Tony F Heinz

Vertically stacked van der Waals (vdW) heterostructures exhibit unique electronic, optical, and thermal properties that can be manipulated by twist-angle engineering. However, the weak phononic coupling at a bilayer interface imposes a fundamental thermal bottleneck for future two-dimensional devices. Using ultrafast electron diffraction, we directly investigated photoinduced nonequilibrium phonon dynamics in MoS2/WS2 at 4° twist angle and WSe2/MoSe2 heterobilayers with twist angles of 7°, 16°, and 25°. We identified an interlayer heat transfer channel with a characteristic timescale of ~20 picoseconds, about one order of magnitude faster than molecular dynamics simulations assuming initial intralayer thermalization. Atomistic calculations involving phonon-phonon scattering suggest that this process originates from the nonthermal phonon population following the initial interlayer charge transfer and …

Phonon polaritons, the hybrid quasiparticles resulting from the coupling of photons and lattice vibrations, have gained significant attention in the field of layered van der Waals heterostructures. Particular interest has been paid to hetero‐bicrystals composed of molybdenum oxide (MoO3) and hexagonal boron nitride (hBN), which feature polariton dispersion tailorable via avoided polariton mode crossings. In this work, we systematically study the polariton eigenmodes in MoO3‐hBN hetero‐bicrystals self‐assembled on ultrasmooth gold using synchrotron infrared nanospectroscopy. We experimentally demonstrate that the spectral gap in bicrystal dispersion and corresponding regimes of negative refraction can be tuned by material layer thickness, and we quantitatively match these results with a simple analytic model. We also investigate polaritonic cavity modes and polariton propagation along “forbidden” directions …

The discoveries of ferromagnetism down to the atomically thin limit in van der Waals (vdW) crystals by mechanical exfoliation have enriched the family of magnetic thin films [C. Gong et al., Nature 546, 265–269 (2017) and B. Huang et al., Nature 546, 270–273 (2017)]. However, compared to the study of traditional magnetic thin films by physical deposition methods, the toolbox of the vdW crystals based on mechanical exfoliation and transfer suffers from low yield and ambient corrosion problem and now is facing new challenges to study magnetism. For example, the formation of magnetic superlattice is difficult in vdW crystals, which limits the study of the interlayer interaction in vdW crystals [M. Gibertini, M. Koperski, A. F. Morpurgo, K. S. Novoselov, Nat. Nanotechnol. 14, 408–419 (2019)]. Here, we report a strategy of interlayer engineering of the magnetic vdW crystal Fe3GeTe2 (FGT) by intercalating quaternary …

Moiré materials provide fertile ground for the correlated and topological quantum phenomena. Among them, the quantum anomalous Hall (QAH) effect, in which the Hall resistance is quantized even under zero magnetic field, is a direct manifestation of the intrinsic topological properties of a material and an appealing attribute for low-power electronics applications. The QAH effect has been observed in both graphene and transition metal dichalcogenide (TMD) moiré materials. It is thought to arise from the interaction-driven valley polarization of the narrow moiré bands. Here, we show that the newly discovered QAH state in AB-stacked MoTe 2/W S e 2 moiré bilayers is not valley polarized but valley coherent. The layer-and helicity-resolved optical spectroscopy measurement reveals that the QAH ground state possesses spontaneous spin (valley) polarization aligned (antialigned) in two TMD layers. In addition …

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 excitonic motion. We present a technique using nanostructured gate electrodes to create tailored potential landscapes for excitons in 2D semiconductors, enabling in situ wave function shaping at the nanoscale. Our approach forms electrostatic traps for excitons in various geometries, such as quantum dots, rings, and arrays thereof. We show independent spectral tuning of spatially separated quantum dots, achieving degeneracy despite material disorder. Owing to the strong light-matter coupling of excitons in 2D semiconductors, we observe unambiguous signatures of confined exciton wave functions in …

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.

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.

