An official website of the United States government
Vertically stacked van der Waals (vdW) heterostructures exhibit unique electronic, optical, and thermal properties that can be manipulated by twist-angle engineering. However, the weak phononic coupling at a bilayer interface imposes a fundamental thermal bottleneck for future two-dimensional devices. Using ultrafast electron diffraction, we directly investigated photoinduced nonequilibrium phonon dynamics in MoS2/WS2at 4° twist angle and WSe2/MoSe2heterobilayers with twist angles of 7°, 16°, and 25°. We identified an interlayer heat transfer channel with a characteristic timescale of ~20 picoseconds, about one order of magnitude faster than molecular dynamics simulations assuming initial intralayer thermalization. Atomistic calculations involving phonon-phonon scattering suggest that this process originates from the nonthermal phonon population following the initial interlayer charge transfer and scattering. Our findings present an avenue for thermal management in vdW heterostructures by tailoring nonequilibrium phonon populations.
more »
« less
This content will become publicly available on December 1, 2025
Observation of interlayer plasmon polaron in graphene/WS2 heterostructures
Abstract Harnessing electronic excitations involving coherent coupling to bosonic modes is essential for the design and control of emergent phenomena in quantum materials. In situations where charge carriers induce a lattice distortion due to the electron-phonon interaction, the conducting states get “dressed, which leads to the formation of polaronic quasiparticles. The exploration of polaronic effects on low-energy excitations is in its infancy in two-dimensional materials. Here, we present the discovery of an interlayer plasmon polaron in heterostructures composed of graphene on top of single-layer WS2. By using micro-focused angle-resolved photoemission spectroscopy during in situ doping of the top graphene layer, we observe a strong quasiparticle peak accompanied by several carrier density-dependent shake-off replicas around the single-layer WS2conduction band minimum. Our results are explained by an effective many-body model in terms of a coupling between single-layer WS2conduction electrons and an interlayer plasmon mode. It is important to take into account the presence of such interlayer collective modes, as they have profound consequences for the electronic and optical properties of heterostructures that are routinely explored in many device architectures involving 2D transition metal dichalcogenides.
more »
« less
- Award ID(s):
- 2011876
- PAR ID:
- 10582621
- Publisher / Repository:
- Nature
- Date Published:
- Journal Name:
- Nature Communications
- Volume:
- 15
- Issue:
- 1
- ISSN:
- 2041-1723
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Tunable Fano resonances and plasmon–exciton coupling are demonstrated at room temperature in hybrid systems consisting of single plasmonic nanoparticles deposited on top of the transition metal dichalcogenide monolayers. By using single Au nanotriangles (AuNTs) on monolayer WS2as model systems, Fano resonances are observed from the interference between a discrete exciton band of monolayer WS2and a broadband plasmonic mode of single AuNTs. The Fano lineshape depends on the exciton binding energy and the localized surface plasmon resonance strength, which can be tuned by the dielectric constant of surrounding solvents and AuNT size, respectively. Moreover, a transition from weak to strong plasmon–exciton coupling with Rabi splitting energies of 100–340 meV is observed by rationally changing the surrounding solvents. With their tunable plasmon–exciton interactions, the proposed WS2–AuNT hybrids can open new pathways to develop active nanophotonic devices.more » « less
-
We fabricated a van der Waals heterostructure of WS 2 –ReSe 2 and studied its charge-transfer properties. Monolayers of WS 2 and ReSe 2 were obtained by mechanical exfoliation and chemical vapor deposition, respectively. The heterostructure sample was fabricated by transferring the WS 2 monolayer on top of ReSe 2 by a dry transfer process. Photoluminescence quenching was observed in the heterostructure, indicating efficient interlayer charge transfer. Transient absorption measurements show that holes can efficiently transfer from WS 2 to ReSe 2 on an ultrafast timescale. Meanwhile, electron transfer from ReSe 2 to WS 2 was also observed. The charge-transfer properties show that monolayers of ReSe 2 and WS 2 form a type-II band alignment, instead of type-I as predicted by theory. The type-II alignment is further confirmed by the observation of extended photocarrier lifetimes in the heterostructure. These results provide useful information for developing van der Waals heterostructure involving ReSe 2 for novel electronic and optoelectronic applications and introduce ReSe 2 to the family of two-dimensional materials to construct van der Waals heterostructures.more » « less
-
Abstract Surface plasmons, collective electromagnetic excitations coupled to conduction electron oscillations, enable the manipulation of light–matter interactions at the nanoscale. Plasmon dispersion of metallic structures depends sensitively on their dimensionality and has been intensively studied for fundamental physics as well as applied technologies. Here, we report possible evidence for gate-tunable hybrid plasmons from the dimensionally mixed coupling between one-dimensional (1D) carbon nanotubes and two-dimensional (2D) graphene. In contrast to the carrier density-independent 1D Luttinger liquid plasmons in bare metallic carbon nanotubes, plasmon wavelengths in the 1D-2D heterostructure are modulated by 75% via electrostatic gating while retaining the high figures of merit of 1D plasmons. We propose a theoretical model to describe the electromagnetic interaction between plasmons in nanotubes and graphene, suggesting plasmon hybridization as a possible origin for the observed large plasmon modulation. The mixed-dimensional plasmonic heterostructures may enable diverse designs of tunable plasmonic nanodevices.more » « less
-
Abstract Nanohybrids based on van der Waals (vdW) heterostructures of two dimensional (2D) atomic materials have recently emerged as a unique scheme for designing high‐performance quantum sensors. This work explores vdW nanohybrids for photodetection, which consist of graphene decorated with intermingled transition‐metal dichalcogenide (TMDC) nanodiscs (TMDC‐NDs) obtained using wafer‐size, layer‐by‐layer growth. The obtained TMDC‐NDs/graphene nanohybrids take advantage of strong quantum confinement in graphene for high charge mobility and hence high photoconductive gain, and localized surface plasmonic resonance (LSPR) enabled on the TMDC‐NDs for enhanced light absorption. Since the LSPR depends on the nanostructure's size and density, intermingled TMDC‐NDs of different kinds of TMDCs, such as WS2(W) and MoS2(M), have been found to allow small‐size, high‐concentration TMDC‐NDs to be achieved for high photoresponse. Remarkably, high photoresponsivity up to 31 A/W (550 nm wavelength and 20 µW cm−2light intensity) has been obtained on the WMW‐NDs/graphene nanohybrids photodetectors made using three consecutive coatings of WS2(1st and 3rd coating) and MoS2(2nd coating), which is considerably higher by a factor of ≈4 than that of the counterparts MoS2‐ND/graphene or WS2‐NDs/graphene devices. This result provides a facile approach to control the size and concentration of the TMDC‐NDs for high‐performance, low‐cost optoelectronic device applications.more » « less
