Scalable single-photon sources in atomically thin MoS2
Julian Klein, Lukas Sigl, Samuel Gyger, Katja Barthelmi, Matthias Florian, Sergio Rey, Takashi Taniguchi, Kenji Watanabe, Frank Jahnke, Christoph Kastl, Val Zwi… 展开作者
Julian Klein, Lukas Sigl, Samuel Gyger, Katja Barthelmi, Matthias Florian, Sergio Rey, Takashi Taniguchi, Kenji Watanabe, Frank Jahnke, Christoph Kastl, Val Zwiller, Klaus D. Jöns, Kai Müller, Ursula Wurstbauer, Jonathan J. Finley, Alexander W. Holleitner
Real-world quantum applications, eg. on-chip quantum networks and quantum cryptography, necessitate large scale integrated single-photon sources with nanoscale footprint for modern information technology. While on-demand and high fidelity implantation of atomic scale single-photon sources in conventional 3D materials suffer from uncertainties due to the crystals dimensionality, layered 2D materials can host point-like centers with inherent confinement to a sub-nm plane. However, previous attempts to truly deterministically control spatial position and spectral homogeneity while maintaining the 2D character have not been realized. Here, we demonstrate the on-demand creation and precise positioning of single-photon sources in atomically thin MoS2 with very narrow ensemble broadening and near-unity fabrication yield. Focused ion beam irradiation creates 100s to 1000s of mono-typical atomistic defects with anti-bunched emission lines with sub-10 nm lateral and 0.7 nm axial positioning accuracy. Our results firmly establish 2D materials as a scalable platform for single-photon emitters with unprecedented control of position as well as photophysical properties owing to the all-interfacial nature.
Transient currents in atomically thin MoTe$_2$ field-effect transistor are measured during cycles of pulses through the gate electrode. The transients are analyzed in light of a newly proposed model for charge trapping dynamics that renders a time-dependent change in threshold voltage the dominant effect on the channel hysteretic behavior over emission currents from the charge traps. The proposed model is expected to be instrumental in understanding the fundamental physics that governs the performance of atomically thin FETs and is applicable to the entire class of atomically thin-based device…
Deposition of clean and defect-free atomically thin two-dimensional crystalline flakes on surfaces by mechanical exfoliation of layered bulk materials has proven to be a powerful technique, but it requires a fast, reliable and non-destructive way to identify the atomically thin flakes among a crowd of thick flakes. In this work, we provide general guidelines to identify ultrathin flakes of TaSe2 by means of optical microscopy and Raman spectroscopy. Additionally, we determine the optimal substrates to facilitate the optical identification of atomically thin TaSe2 crystals. Experimental realiza…
We report the implementation of energy dispersive X-ray spectroscopy for layered semiconductors in the form of atomically thin transition metal dichalcogenides. The technique is based on a scanning electron microscope equipped with a silicon drift detector for energy dispersive X-ray analysis. By optimizing operational parameters in numerical simulations and experiments, we achieve layer-resolving sensitivity for few-layer crystals down to the monolayer limit and demonstrate elemental composition profiling in vertical and lateral heterobilayers of transition metal dichalcogenides. The techniqu…
Atomically-thin molybdenum disulfide is emerging as a new nanomaterial with potential applications in the fields of electronic and photonics. Charge carrier dynamics plays an essential role in determining its electronic and optical properties. We report spatially and temporally resolved pump-probe studies of charge carriers in atomically-thin molybdenum disulfide samples fabricated by mechanical exfoliation. Carriers are injected by interband absorption of a 390-nm pump pulse and detected by measuring differential reflection of a time-delayed and spatially-scanned probe pulse that is tuned to …
We report a naturally-occurring two-dimensional material (graphene that can be viewed as a gigantic flat fullerene molecule, describe its electronic properties and demonstrate all-metallic field-effect transistor, which uniquely exhibits ballistic transport at submicron distances even at room temperature.
