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Moshe Ben Shalom

Publications and source records attributed to Moshe Ben Shalom.

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Polytype-Dependent Upconversion Photoluminescence in 3R-MoS2

Ferroelectric van der Waals materials offer switchable polarization states, yet optical readout of their stacking configurations remains challenging. Here, building on the resonant exciton-exciton annihilation (EEA) mechanism recently identified in 2H-phase TMDs, we report the first observation of upconversion photoluminescence (UPL) in rhombohedral MoS$_2$ and demonstrate that this many-body process is strongly polytype-dependent. Using low-temperature spectroscopy, we observe anti-Stokes emission with superlinear power dependence characteristic of EEA. Beyond serving as an accurate layer-number sensor due to discrete bandgap variations, UPL provides a sensitive probe of stacking order across thicknesses. The two neutral trilayer polytypes, which remain indistinguishable by surface potential measurements and second harmonic generation, exhibit markedly different UPL intensities. This sensitivity persists in thicker samples where multiple configurations coexist. First-principles calculations suggest that the intensity contrast originates primarily from the layer confinement of the annihilating excitons, while energy matching to the $Γ$ final-state manifold provides additional intensity selectivity. Power-dependent spectroscopy further disentangles two distinct annihilation channels originating from different dark exciton valleys, identified through their contrasting intensity scaling and opposite density-induced energy shifts. Crucially, the annihilation process doubles the energy separation of nearly degenerate dark excitons while converting their weak emission into bright signal, providing experimental access to valley-specific responses that are obscured in direct dark-exciton spectroscopy. Our findings demonstrate that ferroelectric configurations provide a new degree of freedom for controlling nonlinear optical processes.

cond-mat.mtrl-sci

Chiral, Electronically Decoupled Layers of 1T'-WS2 Topological Insulator via Neutral-Molecule Intercalation

Monolayer 1T'-WS2 is predicted to be a two-dimensional topological insulator, but its intrinsic electronic properties are masked by strong interlayer coupling in its metallic and superconducting bulk parent phase, 2M-WS2. Isolating monolayers by mechanical exfoliation is also hindered by this coupling, preventing experimental examination of monolayer properties. Here we show that 2M-WS2 undergoes amine intercalation through a simple wet-chemical reaction, yielding superlattices in which the 1T' layers are structurally preserved but electronically decoupled by neutral molecular spacers. Intercalation expands the interlayer spacing from 0.5 to 1-4 nm and reconstructs the stacking while preserving the intralayer 1T' framework. Controlled (de)intercalation reversibly switches the system between a superconducting metal and an insulator with an activation gap matching that of the isolated monolayer. Density functional theory indicates that the electronically decoupled layers retain the nontrivial Z2 topology of the monolayer. Chiral amine intercalation further induces chiroptical activity in WS2 electronic transitions. Overall, the successful intercalation challenges the long-held view that group VIB dichalcogenides are inert toward neutral-molecule intercalation and demonstrates molecular intercalation as a general chemical route for realizing monolayer-like topological-insulator physics and enabling chiral van der Waals superlattices in bulk single crystals.

cond-mat.mtrl-sci

A Sliding Ferroelectric Resonant Tunnel Junction

Ferroelectric tunnel junctions (FTJs) leverage polarization-dependent tunneling through ultrathin barriers to enable two-terminal, non-volatile memory and logic. Although conceptually appealing, the practical implementation of conventional FTJs has been hindered by high coercive voltages, low readout currents, limited cycling endurance, and significant device-to-device variability. Here, we overcome these bottlenecks by introducing the sliding ferroelectric resonant tunnel (SFeRT) junction, integrating three cooperative mechanisms: (i) spontaneous interfacial polarization of atomically thin, depolarization-resilient barriers; (ii) superlubric sliding of shear-solitons, enabling ultra-low-friction, wear-free switching; and (iii) momentum-conserving, elastic resonant tunneling between lattice-aligned graphitic electrodes, providing sensitive readouts at both positive and negative biases. We demonstrate nanometer-scale SFeRT junctions using polar polytypes of hexagonal boron nitride (hBN) or transition metal dichalcogenides (TMDs) as barriers, achieving configurable writing voltages below $0.5$ V and tunable reading biases under $0.1$ V. These devices yield current densities exceeding $50$ nA $μ$m$^{-2}$, with a robust room-temperature ON/OFF ratio $> 7$. The crystalline and polarization integrity of sliding van der Waals (vdW) polytypes, down to the atomically thin limit, ensures exceptional device uniformity and performance that remains scalable down to sub-$0.1$ $μ$m$^{2}$ footprints. Furthermore, we provide a predictive model for SFeRT performance across diverse doping levels, temperatures, electrodes, and polytype configurations. Integrated within a Superlubric Array of Polytypes (SLAP) architecture, SFeRT junctions enable switching energies below $1$ fJ, establishing a scalable and durable foundation for low-energy ``slidetronic'' logic and memory.

