skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Transient Nanoscopy of Exciton Dynamics in 2D Transition Metal Dichalcogenides
Abstract The electronic and optical properties of 2D transition metal dichalcogenides are dominated by strong excitonic resonances. Exciton dynamics plays a critical role in the functionality and performance of many miniaturized 2D optoelectronic devices; however, the measurement of nanoscale excitonic behaviors remains challenging. Here, a near‐field transient nanoscopy is reported to probe exciton dynamics beyond the diffraction limit. Exciton recombination and exciton–exciton annihilation processes in monolayer and bilayer MoS2are studied as the proof‐of‐concept demonstration. Moreover, with the capability to access local sites, intriguing exciton dynamics near the monolayer‐bilayer interface and at the MoS2nano‐wrinkles are resolved. Such nanoscale resolution highlights the potential of this transient nanoscopy for fundamental investigation of exciton physics and further optimization of functional devices.  more » « less
Award ID(s):
2238691 2005194
PAR ID:
10514855
Author(s) / Creator(s):
; ; ; ; ; ;
Publisher / Repository:
Wiley
Date Published:
Journal Name:
Advanced Materials
Volume:
36
Issue:
21
ISSN:
0935-9648
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Tightly bound electron-hole pairs (excitons) hosted in atomically-thin semiconductors have emerged as prospective elements in optoelectronic devices for ultrafast and secured information transfer. The controlled exciton transport in such excitonic devices requires manipulating potential energy gradient of charge-neutral excitons, while electrical gating or nanoscale straining have shown limited efficiency of exciton transport at room temperature. Here, we report strain gradient induced exciton transport in monolayer tungsten diselenide (WSe2) across microns at room temperature via steady-state pump-probe measurement. Wrinkle architecture enabled optically-resolvable local strain (2.4%) and energy gradient (49 meV/μm) to WSe2. We observed strain gradient induced flux of high-energy excitons and emission of funneled, low-energy excitons at the 2.5 μm-away pump point with nearly 45% of relative emission intensity compared to that of excited excitons. Our results strongly support the strain-driven manipulation of exciton funneling in two-dimensional semiconductors at room temperature, opening up future opportunities of 2D straintronic exciton devices. 
    more » « less
  2. Understanding excitonic dynamics in two-dimensional semiconducting transition metal dichalcogenides is important for developing their optoelectronic applications. Recently, transient absorption techniques based on resonant excitonic absorption have been used to study various aspects of excitonic dynamics in these materials. The transient absorption in such measurements originates from phase-space state filling, bandgap renormalization, or screening effects. Here we report a new method to probe excitonic dynamics based on exciton intraband absorption. In this Drude-like process, probe photons are absorbed by excitons in their intraband excitation to higher energy states, causing a transient absorption signal. Although the magnitude of the transient absorption is lower than that of the resonant techniques, the new method is less restrictive on the selection of probe wavelength, has a larger linear range, and can provide complementary information on photocarrier dynamics. Using the WS 2 monolayer and bulk samples as examples, we show that the new method can probe exciton–exciton annihilation at high densities and reveal exciton formation processes. We also found that the exciton intraband absorption cross section of the WS 2 monolayer is on the order of 10 −18 cm 2 . 
    more » « less
  3. Abstract Source/Drain extension doping is crucial for minimizing the series resistance of the ungated channel and reducing the contact resistance of field‐effect transistors (FETs) in complementary metal–oxide–semiconductor (CMOS) technology. 2D semiconductors, such as MoS2and WSe2, are promising channel materials for beyond‐silicon CMOS. A key challenge is to achieve extension doping for 2D monolayer FETs without damaging the atomically thin material. This work demonstrates extension doping with low‐resistance contacts for monolayer WSe2p‐FETs. Self‐limiting oxidation transforms a bilayer WSe2into a hetero‐bilayer of a high‐work‐function WOxSeyon a monolayer WSe2. Then, damage‐free nanolithography defines an undoped nano‐channel, preserving the high on‐current of WOxSey‐doped FETs while significantly improving their on/off ratio. The insertion of an amorphous WOxSeyinterlayer under the contacts achieves record‐low contact resistances for monolayer WSe2over a hole density range of 1012to 1013cm−2(1.2 ± 0.3 kΩ µm at 1013cm−2). The WOxSey‐doped extension exhibits a sheet resistance as low as 10 ± 1 kΩ □−1. Monolayer WSe2p‐FETs with sub‐50 nm channel lengths reach a maximum drain current of 154 µA µm−1with an on/off ratio of 107–108. These results define strategies for nanometer‐scale selective‐area doping in 2D FETs and other 2D architectures. 
    more » « less
  4. Abstract 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 WSe 2 driven 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. 
    more » « less
  5. Abstract Surface acoustic waves (SAWs) propagate along solid-air, solid-liquid, and solid-solid interfaces. Their characteristics depend on the elastic properties of the solid. Combining transmission electron microscopy (TEM) experiments with molecular dynamics (MD) simulations, we probe atomic environments around intrinsic defects that generate SAWs in vertically stacked two-dimensional (2D) bilayers of MoS2. Our joint experimental-simulation study provides insights into SAW-induced structural and dynamical changes and thermomechanical responses of MoS2bilayers. Using MD simulations, we compute mechanical properties from the SAW velocity and thermal conductivity from thermal diffusion of SAWs. The results for Young’s modulus and thermal conductivity of an MoS2monolayer are in good agreement with experiments. The presence of defects, such as nanopores which generate SAWs, reduces the thermal conductivity of 2D-MoS2by an order of magnitude. We also observe dramatic changes in moiré patterns, phonon focusing, and cuspidal structures on 2D-MoS2layers. 
    more » « less