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  1. Abstract

    Group IV‐VI van der Waals crystals (MX, where M = Ge, Sn, and X = S, Se) are receiving increasing attention as semiconducting thermoelectric materials with nontoxic, earth‐abundant composition. Among them, SnSe is considered the most promising as it exhibits a remarkably high thermoelectric figure of merit (ZT), initially attributed to its low lattice thermal conductivity. However, it has been shown that the electronic band structure plays an equally important role in thermoelectric performance. A certain band shape, described as a “pudding mold” and characteristic for all MXs, has been predicted to significantly improveZTby combining good electrical conductivity with high Seebeck coefficient. This subtle feature is explored experimentally for GeS, SnS, and SnSe by means of angle‐resolved photoemission spectroscopy. The technique also allows for the determination of the effective mass and Fermi level position of as‐grown undoped crystals. The findings are supported by ab initio calculations of the electronic band structure. The results greatly contribute to the general understanding of the valence band dispersion of MXs and reinforce their potential as high‐performance thermoelectric materials, additionally giving prospects for designing systems consisting of van der Waals heterostructures.

     
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    Free, publicly-accessible full text available February 1, 2025
  2. Abstract

    Moiré superlattices of semiconducting transition metal dichalcogenides enable unprecedented spatial control of electron wavefunctions, leading to emerging quantum states. The breaking of translational symmetry further introduces a new degree of freedom: high symmetry moiré sites of energy minima behaving as spatially separated quantum dots. We demonstrate the superposition between two moiré sites by constructing a trilayer WSe2/monolayer WS2moiré heterojunction. The two moiré sites in the first layer WSe2interfacing WS2allow the formation of two different interlayer excitons, with the hole residing in either moiré site of the first layer WSe2and the electron in the third layer WSe2. An electric field can drive the hybridization of either of the interlayer excitons with the intralayer excitons in the third WSe2layer, realizing the continuous tuning of interlayer exciton hopping between two moiré sites and a superposition of the two interlayer excitons, distinctively different from the natural trilayer WSe2.

     
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  3. Abstract

    This paper provides comprehensive experimental analysis relating to improvements in the two-dimensional (2D) p-type metal–oxide–semiconductor (PMOS) field effect transistors (FETs) by pure van der Waals (vdW) contacts on few-layer tungsten diselenide (WSe2) with high-k metal gate (HKMG) stacks. Our analysis shows that standard metallization techniques (e.g., e-beam evaporation at moderate pressure ~ 10–5 torr) results in significant Fermi-level pinning, but Schottky barrier heights (SBH) remain small (< 100 meV) when using high work function metals (e.g., Pt or Pd). Temperature-dependent analysis uncovers a more dominant contribution to contact resistance from the channel access region and confirms significant improvement through less damaging metallization techniques (i.e., reduced scattering) combined with strongly scaled HKMG stacks (enhanced carrier density). A clean contact/channel interface is achieved through high-vacuum evaporation and temperature-controlled stepped deposition providing large improvements in contact resistance. Our study reports low contact resistance of 5.7 kΩ-µm, with on-state currents of ~ 97 µA/µm and subthreshold swing of ~ 140 mV/dec in FETs with channel lengths of 400 nm. Furthermore, theoretical analysis using a Landauer transport ballistic model for WSe2SB-FETs elucidates the prospects of nanoscale 2D PMOS FETs indicating high-performance (excellent on-state current vs subthreshold swing benchmarks) towards the ultimate CMOS scaling limit.

     
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  4. Abstract

    2D Janus transition metal dichalcogenides (TMDs) have attracted attention due to their emergent properties arising from broken mirror symmetry and self‐driven polarization fields. While it has been proposed that their vdW superlattices hold the key to achieving superior properties in piezoelectricity and photovoltaic, available synthesis has ultimately limited their realization. Here, the first packed vdW nanoscrolls made from Janus TMDs through a simple one‐drop solution technique are reported. The results, including ab initio simulations, show that the Bohr radius difference between the top sulfur and the bottom selenium atoms within Janus (M = Mo, W) results in a permanent compressive surface strain that acts as a nanoscroll formation catalyst after small liquid interaction. Unlike classical 2D layers, the surface strain in Janus TMDs can be engineered from compressive to tensile by placing larger Bohr radius atoms on top (to yield inverted C scrolls. Detailed microscopy studies offer the first insights into their morphology and readily formed Moiré lattices. In contrast, spectroscopy and FETs studies establish their excitonic and device properties and highlight significant differences compared to 2D flat Janus TMDs. These results introduce the first polar Janus TMD nanoscrolls and introduce inherent strain‐driven scrolling dynamics as a catalyst to create superlattices.

     
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  5. Abstract

    Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long‐lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, second and third harmonic generation in MoSSe and WSSe Janus monolayers is studied. Polarization‐resolved spectroscopy is used to map the full second‐order susceptibility tensor of MoSSe, including its out‐of‐plane components. In addition, the effective third‐order susceptibility and the second‐order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe are measured at room and cryogenic temperatures. This work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next‐generation on‐chip multifaceted photonic devices.

     
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  6. Abstract

    Named after the two‐faced Roman god of transitions, transition metal dichalcogenide (TMD) Janus monolayers have two different chalcogen surfaces, inherently breaking the out‐of‐plane mirror symmetry. The broken mirror symmetry and the resulting potential gradient lead to the emergence of quantum properties such as the Rashba effect and the formation of dipolar excitons. Experimental access to these quantum properties, however, hinges on the ability to produce high‐quality 2D Janus monolayers. Here, these results introduce a holistic 2D Janus synthesis technique that allows real‐time monitoring of the growth process. This prototype chamber integrates in situ spectroscopy, offering fundamental insights into the structural evolution and growth kinetics, that allow the evaluation and optimization of the quality of Janus monolayers. The versatility of this method is demonstrated by synthesizing and monitoring the conversion of SWSe, SNbSe, and SMoSe Janus monolayers. Deterministic conversion and real‐time data collection further aid in conversion of exfoliated TMDs to Janus monolayers and unparalleled exciton linewidth values are reached, compared to the current best standard. The results offer an insight into the process kinetics and aid in the development of new Janus monolayers with high optical quality, which is much needed to access their exotic properties.

     
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  7. Nitrogen doped lutetium hydride has drawn global attention in the pursuit of room-temperature superconductivity near ambient pressure and temperature. However, variable synthesis techniques and uncertainty surrounding nitrogen concentration have contributed to extensive debate within the scientific community about this material and its properties. We used a solid-state approach to synthesize nitrogen doped lutetium hydride at high pressure and temperature (HPT) and analyzed the residual starting materials to determine its nitrogen content. High temperature oxide melt solution calorimetry determined the formation enthalpy of LuH1.96N0.02(LHN) from LuH2and LuN to be −28.4 ± 11.4 kJ/mol. Magnetic measurements indicated diamagnetism which increased with nitrogen content. Ambient pressure conductivity measurements observed metallic behavior from 5 to 350 K, and the constant and parabolic magnetoresistance changed with increasing temperature. High pressure conductivity measurements revealed that LHN does not exhibit superconductivity up to 26.6 GPa. We compressed LHN in a diamond anvil cell to 13.7 GPa and measured the Raman signal at each step, with no evidence of any phase transition. Despite the absence of superconductivity, a color change from blue to purple to red was observed with increasing pressure. Thus, our findings confirm the thermodynamic stability of LHN, do not support superconductivity, and provide insights into the origins of its diamagnetism.

     
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    Free, publicly-accessible full text available March 19, 2025
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  10. Free, publicly-accessible full text available January 1, 2025