Browse
Submit Data
Databases
API
Help

Dataset Information

34 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Identification of twist-angle-dependent excitons in WS₂/WSe₂ heterobilayers.

ABSTRACT: Stacking atomically thin films enables artificial construction of van der Waals heterostructures with exotic functionalities such as superconductivity, the quantum Hall effect, and engineered light-matter interactions. In particular, heterobilayers composed of monolayer transition metal dichalcogenides have attracted significant interest due to their controllable interlayer coupling and trapped valley excitons in moiré superlattices. However, the identification of twist-angle-modulated optical transitions in heterobilayers is sometimes controversial since both momentum-direct (K-K) and -indirect excitons reside on the low energy side of the bright exciton in the monolayer constituents. Here, we attribute the optical transition at ∼1.35 eV in the WS₂/WSe₂ heterobilayer to an indirect Γ-K transition based on a systematic analysis and comparison of experimental photoluminescence spectra with theoretical calculations. The exciton wavefunction obtained by the state-of-the-art GW-Bethe-Salpeter equation approach indicates that both the electron and hole of the excitons are contributed by the WS₂ layer. Polarization-resolved k-space imaging further confirms that the transition dipole moment of this optical transition is dominantly in-plane and is independent of the twist angle. The calculated absorption spectrum predicts that the so-called interlayer exciton peak coming from the K-K transition is located at 1.06 eV, but with a much weaker amplitude. Our work provides new insight into the steady-state and dynamic properties of twist-angle-dependent excitons in van der Waals heterostructures.

SUBMITTER: Wu K

PROVIDER: S-EPMC9252742 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Json Xml

Similar Datasets

Twist-angle dependence of moire excitons in WS2/MoSe2 heterobilayers.

Project description:Moiré lattices formed in twisted van der Waals bilayers provide a unique, tunable platform to realize coupled electron or exciton lattices unavailable before. While twist angle between the bilayer has been shown to be a critical parameter in engineering the moiré potential and enabling novel phenomena in electronic moiré systems, a systematic experimental study as a function of twist angle is still missing. Here we show that not only are moiré excitons robust in bilayers of even large twist angles, but also properties of the moiré excitons are dependant on, and controllable by, the moiré reciprocal lattice period via twist-angle tuning. From the twist-angle dependence, we furthermore obtain the effective mass of the interlayer excitons and the electron inter-layer tunneling strength, which are difficult to measure experimentally otherwise. These findings pave the way for understanding and engineering rich moiré-lattice induced phenomena in angle-twisted semiconductor van der Waals heterostructures.

| S-EPMC7675978 | biostudies-literature

Moire excitons in MoSe2-WSe2 heterobilayers and heterotrilayers.

Project description:Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moiré interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe2-WSe2 stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlayer moiré excitons in different spin and valley configurations. We conclude that the photoluminescence of MoSe2-WSe2 heterobilayer is consistent with joint contributions from radiatively decaying valley-direct interlayer excitons and phonon-assisted emission from momentum-indirect reservoirs that reside in spatially distinct regions of moiré supercells, whereas the heterotrilayer emission is entirely due to momentum-dark interlayer excitons of hybrid-layer valleys. Our results highlight the profound role of interlayer hybridization for transition metal dichalcogenide heterostacks and other realizations of multi-layered semiconductor van der Waals heterostructures.

| S-EPMC7955063 | biostudies-literature

Localization and interaction of interlayer excitons in MoSe2/WSe2 heterobilayers.

