arXiv subjects

Daniel A. Rhodes

Publications and source records attributed to Daniel A. Rhodes.

At least 19 recordsLinked to original sources

arXiv2026

Strain engineering of ultrafast magnetism in the room-temperature vdW ferromagnet Fe3GaTe2

Controlling ultrafast magnetic dynamics is critical to understanding nonequilibrium spin interactions and advancing high-speed spintronics. However, a lack of efficient in situ tuning strategies leaves most ultrafast studies largely dependent on the intrinsic properties of the individual materials. Here we demonstrate continuous strain tuning of both the equilibrium magnetic response and ultrafast demagnetization dynamics in the room-temperature van der Waals ferromagnet Fe3GaTe2. Applying up to 4.2% uniaxial tensile strain increases the coercive field from nearly zero to 100 Oe, consistent with an enhancement of the effective perpendicular magnetic anisotropy. Time-resolved magneto-optical Kerr effect measurements further reveal strain-accelerated ultrafast demagnetization, with 1.2% tensile strain reducing the characteristic demagnetization time by approximately 20%. Remarkably, strain accesses an accelerated demagnetization regime that cannot be reached simply by increasing pump fluence in the unstrained sample. Combined with first-principles calculations, our results resolve that the applied strain modifies the spin-lattice energy transfer, leading to the observed accelerated demagnetization. These findings establish mechanical strain as an effective route for on-demand control of ultrafast magnetic dynamics while reducing the required optical energy by reconfiguring the magnetic energy landscape and associated spin-relaxation pathways.

cond-mat.mtrl-sci↗

arXiv2026

Achieving Large Uniaxial and Homogeneous Strain in Two-Dimensional Materials

Strain engineering is a powerful tool for tuning the electronic, magnetic, and topological properties of two-dimensional (2D) materials and thin films - particularly at high values of strain (>3%) where many electronic, magnetic, and structural transitions have been predicted. However, most approaches to tuning strain in 2D materials are limited below 1.5%, with poor repeatability when cycling strain and low strain transfer when cooling to cryogenic temperatures. Here, we report a high-yield sample preparation and device strain platform that overcomes these limitations, enabling precise, reversible strain tuning up to the intrinsic strain-to-failure of the materials tested herein. In addition, we show that this platform can be used to controllably design uniform linear strain gradients across of 10's of $μ$m, providing a novel route to systematically investigate flexoelectric and flexomagnetic phenomena. Using CrSBr as a model system, we demonstrate uniform uniaxial strain, up to ~4%, with negligible slippage and linear strain gradients of up to 0.06%/$μ$m. We further show that our strain approach is applicable to a broad class of 2D materials, validating its performance for three different phases of transition metal dichalcogenides: 2H-MoTe$_2$, 1T$^\prime$-MoTe$_2$ and T$_\mathrm{d}$-WTe$_2$. In T$_\mathrm{d}$-WTe$_2$, verified by theoretical calculations, we show a continuous redshift of the A$_1^3$ mode, up to a record-breaking ~5.5% strain, with a clear separation of the A$_1^3$ and A$_1^2$ modes starting at 2% strain.

cond-mat.mtrl-sci↗

arXiv2026

Adsorption-Controlled Epitaxy and Twin Control of $γ$-GaSe on GaAs (111)B

The III-Se layered semiconductors, including InSe and GaSe, are promising optoelectronic materials due to their relatively high electron mobilities at room temperature, nonlinear optical responses, ferroelectricity, self-passivated van der Waals surfaces, and ability to alloy and synthesize heterostructures for bandgap engineering. Adsorption control is a widely utilized strategy for controlling the stoichiometry and phase formation of these materials; however, the bounds of the adsorption-controlled growth window for GaSe have not been systematically established. Additionally, challenges with control over polytype and twinning remain. Here, we use molecular beam epitaxy to experimentally map the adsorption-controlled growth window of GaSe films on vicinal GaAs (111)B substrates. The observed phase boundaries show qualitative agreement with Ellingham diagram predictions. All films crystallize in the $γ$ ($R3m$) polytype. Increasing growth and annealing temperature leads to decreased mosaicity measured by x-ray rocking curve and smoother surfaces measured by atomic force microscopy, at the expense of a transition from singly oriented $γ$ to twinned $γ$ with $60\degree$ rotated domains.

