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David G. Mandrus

Publications and source records attributed to David G. Mandrus.

At least 19 recordsLinked to original sources

Strain-Induced Relaxor Multiferroicity at Room Temperature in Hexaferrite BaFe12O19 Thin Films

Multiferroic materials that combine magnetic and electric order at room temperature are rare. Here, we demonstrate strain-induced room-temperature polar order in the ferrimagnetic hexaferrite BaFe12O19. First-principles calculations reveal a strain-tunable energy landscape with multiple competing dipolar configurations and predict that compressive strain favors polar distortions. Using an isostructural Sr1.03Ga10.81Mg0.58Zr0.58O19 substrate, we grow coherently strained BaFe12O19 films with 1.1% in-plane biaxial compression. Second-harmonic generation measurements demonstrate inversion-symmetry breaking and establish a strain-stabilized polar phase that persists to at least 1000 K. Multislice electron ptychography directly reveals enhanced off-centering of Fe3+ ions within the trigonal-bipyramidal sites of the strained films and spatially varying local polarization, demonstrating the formation of polar nanoregions. Path-integral Monte Carlo simulations further show that compressive strain suppresses quantum fluctuations and stabilizes these local polar distortions. Together, these results establish strain-engineered BaFe12O19 as a room-temperature relaxor multiferroic, in which robust ferrimagnetism coexists with nanoscale polar order. Our work demonstrates a route for transforming an incipient ferroelectric ferrimagnetic into a polar magnetic material through epitaxial strain.

cond-mat.mtrl-sci

Complex electronic topography and magnetotransport in an in-plane ferromagnetic kagome metal

The intricate interplay between flat bands, Dirac cones, and magnetism in kagome materials has recently attracted significant attention from materials scientists, particularly in compounds belonging to the RMn6Sn6 family (R = Sc, Y, rare earths), due to their inherent magnetic frustration. Here, we present a detailed investigation of the ferromagnetic (FM) kagome magnet ScMn6(Sn0.78Ga0.22)6 using angle-resolved photoemission spectroscopy (ARPES), magnetotransport measurements, and density functional theory (DFT) calculations. Our findings reveal a paramagnetic-to-FM transition at 375 K, with the in-plane direction serving as the easy magnetization axis. Notably, ARPES measurements reveal a Dirac cone near the Fermi energy, while the Hall resistivity exhibits a substantial contribution from the anomalous Hall effect. Additionally, we observe a flat band spanning a substantial portion of the Brillouin zone, arising from the destructive interference of wave functions in the Mn kagome lattice. Theoretical calculations reveal that the gap in the Dirac cone can be modulated by altering the orientation of the magnetic moment. An out-of-plane orientation produces a gap of approximately 15 meV, while an in-plane alignment leads to a gapless state, as corroborated by ARPES measurements. This comprehensive analysis provides valuable insights into the electronic structure of magnetic kagome materials and paves the way for exploring novel topological phases in this material class.

cond-mat.mtrl-sci

Observation of magnetically switchable quantum geometric photocurrents

In non-centrosymmetric materials, light can be rectified into two types of DC photocurrents, known as injection and shift currents, through the bulk photovoltaic effect. Recent theory has uncovered their deep relation with the two-state quantum geometry of resonant transitions: In non-magnetic crystals, where these currents have been routinely observed, the injection current responds to circular light and probes the Berry curvature, while the shift current responds to linear light and probes the geometric connection. Magnetic crystals have been predicted to show a new set of hitherto unobserved magnetically switchable photocurrents, with the roles of linear and circular light interchanged: A linear injection current, which probes the quantum metric, and a circular shift current, which probes the geometric torsion. In this work, we demonstrate the existence of such currents for the first time, demonstrating the switching of the current by flipping the Néel vector in a van der Waals antiferromagnet. Furthermore, their specific frequency and temperature dependence confirm the assignment of circular shift and linear injection currents. Our work demonstrates a new way to control photocurrents in magnets that are directly tied to geometry and have promising applications in antiferromagnetic spintronics and light harvesting.

cond-mat.mtrl-sci

Crystallizing electrons with artificially patterned lattices

Wigner crystals are typically confined to ultralow temperatures where thermal motion is frozen out. Moiré superlattices in twisted two-dimensional materials have extended their stability to higher temperatures and densities, but rely on delicate stacking that fixes the lattice geometry and limits tunability. Here we demonstrate a lithographic approach that bypasses these constraints. Using high-resolution nanofabrication, we pattern a nanoscale triangular lattice directly into a graphene gate integrated with a monolayer MoSe2 semiconductor. This engineered potential landscape localizes electrons into generalized Wigner crystal states that persist up to 15 K and densities of 2X10^12 cm-2, representing an order of magnitude improvement over pristine monolayer MoSe2. Gate-voltage control allows real-time switching between stable and unstable crystalline states, with the latter exhibiting stochastic telegraph noise from nearly degenerate configurations. This work demonstrates the ability of this platform to transform Wigner crystals from fragile, static phases into reconfigurable quantum matter.

