arXiv subjects

Tony F. Heinz

Publications and source records attributed to Tony F. Heinz.

At least 19 recordsLinked to original sources

arXiv2026

Symmetry-selective nonrelativistic spin splitting in antiferromagnets driven by coherent phonons

Nonrelativistic spin splitting (NRSS) in antiferromagnets (AFMs) enables magnetization-free spin polarization for ultrafast spintronics. Here, we demonstrate that coherent phonons can dynamically induce and control NRSS in collinear AFMs. Excitation of $Γ$-point infrared-active phonons lifts the spin degeneracy of the ground state, while the residual sublattice-connecting symmetries determine the momentum-space form of the induced splitting. Because the relevant infrared modes couple to orthogonal in-plane light polarizations, distinct spin-split phases can be selectively activated by the polarization of the driving field. Using first-principles calculations for MnPS$_3$, we show that a mode that breaks all sublattice-connecting symmetries induces an $s$-wave spin-split state with $Δ(Γ)\neq0$, whereas a symmetry-distinct mode that preserves a sublattice-connecting mirror symmetry generates a $d$-wave altermagnetic state with $Δ(Γ)=0$. In both cases, the spin splitting grows linearly with the phonon amplitude and reverses the induced spin polarization when the displacement is reversed. Our results establish coherent lattice driving as a direct, polarization- and mode-selective route to dynamically induce distinct NRSS phases in AFMs.

cond-mat.mtrl-sci↗

arXiv2026

Moiré enabled spin pumping and preservation in MoSe2/WS2 heterobilayers

The spin degree of freedom is a fundamental quantum mechanical attribute with implications spanning from magnetism to quantum computing. Consequently, the relaxation of spin states for extended, Bloch electrons in solids has been studied for decades as it defines many of their properties and applications. We show that moiré patterns in layered materials can extend spin relaxation times by two orders of magnitude to 1 millisecond and beyond. This is achieved by suppressing spin mixing for electrons in 2D semiconductor heterostructures, particularly in the MoSe2/WS2 system, as we elucidate both experimentally and theoretically. The extended longitudinal lifetime facilitates spin alignment over 50% using only nanowatt levels of optical power. Our findings highlight the potential of moiré engineering for future quantum sensing and information processing.

cond-mat.mes-hall↗

arXiv2026

Interfacial control of hot-carrier extraction and photostability in two-dimensional materials

Two-dimensional transition metal dichalcogenides (TMDCs) are promising materials for next-generation optoelectronic devices, yet their implementation is hindered by limited sample stability and challenges in forming reliable electrical contacts. Here, by utilizing time-domain THz emission spectroscopy we directly probe charge carrier dynamics in monolayer WS2 on gold (Au) and fused silica (SiO2) as a function of interface morphology. For laser excitation above the band gap of WS2, we independently extract effective transport times for both electrons and holes and find that discontinuous WS2 contacts on rough Au generate larger net photocurrents than uniform, strongly coupled interfaces - a counterintuitive observation attributed to imbalanced electron and hole transfer from WS2 to Au. Crucially, we demonstrate that ultrafast charge extraction and separation suppress recombination-driven energy release and thereby prevent photo-induced degradation under ambient conditions, eliminating the need for encapsulation. These findings redefine interfacial design as a central control parameter for both performance and stability in 2D optoelectronic devices.

cond-mat.mtrl-sci↗

arXiv2026

Electric-field-tuned consecutive topological phase transitions between distinct correlated insulators in moire MoTe2/WSe2 heterobilayer

Consecutive topological phase transitions (TPTs) between strongly correlated electronic phases that differ simultaneously in symmetry breaking and topological order are of fundamental interest in condensed matter physics, yet are rarely realized experimentally. We report two consecutive electric-field-driven TPTs at half filling (nu = 1) in angle-aligned MoTe2/WSe2 moire heterobilayers. With increasing out-of-plane displacement field, a geometrically frustrated Mott insulator evolves into a ferromagnetic quantum anomalous Hall (QAH) Mott insulator, i.e., a spin-polarized topological Mott insulator without an observable charge-gap closure, and subsequently into an antiferromagnetic, valley-coherent Mott insulator (VC-AFM) accompanied by a continuous charge-gap collapse and the emergence of a critical metallic state. Layer-resolved magnetic circular dichroism (MCD), magneto-transport, and compressibility measurements jointly determine the phase diagram. The high-field evolution of the antiferromagnetic state reveals a metamagnetic-like transition at a critical field B*, above which a Chern insulating transport response reappears. Our results establish the MoTe2/WSe2 moire platform as a tunable realization of an extended Kane-Mele-Hubbard model hosting sequential correlation-topology-intertwined transitions.

