Ionic liquids (ILs) are a special category of molten salts solely composed of ions with varied molecular symmetry and charge delocalization. The versatility in combining varied cation−anion moieties and in functionalizing ions with different atoms and molecular groups contributes to their peculiar interactions ranging from weak isotropic associations to strong, specific, and anisotropic forces. A delicate interplay among intra-and intermolecular interactions facilitates the formation of heterogeneous microstructures and liquid morphologies, which further contributes to their striking dynamical properties. Microstructural and dynamical heterogeneities of ILs lead to their multifaceted properties described by an inherent designer feature, which makes ILs important candidates for novel solvents, electrolytes, and functional materials in academia and industrial applications. Due to a massive number of combinations of ion pairs with ion species having distinct molecular structures and IL mixtures containing varied molecular solvents, a comprehensive understanding of their hierarchical structural and dynamical quantities is of great significance for a rational selection of ILs with appropriate properties and thereafter advancing their macroscopic functionalities in applications. In this review, we comprehensively trace recent advances in understanding delicate interplay of strong and weak interactions that underpin their complex phase behaviors with a particular emphasis on understanding heterogeneous microstructures and dynamics of ILs in bulk liquids, in mixtures with cosolvents, and in interfacial regions.

We demonstrate strong magnon-photon coupling of a thin-film permalloy device fabricated on a coplanar superconducting resonator. A coupling strength of 0.152 GHz and a cooperativity of 68 are found for a 30-nm-thick permalloy stripe. The coupling strength is tunable by rotating the biasing magnetic field or changing the volume of permalloy. We also observe an enhancement of magnonphoton coupling in the nonlinear regime of the superconducting resonator, which is mediated by the nucleation of dynamic flux vortices. Our results demonstrate a critical step towards future integrated hybrid systems for quantum magnonics and on-chip coherent information transfer.

For a type-II superconductor, when the applied magnetic field is higher than the lower critical value H c1 , the magnetic flux will penetrate into the superconductor and form quantized vortices, which usually are arranged in an Abrikosov lattice. For the newly discovered iron pnictide superconductors, previous measurements have shown that, in electron-doped BaFe 2 As 2 , the vortices form a highly disordered structure 1-3 . In addition, the density of states (DOS) within the vortex cores 1 do not exhibit the Andreev bound states in conventional superconductors 4 -8 . In this Letter, we report the observation of a triangular vortex lattice and the Andreev bound states in hole-doped BaFe 2 As 2 by using a low temperature scanning tunneling microscope (STM). Detailed study of the vortex cores reveals that the spectrum of the Andreev bound states inside the vortex core exhibits a distinct spatial evolution: at the center of the vortex core, it appears as a single peak at 0.5 mV below the Fermi-energy; away from the core center, it gradually evolves into two sub-peaks and they eventually fade out. The drastic differences between the vortex cores of the electron-doped and hole-doped counterparts are illusive to the pairing mechanism of the iron pnictide superconductors.Magnetic flux quantization is one of the important quantum phenomena in the mixed

We have developed an all-atomistic force field for a new class of halogen-free chelated orthoborate-phosphonium ionic liquids. The force field is based on an AMBER framework with determination of force field parameters for phosphorus and boron atoms, as well as refinement of several available parameters. The bond and angle force constants were adjusted to fit vibration frequency data derived from both experimental measurements and ab initio calculations. The force field parameters for several dihedral angles were obtained by fitting torsion energy profiles deduced from ab initio calculations. To validate the proposed force field parameters, atomistic simulations were performed for 12 ionic liquids consisting of tetraalkylphosphonium cations and chelated orthoborate anions. The predicted densities for neat ionic liquids and the [P6,6,6,14][BOB] sample, with a water content of approximately 2.3-2.5 wt %, are in excellent agreement with available experimental data. The potential energy components of 12 ionic liquids were discussed in detail. The radial distribution functions and spatial distribution functions were analyzed and visualized to probe the microscopic ionic structures of these ionic liquids. There are mainly four high-probability regions of chelated orthoborate anions distributed around tetraalkylphosphonium cations in the first solvation shell, and such probability distribution functions are strongly influenced by the size of anions.

The newly developed hydrogen sensor, based on a network of ultrasmall pure palladium nanowires sputter-deposited on a filtration membrane, takes advantage of single palladium nanowires' characteristics of high speed and sensitivity while eliminating their nanofabrication obstacles. However, this new type of sensor, like the single palladium nanowires, cannot distinguish hydrogen concentrations above 3%, thus limiting the potential applications of the sensor. This study reports hydrogen sensors based on a network of ultrasmall Cr-buffered Pd (Pd/Cr) nanowires on a filtration membrane. These sensors not only are able to outperform their pure Pd counterparts in speed and durability but also allow hydrogen detection at concentrations up to 100%. The new networks consist of a thin layer of palladium deposited on top of a Cr adhesion layer 1-3 nm thick. Although the Cr layer is insensitive to hydrogen, it enables the formation of a network of continuous Pd/Cr nanowires with thicknesses of the Pd layer as thin as 2 nm. The improved performance of the Pd/Cr sensors can be attributed to the increased surface area to volume ratio and to the confinement-induced suppression of the phase transition from Pd/H solid solution (α-phase) to Pd hydride (β-phase).

