A radical spin on viologen polymers: organic spin crossover materials in water.

A polymer containing viologen radical cation monomer units is shown to reversibly switch between paramagnetic and diamagnetic states via non-covalent host-guest interactions or temperature control in water. Cycling between diamagnetic and paramagnetic forms is accompanied by changes in optical and magnetic properties.

An organic spin crossover material in water from a covalently linked radical dyad.

A covalently linked viologen radical cation dyad acts as a reversible thermomagnetic switch in water. Cycling between diamagnetic and paramagnetic forms by heating and cooling is accompanied by changes in optical and magnetic properties with high radical fidelity. Thermomagnetic switches in water may eventually find use as novel biological thermometers and in temperature-responsive organic materials where the changes in properties originate from a change in electronic spin configuration rather than a change in structure.

Inverted substrate preferences for photochemical heterolysis arise from conical intersection control.

Heterolytic bond scission is a staple of chemical reactions. While qualitative and quantitative models exist for understanding the thermal heterolysis of carbon-leaving group (C-LG) bonds, no general models connect structure to reactivity for heterolysis in the excited state. CASSCF conical intersection searches were performed to investigate representative systems that undergo photoheterolysis to generate carbocations.

A noncovalently reversible paramagnetic switch in water.

We report an organo-paramagnetic switch consisting of a linked bis(viologen) dication diradical that can be cycled reversibly between diamagnetic and paramagnetic states via noncovalent guest-host chemistry with cucurbit[7]uril (CB[7]) in room-temperature water. Computations suggest that the nature of the interaction between the viologen cation radical units is that of a pi dimer (pimer). Molecules with switchable magnetic properties have possible applications in spintronics, data storage devices, chemical sensors, building blocks for materials with switchable bulk magnetic properties, as well as magnetic resonance probes for biological applications.

Ultra-high-contrast few-cycle pulses for multipetawatt-class laser technology.

We report the generation of few-cycle multiterawatt light pulses with a temporal contrast of 10(10), when measured as close as 2 ps to the pulse's peak. Tens of picoseconds before the main pulse, the contrast value is expected to spread much beyond the measurement limit. Separate measurements of contrast improvement factors at different stages of the laser system indicate that real contrast values may reach 10(19) and 10(14), when measured 50 and 25 ps before the pulse's peak, respectively.

A high resolution, broad energy acceptance spectrometer for laser wakefield acceleration experiments.

Laser wakefield experiments present a unique challenge in measuring the resulting electron energy properties due to the large energy range of interest, typically several 100 MeV, and the large electron beam divergence and pointing jitter >1 mrad. In many experiments the energy resolution and accuracy are limited by the convolved transverse spot size and pointing jitter of the beam. In this paper we present an electron energy spectrometer consisting of two magnets designed specifically for laser wakefield experiments.