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1. The Impact of Parameterized Lateral Mixing on the Antarctic Circumpolar Current in a Coupled Climate Model

   https://doi.org/10.1175/JPO-D-19-0249.1  

   Ragen, Sarah ; Pradal, Marie-Aude ; Gnanadesikan, Anand ( April 2020 , Journal of Physical Oceanography)

   This study examines the impact of changing the lateral diffusion coefficient A_Redion the transport of the Antarctic Circumpolar Current (ACC). The lateral diffusion coefficient A_Rediis poorly constrained, with values ranging across an order of magnitude in climate models. The ACC is difficult to accurately simulate, and there is a large spread in eastward transport in the Southern Ocean (SO) in these models. This paper examines how much of that spread can be attributed to different eddy parameterization coefficients. A coarse-resolution, fully coupled model suite was run with A_Redi= 400, 800, 1200, and 2400 m²s⁻¹. Additionally, two simulations were run withmore »two-dimensional representations of the mixing coefficient based on satellite altimetry. Relative to the 400 m²s⁻¹case, the 2400 m²s⁻¹case exhibits 1) an 11% decrease in average wind stress from 50° to 65°S, 2) a 20% decrease in zonally averaged eastward transport in the SO, and 3) a 14% weaker transport through the Drake Passage. The decrease in transport is well explained by changes in the thermal current shear, largely due to increases in ocean density occurring on the northern side of the ACC. In intermediate waters these increases are associated with changes in the formation of intermediate waters in the North Pacific. We hypothesize that the deep increases are associated with changes in the wind stress curl allowing Antarctic Bottom Water to escape and flow northward.

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2. Exciton-polaron Rydberg states in monolayer MoSe2 and WSe2

   https://doi.org/10.1038/s41467-021-26304-w  

   Liu, Erfu ; van Baren, Jeremiah ; Lu, Zhengguang ; Taniguchi, Takashi ; Watanabe, Kenji ; Smirnov, Dmitry ; Chang, Yia-Chung ; Lui, Chun Hung ( October 2021 , Nature Communications)

   Exciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe₂and WSe₂gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s–3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because themore »trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe₂and WSe₂.

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3. Cascade synthesis and optoelectronic applications of intermediate bandgap Cu3VSe4 nanosheets

   https://doi.org/10.1038/s41598-020-78649-9  

   Liu, Mimi ; Lai, Cheng-Yu ; Zhang, Meng ; Radu, Daniela R. ( December 2020 , Scientific Reports)

   Two-dimensional (2D) ternary materials recently generated interest in optoelectronics and energy-related applications, alongside their binary counterparts. To date, only a few naturally occurring layered 2D ternary materials have been explored. The plethora of benefits owed to reduced dimensionality prompted exploration of expanding non-layered ternary chalcogenides into the 2D realm. This work presents a templating method that uses 2D transition metal dichalcogenides as initiators to be converted into the corresponding ternary chalcogenide upon addition of copper, via a solution-phase synthesis, conducted in high boiling point solvents. The process starts with preparation of VSe₂nanosheets, which are next converted into Cu₃VSe₄sulvanite nanosheetsmore »(NSs) which retain the 2D geometry while presenting an X-ray diffraction pattern identical with the one for the bulk Cu₃VSe₄. Both the scanning electron microscopy and transmission microscopy electron microscopy show the presence of quasi-2D morphology. Recent studies of the sulfur-containing sulvanite Cu₃VS₄highlight the presence of an intermediate bandgap, associated with enhanced photovoltaic (PV) performance. The Cu₃VSe₄nanosheets reported herein exhibit multiple UV–Vis absorption peaks, related to the intermediate bandgaps similar to Cu₃VS₄and Cu₃VSe₄nanocrystals. To test the potential of Cu₃VSe₄NSs as an absorber for solar photovoltaic devices, Cu₃VSe₄NSs thin-films deposited on FTO were subjected to photoelectrochemical testing, showing p-type behavior and stable photocurrents of up to ~ 0.036 mA/cm². The photocurrent shows a ninefold increase in comparison to reported performance of Cu₃VSe₄nanocrystals. This proves that quasi-2D sulvanite nanosheets are amenable to thin-film deposition and could show superior PV performance in comparison to nanocrystal thin-films. The obtained electrical impedance spectroscopy signal of the Cu₃VSe₄ NSs-FTO based electrochemical cell fits an equivalent circuit with the circuit elements of solution resistance (R_s), charge-transfer resistance (R_ct), double-layer capacitance (C_dl), and Warburg impedance (W). The estimated charge transfer resistance value of 300 Ω cm²obtained from the Nyquist plot provides an insight into the rate of charge transfer on the electrode/electrolyte interface.