cond-mat.mes-hall

Dynamic Interfacial Quantum Dipoles in Charge Transfer Heterostructures

Hysteretic gate responses of two-dimensional material heterostructures serve as sensitive probes of the underlying electronic states and hold significant promise for the development of novel nanoelectronic devices. Here we identify a new mechanism of hysteretic behavior in graphene/$h$BN/$α$-$\mathrm{RuCl_3}$ charge transfer field effect devices. The hysteresis loop exhibits a sharp onset under low temperatures and evolves symmetrically relative to the charge transfer equilibrium. Unlike conventional flash memory devices, the charge transfer heterostructure features a transparent tunneling barrier and its hysteretic gate response is induced by the dynamic tuning of interfacial dipoles originating from quantum exchange interactions. The system acts effectively as a ferroelectric and gives rise to remarkable tunability of the hysteretic gate response under external electrical bias. Our work unveils a novel mechanism for engineering hysteretic behaviors via dynamic interfacial quantum dipoles.

cond-mat.mes-hall

Diverse electronic landscape of the kagome metal YbTi3Bi4

Kagome lattices have emerged as an ideal platform for exploring exotic quantum phenomena in materials. Here, we report the discovery of Ti-based kagome metal YbTi3Bi4 which we characterize using angle-resolved photoemission spectroscopy (ARPES) and magneto-transport, in combination with density functional theory calculations. Our ARPES results reveal the complex fermiology of YbTi3Bi4 and provide spectroscopic evidence of four flat bands. Our measurements also show the presence of multiple van Hove singularities originating from Ti 3d orbitals and a linearly-dispersing gapped Dirac-like bulk state at the K point in accord with our theoretical calculations. Our study establishes YbTi3Bi4 as a platform for exploring exotic phases in the wider LnTi3Bi4 (Ln= lanthanide) family of materials.

cond-mat.mes-hall

Cryogenic Nano-Imaging of Excitons in a Monolayer Semiconductor

Excitons, Coulomb bound electron-hole pairs, dominate the optical response of two-dimensional semiconductors across near-infrared and visible frequencies due to their large binding energy and prominent oscillator strength. Previous measurements of excitons in 2D semiconductors have primarily relied on far-field optical spectroscopy techniques which are diffraction limited to several hundred nanometers. To precisely image nanoscale spatial disorder requires an order of magnitude increase in resolution capabilities. Here, we present a study of the exciton spectra of monolayer MoSe2 in the visible range using a cryogenic scattering-type scanning near field optical microscope (s-SNOM) operating down to 11 K. By mapping the spatial variation in the exciton resonance across an hBN encapsulated MoSe2 monolayer, we achieve sub-50 nm spatial resolution and energy resolution below 1 meV. We further investigate the material's near-field spectra and dielectric function, demonstrating the ability of cryogenic visible s-SNOM to reveal nanoscale disorder. Comparison to room temperature measurements illustrate the enhanced capabilities of cryogenic s-SNOM to reveal fine-scale material heterogeneity.

cond-mat.mes-hall

Diverse Magnetic Phase Diagram and Anomalous Hall Effect in Antiferromagetic LuMn$_6$Sn$_6$

The interactions between conduction electrons and magnetism can significantly enhance the Hall signal, a phenomenon known as the anomalous Hall effect (AHE). While the AHE is generally not expected in antiferromagnets, a large AHE is observed in certain antiferromagnets with noncollinear spin textures and nonvanishing Berry curvature. In this work, we present a rich temperature and magnetic phase diagram with eight distinct magnetic phases for the antiferromagnetic kagome compound LuMn$_6$Sn$_6$. The Hall effect analysis in LuMn$_6$Sn$_6$ reveals both intriguing physical phenomena and methodological challenges. In the coplanar canted antiferromagnetic phase, we observe an AHE, which likely originates from the intrinsic effects. At low temperatures, upon entering the ferromagnetic phase, the AHE sharply increases and exceeds the conventional limits expected from intrinsic mechanisms. We also demonstrate the limitations of standard experimental methods in extracting the topological contribution to the Hall effect data. We show the importance of considering magnetoresistance anisotropy when estimating the anomalous and topological Hall effects. These shortcomings in current approaches in partitioning the Hall response necessitate new tools to interpret transport results in complex magnetic materials such as LuMn$_6$Sn$_6$.

