arXiv subjects

James C. Hone

Publications and source records attributed to James C. Hone.

At least 19 recordsLinked to original sources

arXiv2026

Antiferromagnetism-altered plasmon dynamics

The interaction between plasmons and magnons is a long-sought phenomenon with implications for fundamental physics and spintronics applications. In three-dimensional systems, this coupling is suppressed by the large mismatch in energy scales, but two-dimensional (2D) plasmons with gapless dispersion can overlap with magnons over a broad spectral range. Despite numerous theoretical predictions, experimental observation of magnon-plasmon interaction has remained elusive. In this work, we study a first-of-its-kind hybrid plasmon-magnon platform based on 2D materials. By deploying scattering-type scanning near-field optical microscopy (s-SNOM) with terahertz radiation, we image propagating plasmon wavepackets at a graphene/NiPS$_3$ interface and track their dynamics across the antiferromagnetic transition of NiPS$_3$. We observe a clear renormalization of the plasmon-polariton dispersion concurrent with the onset of antiferromagnetic order. With complementary Raman scattering and nano-terahertz spectroscopy, we unveil spectral weight redistribution and dielectric screening changes, potentially associated with the multi-magnon continuum, as the underlying mechanism. These results provide solid evidence of coupling between plasmon and antiferromagnetic order, marking a cornerstone for a potential platform for hybrid magnon-plasmon interactions in 2D materials, opening avenues for coherent spin-plasmon devices and tunable terahertz spintronic components.

cond-mat.str-el↗

arXiv2026

Candidate for a Fractional Topological Insulator in Twisted MoTe2

The interplay among electronic correlation, topology, and time-reversal-symmetry (TRS) often leads to exotic quantum states of matter, as highlighted by the discoveries of fractional Chern insulators (FCIs) in twisted bilayer MoTe2 (tMoTe2). Among the FCIs in tMoTe2, the most robust is at a hole filling factor of v=-2/3 per moiré unit cell. Here, employing pump-probe circular dichroism (CD) measurement on tMoTe2 at twist angles (3.9 and 3.7 degrees), we show that a correlated state at v =-4/3 exhibits an unusual Ising antiferromagnet behavior. The v =-4/3 state with no net magnetization undergoes first order phase transitions at extremely low magnetic fields of ~ 2-6 mT to partially valley polarized (PVP) states. This behavior is notably absent for all other correlated states in tMoTe2 and also disappears for v =-4/3 at higher or lower twist angles (4.0 or 3.3 degree). The observed magnetic signature is consistent with a theoretically proposed fractional topological insulator (FTI), consisting of two copies of v =-2/3 FCIs with opposite chirality in the two K valleys. The experimental results are supported by interacting continuum model calculations that reveal the extreme closeness in energy ( < 1 meV) between the putative FTI and PVP states. Our findings present a candidate FTI with TRS and call for advanced transport and imaging measurements to establish the quantized helical edge modes.

cond-mat.str-el↗

arXiv2026

Ultrafast Charge-Doping via Photo-Thermionic Injection in van der Waals Devices

Van der Waals (vdW) heterostructures of two-dimensional (2D) materials have become a rich playground for the exploration of correlated quantum phases, and recent studies have begun to probe their non-equilibrium dynamics under femtosecond laser excitation. In a time-resolved experiment, optical excitation of the multilayer structure can lead not only to rich dynamic responses from the target layers, such as moiré interfaces, but also to additional device functionality from the layer degree of freedom. Here, we investigate optical excitation in a prototypical moiré device of dual-gated twisted WSe2 bilayers, with few-layer graphite gates and hexagonal boron nitride (hBN) spacers. We establish an ultrafast photodoping mechanism in the moiré bilayer from photo-thermionic emission of the graphite gates. Using transient reflectance experiments, we reveal photo-induced hole injection evidenced by: (i) a shift of gate voltages at which optical signatures of correlated insulators are observed, (ii) a persistent optical signature indicative of charge diffusion at microsecond timescales and local charge buildup from pulse-to-pulse accumulation, and (iii) photoinduced absorption due likely to transient formation of correlated insulators. We further demonstrate that the injected holes can be selectively controlled by tuning the excitation energy, fluence, and gate bias.

