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Seth Ariel Tongay

Publications and source records attributed to Seth Ariel Tongay.

At least 19 recordsLinked to original sources

Universal computational super-resolution framework for imaging of quantum dots

We present a universal deep-learning method that reconstructs super-resolved images of quantum emitters from a single camera frame measurement. Trained on physics-based synthetic data spanning diverse point-spread functions, aberrations, and noise, the network generalizes across experimental conditions without system-specific retraining. We validate the approach on low- and high-density In(Ga)As quantum dots and strain-induced dots in 2D monolayer WSe$_2$, resolving overlapping emitters even under low signal-to-noise and inhomogeneous backgrounds. By eliminating calibration and iterative acquisitions, this single-shot strategy enables rapid, robust computational super-resolution for nanoscale characterization and quantum photonic device fabrication.

quant-ph

Layer-Hybridized Wigner Crystals in MoSe2/WS2 Moiré Superlattice

Transition metal dichalcogenide moiré heterobilayers with type-II band alignment provide a versatile platform for layer-polarized generalized Wigner crystals, in which strong Coulomb interactions drive charge ordering at fractional lattice fillings. With a finite interlayer band offset, an out-of-plane electric field can tune layer-resolved moiré bands through resonance and enable controllable interlayer hybridization. Although hybridized Mott insulators have been previously demonstrated, whether fractional charge-ordered states can survive such hybridization remains elusive. Here we drive an H-stacked MoSe2/WS2 moiré heterobilayer through a type-I-to-type-II band-alignment transition and realize layer-hybridized Mott insulator and generalized Wigner crystals. For fillings below one electron per moiré cell, tunneling delocalizes electrons and modifies Wigner crystallization. However, above one electron per cell, Coulomb repulsion overcomes tunneling and favors layer-separated occupation, stabilizing stronger charge-ordered states. These results establish electrically tunable hybridized moiré heterobilayers as a powerful platform for engineering correlated charge order and exploring fractional Chern phases and emergent magnetism.

cond-mat.mes-hall

Visualizing the Impact of Quenched Disorder on 2D Electron Wigner Solids

Electron Wigner solids (WSs)1-12 provide an ideal system for understanding the competing effects of electron-electron and electron-disorder interactions, a central unsolved problem in condensed matter physics. Progress in this topic has been limited by a lack of single-defect-resolved experimental measurements as well as accurate theoretical tools to enable realistic experiment/theory comparison. Here we overcome these limitations by combining atomically-resolved scanning tunneling microscopy (STM) with neural-quantum-state quantum Monte Carlo (NQS-QMC) simulation of disordered 2D electron WSs to discover new disorder-induced physical regimes of correlated electron behavior. STM was used to image the electron density ($n_e$) dependent evolution of electron WSs in gate-tunable bilayer MoSe2 devices with varying long-range ($n_\mathrm{LR}$) and short-range ($n_\mathrm{SR}$) disorder densities. These images were compared to NQS-QMC simulations using realistic disorder maps extracted from experiment, thus allowing the roles of different disorder types to be disentangled. We identify two distinct physical regimes for disordered electron WSs that depend on $n_\mathrm{SR}$. For $n_\mathrm{SR} \lesssim n_e$ the WS behavior is dominated by long-range disorder and features extensive mixed solid-liquid phases, a new type of local re-entrant melting/crystallization, and prominent Friedel oscillations. In contrast, when $n_\mathrm{SR} \gg n_e$ these features are suppressed and a more robust amorphous WS phase emerges that persists to higher ne, highlighting the importance of short-range disorder in this regime. Our work establishes a powerful framework for studying disordered quantum solids via a combined experimental-theoretical approach.