cond-mat.other

Photoluminescence Detection of Polytype Polarization in r-MoS2 Enabled by Asymmetric Dielectric Environments

The rhombohedral (r) polytypes of transition metal dichalcogenides (TMDs) constitute a novel class of two-dimensional ferroelectric materials, where lateral shifts between parallel layers induce reversible out-of-plane polarization. This emerging field, known as SlideTronics, holds significant potential for next-generation electronic and optoelectronic applications. While extensive studies have investigated the effects of electrical and chemical doping on excitonic signatures in 2H-TMDs, as well as the influence of dielectric environments on their optical properties, the impact of intrinsic polarization in asymmetric environments remains largely unexplored. Here, we demonstrate a striking polarization-dependent photoluminescence (PL) contrast of up to 400\% between ferroelectric domains in bilayer and trilayer rhombohedral molybdenum disulfide (r-MoS2). This pronounced contrast arises from an asymmetric dielectric environment, which induces polarization-dependent shifts in the Fermi energy, leading to a modulation of the exciton-trion population balance. A detailed temperature-dependent line shape analysis of the PL, conducted from 4K to room temperature, reveals domain-specific trends that further reinforce the connection between polarization states and excitonic properties. The persistence of these distinct optical signatures at room temperature establishes PL as a robust and non-invasive probe for ferroelectric domain characterization, particularly in fully encapsulated device architectures where conventional techniques, such as Kelvin probe force microscopy, become impractical.

cond-mat.mtrl-sci

Switching Graphitic Polytypes in Elastically Coupled Islands

Van der Waals polytypes are commensurate configurations of two-dimensional layers with discrete crystalline symmetries and distinct stacking-dependent properties. In graphitic polytypes, the different stacking arrangements of graphene sheets exhibit rich electronic phases, such as intrinsic electric polarizations, orbital magnetizations, superconductivity, and anomalous fractional Hall states. Switching between these metastable periodic configurations by controlling interlayer shifts unlocks intriguing multiferroic responses. Here, we report super-lubricant arrays of polytypes (SLAP) devices, with nanometer-scale islands of Bernal polytypes that switch into Rhombohedral crystals and vice versa under a shear force as low as 6 nano-Newtons. We assemble these four-layer SLAP structures by aligning a pair of graphene bilayers above and under circular cavities in a misaligned spacer layer. Using local current measurements, we detect the shifts between the active bilayers and reveal long-range elastic relaxations outside the cavities that enable efficient nucleation and spontaneous sliding of stacking dislocation inside the islands. We demonstrate configurable, deterministic, and robust polytype switching by confining these boundary strips in narrow cavity channels that connect the islands. Such controlled switching between elastically-coupled single-crystalline islands is appealing for novel multiferroic SlideTronic applications.

cond-mat.mes-hall

Shaping Exciton Polarization Dynamics in 2D Semiconductors by Tailored Ultrafast Pulses

The ultrafast formation of strongly bound excitons in two-dimensional semiconductors provide a rich platform for studying fundamental physics as well as developing novel optoelectronic technologies. While extensive research has explored the excitonic coherence, many-body interactions, and nonlinear optical properties, the potential to study these phenomena by directly controlling their coherent polarization dynamics has not been fully realized. In this work, we use a sub-10fs pulse shaper to study how temporal control of coherent exciton polarization affects the generation of four-wave mixing in monolayer WSe2 under ambient conditions. By tailoring multiphoton pathway interference, we tune the nonlinear response from destructive to constructive interference, resulting in a 2.6-fold enhancement over the four-wave mixing generated by a transform-limited pulse. This demonstrates a general method for nonlinear enhancement by shaping the pulse to counteract the temporal dispersion experienced during resonant light-matter interactions. Our method allows us to excite both 1s and 2s states, showcasing a selective control over the resonant state that produces nonlinearity. By comparing our results with theory, we find that exciton-exciton interactions dominate the nonlinear response, rather than Pauli blocking. This capability to manipulate exciton polarization dynamics in atomically thin crystals lays the groundwork for exploring a wide range of resonant phenomena in condensed matter systems and opens up new possibilities for precise optical control in advanced optoelectronic devices.

