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Register a new userRevealing magnetoelectric coupling effect in polar antiferromagnet Fe$_2$Mo$_3$O$_8$ by static and time resolved second harmonic generation
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We present both static and time-resolved second harmonic generation (SHG) measurements on polar antiferromagnet Fe$_2$Mo$_3$O$_8$ to monitor the evolution of the electric polarization change and its coupling to magnetic order. We find that only one of the second order tensor elements, $chi_{ccc}^{(2)}$ ,shows a prominent change below the Neel temperature $T_N = 60$ K, indicating a magnetic order induced electric polarization change along the c-axis. Time-resolved SHG measurement reveals an ultrafast recovery of the second order tensor element upon the ultrashort laser excitation with fluence above 0.3 $mJ/cm^2$, yielding evidence for a photoinduced ultrafast phase transition from the AFM ordered state to the paramagnetic state. Our work will help understand the spin induced polarization and the ultrafast optical tuning effect in Fe$_{2}$Mo$_{3}$O$_{8}$.
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We report on the structural and spectroscopic characterization of the multiferroic Fe$_2$Mo$_3$O$_8$. Synchrotron x-ray and neutron diffraction, as well as thermal expansion measurements reveal a lattice anomaly at $T_{mathrm{N}}simeq 60,$K but do not show any symmetry lowering in the magnetically ordered state. The lattice parameter $c$ exhibits a non-monotonic behavior with a pronounced minimum around $200,$K, which is also reflected in an anomalous behavior of some of the observed infrared-active optical excitations and parallels the onset of short-range magnetic order. The infrared reflectivity spectra measured between 5 and 300$,$K in the frequency range of $100-8000,$cm$^{-1}$ reveal most of the expected phonon modes in comparison with the eigenfrequencies obtained by density-functional calculations. The $A_1$ phonons show an overall hardening upon cooling, whereas a non-monotonic behavior is observed for some of the $E_1$ modes. These modes also show a strongly increased phonon lifetime below $T_mathrm{N}$, which we associate with the quenched direction of the orbital moment in the magnetically ordered state. A similar increase is observed in the lifetime of the higher-lying $d$-$d$ excitations of the tetrahedral Fe$^{2+}$ site, which become clearly visible below $T_mathrm{N}$ only.
We report on optical excitations in the magnetically ordered phases of multiferroic Fe$_{1.86}$Zn$_{0.14}$Mo$_3$O$_8$ in the frequency range from 10-130 cm$^{-1}$ (0.3-3.9 THz). In the collinear easy-axis antiferromagnetic phase below $T_N=50$~K eleven optically active modes have been observed in finite magnetic fields, assuming that the lowest-lying mode is doubly degenerate. The large number of modes reflects either a more complex magnetic structure than in pure Fe$_{2}$Mo$_3$O$_8$ or that spin stretching modes become active in addition to the usual spin precessional modes. Their magnetic field dependence, for fields applied along the easy axis, reflects the irreversible magnetic-field driven phase transition from the antiferromagnetic ground state to a ferrimagnetic state, while the number of modes remains unchanged in the covered frequency region. We determined selection rules for some of the AFM modes by investigating all polarization configurations and identified magnetic- and electric-dipole active modes as well. In addition to these sharp resonances, a broad electric-dipole active excitation band, which is not influenced by the external magnetic field, occurs below $T_N$ with an onset at 12 cm$^{-1}$. We are able to model this absorption band as a vibronic excitation related to the lowest-lying Fe$^{2+}$ electronic states in tetrahedral environment.
Strong coupling between magnon and electromagnetic wave can lead to the formation of a coupled spinphoton quasiparticle named as magnon-polariton. The phenomenon is well studied for ferromagnetic systems inside microwave cavities in recent years. However, formation of magnon-polariton is rarely seen for an antiferromagnet (AFM) because the strong coupling condition is not easily fulfilled. Here we present time-domain terahertz measurement on a multiferroic polar antiferromagnet Fe2Mo3O8. We find clearly beating between two modes at frequencies above and below the electric-active magnon frequency below TN, which we assign to the formation of AFM magnon-polariton. An ultra-strong spin-photon coupling effect is derived based on the energy level splitting. However, the AFM magnon-polariton is absent in the frequency domain measurement. Our work reveals that the coherent magnon formation driven by the ultrashort THz pulse provides a new way to detect polariton mode splitting.
LiZn$_2$Mo$_3$O$_8$ has been proposed to contain $S~=~1/2$ Mo$_3$O$_{13}$ magnetic clusters arranged on a triangular lattice with antiferromagnetic nearest-neighbor interactions. Here, microwave and terahertz electron spin resonance (ESR), $^7$Li nuclear magnetic resonance (NMR), and muon spin rotation ($mu textrm{SR}$) spectroscopies are used to characterize the local magnetic properties of LiZn$_2$Mo$_3$O$_8$. These results show the magnetism in LiZn$_2$Mo$_3$O$_8$ arises from a single isotropic $S~=~1/2$ electron per cluster and that there is no static long-range magnetic ordering down to $T~=~0.07,textrm{K}$. Further, there is evidence of gapless spin excitations with spin fluctuations slowing down as the temperature is lowered. These data indicate strong spin correlations which, together with previous data, suggest a low-temperature resonating valence-bond state in LiZn$_2$Mo$_3$O$_8$.
By combining single crystal x-ray and neutron diffraction, and the magnetodielectric measurements on single crystal Fe4Nb2O9, we present the magnetic structure and the symmetry-allowed magnetoelectric coupling in Fe4Nb2O9. It undergoes an antiferromagnetic transition at TN=93 K, followed by a displacive transition at TS=70 K. The temperature-dependent dielectric constant of Fe4Nb2O9 is strongly anisotropic with the first anomaly at 93 K due to the exchange striction as a result of the long range spin order, and the second one at 70 K emanating from the structural phase transition primarily driven by the O atomic displacements. Magneticfield induced magnetoelectric coupling was observed in single crystal Fe4Nb2O9 and is compatible with the solved magnetic structure that is characteristic of antiferromagnetically arranged ferromagnetic chains in the honeycomb plane. We propose that such magnetic symmetry should be immune to external magnetic fields to some extent favored by the freedom of rotation of moments in the honeycomb plane, laying out a promising system to control the magnetoelectric properties by magnetic fields.
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