cond-mat.str-el

Propagating Collective Spin-valley Modes in Twisted WSe2

The emergence of neutral collective modes is a hallmark of correlated quantum phases but is often challenging to probe experimentally. In two-dimensional flatband systems, charge responses have been intensively investigated yet neutral excitations remain largely unexplored. In particular, intervalley coherent state (IVC) features a neutral Goldstone mode due to spontaneously broken valley U(1) symmetry. While IVC state has been proposed as a unifying theme across graphene and semiconductor based systems, its defining feature, the neutral Goldstone mode, remains elusive in experiment. Here we investigate space and time resolved transport of neutral modes in twisted WSe2 moire superlattices through a novel ultrafast imaging technique. We uncover two new propagating collective modes with very different velocities, which emerge near the van Hove singularity (VHS) in both intermediate (3.5 to 4 degree) and large (around 5 degree) angle twisted WSe2. The fast-propagating mode has a large speed of about 3 km/s and is consistent with a Goldstone mode for an IVC state, while the slow-moving mode is likely a gapped amplitude mode. They can be understood as the spin-valley analogues of collective modes of a superfluid, whose propagation is imaged for the first time in a condensed matter system. Our study demonstrates a powerful new approach for probing charge-neutral modes in quantum materials and offers key insights into the interplay between charge and spin-valley physics in moire superlattices.

cond-mat.mes-hall

C-band 160 Gbs-1 Zero-bias Graphene Photodetectors: Breaking the Responsivity-Bandwidth Trade-off by Heterostructure Engineering

Graphene photodetectors offer ultrafast response and broadband operation, but their responsivity is typically limited by rapid hot-carrier cooling, leading to a trade-off between sensitivity and speed. Here, we demonstrate that modifying the dielectric environment provides an effective route to control hot-carrier cooling and enhance device performance. By employing a WSe2 encapsulation architecture, we suppress out-of-plane energy dissipation, leading to an increased cooling length (~2.68 um) and a reduced heat-exchange coefficient. As a result, we obtain zero-bias graphene photodetectors with responsivities up to ~0.12 A/W (potentially ~0.4 A/W) while maintaining ultrafast operation beyond the setup-limited 110 GHz bandwidth. The devices enable direct detection at data rates of 120 Gb s-1 (NRZ) and 160 Gb s-1 (PAM-4), with performance achieved using minimal digital signal processing. These results establish dielectric engineering as a key design axis for controlling hot-carrier dynamics, enabling energy-efficient, high-speed optical receivers for next-generation interconnects and AI-driven data systems.

physics.optics

Excitonic Mott transition without population inversion

Exciton dissociation via the excitonic Mott transition (EMT) governs the high-density optical response of semiconductors and sets fundamental limits for optoelectronic devices. The EMT is conventionally linked to the onset of population inversion and the emergence of optical gain. Here, we demonstrate that this paradigm can break down under ultrafast non-equilibrium excitation. Using femtosecond pump-probe optical spectroscopy, we drive a monolayer transition metal dichalcogenide into a dense photoexcited state in which the excitonic resonance is completely quenched within ~100 fs, while the optical gain is entirely absent across the explored fluence range. State-of-the-art real-time ab initio simulations reveal that the EMT is governed by an interplay of strongly nonthermal carrier populations and nonequilibrium dynamical screening of the Coulomb interaction. The quantitative agreement between theory and experiment identifies a distinct, ultrafast pathway to exciton ionization beyond quasi-equilibrium descriptions and demonstrates that population inversion is not a universal prerequisite for the EMT.

cond-mat.mes-hall

Robust valley-polarized excitonic Mott states and doublons enabled by stacking-controlled moiré geometry

