arXiv subjects

Daniel Rhodes

Publications and source records attributed to Daniel Rhodes.

At least 19 recordsLinked to original sources

arXiv2026

Contrasting $\Gamma$- and K-Valley Moir\'e Physics in Twisted Monolayer/Bilayer WSe$_2$

Electronic orbital character plays a central role in determining electronic correlations, spin-orbit coupling, dimensionality, and ultimately the quantum phases of condensed-matter systems. Two-dimensional moir\'e materials have emerged as highly tunable platforms for exploring correlated phenomena, but the role of orbital degrees of freedom remains largely unexplored. Here, we identify twisted monolayer/bilayer WSe$_2$ as a platform in which displacement-field tuning enables moir\'e physics to be realized in both the $K$ and $\Gamma$ valleys. The distinct orbital characters of these valleys give rise to contrasting correlated phases at moir\'e filling factors $\nu=1$ and $\nu=1/3$. At $\nu=1$, the $K$-valley state is a weak insulator, consistent with an antiferromagnetic state near a van Hove singularity in the intermediate-coupling regime, similar to that observed in twisted bilayer WSe$_2$. In contrast, the $\Gamma$-valley state exhibits a pronounced Pomeranchuk effect, consistent with proximity to a Mott transition. At $\nu=1/3$, the $K$ valley hosts a robust generalized Wigner crystal, whereas the $\Gamma$-valley state lies near the crystallization boundary and again exhibits a Pomeranchuk effect, with localization enhanced by increasing temperature or magnetic field. Our work highlights the importance of orbital character in defining quantum phases in moir\'e systems, and identify the $\Gamma$ valley as a promising platform for exploring correlated phenomena near quantum phase transitions, where competing phases and enhanced fluctuations may give rise to unconventional phases.

cond-mat.mes-hall↗

arXiv2025

Sliding multiferroicity in hexagonal stacked CrI3

Developing new multiferroics at the two-dimensional (2D) limit with energy-efficient magnetoelectric coupling can inform the interplay physics of novel orders and advance on-chip high-performance computing applications. Here we apply stacking order engineering to create a new type of 2D multiferroics, namely sliding multiferroics, based on polar hexagonal stacked (H-stacked) CrI3. This new stacking order removes structural inversion symmetry and gives rise to room temperature sliding ferroelectricity, as confirmed by Raman spectroscopy, second harmonic generation spectroscopy and electrical transport measurements. Building upon the gate-dependent reflective magnetic circular dichroism, first-principles calculations, and modeling, sliding ferroelectricity is shown to interplay with an emergent interfacial ferromagnetism via interlayer spin-polarized charge transfer. This coupling mechanism results in non-volatile magnetic switching by as low as 0.4V across the H-stacked CrI3. Our demonstration introduces polar stacking order engineering of 2D magnets as a general approach to create non-volatile 2D multiferroics with efficient magnetoelectric coupling, paving the way for low-power electronics and spintronics at the atomically thin limit.

cond-mat.mtrl-sci↗

arXiv2025

Crystalline superconductor-semiconductor Josephson junctions for compact superconducting qubits

The narrow bandgap of semiconductors allows for thick, uniform Josephson junction barriers, potentially enabling reproducible, stable, and compact superconducting qubits. We study vertically stacked van der Waals Josephson junctions with semiconducting weak links, whose crystalline structures and clean interfaces offer a promising platform for quantum devices. We observe robust Josephson coupling across 2--12 nm (3--18 atomic layers) of semiconducting WSe$_2$ and, notably, a crossover from proximity- to tunneling-type behavior with increasing weak link thickness. Building on these results, we fabricate a prototype all-crystalline merged-element transmon qubit with transmon frequency and anharmonicity closely matching design parameters. We demonstrate dispersive coupling between this transmon and a microwave resonator, highlighting the potential of crystalline superconductor-semiconductor structures for compact, tailored superconducting quantum devices.

cond-mat.mes-hall↗

arXiv2024

Real-Space Imaging of the Band Topology of Transition Metal Dichalcogenides

The topological properties of Bloch bands are intimately tied to the structure of their electronic wavefunctions within the unit cell of a crystal. Here, we show that scanning tunneling microscopy (STM) measurements on the prototypical transition metal dichalcogenide (TMD) semiconductor WSe$_2$ can be used to unambiguously fix the location of the Wannier center of the valence band. Using site-specific substitutional doping, we first determine the position of the atomic sites within STM images, establishing that the maximum electronic density of states at the $K$-point lies between the atoms. In contrast, the maximum density of states at the $\Gamma$ point is at the atomic sites. This signifies that WSe$_2$ is a topologically obstructed atomic insulator, which cannot be adiabatically transformed to the trivial atomic insulator limit.