Project description:Transition metal dichalcogenide (TMD) heterobilayers provide a versatile platform to explore unique excitonic physics via the properties of the constituent TMDs and external stimuli. Interlayer excitons (IXs) can form in TMD heterobilayers as delocalized or localized states. However, the localization of IX in different types of potential traps, the emergence of biexcitons in the high-excitation regime, and the impact of potential traps on biexciton formation have remained elusive. In our work, we observe two types of potential traps in a MoSe2/WSe2 heterobilayer, which result in significantly different emission behavior of IXs at different temperatures. We identify the origin of these traps as localized defect states and the moiré potential of the TMD heterobilayer. Furthermore, with strong excitation intensity, a superlinear emission behavior indicates the emergence of interlayer biexcitons, whose formation peaks at a specific temperature. Our work elucidates the different excitation and temperature regimes required for the formation of both localized and delocalized IX and biexcitons and, thus, contributes to a better understanding and application of the rich exciton physics in TMD heterostructures.

| S-EPMC10616232 | biostudies-literature

Strong interaction between interlayer excitons and correlated electrons in WSe2/WS2 moire superlattice.

Project description:Heterobilayers of transition metal dichalcogenides (TMDCs) can form a moiré superlattice with flat minibands, which enables strong electron interaction and leads to various fascinating correlated states. These heterobilayers also host interlayer excitons in a type-II band alignment, in which optically excited electrons and holes reside on different layers but remain bound by the Coulomb interaction. Here we explore the unique setting of interlayer excitons interacting with strongly correlated electrons, and we show that the photoluminescence (PL) of interlayer excitons sensitively signals the onset of various correlated insulating states as the band filling is varied. When the system is in one of such states, the PL of interlayer excitons is relatively amplified at increased optical excitation power due to reduced mobility, and the valley polarization of interlayer excitons is enhanced. The moiré superlattice of the TMDC heterobilayer presents an exciting platform to engineer interlayer excitons through the periodic correlated electron states.

| S-EPMC8203657 | biostudies-literature

Radiative pattern of intralayer and interlayer excitons in two-dimensional WS2/WSe2 heterostructure.

Project description:Two-dimensional (2D) heterostructures (HS) formed by transition-metal dichalcogenide (TMDC) monolayers offer a unique platform for the study of intralayer and interlayer excitons as well as moiré-pattern-induced features. Particularly, the dipolar charge-transfer exciton comprising an electron and a hole, which are confined to separate layers of 2D semiconductors and Coulomb-bound across the heterojunction interface, has drawn considerable attention in the research community. On the one hand, it bears significance for optoelectronic devices, e.g. in terms of charge carrier extraction from photovoltaic devices. On the other hand, its spatially indirect nature and correspondingly high longevity among excitons as well as its out-of-plane dipole orientation render it attractive for excitonic Bose-Einstein condensation studies, which address collective coherence effects, and for photonic integration schemes with TMDCs. Here, we demonstrate the interlayer excitons' out-of-plane dipole orientation through angle-resolved spectroscopy of the HS photoluminescence at cryogenic temperatures, employing a tungsten-based TMDC HS. Within the measurable light cone, the directly-obtained radiation profile of this species clearly resembles that of an in-plane emitter which deviates from that of the intralayer bright excitons as well as the other excitonic HS features recently attributed to artificial superlattices formed by moiré patterns.

| S-EPMC9050751 | biostudies-literature

Twist Angle mapping in layered WS2 by Polarization-Resolved Second Harmonic Generation.

Project description:Stacked atomically thin transition metal dichalcogenides (TMDs) exhibit fundamentally new physical properties compared to those of the individual layers. The twist angle between the layers plays a crucial role in tuning these properties. Having a tool that provides high-resolution, large area mapping of the twist angle, would be of great importance in the characterization of such 2D structures. Here we use polarization-resolved second harmonic generation (P-SHG) imaging microscopy to rapidly map the twist angle in large areas of overlapping WS2 stacked layers. The robustness of our methodology lies in the combination of both intensity and polarization measurements of SHG in the overlapping region. This allows the accurate measurement and consequent pixel-by-pixel mapping of the twist angle in this area. For the specific case of 30° twist angle, P-SHG enables imaging of individual layers.

| S-EPMC6776617 | biostudies-literature

Controlled edge dependent stacking of WS2-WS2 Homo- and WS2-WSe2 Hetero-structures: A Computational Study.