Based on first-principles calculations and symmetry analysis, we predict atomically thin ($1-N$ layers) 2H group-VIB TMDs $MX_2$ ($M$ = Mo, W; $X$ = S, Se, Te) are large-gap higher-order topological crystalline insulators protected by $C_3$ rotation symmetry. We explicitly demonstrate the nontrivial topological indices and existence of the hallmark corner states with quantized fractional charge for these familiar TMDs with large bulk optical band gaps ($1.64-1.95$ eV for the monolayers), which would facilitate the experimental detection by STM. We find that the well-defined corner states exist…
Clays and micas are receiving attention as materials that, in their atomically thin form, could allow for novel proton conductive, ion selective, osmotic power generation, or solvent filtration membranes. The interest arises from the possibility of controlling their properties by exchanging ions in the crystal lattice. However, the ion exchange process itself remains largely unexplored in atomically thin materials. Here we use atomic-resolution scanning transmission electron microscopy to study the dynamics of the process and reveal the binding sites of individual ions in atomically thin and a…
Atomically thin MoS$_{2}$ crystals have been recognized as a quasi-2D semiconductor with remarkable physics properties. This letter reports our Raman scattering measurements on multilayer and monolayer MoS$_{2}$, especially in the low-frequency range ($<$50 cm$^{-1}$). We find two low-frequency Raman modes with contrasting thickness dependence. With increasing the number of MoS$_{2}$ layers, one shows a significant increase in frequency while the other decreases following a 1/N (N denotes layer-number) trend. With the aid of first-principle calculations we assign the former as the shear mode $…
Two-dimensional (2D) semimetals beyond graphene have been relatively unexplored in the atomically-thin limit. Here we introduce a facile growth mechanism for semimetallic WTe2 crystals, then fabricate few-layer test structures while carefully avoiding degradation from exposure to air. Low-field electrical measurements of 80 nm to 2 um long devices allow us to separate intrinsic and contact resistance, revealing metallic response in the thinnest encapsulated and stable WTe2 devices studied to date (3 to 20 layers thick). High-field electrical measurements and electro-thermal modeling demonstrat…
We show that it is possible to deposit, by mechanical exfoliation on SiO2/Si wafers, atomically thin mica flakes down to a single monolayer thickness. The optical contrast of these mica flakes on top of a SiO2/Si substrate, which depends on their thickness, the illumination wavelength and the SiO2 substrate thickness, can be quantitatively accounted for by a Fresnel law based model. The preparation of atomically thin insulating crystalline sheets will enable the fabrication of ultrathin defect-free insulating substrates, dielectric barriers or planar electron tunneling junctions. Additionally,…
Nanopores in 2D materials are highly desirable for DNA sequencing, yet achieving single-stranded DNA (ssDNA) transport through them is challenging. Using density functional theory calculations and molecular dynamics simulations we show that ssDNA transport through a pore in monolayer hexagonal boron nitride (hBN) is marked by a basic nanomechanical conflict. It arises from the notably inhomogeneous flexural rigidity of ssDNA and causes high friction $\textit{via}$ transient DNA desorption costs exacerbated by solvation effects. For a similarly sized pore in bilayer hBN, its self-passivated ato…
Resolving the momentum degree of freedom of excitons - electron-hole pairs bound by the Coulomb attraction in a photoexcited semiconductor, has remained a largely elusive goal for decades. In atomically thin semiconductors, such a capability could probe the momentum forbidden dark excitons, which critically impact proposed opto-electronic technologies, but are not directly accessible via optical techniques. Here, we probe the momentum-state of excitons in a WSe2 monolayer by photoemitting their constituent electrons, and resolving them in time, momentum and energy. We obtain a direct visual of…
Van der Waals junctions of two-dimensional materials with an atomically sharp interface open up unprecedented opportunities to design and study functional heterostructures. Semiconducting transition metal dichalcogenides have shown tremendous potential for future applications due to their unique electronic properties and strong light-matter interaction. However, many important optoelectronic applications, such as broadband photodetection, are severely hindered by their limited spectral range and reduced light absorption. Here, we present a p-g-n heterostructure formed by sandwiching graphene w…
