Abstract
A systematic study of the consequences of in-plane tensile strain on the correlation between structure/microstructure and magneto-electrical properties of La0.23Pr0.41Ca0.36MnO3/SrTiO3 (001) thin films is performed. At lower film thickness (d≤27 nm) the dominant tensile strain supports layered morphology. At d=41 nm structural/microstructural crossover takes place and at d≥41 nm relaxation induced tilt and dilations of the lattice generate defects like dislocations, which in turn transforms the layer by layer growth into disordered brick type morphology. It appears that the relaxation even at higher thickness (∼81 nm) is partial only and the strain may have a self-sustained nature. The domination of the tensile strain suppresses the ferromagnetic-metallic phase due to the possible electronic reconstruction which could give rise to a magnetically disordered insulator ‘dead’ layer and a sizeable non-magnetic insulator state at d≤27 nm. In this thickness regime the possible selective orbital stabilization could also contribute to carrier localization. At d≥41 nm the severity of the impact of the interfacial electronic reconstruction is reduced with concomitant relaxation of the tensile strain which favors carrier delocalization and yields well defined metallic-ferromagnetic phase transitions. The hysteretic nature of the phase transitions reflects the thermal cycle dependent nature of the metallic-ferromagnetic and insulating antiferromagnetic phases in this strongly phase separated material.
Highlights
The generic perovskite manganese oxides RE1-xAExMnO3 (RE being a trivalent rare earth ion and AE a divalent one, commonly an alkaline earth) are metallic and ferromagnetic over a certain range of x-values, which is dependent on the average size of the RE/AE site cations and the tolerance factor.[1,2,3,4] The major electronic properties of these compounds are controlled by the 3d orbitals and the simultaneous ferromagnetic and metallic behaviors are explained to a certain extent by the double-exchange (DE) mechanism proposed by Zener, wherein it was considered that the interatomic Hund rule exchange was strong and carriers do not change their spin orientation while hoping from one ion to
The slight difference in the chemical stoichiometry of the target and the thin films shows the inexact stoichiometry transfer in the RF magnetron sputtering process employed in the present growth process
We would like to mention that in our earlier study on La0.18P0.40Ca0.42MnO3 thin films we have found similar trend even in compressively strain thin films on LaAlO3 substrates.[24]
Summary
The generic perovskite manganese oxides RE1-xAExMnO3 (RE being a trivalent rare earth ion and AE a divalent one, commonly an alkaline earth) are metallic and ferromagnetic over a certain range of x-values, which is dependent on the average size of the RE/AE site cations and the tolerance factor.[1,2,3,4] The major electronic properties of these compounds are controlled by the 3d orbitals and the simultaneous ferromagnetic and metallic behaviors are explained to a certain extent by the double-exchange (DE) mechanism proposed by Zener, wherein it was considered that the interatomic Hund rule exchange was strong and carriers do not change their spin orientation while hoping from one ion to next. A prototypical low bandwidth compound which shows very prominent multiorder electronic coupling and has been investigated extensively is La1-x-yPryCaxMnO3 In such compounds which exhibit nearly isoenergetic existence of multiple electronic phases (like FM and AFM/COI) even the subtle changes in the substrate induced strain (and the variation in the film thickness) can modify the electronic phase profile and associated phase transitions.[11,15,16,17,18,19,20,21,22,23,24] In addition to the phase transitions, the strain could impact the non-equilibrium states like the magnetic liquid and the strain glass (SRG).[24]. In the present study we have selected a composition in which the electronic phase balance is tilted slightly in favor of the FM metal (the bandwidth in the present study is between those investigated in references 19 and 24) Such a selection gives a possibility of the occurrence of FM-metallic behavior even at sufficiently small film thickness where the tensile strain is very large. In the present study we have investigated films having different thicknesses in the range 13 - 81 nm
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