Embodying bosonic and interactive characteristics in two-dimensional space, excitons in transition metal dichalcogenides (TMDCs) have garnered considerable attention. The utilization of the strong-correlation effects, long-range transport, and valley-dependent properties requires customizing exciton decay dynamics. Vacuum-field manipulation allows radiative decay engineering without disturbing intrinsic material properties. However, conventional flat mirrors cannot customize the radiative decay landscape in TMDC's plane or support vacuum-field interference with desired spectrum and polarization properties. Here, we present a meta-mirror platform resolving the issues with more optical degrees of freedom. For neutral excitons of the monolayer MoSe<sub>2</sub>, the optical layout formed by meta-mirrors manipulated the radiative decay rate in space by 2 orders of magnitude and revealed the statistical correlation between emission intensity and spectral line width. Moreover, the anisotropic meta-mirror demonstrated polarization-dependent radiative decay control. Our platform would be promising to tailor two-dimensional distributions of lifetime, density, diffusion, and polarization of TMDC excitons in advanced opto-excitonic applications.
Strain engineering has quickly emerged as a viable option to modify the electronic, optical, and magnetic properties of 2D materials. However, it remains challenging to arbitrarily control the strain. Here we show that, by creating atomically flat surface nanostructures in hexagonal boron nitride, we achieve an arbitrary on-chip control of both the strain distribution and magnitude on high-quality molybdenum disulfide. The phonon and exciton emissions are shown to vary in accordance with our strain field designs, enabling us to write and draw any photoluminescence color image in a single chip. Moreover, our strain engineering offers a powerful means to significantly and controllably alter the strengths and energies of interlayer excitons at room temperature. This method can be easily extended to other material systems and offers promise for functional excitonic devices.
Abstract We investigate the valley coherence in high and low-quality monolayer MoSe 2 by polarization-resolved photoluminescence spectroscopy. The observed valley coherence is on the order of 10% regardless of the sample quality, proving that the suppression of extrinsic effects does not improve the valley coherence. The valley decoherence time estimated based on the valley coherence time and exciton lifetime is sub-picosecond at the longest, which suggests that intrinsic scattering sources, such as phonons, strongly limit the valley coherence.
Sensitive gas sensors are a key requirement for a large number of applications. Two-dimensional (2D) materials exhibit excellent properties for low power consumption sensing devices due to their ultra-high surface-to-volume ratios. In this work, we used 2D materials such as black phosphorus (BP) for developing a field-effect transistor (FET) gas sensor. We demonstrated C$\mathrm{O}_{2}-$sensing performance at room temperature. A clear shift in current was observed during switching on and off the CO<inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</inf> flow. The ability to enhance the sensor response by modulating the gate voltage highlights the advantage of our FETs over resistor-based sensors. Our results show that the proposed method is a promising strategy to improve 2D materials CO<inf xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</inf> detectors and has a potential for applications in advanced gas-sensing devices.
Two-dimensional (2D) transistors are promising for potential applications in next-generation semiconductor chips. Owing to the atomically thin thickness of 2D materials, the carrier scattering from interfacial Coulomb scatterers greatly suppresses the carrier mobility and hampers transistor performance. However, a feasible method to quantitatively determine relevant Coulomb scattering parameters from interfacial long-range scatterers is largely lacking. Here, we demonstrate a method to determine the Coulomb scattering strength and the density of Coulomb scattering centers in InSe transistors by comprehensively analyzing the low-frequency noise and transport characteristics. Moreover, the relative contributions from long-range and short-range scattering in the InSe transistors can be distinguished. This method is employed to make InSe transistors consisting of various interfaces a model system, revealing the profound effects of different scattering sources on transport characteristics and low-frequency noise. Quantitatively accessing the scattering parameters of 2D transistors provides valuable insight into engineering the interfaces of a wide spectrum of ultrathin-body transistors for high-performance electronics.
Read moreMoiré superlattices of semiconducting transition metal dichalcogenides enable unprecedented spatial control of electron wavefunctions, leading to emerging quantum states. The breaking of translational symmetry further introduces a new degree of freedom: high symmetry moiré sites of energy minima behaving as spatially separated quantum dots. We demonstrate the superposition between two moiré sites by constructing a trilayer WSe<sub>2</sub>/monolayer WS<sub>2</sub> moiré heterojunction. The two moiré sites in the first layer WSe<sub>2</sub> interfacing WS<sub>2</sub> allow the formation of two different interlayer excitons, with the hole residing in either moiré site of the first layer WSe<sub>2</sub> and the electron in the third layer WSe<sub>2</sub>. An electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe<sub>2</sub> layer, realizing the continuous tuning of interlayer exciton hopping between two moiré sites and a superposition of the two interlayer excitons, distinctively different from the natural trilayer WSe<sub>2</sub>.