The emergence of two-dimensional crystals has revolutionized modern solid-state physics. From a fundamental point of view, the enhancement of charge carrier correlations has sparked enormous research activities in the transport- and quantum optics communities. One of the most intriguing effects, in this regard, is the bosonic condensation and spontaneous coherence of many-particle complexes. Here, we find compelling evidence of bosonic condensation of exciton-polaritons emerging from an atomically thin crystal of MoSe2 embedded in a dielectric microcavity under optical pumping. The formation o…
We report on graphene-like exfoliation of the large-area crystalline films and ribbons of bismuth telluride with the thicknesses of a few atoms. It is demonstrated that bismuth telluride, the most important material for thermoelectric industry, can be mechanically separated into its building blocks -[Te-Bi-Te-Bi-Te]- atomic five-folds with the thickness of ~1 nm and even further - to subunits with smaller thicknesses. The atomically-thin crystals can be structured into suspended crystalline ribbons providing quantum confinement in two dimensions. The quasi two-dimensional (2-D) crystals of bis…
Atomically thin layers of transition metal dichalcogenides (TMDCs) exhibit exceptionally strong Coulomb interaction between charge carriers due to the two-dimensional carrier confinement in connection with weak dielectric screening. The van der Waals nature of interlayer coupling makes it easy to integrate TMDC layers into heterostructures with different dielectric or metallic substrates. This allows to tailor electronic and optical properties of these materials, as Coulomb interaction inside atomically thin layers is very susceptible to screening by the environment. Here we theoretically inve…
With the decrease of the dimensions of electronic devices, the role played by electrical contacts is ever increasing, eventually coming to dominate the overall device volume and total resistance. This is especially problematic for monolayers of semiconducting transition metal dichalcogenides (TMDs), which are promising candidates for atomically thin electronics. Ideal electrical contacts to them would require the use of similarly thin electrode materials while maintaining low contact resistances. Here we report a scalable method to fabricate ohmic graphene edge contacts to two representative m…
As a 2D ferromagnetic semiconductor with magnetic ordering, atomically thin chromium triiodide is the latest addition to the family of two-dimensional (2D) materials. However, realistic exploration of CrI3-based devices and heterostructures is challenging, due to its extreme instability under ambient conditions. Here we present Raman characterization of CrI3, and demonstrate that the main degradation pathway of CrI3 is the photocatalytic substitution of iodine by water. While simple encapsulation by Al2O3, PMMA and hexagonal BN (hBN) only leads to modest reduction in degradation rate, minimizi…
Atomically thin semiconductors have dimensions that are commensurate with critical feature sizes of future optoelectronic devices defined using electron/ion beam lithography. Robustness of their emergent optical and valleytronic properties is essential for typical exposure doses used during fabrication. Here, we explore how focused helium ion bombardment affects the intrinsic vibrational, luminescence and valleytronic properties of atomically thin MoS$_{2}$. By probing the disorder dependent vibrational response we deduce the interdefect distance by applying a phonon confinement model. We show…
Atomically thin two-dimensional chalcogenides such as MoS2 monolayers are structurally ideal channel materials for the ultimate atomic electronics. However, a heavy thickness dependence of electrical performance is shown in these ultrathin materials, and the device performance normally degrades while exhibiting a low carrier mobility as compared with corresponding bulks, constituting a main hurdle for application in electronics. In this brief review, we summarize our recent work on electrode/channel contacts and carrier scattering mechanisms to address the origins of this adverse thickness dep…
The metal-insulator transition (MIT) is one of the remarkable electrical transport properties of atomically thin molybdenum disulphide (MoS2). Although the theory of electron-electron interactions has been used in modeling the MIT phenomena in MoS2, the underlying mechanism and detailed MIT process still remain largely unexplored. Here, we demonstrate that the vertical metal-insulator-semiconductor (MIS) heterostructures built from atomically thin MoS2 (monolayers and multilayers) are ideal capacitor structures for probing the electron states in MoS2. The vertical configuration of MIS heterost…
Current-induced domain wall (DW) motion has drawn great attention in the last decades as the key operational principle of emerging magnetic memory devices. As the major driving force of the current-induced DW motion, the spin-orbit torque (SOT) on chiral DWs has been proposed and extensively studied nowadays. However, we demonstrate here that there exists another driving force, which is larger than the SOT in ultra-thin Co films. Moreover, the direction of the present force is found to be opposite to the prediction of the spin-transfer torque (STT), resulting in the DW motion along the current…