cond-mat.str-el↗

arXiv2026

Photoinduced Metal-to-Insulator Transitions in 2D Moiré Devices

Photoexcitation has been utilized to control quantum matter and to uncover metastable phases far from equilibrium. Among demonstrations to date, the most common is the photo-induced transition from correlated insulators to metallic states; however, the reverse process without initial orders has not been observed. Here, we show ultrafast metal-to-insulator transition in gate-doped WS2/WSe2 and WSe2/WSe2 moiré devices using photo-thermionic hole injection from graphite gates. The resulting correlated insulators are metastable, with lifetimes exceeding microseconds. These findings establish an effective mechanism for the ultrafast control of correlated electronic phases in van der Waals heterostructures.

cond-mat.str-el↗

arXiv2025

Hidden States and Dynamics of Fractional Fillings in tMoTe2 Moiré Superlattices

The fractional quantum anomalous Hall (FQAH) effect was recently discovered in twisted MoTe2 bilayers (tMoTe2). Experiments to date have revealed Chern insulators from hole doping at v = -1, -2/3, -3/5, and -4/7 (per moiré unit cell). In parallel, theories predict that, between v = -1 and -3, there exist exotic quantum phases, such as the coveted fractional topological insulators (FTI), fractional quantum spin Hall (FQSH) states, and non-abelian fractional states. Here we employ transient optical spectroscopy on tMoTe2 to reveal nearly 20 hidden states at fractional fillings that are absent in static optical sensing or transport measurements. A pump pulse selectively excites charge across the correlated or pseudo gaps, leading to the disordering (melting) of correlated states. A probe pulse detects the subsequent melting and recovery dynamics via exciton and trion sensing. Besides the known states, we observe additional fractional fillings between v = 0 and -1 and a large number of states on the electron doping side (v > 0). Most importantly, we observe new states at fractional fillings of the Chern bands at v = -4/3, -3/2, -5/3, -7/3, -5/2, and -8/3. These states are potential candidates for the predicted exotic topological phases. Moreover, we show that melting of correlated states occurs on two distinct time scales, 2-4 ps and 180-270 ps, attributed to electronic and phonon mechanisms, respectively. We discuss the differing dynamics of the electron and hole doped states from the distinct moiré conduction and valence bands.

cond-mat.str-el↗

arXiv2024

Optical Band Engineering of Monolayer WSe2 in a Scanning Tunneling Microscope

Intense electromagnetic fields can result in dramatic changes in the electronic properties of solids. These changes are commonly studied using optical probes of the modified electronic structure. Here we use optical-scanning tunneling microscopy (optical-STM) equipped with near-field continuous wave (CW) laser excitation to directly measure the electronic structure of light-dressed states in a monolayer transition metal dichalcogenide (TMD) semiconductor, WSe2. We find that the effective tunneling gap and tunneling density of states are strongly influenced by the intensity of the electromagnetic field when the applied field is resonant with the bandgap of the semiconductor. Our findings indicate that CW laser excitation can be used to generate light-dressed electronic states of quantum materials when confined strongly to the nanoscale.

cond-mat.mtrl-sci↗

arXiv2024

Increased formation of trions and charged biexcitons by above-gap excitation in single-layer $WSe_2$

Two-dimensional semiconductors exhibit pronounced many-body effects and intense optical responses due to strong coulombic interactions. Consequently, subtle differences in photoexcitation conditions can strongly influence how the material dissipates energy during thermalization. Here, using multiple excitation spectroscopies, we show that a distinct thermalization pathway emerges at elevated excitation energies, enhancing the formation of trions and charged biexcitons in single-layer WSe2 by up to 2x and 5x, respectively. Power- and temperature-dependent measurements lend insight into the origin of the enhancement. These observations underscore the complexity of excited state relaxation in monolayer semiconductors, provide insight for the continued development of carrier thermalization models, and highlight the potential to precisely control excitonic yields and probe non-equilibrium dynamics in 2D semiconductors.

