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Probing ultrafast spin dynamics in the antiferromagnetic multiferroic HoMnO$_3$ through a magnon resonance

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 Added by Pamela Bowlan
 Publication date 2016
  fields Physics
and research's language is English




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We demonstrate a new approach for directly measuring the ultrafast energy transfer between elec- trons and magnons, enabling us to track spin dynamics in an antiferromagnet (AFM). In multiferroic HoMnO3, optical photoexcitation creates hot electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced transparency, which builds up over several picoseconds as the spins heat up due to energy transfer from hot elec- trons via phonons. This spin-lattice thermalization time is ?10 times faster than that of typical ferromagnetic (FM) manganites. We qualitatively explain the fundamental differences in spin-lattice thermalization between FM and AFM systems and apply a Boltzmann equation model for treating AFMs. Our work gives new insight into spin-lattice thermalization in AFMs and demonstrates a new approach for directly monitoring the ultrafast dynamics of spin order in these systems.

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The symmetric splitting of two spin-wave branches in an antiferromagnetic resonance (AFR) experiment has been an essential measurement of antiferromagnets for over half a century. In this work, circularly polarized time-domain THz spectroscopy experiments performed on the low symmetry multiferroic h-HoMnO$_3$ reveal an AFR of the Mn sublattice to split asymmetrically in applied magnetic field, with an $approx$ 50% difference in $g$-factors between the high and low energy branches of this excitation. The temperature dependence of the $g$-factors, including a drastic renormalization at the Ho spin ordering temperature, reveals this asymmetry to unambiguously stem from Ho-Mn interactions. Theoretical calculations demonstrate the AFR asymmetry is not explained by conventional Ho-Mn exchange mechanisms alone and are only reproduced if quartic spin interactions are also included in the spin Hamiltonian. Our results provide a paradigm for the optical study of such novel interactions in hexagonal manganites and low symmetry antiferromagnets in general.
In the multiferroic hexagonal manganite HoMnO3, inelastic neutron scattering and synchrotron based THz spectroscopy have been used to investigate the spin waves associated to the Mn order together with Ho crystal field excitations. While the Mn order sets in first below 80 K, a spin reorientation occurs below 37 K, a rare feature in the rare earth manganites. We show that severalHo crystal field excitations are present in the same energy range as the magnons, and that they are all affected by the spin reorientation. Moreover, several anomalous features are observed in the excitations at low temperature. Our analysis and calculations for the Mn spin waves and Ho crystal field excitations support Mn-Ho coupling mechanisms as well as coupling to the lattice affecting the dynamics.
NiNb$_{2}$O$_{6}$ is an almost ideal realization of a 1D spin-1 ferromagnetic Heisenberg chain compound with weak unidirectional anisotropy. Using time-domain THz spectroscopy, we measure the low-energy electrodynamic response of NiNb$_{2}$O$_{6}$ as a function of temperature and external magnetic field. At low temperatures, we find a magnon-like spin-excitation, which corresponds to the lowest energy excitation at $qsim0$. At higher temperatures, we unexpectedly observe a temperature-dependent renormalization of the spin-excitation energy, which has a strong dependence on field direction. Using theoretical arguments, exact diagonalizations and finite temperature dynamical Lanczos calculations, we construct a picture of magnon-magnon interactions that naturally explains the observed renormalization. This unique scenario is a consequence of the spin-1 nature and has no analog in the more widely studied spin-1/2 systems.
Using THz spectroscopy, we show that the spin-wave spectrum of multiferroic BiFeO$_3$ in its high-field canted antiferromagnetic state is well described by a spin model that violates rhombohedral symmetry. We demonstrate that the monoclinic distortion of the canted antiferromagnetic state is induced by the single-ion magnetoelastic coupling between the lattice and the two nearly anti-parallel spins. The revised spin model for BiFeO$_3$ contains two new single-ion anisotropy terms that violate rhombohedral symmetry and depend on the direction of the magnetic field.
Inelastic neutron scattering has been used to study the magneto-elastic excitations in the multiferroic manganite hexagonal YMnO$_3$. An avoided crossing is found between magnon and phonon modes close to the Brillouin zone boundary in the $(a,b)$-plane. Neutron polarization analysis reveals that this mode has mixed magnon-phonon character. An external magnetic field along the $c$-axis is observed to cause a linear field-induced splitting of one of the spin wave branches. A theoretical description is performed, using a Heisenberg model of localized spins, acoustic phonon modes and a magneto-elastic coupling via the single-ion magnetostriction. The model quantitatively reproduces the dispersion and intensities of all modes in the full Brillouin zone, describes the observed magnon-phonon hybridized modes, and quantifies the magneto-elastic coupling. The combined information, including the field-induced magnon splitting, allows us to exclude several of the earlier proposed models and point to the correct magnetic ground state symmetry, and provides an effective dynamic model relevant for the multiferroic hexagonal manganites.
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