Read moreThe monolayer transition-metal dichalcogenides (TMDCs), lacking inversion symmetry, allow the manipulation of excitonic states with valley degree of freedom through circularly polarized light [1-3]. However, with the complex landscape of exciton species in TMDCs, such as spin- or momentum- forbidden dark excitons, the valley depolarization mechanisms, which are of great importance for valleytronic applications, still lack clear understanding. Such measurements require direct access to the momentum and energy coordinate of constituent electrons and holes, but few experimental techniques provide such information. Meanwhile, time- and angle- resolved photoemission spectroscopy (TR-ARPES) has become a powerful tool to study excitons of 2D semiconductors in energy-momentum space [4-7]. In this talk, we focus on our momentum-resolved study on the valley-polarized excitons in monolayer WS 2
Read moreFor almost a century, magnetic oscillations have been a powerful "quantum ruler" for measuring Fermi surface topology. In this study, we used Landau-level spectroscopy to unravel the energy-resolved valley-contrasting orbital magnetism and large orbital magnetic susceptibility that contribute to the energies of Landau levels of twisted double-bilayer graphene. These orbital magnetism effects led to substantial deviations from the standard Onsager relation, which manifested as a breakdown in scaling of Landau-level orbits. These substantial magnetic responses emerged from the nontrivial quantum geometry of the electronic structure and the large length scale of the moiré lattice potential. Going beyond traditional measurements, Landau-level spectroscopy performed with a scanning tunneling microscope offers a complete quantum ruler that resolves the full energy dependence of orbital magnetic properties in moiré quantum matter.
Read moreHigh-temperature cuprate superconductors based van der Waals (vdW) heterostructures hold high technological promise. One of the obstacles hindering their progress is the detrimental effect of disorder on the properties of the vdW-devices-based Josephson junctions (JJs). Here, a new method of fabricating twisted vdW heterostructures made of Bi<sub>2</sub> Sr<sub>2</sub> CuCa<sub>2</sub> O<sub>8+δ</sub> , crucially improving the JJ characteristics and pushing them up to those of the intrinsic JJs in bulk samples, is reported. The method combines cryogenic stacking using a solvent-free stencil mask technique and covering the interface by insulating hexagonal boron nitride crystals. Despite the high-vacuum condition down to 10<sup>-6</sup> mbar in the evaporation chamber, the interface appears to be protected from water molecules during the in situ metal deposition only when fully encapsulated. Comparing the current-voltage curves of encapsulated and unencapsulated interfaces, it is revealed that the encapsulated interfaces' characteristics are crucially improved, so that the corresponding JJs demonstrate high critical currents and sharpness of the superconducting transition comparable to those of the intrinsic JJs. Finally, it is shown that the encapsulated heterostructures are more stable over time.
Read moreElectron–photon temporal correlations in electron energy loss spectroscopy (EELS) and cathodoluminescence (CL) spectroscopies have recently been used to measure the relative quantum efficiency of materials. This combined spectroscopy, named cathodoluminescence excitation (CLE) spectroscopy, allows for the identification of excitation and decay channels, which are hidden in average measurements. Here, we demonstrate that CLE can also be used to measure excitations' decay time. In addition, the decay time as a function of the excitation energy is measured, as the energy for each electron–photon pair is probed. We used two well-known insulating materials to characterize this technique, nanodiamonds with NV0 defects and hexagonal boron nitride (h-BN) with 4.1 eV defects. Both also exhibit marked transition radiations, whose extremely short decay times can be used to characterize the instrumental response function. It is found to be typically 2 ns, in agreement with the expected limit of the EELS detector temporal resolution. The measured lifetimes of NV0 centers in diamond nanoparticles (20–40 ns) and 4.1 eV defect in h-BN flakes (&lt;2 ns) match those reported previously.
