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Antony George

Publications and source records attributed to Antony George.

At least 19 recordsLinked to original sources

Tuning proximity-induced spin-orbit coupling in graphene/WSe$_{2}$ heterostructures

Recently, proximity-induced spin-orbit coupling (SOC) has been observed in heterostructures consisting of monolayer graphene (ML-G) and transition metal dichalcogenides (TMDCs) such as WSe$_{2}$. Successful tuning of SOC in graphene/WSe$_{2}$ heterostructures by applying mechanical pressure and electric fields was also demonstrated in previous studies. In addition, theoretical calculations predicted a strong dependence of the proximity-induced SOC on the twist angle between graphene and TMDC. Here, we put these predictions to experimental test in ML-G/ML-WSe$_{2}$/hBN-heterostructures, where the twist angle is determined by aligning fractured edges, and by crystallographic etching of graphene. By performing weak anti-localization measurements, we determine the strength of the Rasbha-type SOC ($λ_\mathrm{R}$) and the valley-Zeeman-type SOC ($λ_\mathrm{VZ}$). Our experiments confirm a strong twist angle dependence of the proximity-induced SOC in agreement with theoretical predictions. Finally, we demonstrate the tunability of the SOC strength via mechanical pressure, which is in agreement with earlier findings.

cond-mat.mes-hall

Optimized near-field optical response via adaptive tip illumination

The performance of tip-enhanced optical microscopy is often limited by inefficient coupling of the excitation field to the plasmonic tip apex, as well as by thermal drift and optical aberrations. Here, we demonstrate that adaptive wavefront shaping based on Zernike mode provides a practical approach to achieving robust near-field optimisation at the tip apex. Using a sequential feedback algorithm, initially using the near-field signal, we narrow the illumination point-spread function and suppress sidelobes. This demonstrates that Zernike-mode control can be used for both aberration correction and field engineering. In tip-enhanced Raman measurements of a Janus MoSSe monolayer, conventional near-field optimisation increases the signal intensity by around 1.4 fold. A second optimisation step based directly on the Raman-band intensity yields a further 5 to 15 fold enhancement, depending on the specific tips used. These results establish a systematic, optics-based strategy for optimising tip fields, providing a transferable framework for improving tip-enhanced and related near-field spectroscopies.

physics.optics

Enhancement of the WS$_2$ A$_{1\text{g}}$ Raman Mode in MoS$_2$/WS$_2$ Heterostructures

When combined into van der Waals heterostructures, transition metal dichalcogenide monolayers enable the exploration of novel physics beyond their unique individual properties. However, for interesting phenomena such as interlayer charge transfer and interlayer excitons to occur, precise control of the interface and ensuring high-quality interlayer contact is crucial. Here, we investigate bilayer heterostructures fabricated by combining chemical-vapor-deposition-grown MoS$_2$ and exfoliated WS$_2$ monolayers, allowing us to form several heterostructures with various twist angles within one preparation step. In case of sufficiently good interfacial contact, evaluated by photoluminescence quenching, we observe a twist-angle-dependent enhancement of the WS$_2$ A$_{1g}$ Raman mode. In contrast, other WS$_2$ and MoS$_2$ Raman modes (in particular, the MoS$_2$ A$_{1g}$ mode) do not show a clear enhancement under the same experimental conditions. We present a systematic study of this mode-selective effect using nonresonant Raman measurements that are complemented with ab-initio calculations of Raman spectra. We find that the selective enhancement of the WS$_2$ A$_{1g}$ mode exhibits a strong dependence on interlayer distance. We show that this selectivity is related to the A$_{1g}$ eigenvectors in the heterolayer: the eigenvectors are predominantly localized on one of the two layers; yet, the intensity of the MoS$_2$ mode is attenuated because the WS$_2$ layer is vibrating (albeit with much lower amplitude) out of phase, while the WS$_2$ mode is amplified because the atoms on the MoS$_2$ layer are vibrating in phase. To separate this eigenmode effect from resonant Raman enhancement, our study is extended with near-resonant Raman measurements.

