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Molecular design of redox-active materials with higher solubility and greater redox potential windows is instrumental in enhancing the performance of redox flow batteries Here we propose a computational procedure for a systematic evaluation of organic redox-active species by combining machine learning, quantum-mechanical, and classical density functional theory calculations. 1,517 small quinone molecules were generated from the building blocks of benzoquinone, naphthoquinone, and anthraquinone with different substituent groups. The physics-based methods were used to predict HOMO-LUMO gaps and solvation free energies that account for the redox potential differences and aqueous solubility, respectively. The high-throughput calculations were augmented with the quantitative structure-property relationship analyses and machine learning/graph network modeling to evaluate the materials’ overall behavior. The computational procedure was able to reproduce high-performance cathode electrolyte materials consistent with experimental observations and identify new electrolytes for RFBs by screening 100,000 di-substituted quinone molecules, the largest library of redox-active quinone molecules ever investigated. The efficient computational platform may facilitate a better understanding of the structure-function relationship of quinone molecules and advance the design and application of all-organic active materials for RFBs.

 

Robust estimation is an important problem in statistics which aims at providing a reasonable estimator when the data-generating distribution lies within an appropriately defined ball around an uncontaminated distribution. Although minimax rates of estimation have been established in recent years, many existing robust estimators with provably optimal convergence rates are also computationally intractable. In this paper, we study several estimation problems under a Wasserstein contamination model and present computationally tractable estimators motivated by generative adversarial networks (GANs). Specifically, we analyze the properties of Wasserstein GAN-based estimators for location estimation, covariance matrix estimation and linear regression and show that our proposed estimators are minimax optimal in many scenarios. Finally, we present numerical results which demonstrate the effectiveness of our estimators.

 

Smart-coating foils for orthopedic implants prevent infection and provide early diagnosis of instrument failures. 

Materials that rectify light into current in their bulk are desired for optoelectronic applications. In Weyl semimetals that break inversion symmetry, bulk photocurrents may arise due to nonlinear optical processes that are enhanced near the Weyl nodes. However, the photoresponse of these materials is commonly studied by scanning photocurrent microscopy, which convolves the effects of photocurrent generation and collection. Here we directly image the photocurrent flow inside the type-II Weyl semimetals WTe2 and TaIrTe4 using high-sensitivity quantum magnetometry with nitrogen-vacancy centre spins. We elucidate a mechanism for bulk photocurrent generation, which we call the anisotropic photothermoelectric effect, where unequal thermopowers along different crystal axes drive intricate circulations of photocurrent around the photoexcitation. Using overlapping scanning photocurrent microscopy and magnetic imaging at the interior and edges of the sample, we visualize how the anisotropic photothermoelectric effect stimulates the long-range photocurrent collected in our WTe2 and TaIrTe4 devices through the Shockley–Ramo mechanism. Our results highlight a widely relevant source of current flow and will inspire photodetectors that utilize bulk materials with thermoelectric anisotropy. 

Abstract In this paper, we prove one divisibility of the Iwasawa–Greenberg main conjecture for the Rankin–Selberg product of a weight two cusp form and an ordinary complex multiplication form of higher weight, using congruences between Klingen Eisenstein series and cusp forms on $\mathrm {GU}(3,1)$ , generalizing an earlier result of the third-named author to allow nonordinary cusp forms. The main result is a key input in the third-named author’s proof of Kobayashi’s $\pm $ -main conjecture for supersingular elliptic curves. The new ingredient here is developing a semiordinary Hida theory along an appropriate smaller weight space and a study of the semiordinary Eisenstein family.