a search for anisotropic materials where the coupling of charge and spin may affect emergent quantum states. Here, chemical intercalation of the van der Waals magnetic semiconductor CrSBr yields $Li_{0.17(2)} (tetrahydrofuran)_{0.26(3)} CrSBr$, which possess an electronically driven quasi-1D CDW with an onset temperature above room temperature. Concurrently, electron doping increases the magnetic ordering temperature from 132 K to 200 K and switches its interlayer magnetic coupling from antiferromagnetic to ferromagnetic. The spin-polarized nature of the anisotropic bands that give rise to this CDW enforces an intrinsic coupling of charge and spin. The coexistence and interplay of ferromagnetism and charge modulation in this exfoliatable material provides a promising platform for studying tunable quantum phenomena across a range of temperatures and thicknesses.

cond-mat.mtrl-sci↗

arXiv2025

Engineering robust strain transmission in van der Waals heterostructure devices

Atomically thin van der Waals materials provide a highly tunable platform for exploring emergent quantum phenomena in solid state systems. Due to their remarkable mechanical strength, one enticing tuning knob is strain. However, the weak strain transfer of graphite and hBN, which are standard components of high-qualityvdW devices, poses fundamental challenges for high-strain experiments. Here, we investigate strain transmission in less-explored orthorhombic crystals and find robust transmission up to several percent at cryogenic temperatures. We further show that strain can be efficiently transferred through these crystals to other 2D materials in traditional heterostructure devices. Using this capability, we demonstrate in-situ strain and gate control of the optical properties of monolayer WS2 utilizing the high-\k{appa} dielectric insulator Bi2SeO5 as a substrate. These results enable the exploration of combined cryo-strain and gate tuning in a variety of layered systems such as moiré heterostructures, air-sensitive 2D magnets and superconductors, and any gated 2D device.

cond-mat.mes-hall↗

arXiv2024

Exciton Dressing by Extreme Nonlinear Magnons in a Layered Semiconductor

Collective excitations presenting nonlinear dynamics are fundamental phenomena with broad applications. A prime example is nonlinear optics, where diverse frequency mixing processes are central to communication, sensing, wavelength conversion, and attosecond physics. Leveraging recent progress in van der Waals magnetic semiconductors, we demonstrate nonlinear opto-magnonic coupling by presenting exciton states dressed by up to 20 harmonics of magnons, resulting from their nonlinearities, in the layered antiferromagnetic semiconductor CrSBr. We also create tunable optical side bands from sum- and difference-frequency generation between two optically bright magnon modes under symmetry breaking magnetic fields. Moreover, the observed difference-frequency generation mode can be continuously tuned into resonance with one of the fundamental magnons, resulting in parametric amplification of magnons. These findings realize the modulation of the optical frequency exciton with the extreme nonlinearity of magnons at microwave frequencies, which could find applications in magnonics and hybrid quantum systems, and provide new avenues for implementing opto-magnonic devices.

cond-mat.mes-hall↗

arXiv2024

A 2D van der Waals Material for Terahertz Emission with Giant Optical Rectification

Exfoliation and stacking of two-dimensional (2D) van der Waals (vdW) crystals have created unprecedented opportunities in the discovery of quantum phases. A major obstacle to the advancement of this field is the limited spectroscopic access due to a mismatch in sample sizes (1 - 10 micrometer) and wavelengths (0.1 - 1 millimeter) of electromagnetic radiation relevant to their low-energy excitations. Here, we introduce a new member of the 2D vdW material family: a terahertz (THz) emitter. We show intense and broadband THz generation from the vdW ferroelectric semiconductor NbOI2 with optical rectification efficiency over one-order-of-magnitude higher than that of the current standard THz emitter, ZnTe. The NbOI2 THz emitter can be easily integrated into vdW heterostructures for on-chip near-field THz spectroscopy of a target vdW material/device. Our approach provides a general spectroscopic tool for the rapidly expanding field of 2D vdW materials and quantum matter.

cond-mat.mtrl-sci↗

arXiv2024

Electronic Bound States in the Continuum in a 2D Metal

Bound states in the continuum (BICs) are quantum states that remain localized despite existing within a continuum of extended, delocalized states. They defy conventional wave theories and could be instrumental for quantum technologies that rely on the precise control of quantum states. While optical BICs have been realized in photonic systems, achieving electronic bound states in a metallic background remains an ongoing challenge. Here, we observe two defect states that remain localized within the metallic continuum of Pd5AlI2, a two-dimensional van der Waals metal. The emergence of these states is a manifestation of the hopping interference in the Pd5AlI2 lattice. This interference results in a (quasi) flat band and spatially localized eigenstates that are orthogonal to the metallic continuum thus avoiding hybridization with extended states.

cond-mat.mtrl-sci↗

arXiv2024

Coupling of Electronic Transitions to Ferroelectric Order in a 2D Semiconductor

A ferroelectric material often exhibits a soft transvers optical (TO) phonon mode which governs it phase transition. Charge coupling to this ferroelectric soft mode may further mediate emergent physical properties, including superconductivity and defect tolerance. However, direct experimental evidence for such coupling is scarce. Here we show that a photo-launched coherent phonon couples strongly to electronic transitions across the bandgap in the van der Waals (vdW) two-dimensional (2D) ferroelectric semiconductor NbOI2. Using terahertz time-domain spectroscopy and first-principles calculations, we identify this mode as the TO phonon responsible for ferroelectric order. This exclusive coupling occurs only with above-gap electronic transition and is absent in the valence band as revealed by resonant inelastic X-ray scattering. Our findings suggest a new role of the soft TO phonon mode in electronic and optical properties of ferroelectric semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