Photoinduced charge transfer in van der Waals heterostructures occurs on the 100 fs timescale despite weak interlayer coupling and momentum mismatch. However, little is understood about the microscopic mechanism behind this ultrafast process and the role of the lattice in mediating it. Here, using femtosecond electron diffraction, we directly visualize lattice dynamics in photoexcited heterostructures of WSe2/WS2 monolayers. Following the selective excitation of WSe2, we measure the concurrent heating of both WSe2 and WS2 on a picosecond timescale—an observation that is not explained by phonon transport across the interface. Using first-principles calculations, we identify a fast channel involving an electronic state hybridized across the heterostructure, enabling phonon-assisted interlayer transfer of photoexcited electrons. Phonons are emitted in both layers on the femtosecond timescale via this channel …

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and certain topological properties, such as the Berry curvature and the quantum metric tensor, have attracted considerable interest. Here, we report giant room-temperature nonlinearities in non-centrosymmetric two-dimensional topological materials—the Janus transition metal dichalcogenides in the 1 T’ phase, synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently show orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities in 1 T’ MoSSe (e.g., > 50 times higher than 2H MoS2 for 18th order harmonic generation; > 20 times higher than 2H MoS2 for terahertz emission). We …

We report optical pumping and x-ray absorption spectroscopy experiments at the Pohang Accelerator Laboratory free electron laser that probes the electron dynamics of a graphene monolayer adsorbed on copper in the femtosecond regime. By analyzing the results with ab initio theory we infer that the excitation of graphene is dominated by indirect excitation from hot electron-hole pairs created in the copper by the optical laser pulse. However, once the excitation is created in graphene, its decay follows a similar path as in many previous studies of graphene adsorbed on semiconductors, ie, rapid excitation of strongly coupled optical phonons and eventual thermalization. It is likely that the lifetime of the hot electron-hole pairs in copper governs the lifetime of the electronic excitation of the graphene.

We report a coherent layer-by-layer build-up of high-order harmonic generation (HHG) 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 a mid-infrared (MIR) driving laser. We find that the generation is sensitive to both 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 …

The layered transition-metal dichalcogenide material 1T-TaS2 possesses successive phase transitions upon cooling, resulting in strong electron–electron correlation effects and the formation of charge density waves (CDWs). Recently, a dimerized double-layer stacking configuration was shown to form a Peierls-like instability in the electronic structure. To date, no direct evidence for this double-layer stacking configuration using optical techniques has been reported, in particular through Raman spectroscopy. Here, we employ a multiple excitation and polarized Raman spectroscopy to resolve the behavior of phonons and electron–phonon interactions in the commensurate CDW lattice phase of dimerized 1T-TaS2. We observe a distinct behavior from what is predicted for a single layer and probe a richer number of phonon modes that are compatible with the formation of double-layer units (layer dimerization). The …

Van der Waals (vdW) materials have opened up many avenues for discovery through layer assembly, as epitomized by interlayer dipolar excitons that exhibit electrically tunable luminescence, lasing and exciton condensation. Extending interlayer excitons to more vdW layers, however, raises fundamental questions concerning coherence within excitons and coupling between moiré superlattices at multiple interfaces. Here, by assembling angle-aligned WSe2/WS2/WSe2 heterotrilayers, we demonstrate the emergence of quadrupolar excitons. We confirm the exciton’s quadrupolar nature by the decrease in its energy of 12 meV from coherent hole tunnelling between the two outer layers, its tunable static dipole moment under an external electric field and the reduced exciton–exciton interactions. At high exciton density, we also see signatures of a phase of oppositely aligned dipolar excitons, consistent with a …

