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Title: Impact of nanostructuring on the magnetic and magnetocaloric properties of microscale phase-separated La 5/8–yPr yCa 3/8MnO₃ manganites

Abstract

Bulk manganites of the form La 5/8–yPr yCa 3/8MnO₃ (LPCMO) exhibit a complex phase diagram due to coexisting charge-ordered antiferromagnetic (CO/AFM), charge-disordered paramagnetic (PM), and ferromagnetic (FM) phases. Because phase separation in LPCMO occurs on the microscale, reducing particle size to below this characteristic length is expected to have a strong impact on the magnetic properties of the system. Through a comparative study of the magnetic and magnetocaloric properties of single-crystalline (bulk) and nanocrystalline LPCMO (y=3/8) we show that the AFM, CO, and FM transitions seen in the single crystal can also be observed in the large particle sizes (400 and 150 nm), while only a single PM to FM transition is found for the small particles (55 nm). Magnetic and magnetocaloric measurements reveal that decreasing particle size affects the balance of competing phases in LPCMO and narrows the range of fields over which PM, FM, and CO phases coexist. The FM volume fraction increases with size reduction, until CO is suppressed below some critical size, ~100 nm. With size reduction, the saturation magnetization and field sensitivity first increase as long-range CO is inhibited, then decrease as surface effects become increasingly important. The trend that the FM phase is stabilizedmore » on the nanoscale is contrasted with the stabilization of the charge-disordered PM phase occurring on the microscale, demonstrating that in terms of the characteristic phase separation length, a few microns and several hundred nanometers represent very different regimes in LPCMO.« less

Authors:
; ; ; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1103129
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Physical Review. B, Condensed Matter and Materials Physics
Additional Journal Information:
Journal Volume: 86; Journal Issue: 6; Related Information: CHORUS Timestamp: 2017-04-06 05:31:25; Journal ID: ISSN 1098-0121
Publisher:
American Physical Society
Country of Publication:
United States
Language:
English

Citation Formats

Bingham, N. S., Lampen, P., Phan, M. H., Hoang, T. D., Chinh, H. D., Zhang, C. L., Cheong, S. W., and Srikanth, H. Impact of nanostructuring on the magnetic and magnetocaloric properties of microscale phase-separated La5/8–yPryCa3/8MnO₃ manganites. United States: N. p., 2012. Web. doi:10.1103/PhysRevB.86.064420.
Bingham, N. S., Lampen, P., Phan, M. H., Hoang, T. D., Chinh, H. D., Zhang, C. L., Cheong, S. W., & Srikanth, H. Impact of nanostructuring on the magnetic and magnetocaloric properties of microscale phase-separated La5/8–yPryCa3/8MnO₃ manganites. United States. doi:10.1103/PhysRevB.86.064420.
Bingham, N. S., Lampen, P., Phan, M. H., Hoang, T. D., Chinh, H. D., Zhang, C. L., Cheong, S. W., and Srikanth, H. 2012. "Impact of nanostructuring on the magnetic and magnetocaloric properties of microscale phase-separated La5/8–yPryCa3/8MnO₃ manganites". United States. doi:10.1103/PhysRevB.86.064420.
@article{osti_1103129,
title = {Impact of nanostructuring on the magnetic and magnetocaloric properties of microscale phase-separated La5/8–yPryCa3/8MnO₃ manganites},
author = {Bingham, N. S. and Lampen, P. and Phan, M. H. and Hoang, T. D. and Chinh, H. D. and Zhang, C. L. and Cheong, S. W. and Srikanth, H.},
abstractNote = {Bulk manganites of the form La5/8–yPryCa3/8MnO₃ (LPCMO) exhibit a complex phase diagram due to coexisting charge-ordered antiferromagnetic (CO/AFM), charge-disordered paramagnetic (PM), and ferromagnetic (FM) phases. Because phase separation in LPCMO occurs on the microscale, reducing particle size to below this characteristic length is expected to have a strong impact on the magnetic properties of the system. Through a comparative study of the magnetic and magnetocaloric properties of single-crystalline (bulk) and nanocrystalline LPCMO (y=3/8) we show that the AFM, CO, and FM transitions seen in the single crystal can also be observed in the large particle sizes (400 and 150 nm), while only a single PM to FM transition is found for the small particles (55 nm). Magnetic and magnetocaloric measurements reveal that decreasing particle size affects the balance of competing phases in LPCMO and narrows the range of fields over which PM, FM, and CO phases coexist. The FM volume fraction increases with size reduction, until CO is suppressed below some critical size, ~100 nm. With size reduction, the saturation magnetization and field sensitivity first increase as long-range CO is inhibited, then decrease as surface effects become increasingly important. The trend that the FM phase is stabilized on the nanoscale is contrasted with the stabilization of the charge-disordered PM phase occurring on the microscale, demonstrating that in terms of the characteristic phase separation length, a few microns and several hundred nanometers represent very different regimes in LPCMO.},
doi = {10.1103/PhysRevB.86.064420},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
number = 6,
volume = 86,
place = {United States},
year = 2012,
month = 8
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1103/PhysRevB.86.064420

