Reconstructing a three-dimensional ocean sound speed field (SSF) from limited and noisy measurements presents an ill-posed and challenging inverse problem. Existing methods used a number of pre-specified priors (e.g., low-rank tensor and tensor neural network structures) to address this issue. However, the SSFs are often too complex to be accurately described by these pre-defined priors. While utilizing neural network-based priors trained on historical SSF data may be a viable workaround, acquiring SSF data remains a nontrivial task. This work starts with a key observation: Although natural images and SSFs admit fairly different characteristics, their denoising processes appear to share similar traits—as both remove random components from more structured signals. This observation allows us to incorporate deep denoisers trained using extensive natural images to realize zero-shot SSF reconstruction, without any extra training or network modifications. To implement this idea, an alternating direction method of multipliers (ADMM) algorithm using such a deep denoiser is proposed, which is reminiscent of the plug-and-play scheme from medical imaging. Our plug-and-play framework is tailored for SSF recovery such that the learned denoiser can be simultaneously used with other handcrafted SSF priors. Extensive numerical studies show that the new framework largely outperforms state-of-the-art baselines, especially under widely recognized challenging scenarios, e.g., when the SSF samples are taken as tensor fibers. The code is available at https://github.com/OceanSTARLab/DeepPnP.
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Developing synthetically useful enzymatic reactions that are not known in biochemistry and organic chemistry is an important challenge in biocatalysis. Through the synergistic merger of photoredox catalysis and pyridoxal 5′-phosphate (PLP) biocatalysis, we developed a pyridoxal radical biocatalysis approach to prepare valuable noncanonical amino acids, including those bearing a stereochemical dyad or triad, without the need for protecting groups. Using engineered PLP enzymes, either enantiomeric product could be produced in a biocatalyst-controlled fashion. Synergistic photoredox
- pyridoxal radical biocatalysis represents a powerful platform with which to discover previously unknown catalytic reactions and to tame radical intermediates for asymmetric catalysis. -
Abstract This paper presents a stochastic three-dimensional focused transport simulation of solar energetic particles (SEPs) produced by a data-driven coronal mass ejection (CME) shock propagating through a data-driven model of coronal and heliospheric magnetic fields. The injection of SEPs at the CME shock is treated using diffusive shock acceleration of post-shock suprathermal solar wind ions. A time-backward stochastic simulation is employed to solve the transport equation to obtain the SEP time–intensity profile at any location, energy, and pitch angle. The model is applied to a SEP event on 2020 May 29, observed by STEREO-A close to ∼1 au and by Parker Solar Probe (PSP) when it was about 0.33 au away from the Sun. The SEP event was associated with a very slow CME with a plane-of-sky speed of 337 km s−1at a height below 6
R S as reported in the SOHO/LASCO CME catalog. We compute the time profiles of particle flux at PSP and STEREO-A locations, and estimate both the spectral index of the proton energy spectrum for energies between ∼2 and 16 MeV and the equivalent path length of the magnetic field lines experienced by the first arriving SEPs. We find that the simulation results are well correlated with observations. The SEP event could be explained by the acceleration of particles by a weak CME shock in the low solar corona that is not magnetically connected to the observers. -
Abstract Realization of practical sodium metal batteries (SMBs) is hindered due to lack of compatible electrolyte components, dendrite propagation, and poor understanding of anodic interphasial chemistries. Chemically robust liquid electrolytes that facilitate both favorable sodium metal deposition and a stable solid‐electrolyte interphase (SEI) are ideal to enable sodium metal and anode‐free cells. Herein we present advanced characterization of a novel fluorine‐free electrolyte utilizing the [HCB 11 H 11 ] 1− anion. Symmetrical Na cells operated with this electrolyte exhibit a remarkably low overpotential of 0.032 V at a current density of 2.0 mA cm −2 and a high coulombic efficiency of 99.5 % in half‐cell configurations. Surface characterization of electrodes post‐operation reveals the absence of dendritic sodium nucleation and a surprisingly stable fluorine‐free SEI. Furthermore, weak ion‐pairing is identified as key towards the successful development of fluorine‐free sodium electrolytes.more » « less
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Abstract Redox‐active polymers (RAPs) are promising organic electrode materials for affordable and sustainable batteries due to their flexible chemical structures and negligible solubility in the electrolyte. Developing high‐dimensional RAPs with porous structures and crosslinkers can further improve their stability and redox capability by reducing the solubility and enhancing reaction kinetics. This work reports two three‐dimensional (3D) RAPs as stable organic cathodes in Na‐ion batteries (NIBs) and K‐ion batteries (KIBs). Carbonyl functional groups are incorporated into the repeating units of the RAPs by the polycondensation of Tetrakis(4‐aminophenyl)methane and two different dianhydrides. The RAPs with interconnected 3D extended conjugation structures undergo multi‐electron redox reactions and exhibit high performance in both NIBs and KIBs in terms of long cycle life (up to 8000 cycles) and fast charging capability (up to 2 A g−1). The results demonstrate that developing 3D RAPs is an effective strategy to achieve high‐performance, affordable, and sustainable NIBs and KIBs.