Critical speeding-up near the monopole liquid-gas transition in magnetoelectric spin-ice

Competing interactions in the so-called spin-ice compounds stabilize a frustrated ground-state with finite zero-point entropy and, interestingly, emergent magnetic monopole excitations. The properties of these monopoles are at the focus of recent research with particular emphasis on their quantum dynamics. It is predicted that each monopole also possesses an electric dipole moment, which allows to investigate their dynamics via the dielectric function \epsilon(\nu). Here, we report on broadband spectroscopic measurements of \epsilon(\nu) in Dy2Ti2O7 down to temperatures of 200mK with a specific focus on the critical endpoint present for a magnetic field along the crystallographic [111] direction. Clear critical signatures are revealed in the dielectric response when, similarly as in the liquid-gas transition, the density of monopoles changes in a critical manner. Surprisingly, the dielectric relaxation time \tau\ exhibits a critical speeding-up with a significant enhancement of 1/\tau\ as the temperature is lowered towards the critical temperature. Besides demonstrating the magnetoelectric character of the emergent monopole excitations, our results reveal unique critical dynamics near the monopole condensation transition.Comment: Changes: Data shown and discussed as function of internal field H and flux density B, Figs.3&4 rearranged, references adde

Critical slowing down near the multiferroic phase transition in MnWO4_4

By using broadband dielectric spectroscopy in the radiofrequency and microwave range we studied the magnetoelectric dynamics in the multiferroic chiral antiferromagnet MnWO$_4$. Above the multiferroic phase transition at $T_{N2} \approx 12.6$ K we observe a critical slowing down of the corresponding magnetoelectric fluctuations resembling the soft-mode behavior in canonical ferroelectrics. This electric field driven excitation carries much less spectral weight than ordinary phonon modes. Also the critical slowing down of this mode scales with an exponent larger than one which is expected for magnetic second order phase transition scenarios. Therefore the investigated dynamics have to be interpreted as the softening of an electrically active magnetic excitation, an electromagnon.Comment: 5 pages, 4 figures, appendi

Multiferroicity and colossal magneto-capacitance in Cr-thiospinels

The sulfur based Cr-spinels RCr2S4 with R = Cd and Hg exhibit the coexistence of ferromagnetic and ferroelectric properties together with a pronounced magnetocapacitive coupling. While in CdCr2S4 purely ferromagnetic order is established, in HgCr2S4 a bond-frustrated magnetic ground state is realized, which, however, easily can be driven towards a ferromagnetic configuration in weak magnetic fields. This paper shall review our recent investigation for both compounds. Besides the characterization of the magnetic properties, the complex dielectric permittivity was studied by means of broadband dielectric spectroscopy as well as measurements of polarization hysteresis and pyro-currents. The observed colossal magneto-capacitive effect at the magnetic transition seems to be driven by an enormous variation of the relaxation dynamics.Comment: 10 pages, 11 figure

Colossal magnetocapacitance and colossal magnetoresistance in HgCr2S4

We present a detailed study of the dielectric and charge transport properties of the antiferromagnetic cubic spinel HgCr2S4. Similar to the findings in ferromagnetic CdCr2S4, the dielectric constant of HgCr2S4 becomes strongly enhanced in the region below 60 - 80 K, which can be ascribed to polar relaxational dynamics triggered by the onset of ferromagnetic correlations. In addition, the observation of polarization hysteresis curves indicates the development of ferroelectric order below about 70 K. Moreover, our investigations in external magnetic fields up to 5 T reveal the simultaneous occurrence of magnetocapacitance and magnetoresistance of truly colossal magnitudes in this material.Comment: 4 pages, 4 figure

Multiferroic behavior in CdCr2X4 (X = S, Se)

The recently discovered multiferroic material CdCr2S4 shows a coexistence of ferromagnetism and relaxor ferroelectricity together with a colossal magnetocapacitive effect. The complex dielectric permittivity of this compound and of the structurally related CdCr2Se4 was studied by means of broadband dielectric spectroscopy using different electrode materials. The observed magnetocapacitive coupling at the magnetic transition is driven by enormous changes of the relaxation dynamics induced by the development of magnetic order

