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Marcos H. D. Guimarães

Publications and source records attributed to Marcos H. D. Guimarães.

At least 19 recordsLinked to original sources

Magnetic field induced modulation of heat transport in CrPS$_4$ probed by TaIrTe$_4$ transverse Seebeck thermometry

Understanding and controlling heat flow in low-dimensional magnetic materials is central to thermoelectrics and spin caloritronics. One of the challenges is the absence of sensitive probes of small, field-dependent modulations in thermal transport. Here we demonstrate transverse Seebeck thermometry using exfoliated TaIrTe$_4$ as a probe of thermal conductivity modulated by an external magnetic field on a van der Waals magnet, CrPS$_4$. With a temperature gradient oriented at $45^\circ$ to its principal crystallographic axes, TaIrTe$_4$ exhibits a transverse thermopower exceeding $200~\mathrm{μV\,K^{-1}}$ for 900 nm wide and 30 $μ$m long electrodes, enabling precise detection of variations in the local temperature gradients. Exploiting this with CrPS$_4$ in a nonlocal geometry, we resolve distinct field dependent thermal conductivity changes associated with both the spin-flip and spin-flop magnetic transitions which we attribute to variations in the magnon$-$phonon coupling in CrPS$_4$. At 5 K, the transverse Seebeck response is modulated by more than 8$\%$ by an external magnetic field, demonstrating strong magnetic control of heat transport in CrPS$_4$. This all van der Waals platform offers high sensitivity to modulations of thermal conductivity and a broad adaptability to a wide range of exfoliated magnetic systems.

cond-mat.mes-hall↗

Observation of room temperature intrinsic nonlinear thermoelectric effects in low-dimensional semimetals

Nonreciprocal control of thermoelectric responses offers a promising strategy for next-generation thermal-management and energy-conversion. While nonlinear electrical transport has recently emerged as an intrinsic property of low-symmetry quantum materials, their thermoelectric counterparts have not been demonstrated. Here, exploiting harmonic detection with gradient-reversal techniques, we report intrinsic nonlinear thermoelectric responses up to room temperature in the low-symmetry type-II Weyl semimetals $T_\mathrm{d}$-WTe$_2$ and TaIrTe$_4$ in the absence of magnetic fields or magnetic materials. We resolve all symmetry-allowed components of the second-order thermoelectric tensor, including the nonlinear Seebeck, nonlinear Nernst, and nonlinear mixed-directional thermoelectric effects and demonstrate that both Berry-curvature-related and scattering-induced contributions govern the different nonlinear thermoelectric responses. Our results show that nonlinear thermoelectricity arises intrinsically from reduced crystal symmetry and that engineering effects related to scattering in these materials provides a versatile platform for exploring higher-order heat-to-charge current conversion beyond the linear response.

cond-mat.mes-hall↗

Effect of pressure on the magnetic properties of (Co$_{0.5}$Fe$_{0.5}$)$_5$GeTe$_2$

Cobalt-doped Fe$_5$GeTe$_2$ possesses a rich magnetic phase diagram as a function of Co concentration. The nature of magnetic order in (Co$_{0.5}$Fe$_{0.5}$)$_5$GeTe$_2$ is especially interesting, as it has been shown to exhibit ferromagnetic order, A-type antiferromagnetic (AFM) order, or potentially both at the same time. Here we present magnetoresistance measurements on antiferromagnetic (Co$_{0.5}$Fe$_{0.5}$)$_5$GeTe$_2$ at a series of pressures and extract the anisotropy and interlayer exchange fields using the two-sublattice model. We show a 50 % increase of the interlayer exchange at 2 GPa, highlighting the sensitivity of magnetic properties to interlayer distance. In addition, we find that the sharp hysteretic transitions observed within the AFM state can be qualitatively described by a linear chain model, which suggests an even-odd effect as a function of layer number instead of a coexisting ferromagnetic phase.

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Valley-controlled many-body exciton interactions in monolayer WSe$_2$ phototransistors

Many-body exciton interactions shape the optoelectronic response of atomically-thin transition metal dichalcogenides, yet optical control of these interactions remains largely unexplored. To date, modulation of exciton-exciton interactions has primarily relied on electrical gating or van der Waals engineering. Here, we demonstrate all-optical control of many-body exciton interactions in monolayer WSe$_2$ via valley-selective excitation using polarization-resolved pulsed-laser photocurrent spectroscopy. Circular excitation selectively populates excitons in a single valley, whereas linear excitation populates both valleys, inducing a valley-dependent nonlinear photoresponse. We observe helicity-dependent exciton renormalization, alongside a two-fold enhancement of sublinear photocurrent scaling under circular excitation, reflecting single-valley population of interacting excitons. A microscopic model incorporating intervalley-exchange and exciton-exciton annihilation mediated by dark and bright exciton populations reproduces the nonlinear valley-selective response. These results establish the valley degree of freedom as an all-optical control parameter for tuning many-body excitonic effects and, exploring correlated exciton states and valleytronic applications in two-dimensional semiconductors.

