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.
Excitons are elementary optical excitation in semiconductors. The ability to manipulate and transport these quasiparticles would enable excitonic circuits and devices for quantum photonic technologies. Recently, interlayer excitons in 2D semiconductors have emerged as a promising candidate for engineering excitonic devices due to their long lifetime, large exciton binding energy, and gate tunability. However, the charge-neutral nature of the excitons leads to weak response to the in-plane electric field and thus inhibits transport beyond the diffusion length. Here, we demonstrate the directional transport of interlayer excitons in bilayer WSe2driven by the propagating potential traps induced by surface acoustic waves (SAW). We show that at 100 K, the SAW-driven excitonic transport is activated above a threshold acoustic power and reaches 20 μm, a distance at least ten times longer than the diffusion length and only limited by the device size. Temperature-dependent measurement reveals the transition from the diffusion-limited regime at low temperature to the acoustic field-driven regime at elevated temperature. Our work shows that acoustic waves are an effective, contact-free means to control exciton dynamics and transport, promising for realizing 2D materials-based excitonic devices such as exciton transistors, switches, and transducers up to room temperature.
- Publication Date:
- NSF-PAR ID:
- 10381714
- Journal Name:
- Nature Communications
- Volume:
- 13
- Issue:
- 1
- ISSN:
- 2041-1723
- Publisher:
- Nature Publishing Group
- Sponsoring Org:
- National Science Foundation
More Like this
-
Abstract -
Strong interactions between excitons are a characteristic feature of two-dimensional (2D) semiconductors, determining important excitonic properties, such as exciton lifetime, coherence, and photon-emission efficiency. Rhenium disulfide (ReS2), a member of the 2D transition-metal dichalcogenide (TMD) family, has recently attracted great attention due to its unique excitons that exhibit excellent polarization selectivity and coherence features. However, an in-depth understanding of exciton-exciton interactions in ReS2 is still lacking. Here we used ultrafast pump-probe spectroscopy to study exciton-exciton interactions in monolayer (1L), bilayer (2L), and triple layer ReS2. We directly measure the rate of exciton-exciton annihilation, a representative Auger-type interaction between excitons. It decreases with increasing layer number, as observed in other 2D TMDs. However, while other TMDs exhibit a sharp weakening of exciton-exciton annihilation between 1L and 2L, such behavior was not observed in ReS2. We attribute this distinct feature in ReS2 to the relatively weak interlayer coupling, which prohibits a substantial change in the electronic structure when the thickness varies. This work not only highlights the unique excitonic properties of ReS2 but also provides novel insight into the thickness dependence of exciton-exciton interactions in 2D systems.
-
Due to their atomic thinness with reduced dielectric screening, two-dimensional materials can possess a stable excitonic population at room temperature. This is attractive for future excitonic devices, where excitons are used to carry energy or information. In excitonic devices, controlling transport of the charge-neutral excitons is a key element. Here we show that exciton transport in a MoSe 2 monolayer semiconductor can be effectively controlled by dielectric screening. A MoSe 2 monolayer was partially covered with a hexagonal boron nitride flake. Photoluminescence measurements showed that the exciton energy in the covered region is about 12 meV higher than that in the uncovered region. Spatiotemporally resolved differential reflection measurements performed at the junction between the two regions revealed that this energy offset is sufficient to drive excitons across the junction for about 50 ps over a distance of about 200 nm. These results illustrate the feasibility of using van der Waals dielectric engineering to control exciton transport and contribute to understanding the effects of the dielectric environment on the electronic and optical properties of two-dimensional semiconductors.
-
Abstract Excitons are spin integer particles that are predicted to condense into a coherent quantum state at sufficiently low temperature. Here by using photocurrent imaging we report experimental evidence of formation and efficient transport of non-equilibrium excitons in Bi2-xSbxSe3nanoribbons. The photocurrent distributions are independent of electric field, indicating that photoexcited electrons and holes form excitons. Remarkably, these excitons can transport over hundreds of micrometers along the topological insulator (TI) nanoribbons before recombination at up to 40 K. The macroscopic transport distance, combined with short carrier lifetime obtained from transient photocurrent measurements, indicates an exciton diffusion coefficient at least 36 m2 s−1, which corresponds to a mobility of 6 × 104 m2 V−1 s−1at 7 K and is four order of magnitude higher than the value reported for free carriers in TIs. The observation of highly dissipationless exciton transport implies the formation of superfluid-like exciton condensate at the surface of TIs.
-
Strain engineering is a powerful tool in designing artificial platforms for high-temperature excitonic quantum devices. Combining strong light-matter interaction with robust and mobile exciton quasiparticles, two-dimensional transition metal dichalcogenides (2D TMDCs) hold great promise in this endeavor. However, realizing complex excitonic architectures based on strain-induced electronic potentials alone has proven to be exceptionally difficult so far. Here, we demonstrate deterministic strain engineering of both single-particle electronic bandstructure and excitonic many-particle interactions. We create quasi-1D transport channels to confine excitons and simultaneously enhance their mobility through locally suppressed exciton-phonon scattering. Using ultrafast, all-optical injection and time-resolved readout, we realize highly directional exciton flow with up to 100% anisotropy both at cryogenic and room temperatures. The demonstrated fundamental modification of the exciton transport properties in a deterministically strained 2D material with effectively tunable dimensionality has broad implications for both basic solid-state science and emerging technologies.
