Cycling LiCoO2 to above 4.5 V for higher capacity is enticing; however, hybrid O anion- and Co cation-redox (HACR) at high voltages facilitates intrinsic Oα - (α < 2) migration, causing oxygen loss, phase collapse, and electrolyte decomposition that severely degrade the battery cyclability. Hereby, commercial LiCoO2 particles are operando treated with selenium, a well-known anti-aging element to capture oxygen-radicals in the human body, showing an "anti-aging" effect in high-voltage battery cycling and successfully stopping the escape of oxygen from LiCoO2 even when the cathode is cycled to 4.62 V. Ab initio calculation and soft X-ray absorption spectroscopy analysis suggest that during deep charging, the precoated Se will initially substitute some mobile Oα - at the charged LiCoO2 surface, transplanting the pumped charges from Oα - and reducing it back to O2- to stabilize the oxygen lattice in prolonged cycling. As a result, the material retains 80% and 77% of its capacity after 450 and 550 cycles under 100 mA g-1 in 4.57 V pouch full-cells matched with a graphite anode and an ultralean electrolyte (2 g Ah-1 ).

A Surface Se-Substituted LiCo[O 2- δ Se δ ] Cathode with Ultrastable High-Voltage Cycling in Pouch Full-Cells

Topological insulators possess completely different spin-orbit coupled bulk and surface electronic spectra that are each predicted to exhibit exotic responses to light. Here we report time-resolved fundamental and second harmonic optical pump-probe measurements on the topological insulator Bi_2Se_3 to independently measure its photoinduced charge and spin dynamics with bulk and surface selectivity. Our results show that a transient net spin density can be optically induced in both the bulk and surface, which may drive spin transport in topological insulators. By utilizing a novel rotational anisotropy analysis we are able to separately resolve the spin depolarization, intraband cooling, and interband recombination processes following photoexcitation, which reveal that spin and charge degrees of freedom relax on very different time scales owing to strong spin-orbit coupling.

https://link.aps.org/accepted/10.1103/PhysRevLett.107.077401

Selective Probing of Photoinduced Charge and Spin Dynamics in the Bulk and Surface of a Topological Insulator

The shuttling behavior and sluggish conversion kinetics of intermediate lithium polysulfides (LiPS) represent the main obstacles to the practical application of lithium–sulfur batteries (LSBs). Herein, an innovative sulfur host is proposed, based on an iodine‐doped bismuth selenide (I‐Bi2Se3), able to solve these limitations by immobilizing the LiPS and catalytically activating the redox conversion at the cathode. The synthesis of I‐Bi2Se3 nanosheets is detailed here and their morphology, crystal structure, and composition are thoroughly. Density‐functional theory and experimental tools are used to demonstrate that I‐Bi2Se3 nanosheets are characterized by a proper composition and micro‐ and nano‐structure to facilitate Li+ diffusion and fast electron transportation, and to provide numerous surface sites with strong LiPS adsorbability and extraordinary catalytic activity. Overall, I‐Bi2Se3/S electrodes exhibit outstanding initial capacities up to 1500 mAh g−1 at 0.1 C and cycling stability over 1000 cycles, with an average capacity decay rate of only 0.012% per cycle at 1 C. Besides, at a sulfur loading of 5.2 mg cm−2, a high areal capacity of 5.70 mAh cm−2 at 0.1 C is obtained with an electrolyte/sulfur ratio of 12 µL mg−1. This work demonstrated that doping is an effective way to optimize the metal selenide catalysts in LSBs.

Enhanced Polysulfide Conversion with Highly Conductive and Electrocatalytic Iodine‐Doped Bismuth Selenide Nanosheets in Lithium–Sulfur Batteries

Plasmonic and dielectric Mie resonances in subwavelength nanostructures provide an efficient way to manipulate light below the diffraction limit that has fostered the growth of plasmonics and nanophotonics. Plasmonic resonances have been mainly related with the excitation of free charge carriers, initially in metals, and dielectric Mie resonances have been identified in Si nanostructures. Remarkably, although much less studied, semi-metals, semiconductors and topological insulators of the p-block enable plasmonic resonances without free charge carriers and dielectric Mie resonances with enhanced properties compared with Si. In this review, we explain how interband transitions in these materials show a major role in this duality. We evaluate the plasmonic and Mie performance of nanostructures made of relevant p-block elements and compounds, especially Bi, and discuss their promising potential for applications ranging from switchable plasmonics and nanophotonics to energy conversion, especially photocatalysis.