cond-mat.mtrl-sci↗

arXiv2024

Quantum Noise Spectroscopy of Criticality in an Atomically Thin Magnet

Dynamic critical fluctuations in magnetic materials encode important information about magnetic ordering in the associated critical exponents. Using nitrogen-vacancy centers in diamond, we implement $T_2$ (spin-decoherence) noise magnetometry to study critical dynamics in a 2D Van der Waals magnet CrSBr. By analyzing NV decoherence on time scales approaching the characteristic correlation time $τ_c$ of critical fluctuations, we extract the critical exponent $ν$ for the correlation length. Our result deviates from the Ising prediction and highlights the role of long-range dipolar interactions in 2D CrSBr. Furthermore, analyzing the divergence of the correlation length suggests the possibility of 2D-XY criticality in CrSBr in a temperature window near $T_C$ where static magnetic domains are absent. Our work provides a first demonstration of $T_2$ noise magnetometry to quantitatively analyze critical scaling behavior in 2D materials.

cond-mat.mes-hall↗

arXiv2024

Deep learning analysis of polaritonic waves images

Deep learning (DL) is an emerging analysis tool across sciences and engineering. Encouraged by the successes of DL in revealing quantitative trends in massive imaging data, we applied this approach to nano-scale deeply sub-diffractional images of propagating polaritonic waves in complex materials. We developed a practical protocol for the rapid regression of images that quantifies the wavelength and the quality factor of polaritonic waves utilizing the convolutional neural network (CNN). Using simulated near-field images as training data, the CNN can be made to simultaneously extract polaritonic characteristics and materials parameters in a timescale that is at least three orders of magnitude faster than common fitting/processing procedures. The CNN-based analysis was validated by examining the experimental near-field images of charge-transfer plasmon polaritons at Graphene/α-RuCl3 interfaces. Our work provides a general framework for extracting quantitative information from images generated with a variety of scanning probe methods.

cond-mat.mtrl-sci↗

arXiv2024

Time-Domain Signatures of Distinct Correlated Insulators in a Moiré Superlattice

Among expanding discoveries of quantum phases in moiré superlattices, correlated insulators stand out as both the most stable and most commonly observed. Despite the central importance of these states in moiré physics, little is known about their underlying nature. Here, we use pump-probe spectroscopy to show distinct time-domain signatures of correlated insulators at fillings of one (v = -1) and two (v = -2) holes per moiré unit cell in the angle-aligned WSe2/WS2 system. Following photo-doping, we find that the disordering time of the v = -1 state is independent of excitation density (n_ex), as expected from the characteristic phonon response time associated with a polaronic state. In contrast, the disordering time of the v = -2 state scales with (n_ex)^-0.5, in agreement with plasmonic screening from free holons and doublons. These states display disparate reordering behavior dominated either by first order (v = -1) or second order (v = -2) recombination, suggesting the presence of Hubbard excitons and free carrier-like holons/doublons, respectively. Our work delineates the roles of electron-phonon (e-ph) versus electron-electron (e-e) interactions in correlated insulators on the moiré landscape and establishes non-equilibrium responses as mechanistic signatures for distinguishing and discovering quantum phases.

cond-mat.str-el↗

arXiv2024

Controlled Interlayer Exciton Ionization in an Electrostatic Trap in Atomically Thin Heterostructures