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4. Designing catalysts for water splitting based on electronic structure considerations

   https://doi.org/10.1088/2516-1075/ab7d86  

   Razek, Sara Abdel ; Popeil, Melissa R. ; Wangoh, Linda ; Rana, Jatinkumar ; Suwandaratne, Nuwanthi ; Andrews, Justin L. ; Watson, David F. ; Banerjee, Sarbajit ; Piper, Louis F. J. ( April 2020 , Electronic Structure)

   The disproportionation of H₂O into solar fuels H₂and O₂, or water splitting, is a promising strategy for clean energy harvesting and storage but requires the concerted action of absorption of photons, separation of excitons, charge diffusion to catalytic sites and catalysis of redox processes. It is increasingly evident that the rational design of photocatalysts for efficient water splitting must employ hybrid systems, where the different components perform light harvesting, charge separation and catalysis in tandem. In this topical review, we report on the recent development of a new class of hybrid photocatalysts that employs M_xV₂O₅(M = p-block cation) nanowiresmore »in order to engineer efficient charge transfer from the photoactive chalcogenide quantum dots (QDs) to the water-splitting and hydrogen evolving catalysts. Herein, we summarize the oxygen-mediated lone pair mechanism used to modulate the energy level and orbital character of mid-gap states in the M_xV₂O₅nanowires. The electronic structure of M_xV₂O₅is discussed in terms of density functional theory and hard x-ray photoelectron spectroscopy (HAXPES) measurements. The principles of HAXPES are explained within the context of its unique sensitivity to metal 5(6)s orbitals and ability to non-destructively study buried interface alignments of quantum dot decorated nanowires i.e., M_xV₂O₅/CdX (X = S, Se, Te). We illustrate with examples how the M_xV₂O₅/CdX band alignments can be rationally engineered for ultra-fast charge-transfer of photogenerated holes from the quantum dot to the nanowires; thereby suppressing anodic photo-corrosion in the CdX QDs and enabling efficacious hydrogen evolution.

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5. The influence of crystal thickness and interlayer interactions on the properties of heavy ion irradiated MoS ₂

   https://doi.org/10.1088/2053-1583/ab817b  

   Isherwood, Liam H. ; Hennighausen, Zachariah ; Son, Seok-Kyun ; Spencer, Ben F. ; Wady, Paul T. ; Shubeita, Samir M. ; Kar, Swastik ; Casiraghi, Cinzia ; Baidak, Aliaksandr ( May 2020 , 2D Materials)

   Ion irradiation is a versatile tool to introduce controlled defects into two-dimensional (2D) MoS₂on account of its unique spatial resolution and plethora of ion types and energies available. In order to fully realise the potential of this technique, a holistic understanding of ion-induced defect production in 2D MoS₂crystals of different thicknesses is mandatory. X-ray photoelectron spectroscopy, electron diffraction and Raman spectroscopy show that thinner MoS₂crystals are more susceptible to radiation damage caused by 225 keV Xe⁺ions. However, the rate of defect production in quadrilayer and bulk crystals is not significantly different under our experimental conditions. The rate at whichmore »S atoms are sputtered as a function of radiation exposure is considerably higher for monolayer MoS₂, compared to bulk crystals, leading to MoO₃formation. P-doping of MoS₂is observed and attributed to the acceptor states introduced by vacancies and charge transfer interactions with adsorbed species. Moreover, the out-of-plane vibrational properties of irradiated MoS₂crystals are shown to be strongly thickness-dependent: in mono- and bilayer MoS₂, the confinement of phonons by defects results in a blueshift of the$A_{1g}$mode. Whereas, a redshift is observed in bulk crystals due to attenuation of the effective restoring forces acting on S atoms caused by vacancies in adjacent MoS₂layers. Consequently, the$A_{1g}$frequency of tri- and quadrilayer crystals is statistically invariant on account oft competition between phonon confinement effects and interlayer interactions. The$A_{1g}$linewidth is observed to decrease in bi- and trilayer crystals after low dose irradiation and is attributed to layer decoupling. This work shows that there is a complex interplay between defect production, crystal thickness and interlayer interactions in MoS₂. Our results demonstrate that ion irradiation is an effective tool to modulate the electronic, vibrational and structural properties of MoS₂, which may prove beneficial for practical applications.

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