cond-mat.mtrl-sci↗

arXiv2025

Superconducting Sn-Intercalated TaSe$_2$: Structural Diversity Obscured by Routine Characterization Techniques

Using Sn-intercalated TaSe$_2$ as a model system, we demonstrate the presence of structural heterogeneity captured by single-crystal X-ray diffraction (SCXRD) and scanning transmission electron microscopy (STEM) that eludes the routine characterization techniques of powder X-ray diffraction, Raman spectroscopy, and electronic transport measurements. From a single growth composition (1:1:2 Sn:Ta:Se), we obtained crystals diverse in stoichiometry and structure, with near-continuous intercalation for Sn$_x$TaSe$_2$ from $0\lesssim{x}\lesssim1$. Using SCXRD, we found global structural diversity, identifying three new structure types: Sn$_{0.18}$TaSe$_{2.0}$/Sn$_{0.08}$TaSe$_{1.96}$ ($R3m$), Sn$_{0.16}$TaSe$_{2.0}$ ($P6_3/mmc$), and Sn$_{1.2}$TaSe$_{1.9}$ ($Fmm2$). Using STEM, we observed local structural diversity, manifested as regions of highly variable stacking within a single crystal. In contrast, powder X-ray diffraction did not resolve all observed global structures. Raman spectroscopy was unable to distinguish between different structures or compositions in the standard measurement range. Electronic transport measurements showed consistent superconductivity and charge density wave behavior irrespective of Sn-intercalation amount. Our results indicate that routine approaches to characterization of intercalated transition metal dichalcogenides may be inadequate for capturing the diversity of this family of materials, highlighting the need for high-resolution structural characterization when examining the properties of van der Waals-layered compounds.

cond-mat.mtrl-sci↗

arXiv2025

Quantum melting of generalized electron crystal in twisted bilayer MoSe2

Electrons can form an ordered solid crystal phase ascribed to the interplay between Coulomb repulsion and kinetic energy. Tuning these energy scales can drive a phase transition from electron solid to liquid, i.e. melting of Wigner crystal. Generalized Wigner crystals (GWCs) pinned to moire superlattices have been reported by optical and scanning-probe-based methods. Using transport measurements to investigate GWCs is vital to a complete characterization, however, still poses a significant challenge due to difficulties in making reliable electrical contacts. Here, we report the electrical transport detection of GWCs at fractional fillings nu = 2/5, 1/2, 3/5, 2/3, 8/9, 10/9, and 4/3 in twisted bilayer MoSe2. We further observe that these GWCs undergo continuous quantum melting transitions to liquid phases by tuning doping density, magnetic and displacement fields, manifested by quantum critical scaling behaviors. Our findings establish twisted bilayer MoSe2 as a novel system to study strongly correlated states of matter and their quantum phase transitions.

cond-mat.str-el↗

arXiv2024

Two-Fold Anisotropic Superconductivity in Bilayer T$_d$-MoTe$_2$

Noncentrosymmetric 2D superconductors with large spin-orbit coupling offer an opportunity to explore superconducting behaviors far beyond the Pauli limit. One such superconductor, few-layer T$_d$-MoTe$_2$, has large upper critical fields that can exceed the Pauli limit by up to 600%. However, the mechanisms governing this enhancement are still under debate, with theory pointing towards either spin-orbit parity coupling or tilted Ising spin-orbit coupling. Moreover, ferroelectricity concomitant with superconductivity has been recently observed in the bilayer, where strong changes to superconductivity can be observed throughout the ferroelectric transition pathway. Here, we report the superconducting behavior of bilayer T$_d$-MoTe$ _2$ under an in-plane magnetic field, while systematically varying magnetic field angle and out-of-plane electric field strength. We find that superconductivity in bilayer MoTe$_2$ exhibits a two-fold symmetry with an upper critical field maxima occurring along the b-axis and minima along the a-axis. The two-fold rotational symmetry remains robust throughout the entire superconducting region and ferroelectric hysteresis loop. Our experimental observations of the spin-orbit coupling strength (up to 16.4 meV) agree with the spin texture and spin splitting from first-principles calculations, indicating that tilted Ising spin-orbit coupling is the dominant underlying mechanism.

