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Monolayers of Ti3C2Tx MXene and bilayer structures formed by partially overlapping monolayer flakes exhibit opposite sensing responses to a large scope of molecular analytes. When exposed to reducing analytes, monolayer MXene flakes show increased electrical conductivity, i.e., an n-type behavior, while bilayer structures become less conductive, exhibiting a p-type behavior. On the contrary, both monolayers and bilayers show unidirectional sensing responses with increased resistivity when exposed to oxidizing analytes. The sensing responses of Ti3C2Tx monolayers and bilayers are dominated by entirely different mechanisms. The sensing behavior of MXene monolayers is dictated by the charge transfer from adsorbed molecules and the response direction is consistent with the donor/acceptor properties of the analyte and the intrinsic n-type character of Ti3C2Tx. In contrast, the bilayer MXene structures always show the same response regardless of the donor/acceptor character of the analyte, and the resistivity always increases because of the intercalation of molecules between the Ti3C2Tx layers. This study explains the sensing behavior of bulk MXene sensors based on multiflake assemblies, in which this intercalation mechanism results in universal increase in resistance that for many analytes is seemingly inconsistent with the n-type character of the material. By scaling MXene sensors down from multiflake to single-flake level, we disentangled the charge transfer and intercalation effects and unraveled their contributions. In particular, we show that the charge transfer has a much faster kinetics than the intercalation process. Finally, we demonstrate that the layer-dependent gas sensing properties of MXenes can be employed for the design of sensor devices with enhanced molecular recognition. 

We report the modification of a gas phase ultrafast electron diffraction (UED) instrument that enables experiments with both gas and condensed matter targets, where a time-resolved experiment with sub-picosecond resolution is demonstrated with solid state samples. The instrument relies on a hybrid DC-RF acceleration structure to deliver femtosecond electron pulses on the target, which is synchronized with femtosecond laser pulses. The laser pulses and electron pulses are used to excite the sample and to probe the structural dynamics, respectively. The new system is added with capabilities to perform transmission UED on thin solid samples. It allows for cooling samples to cryogenic temperatures and to carry out time-resolved measurements. We tested the cooling capability by recording diffraction patterns of temperature dependent charge density waves in 1T-TaS2. The time-resolved capability is experimentally verified by capturing the dynamics in photoexcited single-crystal gold. 

Few-layered HfS₃nanoribbons exhibit n-type conductivity and a large photoresponse to visible light. The photocurrent strongly depends on the polarization direction of the excitation laser due to the highly anisotropic quasi-1D crystal structure of HfS₃. 

X-ray photoemission spectroscopy (XPS) has been used to examine the interaction between Au and HfS 3 at the Au/HfS 3 interface. XPS measurements reveal dissociative chemisorption of O 2 , leading to the formation of an oxide of Hf at the surface of HfS 3 . This surface hafnium oxide, along with the weakly chemisorbed molecular species, such as O 2 and H 2 O, are likely responsible for the observed p-type characteristics of HfS 3 reported elsewhere. HfS 3 devices exhibit n-type behaviour if measured in vacuum but turn p-type in air. Au thickness-dependent XPS measurements provide clear evidence of band bending as the S 2p and Hf 4f core-level peak binding energies for Au/HfS 3 are found to be shifted to higher binding energies. This band bending implies formation of a Schottky-barrier at the Au/HfS 3 interface, which explains the low measured charge carrier mobilities of HfS 3 -based devices. The transistor measurements presented herein also indicate the existence of a Schottky barrier, consistent with the XPS core-level binding energy shifts, and show that the bulk of HfS 3 is n-type. 

Abstract One of the exceptional features of the van der Waals (vdW) ferroelectrics is the existence of stable polarization at a level of atomically thin monolayers. This ability to withstand a detrimental effect of the depolarization fields gives rise to complex domain configurations characterized, among others, by the presence of layered “antipolar” head‐to‐head (H‐H) or tail‐to‐tail (T‐T) dipole arrangements. In this study, tomographic piezoresponse force microscopy (TPFM) is employed to study the 3D polarization arrangement in vdW ferroelectricα‐In₂Se₃. Sequential removal of thin layers from the polar surface using the PFM tip reveals a complex 3D profile of the domain walls in theα‐In₂Se₃crystals. Antiparallel domain layers stacked along the polar direction are also observed by PFM imaging of the non‐polar surfaces showing that H‐H and T‐T domain boundaries are commonly present inα‐In₂Se₃. Application of TPFM to the electrically written domains allows evaluation of their geometrical lateral‐to‐vertical size aspect ratio, which shows a strong prevalence for the sidewise expansion in comparison to the forward growth. LocalI–Vmeasurements reveal a strong polarization direction dependence of conductivity due to the modulation of the energy barrier height as corroborated by theoretical modeling.