Boosting the sensitivity of solid-state gas sensors by incorporating nanostructured materials as the active sensing element can be complicated by interfacial effects. Interfaces at nanoparticles, grains, or contacts may result in non-linear current-voltage response, high electrical resistance, and ultimately, electric noise that limits the sensor read-out. Here we report the possibility to prepare nominally one atom thin, electrically continuous metals, by straightforward physical vapor deposition on the carbon zero-layer grown epitaxially on silicon carbide. With platinum as the metal, its el…
As hosts for tightly-bound electron-hole pairs carrying quantized angular momentum, atomically-thin semiconductors of transition metal dichalcogenides provide an appealing platform for optically addressing the valley degree of freedom. In particular, the valleytronic properties of neutral and charged excitons in these systems have been widely investigated. Meanwhile, correlated quantum states involving more particles are so far elusive and controversial. Here we present experimental evidence for valleytronic four-particle biexcitons and five-particle exciton-trions in high-quality monolayer tu…
We introduce a computational database with calculated structural, thermodynamic, electronic, magnetic, and optical properties of 820 one-dimensional materials. The materials are systematically selected and exfoliated from experimental databases of crystal structures based on a dimensionality scoring parameter. The database is furthermore expanded by chemical element substitution in the materials. The materials are investigated in both their bulk form and as isolated one-dimensional components. We discuss the methodology behind the database, give an overview of some of the calculated properties…
Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. …
Tuning the electronic properties of a material by subjecting it to strain constitutes an important strategy to enhance the performance of semiconducting electronic devices. Using local strain, confinement potentials for excitons can be engineered, with exciting possibilities for trapping excitons for quantum optics and for efficient collection of solar energy. Two-dimensional materials are able to withstand large strains before rupture, offering a unique opportunity to introduce large local strains. Here, we study atomically thin MoS2 layers with large local strains of up to 2.5% induced by co…
In monolayers of transition metal dichalcogenides the nonlocal nature of the effective dielectric screening leads to large binding energies of excitons. Additional lateral confinement gives rise to exciton localization in quantum dots. By assuming parabolic confinement for both the electron and the hole, we derive model wave functions for the relative and the center-of-mass motions of electron-hole pairs, and investigate theoretically resonant energy transfer among excitons localized in two neighboring quantum dots. We quantify the probability of energy transfer for a direct-gap transition by …
The electronic properties of ultrathin crystals of molybdenum disulfide consisting of N = 1, 2, ... 6 S-Mo-S monolayers have been investigated by optical spectroscopy. Through characterization by absorption, photoluminescence, and photoconductivity spectroscopy, we trace the effect of quantum confinement on the material's electronic structure. With decreasing thickness, the indirect band gap, which lies below the direct gap in the bulk material, shifts upwards in energy by more than 0.6 eV. This leads to a crossover to a direct-gap material in the limit of the single monolayer. Unlike the bulk…
In order to deepen in the knowledge of the vibrational properties of 2-dimensional MoS2 atomic layers, a complete and systematic Raman scattering analysis has been performed using both bulk single crystal MoS2 samples and atomically thin MoS2 layers. Raman spectra have been measured under non-resonant and resonant conditions using seven different excitation wavelengths from near-infrared (NIR) to ultraviolet (UV). These measurements have allowed to observe and identify 41 peaks, among which 22 have not been previously experimentally observed for this compound, characterizing the existence of d…
The aim of this work is to study the electrostatic screening by single and few-layer MoS2 sheets by means of electrostatic force microscopy in combination with a non-linear Thomas-Fermi Theory to interpret the experimental results. We find that a continuum model of decoupled layers, which satisfactorily reproduces the electrostatic screening for graphene and graphite, cannot account for the experimental observations. A three-dimensional model with an interlayer hopping parameter can on the other hand successfully account for the observed electric field screening by MoS2 nanolayers, pointing ou…