Read moreWe report a 250-fold photoluminescence enhancement of V B - spin-defects in hBN by coupling them to nanopatch antennas (NPA). Considering the relative size of the NPAs and laser-spot, an actual enhancement of 1695 times is determined.
Read moreAbstract Modulation of the Fermi level using an ultraviolet (UV)-assisted photochemical method is demonstrated in tungsten diselenide monolayers. Systematic shifts and relative intensities between charged and neutral exciton species indicate a progressive and controllable decrease of the electron density and switch tungsten diselenide from n-type to a p-type semiconductor. The presence of chlorine in the 2D crystal shifts the Fermi level closer to the valence band while the effect can be only partially reversible via continuous wave laser rastering process. Chlorine species in the lattice are validated by x-ray photoelectron spectroscopy, while density functional theory calculations predict that adsorption of chlorine on the selenium vacancy sites leads to p-type doping. The results of our study indicate that photochemical techniques have the potential to enhance the performance of various 2D materials, making them suitable for integrated optoelectronics such as lateral nanopatterned p–n junctions.
Read more${\mathrm{MoS}}_{2}$ is an emergent van der Waals material that shows promising prospects in semiconductor industry and optoelectronic applications. However, its electronic properties are not yet fully understood. In particular, the nature of the insulating state at low carrier density deserves further investigation, as it is important for fundamental research and applications. In this study we investigate the insulating state of a dual-gated exfoliated bilayer ${\mathrm{MoS}}_{2}$ field-effect transistor by performing magnetotransport experiments. We observe a positive and nonsaturating magnetoresistance, in a regime where only one band contributes to electron transport. At low electron density ($\ensuremath{\sim}1.4\ifmmode\times\else\texttimes\fi{}{10}^{12}\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}2}$) and a perpendicular magnetic field of 7 Tesla the resistance exceeds by more than one order of magnitude the zero field resistance and exponentially drops with increasing temperature. We attribute this observation to strong electron localization. Both temperature and magnetic field dependence can, at least qualitatively, be described by the Efros-Shklovskii law, predicting the formation of a Coulomb gap in the density of states due to Coulomb interactions. However, the localization length obtained from fitting the temperature dependence exceeds by more than one order of magnitude the one obtained from the magnetic field dependence. We attribute this discrepancy to the presence of a nearby metallic gate, which provides electrostatic screening and thus reduces long-range Coulomb interactions. The result of our study suggests that the insulating state of ${\mathrm{MoS}}_{2}$ originates from a combination of disorder-driven electron localization and Coulomb interactions.
Read moreAbstract Recently, magic-angle twisted bilayer graphene (MATBLG) has emerged with various interaction-driven novel quantum phases at the commensurate fillings of the moiré superlattice, while the charge neutrality point (CNP) remains mostly a trivial insulator. Here, we show an emerging phase of compensated semimetallicity at the CNP of twisted double bilayer graphene (TDBLG), a close cousin of MATBLG, with signatures of electronic correlation. Using electrical and thermal transport, we find two orders of magnitude enhancement of the thermopower at magnetic fields much smaller than the extreme quantum limit, accompanied by large magnetoresistance ( ~ 2500%) at CNP, providing strong experimental evidence of compensated semimetallicity at CNP of TDBLG. Moreover, at low temperatures, we observe unusual sublinear temperature dependence of resistance. A recent theory 1 predicts the formation of an excitonic metal near CNP, where small electron and hole pockets co-exist. We understand this sublinear temperature dependence in terms of critical fluctuations in this theory.
Read moreAbstract We examined the exciton energy transfer process in a lateral heteromonolayer of WSe 2 –MoSe 2 at low temperature. Position-dependent photoluminescence (PL) and PL excitation spectroscopy measurements revealed the occurrence of exciton energy transport from WSe 2 to MoSe 2 both at RT and 15 K. The effective energy transport distance in WSe 2 was longer at 15 K than at RT, suggesting that the dark excitons with longer diffusion length than bright excitons preferentially contributed to the exciton energy transport across the heterojunction interface at 15 K. Additionally, we observed that no valley information was transported from WSe 2 to MoSe 2 via the energy transfer process. This study provides useful insights for the development of excitonic devices based on exciton transport in transition metal dichalcogenides.