cond-mat.mtrl-sci↗

arXiv2023

Interplay of valley polarized dark trion and dark exciton-polaron in monolayer WSe2

The interactions between charges and excitons involve complex many-body interactions at high densities. The exciton-polaron model has been adopted to understand the Fermi sea screening of charged excitons in monolayer transition metal dichalcogenides. The results provide good agreement with absorption measurements, which are dominated by dilute bright exciton responses. Here we investigate the Fermi sea dressing of spin-forbidden dark excitons in monolayer WSe2. With a Zeeman field, the valley-polarized dark excitons show distinct p-doping dependence in photoluminescence when the carriers reach a critical density. This density can be interpreted as the onset of strongly modified Fermi sea interactions and shifts with increasing exciton density. Through valley-selective excitation and dynamics measurements, we also infer an intervalley coupling between the dark trions and exciton-polarons mediated by the many-body interactions. Our results reveal the evolution of Fermi sea screening with increasing exciton density and the impacts of polaron-polaron interactions, which lay the foundation for understanding electronic correlations and many-body interactions in 2D systems.

cond-mat.mes-hall↗

arXiv2023

Spin-selective magneto-conductivity in WSe$_2$

Material systems that exhibit tunable spin-selective conductivity are key components of spintronic technologies. Here we demonstrate a novel type of spin-selective transport, based on the unusual Landau level (LL) sequence observed in bilayer WSe$_2$ under large applied magnetic fields. We find that the conductivity depends strongly on the relative iso-spin ordering between conducting electrons in a partially filled LL and the localized electrons of lower energy filled LLs, with conductivity observed to be almost completely suppressed when the spin-ratio and field-tuned Coulomb energy exceed a critical threshold. Switching between "on/off" states is achievable through either modulation of the external magnetic or electric fields, with many-body interaction driving a collective switching mechanism. In contrast to magnetoresistive heterostructures, this system achieves electrically tunable spin filtering within a single material, driven by interaction between free and localized spins residing in energy-separated spin/valley polarized bands. Similar spin-selective conductivity may be realizable in multi-flat band systems at zero magnetic field.

cond-mat.mes-hall↗

arXiv2022

Electron spin resonance and collective excitations in magic-angle twisted bilayer graphene

In a strongly correlated system, collective excitations contain key information regarding the electronic order of the underlying ground state. An abundance of collective modes in the spin and valley isospin channels of magic-angle graphene moir\'e bands has been alluded to by a series of recent experiments. However, direct observation of collective excitations has remained elusive due to the lack of a spin probe. In this work, we use a resistively-detected electron spin resonance technique to look for low-energy collective excitations in magic-angle twisted bilayer graphene. We report direct observation of collective modes in the form of microwave-induced resonance near half filling of the moir\'e flatbands. The frequency-magnetic field dependence of these resonance modes sheds light onto the nature of intervalley spin coupling, allowing us to extract parameters such as intervalley exchange interaction and spin stiffness. Two independent observations testify that the generation and detection of the microwave resonance relies on the strong correlation within the flat moir\'e energy band. First, the onset of robust resonance response coincides with the spontaneous flavor polarization at half moir\'e filling, and remains absent in the density range where the underlying Fermi surface is isospin unpolarized. Second, we performed the same resonance measurement on graphene monolayer and bilayer samples, including twisted bilayer with a large twist angle, where flatband physics is absent. We observe no indication of resonance response in these samples across a large range of carrier density, microwave frequency and power. A natural explanation is that the resonance response near the magic angle originates from "Dirac revivals" and the resulting isospin order.

cond-mat.mes-hall↗

arXiv2022

A new flavor of correlation and superconductivity in small twist-angle trilayer graphene