Atomically-thin moiré superlattices offer an optically accessible platform for interacting bosons, where strong onsite repulsion $U_{xx}$ suppresses double occupancy and supports excitonic Mott states at unit filling. However, moiré confinement also enhances phonon- and disorder-assisted relaxation, challenging the robustness of these correlated states under dissipation. Here we show that strengthening the intersite exciton repulsion $V_{xx}$ between neighboring moiré cells offers a distinct route to stabilizing unit-filling excitonic Mott states. In H-stacked WSe2/WS2, moiré confinement endows interlayer excitons with an out-of-plane dipole and a pronounced in-plane quadrupolar charge distribution. Helicity-resolved transient photoluminescence, supported by first-principles-informed modelling, reveals that this quadrupolar geometry increases $V_{xx}$ at unit filling by at least a factor of two relative to the dipolar R-stacked excitons. Despite a slight reduction in $U_{xx}$, the enhanced $V_{xx}$ yields a long-lived, valley-polarized excitonic Mott state at unit filling that persists for ~12 ns - more than twice as long as in R-stacks - and remains robust up to ~50 K. Beyond unit filling, the same geometry supports valley-polarized doublons with fourfold longer lifetimes than in R-stacks. These results establish moiré-geometric control of intersite interactions as a route to stabilizing excitonic Mott states and doublons against dissipation in solids.

cond-mat.mes-hall

Robust Interlayer Exciton Interplay in Twisted van der Waals Heterotrilayer on a Broadband Bragg Reflector up to Room Temperature

We report robust room temperature interlayer excitons in transition metal dichalcogenide heterostructures engineered via precise stacking orientation and twist-angle control. We integrate 2H-stacked MoSe$_{2}$/$^{1}$WSe$_{2}$/$^{2}$WSe$_{2}$ heterotrilayer onto a chirped distributed Bragg reflector that acts as a backside mirror. This way, we fabricate a platform that hosts distinct heterotrilayer, heterobilayer, and homobilayer regions with enhanced excitonic features at elevated temperatures. Although the heterobilayer supports temperature-tunable singlet and triplet interlayer excitons, it exhibits low emission yield at 4 K. In comparison, the heterotrilayer shows remarkable excitonic properties, including pronounced band modulation, intervalley interlayer exciton transitions, and a tenfold photoluminescence enhancement along with a sevenfold increase in exciton decay time at cryogenic temperatures compared to the heterobilayer system. Temperature-dependent studies reveal intriguing interlayer exciton dynamics in the heterotrilayer, including the emergence of valley-polarized interlayer excitons, and the ability to maintain optical stability up to room temperature. Our results establish a clear strategy for engineering excitonic states across multilayer van der Waals heterostructures from 4 K to room temperature, providing a versatile platform for excitonic optoelectronics, quantum photonics, and tunable long-lived interlayer exciton states in scalable TMD heterostructures.

cond-mat.mes-hall

Optical properties of Fermi polarons in a GaInP/MoSe2 monolayer heterostructure

Engineering optical properties, such as luminescence purity and charge transfer, is crucial for harnessing the application potential of atomically thin transition metal dichalcogenides (TMDCs). While electrostatic gating is widely applied to gain charge control in TMDC monolayers, charge transfer can also be engineered via coupling of TMDC monolayers at semiconductor III/V, organic, or van der Waals interfaces. This confers great advantages, such as ease in implementation and compatibility in device integration. Here, we shed light on the optical properties of many-particle complexes emerging at the GaInP/MoSe2 interface as a highly relevant material combination to manipulate the optical properties of TMDCs in integrated photonic devices. Our study verifies its nature as a type II hetero-interface, which bears the feasibility to display disorder-free photoluminescence. Through optical absorption measurements, we verify that the charged complexes acquire substantial oscillator strength. Furthermore, temperature-dependent photoluminescence, supported by a microscopic theory framework, evidences the suppression of the characteristic carrier recoil effect that was previously observed in the photoluminescence of trions in TMDCs. These phenomena allow us to identify the optical signatures at the TMDC-GaInP interface as Fermi polaron quasiparticle resonances, which are of high importance in researching Bose-Fermi mixtures in condensed matter systems.

cond-mat.mtrl-sci

Observation of moiré trapped biexciton through sub-diffraction-limit probing using hetero-bilayer on nanopillar