Atomically thin semiconductor heterostructures provide a two-dimensional (2D) device platform for creating high densities of cold, controllable excitons. Interlayer excitons (IEs), bound electrons and holes localized to separate 2D quantum well layers, have permanent out-of-plane dipole moments and long lifetimes, allowing their spatial distribution to be tuned on demand. Here, we employ electrostatic gates to trap IEs and control their density. By electrically modulating the IE Stark shift, electron-hole pair concentrations above $2\times10^{12}$ cm$^{-2}$ can be achieved. At this high IE density, we observe an exponentially increasing linewidth broadening indicative of an IE ionization transition, independent of the trap depth. This runaway threshold remains constant at low temperatures, but increases above 20 K, consistent with the quantum dissociation of a degenerate IE gas. Our demonstration of the IE ionization in a tunable electrostatic trap represents an important step towards the realization of dipolar exciton condensates in solid-state optoelectronic devices.

cond-mat.mes-hall↗

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↗

arXiv2024

Twisted nonlinear optics in monolayer van der Waals crystals

In addition to a plethora of emergent phenomena, the spatial topology of optical vortices enables an array of applications spanning communications to quantum photonics. Nonlinear optics is essential in this context, providing access to an infinitely large set of quantum states associated with the orbital angular momentum of light. Nevertheless, the realization of such processes have failed to keep pace with the ever-growing need to shrink the fundamental length-scale of photonic technologies to the nanometer regime6. Here, we push the boundaries of vortex nonlinear optics to the ultimate limits of material dimensionality. By exploiting second and third-order frequency-mixing processes in semiconducting monolayers, we demonstrate the independent manipulation of the wavelength, orbital angular momentum, and spatial distribution of vortex light-fields. Due to the atomically-thin nature of the host quantum material, this control spans a broad spectral bandwidth in a highly-integrable platform, unconstrained by the traditional limits of bulk nonlinear optical materials. Our work heralds a new avenue for ultra-compact and scalable hybrid nanotechnologies empowered by twisted nonlinear light-matter interactions in van der Waals quantum nanomaterials.

physics.optics↗

arXiv2024

Coherent Modulation of Two-Dimensional Moiré States with On-Chip THz Waves

Van der Waals (vdW) structures of two-dimensional materials host a broad range of physical phenomena. New opportunities arise if different functional layers may be remotely modulated or coupled in a device structure. Here we demonstrate the in-situ coherent modulation of moiré excitons and correlated Mott insulators in transition metal dichalcogenide (TMD) homo- or hetero-bilayers with on-chip terahertz (THz) waves. Using common dual-gated device structures, each consisting of a TMD moiré bilayer sandwiched between two few-layer graphene (fl-Gr) gates with hexagonal boron nitride (h-BN) spacers, we launch coherent phonon wavepackets at ~0.4-1 THz from the fl-Gr gates by femtosecond laser excitation. The waves travel through the h-BN spacer, arrive at the TMD bilayer with precise timing, and coherently modulate the moiré excitons or the Mott states. These results demonstrate that the fl-Gr gates, often used for electrical control of the material properties, can serve as effective on-chip opto-elastic transducers to generate THz waves for the coherent control and vibrational entanglement of functional layers in commonly used moiré devices.

cond-mat.mes-hall↗

arXiv2024

Anomalous Landau level gaps near magnetic transitions in monolayer WSe$_2$

First-order phase transitions produce abrupt changes to the character of both ground and excited electronic states. Here we conduct electronic compressibility measurements to map the spin phase diagram and Landau level (LL) energies of monolayer WSe$_2$ in a magnetic field. We resolve a sequence of first-order phase transitions between completely spin-polarized LLs and states with LLs of both spins. Unexpectedly, the LL gaps are roughly constant over a wide range of magnetic fields below the transitions, which we show reflects a preference for opposite spin excitations of the spin-polarized ground state. These transitions also extend into compressible regimes, with a sawtooth boundary between full and partial spin polarization. We link these observations to the important influence of LL filling on the exchange energy beyond a smooth density-dependent contribution. Our results show that WSe$_2$ realizes a unique hierarchy of energy scales where such effects induce re-entrant magnetic phase transitions tuned by density and magnetic field.

cond-mat.mes-hall↗

arXiv2023

Highly tunable room-temperature plexcitons in monolayer WSe2 /gap-plasmon nanocavities