When layers of graphene are rotationally misaligned by the magic angle, the moiré superlattice features extremely flat bands. Due to the enhanced density of states, the Coulomb interaction induces a variety of instabilities. The most prominent occur at integer filling and are therefore commonly attributed to spontaneous polarization of the moiré unit cell's `flavor' degrees of freedom -- spin, valley, and the flat-band degeneracy. As the dominant member of the hierarchy, these correlated states are thought to crucially determine further instabilities at lower energy scales, such as superconductivity and weaker incompressible states at fractional filling. In this work, we examine the behavior of twisted trilayer graphene in a window of twist angle around $1.3^{\circ}$, well below the expected magic angle of $1.55^{\circ}$. In this small twist angle regime, we find surprisingly narrow bands, which are populated with both an abundance of correlation-driven states at fractional filling as well as robust superconductivity. The absence of linear-in-$T$ resistivity without significant reduction of the superconducting transition temperature, provides insights into the origin of both phenomena. Most remarkably, the hierarchy between integer and fractional filling is absent, indicating that flavor polarization does not play a governing role. The prominence of fractional filling in the small twist angle regime also points towards a longer-range effective Coulomb interaction. Combined, our results shed new light on outstanding questions in the field, while establishing the small twist angle regime as a new paradigm for exploring novel flavors of moiré physics.

cond-mat.mes-hall↗

arXiv2021

Zero-field superconducting diode effect in small-twist-angle trilayer graphene

The critical current of a superconductor can be different for opposite directions of current flow when both time-reversal and inversion symmetry are broken. %When time-reversal and inversion symmetry are simultaneously broken, the critical current of a 2D superconductor is expected to depend on the directions of current flow. Such nonreciprocal behavior in superconducting transport, which creates a superconducting diode, has recently been demonstrated experimentally by breaking these symmetries with an applied magnetic field \cite{Ando2020diodes} or by construction of a magnetic tunnel junction \cite{Diez2021magnetic}. Here we report an intrinsic superconducting diode effect which is present at zero external magnetic field in mirror symmetric twisted trilayer graphene (tTLG). Such nonreciprocal behavior, with sign that can be reversed through training with an out-of-plane magnetic field, provides direct evidence of the microscopic coexistence between superconductivity and time-reversal symmetry breaking. In addition to the magnetic-field trainability, we show that the zero-field diode effect can be controlled by varying carrier density or twist angle. In accordance with these experimental controls, a natural interpretation for the origin of the intrinsic diode effect is an imbalance in valley occupation of the underlying Fermi surface, which likely leads to finite-momentum Cooper pairing and nematicity in the superconducting phase.

cond-mat.mes-hall↗

arXiv2021

Manipulation of Exciton Dynamics in Single-Layer WSe2 Using a Toroidal Dielectric Metasurface

Recent advances in emerging atomically thin transition metal dichalcogenide semiconductors with strong light-matter interactions and tunable optical properties provide novel approaches for realizing new material functionalities. Coupling two-dimensional semiconductors with all-dielectric resonant nanostructures represents an especially attractive opportunity for manipulating optical properties in both the near-field and far-field regimes. Here, by integrating single-layer WSe2 and titanium oxide (TiO2) dielectric metasurfaces with toroidal resonances, we realized robust exciton emission enhancement over one order of magnitude at both room and low temperatures. Furthermore, we could control exciton dynamics and annihilation by using temperature to tailor the spectral overlap of excitonic and toroidal resonances, allowing us to selectively enhance the Purcell effect. Our results provide rich physical insight into the strong light-matter interactions in single-layer TMDs coupled with toroidal dielectric metasurfaces, with important implications for optoelectronics and photonics applications.

cond-mat.mes-hall↗

arXiv2021

Bilayer WSe$_2$ as a natural platform for interlayer exciton condensates in the strong coupling limit

Exciton condensates (EC) are macroscopic coherent states arising from condensation of electron-hole pairs. Bilayer heterostructures, consisting of two-dimensional electron and hole layers separated by a tunnel barrier, provide a versatile platform to realize and study EC. The tunnel barrier suppresses recombination yielding long-lived excitons. However, this separation also reduces interlayer Coulomb interactions, limiting the exciton binding strength. Here, we report the observation of EC in naturally occurring 2H-stacked bilayer WSe$_2$. In this system, the intrinsic spin-valley structure suppresses interlayer tunneling even when the separation is reduced to the atomic limit, providing access to a previously unattainable regime of strong interlayer coupling. Using capacitance spectroscopy, we investigate magneto-EC, formed when partially filled Landau levels (LL) couple between the layers. We find that the strong-coupling EC show dramatically different behaviour compared with previous reports, including an unanticipated variation of the EC robustness with the orbital number, and find evidence for a transition between two types of low-energy charged excitations. Our results provide a demonstration of tuning EC properties by varying the constituent single-particle wavefunctions.

