An official website of the United States government
Abstract The ability to modulate optical and electrical properties of two-dimensional (2D) semiconductors has sparked considerable interest in transition metal dichalcogenides (TMDs). Herein, we introduce a facile strategy for modulating optoelectronic properties of monolayer MoSe2with external light. Photochromic diarylethene (DAE) molecules formed a 2-nm-thick uniform layer on MoSe2, switching between its closed- and open-form isomers under UV and visible irradiation, respectively. We have discovered that the closed DAE conformation under UV has its lowest unoccupied molecular orbital energy level lower than the conduction band minimum of MoSe2, which facilitates photoinduced charge separation at the hybrid interface and quenches photoluminescence (PL) from monolayer flakes. In contrast, open isomers under visible light prevent photoexcited electron transfer from MoSe2to DAE, thus retaining PL emission properties. Alternating UV and visible light repeatedly show a dynamic modulation of optoelectronic signatures of MoSe2. Conductive atomic force microscopy and Kelvin probe force microscopy also reveal an increase in conductivity and work function of MoSe2/DAE with photoswitched closed-form DAE. These results may open new opportunities for designing new phototransistors and other 2D optoelectronic devices.
more »
« less
This content will become publicly available on December 1, 2025
Confinement of excited states in two-dimensional, in-plane, quantum heterostructures
Abstract Two-dimensional (2D) semiconductors are promising candidates for optoelectronic application and quantum information processes due to their inherent out-of-plane 2D confinement. In addition, they offer the possibility of achieving low-dimensional in-plane exciton confinement, similar to zero-dimensional quantum dots, with intriguing optical and electronic properties via strain or composition engineering. However, realizing such laterally confined 2D monolayers and systematically controlling size-dependent optical properties remain significant challenges. Here, we report the observation of lateral confinement of excitons in epitaxially grown in-plane MoSe2quantum dots (~15-60 nm wide) inside a continuous matrix of WSe2monolayer film via a sequential epitaxial growth process. Various optical spectroscopy techniques reveal the size-dependent exciton confinement in the MoSe2monolayer quantum dots with exciton blue shift (12-40 meV) at a low temperature as compared to continuous monolayer MoSe2. Finally, single-photon emission (g2(0) ~ 0.4) was also observed from the smallest dots at 1.6 K. Our study opens the door to compositionally engineered, tunable, in-plane quantum light sources in 2D semiconductors.
more »
« less
- Award ID(s):
- 2039351
- PAR ID:
- 10584893
- Publisher / Repository:
- Springer 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
-
-
Establishing a coherent interaction between a material resonance and an optical cavity is a necessary first step to study semiconductor quantum optics. Here we report on the signature of a coherent interaction between a two-dimensional excitonic transition in monolayer MoSe2and a zero-dimensional, ultra-low mode volume (Vm ∼ 2(λ/n)3) on-chip photonic crystal nanocavity. This coherent interaction manifests as a dispersive shift of the cavity transmission spectrum, when the exciton-cavity detuning is decreased via temperature tuning. The exciton-cavity coupling is estimated to be ≈6.5 meV, with a cooperativity of ≈4.0 at 80 K, showing our material system is on the verge of strong coupling. The small mode-volume of the resonator is instrumental in reaching the strongly nonlinear regime, while on-chip cavities will help create a scalable quantum photonic platform.more » « less
-
The interplay between dimensionality and anisotropicity leads to intriguing optoelectronic properties and exciton dynamics in low dimensional semiconductors. In this study we use nanostructured phosphorene as a prototypical example to unfold such complex physics and develop a general first-principles framework to study exciton dynamics in low dimensional systems. Specifically we derived the radiative lifetime and light emission intensity from 2D to 0D systems based on many body perturbation theory, and investigated the dimensionality and anisotropicity effects on radiative recombination lifetime both at 0 K and finite temperature, as well as polarization and angle dependence of emitted light. We show that the radiative lifetime at 0 K increases by an order of 103 with the lowering of one dimension (i.e. from 2D to 1D nanoribbons or from 1D to 0D quantum dots). We also show that obtaining the radiative lifetime at finite temperature requires accurate exciton dispersion beyond the effective mass approximation. Finally, we demonstrate that monolayer phosphorene and its nanostructures always emit linearly polarized light consistent with experimental observations, different from in-plane isotropic 2D materials like MoS2 and h-BN that can emit light with arbitrary polarization, which may have important implications for quantum information applications.more » « less
-
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 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.more » « less
-
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.more » « less
