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Magnetic relaxation phenomena in Cu$_2$OSeO$_3$ and phase diagram

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 Added by Fengjiao Qian
 Publication date 2016
  fields Physics
and research's language is English




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We present an investigation of the magnetic field-temperature phase diagram of Cu$_2$OSeO$_3$ based on DC magnetisation and AC susceptibility measurements covering a broad frequency range of four orders of magnitude, from very low frequencies reaching 0.1 Hz up to 1 kHz. The experiments were performed in the vicinity of $T_C=58.2$ K and around the skyrmion lattice A-phase. At the borders between the different phases the characteristic relaxation times reach several milliseconds and the relaxation is non-exponential. Consequently the borders between the different phases depend on the specific criteria and frequency used and an unambiguous determination is not possible.



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93 - F. Qian , H. Wilhelm , A. Aqeel 2016
The magnetic phase diagram of the chiral magnet Cu$_2$OSeO$_3$ has been investigated by dc magnetisation and ac susceptibility over a very large frequency range from 0.1 Hz up to 1 kHz and temperatures below 50 K. Qualitatively different phase diagrams have been obtained by applying the magnetic field along the easy $langle100rangle$ or the hard $langle110rangle$ crystallographic directions. Strong $chi$ appears close to $B_{c2}$, but only below 30 K and is more pronounced when $B$ is applied along $langle100rangle$. In addition, the transition from the helical to the conical phase leads to two adjacent $B_{c1}$ lines below 50 K. The frequency dependence of $chi$ indicates the existence of very broad distributions of relaxation times both at $B_{c1}$ and $B_{c2}$. The associated very long characteristic times eventually prevent the system from reaching thermal equilibrium at low temperatures and lead to thermal hysteresis.
Magnetic skyrmions are nano-sized topological spin textures stabilized by a delicate balance of magnetic energy terms. The chemical substitution of the underlying crystal structure of skyrmion-hosting materials offers a route to manipulate these energy contributions, but also introduces additional effects such as disorder and pinning. While the effects of doping and disorder have been well studied in B20 metallic materials such as Fe$_{1-x}$Co$_x$Si and Mn$_{1-x}$Fe$_x$Si, the consequences of chemical substitution in the magnetoelectric insulator Cu$_2$OSeO$_3$ have not been fully explored. In this work, we utilize a combination of AC magnetometry and small angle neutron scattering to investigate the magnetic phase transition dynamics in pristine and Zn-substituted Cu$_2$OSeO$_3$. The results demonstrate that the first order helical-conical phase transition exhibits two thermally separated behavioural regimes: at high temperatures, the helimagnetic domains transform by large-scale, continuous rotations, while at low temperatures, the two phases coexist. Remarkably, the effects of pinning in the substituted sample are less prevalent at low temperatures, compared to high temperatures, despite the reduction of available thermal activation energy. We attribute this behaviour to the large, temperature-dependent, cubic anisotropy unique to Cu$_2$OSeO$_3$, which becomes strong enough to overcome the pinning energy at low temperatures. Consideration and further exploration of these effects will be crucial when engineering skyrmion materials towards future applications.
We report small angle X-ray scattering (SAXS) measurements of the skyrmion lattice in two 200~nm thick Cu$_2$OSeO$_3$ lamellae aligned with the applied magnetic field parallel to the out of plane [110] or [100] crystallographic directions. Our measurements show that the equilibrium skyrmion phase in both samples is expanded significantly compared to bulk crystals, existing between approximately 30 and 50~K over a wide region of magnetic field. This skyrmion state is elliptically distorted at low fields for the [110] sample, and symmetric for the [100] sample, possibly due to crystalline anisotropy becoming more important at this sample thickness than it is in bulk samples. Furthermore, we find that a metastable skyrmion state can be observed at low temperature by field cooling through the equilibrium skyrmion pocket in both samples. In contrast to the behavior in bulk samples, the volume fraction of metastable skyrmions does not significantly depend on cooling rate. We show that a possible explanation for this is the change in the lowest temperature of the skyrmion state in this lamellae compared to bulk, without requiring different energetics of the skyrmion state.
The cubic chiral helimagnets with the $P2_13$ space group represent a group of compounds in which the stable skyrmion-lattice state is experimentally observed. The key parameter that controls the energy landscape of such systems and determines the emergence of a topologically nontrivial magnetic structures is the Dzyaloshinskii-Moriya interaction (DMI). Chemical substitution is recognized as a convenient instrument to tune the DMI in real materials and has been successfully utilized in studies of a number of chiral magnets, such as MnSi, FeGe, MnGe, and others. In our study, we applied small-angle neutron scattering to investigate how chemical substitution influences the skyrmionic properties of an insulating helimagnet Cu$_2$OSeO$_3$ when Cu ions are replaced by either Zn or Ni. Our results demonstrate that the DMI is enhanced in the Ni-substituted compounds (Cu,Ni)$_2$OSeO$_3$, but weakened in (Cu,Zn)$_2$OSeO$_3$. The observed changes in the DMI strength are reflected in the magnitude of the spin-spiral propagation vector and the temperature stability of the skyrmion phase.
We report small angle neutron scattering (SANS) measurements of the skyrmion lattice in (Cu$_{0.976}$Zn$_{0.024}$)$_2$OSeO$_3$ under the application of an electric field. These measurements show an expansion of the skyrmion lattice stability region with electric field similar to that seen in pristine Cu$_2$OSeO$_3$. Furthermore, using time-resolved SANS, we observe the slow formation of skyrmions after an electric or magnetic field is applied, which has not been observed in pristine Cu$_2$OSeO$_3$ crystals. The measured formation times are dramatically longer than the corresponding skyrmion destruction times after the external field is removed, and increase exponentially from 100~s at 52.5~K to 10,000~s at 51.5~K. This thermally activated behaviour indicates an energy barrier for skyrmion formation of 1.57(2)~eV, the size of which demonstrates the huge cost for creating these complex chiral objects.
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