cond-mat.str-el

Diverse electronic topography in a distorted kagome metal LaTi3Bi4

Recent reports on a family of kagome metals of the form LnTi3Bi4 (Ln = Lanthanide) has stoked interest due to the combination of highly anisotropic magnetism and a rich electronic structure. The electronic structure near the Fermi level is proposed to exhibit Dirac points and van Hove singularities. In this manuscript, we use angle resolved photoemission spectroscopy measurements in combination with density functional theory calculations to investigate the electronic structure of a newly discovered kagome metal LaTi3Bi4. Our results reveal multiple van Hove singularities (VHSs) with one VHS located in the vicinity of the Fermi level. We clearly observe two flat bands, which originate from the destructive interference of wave functions within the Ti kagome motif. These flat bands and VHSs originate from Ti d orbitals and are very responsive to the polarization of the incident beam. We notice a significant anisotropy in the electronic structure, resulting from the breaking of six fold rotational symmetry in this material. Our findings demonstrate this new family of Ti based kagome material as a promising platform to explore novel emerging phenomena in the wider LnTi3Bi4 (Ln= lanthanide) family of materials.

cond-mat.mtrl-sci

Spontaneously formed phonon frequency combs in van der Waals solid CrXTe$_3$ (X=Ge,Si)

Optical phonon engineering through nonlinear effects has been utilized in ultrafast control of material properties. However, nonlinear optical phonons typically exhibit rapid decay due to strong mode-mode couplings, limiting their effectiveness in temperature or frequency sensitive applications. In this study, we report the observation of long-lived nonlinear optical phonons through the spontaneous formation of phonon frequency combs in the van der Waals material CrXTe$_3$ (X=Ge, Si) using high-resolution Raman scattering. Unlike conventional optical phonons, the highest $A_g$ mode in CrGeTe$_3$ splits into equidistant, sharp peaks forming a frequency comb that persists for hundreds of oscillations and survives up to 100K before decaying. These modes correspond to localized oscillations of Ge$_2$Te$_6$ clusters, isolated from Cr hexagons, behaving as independent quantum oscillators. Introducing a cubic nonlinear term to the harmonic oscillator model, we simulate the phonon time evolution and successfully replicate the observed comb structure. Similar frequency comb behavior is observed in CrSiTe$_3$, demonstrating the generalizability of this phenomenon. Our findings reveal that Raman scattering effectively probes high-frequency nonlinear phonon modes, providing new insight into generating long-lived, tunable phonon frequency combs with applications in ultrafast material control and phonon-based technologies.

cond-mat.mes-hall

Imprinting spin patterns by local strain control in a van der Waals antiferromagnet

Van der Waals magnets provide opportunities for exploring low-dimensional magnetism and spintronic phenomena. The Mermin-Wagner theorem states that long-range correlations in reduced dimensions are stabilized and controlled by magnetic anisotropy. In this study, we meticulously create and control the in-plane easy-axis magnetic anisotropy within two-dimensional (2D) van der Waals antiferromagnet MnPSe3 via a novel method involving topography and therefore strain control by using a micro-patterned substrate. By transposing the MnPSe3 thin flakes onto a substrate patterned with micro-scale grooves, we introduce local uniaxial strain pattern, which not only locks the spin direction to the strain direction but also replicates the groove pattern in the spin orientation distribution. Our approach generates spin orientations that correspond to the substrate patterns, therefore having the potential to significantly advance spintronic devices by offering a unique method for manipulating and designing spin textures in easy-plane magnets.

cond-mat.mtrl-sci

Unconventional Unidirectional Magnetoresistance in vdW Heterostructures

Electrical readout of magnetic states is a key to realize novel spintronics devices for efficient computing and data storage. Unidirectional magnetoresistance (UMR) in bilayer systems, consisting of a spin source material and a magnetic layer, refers to a change in the longitudinal resistance upon the reversal of magnetization, which typically originates from the interaction of spin-current and magnetization at the interface. Because of UMR s linear dependence on applied charge current and magnetization, it can be used to electrically read the magnetization state. However, in conventional spin source materials, the spin polarization of an electric field induced spin current is restricted to be in the film plane and hence the ensuing UMR can only respond to the in plane component of the magnetization. On the other hand, magnets with perpendicular magnetic anisotropy (PMA) are highly desired for magnetic memory and spin-logic devices, while the electrical read out of PMA magnets through UMR is critically missing. Here, we report the discovery of an unconventional UMR in bilayer heterostructures of a topological semimetal (WTe2) and a PMA ferromagnetic insulator (Cr2Ge2Te6, CGT), which allows to electrically read the up and down magnetic states of the CGT layer by measuring the longitudinal resistance. Our theoretical calculations based on a tight binding model show that the unconventional UMR originates from the interplay of crystal symmetry breaking in WTe2 and magnetic exchange interaction across the WTe2 and CGT interface. Combining with the ability of WTe2 to obtain magnetic field free switching of the PMA magnets, our discoveries open an exciting pathway to achieve two terminal magnetic memory devices that operate solely on the spin orbit torque and UMR, which is critical for developing next-generation non volatile and low power consumption data storage technologies.