cond-mat.mes-hall

Valley-dependent emission patterns enabled by plasmonic nanoantennas

Selective control over the emission pattern of valley-polarized excitons in monolayer transition metal dichalcogenides is crucial for developing novel valleytronic, quantum information, and optoelectronic devices. While significant progress has been made in directionally routing photoluminescence from these materials, key challenges remain: notably, how to link routing effects to the degree of valley polarization, and how to distinguish genuine valley-dependent routing from spin-momentum coupling - an optical phenomenon related to electromagnetic scattering but not the light source itself. In this study, we address these challenges by experimentally and numerically establishing a direct relationship between the intrinsic valley polarization of the emitters and the farfield emission pattern, enabling an accurate assessment of valley-selective emission routing. We report valley-selective manipulation of the angular emission pattern of monolayer tungsten diselenide mediated by gold nanobar dimer antennas at cryogenic temperature. Experimentally, we study changes in the system's emission pattern for different circular polarization states of the excitation, demonstrating a valley-selective circular dichroism in photoluminescence of 6%. These experimental findings are supported by a novel numerical approach based on the principle of reciprocity, which allows modeling valley-selective emission in periodic systems. We further show numerically, that these valley-selective directional effects are a symmetry-protected property of the nanoantenna array owing to its extrinsic chirality for oblique emission angles, and can significantly be enhanced when tailoring the distribution of emitters. This renders our nanoantenna-based system a robust platform for valleytronic processing.

physics.optics

Role of Coherence in Polarization Response of Hybrid Monolayer MoS$_2$-Gold Nanoparticle Systems

Monolayers of transition metal dichacogenides show strong second-order nonlinearity and symmetry-driven selection rules from their three-fold lattice symmetry. This process resembles the valley-contrasting selection rules for photoluminescence in these materials. However, the underlying physical mechanisms fundamentally differ since second harmonic generation is a coherent process, whereas photoluminescence is incoherent, leading to distinct interactions with photonic nanoresonators. In this study, we investigate the far-field circular polarization properties of second harmonic generation from MoS$_2$ monolayers resonantly interacting with spherical gold nanoparticles. Our results indicate that the coherence of the second harmonic allows its polarization to be mostly preserved, unlike in an incoherent process, where the polarization is scrambled. These findings provide important insights for future applications in valleytronics and quantum nanooptics, where both coherent and incoherent processes can be probed in such hybrid systems without altering sample geometry or operational wavelength.

physics.optics

Photoluminescence-Based Gas Sensing with MoS2 Monolayers

Two-dimensional transition metal dichalcogenides (TMDs) are highly appealing for gas sensors, lab-on-a-chip devices and bio-sensing applications because of their strong light-matter interaction and high surface-to-volume ratio. The ability to grow these van der Waals materials on different substrates and waveguide geometries opens a horizon toward scalable on-chip photonic nanodevices. Here, we report on a versatile technique for real time remote optical gas sensing using two-dimensional TMDs. The adsorption of the gas molecules on the monolayer surface provides a gateway for gas sensing based on charge-transfer-induced photoluminescence variation. For gases that are weakly adsorbed on the surface of monolayer TMDs, purging the monolayers' surface by an inert gas like N2 can desorb gases from the monolayers at room temperature. We demonstrate CO, NO and NO2 detection by monitoring photoluminescence from semiconducting MoS2 monolayers grown on SiO2/Si chips at a level of 10 ppm with fast response time. Observations are supported by our density functional theory calculations, which predict a significant interaction between these gases and MoS2 monolayers. These findings may lead to advances in remote sensing, surface-sensitive bioanalytics and lab-on-a-chip sensors.

physics.app-ph

Influence of resonant plasmonic nanoparticles on optically accessing the valley degree of freedom in 2D semiconductors