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Impact of current-induced magnons on spin-orbit torque analysis

The second-harmonic Hall technique is a widely used, sensitive method for studying the spin-orbit torques generated by charge current. It exploits the dependence of the Hall resistance on the magnetization direction, although thermal phenomena also contribute. Historically, deviations from the expected magnetic field dependence have usually been neglected. Based on our studies on permalloy/platinum bilayers, we show that a counterpart to the magnon-related spin-flip unidirectional magnetoresistance - known to appear in the second-harmonic longitudinal resistance - appears in the Hall data, and that describing the results in a wide field range with these contributions is essential to accurately estimate the torques.

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Room Temperature Anisotropic Photoresponse in Low-Symmetry van der Waals Semiconductor CrPS$_4$

The crystalline and optical anisotropy of low-symmetry two-dimensional (2D) materials can enable strong dichroic responses, enhancing polarization contrast for photonic and optoelectronic devices. Here, we unveil pronounced optical and optoelectronic anisotropy in chromium thiophosphate CrPS$_4$ arising from the strong coupling between light polarization and its intrinsic crystal symmetry. Linearly polarized reflectivity and scanning photocurrent measurements in the 1.37-2.48 eV range reveal a robust dichroic response. The linear dichroism in reflection RLD reaches ~50, while in photocurrent PCLD it increases to ~60, with a sign reversal of the RLD between 1.6-1.8 eV, enabling strong narrow-band polarization contrast at room temperature. We attribute these anisotropic responses to the interaction between polarized light and Cr$^{3+}$ d-orbital T$_1$ and T$_2$ transitions. Spatially resolved photocurrent mapping further shows that the photocurrent is strongly dependent on the crystallographic axis: a 3-fold enhancement is obtained along the b-axis compared to the a-axis, yielding a clear 180° modulation of photoresponse across different contact orientations. Together, our findings establish CrPS$_4$ as a highly anisotropic 2D semiconductor with strong linear dichroism and polarization-sensitive photoresponse at room temperature. These characteristics highlight CrPS4 as a promising platform for narrow-band polarized photodetectors, anisotropic photo-transport, and future 2D spintronic and magneto-optical devices.

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Unveiling Photoluminescence Signatures of Magneto-Optical Coupling in Layered Hybrid Manganese Chloride Perovskites

Understanding the interplay between magnetic ordering and light emission is crucial for developing magneto-optical technologies. However, this phenomenon is poorly understood since observations of this coupling vary significantly across materials. In this context, hybrid organic-inorganic metal halide perovskites (HOIPs) that incorporate Mn2+ ions are a chemically and structurally tunable platform for exploring this phenomenon, since they exhibit magnetic ordering and photoluminescence (PL) emission. Here, we study two antiferromagnetic Mn-based HOIPs with different organic cations that result in distinct lattice stiffness, Mn2+-Mn2+ distance and octahedral distortion. Temperature-dependent PL excitation spectroscopy reveals changes in crystal field splitting energy and Racah parameters well above the Néel temperature (TN), indicating the emergence of Mn2+-Mn2+ magnetic interactions prior to reach long-range magnetic ordering. These variations align with the observed changes in temperature-PL evolution. The compound with a more rigid lattice shows stronger changes closer to TN, suggesting combined effects of magnetic polarons and spin-canting. In contrast, magnetic polaron-induced magnetic modifications prevail in the HOIP with a softer lattice. These results reveal the complexity of the magneto-optical coupling in Mn-based HOIPs and provide new insights into this field extensible to other 2D materials that exhibit this phenomenon with potential for advanced magneto-optical applications.

cond-mat.mtrl-sci↗

Atomically-Thin Transition Metal Dichalcogenide Nanolasers: Challenges and Opportunities

