High-pressure X-ray photon correlation spectroscopy at fourth-generation synchrotron sources.

A new experimental setup combining X-ray photon correlation spectroscopy (XPCS) in the hard X-ray regime and a high-pressure sample environment has been developed to monitor the pressure dependence of the internal motion of complex systems down to the atomic scale in the multi-gigapascal range, from room temperature to 600 K. The high flux of coherent high-energy X-rays at fourth-generation synchrotron sources solves the problems caused by the absorption of diamond anvil cells used to generate high pressure, enabling the measurement of the intermediate scattering function over six orders of magnitude in time, from 10-3 s to 103 s. The constraints posed by the high-pressure generation such as the preservation of X-ray coherence, as well as the sample, pressure and temperature stability, are discussed, and the feasibility of high-pressure XPCS is demonstrated through results obtained on metallic glasses.

Chemically-driven autonomous Janus electromagnets as magnetotactic swimmers.

An electromagnet is a particular device that takes advantage of electrical currents to produce concentrated magnetic fields. The most well-known example is a conventional solenoid, having the form of an elongated coil and creating a strong magnetic field through its center when it is connected to a current source. Spontaneous redox reactions located at opposite ends of an anisotropic Janus swimmer can effectively mimic a standard power source, due to their ability to wirelessly generate a local electric current. Herein, we propose the coupling of thermodynamically spontaneous redox reactions occurring at the extremities of a hybrid Mg/Pt Janus swimmer with a solenoidal geometry to generate significant magnetic fields. These chemically driven electromagnets, spontaneously transform the redox-induced electric current into a magnetic field with a strength in the range of µT, upon contact with an acidic medium. Such on-board magnetization allows them to perform compass-like rotational motion and magnetotactic displacement in the presence of external magnetic field gradients, without the need of using ferromagnetic materials for the swimmer design. The torque force experienced by the swimmer is proportional to the internal redox current, and by varying the composition of the solution, it is possible to fine-tune its angular velocity.

Evidence of polyamorphic transitions during densified SiO2 glass annealing.

In situ X-ray scattering monitoring is carried out during temperature annealing on different densified SiO2 glasses. Density fluctuations and intermediate range coherence from X-ray scattering (small-angle X-ray scattering) and diffraction (wide angle X-ray scattering) evidence a maximum in their evolution at the same relaxation time. These extrema confirm the existence of an intermediate transitory disordered state between the two more ordered high and low density amorphous states. We propose that the existence of this transitory state confirms the existence of two mega basins in the energy landscape and therefore an amorphous-amorphous transition. Including older Raman results, we show that this intermediate disorder state implies similar mechanisms at all length scales from a few angstroms to 5 nm.

Endogenous and exogenous wireless multimodal light-emitting chemical devices.

Multimodal imaging is a powerful and versatile approach that integrates and correlates multiple optical modalities within a single device. This concept has gained considerable attention due to its potential applications ranging from sensing to medicine. Herein, we develop several wireless multimodal light-emitting chemical systems by coupling two light sources based on different physical principles: electrochemiluminescence (ECL) occurring at the electrode interface and a light-emitting diode (LED) switched on by an electrochemically triggered electron flow. Endogenous (thermodynamically spontaneous redox process) and exogenous (requiring an external power source) bipolar electrochemistry acts as a driving force to trigger both light emissions at different wavelengths. The results presented here interconnect optical imaging and electrochemical reactions, providing a novel and so far unexplored alternative to design autonomous hybrid systems with multimodal and multicolor optical readouts for complex bio-chemical systems.