We describe a multispeckle dynamic light scattering technique capable of resolving the motion of scattering sites in cases that this motion changes systematically with time. The method is based on the visibility of the speckle pattern formed by the scattered light as detected by a single exposure of a digital camera. Whereas previous multispeckle methods rely on correlations between images, here the connection with scattering site dynamics is made more simply in terms of the variance of intensity among the pixels of the camerafor the specified exposure duration. The essence is that the speckle pattern is more visible, i.e., the variance of detected intensity levels is greater, when the dynamics of the scattering site motion is slow compared to the exposure time of the camera. The theory for analyzing the moments of the spatial intensity distribution in terms of the electric-field autocorrelation is presented. It is tested for two well-understood samples, a colloidal suspension of Brownian particles and a coarsening foam, where the dynamics can be treated as stationary and hence can be benchmarked by traditional methods. However, our speckle-visibility method is particularly appropriate for samples in which the dynamics vary with time, either slowly or rapidly, limited only by the exposure time fidelity of the camera. Potential applications range from soft-glassy materials, to granular avalanches, to flowmetry of living tissue. We describe a multispeckle dynamic light scattering technique capable of resolving the motion of scattering sites in cases that this motion changes systematically with time. The method is based on the visibility of the speckle pattern formed by the scattered light as detected by a single exposure of a digital camera. Whereas previous multispeckle methods rely on correlations between images, here the connection with scattering site dynamics is made more simply in terms of the variance of intensity among the pixels of the camera for the specified exposure duration. The essence is that the speckle pattern is more visible, i.e., the variance of detected intensity levels is greater, when the dynamics of the scattering site motion is slow compared to the exposure time of the camera. The theory for analyzing the moments of the spatial intensity distribution in terms of the electric-field autocorrelation is presented. It is tested for two well-understood samples, a colloidal suspension of Brownian particles and a coarsening foam, where the dynamics can be treated as stationary and hence can be benchmarked by traditional methods. However, our speckle-visibility method is particularly appropriate for samples in which the dynamics vary with time, either slowly or rapidly, limited only by the exposure time fidelity of the camera. Potential applications range from soft-glassy materials, to granular avalanches, to flowmetry of living tissue.
In this study we embed phase pure natural cubic-FeS 2 (pyrite) in a stabilized polyacrylonitrile (PAN) matrix. The PAN matrix confi nes FeS 2 's electroactive species (Fe 0 and S n 2− ) for good reversibility and effi ciency. Additionally, the stabilized PAN matrix can accommodate the 160% volume expansion of FeS 2 upon full discharge because it is not fully carbonized. At room temperature, our PAN-FeS 2 electrode delivers a specifi c capacity of 470 mAh g −1 on its 50th discharge. Using high-resolution transmission electron microscopy (HRTEM) we confi rm that FeS 2 particles are embedded in the PAN matrix and that FeS 2 's mobile electroactive species are confi ned during cycling. We also observe the formation of orthorhombic-FeS 2 at full charge, which validates the results of our previous all-solid-state FeS 2 battery study.The energy density of conventional Li-ion batteries with LiMO 2 (M = transition metal) cathodes and graphitic anodes is approaching a practical upper limit after two decades of optimization. In order to improve the energy density of Li-ion batteries further, new cathodes must be developed with capacities that compare to those of advanced anodes such as Si. [ 1 ] The FeS 2 conversion chemistry is a promising candidate to replace the LiMO 2 intercalation chemistry because FeS 2 is inexpensive, energy dense, and environmentally benign. The four electron reduction of cubic-FeS 2 (pyrite) with lithium (FeS 2 + 4Li + + 4e −
In this paper we demonstrate an all-solid-state Li-ion battery with a specific energy of 225 mWh g−1 based upon the combined mass of both the composite anode and cathode. To realize this full cell, we pair an iron sulfide and sulfur composite cathode with a Si-based anode. The anode active material is a Si-Ti-Ni alloy with good ionic and electronic conductivity that attains a stable specific capacity of 400 mAh g−1 based upon the total mass of the composite anode. To our knowledge, this is the highest stable Si-based all-solid-state anode specific capacity reported to date. To utilize both a lithium free anode and cathode, we adopt a pre-lithiation technique involving stabilized lithium metal powder. This is the first time that this technique has been demonstrated in an all-solid-state battery.
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