cond-mat.supr-con↗

arXiv2024

Gate-Tunable Multi-Band van der Waals Photodetector and Polarization Sensor

A single photodetector with tunable detection wavelengths and polarization sensitivity can potentially be harnessed for diverse optical applications ranging from imaging and sensing to telecommunications. Such a device will require the combination of multiple material systems with different structures, bandgaps, and photoelectrical responses, which is extremely difficult to engineer using traditional epitaxial films. Here, we develop a multi-functional and high-performance photosensor using all van der Waals materials. The device features a gate-tunable spectral response that is switchable between near-infrared/visible and short-/mid-wave infrared, as well as broadband operation, at room temperature. The linear polarization sensitivity in the telecommunications O-band can also be directly modulated between horizontal, vertical, and nonpolarizing modes. These effects originate from the balance of photocurrent generation in two of the active layers that can be manipulated by an electric field. The photodetector features high detectivity (>109 cmHz1/2W-1) together with fast operation speed (~ 1 MHz) and can be further exploited for dual visible and infrared imaging.

physics.optics↗

arXiv2024

Stoner instabilities and Ising excitonic states in twisted transition metal dichalcogenides

Moiré transition metal dichalcogenide (TMD) systems provide a tunable platform for studying electron-correlation driven quantum phases. Such phases have so far been found at rational fillings of the moiré superlattice, and it is believed that lattice commensurability plays a key role in their stability. In this work, we show via magnetotransport measurements on twisted WSe2 that new correlated electronic phases can exist away from commensurability. The first phase is an antiferromagnetic metal that is driven by proximity to the van Hove singularity. The second is a re-entrant magnetic field-driven insulator. This insulator is formed from a small and equal density of electrons and holes with opposite spin projections - an Ising excitonic insulator.

cond-mat.str-el↗

arXiv2023

Transport Study of Charge Carrier Scattering in Monolayer WSe$_2$

Employing flux-grown single crystal WSe$_2$, we report charge carrier scattering behaviors measured in $h$-BN encapsulated monolayer field effect transistors. We perform quantum transport measurements across various hole densities and temperatures and observe a non-monotonic change of transport mobility $μ$ as a function of hole density in the degenerately doped sample. This unusual behavior can be explained by energy dependent scattering amplitude of strong defects calculated using the T-matrix approximation. Utilizing long mean-free path ($>$500 nm), we demonstrate the high quality of our electronic devices by showing quantized conductance steps from an electrostatically-defined quantum point contact. Our results show the potential for creating ultra-high quality quantum optoelectronic devices based on atomically thin semiconductors.

cond-mat.mes-hall↗

arXiv2023

Programmable Nanowrinkle-Induced Room-Temperature Exciton Localization in Monolayer WSe2

Localized states in two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been the subject of intense study, driven by potential applications in quantum information science. Despite the rapidly growing knowledge surrounding these emitters, their microscopic nature is still not fully understood, limiting their production and application. Motivated by this challenge, and by recent theoretical and experimental evidence showing that nanowrinkles generate localized room-temperature emitters, we demonstrate a method to intentionally induce wrinkles with collections of stressors, showing that long-range wrinkle direction and position are controllable with patterned array design. Nano-photoluminescence (nano-PL) imaging combined with detailed strain modeling based on measured wrinkle topography establishes a correlation between wrinkle properties, particularly shear strain, and localized exciton emission. Beyond the array-induced super-wrinkles, nano-PL spatial maps further reveal that the strain environment around individual stressors is heterogeneous due to the presence of fine wrinkles that are less deterministic. Detailed nanoscale hyperspectral images uncover a wide range of low-energy emission peaks originating from these fine wrinkles, and show that the states can be tightly confined to regions < 10 nm, even in ambient conditions. These results establish a promising potential route towards realizing room temperature quantum emission in 2D TMDC systems.