The valley degree of freedom is one of the most intriguing properties of atomically thin transition metal dichalcogenides. Together with the possibility to address this degree of freedom by valley-contrasting optical selection rules, it has the potential to enable a completely new class of future electronic and optoelectronic devices. Resonant optical nanostructures emerge as promising tools for interacting with and controlling the valley degree of freedom at the nanoscale. However, a critical understanding gap remains in how nanostructures and their nearfields affect the circular polarization properties of valley-selective emission hindering further developments in this field. In order to address this issue, our study delves into the experimental investigation of a hybrid model system where valley-specific emission from a monolayer of molybdenum disulfide is interacting with a resonant plasmonic nanosphere. Contrary to the simple intuition suggesting that a centrosymmetric nanoresonator preserves the degree of circular polarization in the forward scattered farfield by angular momentum conservation, our cryogenic photoluminescence microscopy reveals that the light emitted from the nanoparticle position is largely unpolarized, i.e. we observe depolarization. We rigorously study the nature of this phenomenon numerically considering the monolayer-nanoparticle interaction at different levels including excitation and emission. In doing so, we find that the farfield degree of polarization strongly reduces in the hybrid system when including excitons emitting from outside of the system's symmetry point, which in combination with depolarisation at the excitation level causes the observed effect. Our results highlight the importance of considering spatially distributed emitters for precise predictions of polarization responses in these hybrid systems.

physics.optics

Kapitza-resistance-like exciton dynamics in atomically flat MoSe$_{2}$-WSe$_{2}$ lateral heterojunction

Being able to control the neutral excitonic flux is a mandatory step for the development of future room-temperature two-dimensional excitonic devices. Semiconducting Monolayer Transition Metal Dichalcogenides (TMD-ML) with extremely robust and mobile excitons are highly attractive in this regard. However, generating an efficient and controlled exciton transport over long distances is a very challenging task. Here we demonstrate that an atomically sharp TMD-ML lateral heterostructure (MoSe$_{2}$-WSe$_{2}$) transforms the isotropic exciton diffusion into a unidirectional excitonic flow through the junction. Using tip-enhanced photoluminescence spectroscopy (TEPL) and a modified exciton transfer model, we show a discontinuity of the exciton density distribution on each side of the interface. We introduce the concept of exciton Kapitza resistance, by analogy with the interfacial thermal resistance referred to as Kapitza resistance. By comparing different heterostructures with or without top hexagonal boron nitride (hBN) layer, we deduce that the transport properties can be controlled, over distances far greater than the junction width, by the exciton density through near-field engineering and/or laser power density. This work provides a new approach for controlling the neutral exciton flow, which is key toward the conception of excitonic devices.

cond-mat.mes-hall

Interface engineering of charge-transfer excitons in 2D lateral heterostructures

The existence of bound charge transfer (CT) excitons at the interface of monolayer lateral heterojunctions has been debated in literature, but contrary to the case of interlayer excitons in vertical heterostructure their observation still has to be confirmed. Here, we present a microscopic study investigating signatures of bound CT excitons in photoluminescence spectra at the interface of hBN-encapsulated lateral MoSe$_2$-WSe$_2$ heterostructures. Based on a fully microscopic and material-specific theory, we reveal the many-particle processes behind the formation of CT excitons and how they can be tuned via interface- and dielectric engineering. For junction widths smaller than the Coulomb-induced Bohr radius we predict the appearance of a low-energy CT exciton. The theoretical prediction is compared with experimental low-temperature photoluminescence measurements showing emission in the bound CT excitons energy range. Our joint theory-experiment study presents a significant step towards a microscopic understanding of optical properties of technologically promising 2D lateral heterostructures.

cond-mat.mes-hall

Direct Growth of Monolayer MoS$_2$ on Nanostructured Silicon Waveguides

We report for the first time the direct growth of Molybdenum disulfide (MoS$_2$) monolayers on nanostructured silicon-on-insulator waveguides. Our results indicate the possibility of utilizing the Chemical Vapour Deposition (CVD) on nanostructured photonic devices in a scalable process. Direct growth of 2D material on nanostructures rectifies many drawbacks of the transfer-based approaches. We show that the van der Waals materials grow conformally across the curves, edges, and the silicon-SiO$_2$ interface of the waveguide structure. Here, the waveguide structure used as a growth substrate is complex not just in terms of its geometry but also due to the two materials (Si and SiO$_2$) involved. A transfer-free method like this yields a novel approach for functionalizing nanostructured, integrated optical architectures with an optically active direct semiconductor.