Quantum Noise Spectroscopy of Criticality in an Atomically Thin Magnet

Dynamic critical fluctuations in magnetic materials encode important information about magnetic ordering in the associated critical exponents. Using nitrogen-vacancy centers in diamond, we implement $T_2$ (spin-decoherence) noise magnetometry to study critical dynamics in a 2D Van der Waals magnet CrSBr. By analyzing NV decoherence on time scales approaching the characteristic correlation time $τ_c$ of critical fluctuations, we extract the critical exponent $ν$ for the correlation length. Our result deviates from the Ising prediction and highlights the role of long-range dipolar interactions in 2D CrSBr. Furthermore, analyzing the divergence of the correlation length suggests the possibility of 2D-XY criticality in CrSBr in a temperature window near $T_C$ where static magnetic domains are absent. Our work provides a first demonstration of $T_2$ noise magnetometry to quantitatively analyze critical scaling behavior in 2D materials.

cond-mat.mes-hall↗

arXiv2024

Imaging strain-controlled magnetic reversal in thin CrSBr

Two-dimensional materials are extraordinarily sensitive to external stimuli, making them ideal for studying fundamental properties and for engineering devices with new functionalities. One such stimulus, strain, affects the magnetic properties of the layered magnetic semiconductor CrSBr to such a degree that it can induce a reversible antiferromagnetic-to-ferromagnetic phase transition. Given the pervasiveness of non-uniform strain in exfoliated two-dimensional magnets, it is crucial to understand its impact on their magnetic behavior. Using scanning SQUID-on-lever microscopy, we directly image the effects of spatially inhomogeneous strain on the magnetization of layered CrSBr as it is polarized by a field applied along its easy axis. The evolution of this magnetization and the formation of domains is reproduced by a micromagnetic model, which incorporates the spatially varying strain and the corresponding changes in the local interlayer exchange stiffness. The observed sensitivity to small strain gradients along with similar images of a nominally unstrained CrSBr sample suggest that unintentional strain inhomogeneity influences the magnetic behavior of exfoliated samples and must be considered in the design of future devices.

cond-mat.mes-hall↗

arXiv2024

Frustrated hopping from orbital decoration of a primitive two-dimensional lattice

Materials hosting flat electronic bands are a central focus of condensed matter physics as promising venues for novel electronic ground states. Two-dimensional (2D) geometrically frustrated lattices such as the kagome, dice, and Lieb lattices are attractive targets in this direction, anticipated to realize perfectly flat bands. Synthesizing these special structures, however, poses a formidable challenge, exemplified by the absence of solid-state materials realizing the dice and Lieb lattices. An alternative route leverages atomic orbitals to create the characteristic electron hopping of geometrically frustrated lattices. This strategy promises to expand the list of candidate materials to simpler structures, but is yet to be demonstrated experimentally. Here, we report the realization of frustrated hopping in the van der Waals (vdW) intermetallic Pd$_5$AlI$_2$, emerging from orbital decoration of a primitive square lattice. Using angle-resolved photoemission spectroscopy and quantum oscillations measurements, we demonstrate that the band structure of Pd$_5$AlI$_2$ includes linear Dirac-like bands intersected at their crossing point by a flat band, essential characteristics of frustrated hopping in the Lieb and dice lattices. Moreover, Pd$_5$AlI$_2$ is exceptionally stable, with the unusual bulk band structure and metallicity persisting in ambient conditions down to the monolayer limit. Our ability to realize an electronic structure characteristic of geometrically frustrated lattices establishes orbital decoration of primitive lattices as a new approach towards electronic structures that remain elusive to prevailing lattice-centric searches.

cond-mat.str-el↗

arXiv2024

Uniaxial plasmon polaritons $\textit{via}$ charge transfer at the graphene/CrSBr interface

Graphene is a privileged 2D platform for hosting confined light-matter excitations known as surface plasmon-polaritons (SPPs), as it possesses low intrinsic losses with a high degree of optical confinement. However, the inherently isotropic optical properties of graphene limit its ability to guide and focus SPPs, making it less suitable than anisotropic elliptical and hyperbolic materials as a platform for polaritonic lensing and canalization. Here, we present the graphene/CrSBr heterostructure as an engineered 2D interface that hosts highly anisotropic SPP propagation over a wide range of frequencies in the mid-infrared and terahertz. Using a combination of scanning tunneling microscopy (STM), scattering-type scanning near-field optical microscopy (s-SNOM), and first-principles calculations, we demonstrate mutual doping in excess of 10$^{13}$ cm$^{-2}$ holes/electrons between the interfacial layers of graphene/CrSBr heterostructures. SPPs in graphene activated by charge transfer interact with charge-induced anisotropic intra- and interband transitions in the interfacial doped CrSBr, leading to preferential SPP propagation along the quasi-1D chains that compose each CrSBr layer. This multifaceted proximity effect both creates SPPs and endows them with anisotropic transport and propagation lengths that differ by an order-of-magnitude between the two in-plane crystallographic axes of CrSBr.

cond-mat.mes-hall↗