cond-mat.mes-hall

Magnetic field control of continuous Néel vector rotation and Néel temperature in a van der Waals antiferromagnet

In a collinear antiferromagnet, spins tend to cant towards the direction of an applied magnetic field, thereby decreasing the energy of the system. The canting angle becomes negligible when the magnetic field is small so that the induced anisotropic energy is substantially lower than the exchange energy. However, this tiny anisotropy can play a significant role when the intrinsic anisotropy of the antiferromagnet is small. In our work, we conduct direct imaging of the Néel vector in a two-dimensional easy-plane antiferromagnet, MnPSe$_3$, with negligible spin canting under an external in-plane magnetic field. The small inherent in-plane anisotropy allows for the continuous rotation of the Néel vector by ramping up the magnetic field in samples from the bulk to the monolayer. In monolayer samples, the applied magnetic field elevates the Néel temperature 10$\%$ at 5 tesla, as the combination of intrinsic and field-induced anisotropies set a critical temperature scale for fluctuations of the otherwise disordered Néel vector field. Our study illuminates the contribution of field-induced anisotropy in two dimensional magnets with in-plane anisotropy. We also demonstrate that the strain can tune the spin flop transition field strength by one order of magnitude.

cond-mat.mtrl-sci

Ultra-broadband bright light emission from a one-dimensional inorganic van der Waals material

One-dimensional (1D) van der Waals materials have emerged as an intriguing playground to explore novel electronic and optical effects. We report on inorganic one-dimensional SbPS4 nanotubes bundles obtained via mechanical exfoliation from bulk crystals. The ability to mechanically exfoliate SbPS4 nanobundles offers the possibility of applying modern 2D material fabrication techniques to create mixed-dimensional van der Waals heterostructures. We find that SbPS4 can readily be exfoliated to yield long (> 10 μm) nanobundles with thicknesses that range from of 1.3 - 200 nm. We investigated the optical response of semiconducting SbPS4 nanobundles and discovered that upon excitation with blue light, they emit bright and ultra-broadband red light with a quantum yield similar to that of hBN-encapsulated MoSe2. We discovered that the ultra-broadband red light emission is a result of a large ~1 eV exciton binding energy and a ~200 meV exciton self-trapping energy, unprecedented in previous material studies. Due to the bright and ultra-broadband light emission, we believe that this class of inorganic 1D van der Waals semiconductors has numerous potential applications including on-chip tunable nanolasers, and applications that require ultra-violet to visible light conversion such as lighting and sensing. Overall, our findings open avenues for harnessing the unique characteristics of these nanomaterials, advancing both fundamental research and practical optoelectronic applications.

cond-mat.mtrl-sci

Charge-transfer Contact to a High-Mobility Monolayer Semiconductor

Two-dimensional (2D) semiconductors, such as the transition metal dichalcogenides, have demonstrated tremendous promise for the development of highly tunable quantum devices. Realizing this potential requires low-resistance electrical contacts that perform well at low temperatures and low densities where quantum properties are relevant. Here we present a new device architecture for 2D semiconductors that utilizes a charge-transfer layer to achieve large hole doping in the contact region, and implement this technique to measure magneto-transport properties of high-purity monolayer WSe$_2$. We measure a record-high hole mobility of 80,000 cm$^2$/Vs and access channel carrier densities as low as $1.6\times10^{11}$ cm$^{-2}$, an order of magnitude lower than previously achievable. Our ability to realize transparent contact to high-mobility devices at low density enables transport measurement of correlation-driven quantum phases including observation of a low temperature metal-insulator transition in a density and temperature regime where Wigner crystal formation is expected, and observation of the fractional quantum Hall effect under large magnetic fields. The charge transfer contact scheme paves the way for discovery and manipulation of new quantum phenomena in 2D semiconductors and their heterostructures.

cond-mat.mes-hall

Signatures of Z$_3$ Vestigial Potts-nematic order in van der Waals antiferromagnets