Citation Metrics:
Cited by: 23works
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  • The La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}Mn{sub 1−x}Fe{sub x}O{sub 3} (x=0, 0.1, 0.2 and 0.3) samples have been elaborated by the solid-state reaction method. X-ray powder diffraction shows that all the samples crystallize in a rhombohedric phase with R3{sup ¯}c space group. The variation of magnetization as a function of temperature and applied magnetic field was carried out. The samples for x=0 and 0.1 exhibit a FM–PM transition at the Curie temperature T{sub C}, however, for x=0.2 and 0.3 exhibit an AFM–PM one at the Neel temperature T{sub N}, when the temperature increases. A magneto-caloric effect has been calculated in terms ofmore » isothermal magnetic entropy change. A large magneto-caloric effect has been observed, the maximum entropy change, |ΔS{sub M}{sup max}|, reaches the highest value of 3.28 J/kgK under a magnetic field change of 5 T with an RCP value of 220 J/kg for La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}MnO{sub 3} composition, which will be an interesting compound for application materials working as magnetic refrigerants near room temperature. - Graphical abstract: Magnetic entropy change versus temperature and applied magnetic field for x=0.1 (a) and RCP versus applied magnetic field for x=0, 0.1 (b). - Highlights: • The La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}Mn{sub 1−x}Fe{sub x}O{sub 3} (0≤x≤0.3) polycrystalline samples were prepared by the solid state reaction method. • Crystalline and magnetic structures were investigated using DRX and magnetization measurements. • The magnetocaloric (MC) effect was estimated versus magnetic field and temperatures. • Compounds with x=0, 0.1 exhibit great potential for magnetic refrigeration at room temperature.« less
  • In this work, we report the effect of Na doping on the structural, magnetic and magnetocaloric properties in La{sub 0.8}Ca{sub 0.2−x}Na{sub x}MnO{sub 3} powder samples. Our polycristalline samples have been synthesized using the solid-state reaction method at high temperatures. The parent compound La{sub 0.8}Ca{sub 0.2}MnO{sub 3} crystallizes in the orthorhombic system with Pbnm space group. Na doping induces a structural transition from orthorhombic (Pbnm space group) to rhombohedral (R-3C space group) symmetry. Magnetization measurements versus temperature in a magnetic applied field of 50 mT showed that all our investigated samples display a paramagnetic-ferromagnetic transition with decreasing temperature. The Curie temperaturemore » T{sub C} increases with Na content from 240 K for x=0 to 330 K for x=0.2. A large magnetocaloric effect has been observed in all samples, the maximum entropy change, |∆S{sub M}|{sub max}, shifts to smaller values with increasing Na content, from4.56 J/kg K (x=0.05) to 2.3 J/kg K (x=0.2) under a magnetic field change ∆µ{sub 0}H of 2 T. For the same applied magnetic field of 2 T, the Relative Cooling Power (RCP) values are found to be constant around 91 J/kg. - Graphical abstract: Sodium doping induces an increase of T{sub C} from 240 K for x=0 to 330 K for x=0.2. - Highlights: • La{sub 0.8}Ca{sub 0.2−x}Na{sub x}MnO{sub 3} are synthesized using the ceramic method at high temperatures. • Na doping induces a structural transition from Pbnm to R-3C space group. • T{sub C} increases with Na content from 240 K for x=0 to 330 K for x=0.2. • RCP is constant around 91 J/kg for all compounds under 2 T.« less
  • Cited by 4
  • We prepared orthorhombic La{sub 0.7−x}Y{sub x}Ca{sub 0.3}MnO{sub 3} samples (x = 0, 0.04, 0.06, and 0.08) by conventional solid-state reaction and then studied their magnetic properties and magnetocaloric (MC) effect based on magnetization versus temperature and magnetic-field measurements, M(T, H). The experimental results revealed that an x increase in La{sub 0.7−x}Y{sub x}Ca{sub 0.3}MnO{sub 3} reduced the ferromagnetic-paramagnetic transition temperature (T{sub C}) from 260 K (for x = 0) to ∼126 K (for x = 0.08). Around the T{sub C}, maximum magnetic-entropy changes for a magnetic-field variation interval H = 50 kOe are about 10.7, 8.5, 7.4, and 5.8 J·kg{sup −1}·K{sup −1} for x = 0, 0.04, 0.06, and 0.08, respectively, corresponding to refrigerantmore » capacities RC = 250–280 J·kg{sup −1}. These values are comparable to those of some conventional MC materials, revealing the applicability of La{sub 0.7−x}Y{sub x}Ca{sub 0.3}MnO{sub 3} in magnetic refrigeration. Using the Arrott method and scaling hypothesis as analyzing high-field M(H, T) data, and the universal-curve construction of the magnetic entropy change, we found a magnetic-phase separation. While the samples x = 0−0.06 exhibit a first-order magnetic phase transition, x = 0.08 exhibits the crossover of the first-to-second-order phase transformation (with its critical-exponent values close to those expected for the tricritical mean-field theory) and has the presence of ferromagnetic clusters even above the T{sub C}. Such the variations in the magnetism and MC effect are related to the changes in structural parameters caused by the Y substitution for La because Y doping does not change the concentration ratio of Mn{sup 3+}/Mn{sup 4+}.« less
  • A technology for obtaining single-phase ceramic samples of La{sub 1-x}K{sub x}MnO{sub 3} manganites, as well as the dependence of their structure parameters on the potassium content, is described. The magnetocaloric effect in the samples has been measured by two direct methods, the classical method and the magnetic field modulation method, and has been calculated from the specific heat data. The values of the magnetocaloric effect obtained by these methods are significantly different. The observed discrepancies have been explained. Correlation between the doping level and the value of the effect has been found. It has been shown that the magnetic-field dependencemore » of variation of the magnetic entropy near T{sub C} in weak fields corresponds to theoretical calculations and that the value of the magnetocaloric effect in high magnetic fields can be predicted using this dependence.« less