physics.app-ph

Tuning nanowire lasers via hybridization with two-dimensional materials

Mixed dimensional hybrid structures have recently gained increasing attention as promising building blocks for novel electronic and optoelectronic devices. In this context, hybridization of semiconductor nanowires with two-dimensional materials could offer new ways to control and modulate lasing at the nanoscale. In this work, we deterministically fabricate hybrid mixed-dimensional heterostructures composed of ZnO nanowires and MoS2 monolayers with micrometer control over their relative position. First, we show that our deterministic fabrication method does not degrade the optical properties of the ZnO nanowires. Second, we demonstrate that the lasing wavelength of ZnO nanowires can be tuned by several nanometers by hybridization with CVD-grown MoS2 monolayers. We assign this spectral shift of the lasing modes to an efficient carrier transfer at the heterointerface and the subsequent increase of the optical band gap in ZnO (Moss-Burstein effect).

physics.optics

One pot chemical vapor deposition of high optical quality large area monolayer Janus transition metal dichalcogenides

We report one-pot chemical vapor deposition (CVD) growth of large-area Janus SeMoS monolayers, with the asymmetric top (Se) and bottom (S) chalcogen atomic planes with respect to the central transition metal (Mo) atoms. The formation of these two-dimensional semiconductor monolayers takes place upon the thermodynamic equilibrium-driven exchange of the bottom Se atoms of the initially grown MoSe2 single crystals on gold foils with S atoms. The growth process is characterized by complementary experimental techniques including Raman and X-ray photoelectron spectroscopy and the growth mechanisms are rationalized by first principle calculations. The remarkably high optical quality of the synthesized Janus monolayers is demonstrated by optical and magneto-optical measurements which reveal the strong exciton-phonon coupling and enable to obtain the exciton g-factor of -3.3.

cond-mat.mtrl-sci

Exciton spectroscopy and diffusion in MoSe2-WSe2 lateral heterostructures encapsulated in hexagonal boron nitride

Chemical vapor deposition (CVD) allows lateral edge epitaxy of transition metal dichalcogenide heterostructures with potential applications in optoelectronics. Critical for carrier and exciton transport is the quality of the two materials that constitute the monolayer and the nature of the lateral heterojunction. Important details of the optical properties were inaccessible in as-grown heterostructure samples due to large inhomogeneous broadening of the optical transitions. Here we perform optical spectroscopy at T = 4 K and also at 300 K to access the optical transitions in CVD grown MoSe2-WSe2 lateral heterostructures that are transferred from the growth-substrate and are encapsulated in hBN. Photoluminescence (PL), reflectance contrast and Raman spectroscopy reveal considerably narrowed optical transition linewidth similar to high quality exfoliated monolayers. In high-resolution transmission electron microscopy (HRTEM) we find near-atomically sharp junctions with a typical extent of 3nm for the covalently bonded MoSe2-WSe2. In PL imaging experiments we find effective excitonic diffusion length that are longer for WSe2 than for MoSe2 at low T=4 K, whereas at 300 K this trend is reversed.

cond-mat.mtrl-sci

Signatures of multi-band effects in high-harmonic generation in monolayer MoS$_2$

High-harmonic generation (HHG) in solids has been touted as a way to probe ultrafast dynamics and crystal symmetries in condensed matter systems. Here, we investigate the polarization properties of high-order harmonics generated in monolayer MoS$_2$, as a function of crystal orientation relative to the mid-infrared laser field polarization. At several different laser wavelengths we experimentally observe a prominent angular shift of the parallel-polarized odd harmonics for energies above approximately 3.5 eV, and our calculations indicate that this shift originates in subtle differences in the recombination dipole strengths involving multiple conduction bands. This observation is material specific and is in addition to the angular dependence imposed by the dynamical symmetry properties of the crystal interacting with the laser field, and may pave the way for probing the vectorial character of multi-band recombination dipoles.

cond-mat.mtrl-sci

All-optical polarization and amplitude modulation of second-harmonic generation in atomically thin semiconductors