cond-mat.mes-hall↗

arXiv2021

Spin-orbit driven ferromagnetism at half moir\'e filling in magic-angle twisted bilayer graphene

Strong electron correlation and spin-orbit coupling (SOC) provide two non-trivial threads to condensed matter physics. When these two strands of physics come together, a plethora of quantum phenomena with novel topological order have been predicted to emerge in the correlated SOC regime. In this work, we examine the combined influence of electron correlation and SOC on a 2-dimensional (2D) electronic system at the atomic interface between magic-angle twisted bilayer graphene (tBLG) and a tungsten diselenide (\WSe) crystal. In such a structure, strong electron correlation within the moir\'e flatband stabilizes correlated insulating states at both quarter and half-filling, whereas SOC transforms these Mott-like insulators into ferromagnets, evidenced by robust anomalous Hall effect with hysteretic switching behavior. The coupling between spin and valley degrees of freedom is unambiguously demonstrated as the magnetic order is shown to be tunable with an in-plane magnetic field, or a perpendicular electric field. In addition, we examine the influence of SOC on the isospin order and stability of superconductivity. Our findings establish an efficient experimental knob to engineer topological properties of moir\'e bands in twisted bilayer graphene and related systems.

cond-mat.mes-hall↗

arXiv2020

Moiré metrology of energy landscapes in van der Waals heterostructures

The emerging field of twistronics, which harnesses the twist angle between two-dimensional materials, represents a promising route for the design of quantum materials, as the twist-angle-induced superlattices offer means to control topology and strong correlations. At the small twist limit, and particularly under strain, as atomic relaxation prevails, the emergent moiré superlattice encodes elusive insights into the local interlayer interaction. Here we introduce moiré metrology as a combined experiment-theory framework to probe the stacking energy landscape of bilayer structures at the 0.1 meV/atom scale, outperforming the gold-standard of quantum chemistry. Through studying the shapes of moiré domains with numerous nano-imaging techniques, and correlating with multi-scale modelling, we assess and refine first-principle models for the interlayer interaction. We document the prowess of moiré metrology for three representative twisted systems: bilayer graphene, double bilayer graphene and H-stacked $MoSe_2/WSe_2$. Moiré metrology establishes sought after experimental benchmarks for interlayer interaction, thus enabling accurate modelling of twisted multilayers.

cond-mat.mes-hall↗

arXiv2020

Enhanced Superconductivity in Monolayer $T_d$-MoTe$_2$ with Tilted Ising Spin Texture

Crystalline two-dimensional (2D) superconductors with low carrier density are an exciting new class of materials in which superconductivity coexists with strong interactions, the effects of complex topology are not obscured by disorder, and electronic properties can be strongly tuned by electrostatic gating. Very recently, two such materials, 'magic-angle' twisted bilayer graphene and monolayer $T_d$-WTe$_2$, have been reported to show superconductivity at temperatures near 1 K. Here we report superconductivity in semimetallic monolayer $T_d$-MoTe$_2$. The critical temperature $T_\textrm{c}$ reaches 8 K, a sixty-fold enhancement as compared to the bulk. This anomalous increase in $T_\textrm{c}$ is only observed in monolayers, and may be indicative of electronically mediated pairing. Reflecting the low carrier density, the critical temperature, magnetic field, and current density are all tunable by an applied gate voltage, revealing a superconducting dome that extends across both hole and electron pockets. The temperature dependence of the in-plane upper critical field is distinct from that of $2H$ transition metal dichalcogenides (TMDs), consistent with a tilted spin texture as predicted by \textit{ab initio} theory.

cond-mat.supr-con↗

arXiv2020

Optical Measurement of Pseudo-Spin Texture of the Exciton Fine-Structure in Monolayer WSe2 within the Light Cone