/pdf/interband-transitions-in-semi-metals-semiconductors-and-2qnfpqvqct.pdf

Interband transitions in semi-metals, semiconductors, and topological insulators: a new driving force for plasmonics and nanophotonics [Invited]

The growing demand for electronic devices, smart devices, and the Internet of Things constitutes the primary driving force for marching down the path of decreased critical dimension and increased circuit intricacy of integrated circuits. However, as sub-10 nm high-volume manufacturing is becoming the mainstream, there is greater awareness that defects introduced by original equipment manufacturer components impact yield and manufacturing costs. The identification, positioning, and classification of these defects, including random particles and systematic defects, are becoming more and more challenging at the 10 nm node and beyond. Very recently, the combination of conventional optical defect inspection with emerging techniques such as nanophotonics, optical vortices, computational imaging, quantitative phase imaging, and deep learning is giving the field a new possibility. Hence, it is extremely necessary to make a thorough review for disclosing new perspectives and exciting trends, on the foundation of former great reviews in the field of defect inspection methods. In this article, we give a comprehensive review of the emerging topics in the past decade with a focus on three specific areas: (a) the defect detectability evaluation, (b) the diverse optical inspection systems, and (c) the post-processing algorithms. We hope, this work can be of importance to both new entrants in the field and people who are seeking to use it in interdisciplinary work.

Optical wafer defect inspection at the 10 nm technology node and beyond

An understanding of the aging and oxidation of the (0001) surface of Bi2Se3 is critical to a comprehensive physical picture of its topologically protected surface states. Here, the authors contribute new experimental observations about the aging and oxidation process. The authors find that surface aging in ambient conditions occurs in two major steps. Within 2 h of exfoliation, a series of ∼3.2 A high islands are observed by atomic force microscopy over approximately 10% of the surface. Subsequently, patch growth stops, and oxidation begins after the 2 h and continues until one quintuple layer has been oxidized. X-ray photoelectron spectroscopy shows no sign of oxidation before ∼120 min of exposure to air, and the oxygen 1 s peak, as well as oxidized Se 3d and Bi 4d peaks, are clearly present after ∼190 min of ambient exposure. Variable angle spectroscopic ellipsometry indicates that the oxidation of a full quintuple layer occurs on the time scale of days. These results are in good agreement with the time...

Surface oxidation of the topological insulator Bi2Se3

A comprehensive picture of the aging and oxidation of the (0001) surface of Bi2Se3 is critical to understanding the physical origin of changes in its topologically protected surface states. We find that surface aging in ambient conditions occurs in two major steps. Within two hours of exfoliation, a series of ~ 3.6 A high islands are observed by atomic force microscopy over approximate 10% of the surface. Subsequently, patch growth stops, and oxidation begins after the two hours and continues until one quintuple layer has been oxidized. X-ray photoelectron spectroscopy shows no sign of oxidation before ~ 120 minutes of exposure to air, and the oxygen 1s peak is clearly present after ~ 190 minutes of ambient exposure. Variable angle spectroscopic ellipsometry also indicates that the oxidation of a full quintuple layer occurs on the time scale of days. These results are in good agreement with the time dependent changes previously observed in the surface crystal structure by second harmonic generation. In addition to providing the ability to non-destructively measure oxide on the surface of Bi2Se3 crystals, ellipsometry can be used to identify the thickness of Bi2Se3 flakes. These results are consistent with non-linear optical methods including rotational anisotropy second harmonic generation, which follow the time dependence of the changes to the top quintuple layer.

Surface Oxidation of the Topological Insulator Bi2Se3

A Dissertation Submitted to the State University of New York in Partial Fulfillment of the Requirements for the Degree of
 Doctor of Philosophy SUNY Polytechnic Institute Colleges of Nanoscale Science and Engineering

Assessing a Multi-Electron Beam Application Approach for Semiconductor Process Metrology

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Surface oxidation of the topological insulator Bi2Se3

Surface Oxidation of the Topological Insulator Bi2Se3

Assessing a Multi-Electron Beam Application Approach for Semiconductor Process Metrology