Confinement of long-lived interlayer excitons in WS$_2$/WSe$_2$ heterostructures
Alejandro R. -P. Montblanch, Dhiren M. Kara, Ioannis Paradisanos, Carola M. Purser, Matthew S. G. Feuer, Evgeny M. Alexeev, Lucio Stefan, Ying Qin, Mark Blei, G… 展开作者
Alejandro R. -P. Montblanch, Dhiren M. Kara, Ioannis Paradisanos, Carola M. Purser, Matthew S. G. Feuer, Evgeny M. Alexeev, Lucio Stefan, Ying Qin, Mark Blei, Gang Wang, Alisson R. Cadore, Pawel Latawiec, Marko Lončar, Sefaattin Tongay, Andrea C. Ferrari, Mete Atatüre
Interlayer excitons in layered materials constitute a novel platform to study many-body phenomena arising from long-range interactions between quantum particles. The ability to localise individual interlayer excitons in potential energy traps is a key step towards simulating Hubbard physics in artificial lattices. Here, we demonstrate spatial localisation of long-lived interlayer excitons in a strongly confining trap array using a WS$_{2}$/WSe$_{2}$ heterostructure on a nanopatterned substrate. We detect long-lived interlayer excitons with lifetime approaching 0.2 ms and show that their confinement results in a reduced lifetime in the microsecond range and stronger emission rate with sustained optical selection rules. The combination of a permanent dipole moment, spatial confinement and long lifetime places interlayer excitons in a regime that satisfies one of the requirements for observing long-range dynamics in an optically resolvable trap lattice.
Interlayer excitons (IXs) possess a much longer lifetime than intralayer excitons due to the spatial separation of the electrons and holes; hence, they have been pursued to create exciton condensates for decades. The recent emergence of two-dimensional (2D) materials, such as transition metal dichalcogenides (TMDs), and of their van der Waals heterostructures (HSs), in which two different 2D materials are layered together, has created new opportunities to study IXs. Here we present the observation of IX gases within two stacked structures consisting of hBN/WSe$_2$/hBN/p: WSe$_2$/hBN. The IX en…
Moiré superlattices in van der Waals heterostructures have emerged as a powerful tool for engineering novel quantum phenomena. Here we report the observation of a correlated interlayer exciton insulator in a double-layer heterostructure composed of a WSe2 monolayer and a WS2/WSe2 moiré bilayer that are separated by an ultrathin hexagonal boron nitride (hBN). The moiré WS2/WSe2 bilayer features a Mott insulator state at hole density p/p0 = 1, where p0 corresponds to one hole per moiré lattice site. When electrons are added to the Mott insulator in the WS2/WSe2 moiré bilayer and an equal number …
The optical spectra of vertically stacked MoSe$_2$/WSe$_2$ heterostructures contain additional 'interlayer' excitonic peaks that are absent in the individual monolayer materials and exhibit a significant spatial charge separation in out-of-plane direction. Extending on a previous study, we used a many-body perturbation theory approach to simulate and analyse the excitonic spectra of MoSe$_2$/WSe$_2$ heterobilayers with three stacking orders, considering both momentum-direct and momentum-indirect excitons. We find that the small oscillator strengths and corresponding optical responses of the in…
Coherent coupling between excitons is at the heart of many-body interactions with transition metal dichalcogenide (TMD) heterostructures as an emergent platform for the investigation of these interactions. We employ multi-dimensional coherent spectroscopy on monolayer MoSe\textsubscript{2}/WSe\textsubscript{2} heterostructures and observe coherent coupling between excitons spatially localized in monolayer MoSe$_2$ and WSe$_2$. Through many-body spectroscopy, we further observe the absorption state arising from free interlayer electron-hole pairs. This observation yields a spectroscopic measure…
We demonstrate gate-tunable resonant tunneling and negative differential resistance between two rotationally aligned bilayer graphene sheets separated by bilayer WSe2. We observe large interlayer current densities of 2 uA/um2 and 2.5 uA/um2, and peak-to-valley ratios approaching 4 and 6 at room temperature and 1.5 K, respectively, values that are comparable to epitaxially grown resonant tunneling heterostructures. An excellent agreement between theoretical calculations using a Lorentzian spectral function for the two-dimensional (2D) quasiparticle states, and the experimental data indicates th…
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 MoSe$_2$-WSe$_2$ 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 interlay…