cond-mat.str-el↗

arXiv2026

Direct nanoscale mapping of band alignment in single-layer semiconducting lateral heterojunctions

Atomic-scale control over band alignment in single-layer lateral heterostructures (LHSs) of dissimilar transition metal dichalcogenides (TMDCs) is critical for nextgeneration electronic, optoelectronic, and quantum technologies. However, direct experimental access to interfacial electronic states with nanometer precision remains a significant challenge. Here, we employ angle-resolved photoemission spectroscopy with nanoscale spatial resolution (nanoARPES) to directly map the epitaxial alignment and valence band evolution across MoSe2-WSe2 LHSs. By combining nanoARPES with spatially resolved photoluminescence, we correlate the evolution of the valence band maximum and exciton features across both atomically sharp and compositionally graded diffusive interfaces. We identified type-II band alignments governed by both material composition and interstitial-induced modifications of band offsets, in close agreement with density functional theory calculations. These results reveal fundamental mechanisms of electronic structure modulation at 1D TMDC heterointerfaces and provide a robust platform for tailored band engineering in van der Waals materials.

cond-mat.mes-hall↗

arXiv2026

Exciton-polaron Umklapp scattering in Wigner crystals

Strong Coulomb interactions in two-dimensional (2D) semiconductors give rise to tightly bound excitons, exciton polarons, and correlated electronic phases such as Wigner crystals (WCs), yet their mutual interplay remains poorly understood. Here we report the observation of multi-branch excitonic Umklapp scattering in both electron and hole WCs realized in ultraclean monolayer WSe$_2$, exhibiting exceptionally high melting temperatures (T$_c$ $\approx$ 20-30 K). Robust Wigner crystallization activates multiple finite-momentum optical resonances, including quasilinearly dispersing, light-like excitons and exciton polarons, extending far beyond the single excitonic Umklapp feature reported previously. Helicity-resolved magneto-optical measurements reveal a pronounced valley dependence of the scattering processes. Combined experiment and theory identify a polaron-induced brightening mechanism in which exciton polarons transfer oscillator strength from bright zero-momentum states to otherwise dark finite-momentum states, explaining the emergence of multiple Umklapp branches where conventional exciton-WC scattering is ineffective. These results establish WC polarons as a new quasiparticle paradigm and introduce polaron-induced Umklapp scattering as a general route to accessing finite-momentum many-body excitations in 2D quantum materials.

cond-mat.mes-hall↗

arXiv2025

Room-temperature valley-selective emission in Si-MoSe2 heterostructures enabled by high-quality-factor chiroptical cavities

Transition metal dichalcogenides possess valley pseudospin, enabling coupling between photon spin and electron spin for classical and quantum information processing. However, rapid valley-dephasing processes have impeded the development of scalable, high-performance valleytronic devices operating at room temperature. Here we demonstrate that a chiral resonant metasurface can enable room-temperature valley-selective emission in MoSe2 monolayers independent of excitation polarization. This platform provides circular eigen-polarization states with a high quality factor (Q-factor) and strong chiral near-field enhancement. The fabricated Si chiral metasurfaces exhibit chiroptical resonances with Q-factors up to 450 at visible wavelengths. We reveal degrees of circular polarization (DOP) reaching a record high of 0.5 at room temperature. Our measurements show that the high DOP can be attributed to the significantly increased chiroptical local density of states, which enhances valley-specific radiative transition rates by a factor of ~13. Our work could facilitate the development of ultracompact chiral classical and quantum light sources.

physics.optics↗

arXiv2025

Terahertz field-induced giant symmetry modulations in a van der Waals antiferromagnet