Low energy consumption nanolasers are crucial for advancing on-chip integrated optical interconnects and photonic integrated circuits. Monolayer transition metal dichalcogenides (TMDs) have emerged as an energy-efficient alternative to traditional semiconductor materials for nanolaser optical gain medium, promising ultralow lasing threshold powers. While several studies suggest that TMDs meet the criteria for lasing, whether true lasing has been achieved remains a topic of heavy debate within the scientific community. In this perspective, we offer an overview of the field, outlining the key characteristics of laser light and methods for testing these properties in TMD-based devices. We then conduct a thorough review of recent reports claiming lasing, assessing the findings against established criteria for laser light emission. Finally, we discuss future research directions and applications, highlighting the key challenges that must be addressed to realize practical TMD-based nanolasers.

physics.optics↗

Roadmap on Quantum Magnetic Materials

Fundamental research on two-dimensional (2D) magnetic systems based on van der Waals materials has been gaining traction rapidly since their recent discovery. With the increase of recent knowledge, it has become clear that such materials have also a strong potential for applications in devices that combine magnetism with electronics, optics, and nanomechanics. Nonetheless, many challenges still lay ahead. Several fundamental aspects of 2D magnetic materials are still unknown or poorly understood, such as their often-complicated electronic structure, optical properties, and magnetization dynamics, and their magnon spectrum. To elucidate their properties and facilitate integration in devices, advanced characterization techniques and theoretical frameworks need to be developed or adapted. Moreover, developing synthesis methods which increase critical temperatures and achieve large-scale, high-quality homogeneous thin films is crucial before these materials can be used for real-world applications. Therefore, the field of 2D magnetic materials provides many challenges and opportunities for the discovery and exploration of new phenomena, as well as the development of new applications. This Roadmap presents the background, challenges, and potential research directions for various relevant topics in the field on the fundamentals, synthesis, characterization, and applications. We hope that this work can provide a strong starting point for young researchers in the field and provide a general overview of the key challenges for more experienced researchers.

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Light-matter interactions in layered materials and heterostructures: from moiré physics and magneto-optical effects to ultrafast dynamics and hybrid meta-photonics

Layered two-dimensional (2D) materials have revolutionized how we approach light-matter interactions, offering unprecedented optical and electronic properties with the potential for vertical heterostructures and manipulation of spin-valley degrees of freedom. The discovery of moiré physics in twisted heterostructures has further unlocked new possibilities for controlling the band structure of tailored semiconductor heterostructures. In parallel, the integration of 2D materials with hybrid photonic structures and ultrafast studies on their optical and spin-valley properties has revealed a wealth of novel physical phenomena. This perspective highlights the recent advances in our understanding of light-matter interactions in moiré and 2D systems, with a particular emphasis on ultrafast processes and the integration of these materials into photonic platforms. We explore the implications for optoelectronics and emerging photonic technologies, positioning 2D materials as a transformative tool for next-generation devices.

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Spin Hall magnetoresistance in Pt/(Ga,Mn)N devices

Diluted magnetic semiconductors (DMS) have attracted significant attention for their potential in spintronic applications. Particularly, magnetically-doped GaN is highly attractive due to its high relevance for the CMOS industry and the possibility of developing advanced spintronic devices which are fully compatible with the current industrial procedures. Despite this interest, there remains a need to investigate the spintronic parameters that characterize interfaces within these systems. Here, we perform spin Hall magnetoresistance (SMR) measurements to evaluate the spin transfer at a Pt/(Ga,Mn)N interface. We determine the transparency of the interface through the estimation of the real part of the spin mixing conductance finding $G_r = 2.6\times 10^{14} \, Ω^{-1} m^{-2}$, comparable to state-of-the-art yttrium iron garnet (YIG)/Pt interfaces. Moreover, the magnetic ordering probed by SMR above the (Ga,Mn)N Curie temperature TC provides a broader temperature range for the efficient generation and detection of spin currents, relaxing the conditions for this material to be applied in new spintronic devices.

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Locally Phase-Engineered MoTe$_2$ for Near-Infrared Photodetectors