Layered van der Waals magnets have attracted much recent attention as a promising and versatile platform for exploring intrinsic two-dimensional magnetism. Within this broader class, the transition metal phosphorous trichalcogenides $M$P$X_3$ stand out as particularly interesting, as they provide a realization of honeycomb lattice magnetism and are known to display a variety of magnetic ordering phenomena as well as superconductivity under pressure. One example, found in a number of different materials, is commensurate single-$Q$ zigzag antiferromagnetic order, which spontaneously breaks the spatial threefold $(C_3)$ rotation symmetry of the honeycomb lattice. The breaking of multiple distinct symmetries in the magnetic phase suggests the possibility of a sequence of distinct transitions as a function of temperature, and a resulting intermediate $\mathbb{Z}_3$-nematic phase which exists as a paramagnetic vestige of zigzag magnetic order -- a scenario known as vestigial ordering. Here, we report the observation of key signatures of vestigial Potts-nematic order in rhombohedral FePSe$_3$. By performing linear dichroism imaging measurements -- an ideal probe of rotational symmetry breaking -- we find that the $C_3$ symmetry is already broken above the Néel temperature. We show that these observations are explained by a general Ginzburg-Landau model of vestigial nematic order driven by magnetic fluctuations and coupled to residual strain. An analysis of the domain structure as temperature is lowered and a comparison with zigzag-ordered monoclinic FePS$_3$ reveals a broader applicability of the Ginzburg-Landau model in the presence of external strain, and firmly establishes the $M$P$X_3$ magnets as a new experimental venue for studying the interplay between Potts-nematicity, magnetism and superconductivity.

cond-mat.str-el

Universal sublinear resistivity in vanadium kagome materials hosting charge density waves

The recent discovery of a charge density (CDW) state in ScV$_6$Sn$_6$ at $T_{\textrm{CDW}}$ = 91 K offers new opportunities to understand the origins of electronic instabilities in topological kagome systems. By comparing to the isostructural non-CDW compound LuV$_6$Sn$_6$, we unravel interesting electrical transport properties in ScV$_6$Sn$_6$, above and below the charge ordering temperature. We observed that by applying a magnetic field along the $a$ axis, the temperature behavior of the longitudinal resistivity in ScV$_6$Sn$_6$ changes from metal-like to insulator-like above the CDW transition. We show that in the charge ordered state ScV$_6$Sn$_6$ follows the Fermi liquid behavior while above that, it transforms into a non-Fermi liquid phase in which the resistivity varies sublinearly over a broad temperature range. The sublinear resistivity, which scales by $T^{3/5}$ is a common feature among other vanadium-containing kagome compounds exhibiting CDW states such as KV$_3$Sb$_5$, RbV$_3$Sb$_5$, and CsV$_3$Sb$_5$. By contrast, the non-Fermi liquid behavior does not occur in LuV$_6$Sn$_6$. We explain the $T^{3/5}$ universal scaling behavior from the Coulomb scattering between Dirac electrons and Van Hove singularities; common features in the electronic structure of kagome materials. Finally, we show anomalous Hall-like behavior in ScV$_6$Sn$_6$ below $T_{\textrm{CDW}}$, which is absent in the Lu compound. Comparing the transport properties of ScV$_6$Sn$_6$ and LuV$_6$Sn$_6$ is valuable to highlight the impacts of the unusual CDW in the Sc compound.

cond-mat.str-el

Direct visualization of the charge transfer in Graphene/$α$-RuCl$_3$ heterostructure

We investigate the electronic properties of a graphene and $α$-ruthenium trichloride (hereafter RuCl$_3$) heterostructure, using a combination of experimental and theoretical techniques. RuCl$_3$ is a Mott insulator and a Kitaev material, and its combination with graphene has gained increasing attention due to its potential applicability in novel electronic and optoelectronic devices. By using a combination of spatially resolved photoemission spectroscopy, low energy electron microscopy, and density functional theory (DFT) calculations we are able to provide a first direct visualization of the massive charge transfer from graphene to RuCl$_3$, which can modify the electronic properties of both materials, leading to novel electronic phenomena at their interface. The electronic band structure is compared to DFT calculations that confirm the occurrence of a Mott transition for RuCl$_3$. Finally, a measurement of spatially resolved work function allows for a direct estimate of the interface dipole between graphene and RuCl$_3$. The strong coupling between graphene and RuCl$_3$ could lead to new ways of manipulating electronic properties of two-dimensional lateral heterojunction. Understanding the electronic properties of this structure is pivotal for designing next generation low-power opto-electronics devices.

cond-mat.mtrl-sci