An official website of the United States government
Abstract The removal of heavy metal contaminants from water is important for public health, and recently many two-dimensional (2D) materials with high specific surface areas are being studied as promising new active components in water purification. In particular, 2D MoS2nanosheets have been used for the removal of various heavy metals, but usually in either in complex geometries and composites, or in the chemically exfoliated metallic 1T-MoS2phase. However, the interaction of heavy metals dissolved in water with unmodified semiconducting 2H-MoS2is not well studied. In this paper, we report a detailed fundamental investigation of how Pb2+ions interact with 2H-MoS2. We observe small solid clusters that form on the MoS2surfaces after exposing them to Pb(NO3)2aqueous solutions as shown by atomic force microscopy and transmission electron microscopy, and for liquid phase exfoliated MoS2we observe the nanosheets precipitating out of dispersion along with insoluble solid granules. We use a combination of x-ray photoelectron spectroscopy and x-ray diffraction to identify these solid clusters and granules as primarily PbSO4with some PbMoO4. We put forth an interaction mechanism that involves MoS2defects acting as initiation sites for the partial dissolution in aqueous oxygenated conditions which produces MoO42−and SO42−ions to form the solids with Pb2+. These results are an important contribution to our fundamental understanding of how MoS2interacts with metal ions and will influence further efforts to exploit MoS2for water remediation applications.
more »
« less
Probing phonon focusing, thermomechanical behavior, and moiré patterns in van der Waals architectures using surface acoustic waves
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
- Award ID(s):
- 2240407
- PAR ID:
- 10518627
- Publisher / Repository:
- Nature Publishing Group
- Date Published:
- Journal Name:
- npj Computational Materials
- Volume:
- 10
- Issue:
- 1
- ISSN:
- 2057-3960
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Surface acoustic waves (SAWs) that propagate on the surface of a solid at MHz frequencies are widely used in sensing, communication, and acoustic tweezers. However, their properties are difficult to be tuned electrically, and current devices suffer from complicated configurations, complicated tuning mechanisms, or small ranges of tunability. Here a structure featuring a thin‐film transistor configuration is proposed to achieve electrically tunable SAW propagation based on conductivity tuning. When a DC gate voltage is applied, the on‐site conductivity of the piezoelectric substrate is modulated, which leads to velocity and amplitude tuning of SAWs. The use of carbon nanotubes and crystalline nanocellulose as the channel and gate materials results in high tuning capacity and low gate voltage requirement. The tunability is manifested by a 2.5% phase velocity tuning and near 10 dB on/off switching of the signals. The proposed device holds the potential for the next generation SAW‐based devices.more » « less
-
Abstract Realizing stimulated emission from defects in 2D‐layered semiconductors has the potential to enhance the sensitivity of characterizing their defects. However, stimulated emission from defects in layered materials presents a different set of challenges in carrier lifetime and energy level design and is not achieved so far. Here, photoluminescence (PL) spectroscopy, Raman spectroscopy, and first‐principles theory are combined to reveal an anomalous PL intensity–temperature relation and strong polarization effects at a defect emission peak in annealed multilayer MoS2, suggesting defect‐based stimulated emission. The emergence of stimulated emission behavior is also controllable (by temperature) and reversible. The observed stimulated emission behavior is supported by a three‐level system involving two defect levels from chalcogen vacancies and a pump level from the conduction band edge. First‐principles calculations show that the special indirect gap that enables stimulated emission is not native to pristine bulk MoS2and only emerges under thermal strain.more » « less
-
Abstract Two-dimensional (2D) materials have garnered significant attention in recent years due to their atomically thin structure and unique electronic and optoelectronic properties. To harness their full potential for applications in next-generation electronics and photonics, precise control over the dielectric environment surrounding the 2D material is critical. The lack of nucleation sites on 2D surfaces to form thin, uniform dielectric layers often leads to interfacial defects that degrade the device performance, posing a major roadblock in the realization of 2D-based devices. Here, we demonstrate a wafer-scale, low-temperature process (<250 °C) using atomic layer deposition (ALD) for the synthesis of uniform, conformal amorphous boron nitride (aBN) thin films. ALD deposition temperatures between 125 and 250 °C result in stoichiometric films with high oxidative stability, yielding a dielectric strength of 8.2 MV/cm. Utilizing a seed-free ALD approach, we form uniform aBN dielectric layers on 2D surfaces and fabricate multiple quantum well structures of aBN/MoS2and aBN-encapsulated double-gated monolayer (ML) MoS2field-effect transistors to evaluate the impact of aBN dielectric environment on MoS2optoelectronic and electronic properties. Our work in scalable aBN dielectric integration paves a way towards realizing the theoretical performance of 2D materials for next-generation electronics.more » « less
-
null (Ed.)Abstract Piezoelectric surface acoustic waves (SAWs) are powerful for investigating and controlling elementary and collective excitations in condensed matter. In semiconductor two-dimensional electron systems SAWs have been used to reveal the spatial and temporal structure of electronic states, produce quantized charge pumping, and transfer quantum information. In contrast to semiconductors, electrons trapped above the surface of superfluid helium form an ultra-high mobility, two-dimensional electron system home to strongly-interacting Coulomb liquid and solid states, which exhibit non-trivial spatial structure and temporal dynamics prime for SAW-based experiments. Here we report on the coupling of electrons on helium to an evanescent piezoelectric SAW. We demonstrate precision acoustoelectric transport of as little as ~0.01% of the electrons, opening the door to future quantized charge pumping experiments. We also show SAWs are a route to investigating the high-frequency dynamical response, and relaxational processes, of collective excitations of the electronic liquid and solid phases of electrons on helium.more » « less