Transition metal dichalcogenides (TMDs) are ideal systems for two-dimensional (2D) optoelectronic applications, owing to their strong light-matter interaction and various band gap energies. New techniques to modify the crystallographic phase of TMDs have recently been discovered, allowing the creation of lateral heterostructures and the design of all-2D circuitry. Thus far, the potential benefits of phase-engineered TMD devices for optoelectronic applications are still largely unexplored. The dominant mechanisms involved in the photocurrent generation in these systems remain unclear, hindering further development of new all-2D optoelectronic devices. Here, we fabricate locally phase-engineered MoTe$_{2}$ optoelectronic devices, creating a metal (1T') semiconductor (2H) lateral junction and unveil the main mechanisms at play for photocurrent generation. We find that the photocurrent originates from the 1T'-2H junction, with a maximum at the 2H MoTe$_{2}$ side of the junction. This observation, together with the non-linear IV-curve, indicates that the photovoltaic effect plays a major role on the photon-to-charge current conversion in these systems. Additionally, the 1T'-2H MoTe$_{2}$ heterojunction device exhibits a fast optoelectronic response over a wavelength range of 700 nm to 1100 nm, with a rise and fall times of 113 $μ$s and 110 $μ$s, two orders of magnitude faster when compared to a directly contacted 2H MoTe$_{2}$ device. These results show the potential of local phase-engineering for all-2D optoelectronic circuitry.

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Crystallographic-dependent bilinear magnetoelectric resistance in a thin WTe$_2$ layer

The recently reported Bilinear Magnetoeletric Resistance (BMR) in novel materials with rich spin textures, such as bismuth selenide (Bi$_2$Se$_3$) and tungsten ditelluride (WTe$_2$), opens new possibilities for probing the spin textures via magneto-transport measurements. By its nature, the BMR effect is directly linked to the crystal symmetry of the materials and its spin texture. Therefore, understanding the crystallographic dependency of the effect is crucial. Here we report the observation of crystallographic-dependent BMR in thin WTe$_2$ layers and explore how it is linked to its spin textures. The linear response measured in first harmonic signals and the BMR measured in second harmonic signals are both studied under a wide range of magnitudes and directions of magnetic field, applied current and at different temperatures. We discover a three-fold symmetry contribution of the BMR when current is applied along the a-axis of the WTe$_2$ thin layer at 10 K, which is absent for when current is applied along the b-axis.

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Charge dynamics in the 2D/3D semiconductor heterostructure WSe$_2$/GaAs

Understanding the relaxation and recombination processes of excited states in two-dimensional (2D)/three-dimensional (3D) semiconductor heterojunctions is essential for developing efficient optical and (opto)electronic devices which integrate new 2D materials with more conventional 3D ones. In this work, we unveil the carrier dynamics and charge transfer in a monolayer of WSe$_2$ on a GaAs substrate. We use time-resolved differential reflectivity to study the charge relaxation processes involved in the junction and how they change when compared to an electrically decoupled heterostructure, WSe$_2$/hBN/GaAs. We observe that the monolayer in direct contact with the GaAs substrate presents longer optically-excited carrier lifetimes (3.5 ns) when compared with the hBN-isolated region (1 ns), consistent with a strong reduction of radiative decay and a fast charge transfer of a single polarity. Through low-temperature measurements, we find evidence of a type-II band alignment for this heterostructure with an exciton dissociation that accumulates electrons in the GaAs and holes in the WSe$_2$. The type-II band alignment and fast photo-excited carrier dissociation shown here indicate that WSe$_2$/GaAs is a promising junction for new photovoltaic and other optoelectronic devices, making use of the best properties of new (2D) and conventional (3D) semiconductors.

cond-mat.mes-hall↗

The Role of Self-Torques in Transition Metal Dichalcogenide/Ferromagnet Bilayers

Recently, transition metal dichalcogenides (TMDs) have been extensively studied for their efficient spin-orbit torque generation in TMD/ferromagnetic bilayers, owing to their large spin-orbit coupling, variety in crystal symmetries, and pristine interfaces. Although the TMD layer was considered essential for the generation of the observed SOTs, recent reports show the presence of a self-torque in single-layer ferromagnetic devices with magnitudes comparable to TMD/ferromagnetic devices. Here, we perform second-harmonic Hall SOT measurements on metal-organic chemical vapor deposition (MOCVD) grown MoS$_{2}$/permalloy/Al$_{2}$O$_{3}$ devices and compare them to a single-layer permalloy/Al$_{2}$O$_{3}$ device to accurately disentangle the role of self-torques from contributions from the TMD layer. We report a damping-like self-torque conductivity of opposite sign in our single-layer permalloy/Al$_{2}$O$_{3}$ device compared to one MoS$_{2}$/permalloy/Al$_{2}$O$_{3}$ device, and find no significant one for all other MoS$_{2}$/permalloy/Al$_{2}$O$_{3}$ devices. This indicates a competition between the self-torque and the torque arising from the TMD layer, which would reduce the observed torque in these bilayers. In addition, we find a field-like spin-torque conductivity of comparable magnitude to control MoS$_{2}$/permalloy/Al$_{2}$O$_{3}$ devices, indicating only a minor role of the MoS$_{2}$ layer. Finally, we find a linear dependence of the SOT conductivity on the Hall bar leg/channel width ratio of our devices, indicating that the Hall bar dimensions are of significant importance for the reported SOT strength. Our results accentuate the importance of delicate details, like device asymmetry, Hall bar dimensions, and self-torque generation, for the correct disentanglement of the microscopic origins underlying the SOTs, essential for future energy-efficient spintronic applications.