Strong-field terahertz (THz) excitations enable dynamic control over electronic, lattice and symmetry degrees of freedom in quantum materials. Here, we uncover pronounced terahertz-induced symmetry modulations and coherent phonon dynamics in the van der Waals antiferromagnet MnPS3, in which inversion symmetry is broken by its antiferromagnetic spin configuration. Time-resolved second harmonic generation measurements reveal long-lived giant oscillations in the antiferromagnetic phase, with amplitudes comparable to the equilibrium signal, driven by phonons involving percent-level atomic displacements relative to the equilibrium bond lengths. The temporal evolution of the rotational anisotropy patterns indicate a dynamic breaking of mirror symmetry, modulated by two vibrational modes at 1.7 THz and 4.5 THz, with the former corresponding to a hidden mode not observed in equilibrium spectroscopy. We show that these effects arise in part from a field-induced charge rearrangement mechanism that lowers the local crystal symmetry, and couples to the phonon modes. A long-lived field-driven response was uncovered with a complex THz polarization dependence which, in comparison to theory, indicates evidence for an antiferromagnetic-to-ferrimagnetic transition. Our results establish an effective field-tunable pathway for driving excitations otherwise weak in equilibrium, and for manipulating magnetism in low-dimensional materials via dynamical modulation of symmetry.

cond-mat.str-el↗

arXiv2025

Nonresonant Raman control of ferroelectric polarization

Important advances have recently been made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light-matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes has been experimentally observed and proposed for dynamic material control, but the resulting atomic excursion has been limited to perturbative levels. Here, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.

physics.optics↗

arXiv2025

Roadmap for Photonics with 2D Materials

Triggered by the development of exfoliation and the identification of a wide range of extraordinary physical properties in self-standing films consisting of one or few atomic layers, two-dimensional (2D) materials such as graphene, transition metal dichalcogenides (TMDs), and other van der Waals (vdW) crystals currently constitute a wide research field protruding in multiple directions in combination with layer stacking and twisting, nanofabrication, surface-science methods, and integration into nanostructured environments. Photonics encompasses a multidisciplinary collection of those directions, where 2D materials contribute with polaritons of unique characteristics such as strong spatial confinement, large optical-field enhancement, long lifetimes, high sensitivity to external stimuli (e.g., electric and magnetic fields, heating, and strain), a broad spectral range from the far infrared to the ultraviolet, and hybridization with spin and momentum textures of electronic band structures. The explosion of photonics with 2D materials as a vibrant research area is producing breakthroughs, including the discovery and design of new materials and metasurfaces with unprecedented properties as well as applications in integrated photonics, light emission, optical sensing, and exciting prospects for applications in quantum information, and nanoscale thermal transport. This Roadmap summarizes the state of the art in the field, identifies challenges and opportunities, and discusses future goals and how to meet them through a wide collection of topical sections prepared by leading practitioners.

cond-mat.mtrl-sci↗

arXiv2024

Chemically Tailored Growth of 2D Semiconductors via Hybrid Metal-Organic Chemical Vapor Deposition

Two-dimensional (2D) semiconducting transition-metal dichalcogenides (TMDCs) are an exciting platform for new excitonic physics and next-generation electronics, creating a strong demand to understand their growth, doping, and heterostructures. Despite significant progress in solid-source (SS-) and metal-organic chemical vapor deposition (MOCVD), further optimization is necessary to grow highly crystalline 2D TMDCs with controlled doping. Here, we report a hybrid MOCVD growth method that combines liquid-phase metal precursor deposition and vapor-phase organo-chalcogen delivery to leverage the advantages of both MOCVD and SS-CVD. Using our hybrid approach, we demonstrate WS$_2$ growth with tunable morphologies - from separated single-crystal domains to continuous monolayer films - on a variety of substrates, including sapphire, SiO$_2$, and Au. These WS$_2$ films exhibit narrow neutral exciton photoluminescence linewidths down to 33 meV and room-temperature mobility up to 34 - 36 cm$^2$V$^-$$^1$s$^-$$^1$). Through simple modifications to the liquid precursor composition, we demonstrate the growth of V-doped WS$_2$, MoxW$_1$$_-$$_x$S$_2$ alloys, and in-plane WS$_2$-MoS$_2$ heterostructures. This work presents an efficient approach for addressing a variety of TMDC synthesis needs on a laboratory scale.