Read moreThe moiré potential, induced by stacking two monolayer semiconductors with slightly different lattice mismatches, acts as periodic quantum confinement for optically generated excitons, resulting in spatially ordered zero-dimensional quantum systems. However, there are limitations to exploring intrinsic optical properties of moiré excitons due to ensemble emissions and broadened emissions from many peaks caused by the inhomogeneity of the moiré potential. In this study, we proposed a microfabrication technique based on focused Ga<sup>+</sup> ion beams, which enables us to control the number of peaks originating from the moiré potential and thus explore unknown moiré optical characteristics of WSe<sub>2</sub>/MoSe<sub>2</sub> heterobilayer. By taking advantage of this approach, we reveal emissions from a single moiré exciton and charged moiré exciton (trion) under electrostatic doping conditions. We show the momentum dark moiré trion state above the bright trion state with a splitting energy of approximately 4 meV and clarify that the dynamics are determined by the initial trion population in the bright state. Furthermore, the degree of negative circularly polarized emissions and their valley dynamics of moiré trions are dominated by a very long valley relaxation process lasting ∼700 ns. Our findings on microfabricated heterobilayer could be viewed as an extension of our groundbreaking efforts in the field of quantum optics application using moiré superlattices.
Read moreAbstract 2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto‐electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient‐reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient‐reactive 2D antiferromagnetic semiconductor NiI 2 . The resulting gate‐tunable transistors show band‐like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI 2 , revealing a Hall mobility of 15 cm 2 V −1 s −1 at 1.7 K. These devices also allow direct electrical probing of the thickness‐dependent multiferroic phase transition temperature of NiI 2 from 59 K (bulk) to 28 K (monolayer).
Read moreAbstract Hybrid two‐dimensional materials consisting of graphene and hexagonal boron nitride ( h ‐BN) have drawn significant interest due to their tunable bandgap and electrical properties. Considering their composition‐dependent properties, ohmic current injection and the development of h ‐BN‐based optoelectronic and high‐power electronic devices should be achievable by controlling the C concentration. In this study, electrical and optical characterizations of single‐crystal h ‐BN synthesized under high‐pressure and high‐temperature (HPHT) are conducted by varying C concentrations via post‐growth diffusion. Low C‐doped h ‐BN ( h ‐BN:C) with ≈0.1 at% C exhibits nonohmic conduction within a voltage range of ±100 V at all temperatures. In contrast, high h ‐BN:C (≈10 at% C) containing C domains and graphite/graphene layers shows additional luminescence peaks and initially exhibits nonohmic conduction at 298 K, which then transforms to ohmic conduction after breakdown‐like behavior at 598 K. This phenomenon, observed only in the high h ‐BN:C devices, is attributed to the C‐containing conductive path formed on the channel surface through C drift and local dielectric breakdown of h ‐BN mother phase, indicating that ohmic conduction itself does not guarantee the current flow in the conduction/valence bands in h ‐BN:C. With these findings, the present thorough and fruitful characterizations are beneficial for the development of h ‐BN:C‐based devices.
Read moreWe report on a tunable---by magnetic field and gate voltage---conversion of terahertz radiation into a dc current in spatially modulated bilayer graphene. We experimentally demonstrate that the underlying physics is related to the so-called ratchet effect. Our key findings are the direct observation of a sharp cyclotron resonance in the photocurrent and the demonstration of two effects caused by electron-electron interaction: the plasmonic splitting of the resonance due to long-range Coulomb coupling and the partial suppression of its second harmonic due to fast interparticle collisions. We develop a theory, which perfectly fits our data. We argue that the ratchet current is generated in the hydrodynamic regime of nonideal electron liquid.
Read moreTwo-dimensional flat-band systems have recently attracted considerable interest due to the rich physics unveiled by emergent phenomena and correlated electronic states at van Hove singularities. However, the difficulties in electrically detecting the flat-band position in field-effect structures are slowing down the investigation of their properties. In this work, we use indium selenide (InSe) as a flat-band system due to a van Hove singularity at the valence-band edge in a few-layer form of the material without the requirement of a twist angle. We investigate tunnelling photocurrents in gated few-layer InSe structures and relate them to ambipolar transport and photoluminescence measurements. We observe an appearance of a sharp change in tunnelling mechanisms due to the presence of the van Hove singularity at the flat band. We further corroborate our findings by studying tunnelling currents as a reliable probe for the flat-band position up to room temperature. Our results create an alternative approach to studying flat-band systems in heterostructures of two-dimensional materials.
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