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Register a new userInfluence of oxygen isotope exchange on the ground state of manganites
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Added by
Vera N. Smolyaninova
Publication date
2001
fields
Physics
and research's language is
English
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We report a study of oxygen isotope effects on low temperature specific heat, magnetization, and resistivity of La$_{1-x}$Ca$_{x}$MnO$_{3}$ and (La$_{1-y}$Pr$_{y})_{0.67}$Ca$_{0.33}$MnO$_{3}$. For the metallic compositions of La$_{1-x}$Ca$_{x}$MnO$_{3}$ and for charge-ordered La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ no change in low temperature specific heat has been detected with $^{16}$O -$^{18}$O exchange, while compounds of (La$_{1-y}$Pr$_{y})_{0.67}$Ca$_{0.33}$MnO$_{3}$ (0.4<y<0.6) show a significant change in low temperature properties. The low temperature specific heat indicates a presence of the charge-ordered phase even in compositions of (La$_{1-y}$Pr$_{y})_{0.67}$Ca$_{0.33}$MnO$_{3}$ which are metallic at low temperatures. We suggest that the changes induced by the oxygen isotope exchange are caused by an increase of the charge-ordered phase in $^{18}$O samples.
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In this paper, we discuss the most deleterious effect of charge state modification at the Mn site on the ground state of the CMR manganites.
Oxygen isotope effects on the transport properties have been studied in high-quality epitaxial thin films of La_{0.75}Ca_{0.25}MnO_{3} and Nd_{0.7}Sr_{0.3}MnO_{3}. In the paramagnetic state, the resistivity can be well fitted by rho (T) = (A/sqrt{T})exp(E_{rho}/k_{B}T) with the parameters A and E_{a} depending strongly on the oxygen isotope mass. The resistivity below 80 K almost perfectly follows rho = rho_{o}+ Bomega_{s}/sinh^{2}(hbaromega_{s}/2k_{B}T) with hbaromega_{s}/k_{B} sim 100 K. Both rho_{o} and B increase by about 15(3)% upon raplacing $^{16}$O by $^{18}$O. The results provide quantitative constraints on the basic physics of manganites.
We study the mechanism of orbital-order melting observed at temperature T_OO in the series of rare-earth manganites. We find that many-body super-exchange yields a transition-temperature T_KK that decreases with decreasing rare-earth radius, and increases with pressure, opposite to the experimental T_OO. We show that the tetragonal crystal-field splitting reduces T_KK further increasing the discrepancies with experiments. This proves that super-exchange effects, although very efficient, in the light of the experimentally observed trends, play a minor role for the melting of orbital ordering in rare-earth manganites.
In a recent paper, Nagaev cited the unpublished paper by Franck et al.to support his theoretical model for the mechanism of the giant isotope effect observed in La_{1-x}Ca_{x}MnO_{3+y} (x = 0.20, y > 0). His model suggests that the off-stoichiometric oxygen content depends strongly on the oxygen isotope mass, which leads to a giant oxygen-isotope effect. Here I show that his theoretical model is not consistent with any experimental results (even the results recently published by Franck et al.), and his estimate of polaronic bandwidth is wrong due to his misuse of polaronic theories.
Magnetism of transition metal (TM) oxides is usually described in terms of the Heisenberg model, with orientation-independent interactions between the spins. However, the applicability of such a model is not fully justified for TM oxides because spin polarization of oxygen is usually ignored. In the conventional model based on the Anderson principle, oxygen effects are considered as a property of the TM ion and only TM interactions are relevant. Here, we perform a systematic comparison between two approaches for spin polarization on oxygen in typical TM oxides. To this end, we calculate the exchange interactions in NiO, MnO, and hematite (Fe2O3) for different magnetic configurations using the magnetic force theorem. We consider the full spin Hamiltonian including oxygen sites, and also derive an effective model where the spin polarization on oxygen renormalizes the exchange interactions between TM sites. Surprisingly, the exchange interactions in NiO depend on the magnetic state if spin polarization on oxygen is neglected, resulting in non-Heisenberg behavior. In contrast, the inclusion of spin polarization in NiO makes the Heisenberg model more applicable. Just the opposite, MnO behaves as a Heisenberg magnet when oxygen spin polarization is neglected, but shows strong non-Heisenberg effects when spin polarization on oxygen is included. In hematite, both models result in non-Heisenberg behavior. General applicability of the magnetic force theorem as well as the Heisenberg model to TM oxides is discussed.
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