No abstract

Absorbance spectra of two ionic liquids, the short alkyl chain N-trimethyl-N-propylammonium bis(trifluoromethanesulfonyl)imide (TMPA-TFSI) and the longer chain N-trimethyl-N-hexylammonium bis(trifluoromethanesulfonyl)imide (TMHA-TFSI) are reported as a function of pressure and temperature. The occurrence of various phase transitions is evidenced by the changes in the relative concentration of the cisoid and transoid conformers of their common TFSI anion. The infrared spectrum of TMPA-TFSI was measured at 300 K with an applied pressure varying over the 0-5 GPa range. Above 0.2 GPa only the trans conformer is detected, suggesting the occurrence of a pressure induced crystallization. When pressure is applied to TMHA-TFSI at T = 310 K, both TFSI conformers subsist up to ∼11 GPa. However, the clear change of their intensity ratio observed around 2 GPa, suggests the onset of a glass phase as supported by measurements carried out at 4.2 GPa along a cooling/heating cycle. A careful analysis of the spectra collected along different p-T thermodynamic paths shows the occurrence of a cold crystallization at 295 K on heating from 139 K along the p = 0.5 GPa isobar. The rich phase diagrams of the two ionic liquids is the result of the competition among the anion-cation intermolecular interactions, the lower energy of trans-TFSI with respect to cis-TFSI and the smaller volume of cis-TFSI with respect to trans-TFSI.

International audienceWe have studied the MnGe chiral magnet below T N = 170 K, by magnetic measurements, Mössbauer spectroscopy, and by neutron diffraction at ambient and under nonhydrostatic pressure. At ambient pressure, we observe the coexistence of two magnetic phases belonging to the same crystal phase in a large temperature range (down to 100 K) below T N : ferromagnetically correlated rapidly fluctuating spins coexist with frozen spins involved in the helical order. Applying a uniaxial pressure component induces a strong magnetic texture, where most of the helical axes reorient along the stress axis. The magnetic texture persists in the fluctuating chiral state up to T N. Our results suggest that the zero field ground state at ambient pressure is a multidomain state consisting of helical domains with random orientations rather than a three-dimensional skyrmion lattice. They show the presence of an unusually broad transition to paramagnetism with a dynamical phase separation triggered by temperature

A method to map spin-resolved electron distribution from combined polarized neutron and X-ray diffraction is described and applied for the first time to a molecular magnet and it is shown that spin up density is 5% more contracted than spin down density.

New crystallographic tools were developed to access a more precise description of the spin-dependent electron density of magnetic crystals. The method combines experimental information coming from high-resolution X-ray diffraction (XRD) and polarized neutron diffraction (PND) in a unified model. A new algorithm that allows for a simultaneous refinement of the charge- and spin-density parameters against XRD and PND data is described. The resulting software MOLLYNX is based on the well known Hansen-Coppens multipolar model, and makes it possible to differentiate the electron spins. This algorithm is validated and demonstrated with a molecular crystal formed by a bimetallic chain, MnCu(pba)(H(2)O)(3)·2H(2)O, for which XRD and PND data are available. The joint refinement provides a more detailed description of the spin density than the refinement from PND data alone.

International audienceWe have studied by muon spin resonance (mu SR) the helical ground state and fluctuating chiral phase recently observed in the MnGe chiral magnet. At low temperature, the muon polarization shows double-period oscillations at short-time scales. Their analysis, akin to that recently developed for MnSi [A. Amato et al., Phys. Rev. B 89, 184425 (2014)], provides an estimation of the field distribution induced by the Mn helical order at the muon site. The refined muon position agrees nicely with ab initio calculations. With increasing temperature, an inhomogeneous fluctuating chiral phase sets in, characterized by two well-separated frequency ranges which coexist in the sample. Rapid and slow fluctuations, respectively, associated with short-range and long-range ordered helices, coexist in a large temperature range below T-N = 170 K. We discuss the results with respect to MnSi, taking the short helical period, metastable quenched state, and peculiar band structure of MnGe into account

We study the evolution of helical magnetism in MnGe chiral magnet upon partial substitution of Mn for non magnetic 3d-Co and 4d-Rh ions. At high doping levels, we observe spin helices with very long periods -more than ten times larger than in the pure compound-and sizable ordered moments. This behavior calls for a change in the energy balance of interactions leading to the stabilization of the observed magnetic structures. Strikingly, neutron scattering unambiguously shows a double periodicity in the observed spectra at x > ∼ 0.45 and > ∼ 0.25 for Co-and Rh-doping, respectively. In analogy with observations made in cholesteric liquid crystals, we suggest that it reveals the presence of magnetic twist-grain-boundary phases, involving a dense short-range correlated network of screw dislocations. The dislocation cores are described as smooth textures made of non-radial double-core skyrmions.

International audienceItinerant magnets generally exhibit pressure-induced transitions towards nonmagnetic states. Using synchrotron-based x-ray diffraction and emission spectroscopy, the evolution of the lattice and spin moment in the chiral magnet MnGe was investigated in the paramagnetic state and under pressures up to 38 GPa. The collapse of the spin moment takes place in two steps. A first-order transition with a huge hysteresis around 7 GPa transforms the system from the high-spin state at ambient pressure to a low-spin state. The coexistence of spin states and observation of history-depending irreversibility is explained as the effect of long-range elastic strains mediated by magnetovolume coupling. Only in a second transition, at about 23 GPa, does the spin moment collapse