physics.optics

Switchable Crystalline Islands in Super Lubricant Arrays

Expanding the performance of field effect devices is a key challenge of the ever-growing chip industry at the core of current technologies. A highly desired nonvolatile response in tiny multiferroic transistors is expected by electric field control of atomic movements rather than the typical electronic redistribution. Recently, such field effect control of structural transitions was established in commensurate stacking configurations of honeycomb van der Waals (vdW) polytypes by sliding narrow boundary dislocations between oppositely polarized domains. The interfacial ferroelectric response, however, relied on preexisting boundary strips between relatively large micron-scale domains, severely limiting practical implementations. Here, we report the robust switching of single-domain polytypes in nm-scale islands embedded in super lubricant vdW arrays. We etch cavities into a thin layered spacer and then encapsulate it with parallel functional flakes. The incommensurate flakes above and under the spacer sag and touch at each cavity to form uniform crystalline islands free from interlayer deformations. By imaging the polytypes' ferroelectric response, we observe reversible nucleation and annihilation of boundary strips and geometry-adaptable hysteresis loops. Using mechanical stress, we accurately position the boundary strip, modify the interlayer twist angle, and nucleate intermediate polar domain patterns. By precisely designing the size, shape, symmetry, and distribution of the islands in these Super Lubricant Arrays of Polytype (SLAP), we envision numerous device functionalities and SlideTronics applications. These range from ultra-sensitive detectors of atomic-scale shifts to nonvolatile multi-ferroic tunneling transistors with tunable coercive switching fields, and even elastically-coupled memory cells for neuromorphic architectures.

cond-mat.mtrl-sci

Sliding van der Waals Polytypes

Compared to electronic phase transitions, structural phase transitions of crystals are challenging to control due to the energy cost of breaking dense solid bonds. Recently, however, electric field switching of stacking configuration between honeycomb layers, held together by relatively weak van der Waals (vdW) attractions, was demonstrated. In response to the external fields, the layers slide between commensurate meta-stable configurations with discrete symmetries and distinct lattice orientations. These 2D vdW polytypes host diverse electronic orders such as ferroelectricity and magnetism, providing multiferroic switching via lubricant sliding of incommensurate boundary strips. Ahead, we address recent observations in honeycomb polytypes and identify remaining challenges for extending this conceptual "SlideTronics" mechanism into rapid, local, and practical multiferroic devices. The stacking energies, symmetries, and orbital overlaps that underlie the band structures and internal charge distributions are discussed, along with poly-properties like interfacial-ferroelectricity, ladder-like cumulative polarization, superconductivity, and orbital magnetic orders. Distinct from conventional 3D multiferroic crystals, the 2D vdW assembly and the sliding switching mechanism open poly-opportunities for novel device concepts.

cond-mat.mes-hall

Polarization Saturation in Multi-layered Interfacial Ferroelectrics

Van der Waals (vdW) polytypes of broken inversion and mirror symmetries were recently shown to exhibit switchable electric polarization even at the ultimate two-layer thin limit. Their out-of-plane polarization was found to accumulate in a ladder-like fashion with each successive layer, offering 2D building blocks for the bottom-up construction of 3D ferroelectrics. Here, we demonstrate experimentally that beyond a critical stack thickness, the accumulated polarization in rhombohedral polytypes of molybdenum disulfide (r-MoS2) saturates. The underlying saturation mechanism, deciphered via DFT and self-consistent Poisson-Schrödinger calculations, point to a purely electronic redistribution involving: (1) polarization-induced bandgap closure that allows for cross-stack charge transfer and the emergence of free surface charge; (2) reduction of the polarization saturation value, as well as the critical thickness at which it is obtained, by the presence of free carriers. The resilience of polar layered structures to atomic surface reconstruction, which is essentially unavoidable in polar 3D crystals, potentially allows for the design of new devices with mobile surface charges. Our findings, which are of general nature, should be accounted for when designing switching and/or conductive devices based on ferroelectric layered materials.