Magnetic-field-induced critical dynamics in magnetoelectric TbPO4_4

We report on the magnetoelectric dynamics in the linear magnetoelectric antiferromagnet TbPO$_4$ studied by broadband dielectric spectroscopy. For the phase transition into the magnetoelectric antiferromagnetic phase at $T_{N} \approx 2.3$ K, a finite magnetic field $H$ induces critical behavior in the quasi-static permittivity $\varepsilon'$. Plotting the corresponding anomaly as function of $T/T_N(H)$, we observe the scaling behavior $\Delta \varepsilon' \propto H^2$, a clear fingerprint of linear magnetoelectric antiferromagnets. Above the phase transition, we find a critical slowing down of the ferroic fluctuations in finite magnetic field. This behaviour can be understood via a magnetic-field-induced relaxational response that resembles the soft-mode behaviour in canonical ferroelectrics and multiferroics

Context-dependent detection of fungal parasites in four ant species

The reaction between the allyl radical (C3H5˙) and acetylene (C2H2) in a heated microtubular reactor has been studied at the VUV beamline of the Swiss Light Source. The reaction products are sampled from the reactor and identified by their photoion mass-selected threshold photoelectron spectra (ms-TPES) by means of imaging photoelectron photoion coincidence spectroscopy. Cyclopentadiene is identified as the sole reaction product by comparison of the measured photoelectron spectrum with that of cyclopentadiene. With the help of quantum-chemical computations of the C5H7 potential energy surface, the C2H2 + C3H5˙ association reaction is confirmed to be the rate determining step, after which H-elimination to form C5H6 is prompt in the absence of re-thermalization at low pressures. The formation of cyclopentadiene as the sole product from the allyl + acetylene reaction offers a direct path to the formation of cyclic hydrocarbons under combustion relevant conditions. Subsequent reactions of cyclopentadiene may lead to the formation of the smallest polycyclic aromatic molecule, naphthalene

Polar phonons and spin-phonon coupling in HgCr2S4 and CdCr2S4

Polar phonons of HgCr2S4 and CdCr2S4 are studied by far-infrared spectroscopy as a function of temperature and external magnetic field. Eigenfrequencies, damping constants, effective plasma frequencies and Lyddane-Sachs-Teller relations, and effective charges are determined. Ferromagnetic CdCr2S4 and antiferromagnetic HgCr2S4 behave rather similar. Both compounds are dominated by ferromagnetic exchange and although HgCr2S4 is an antiferromagnet, no phonon splitting can be observed at the magnetic phase transition. Temperature and magnetic field dependence of the eigenfrequencies show no anomalies indicating displacive polar soft mode behavior. However, significant effects are detected in the temperature dependence of the plasma frequencies indicating changes in the nature of the bonds and significant charge transfer. In HgCr2S4 we provide experimental evidence that the magnetic field dependence of specific polar modes reveal shifts exactly correlated with the magnetization showing significant magneto-dielectric effects even at infrared frequencies.Comment: 8 pages, 8 figure

Electron-phonon and spin-phonon coupling in NaV2_{2}O5_{5}: charge fluctuations effect

We show that the asymmetric crystal environment of the V site in the ladder compound NaV$_{2}$O$_{5}$ leads to a strong coupling of vanadium 3d electrons to phonons. This coupling causes fluctuations of the charge on the V ions, and favors a transition to a charge-ordered state at low temperatures. In the low temperature phase the charge fluctuations modulate the spin-spin superexchange interaction, resulting in a strong spin-phonon coupling.Comment: Europhysics Letters, to be publishe

31P NMR study of Na2CuP2O7: a S=1/2 two-dimensional Heisenberg antiferromagnetic system

The magnetic properties of Na2CuP2O7 were investigated by means of 31P nuclear magnetic resonance (NMR), magnetic susceptibility, and heat capacity measurements. We report the 31P NMR shift, the spin-lattice 1/T1, and spin-spin 1/T2 relaxation-rate data as a function of temperature T. The temperature dependence of the NMR shift K(T) is well described by the S=1/2 square lattice Heisenberg antiferromagnetic (HAF) model with an intraplanar exchange of J/k_B \simeq 18\pm2 K and a hyperfine coupling A = (3533\pm185) Oe/mu_B. The 31P NMR spectrum was found to broaden abruptly below T \sim 10 K signifying some kind of transition. However, no anomaly was noticed in the bulk susceptibility data down to 1.8 K. The heat capacity appears to have a weak maximum around 10 K. With decrease in temperatures, the spin-lattice relaxation rate 1/T1 decreases monotonically and appears to agree well with the high temperature series expansion expression for a S = 1/2 2D square lattice.Comment: 12 pages, 8 figures, submitted to J. Phys.: Cond. Ma