Atomically thin two-dimensional (2D) materials face significant energy barriers for synthesis and processing into functional metastable phases such as Janus structures. Here, the controllable implantation of hyperthermal species from pulsed laser deposition (PLD) plasmas is introduced as a top-down method to compositionally engineer 2D monolayers. The kinetic energies of Se clusters impinging on suspended monolayer WS2 crystals were controlled in the <10 eV/atom range with in situ plasma diagnostics to determine the thresholds for selective top layer replacement of sulfur by selenium for the formation of high quality WSSe Janus monolayers at low (300 °C) temperatures and bottom layer replacement for complete conversion to WSe2. Atomic-resolution electron microscopy and spectroscopy in tilted geometry confirm the WSSe Janus monolayer. Molecular dynamics simulations reveal that Se clusters implant to form disordered metastable alloy regions, which then recrystallize to form highly ordered structures, demonstrating low-energy implantation by PLD for the synthesis of 2D Janus layers and alloys of variable composition.
We report here details of steady-state and time-resolved spectroscopy of excitonic dynamics for Janus transition metal dichalcogenide monolayers, including MoSSe and WSSe, which were synthesized by low-energy implantation of Se into transition metal disulfides. Absorbance and photoluminescence spectroscopic measurements determined the room-temperature exciton resonances for MoSSe and WSSe monolayers. Transient absorption measurements revealed that the excitons in Janus structures form faster than those in pristine transition metal dichalcogenides by about 30% due to their enhanced electron−phonon interaction by the built-in dipole moment. By combining steady-state photoluminescence quantum yield and time-resolved transient absorption measurements, we find that the exciton radiative recombination lifetime in Janus structures is significantly longer than in their pristine samples, supporting the predicted spatial separation of the electron and hole wave functions due to the built-in dipole moment. These results provide fundamental insight in the optical properties of Janus transition metal dichalcogenides.
Two‐dimensional (2D) palladium diselenide (PdSe2) has strong interlayer coupling and a puckered pentagonal structure, leading to remarkable layer‐dependent electronic structures and highly anisotropic in‐plane optical and electronic properties. However, the lack of high‐quality, 2D PdSe2 crystals grown by bottom‐up approaches limits the study of their exotic properties and practical applications. In this work, chemical vapor deposition growth of highly crystalline few‐layer (≥2 layers) PdSe2 crystals on various substrates is reported. The high quality of the PdSe2 crystals is confirmed by low‐frequency Raman spectroscopy, scanning transmission electron microscopy, and electrical characterization. In addition, strong in‐plane optical anisotropy is demonstrated via polarized Raman spectroscopy and second‐harmonic generation maps of the PdSe2 flakes. A theoretical model based on kinetic Wulff construction theory and density functional theory calculations is developed and described the observed evolution of “square‐like” shaped PdSe2 crystals into rhombus due to the higher nucleation barriers for stable attachment on the (1,1) and (1,−1) edges, which results in their slower growth rates. Few‐layer PdSe2 field‐effect transistors reveal tunable ambipolar charge carrier conduction with an electron mobility up to ≈294 cm2 V−1 s−1, which is comparable to that of exfoliated PdSe2, indicating the promise of this anisotropic 2D material for electronics.
The unique optical properties of surface plasmon resonances in nanostructured materials have attracted considerable attention, broadly impacting both fundamental research and applied technologies ranging from sensing and optoelectronics to quantum computing. Electron energy-loss spectroscopy (EELS) in the transmission electron microscope has revealed valuable information about the full plasmonic spectrum of these materials with nanoscale spatial resolution. Here we report a novel approach for experimentally accessing the photon-stimulated electron energy-gain and stimulated electron energy-loss responses of individual plasmonic nanoparticles via the simultaneous irradiation of a continuous wave laser and continuous current, monochromated electron probe. Stimulated gain and loss probabilities are equivalent and increase linearly in the low-irradiance range of 0.5 × 108 to 4 × 108 W/m2, above which excessive heating reduces the observed probabilities; importantly in our low-irradiance regime, the photon energy must be tuned in resonance with the plasmon energy for the stimulated gain and loss peaks to emerge. Theoretical modeling based on Fermi’s golden rule elucidates how the plasmon resonantly and coherently shuttles energy quanta between the electron probe and the radiation field and vice versa in stimulated electron energy-loss and -gain events. This study opens a fundamentally new approach to explore the quantum physics of excited-state plasmon resonances that does not rely on high-intensity laser pulses or any modification to the EELS detector.
A new optical delivery system has been developed for the (scanning) transmission electron microscope. Here we describe the in situ and “rapid ex situ” photothermal heating modality of the system, which delivers >200 mW of optical power from a fiber-coupled laser diode to a 3.7 μm radius spot on the sample. Selected thermal pathways can be accessed via judicious choices of the laser power, pulse width, number of pulses, and radial position. The long optical working distance mitigates any charging artifacts and tremendous thermal stability is observed in both pulsed and continuous wave conditions, notably, no drift correction is applied in any experiment. To demonstrate the optical delivery system’s capability, we explore the recrystallization, grain growth, phase separation, and solid state dewetting of a Ag0.5Ni0.5 film. Finally, we demonstrate that the structural and chemical aspects of the resulting dewetted films was assessed.
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