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Magnetic field control of light-induced spin accumulation in monolayer MoSe$_2$

Semiconductor transition metal dichalcogenides (TMDs) have equivalent dynamics for their two spin/valley species. This arises from their energy-degenerated spin states, connected via time-reversal symmetry. When an out-of-plane magnetic field is applied, time-reversal symmetry is broken and the energies of the spin-polarized bands shift, resulting in different bandgaps and dynamics in the K$_+$ and K$_-$ valleys. Here, we use time-resolved Kerr rotation to study the magnetic field dependence of the spin dynamics in monolayer MoSe$_2$. We show that the magnetic field can control the light-induced spin accumulation of the two valley states, with a small effect on the recombination lifetimes. We unveil that the magnetic field-dependent spin accumulation is in agreement with hole spin dynamics at the longer timescales, indicating that the electron spins have faster relaxation rates. We propose a rate equation model that suggests that lifting the energy-degeneracy of the valleys induces an ultrafast spin-flip toward the stabilization of the valley with the higher valence band energy. Our results provide an experimental insight into the ultrafast charge and spin dynamics in TMDs and a way to control it, which will be useful for the development of new spintronic and valleytronic applications.

cond-mat.mes-hall↗

Unconventional spin Hall effects in nonmagnetic solids

Direct and inverse spin Hall effects lie at the heart of novel applications that utilize spins of electrons as information carriers, allowing generation of spin currents and detecting them via the electric voltage. In the standard arrangement, applied electric field induces transverse spin current with perpendicular spin polarization. Although conventional spin Hall effects are commonly used in spin-orbit torques or spin Hall magnetoresistance experiments, the possibilities to configure electronic devices according to specific needs are quite limited. Here, we investigate unconventional spin Hall effects that have the same origin as conventional ones, but manifest only in low-symmetry crystals where spin polarization, spin current and charge current are not enforced to be orthogonal. Based on the symmetry analysis for all 230 space groups, we have identified crystal structures that could exhibit unusual configurations of charge-to-spin conversion. The most relevant geometries have been explored in more detail; in particular, we have analyzed the collinear components yielding transverse charge and spin current with spin polarization parallel to one of them, as well as the longitudinal ones, where charge and spin currents are parallel. In addition, we have demonstrated that unconventional spin Hall effect can be induced by controllable breaking the crystal symmetries by an external electric field, which opens a perspective for external tuning of spin injection and detection by electric fields. The results have been confirmed by density functional theory calculations performed for various materials relevant for spintronics. We are convinced that our findings will stimulate further computational and experimental studies of unconventional spin Hall effects.

cond-mat.mtrl-sci↗

Anisotropic Laser-Pulse-Induced Magnetization Dynamics in van der Waals Magnet Fe$_3$GeTe$_2$

Femtosecond laser-pulse excitation provides an energy efficient and fast way to control magnetization at the nanoscale, providing great potential for ultrafast next-generation data manipulation and nonvolatile storage devices. Ferromagnetic van der Waals materials have garnered much attention over the past few years due to their low dimensionality, excellent magnetic properties, and large response to external stimuli. Nonetheless, their behaviour upon fs laser-pulse excitation remains largely unexplored. Here, we investigate the ultrafast magnetization dynamics of a thin flake of Fe$_3$GeTe$_2$ (FGT) and extract its intrinsic magnetic properties using a microscopic framework. We find that our data is well described by our modelling, with FGT undergoing a slow two-step demagnetization, and we experimentally extract the spin-relaxation timescale as a function of temperature, magnetic field and excitation fluence. Our observations indicate a large spin-flip probability in agreement with a theoretically expected large spin-orbit coupling, as well as a weak interlayer exchange coupling. The spin-flip probability is found to increase when the magnetization is pulled away from its quantization axis, opening doors to an external control over the spins in this material. Our results provide a deeper understanding of the dynamics van der Waals materials upon fs laser-pulse excitation, paving the way towards two-dimensional materials-based ultrafast spintronics.

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