Interlayer excitons were observed at the heterojunctions in van der Waals heterostructures (vdW HSs). However, it is not known how the excitonic phenomena are affected by the stacking order. Here, we report twist-angle-dependent interlayer excitons in MoSe/WSe vdW HSs based on photoluminescence (PL) and vdW-corrected density functional theory calculations. The PL intensity of the interlayer excitons depends primarily on the twist angle: It is enhanced at coherently stacked angles of 0° and 60° (owing to strong interlayer coupling) but disappears at incoherent intermediate angles. The calculations confirm twist-angle-dependent interlayer coupling: The states at the edges of the valence band exhibit a long tail that stretches over the other layer for coherently stacked angles; however, the states are largely confined in the respective layers for intermediate angles. This interlayer hybridization of the band edge states also correlates with the interlayer separation between MoSe and WSe layers. Furthermore, the interlayer coupling becomes insignificant, irrespective of twist angles, by the incorporation of a hexagonal boron nitride monolayer between MoSe and WSe.
Chemical transformation of existing two-dimensional (2D) materials can be crucial in further expanding the 2D crystal palette required to realize various functional heterostructures. In this work, we demonstrate a 2D 'on-stack' chemical conversion of single-layer crystalline MoS 2 into MoO 3 with a precise layer control that enables truly 2D MoO 3 and MoO 3 /MoS 2 heterostructures. To minimize perturbation of the 2D morphology, a nonthermal oxidation using O 2 plasma was employed. The early stage of the reaction was characterized by a defect-induced Raman peak, drastic quenching of photoluminescence (PL) signals and sub-nm protrusions in atomic force microscopy images. As the reaction proceeded from the uppermost layer to the buried layers, PL and optical second harmonic generation signals showed characteristic modulations revealing a layer-by-layer conversion. The plasma-generated 2D oxides, confirmed as MoO 3 by x-ray photoelectron spectroscopy, were found to be amorphous but extremely flat with a surface roughness of 0.18 nm, comparable to that of 1L MoS 2 . The rate of oxidation quantified by Raman spectroscopy decreased very rapidly for buried sulfide layers due to protection by the surface 2D oxides, exhibiting a pseudo-self-limiting behavior. As exemplified in this work, various on-stack chemical transformations can be applied to other 2D materials in forming otherwise unobtainable materials and complex heterostructures, thus expanding the palette of 2D material building blocks.
During Wallerian degeneration, Schwann cells lose their characteristic of myelinating axons and shift into the state of developmental promyelinating cells. This recharacterized Schwann cell guides newly regrowing axons to their destination and remyelinates reinnervated axons. This Schwann cell dynamics during Wallerian degeneration is associated with oxidative events. Heme oxygenases (HOs) are involved in the oxidative degradation of heme into biliverdin/bilirubin, ferrous iron, and carbon monoxide. Overproduction of ferrous iron by HOs increases reactive oxygen species, which have deleterious effects on living cells. Thus, the key molecule for understanding the exact mechanism of Wallerian degeneration in the peripheral nervous system is likely related to oxidative stress-mediated HOs in Schwann cells. In this study, we demonstrate that demyelinating Schwann cells during Wallerian degeneration highly express HO1, not HO2, and remyelinating Schwann cells during nerve regeneration decrease HO1 activation to levels similar to those in normal myelinating Schwann cells. In addition, HO1 activation during Wallerian degeneration regulates several critical phenotypes of recharacterized repair Schwann cells, such as demyelination, transdedifferentiation, and proliferation. Thus, these results suggest that oxidative stress in Schwann cells after peripheral nerve injury may be regulated by HO1 activation during Wallerian degeneration and oxidative-stress-related HO1 activation in Schwann cells may be helpful to study deeply molecular mechanism of Wallerian degeneration.
Understanding the nature of molecular excitons in low-dimensional molecular solids is of paramount importance in fundamental photophysics and various applications such as energy harvesting, switching electronics and display devices. Despite this, the spatial evolution of molecular excitons and their transition dipoles have not been captured in the precision of molecular length scales. Here we show in-plane and out-of-plane excitonic evolution in quasilayered two-dimensional (2D) perylene-3, 4, 9, 10-tetracarboxylic dianhydride (PTCDA) crystals assembly-grown on hexagonal boron nitride (hBN) crystals. Complete lattice constants with orientations of two herringbone-configured basis molecules are determined with polarization-resolved spectroscopy and electron diffraction methods. In the truly 2D limit of single layers, two Frenkel emissions Davydov-split by Kasha-type intralayer coupling exhibit energy inversion with decreasing temperature, which enhances excitonic coherence. As the thickness increases, the transition dipole moments of newly emerging charge transfer excitons are reoriented because of mixing with the Frenkel states. The current spatial anatomy of 2D molecular excitons will inspire a deeper understanding and groundbreaking applications of low-dimensional molecular systems.
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