This paper reports the synthesis and detailed characterization of graphite thin films produced by thermal decomposition of the (0001) face of a 6H-SiC wafer, demonstrating the successful growth of single crystalline films down to approximately one graphene layer. The growth and characterization were carried out in ultrahigh vacuum (UHV) conditions. The growth process and sample quality were monitored by low-energy electron diffraction, and the thickness of the sample was determined by core level x-ray photoelectron spectroscopy. High-resolution angle-resolved photoemission spectroscopy shows c…
Two-dimensional dilute magnetic semiconductors can provide fundamental insights in the very nature of magnetic orders and their manipulation through electron and hole doping. Despite the fundamental physics, due to the large charge density control capability in these materials, they can be extremely important in spintronics applications such as spin valve and spin-based transistors. In this article, we studied a two-dimensional dilute magnetic semiconductors consisting of phosphorene monolayer doped with cobalt atoms in substitutional and interstitial defects. We show that these defects can be…
We demonstrate a new approach for dynamically manipulating the optical response of an atomically thin semiconductor, a monolayer of MoSe2, by suspending it over a metallic mirror. First, we show that suspended van der Waals heterostructures incorporating a MoSe2 monolayer host spatially homogeneous, lifetime-broadened excitons. Then, we interface this nearly ideal excitonic system with a metallic mirror and demonstrate control over the exciton-photon coupling. Specifically, by electromechanically changing the distance between the heterostructure and the mirror, thereby changing the local photo…
We study the thermal effects on the frictional properties of atomically thin sheets. We simulate a simple model based on the Prandtl-Tomlinson model that reproduces the layer dependence of friction and strengthening effects seen in AFM experiments. We investigate sliding at constant speed as well as reversing direction. We also investigate contact aging: the changes that occur to the contact when the sliding stops completely. We compare the numerical results to analytical calculations based on Kramers rates. We find that there is a slower than exponential contact aging that weakens the contact…
The discovery of graphene some ten years ago was the first proof of a free-standing two-dimensional (2D) solid phase. Here, using quantum molecular dynamics simulations of nanoscale gold patches suspended in graphene pores, we predict the existence of an atomically thin, free-standing 2D liquid phase. The liquid phase, enabled by the exceptional planar stability of gold due to relativistic effects, demonstrates extreme fluxionality of metal nanostructures and opens possibilities for a variety of nanoscale phenomena.
We report the first direct spectroscopic evidence for coherent electronic coupling between excitons and trions in atomically thin transition metal dichalcogenides, specifically monolayer MoSe2. Signatures of coupling appear as isolated cross-peaks in two-color pump-probe spectra, and the lineshape of the peaks reveals that the coupling originates from many-body interactions. Excellent agreement between the experiment and density matrix calculations suggests the formation of a correlated exciton-trion state due to their coupling.
Atomically-thin black phosphorus (BP) is an emerging two dimensional (2D) material exhibiting bright photoluminescence in the near infrared. Coupling its radiation to photonic nanostructures will be an important step toward the realization of 2D material based nanophotonic devices that operate efficiently in the near infrared, which includes the technologically important optical telecommunication wavelength bands. In this letter, we demonstrate the optical coupling between atomically-thin BP and a 2D photonic crystal nanocavity. We employed a home-build dry transfer apparatus for placing a thi…
We studied multi-exciton dynamics in monolayer WSe2 using nonlinear photoluminescence (PL) spectroscopy and Monte Carlo simulations. We observed strong nonlinear saturation behavior of exciton PL with increasing excitation power density, and long-distance exciton diffusion reaching several micrometers. We demonstrated that the diffusion-assisted exciton-exciton annihilation model accounts for the observed nonlinear PL behavior. The long-distance exciton diffusion and subsequent efficient exciton-exciton annihilation process determined the unusual multi-exciton dynamics in atomically thin layer…
A theory is presented for the modification of bandgaps in atomically thin boron nitride (BN) by attractive interactions mediated through phonons in a polarizable substrate, or in the BN plane. Gap equations are solved, and gap enhancements are found to range up to 70% for dimensionless electron-phonon coupling λ=1, indicating that a proportion of the measured BN bandgap may have a phonon origin.