cond-mat.mes-hall↗

arXiv2023

Coupled Ferroelectricity and Superconductivity in Bilayer $T_d$-MoTe$_2$

Achieving electrostatic control of quantum phases is at the frontier of condensed matter research. Recent investigations have revealed superconductivity tunable by electrostatic doping in twisted graphene heterostructures and in two-dimensional (2D) semimetals such as WTe$_2$. Some of these systems have a polar crystal structure that gives rise to ferroelectricity, in which the interlayer polarization exhibits bistability driven by external electric fields. Here we show that bilayer $T_d$-MoTe$_2$ simultaneously exhibits ferroelectric switching and superconductivity. Remarkably, a field-driven, first-order superconductor-to-normal transition is observed at its ferroelectric transition. Bilayer $T_d$-MoTe$_2$ also has a maximum in its superconducting transition temperature ($T_\textrm{c}$) as a function of carrier density and temperature, allowing independent control of the superconducting state as a function of both doping and polarization. We find that the maximum $T_\textrm{c}$ is concomitant with compensated electron and hole carrier densities and vanishes when one of the Fermi pockets disappears with doping. We argue that this unusual polarization-sensitive 2D superconductor is driven by an interband pairing interaction associated with nearly nested electron and hole Fermi pockets.

cond-mat.supr-con↗

arXiv2023

Two-step flux synthesis of ultrapure transition metal dichalcogenides

Here, we describe synthesis of TMD crystals using a two-step flux growth method that eliminates a major potential source of contamination. Detailed characterization of TMDs grown by this two-step method reveals charged and isovalent defects with densities an order of magnitude lower than in TMDs grown by a single-step flux technique. Initial temperature-dependent electrical transport measurements of monolayer WSe2 yield room-temperature hole mobility above 840 cm2/Vs and low-temperature disorder-limited mobility above 44,000 cm2/Vs. Electrical transport measurements of graphene-WSe2 heterostructures fabricated from the two-step flux grown WSe2 also show superior performance: higher graphene mobility, lower charged impurity density, and well-resolved integer quantum Hall states.

cond-mat.mtrl-sci↗

arXiv2022

Dissipation-enabled hydrodynamic conductivity in a tunable bandgap semiconductor

Electronic transport in the regime where carrier-carrier collisions are the dominant scattering mechanism has taken on new relevance with the advent of ultraclean two-dimensional materials. Here we present a combined theoretical and experimental study of ambipolar hydrodynamic transport in bilayer graphene demonstrating that the conductivity is given by the sum of two Drude-like terms that describe relative motion between electrons and holes, and the collective motion of the electron-hole plasma. As predicted, the measured conductivity of gapless, charge-neutral bilayer graphene is sample- and temperature-independent over a wide range. Away from neutrality, the electron-hole conductivity collapses to a single curve, and a set of just four fitting parameters provides quantitative agreement between theory and experiment at all densities, temperatures, and gaps measured. This work validates recent theories for dissipation-enabled hydrodynamic conductivity and creates a link between semiconductor physics and the emerging field of viscous electronics.

cond-mat.mes-hall↗

arXiv2022

High-Performance Mid-IR to Deep-UV van der Waals Photodetectors Capable of Local Spectroscopy at Room Temperature

The ability to perform broadband optical spectroscopy with sub-diffraction-limit resolution is highly sought-after for a wide range of critical applications. However, sophisticated tip-enhanced techniques are currently required to achieve this goal. We bypass this challenge by demonstrating an extremely broadband photodetector based on a two-dimensional (2D) van der Waals heterostructure that is sensitive to light across over a decade in energy from the mid-infrared (MIR) to deep-ultraviolet (DUV) at room temperature. The devices feature high detectivity (> 10^9 cm Hz^1/2 W^-1) together with high bandwidth (2.1 MHz). The active area can be further miniaturized to submicron dimensions, far below the diffraction limit for the longest detectable wavelength of 4.1 um, enabling such devices for facile measurements of local optical properties on atomic-layer-thickness samples placed in close proximity. This work can lead to the development of low-cost and high-throughput photosensors for hyperspectral imaging at the nanoscale.