The advancement of quantum photonic technologies relies on the ability to precisely control the degrees of freedom of optically active states. Here, we realize real-time, room-temperature tunable strong plasmon-exciton coupling in 2D semiconductor monolayers enabled by a general approach that combines strain engineering plus force- and voltage-adjustable plasmonic nanocavities. We show that the exciton energy and nanocavity plasmon resonance can be controllably toggled in concert by applying pressure with a plasmonic nanoprobe, allowing in operando control of detuning and coupling strength, with observed Rabi splittings >100 meV. Leveraging correlated force spectroscopy, nano-photoluminescence (nano-PL) and nano-Raman measurements, augmented with electromagnetic simulations, we identify distinct polariton bands and dark polariton states, and map their evolution as a function of nanogap and strain tuning. Uniquely, the system allows for manipulation of coupling strength over a range of cavity parameters without dramatically altering the detuning. Further, we establish that the tunable strong coupling is robust under multiple pressing cycles and repeated experiments over multiple nanobubbles. Finally, we show that the nanogap size can be directly modulated via an applied DC voltage between the substrate and plasmonic tip, highlighting the inherent nature of the concept as a plexcitonic nano-electro-mechanical system (NEMS). Our work demonstrates the potential to precisely control and tailor plexciton states localized in monolayer (1L) transition metal dichalcogenides (TMDs), paving the way for on-chip polariton-based nanophotonic applications spanning quantum information processing to photochemistry.

physics.optics↗

arXiv2023

Visualizing moiré ferroelectricity via plasmons and nano-photocurrent in graphene/twisted-WSe2 structures

Ferroelectricity, a spontaneous and reversible electric polarization, is found in certain classes of van der Waals (vdW) material heterostructures. The discovery of ferroelectricity in twisted vdW layers provides new opportunities to engineer spatially dependent electric and optical properties associated with the configuration of moiré superlattice domains and the network of domain walls. Here, we employ near-field infrared nano-imaging and nano-photocurrent measurements to study ferroelectricity in minimally twisted WSe2. The ferroelectric domains are visualized through the imaging of the plasmonic response in a graphene monolayer adjacent to the moiré WSe2 bilayers. Specifically, we find that the ferroelectric polarization in moiré domains is imprinted on the plasmonic response of the graphene. Complementary nano-photocurrent measurements demonstrate that the optoelectronic properties of graphene are also modulated by the proximal ferroelectric domains. Our approach represents an alternative strategy for studying moiré ferroelectricity at native length scales and opens promising prospects for (opto)electronic devices.

cond-mat.mes-hall↗

arXiv2023

Spontaneous Exciton Dissociation in Transition Metal Dichalcogenide Monolayers

Since the seminal work on MoS2 monolayers, photoexcitation in atomically-thin transition metal dichalcogenides (TMDCs) has been assumed to result in excitons with large binding energies (~ 200-600 meV). Because the exciton binding energies are order-of-magnitude larger than thermal energy at room temperature, it is puzzling that photocurrent and photovoltage generation have been observed in TMDC-based devices, even in monolayers with applied electric fields far below the threshold for exciton dissociation. Here, we show that the photoexcitation of TMDC monolayers results in a substantial population of free charges. Performing ultrafast terahertz (THz) spectroscopy on large-area, single crystal WS2, WSe2, and MoSe2 monolayers, we find that ~10% of excitons spontaneously dissociate into charge carriers with lifetimes exceeding 0.2 ns. Scanning tunnelling microscopy reveals that photo-carrier generation is intimately related to mid-gap defect states, likely via trap-mediated Auger scattering. Only in state-of-the-art quality monolayers14, with mid-gap trap densities as low as 10^9 cm^-2, does intrinsic exciton physics start to dominate the THz response. Our findings reveal that excitons or excitonic complexes are only the predominant quasiparticles in photo-excited TMDC monolayers at the limit of sufficiently low defect densities.

cond-mat.mes-hall↗