Several theoretical predictions have claimed that the neutral exciton of TMDCs splits into a transversal and longitudinal exciton branch, with the longitudinal one, which is the upper branch, exhibiting an extraordinary strong dispersion in the meV range within the light cone. Historically, this was linked for semiconductor quantum wells to strong far-field optical dipole coupling, or strong electronic long-range exchange interactions, describing two sides of the same coin. Recently, experiments utilizing Fourier-space spectroscopy have shown that the exciton (exciton-polariton) dispersion can indeed be measured for high-quality hexagonal-BN-encapsulated WSe2 monolayer samples and can confirm the energy scale. Here, the exciton fine-structure's pseudo-spin and the valley polarization are investigated as a function of the centre-of-mass-momentum and excitation-laser detuning. For quasi-resonant excitation, a strong dispersion featuring a pronounced momentum-dependent helicity is observed. By increasing the excitation energy step-wise towards and then above the electronic band gap, the dispersion and the helicity systematically decrease due to contributions of incoherent excitons and emission from plasma. The decline of the helicity with centre-of-mass momentum can be phenomenologically modelled by the Maialle-Silva-Sham mechanism using the exciton splitting as the source of an effective magnetic field.

cond-mat.mes-hall↗

arXiv2019

Enhanced nonlinear interaction of polaritons via excitonic Rydberg states in monolayer WSe2

Strong optical nonlinearities play a central role in realizing quantum photonic technologies. In solid state systems, exciton-polaritons, which result from the hybridization of material excitations and cavity photons, are an attractive candidate to realize such nonlinearities. Here, the interaction between excitons forms the basis of the polaritonic nonlinearity. While the interaction between ground state excitons generates a notable optical nonlinearity, the strength of such ground state interactions is generally not sufficient to reach the regime of quantum nonlinear optics and strong single-polariton interactions. Excited states, however, feature enhanced interactions and therefore hold promise for accessing the quantum domain of single-photon nonlinearities, as demonstrated with high-lying Rydberg states of cold atomic systems. Excitons in excited states have recently been observed in monolayer transition metal dichalcogenides. Here we demonstrate the formation of exciton-polaritons using the first excited excitonic state in monolayer tungsten diselenide (WSe2) embedded in a microcavity. Owing to the larger exciton size compared to their ground state counterpart, the realized polaritons exhibit an enhanced nonlinear response by more than an order of magnitude, as evidenced through a modification of the cavity Rabi splitting. The demonstration of excited exciton-polaritons in two-dimensional semiconductors and their enhanced nonlinear response presents the first step towards the generation of strong photon interactions in solid state systems, a necessary building block for quantum photonic technologies.

cond-mat.mtrl-sci↗

arXiv2019

Direct Measurement of the Radiative Pattern of Bright and Dark Excitons and Exciton Complexes in Encapsulated Tungsten Diselenide

The optical properties of particularly the tungsten-based transition-metal dichalcogenides are strongly influenced by the presence of dark excitons. Recently, theoretical predictions as well as indirect experimental insights have shown that two different dark excitons exist within the light cone. While one is completely dark, the other one is only dipole forbidden out-of-plane, hence referred to as grey exciton. Here, we present angle-resolved spectroscopic data of a high-quality hexagonal-BN-encapsulated WSe2 monolayer with which we directly obtain the radiation pattern of this grey exciton that deviates from that of the bright exciton and other exciton complexes obtained at cryogenic temperatures.

cond-mat.mes-hall↗

arXiv2019

Magnetic field mixing and splitting of bright and dark excitons in monolayer MoSe2

Monolayers of semiconducting transition metal dichalcogenides (TMDCs) with unique spin-valley contrasting properties and remarkably strong excitonic effects continue to be a subject of intense research interests. These model 2D semiconductors feature two fundamental intravalley excitons species - optically accessible ' bright' excitons with anti-parallel spins and optically inactive 'dark' excitons with parallel spins. For applications exploiting radiative recombination of bright excitons or long lifetime dark excitons, it is essential to understand the radiative character of the exciton ground state and establish the energy separation between the lowest energy bright and dark excitons. Here, we report a direct spectroscopic measure of dark excitons in monolayer MoSe$_2$ encapsulated in hexagonal boron nitride. By applying strong in-plane magnetic field, we induce mixing and splitting of bright and dark exciton branches, which enables an accurate spectroscopic determination of their energies. We confirm the bright character of the exciton ground state separated by a 1.5~meV gap from the higher energy dark exciton state, much smaller compared to the previous theoretical expectations. These findings provide critical information for further improvement of the accurate theoretical description of TMDCs electronic structure.

cond-mat.mes-hall↗