physics.optics↗

arXiv2021

Tunable exciton-optomechanical coupling in suspended monolayer MoSe2

The strong excitonic effect in monolayer transition metal dichalcogenide (TMD) semiconductors has enabled many fascinating light-matter interaction phenomena. Examples include strongly coupled exciton-polaritons and nearly perfect atomic monolayer mirrors. The strong light-matter interaction also opens the door for dynamical control of mechanical motion through the exciton resonance of monolayer TMDs. Here we report the observation of exciton-optomechanical coupling in a suspended monolayer MoSe2 mechanical resonator. By moderate optical pumping near the MoSe2 exciton resonance, we have observed optical damping and anti-damping of mechanical vibrations as well as the optical spring effect. The exciton-optomechanical coupling strength is also gate-tunable. Our observations can be understood in a model based on photothermal backaction and gate-induced mirror symmetry breaking in the device structure. The observation of gate-tunable exciton-optomechanical coupling in a monolayer semiconductor may find applications in nanoelectromechanical systems (NEMS) and in exciton-optomechanics.

cond-mat.mes-hall↗

arXiv2021

Evidence of high-temperature exciton condensation in 2D atomic double layers

A Bose-Einstein condensate is the ground state of a dilute gas of bosons, such as atoms cooled to temperatures close to absolute zero. With much smaller mass, excitons (bound electron-hole pairs) are expected to condense at significantly higher temperatures. Here we study electrically generated interlayer excitons in MoSe2/WSe2 atomic double layers with density up to 10^12 cm-2. The interlayer tunneling current depends only on exciton density, indicative of correlated electron-hole pair tunneling. Strong electroluminescence (EL) arises when a hole tunnels from WSe2 to recombine with electron in MoSe2. We observe a critical threshold dependence of the EL intensity on exciton density, accompanied by a super-Poissonian photon statistics near threshold, and a large EL enhancement peaked narrowly at equal electron-hole densities. The phenomenon persists above 100 K, which is consistent with the predicted critical condensation temperature. Our study provides compelling evidence for interlayer exciton condensation in two-dimensional atomic double layers and opens up exciting opportunities for exploring condensate-based optoelectronics and exciton-mediated high-temperature superconductivity.

cond-mat.mes-hall↗

arXiv2021

Quantum Criticality in Twisted Transition Metal Dichalcogenides

In moiré heterostructures, gate-tunable insulating phases driven by electronic correlations have been recently discovered. Here, we use transport measurements to characterize the gate-driven metal-insulator transitions and the metallic phase in twisted WSe$_2$ near half filling of the first moiré subband. We find that the metal-insulator transition as a function of both density and displacement field is continuous. At the metal-insulator boundary, the resistivity displays strange metal behaviour at low temperature with dissipation comparable to the Planckian limit. Further into the metallic phase, Fermi-liquid behaviour is recovered at low temperature which evolves into a quantum critical fan at intermediate temperatures before eventually reaching an anomalous saturated regime near room temperature. An analysis of the residual resistivity indicates the presence of strong quantum fluctuations in the insulating phase. These results establish twisted WSe$_2$ as a new platform to study doping and bandwidth controlled metal-insulator quantum phase transitions on the triangular lattice.

cond-mat.mes-hall↗

arXiv2021

Intrinsic Donor-Bound Excitons in Ultraclean Monolayer Semiconductors

The monolayer transition metal dichalcogenides are an emergent semiconductor platform exhibiting rich excitonic physics with coupled spin-valley degree of freedom and optical addressability. Here, we report a new series of low energy excitonic emission lines in the photoluminescence spectrum of ultraclean monolayer WSe2. These excitonic satellites are composed of three major peaks with energy separations matching known phonons, and appear only with electron doping. They possess homogenous spatial and spectral distribution, strong power saturation, and anomalously long population (> 6 $μ$s) and polarization lifetimes (> 100 ns). Resonant excitation of the free inter- and intra-valley bright trions leads to opposite optical orientation of the satellites, while excitation of the free dark trion resonance suppresses the satellites photoluminescence. Defect-controlled crystal synthesis and scanning tunneling microscopy measurements provide corroboration that these features are dark excitons bound to dilute donors, along with associated phonon replicas. Our work opens opportunities to engineer homogenous single emitters and explore collective quantum optical phenomena using intrinsic donor-bound excitons in ultraclean 2D semiconductors.

cond-mat.mes-hall↗