An official website of the United States government
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
Dimensionality and Anisotropicity Dependence of Radiative Recombination in Nanostructured Phosphorene
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
- Award ID(s):
- 1760260
- PAR ID:
- 10096999
- Date Published:
- Journal Name:
- Journal of Materials Chemistry C
- ISSN:
- 2050-7526
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
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.more » « less
-
One-dimensional (1D) van der Waals materials have emerged as an intriguing playground to explore novel electronic and optical effects. We report on inorganic one-dimensional SbPS4 nanotube bundles obtained via mechanical exfoliation from bulk crystals. The ability to mechanically exfoliate SbPS4 nanobundles offers the possibility of applying modern 2D material fabrication techniques to create mixed-dimensional van der Waals heterostructures. We find that SbPS4 can readily be exfoliated to yield long (>10 μm) nanobundles with thicknesses that range from 1.3 to 200 nm. We investigated the optical response of semiconducting SbPS4 nanobundles and discovered that upon excitation with blue light, they emit bright and ultra-broadband red light with a quantum yield similar to that of hBN-encapsulated MoSe2. We discovered that the ultra-broadband red light emission is a result of a large ∼1 eV exciton binding energy and a ∼200 meV exciton self-trapping energy, unprecedented in previous material studies. Due to the bright and ultra-broadband light emission, we believe that this class of inorganic 1D van der Waals semiconductors has numerous potential applications, including on-chip tunable nanolasers, and applications that require ultraviolet to visible light conversion, such as lighting and sensing. Overall, our findings open avenues for harnessing the unique characteristics of these nanomaterials, advancing both fundamental research and practical optoelectronic applications.<more » « less
-
Topological photonics allows for the deterministic creation of electromagnetic modes of any dimensionality lesser than that of the system. In the context of two-dimensional systems such as metasurfaces, topological photonics enables trapping of light in 0D cavities defined by boundaries of higher-order topological insulators and topological defects, as well as guiding of optical fields along 1D boundaries between topologically distinct domains. More importantly, it allows engineering interactions of topological modes with radiative continuum, which opens new opportunities to control light-matter interactions, scattering, generation, and emission of light. This review article aims at highlighting recent work in the field focusing on the control of radiation and generation of light in topological metasurfaces.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
- Free Publicly Accessible Full Text
-
Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1039/C9TC02214G