Based on \emph{ab initio} theoretical calculations of the optical spectra of vertical heterostructures of MoSe$_2$ (or MoS$_2$) and WSe$_2$ sheets, we reveal two spin-orbit-split Rydberg series of excitonic states below the \textsl{A} excitons of MoSe$_2$ and WSe$_2$ with a significant binding energy on the order of 250\,meV for the first excitons in the series. At the same time, we predict crystalographically aligned MoSe$_2$/WSe$_2$ heterostructures to exhibit an indirect fundamental band gap. Due to the type-II nature of the MoSe$_2$/WSe$_2$ heterostructure, the indirect transition and the …
Two-dimensional (2D) materials, such as graphene1, boron nitride2, and transition metal dichalcogenides (TMDs)3-5, have sparked wide interest in both device physics and technological applications at the atomic monolayer limit. These 2D monolayers can be stacked together with precise control to form novel van der Waals heterostructures for new functionalities2,6-9. One highly coveted but yet to be realized heterostructure is that of differing monolayer TMDs with type II band alignment10-12. Their application potential hinges on the fabrication, understanding, and control of bonded monolayers, w…
We report on the far-field photoluminescence intensity distribution of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks as measured by back focal plane imaging in the temperature range between 1.7 K and 20 K. By comparing the data with an analytical model describing the dipolar emission pattern in a dielectric environment, we are able to obtain the relative contributions of the in- and out-of-plane transition dipole moments associated to the interlayer exciton photon emission. We determine the transition dipole moments for all observed interlayer exciton transitions to be (99 $\pm$ 1)%…
In this paper, we employ a fully microscopic approach to the study of interlayer excitons in hetero-bilayers. We use Fowler's and Karplus' method to access the dynamical polarizability of non--interacting interlayer excitons in a $\mathrm{WSe}_{2}/\mathrm{WS}_{2}$--based van der Waals heterostructure. Following from the calculation of the linear polarizability, we consider Svendsen's variational method to the calculation of the dynamic third--order polarizability. With this variational method, we study both two--photon absorption and third--harmonic generation processes for interlayer excitons…
The nanoscale periodic potentials introduced by moiré patterns in semiconducting van der Waals (vdW) heterostructures provide a new platform for designing exciton superlattices. To realize these applications, a thorough understanding of the localization and delocalization of interlayer excitons in the moiré potentials is necessary. Here, we investigated interlayer exciton dynamics and transport modulated by the moiré potentials in WS$_2$-WSe$_2$ heterobilayers in time, space, and momentum domains using transient absorption microscopy combined with first-principles calculations. Experimental re…
Moiré superlattices provide a powerful way to engineer properties of electrons and excitons in two-dimensional van der Waals heterostructures. The moiré effect can be especially strong for interlayer excitons, where electrons and holes reside in different layers and can be addressed separately. In particular, it was recently proposed that the moiré superlattice potential not only localizes interlayer exciton states at different superlattice positions, but also hosts an emerging moiré quasi-angular momentum (QAM) that periodically switches the optical selection rules for interlayer excitons at …
Photoexcited intralayer excitons in van der Waals heterostructures (vdWHs) with type-II band alignment have been observed to tunnel into interlayer excitons on ultrafast timescales. Such interlayer excitons have sufficiently long lifetimes that inducing dissociation with external in-plane electric fields becomes an attractive option of improving efficiency of photocurrent devices. In the present paper, we calculate interlayer exciton binding energies, Stark shifts, and dissociation rates for six different transition metal dichalcogenide (TMD) vdWHs using a numerical procedure based on exterior…
Transition metal dichalcogenides (TMDCs) heterostructure with a type II alignment hosts unique interlayer excitons with the possibility of spin-triplet and spin-singlet states. However, the associated spectroscopy signatures remain elusive, strongly hindering the understanding of the Moire potential modulation of the interlayer exciton. In this work, we unambiguously identify the spin-singlet and spin-triplet interlayer excitons in the WSe2/MoSe2 hetero-bilayer with a 60-degree twist angle through the gate- and magnetic field-dependent photoluminescence spectroscopy. Both the singlet and tripl…