Second-harmonic generation is of paramount importance in several fields of science and technology, including frequency conversion, self-referencing of frequency combs, nonlinear spectroscopy and pulse characterization. Advanced functionalities are enabled by modulation of the harmonic generation efficiency, which can be achieved with electrical or all-optical triggers. Electrical control of the harmonic generation efficiency offers large modulation depth at the cost of low switching speed, by contrast to all-optical nonlinear devices, which provide high speed and low modulation depth. Here we demonstrate all-optical modulation of second-harmonic generation in MoS2 with a modulation depth of close to 100% and speed limited only by the fundamental pulse duration. This result arises from a combination of D3h crystal symmetry and the deep subwavelength thickness of the sample, it can therefore be extended to the whole family of transition metal dichalcogenides to provide great flexibility in the design of advanced nonlinear optical devices such as high-speed integrated frequency converters, broadband autocorrelators for ultrashort pulse characterization, and tunable nanoscale holograms.

physics.optics

Tuning exciton recombination rates in doped transition metaldichalcogenides

Monolayer transition metal dichalcogenides (TMDs) are direct gap semiconductors that hold great promise for advanced applications in photonics and optoelectronics. Understanding the interplay between their radiative and non-radiative recombination pathways is thus of crucial importance not only for fundamental studies but also for the design of future nanoscale on-chip devices. Here, we investigate the interplay between doping and exciton-exciton annihilation (EEA) and their impact on the photoluminescence quantum yield in different TMD samples and related heterostructures. We demonstrate that the EEA threshold increases in highly doped samples, where the radiative and non-radiative recombination of trions dominates.

cond-mat.mes-hall

In-fiber second-harmonic generation with embedded two-dimensional materials

Silica-based optical fibers are a workhorse of nonlinear optics. They have been used to demonstrate nonlinear phenomena such as solitons and self-phase modulation. Since the introduction of the photonic crystal fiber, they have found many exciting applications, such as supercontinuum white light sources and third-harmonic generation, among others. They stand out by their low loss, large interaction length, and the ability to engineer its dispersive properties, which compensate for the small chi(3) nonlinear coefficient. However, they have one fundamental limitation: due to the amorphous nature of silica, they do not exhibit second-order nonlinearity, except for minor contributions from surfaces. Here, we demonstrate significant second-harmonic generation in functionalized optical fibers with a monolayer of highly nonlinear MoS2 deposited on the fiber guiding core. The demonstration is carried out in a 3.5 mm short piece of exposed core fiber, which was functionalized in a scalable process CVD-based process, without a manual transfer step. This approach is scalable and can be generalized to other transition metal dichalcogenides and other waveguide systems. We achieve an enhancement of more than 1000x over a reference sample of equal length. Our simple proof-of-principle demonstration does not rely on either phase matching to fundamental modes, or ordered growth of monolayer crystals, suggesting that pathways for further improvement are within reach. Our results do not just demonstrate a new path towards efficient in-fiber SHG-sources, instead, they establish a platform with a new route to chi(2)-based nonlinear fiber optics, optoelectronics, and photonics platforms, integrated optical architectures, and active fiber networks.

physics.optics

Scalable functionalization of optical fibers using atomically thin semiconductors

Atomically thin transition metal dichalcogenides are highly promising for integrated optoelectronic and photonic systems due to their exciton-driven linear and nonlinear interaction with light. Integrating them into optical fibers yields novel opportunities in optical communication, remote sensing, and all-fiber optoelectronics. However, scalable and reproducible deposition of high quality monolayers on optical fibers is a challenge. Here, we report the chemical vapor deposition of monolayer MoS2 and WS2 crystals on the core of microstructured exposed core optical fibers and their interaction with the fibers' guided modes. We demonstrate two distinct application possibilities of 2D-functionalized waveguides to exemplify their potential. First, we simultaneously excite and collect excitonic 2D material photoluminescence with the fiber modes, opening a novel route to remote sensing. Then we show that third harmonic generation is modified by the highly localized nonlinear polarization of the monolayers, yielding a new avenue to tailor nonlinear optical processes in fibers. We anticipate that our results may lead to significant advances in optical fiber based technologies.

physics.app-ph