physics.app-ph↗

arXiv2024

Direct Exfoliation of Nanoribbons from Bulk van der Waals Crystals

Confinement of monolayers into quasi-one-dimensional atomically-thin nanoribbons could lead to novel quantum phenomena beyond those achieved in their bulk and monolayer counterparts. However, current experimental availability of nanoribbon species beyond graphene has been limited to bottom-up synthesis or top-down patterning. In this study, we introduce a versatile and direct lithography-free approach to exfoliate a variety of bulk van der Waals (vdW) crystals into nanoribbons. Akin to the Scotch tape exfoliation in producing monolayers, this technique provides convenient access to a wide range of nanoribbons derived from their corresponding bulk crystals, including MoS2, WS2, MoSe2, WSe2, MoTe2, WTe2, ReS2, and hBN. The nanoribbons are single-crystalline, parallel-aligned, flat, and have high aspect ratio. We demonstrated the electrical, magnetic, and optical properties from the confinement, strain, and edge configurations of these nanoribbons. This versatile preparation technique will pave the way for future experimental investigation and broad applications in optoelectronic, sensing, electronic and quantum devices.

cond-mat.mtrl-sci↗

arXiv2023

Millimeter-scale exfoliation of hBN with tunable flake thickness

As a two-dimensional (2D) dielectric material, hexagonal boron nitride (hBN) is in high demand for applications in photonics, nonlinear optics, and nanoelectronics. Unfortunately, the high-throughput preparation of macroscopic-scale, high-quality hBN flakes with controlled thickness is an ongoing challenge, limiting device fabrication and technological integration. Here, we present a metal thin-film exfoliation method to prepare hBN flakes with millimeter-scale dimension, near-unity yields, and tunable flake thickness distribution from 1-7 layers, a substantial improvement over scotch tape exfoliation. The single crystallinity and high quality of the exfoliated hBN are demonstrated with optical microscopy, atomic force microscopy, Raman spectroscopy, and second harmonic generation. We further explore a possible mechanism for the effectiveness and selectivity based on thin-film residual stress measurements, density functional theory calculations, and transmission electron microscopy imaging of the deposited metal films. We find that the magnitude of the residual tensile stress induced by thin film deposition plays a key role in determining exfoliated flake thickness in a manner which closely resembles 3D semiconductor spalling. Lastly, we demonstrate that our exfoliated, large-area hBN flakes can be readily incorporated as encapsulating layers for other 2D monolayers. Altogether, this method brings us one step closer to the high throughput, mass production of hBN-based 2D photonic, optoelectronic, and quantum devices.

cond-mat.mtrl-sci↗

arXiv2023

Quantum control of exciton wavefunctions in 2D semiconductors

Excitons -- bound electron-hole pairs -- play a central role in light-matter interaction phenomena, and are crucial for wide-ranging applications from light harvesting and generation to quantum information processing. A long-standing challenge in solid-state optics has been to achieve precise and scalable control over the quantum mechanical state of excitons in semiconductor heterostructures. Here, we demonstrate a technique for creating tailored and tunable potential landscapes for optically active excitons in 2D semiconductors that enables in-situ wavefunction shaping at the nanoscopic lengthscale. Using nanostructured gate electrodes, we create localized electrostatic traps for excitons in diverse geometries such as quantum dots and rings, and arrays thereof. We show independent spectral tuning of multiple spatially separated quantum dots, which allows us to bring them to degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wavefunctions in optical reflection and photoluminescence measurements. Our work introduces a new approach to engineering exciton dynamics and interactions at the nanometer scale, with implications for novel optoelectronic devices, topological photonics, and many-body quantum nonlinear optics.

cond-mat.mes-hall↗

arXiv2023

Achiral dielectric metasurfaces for spectral and polarization control of valley specific light emission from monolayer MoS2

Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically accessed and manipulated for quantum information processing. Here, we integrate MoS2 with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface Mie modes, the intensity and lifetime of the emission of neutral excitons, trions and defect bound excitons can be enhanced, while the spectral shape can be modified. Additionally, we demonstrate the symmetric enhancement of the degree-of-polarization (DOP) of neutral exciton and trions via valley-resolved PL measurements, and find that the DOP can be as high as 24% for exciton emission and 34% for trion emission at 100K. These results can be understood by analyzing the near-field impact of metasurface resonators on both the chiral absorption of MoS2 emitters as well as the enhanced emission from the Purcell effect. Combining Si-compatible photonic design with large-scale (mm-scale) 2D materials integration, our work makes an important step towards on-chip valleytronic applications approaching room-temperature operation.

physics.optics↗

arXiv2022

High-harmonic generation from artificially stacked 2D crystals

We report a coherent layer-by-layer high-order harmonic generation (HHG) build-up in artificially stacked transition metal dichalcogenides (TMDC) crystals in their various stacking configurations. In the experiments, millimeter-sized single crystalline monolayers are synthesized using the gold foil-exfoliation method, followed by artificially stacking on a transparent substrate. High-order harmonics up to the 19th order are generated by the interaction with an ultrafast mid-infrared (MIR) driving laser. We find that the generation is sensitive to the number of layers and their relative orientation. For AAAA stacking configuration, both odd- and even-orders exhibit a quadratic increase in intensity as a function of the number of layers, which is a signature of constructive interference of high-harmonic emission from successive layers. Particularly, we observe some deviations from this scaling at photon energies above the bandgap, which is explained by self-absorption effects. For AB and ABAB stacking, even-order harmonics remain below the detection level, consistent with the presence of inversion symmetry. Our study confirms the capability of producing non-perturbative high-order harmonics from stacked layered materials subjected to intense MIR fields without damaging samples. It has implications for optimizing solid-state HHG sources at the nano-scale and developing high-harmonics as an ultrafast probe of artificially stacked layered materials. Because the HHG process is a strong-field driven process, it has the potential to probe high-momentum and energy states in the bandstructure combined with atomic-scale sensitivity in real space, making it an attractive probe of novel material structures such as the Moiré pattern.

physics.optics↗

arXiv2022

Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-ray Spectroscopy

The electronic excitation occurring on adsorbates at ultrafast time scales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast temporal evolution of X-ray absorption spectroscopy (XAS) and X-ray emission spectroscopy (XES) of a simple well known adsorbate prototype system, namely carbon (C) atoms adsorbed on a nickel (Ni(100)) surface, following intense laser optical pumping at 400 nm. We observe ultrafast (~100 fs) changes in both XAS and XES showing clear signatures of the formation of a hot electron-hole pair distribution on the adsorbate. This is followed by slower changes on a few ps time scale, shown to be consistent with thermalization of the complete C/Ni system. Density functional theory spectrum simulations support this interpretation.

physics.chem-ph↗

arXiv2022

Floquet engineering of strongly-driven excitons in monolayer tungsten disulfide

Interactions of quantum materials with strong-laser fields can induce exotic nonequilibrium electronic states. Monolayer transition-metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement, offer exceptional opportunities toward Floquet engineering of quasiparticle electron-hole states, or excitons. Strong-field driving has a potential to achieve enhanced control of electronic band structure, thus a possibility to open a new realm of exciton light-matter interactions. However, experimental implementation of strongly-driven excitons has so far remained out of reach. Here, we use mid-infrared laser pulses below the optical bandgap to excite monolayer tungsten disulfide up to a field strength of 0.3 V/nm, and demonstrate strong-field light dressing of excitons in the excess of a hundred millielectronvolt. Our high-sensitivity transient absorption spectroscopy further reveals formation of a virtual absorption feature below the 1s-exciton resonance, which is assigned to a light-dressed sideband from the dark 2p-exciton state. Quantum-mechanical simulations substantiate the experimental results and enable us to retrieve real-space movies of the exciton dynamics. This study advances our understanding of the exciton dynamics in the strong-field regime, and showcases the possibility of harnessing ultrafast, strong-field phenomena in device applications of two-dimensional materials.

cond-mat.mtrl-sci↗