Strain provides a powerful method to study 2D monolayers and to tune their properties. The same approach also has great potential for van-der-Waals (vdW) heterostructures. However, we need to understand how strain can be applied to vertically stacked vdW structures, for which strain transfer from one layer to the next remains little explored. In our experiment, we fabricated vertical heterostructures consisting of transition metal dichalcogenides (TMDCs) monolayers that were deposited on a flexible substrate. These TMDC heterostructures allowed us to read out separately the strain in each monolayer by photoluminescence measurements. We find that, in TMDC heterostructures with large twist angles (>5°), strain transfer is limited. However, for aligned heterostructures with small twist angles (≤5°), near unity strain transfer efficiency is observed. We correlate this finding with the moiré domains formed in the …

Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically manipulated for quantum information processing. Here, we integrate MoS2 monolayers with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface electric and magnetic Mie modes, the intensity and lifetime of the emission of neutral excitons, trions, and defect bound excitons can be enhanced and shortened, respectively, while the spectral shape can be modified. Additionally, the degree of polarization (DOP) of exciton and trion emission from the valley can be symmetrically enhanced at 100 K. The DOP increase is attributed to both the metasurface-enhanced chiral absorption of light and the metasurface-enhanced exciton emission from the Purcell effect. Combining Si-compatible photonic design with large …

Interactions of quantum materials with strong laser fields can induce exotic non-equilibrium electronic states, , , , –. Monolayer transition metal dichalcogenides, a new class of direct-gap semiconductors with prominent quantum confinement, offer exceptional opportunities for the Floquet engineering of excitons, which are quasiparticle electron–hole correlated states. Strong-field driving has the potential to achieve enhanced control of the electronic band structure and thus the possibility of opening a new realm of exciton light–matter interactions. However, a full characterization of strong-field driven exciton dynamics, has been difficult. Here we use mid-infrared laser pulses below the optical bandgap to excite monolayer tungsten disulfide and demonstrate strong-field light dressing of excitons in excess of a hundred millielectronvolts. Our high-sensitivity transient absorption spectroscopy further reveals the formation of …

Low-dimensional, strongly anisotropic nanomaterials can support hyperbolic phonon polaritons, which feature strong light–matter interactions that can enhance their capabilities in sensing and metrology tasks. In this work, we report hyperbolic polaritonic rulers, based on microscale α-phase molybdenum trioxide (α-MoO3) waveguides and resonators suspended over an ultraflat gold substrate, which exhibit near-field polaritonic characteristics that are exceptionally sensitive to device geometry. Using scanning near-field optical microscopy, we show that these systems support strongly confined image polariton modes that exhibit ideal antisymmetric gap polariton dispersion, which is highly sensitive to air gap dimensions and can be described and predicted using a simple analytic model. Dielectric constants used for modeling are accurately extracted using near-field optical measurements of α-MoO3 waveguides in …

We directly image valley-polarized excitons in a WSe 2/MoS 2 heterostructure using time-and angle-resolved micro photoemission spectroscopy, before and after interlayer exciton formation.

Under strong electromagnetic excitation, electron–hole (e-h) pairs may be generated in solids, which are subsequently driven to high energy and high momentum, producing high harmonics (HH) of the driving field. The HH efficiency depends on the degree of coherence between the driven electron and hole created by the laser field. Here, we disrupt this e-h coherence in an atomically thin semiconductor by photodoping via incoherent e-h pairs. We observe a strong, systematic harmonic order-dependent intensity reduction. This trend is explained by an exponential decay of the inter-band polarization, proportional to the sub-cycle excursion time of the e-h pair. Our study provides a platform to probe the importance of many-body effects, such as excitation density-dependent decoherence time for strongly driven electrons without the need of ultrashort laser pulses.

We demonstrate the growth, assembly, and characterization of ultrahigh quality polaritonic systems based on α-MoO3 microplates and nanoribbons. These micro- and nanostructures are bottom-up-synthesized single crystals with minimal impurities. By optimizing the growth conditions, we also realize morphology control of the α-MoO3 structures. We observe highly confined polariton modes in the individual structures by using scattering-type scanning near-field optical microscopy. These highly confined polariton modes are of fundamental and technological interest.