Atomically thin transition metal dichalcogenides have emerged as promising candidates for sensitive photodetection. Here, we report a photoconductivity study of biased mono- and bilayer molybdenum disulfide field-effect transistors. We identify photovoltaic and photoconductive effects, which both show strong photogain. The photovoltaic effect is described as a shift in transistor threshold voltage due to charge transfer from the channel to nearby molecules, including SiO2 surface-bound water. The photoconductive effect is attributed to the trapping of carriers in band tail states in the molybd…
We demonstrate the continuous tuning of the electronic structure of atomically thin MoS2 on flexible substrates by applying a uniaxial tensile strain. A redshift at a rate of ~70 meV per percent applied strain for direct gap transitions, and at a rate 1.6 times larger for indirect gap transitions, have been determined by absorption and photoluminescence spectroscopy. Our result, in excellent agreement with first principles calculations, demonstrates the potential of twodimensional crystals for applications in flexible electronics and optoelectronics.
Localization of charge carriers in monolayers (MLs) of transition metal dichalcogenides (TMDs) dramatically increases spin and valley coherence times, and, by analogy with other systems, the role of the hyperfine interaction should enhance. We perform theoretical analysis of the intervalley hyperfine interaction in TMD MLs based on the group representation theory. We demonstrate, that the spin-valley locking leads to the helical structure of the in-plane hyperfine interaction. In the upper valence band the hyperfine interaction is shown to be of the Ising type, which can be used for fabricatio…
Phononic crystals and acoustic meta-materials are used to tailor phonon and sound propagation properties by facilitating artificial, periodic structures. Analogous to photonic crystals, phononic band gaps can be created, which influence wave propagation and, more generally, allow engineering of the acoustic properties of a system. Beyond that, nonlinear phenomena in periodic structures have been extensively studied in photonic crystals and atomic Bose-Einstein Condensates in optical lattices. However, creating nonlinear phononic crystals or nonlinear acoustic meta-materials remains challenging…
The electron transport properties of atomically thin semiconductors such as MoS2 have attracted significant recent scrutiny and controversy. In this work, the scattering mechanisms responsible for limiting the mobility of single layer semiconductors are evaluated. The roles of individual scattering rates are tracked as the 2D electron gas density is varied over orders of magnitude at various temperatures. From a comparative study of the individual scattering mechanisms, we conclude that all current reported values of mobilities in atomically thin transition-metal dichalcogenide semiconductors …
Atomically thin semiconductors such as transition metal dichalcogenide (TMD) monolayers exhibit a very strong Coulomb interaction, giving rise to a rich exciton landscape. This makes these materials highly attractive for efficient and tunable optoelectronic devices. In this article, we review the recent progress in the understanding of exciton optics, dynamics and transport, which crucially govern the operation of TMD-based devices. We highlight the impact of hBN-encapsulation, which reveals a plethora of many-particle states in optical spectra, and we outline the most novel breakthroughs in t…
We systematically measure the dielectric function of atomically thin MoS2 films with different layer numbers and demonstrate that excitonic effects play a dominant role in the dielectric function when the films are less than 5-7 layers thick. The dielectric function shows an anomalous dependence on the layer number. It decreases with the layer number increasing when the films are less than 5-7 layers thick but turns to increase with the layer number for thicker films. We show that this is because the excitonic effect is very strong in the thin MoS2 films and its contribution to the dielectric …
The ability to modulate light at high speeds is of paramount importance for telecommunications, information processing, and medical imaging technologies. This has stimulated intense efforts to master optoelectronic switching at visible and near-infrared frequencies, although coping with current computer speeds in integrated architectures still remains a major challenge. As a partial success, midinfrared light modulation has been recently achieved through gating patterned graphene. Here we show that atomically thin noble metal nanoislands can extend optical modulation to the visible and near-in…
Modification of electromagnetic quantum fluctuations in the form of quadrature-squeezing is a central quantum resource, which can be generated from nonlinear optical processes. Such a process is facilitated by coherent two-photon excitation of the strongly bound biexciton in atomically thin semiconductors. We show theoretically that interfacing an atomically thin semiconductor with an optical cavity allows to harness this two-photon resonance and use the biexcitonic parametric gain to generate squeezed light with input power an order of magnitude below current state-of-the-art devices with con…