The ability to tune the degree of interaction among particles at the nanoscale is highly intriguing. The spectroscopic signature of such interaction is often subtle and requires special probes to observe. To this end, inter-layer excitons trapped in the periodic potential wells of a moiré superlattice offer rich interaction physics, specifically due to the presence of both attractive and repulsive components in the interaction. Here we show that the Coulomb force between two inter-layer excitons switches from repulsive to attractive when the length scale reduces from inter-moiré-pocket to intra-moiré-pocket in a WS$_2$/WSe$_2$ hetero-bilayer - thanks to the complex competition between direct and exchange interaction. The finding is a departure from the usual notion of repelling inter-layer excitons due to layer polarization. This manifests as the simultaneous observation of an anomalous superlinear power-law of moiré exciton and a stabilization of moiré trapped biexciton. The experimental observation is facilitated by placing the hetero-bilayer on a polymer-nanopillar/gold-film stack which significantly reduces the inhomogeneous spectral broadening by selectively probing a smaller ensemble of moiré pockets compared with a flat sample. This creates an interesting platform to explore interaction among moiré trapped excitons and higher order quasiparticles.

cond-mat.mes-hall

Electrical Control of Excitons in Bare-MoSe2 and MoSe2/NbSe2 Heterostructure

Monolayer transition metal dichalcogenides (TMDCs) are promising materials for next-generation optoelectronic devices, owing to their strong excitonic responses and atomic thickness. Controlling their light emission electrically is a crucial step towards realizing practical nanoscale optoelectronic devices such as light-emitting diodes and optical modulators. However, photoluminescence (PL) quenching in van der Waals TMDC/metal heterostructures, caused by ultrafast interlayer charge or energy transfer, impedes such electrical modulation. Here, we investigate monolayer-MoSe2/bulk-NbSe2 heterostructures and demonstrate that a vertical electric field can effectively recover the PL intensity up to ~ 80% of bare-MoSe2. Furthermore, our analysis reveals that the room temperature PL intensity can be tuned by nearly three orders of magnitude in bare-MoSe2 and by about one order of magnitude in MoSe2/NbSe2 heterostructures. First-principles calculations incorporating spin-orbit coupling reveal that the perpendicular electric fields drive a transition from a direct to an indirect bandgap, fundamentally altering the optical response in the heterostructure. Unlike bare-MoSe2, the heterostructure exhibits a pronounced thermal dependence of the enhancement factor, implying that exciton lifetime dominates over interfacial transfer processes. Our findings demonstrate reversible, electric-field-driven PL control at a TMDC/metal interface, providing a pathway to electrically tunable light emission and improved contact engineering in two-dimensional optoelectronic devices.

physics.app-ph

Temperature-dependent Optical and Polaritonic Properties of hBN-encapsulated Monolayer TMDs

Monolayer transition metal dichalcogenides (TMDs) support robust excitons in the visible to near-infrared spectral range. Their reduced dielectric screening results in large binding energies, and combined with a direct bandgap in monolayer form, these excitons dominate the optical response of TMDs. In this work, we present a comprehensive investigation of the temperature-dependent optical and polaritonic properties of high-quality, flux-grown $\mathrm{WS_2}$, $\mathrm{MoS_2}$, $\mathrm{WSe_2}$, and $\mathrm{MoSe_2}$ monolayers, encapsulated by hBN, in the full temperature range between $5-300 \mathrm{K}$. Using reflection spectroscopy measurements, we evaluate and compare the optical and polaritonic constituents of the TMD excitons in terms of oscillator strength, linewidth and negative permittivity. We find that it is $\mathrm{MoSe_2}$ that exhibits the most pronounced optical and polaritonic response, stemming from its rapid linewidth narrowing at low temperatures, as compared to the temperature-dependent response of the other TMDs. In addition, we find that all four TMDs exhibits a temperature-dependent negative real part permittivity, thus supporting surface-exciton-polaritons. We derive their dispersion relation, confinement factors and losses, similarly revealing that $\mathrm{MoSe_2}$ exhibit enhanced polaritonic properties. These findings establish a comparative framework for understanding the optical and polaritonic properties of monolayer TMDs, with implications on their utilization in optoelectronic devices based on 2D semiconductors.