Biomedical investigations reveal that excessive formaldehyde generation is possibly a critical factor for tissue cancerization, cancer progression and metastasis. Responsive molecular probes that can detect lysosomal formaldehyde in live cells and tumors and monitor drug-triggered formaldehyde scavenging contribute potentially to future cancer diagnosis and treatment monitoring. Herein, a novel "dual-key-and-lock" strategy-based ruthenium(II) complex probe, Ru-FA, is reported as an effective tool for formaldehyde detection in vitro and in vivo. Ru-FA shows weak luminescence due to photon-induced electron transfer (PET) process from Ru(II) centre to electron withdrawing group 2,4-dinitrobenzene (DNB). Triggered by the specific reaction with formaldehyde (first "key") in an acidic microenvironment (second "key"), DNB is cleaved from Ru-FA, affording an emissive Ru(II) complex derivative, Ru-NR. Spectrometric analysis including steady-state and time-gated luminescence indicates that Ru-FA is favourable to be used as the probe for quantification of formaldehyde in human sera and mouse organs. Ru-FA is biocompatible and cell membrane permeable. Together with its smart "dualkey-and-lock" response to formaldehyde, luminescence imaging of lysosomal formaldehyde in live cells, visualization of tumor-derived endogenous formaldehyde and monitoring of formaldehyde scavenging in mice were achieved, followed by the successful demonstration on detection of formaldehyde in tumors and other organs. These in vivo and in vitro detection confirm not only the excessive formaldehyde generation in tumors, but also the efficient drug administration to scavenge formaldehyde, demonstrating the potential application of Ru-FA in cancer diagnosis and treatment monitoring through lysosomal formaldehyde detection.

Atomistic simulations have been performed to investigate the microscopic structural organization of aqueous solutions of trihexyltetradecylphosphonium bis(oxalato)borate ([P6,6,6,14][BOB]) ionic liquid (IL). The evolution of the microscopic liquid structure and the local ionic organization of IL/water mixtures as a function of the water concentration is visualized and systematically analyzed via radial and spatial distribution functions, coordination numbers, hydrogen bond network, and water clustering analysis. The microscopic liquid structure in neat IL is characterized by a connected apolar network composed of the alkyl chains of [P6,6,6,14] cations and isolated polar domains consisting of the central segments of [P6,6,6,14] cations and [BOB] anions, and the corresponding local ionic environment is described by direct contact ion pairs. In IL/water mixtures with lower water mole fractions, the added water molecules are dispersed and embedded in cavities between neighboring ionic species and the local ionic structure is characterized by solvent-shared ion pairs through cation-water-anion triple complexes. With a gradual increase in the water concentration in IL/water mixtures, the added water molecules tend to aggregate and form small clusters, intermediate chain-like structures, large aggregates, and eventually a water network in water concentrated simulation systems. A further progressive dilution of IL/water mixtures leads to the formation of self-organized micelle-like aggregates characterized by a hydrophobic core and hydrophilic shell consisting of the central polar segments in [P6,6,6,14] cations and [BOB] anions in a highly branched water network. The striking structural evolution of the [P6,6,6,14][BOB] IL/water mixtures is rationalized by the competition between favorable hydrogen bonded interactions and strong electrostatic interactions between the polar segments in ionic species and the dispersion interactions between the hydrophobic alkyl chains in [P6,6,6,14] cations.

The delicate trade-off between hydrogen bonding and π-type coordinations plays a pivotal role in stabilizing molecular structures in ionic liquids bearing multiple hydrogen bonding sites and heteroaromatic ring planes. By performing extensive atomistic simulations, we have investigated the effect of aliphatic chain length in imidazolium cations on liquid morphologies, hydrogen bonding and π-type structures, and the corresponding dynamical quantities in imidazolium bis(oxalato)borate ionic liquids. The liquid morphologies are characterized by segregated apolar clusters (domains) within polar framework in liquid samples with short aliphatic chains in imidazolium cations and are transformed to spongelike polar and apolar arrangements in liquid matrices with lengthening aliphatic chains in imidazolium cations. Such a striking evolution of liquid morphologies of imidazolium bis(oxalato)borate ionic liquids is qualitatively characterized by total and partial X-ray scattering static structural factors. Preferential hydrogen bonds and distinctive π-type coordinations among imidazolium and oxalato ring planes coexist in ionic liquid matrices. A gradual addition of methylene units to imidazolium cations leads to a substantial increase in hydrogen bonding strength, which, however, results in decreased π-type coordinations between imidazolium and oxalato ring planes, indicating distinct competitive structural characteristics between hydrogen bonding and π-type associations between imidazolium and oxalato ring planes. A prevalent cooperative feature is observed in continuous and intermittent hydrogen bonding dynamics and in translational and reorientational dynamics of imidazolium and oxalato ring planes with lengthening aliphatic chains in imidazolium cations. The competitive structural trade-off and cooperative dynamical interplay of hydrogen bonding and π-type interactions between imidazolium cations and bis(oxalato)borate anions are intrinsically correlated with short-range collective interactions between alkyl units in imidazolium cations and long-range Coulombic interactions between imidazolium and oxalato ring planes in heterogeneous ionic environments.