Project description:Transition Metal Dichalcogenides (TMDs) are one of the most studied two-dimensional materials in the last 5-10 years due to their extremely interesting layer dependent properties. Despite the presence of vast research work on TMDs, the complex relation between the electro-chemical and physical properties make them the subject of further research. Our main objective is to provide a better insight into the electronic structure of TMDs. This will help us better understand the stability of the bilayer post growth homo/hetero products based on the various edge-termination, and different stacking of the two layers. In this regard, two Tungsten (W) based non-periodic chalcogenide flakes (sulfides and selenides) were considered. An in-depth analysis of their different edge termination and stacking arrangement was performed via Density Functional Theory method using VASP software. Our finding indicates the preference of chalcogenide (c-) terminated structures over the metal (m-) terminated structures for both homo and heterobilayers, and thus strongly suggests the nonexistence of the m-terminated TMDs bilayer products.

| S-EPMC6997452 | biostudies-literature

Coherent Phonons in van der Waals MoSe2/WSe2 Heterobilayers.

Project description:The increasing role of two-dimensional (2D) devices requires the development of new techniques for ultrafast control of physical properties in 2D van der Waals (vdW) nanolayers. A special feature of heterobilayers assembled from vdW monolayers is femtosecond separation of photoexcited electrons and holes between the neighboring layers, resulting in the formation of Coulomb force. Using laser pulses, we generate a 0.8 THz coherent breathing mode in MoSe2/WSe2 heterobilayers, which modulates the thickness of the heterobilayer and should modulate the photogenerated electric field in the vdW gap. While the phonon frequency and decay time are independent of the stacking angle between the MoSe2 and WSe2 monolayers, the amplitude decreases at intermediate angles, which is explained by a decrease in the photogenerated electric field between the layers. The modulation of the vdW gap by coherent phonons enables a new technology for the generation of THz radiation in 2D nanodevices with vdW heterobilayers.

| S-EPMC10510584 | biostudies-literature

Twist angle-dependent conductivities across MoS2/graphene heterojunctions.

Project description:Van der Waals heterostructures stacked from different two-dimensional materials offer a unique platform for addressing many fundamental physics and construction of advanced devices. Twist angle between the two individual layers plays a crucial role in tuning the heterostructure properties. Here we report the experimental investigation of the twist angle-dependent conductivities in MoS2/graphene van der Waals heterojunctions. We found that the vertical conductivity of the heterojunction can be tuned by ?5 times under different twist configurations, and the highest/lowest conductivity occurs at a twist angle of 0°/30°. Density functional theory simulations suggest that this conductivity change originates from the transmission coefficient difference in the heterojunctions with different twist angles. Our work provides a guidance in using the MoS2/graphene heterojunction for electronics, especially on reducing the contact resistance in MoS2 devices as well as other TMDCs devices contacted by graphene.

| S-EPMC6172227 | biostudies-literature

Lattice Reconstruction in MoSe2-WSe2 Heterobilayers Synthesized by Chemical Vapor Deposition.

Project description:Vertical van der Waals heterostructures of semiconducting transition metal dichalcogenides realize moiré systems with rich correlated electron phases and moiré exciton phenomena. For material combinations with small lattice mismatch and twist angles as in MoSe2-WSe2, however, lattice reconstruction eliminates the canonical moiré pattern and instead gives rise to arrays of periodically reconstructed nanoscale domains and mesoscopically extended areas of one atomic registry. Here, we elucidate the role of atomic reconstruction in MoSe2-WSe2 heterostructures synthesized by chemical vapor deposition. With complementary imaging down to the atomic scale, simulations, and optical spectroscopy methods, we identify the coexistence of moiré-type cores and extended moiré-free regions in heterostacks with parallel and antiparallel alignment. Our work highlights the potential of chemical vapor deposition for applications requiring laterally extended heterosystems of one atomic registry or exciton-confining heterostack arrays.

| S-EPMC10214437 | biostudies-literature