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Register a new userMultiferroic behavior in the new double-perovskite Lu$_2$MnCoO$_6$
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We present a new member of the multiferroic oxides, Lu$_2$MnCoO$_6$, which we have investigated using X-ray diffraction, neutron diffraction, specific heat, magnetization, electric polarization, and dielectric constant measurements. This material possesses an electric polarization strongly coupled to a net magnetization below 35 K, despite the antiferromagnetic ordering of the $S = 3/2$ Mn$^{4+}$ and Co$^{2+}$ spins in an $uparrow uparrow downarrow downarrow$ configuration along the c-direction. We discuss the magnetic order in terms of a condensation of domain boundaries between $uparrow uparrow$ and $downarrow downarrow$ ferromagnetic domains, with each domain boundary producing a net electric polarization due to spatial inversion symmetry breaking. In an applied magnetic field the domain boundaries slide, controlling the size of the net magnetization, electric polarization, and magnetoelectric coupling.
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A$_2$BB$^prime$X$_6$ halide double perovskites based on bismuth and silver have recently been proposed as potential environmentally-friendly alternatives to lead-based hybrid halide perovskites. In particular, Cs$_2$BiAgX$_6$ (X = Cl, Br) have been synthesized and found to exhibit band gaps in the visible range. However, the band gaps of these compounds are indirect, which is not ideal for applications in thin film photovoltaics. Here, we propose a new class of halide double perovskites, where the B$^{3+}$ and B$^{+}$ cations are In$^{3+}$ and Ag$^{+}$, respectively. Our first-principles calculations indicate that the hypothetical compounds Cs$_2$InAgX$_6$ (X = Cl, Br, I) should exhibit direct band gaps between the visible (I) and the ultraviolet (Cl). Based on these predictions, we attempt to synthesize Cs$_2$InAgCl$_6$ and Cs$_2$InAgBr$_6$, and we succeed to form the hitherto unknown double perovskite Cs$_2$InAgCl$_6$. X-ray diffraction yields a double perovskite structure with space group $Fmoverline{3}m$. The measured band gap is 3.3 eV, and the compound is found to be photosensitive and turns reversibly from white to orange under ultraviolet illumination. We also perform an empirical analysis of the stability of Cs$_2$InAgX$_6$ and their mixed halides based on Goldschmidts rules, and we find that it should also be possible to form Cs$_2$InAg(Cl$_{1-x}$Br$_{x}$)$_6$ for $x<1$. The synthesis of mixed halides will open the way to the development of lead-free double perovskites with direct and tunable band gaps.
Identification of kinetic and thermodynamic factors that control crystal nucleation and growth represents a central challenge in materials synthesis. Here we report that apparently defect-free growth of La$_2$MnNiO$_6$ (LMNO) thin films supported on SrTiO$_3$ (STO) proceeds up to $1-5$ nm, after which it is disrupted by precipitation of NiO phases. Local geometric phase analysis and ensemble-averaged X-ray reciprocal space mapping show no change in the film strain away from the interface, indicating that mechanisms other than strain relaxation induce the formation of the NiO phases. $Ab , initio$ simulations suggest that oxygen vacancies become more likely with increasing thickness, due to the electrostatic potential build-up associated with the polarity mismatch at the film-substrate interface, this, in turn, promotes the formation of Ni-rich regions. These results suggest that the precipitate-free region could be extended further by increasing the oxygen chemical potential through the use of an elevated oxygen pressure or by incorporating electron redistributing dopants to suppress the built-in potential.
We study the magnetic properties of CaFeTi$_2$O$_6$ (CFTO) by high-field magnetization and specific heat measurements. While the magnetic susceptibility data yield a vanishingly small Curie-Weiss temperature, the magnetic moments are not fully polarized in magnetic field up to 60 T, which reveals a large spin exchange energy scale. Yet, the system shows no long range magnetic order but a spin-glass-like state below 5.5 K in zero field, indicating strong magnetic frustration in this system. Applying magnetic field gradually suppresses the spin-glass-like state and gives rise to a potential quantum spin liquid state whose low-temperature specific heat exhibits a $T^{1.6}$ power-law. Crucially, conventional mechanisms for frustration do not apply to this system as it possesses neither apparent geometrical frustration nor exchange frustration. We suggest that the orbital modulation of exchange interaction is likely the source of hidden frustration in CFTO, and its full characterization may open a new route in the quest for quantum spin liquids.
We investigate a magnetic hysteresis loop with a remanent moment that couples to electric polarization to create coupled hysteretic multiferroic behavior in Lu2MnCoO6. Measurements of elastic neutron diffraction, muon spin relaxation, and micro-Hall magnetometry demonstrate an unusual mechanism for the magnetic hysteresis, namely the hysteretic evolution of a microscopic magnetic order, and not classic ferromagnetic domain effects. We show how the frustrated spin system evolves from antiferromagnetism with an incommensurate long-wavelength modulation and strong fluctuations towards a net magnetism. We also clarify the different temperature scales for the onset of ordering, dynamics, and hysteresis.
Sr$_2$CuWO$_6$ is a double perovskite proposed to be at the border between two and three dimensional magnetism, with a square lattice of $S=frac{1}{2}$ Cu$^{2+}$ ions. We have used inelastic neutron scattering to investigate the spin wave excitations of the system, to find out how they evolve as a function of temperature, as well as to obtain information about the magnetic exchange interactions. We observed well defined dispersive spin wave modes at $6$~K, which partially survive above the magnetic ordering temperature, $T_N=24$~K. Linear spin wave theory is used to determine the exchange interactions revealing them to be highly two-dimensional in nature. Density functional theory calculations are presented supporting this experimental finding, which is in contrast to a previous emph{ab-initio} study of the magnetic interactions. Our analysis confirms that not the nearest neighbour, but the next nearest neighbour interactions in the tetragonal $ab$ plane are the strongest. Low incident energy measurements reveal the opening of a $0.6(1)$~meV gap below $T_N$, which suggests the presence of a very weak single ion anisotropy term in the form of an easy axis along $hat{mathbf{a}}$.
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