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Register a new userInterplay of Spin, Lattice, and Charge Degrees of Freedom in Ca3Mn2O7
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From low-temperature Synchrotron X-ray diffraction, a precise thermal characterization of octahedral distortions in single phase Ruddlesden-Popper Ca3Mn2O7 is performed. Highly sensitive close-steps temperature dependences of Mn-O-Mn bond angles connecting MnO6 octahedra clearly reveal signature of the spin-ordering in the system. Spin-lattice coupling is thus established via the structural distortions responsible for evolution of the magnetic state. Further, temperature anomalies observed here in volume and polarization-measure of the unit cell highlight the interplay between spin, lattice and charge degrees of freedom. Dipole-relaxation characteristics examined under applied magnetic field consistently corroborate the concurrent magnetic and structural changes, in terms of genuine and intrinsic magneto-dielectricity.
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Dielectric study on Ca3Mn2O7 features relaxor-like segmented dynamics below the antiferromagnetic ordering. Dipolar relaxations of different origin are spectrally resolved exhibiting distinct H-field alterations. This identifies their allegiance to different magnetic sub-phases and establishes dual coupling of electrical, magnetic, and structural degrees of freedom. Further, strong spin-lattice coupling has been affirmed with Raman spectroscopy across the magnetic ordering. Short-range electrical correlations collaterally cause measurable harmonic dielectric response in the system. The c{hi}_3^e-susceptibility signal yields genuine harmonic magneto-dielectricity, consistent with but exhibiting two orders of magnitude larger H-field effect, vis-`a-vis that obtained in the fundamental dielectric constant {epsilon}.
Electrons in condensed matter have internal degrees of freedom, such as charge, spin and orbital, leading to various forms of ordered states through phase transitions. However, in individual materials, a charge/spin/orbital ordered state of the lowest temperature is normally uniquely determined in terms of the lowest-energy state, i.e., the ground state. Here, we summarize recent results showing that under rapid cooling, this principle does not necessarily hold, and thus, the cooling rate is a control parameter of the lowest-temperature state beyond the framework of the thermo-equilibrium phase diagram. Although the cooling rate utilized in low-temperature experiments is typically 2*10^-3 - 4*10^-1 K/s, the use of optical/electronic pulses facilitate rapid cooling, such as 10^2-10^3 K/s. Such an unconventionally high cooling rate allows some systems to kinetically avoid a first-order phase transition, resulting in a quenched charge/spin state that differs from the ground state. We also demonstrate that quenched states can be exploited as a non-volatile state variable when designing phase-change memory functions. The present findings suggest that rapid cooling is useful for exploring and controlling the metastable electronic/magnetic state that is potentially hidden behind the ground state.
The local structure and electronic properties of Rb$_{1-x}$Fe$_{2-y}$Se$_2$ are investigated by means of site selective polarized x-ray absorption spectroscopy at the iron and selenium K-edges as a function of pressure. A combination of dispersive geometry and novel nanodiamond anvil pressure-cell has permitted to reveal a step-like decrease in the Fe-Se bond distance at $psimeq11$ GPa. The position of the Fe K-edge pre-peak, which is directly related to the position of the chemical potential, remains nearly constant until $sim6$ GPa, followed by an increase until $psimeq 11$ GPa. Here, as in the local structure, a step-like decrease of the chemical potential is seen. Thus, the present results provide compelling evidence that the origin of the reemerging superconductivity in $A_{1-x}$Fe$_{2-y}$Se$_2$ in vicinity of a quantum critical transition is caused mainly by the changes in the electronic structure.
Temperature and magnetic field studies of the elastic constants of the chromium spinel CdCr_2O_4 show pronounced anomalies related to strong spin-phonon coupling in this frustrated antiferromagnet. A detailed comparison of the longitudinal acoustic mode propagating along the [111] direction with theory based on an exchange-striction mechanism leads to an estimate of the strength of the magneto-elastic interaction. The derived spin-phonon coupling constant is in good agreement with previous determinations based on infrared absorption. Further insight is gained from intermediate and high magnetic field experiments in the field regime of the magnetization plateau. The role of the antisymmetric Dzyaloshinskii-Moriya interaction discussed and we compare the spin-phonon coupling in CdCr_2O_4 in both the ordered and disordered states.
Femtosecond laser excitation of solid-state systems creates non-equilibrium hot electrons that cool down by transferring their energy to other degrees of freedom and ultimately to lattice vibrations of the solid. By combining ab initio calculations with ultrafast diffuse electron scattering we gain a detailed understanding of the complex non-equilibrium energy transfer between electrons and phonons in laser-excited Ni metal. Our experimental results show that the wavevector resolved population dynamics of phonon modes is distinctly different throughout the Brillouin zone and are in remarkable agreement with our theoretical results. We find that zone-boundary phonon modes become occupied first. As soon as the energy in these modes becomes larger than the average electron energy a backflow of energy from lattice to electronic degrees of freedom occurs. Subsequent excitation of lower-energy phonon modes drives the thermalization of the whole system on the picosecond timescale. We determine the evolving non-equilibrium phonon occupations which we find to deviate markedly from thermal occupations.
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