cond-mat.mtrl-sci

Spontaneous Electric Polarization in Graphene Polytypes

A crystalline solid is a periodic sequence of identical cells, each containing one or more atoms. If the constituting unit cell is not centrosymmetric, charge may distribute unevenly between the atoms, resulting in internal electric polarization. This effect serves as the basis for numerous ferroelectric, piezoelectric, and pyroelectric phenomena. In nearly all polar materials, including multilayered van der Waals stacks that were recently found to exhibit interfacial polarization, inversion symmetry is broken by having two or more atomic species within the unit cell. Here, we show that even elemental crystals, consisting of one type of atom, and composed of non-polar centrosymmetric layers, exhibit electric polarization if arranged in an appropriate three-dimensional architecture. This concept is demonstrated here for inversion and mirror asymmetric mixed-stacking tetra-layer polytypes of non-polar graphene sheets. Furthermore, we find that the room temperature out-of-plane electric polarization increases with external electrostatic doping, rather than decreases owing to screening. Using first-principles calculations, as well as tight-binding modeling, we unveil the origin of polytype-induced polarization and its dependence on doping. Extension of this idea to graphene multilayers suggests that solely by lateral shifts of constituent monolayers one can obtain multiple meta-stable interlayer stacking sequences that may allow for even larger electrical polarization.

cond-mat.mtrl-sci

Cumulative Polarization Coexisting with Conductivity at Interfacial Ferroelectrics

Ferroelectricity in atomically thin bilayer structures has been recently predicted1 and measured[2-4] in two-dimensional (2D) materials with hexagonal non-centrosymmetric unit-cells. Interestingly, the crystal symmetry translates lateral shifts between parallel 2D layers to a change of sign in their out-of-plane electric polarization, a mechanism referred to as "Slide-Tronics"[4]. These observations, however, have been restricted to switching between only two polarization states under low charge carrier densities[5-12], strongly limiting the practical application of the revealed phenomena[13]. To overcome these issues, one needs to explore the nature of the polarization that arises in multi-layered van der Waals (vdW) stacks, how it is governed by intra- and inter-layer charge redistribution, and to which extent it survives the introduction of mobile charge carriers, all of which are presently unknown14. To explore these questions, we conduct surface potential measurements of parallel WSe2 and MoS2 multi-layers with aligned and anti-aligned configurations of the polar interfaces. We find evenly spaced, nearly decoupled potential steps, indicating highly confined interfacial electric fields, which provide means to design multi-state "ladder ferroelectrics". Furthermore, we find that the internal polarization remains significant upon electrostatic doping of a mobile charge carrier density as high as 1013 cm-2, with substantial in-plane conductivity. Using first-principles calculations based on density functional theory (DFT), we trace the extra charge redistribution in real and momentum space and identify an eventual doping-induced depolarization mechanism.

cond-mat.mtrl-sci

Interfacial Ferroelectricity by van-der-Waals Sliding

Despite their ionic nature, many layered diatomic crystals avoid internal electric polarization by forming a centrosymmetric lattice at their optimal anti-parallel van-der-Waals stacking. Here, we report a stable ferroelectric order emerging at the interface between two naturally-grown flakes of hexagonal-boron-nitride, which are stacked together in a metastable non-centrosymmetric parallel orientation. We observe alternating domains of inverted normal polarization, caused by a lateral shift of one lattice site between the domains. Reversible polarization switching coupled to lateral sliding is achieved by scanning a biased tip above the surface. Our calculations trace the origin of the phenomenon to a subtle interplay between charge redistribution and ionic displacement, and our minimal cohesion model predicts further venues to explore the unique "slidetronics" switching.

cond-mat.mes-hall

Quantum Hall response to time-dependent strain gradients in graphene

Mechanical deformations of graphene induce a term in the Dirac Hamiltonian which is reminiscent of an electromagnetic vector potential. Strain gradients along particular lattice directions induce local pseudomagnetic fields and substantial energy gaps as indeed observed experimentally. Expanding this analogy, we propose to complement the pseudomagnetic field by a pseudoelectric field, generated by a time dependent oscillating stress applied to a graphene ribbon. The joint Hall-like response to these crossed fields results in a strain-induced charge current along the ribbon. We analyze in detail a particular experimental implementation in the (pseudo) quantum Hall regime with weak intervalley scattering. This allows us to predict an (approximately) quantized Hall current which is unaffected by screening due to diffusion currents.