Charge separated interlayer excitons in transition metal dichalcogenide (TMDC) heterobilayers are being explored for moiré exciton lattices and exciton condensates. The presence of permanent dipole moments and the poorly screened Coulomb interaction make many body interactions particularly strong for interlayer excitons. Here we reveal two distinct phase transitions for interlayer excitons in the MoSe2/WSe2 heterobilayer using time and spatially resolved photoluminescence imaging: from trapped excitons in the moiré-potential to the modestly mobile exciton gas as exciton density increases to ne…
Van der Waals (vdW) heterostructures are receiving great attentions due to their intriguing properties and potentials in many research fields. The flow of charge carriers in vdW heterostructures can be efficiently rectified by the inter-layer coupling between neighboring layers, offering a rich collection of functionalities and a mechanism for designing atomically thin devices. Nevertheless, non-uniform contact in larger-area heterostructures reduces the device efficiency. In this work, ion irradiation had been verified as an efficient technique to enhance the contact and interlayer coupling i…
High-Energy Interlayer Exciton Ensembles in MoSe$_2$/WSe$_2$ Heterostructures by Laguerre-Gaussian Excitation
Walter Schottky Institute and Physics Department, TU Munich（慕尼黑工业大学沃尔特·肖特基研究所与物理系）；Munich Center for Quantum Science and Technology (MCQST)（慕尼黑量子科学与技术中心）；Institute of Physics, University of Münster（明斯特大学物理研究所）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国立材料研究所材料纳米架构研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国立材料研究所电子与光学材料研究中心）
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 phot…
Hybridisation of electronic bands of two-dimensional materials, assembled into twistronic heterostructures, enables one to tune their optoelectronic properties by selecting conditions for resonant interlayer hybridisation. Resonant interlayer hybridisation qualitatively modifies the excitons in such heterostructures, transforming these optically active modes into superposition states of interlayer and intralayer excitons. For MoSe$_2$/WSe$_2$ heterostructures, strong hybridization occurs between the holes in the spin-split valence band of WSe$_2$ and in the top valence band of MoSe$_2$, especi…
Exciton condensates (EC) are macroscopic coherent states arising from condensation of electron-hole pairs. Bilayer heterostructures, consisting of two-dimensional electron and hole layers separated by a tunnel barrier, provide a versatile platform to realize and study EC. The tunnel barrier suppresses recombination yielding long-lived excitons. However, this separation also reduces interlayer Coulomb interactions, limiting the exciton binding strength. Here, we report the observation of EC in naturally occurring 2H-stacked bilayer WSe$_2$. In this system, the intrinsic spin-valley structure su…
The availability of accessible fabrication methods based on deterministic transfer of atomically thin crystals has been essential for the rapid expansion of research into van der Waals heterostructures. An inherent issue of these techniques is the deformation of the polymer carrier film during the transfer, which can lead to highly non-uniform strain induced in the transferred two-dimensional material. Here, using a combination of optical spectroscopy, atomic force and Kelvin probe force microscopy, we show that the presence of nanometer scale wrinkles formed due to transfer-induced stress rel…
Ultrafast charge transfer processes provide a facile way to create interlayer excitons in directly contacted transition metal dichalcogenide (TMD) layers. More sophisticated heterostructures composed of TMD/hBN/TMD enable new ways to control interlayer exciton properties and achieve novel exciton phenomena, such as exciton insulators and condensates, where longer lifetimes are desired. In this work, we experimentally study the charge transfer dynamics in a heterostructure composed of a 1 nm thick hBN spacer between MoSe$_{2}$ and WSe$_{2}$ monolayers. We observe the hole transfer from MoSe$_{2…
Interlayer excitons (IXs) in hetero-bilayers of transition metal dichalcogenides (TMDs) represent an exciting emergent class of long-lived dipolar composite bosons in an atomically thin, near-ideal two-dimensional (2D) system. The long-range interactions that arise from the spatial separation of electrons and holes can give rise to novel quantum, as well as classical multi-particle correlation effects. In order to acquire a detailed understanding of the possible many-body effects, the fundamental interactions between individual IXs have to be studied. Here, we trap a tunable number of dipolar …
