Generation and Detection of Spin Currents in Semiconductor Nanostructures with Strong Spin-Orbit Interaction.

Storing, transmitting, and manipulating information using the electron spin resides at the heart of spintronics. Fundamental for future spintronics applications is the ability to control spin currents in solid state systems. Among the different platforms proposed so far, semiconductors with strong spin-orbit interaction are especially attractive as they promise fast and scalable spin control with all-electrical protocols. Here we demonstrate both the generation and measurement of pure spin currents in semiconductor nanostructures. Generation is purely electrical and mediated by the spin dynamics in materials with a strong spin-orbit field. Measurement is accomplished using a spin-to-charge conversion technique, based on the magnetic field symmetry of easily measurable electrical quantities. Calibrating the spin-to-charge conversion via the conductance of a quantum point contact, we quantitatively measure the mesoscopic spin Hall effect in a multiterminal GaAs dot. We report spin currents of 174 pA, corresponding to a spin Hall angle of 34%.

Materials processing routes to trap-free halide perovskites.

Photovoltaic devices based on lead iodide perovskite films have seen rapid advancements, recently achieving an impressive 17.9% certified solar power conversion efficiency. Reports have consistently emphasized that the specific choice of growth conditions and chemical precursors is central to achieving superior performance from these materials; yet the roles and mechanisms underlying the selection of materials processing route is poorly understood. Here we show that films grown under iodine-rich conditions are prone to a high density of deep electronic traps (recombination centers), while the use of a chloride precursor avoids the formation of key defects (Pb atom substituted by I) responsible for short diffusion lengths and poor photovoltaic performance. Furthermore, the lowest-energy surfaces of perovskite crystals are found to be entirely trap-free, preserving both electron and hole delocalization to a remarkable degree, helping to account for explaining the success of polycrystalline perovskite films. We construct perovskite films from I-poor conditions using a lead acetate precursor, and our measurement of a long (600 ± 40 nm) diffusion length confirms this new picture of the importance of growth conditions.

Insulating state and giant nonlocal response in an InAs/GaSb quantum well in the quantum Hall regime.

We present transport measurements performed in InAs/GaSb double quantum wells. At the electron-hole crossover tuned by a gate voltage, a strong increase in the longitudinal resistivity is observed with increasing perpendicular magnetic field. Concomitantly with a local resistance exceeding the resistance quantum by an order of magnitude, we find a pronounced nonlocal resistance signal of almost similar magnitude. The coexistence of these two effects is reconciled in a model of counterpropagating and dissipative quantum Hall edge channels providing backscattering, shorted by a residual bulk conductivity.

Quantification and modeling of mechanical degradation in lithium-ion batteries based on nanoscale imaging.

Capacity fade in lithium-ion battery electrodes can result from a degradation mechanism in which the carbon black-binder network detaches from the active material. Here we present two approaches to visualize and quantify this detachment and use the experimental results to develop and validate a model that considers how the active particle size, the viscoelastic parameters of the composite electrode, the adhesion between the active particle and the carbon black-binder domain, and the solid electrolyte interphase growth rate impact detachment and capacity fade. Using carbon-silicon composite electrodes as a model system, we demonstrate X-ray nano-tomography and backscatter scanning electron microscopy with sufficient resolution and contrast to segment the pore space, active particles, and carbon black-binder domain and quantify delamination as a function of cycle number. The validated model is further used to discuss how detachment and capacity fade in high-capacity materials can be minimized through materials engineering.

Combining operando synchrotron X-ray tomographic microscopy and scanning X-ray diffraction to study lithium ion batteries.

We present an operando study of a lithium ion battery combining scanning X-ray diffraction (SXRD) and synchrotron radiation X-ray tomographic microscopy (SRXTM) simultaneously for the first time. This combination of techniques facilitates the investigation of dynamic processes in lithium ion batteries containing amorphous and/or weakly attenuating active materials. While amorphous materials pose a challenge for diffraction techniques, weakly attenuating material systems pose a challenge for attenuation-contrast tomography. Furthermore, combining SXRD and SRXTM can be used to correlate processes occurring at the atomic level in the crystal lattices of the active materials with those at the scale of electrode microstructure. To demonstrate the benefits of this approach, we investigate a silicon powder electrode in lithium metal half-cell configuration. Combining SXRD and SRXTM, we are able to (i) quantify the dissolution of the metallic lithium electrode and the expansion of the silicon electrode, (ii) better understand the formation of the Li15Si4 phase, and (iii) non-invasively probe kinetic limitations within the silicon electrode. A simple model based on the 1D diffusion equation allows us to qualitatively understand the observed kinetics and demonstrates why high-capacity electrodes are more prone to inhomogeneous lithiation reactions.

Quantifying microstructural dynamics and electrochemical activity of graphite and silicon-graphite lithium ion battery anodes.

Despite numerous studies presenting advances in tomographic imaging and analysis of lithium ion batteries, graphite-based anodes have received little attention. Weak X-ray attenuation of graphite and, as a result, poor contrast between graphite and the other carbon-based components in an electrode pore space renders data analysis challenging. Here we demonstrate operando tomography of weakly attenuating electrodes during electrochemical (de)lithiation. We use propagation-based phase contrast tomography to facilitate the differentiation between weakly attenuating materials and apply digital volume correlation to capture the dynamics of the electrodes during operation. After validating that we can quantify the local electrochemical activity and microstructural changes throughout graphite electrodes, we apply our technique to graphite-silicon composite electrodes. We show that microstructural changes that occur during (de)lithiation of a pure graphite electrode are of the same order of magnitude as spatial inhomogeneities within it, while strain in composite electrodes is locally pronounced and introduces significant microstructural changes.