cond-mat.mes-hall

Fluidity Onset in Graphene

Viscous electron fluids have emerged recently as a new paradigm of strongly-correlated electron transport in solids. Here we report on a direct observation of the transition to this long-sought-for state of matter in a high-mobility electron system in graphene. Unexpectedly, the electron flow is found to be interaction-dominated but non-hydrodynamic (quasiballistic) in a wide temperature range, showing signatures of viscous flows only at relatively high temperatures. The transition between the two regimes is characterized by a sharp maximum of negative resistance, probed in proximity to the current injector. The resistance decreases as the system goes deeper into the hydrodynamic regime. In a perfect darkness-before-daybreak manner, the interaction-dominated negative response is strongest at the transition to the quasiballistic regime. Our work provides the first demonstration of how the viscous fluid behavior emerges in an interacting electron system.

cond-mat.mes-hall

Imaging resonant dissipation from individual atomic defects in graphene

Conversion of electric current into heat involves microscopic processes that operate on nanometer length-scales and release minute amounts of power. While central to our understanding of the electrical properties of materials, individual mediators of energy dissipation have so far eluded direct observation. Using scanning nano-thermometry with sub-micro K sensitivity we visualize and control phonon emission from individual atomic defects in graphene. The inferred electron-phonon 'cooling power spectrum' exhibits sharp peaks when the Fermi level comes into resonance with electronic quasi-bound states at such defects, a hitherto uncharted process. Rare in the bulk but abundant at graphene's edges, switchable atomic-scale phonon emitters define the dominant dissipation mechanism. Our work offers new insights for addressing key materials challenges in modern electronics and engineering dissipation at the nanoscale.

cond-mat.mes-hall

Nanoscale thermal imaging of dissipation in quantum systems

Energy dissipation is a fundamental process governing the dynamics of physical, chemical, and biological systems. It is also one of the main characteristics distinguishing quantum and classical phenomena. In condensed matter physics, in particular, scattering mechanisms, loss of quantum information, or breakdown of topological protection are deeply rooted in the intricate details of how and where the dissipation occurs. Despite its vital importance the microscopic behavior of a system is usually not formulated in terms of dissipation because the latter is not a readily measureable quantity on the microscale. Although nanoscale thermometry is gaining much recent interest, the existing thermal imaging methods lack the necessary sensitivity and are unsuitable for low temperature operation required for study of quantum systems. Here we report a superconducting quantum interference nano-thermometer device with sub 50 nm diameter that resides at the apex of a sharp pipette and provides scanning cryogenic thermal sensing with four orders of magnitude improved thermal sensitivity of below 1 μK/Hz1/2. The non-contact non-invasive thermometry allows thermal imaging of very low nanoscale energy dissipation down to the fundamental Landauer limit of 40 fW for continuous readout of a single qubit at 1 GHz at 4.2 K. These advances enable observation of dissipation due to single electron charging of individual quantum dots in carbon nanotubes and reveal a novel dissipation mechanism due to resonant localized states in hBN encapsulated graphene, opening the door to direct imaging of nanoscale dissipation processes in quantum matter.

cond-mat.mes-hall

Anomalous response to gate voltage application in mesoscopic LaAlO_3/SrTiO_3 devices

We report on resistivity and Hall measurements performed on a series of narrow mesa devices fabricated from LaAlO_3/SrTiO_3 single interface heterostructure with a bridge width range of 1.5-10 microns. Upon applying back-gate voltage of the order of a few Volts, a strong increase in the sample resistance (up to factor of 35) is observed, suggesting a relatively large capacitance between the Hall-bar and the gate. The high value of this capacitance is due to the device geometry, and can be explained within an electrostatic model using the Thomas Fermi approximation. The Hall coefficient is sometimes a non-monotonic function of the gate voltage. This behavior is inconsistent with a single conduction band model. We show that a theoretical two-band model is consistent with this transport behavior, and indicates a metal to insulator transition in at least one of these bands.

cond-mat.mes-hall