Transition metal dichalcogenide heterobilayers offer attractive opportunities to realize lattices of interacting bosons with several degrees of freedom. Such heterobilayers can feature moiré patterns that modulate their electronic band structure, leading to spatial confinement of single interlayer excitons (IXs) that act as quantum emitters with $C_3$ symmetry. However, the narrow emission linewidths of the quantum emitters contrast with a broad ensemble IX emission observed in nominally identical heterobilayers, opening a debate regarding the origin of IX emission. Here we report the continuo…
Coupling degrees of freedom of distinct nature plays a critical role in numerous physical phenomena. The recent emergence of layered materials provides a laboratory for studying the interplay between internal quantum degrees of freedom of electrons. Here, we report experimental signatures of new coupling phenomena connecting real spin with layer pseudospins in bilayer WSe2. In polarization-resolved photoluminescence measurements, we observe large spin orientation of neutral and charged excitons generated by both circularly and linearly polarized light, with a splitting of the trion spectrum in…
We investigate valley dynamics associated with trions in monolayer tungsten diselenide (WSe2) using polarization resolved two-color pump-probe spectroscopy. When tuning the pump and probe energy across the trion resonance, distinct trion valley polarization dynamics are observed as a function of energy and attributed to the intra-valley and inter-valley trions in monolayer WSe2. We observe no decay of a near-unity valley polarization associated with the intra-valley trions during ~ 25 ps, while the valley polarization of the inter-valley trions exhibits a fast decay of ~ 4 ps. Furthermore, we …
Moire-Engineered Excitonic Landscape and Phonon-Mediated Recombination in Twisted WSe2 Bilayers
Indian Institute of Technology Mandi（印度技术学院曼迪分校）；CSIR-National Physical Laboratory（印度科学工业研究理事会国家物理实验室）；Academy of Scientific and Innovative Research (AcSIR)（科学与创新研究学院）；Indian Institute of Science（印度科学学院）；National Institute of Material Science（国家物质科学研究所）
Vertically stacked van der Waals heterostructures constitute a promising platform for providing tailored band alignment with enhanced excitonic systems. Here we report observations of neutral and charged interlayer excitons in trilayer WSe2-MoSe2-WSe2 van der Waals heterostructures and their dynamics. The addition of a WSe2 layer in the trilayer leads to significantly higher photoluminescence quantum yields and tunable spectral resonance compared to its bilayer heterostructures at cryogenic temperatures. The observed enhancement in the photoluminescence quantum yield is due to significantly la…
Twisted layers of atomically thin two-dimensional materials realize a broad range of novel quantum materials with engineered optical and transport phenomena arising from spin and valley degrees of freedom and strong electron correlations in hybridized interlayer bands. Here, we report experimental and theoretical studies of WSe$_2$ homobilayers obtained in two stable configurations of 2H ($60^\circ$ twist) and 3R ($0^\circ$ twist) stackings by controlled chemical vapor synthesis of high-quality large-area crystals. Using optical absorption and photoluminescence spectroscopy at cryogenic temper…
Monolayer transition metal dichalcogenides are a promising platform to investigate many-body interactions of excitonic complexes. In monolayer tungsten diselenide, the ground-state exciton is dark (spin-indirect), and the valley degeneracy allows low-energy dark momentum-indirect excitons to form. Interactions between the dark exciton species and the optically accessible bright exciton (X) are likely to play significant roles in determining the optical properties of X at high power, as well as limiting the ultimate exciton densities that can be achieved, yet so far little is known about these …
The predicted formation of moire superlattices leading to confined excitonic states in heterostructures formed by stacking two lattice mismatched transition metal dichalcogenide (TMD) monolayers was recently experimentally confirmed. Such periodic potential in TMD heterostructure functions as a diffusion barrier that affects the energy transport and dynamics of interlayer excitons (electron and hole spatially concentrated in different monolayers). Understanding the transport of excitons under such condition is essential to establish the material system as a next generation device platform. In …
Layer-Dependent Interfacial Coupling and Exciton Pinning in WSe2/Graphene Heterostructures
Empa – Swiss Federal Laboratories for Materials Science and Technology（瑞士联邦材料科技研究所）；University of Basel（巴塞尔大学）；Swiss Nanoscience Institute, University of Basel（巴塞尔大学瑞士纳米科学研究所）；The Pennsylvania State University（宾夕法尼亚州立大学）