physics.optics

Strong Correlation Driven Quadrupolar to Dipolar Exciton Transitions in a Trilayer Moiré Superlattice

The additional layer degree of freedom in trilayer moiré superlattices of transition metal dichalcogenides enables the emergence of novel excitonic species, such as quadrupolar excitons, which exhibit unique excitonic interactions and hold promise for realizing intriguing excitonic phases and their quantum phase transitions. Concurrently, the presence of strong electronic correlations in moiré superlattices, as exemplified by the observations of Mott insulators and generalized Wigner crystals, offers a direct route to manipulate these new excitonic states and resulting collective excitonic phases. Here, we demonstrate that strong exciton-exciton and electron-exciton interactions, both stemming from robust electron correlations, can be harnessed to controllably drive transitions between quadrupolar and dipolar excitons. This is achieved by tuning either the exciton density or electrostatic doping in a trilayer semiconducting moiré superlattice. Our findings not only advance the fundamental understanding of quadrupolar excitons but also usher in new avenues for exploring and engineering many-body quantum phenomena through novel correlated excitons in semiconducting moiré systems.

cond-mat.mes-hall

The Transmission Line Model for 2D Materials and van der Waals Heterostructures

Van der Waals heterostructures (VdWHs) composed of 2D materials have attracted significant attention in recent years due to their intriguing optical properties, such as strong light-matter interactions and large intrinsic anisotropy. In particular, VdWHs support a variety of polaritons-hybrid quasiparticles arising from the coupling between electromagnetic waves and material excitations-enabling the confinement of electromagnetic radiation to atomic scales. The ability to predict and simulate the optical response of 2D materials heterostructures is thus of high importance, being commonly performed until now via methods such as the TMM, or Fresnel equations. While straight forward, these often yield long and complicated expressions, limiting intuitive and simple access to the underlying physical mechanisms that govern the optical response. In this work, we demonstrate the adaptation of the transmission line model for VdWHs, based on expressing its constituents by distributed electrical circuit elements described by their admittance. Since the admittance carries fundamental physical meaning of the material response to electromagnetic fields, the approach results in a system of propagating voltage and current waves, offering a compact and physically intuitive formulation that simplifies algebraic calculations, clarifies the conditions for existence of physical solutions, and provides valuable insight into the fundamental physical response. To demonstrate this, we derive the transmission line analogs of bulk to monolayer 2D materials and show it can be used to compute the reflection/transmission coefficients, polaritonic dispersion relations, and electromagnetic field distributions in a variety of VdWHs, and compare them to experimental measurements yielding very good agreement. This method provides a valuable tool for exploring and understanding the optical response of layered 2D systems.

physics.optics

SparseC-AFM: a deep learning method for fast and accurate characterization of MoS$_2$ with C-AFM

The increasing use of two-dimensional (2D) materials in nanoelectronics demands robust metrology techniques for electrical characterization, especially for large-scale production. While atomic force microscopy (AFM) techniques like conductive AFM (C-AFM) offer high accuracy, they suffer from slow data acquisition speeds due to the raster scanning process. To address this, we introduce SparseC-AFM, a deep learning model that rapidly and accurately reconstructs conductivity maps of 2D materials like MoS$_2$ from sparse C-AFM scans. Our approach is robust across various scanning modes, substrates, and experimental conditions. We report a comparison between (a) classic flow implementation, where a high pixel density C-AFM image (e.g., 15 minutes to collect) is manually parsed to extract relevant material parameters, and (b) our SparseC-AFM method, which achieves the same operation using data that requires substantially less acquisition time (e.g., under 5 minutes). SparseC-AFM enables efficient extraction of critical material parameters in MoS$_2$, including film coverage, defect density, and identification of crystalline island boundaries, edges, and cracks. We achieve over 11x reduction in acquisition time compared to manual extraction from a full-resolution C-AFM image. Moreover, we demonstrate that our model-predicted samples exhibit remarkably similar electrical properties to full-resolution data gathered using classic-flow scanning. This work represents a significant step toward translating AI-assisted 2D material characterization from laboratory research to industrial fabrication. Code and model weights are available at github.com/UNITES-Lab/sparse-cafm.

cs.CV

Tuning relaxation and nonlinear upconversion of valley-exciton-polaritons in a monolayer semiconductor

Controlling exciton relaxation and energy conversion pathways via their coupling to photonic modes is a central task in cavity-mediated quantum materials research. In this context, the light-matter hybridization in optical cavities can lead to intriguing effects, such as modified carrier transport, enhancement of optical quantum yield, and control of chemical reaction pathways. Here, we investigate the impact of the strong light-matter coupling regime on energy conversion, both in relaxation and upconversion schemes, by utilizing a strongly charged MoSe2 monolayer embedded in a spectrally tunable open-access cavity. We find that the charge carrier gas yields a significantly modified photoluminescence response of cavity exciton-polaritons, dominated by an intra-cavity like pump scheme. In addition, upconversion luminescence emerges from a population transfer from fermionic trions to bosonic exciton-polaritons. Due to the availability of multiple optical modes in the tunable open cavity, it seamlessly meets the cavity-enhanced double resonance condition required for an efficient upconversion. The latter can be actively tuned via the cavity length in-situ, displaying nonlinear scaling in intensity and fingerprints of the valley polarization. This suggests mechanisms that include both trion-trion Auger scattering and phonon absorption as its underlying microscopic origin.

cond-mat.mes-hall

The Importance of Pure Dephasing in the Optical Response of Excitons in High-quality van der Waals Heterostructures

Excitons in monolayer transition metal dichalcogenides (TMDs) dominate their optical response due to exceptionally large binding energies arising from their two-dimensional nature. Several theoretical models have been proposed to describe this excitonic behavior, however, it remains unclear which model most accurately captures the underlying physical properties of the response. In this work, we experimentally measure the optical response of high-quality monolayer TMD heterostructures and compare the results with the different theoretical models to address this uncertainty. We find that in high-quality heterostructures, quantum mechanical interactions in the form of pure dephasing plays a dominant role, which has been challenging to isolate experimentally in previous studies. Furthermore, accounting for an additional decay rate to the commonly used radiative and non-radiative rates is found to be important for the accurate description of the excitonic response. These findings establish a robust framework for understanding and predicting the optical properties of TMD-based heterostructures, crucial for both fundamental research and optoelectronic applications.

cond-mat.mes-hall

Anomalously Enhanced Diffusivity of Moiré Excitons via Manipulating the Interplay with Correlated Electrons

Semiconducting transitional metal dichalcogenides (TMDCs) moiré superlattice provides an exciting platform for manipulating excitons. The in-situ control of moiré potential confined exciton would usher in unprecedented functions of excitonic devices but remains challenging. Meanwhile, as a dipolar composite boson, interlayer exciton in the type-II aligned TMDC moiré superlattice strongly interacts with fermionic charge carriers. Here, we demonstrate active manipulation of the exciton diffusivity by tuning their interplay with correlated carriers in moiré potentials. At fractional fillings where carriers are known to form generalized Wigner crystals, we observed suppressed diffusivity of exciton. In contrast, in Fermi liquid states where carriers dynamically populate all moiré traps, the repulsive carrier-exciton interaction can effectively reduce the moiré potential confinement seen by the exciton, leading to enhanced diffusivity with the increase of the carrier density. Notably, the exciton diffusivity is enhanced by orders of magnitude near the Mott insulator state, and the enhancement is much more pronounced for the 0-degree than the 60-degree aligned WS2/WSe2 heterobilayer due to the more localized nature of interlayer excitons. Our study inspires further engineering and controlling exotic excitonic states in TMDC moiré superlattices for fascinating quantum phenomena and novel excitonic devices.

cond-mat.mes-hall