Chemically inducing room temperature spin-crossover in double layered magnetic refrigerants Pr1.4+xSr1.6-xMn2O7 (0.0 ≤ x ≤ 0.5)

doi:10.1016/j.jmst.2022.01.035

Abstract

Abstract:

The height of total entropy (ST) for a magnetic refrigerant material is essentially concerned with the magnetic and structural transitions. However, the participation of such transitions in layered materials is not well understood. Therefore, the purpose of this work is to investigate the interplay between double layer lattice with their single perovskite counterpart, to achieve optimal magnetocaloric performance. A series of self-doped Pr_1.4+_xSr_1.6-_xMn₂O₇ (0.0 ≤ x ≤ 0.5) Ruddlesden-Popper (R-P) perovskite have been prepared through the solid-state sintering method. With increasing the Pr-stoichiometry, the lattice faults have increased and the double layer lattice dramatically disintegrates into single perovskite structure. Due to the reduction of bilayer R-P phase into single perovskite the spin crossover occurs from weak bilayer (T_C = 304 K) interactions towards the strong three-dimensional (T_C = 308 K) interactions respectively. This series consistently develops thermomagnetic irreversibility in zero-field cooled (ZFC)-field cooled (FC) magnetization, which is indicative of a spin-glass state. The glassy nature has been ascribed collectively to the lattice strain produced because of dislocations and to an antiferromagnetic phase segregated at the surface. The maximum value of temperature average entropy change (TEC) and adiabatic temperature (ΔT_ad) has enhanced nearly by 4 folds from 0.53 J kg^-1 K^-1, 0.59 K (for x = 0.0) up to 1.85 J kg^-1 K^-1, 10 K (for x = 0.5) at 2.5 T, respectively. Additionally, the room temperature relative cooling power has improved from 26.94 J/kg up to 77.84 J/kg with an applied field of 2.5 T. Our findings in this work suggest that the controlled reduction of double layer lattice into single perovskite and/or existence of both phases simultaneously in bilayer R-P manganites may be very effective in obtaining the desirable characteristics of magnetocaloric effects.

Key words: Magnetic refrigerant, Bilayer manganites, Magnetocaloric effect, Ruddlesden-popper perovskite, Relative cooling power

Akshay Kumar, Kavita Kumari, Mohit K. Sharma, Ankush Vij, Shalendra Kumar, Seok-Hwan Huh, Bon Heun Koo. Chemically inducing room temperature spin-crossover in double layered magnetic refrigerants Pr_1.4+_xSr_1.6-_xMn₂O₇ (0.0 ≤ x ≤ 0.5)[J]. J. Mater. Sci. Technol., 2022, 124: 232-242.

Figures/Tables 10

Fig. 1. (a) The XRD profiles of PSMO indicating the reduction in the intensity of reflections corresponding to double perovskite phase and/or evolution in the reflections of single perovskite and PrO2/Pr(OH)3 phases. (b) The calculated fractions of each phase with respect to the stoichiometric concentration of Pr. As the first approximation the fractions of PrO2 + Pr(OH)3 has been considered in a single unit.

Table 1. The agreement parameters obtained from the Rietveld refinement of XRD profiles for Pr1.4+xSr1.6-xMn2O7 (0.0 ≤ x ≤ 0.5) compounds, variation in Unit cell constants, Mn-O bonds and fractions of I4/mmm, Pnma and PrO2/Pr(OH)3 phases.

Contents	x = 0.0	x = 0.1	x = 0.2	x = 0.3	x = 0.4	x = 0.5
Tetragonal (R-P phase) unit cell parameters (Å) a = b; ≠ c	3.85031; 20.12910	3.85094; 20.12841	3.85034; 20.12300	3.84981; 20.09710	3.84966; 20.07420	3.84997; 20.10020
Unit cell volume (Å³)	298.41166	298.49892	298.32582	297.85983	297.49726	297.9365
Mn-O(1) (Å)	1.97748	1.99212	1.98272	2.01413	1.97008	1.97488
Mn-O(2) (Å)	1.6057	1.68757	1.73943	1.81738	1.66435	1.50051
Mn-O(3) (Å)	1.92565	1.92573	1.92758	1.93367	1.92756	1.9271
O(3)-Mn-O(3) (Å)	177.4124	176.1314	174.2674	169.086	173.8989	174.6314
χ²	3.27	2.56	2.15	2.69	2.54	2.04
R_wp	11.2	8.9	9.43	10.6	10.2	9.22
R_p	13.1	10.4	10.9	11.6	10.7	10.1
R_F	3.6	2.95	2.67	2.92	2.85	2.63
Phase Fractions (%)
I4/mmm (Double perovskite)	80.73 ± 0.97	54.99 ± 0.57	32.76 ± 0.35	30.57 ± 0.39	26.88 ± 0.43	11.52 ± 0.17
Pnma (Single perovskite)	13.2 ± 0.7	36.79 ± 1.07	48.47 ± 0.79	52.79 ± 0.99	53.13 ± 1.29	73.84 ± 0.89
PrO₂/Pr(OH)₃	6.08 ± 0.17	8.22 ± 0.41	18.77 ± 0.69	16.63 ± 0.50	19.98 ± 0.50	14.64 ± 0.26

Fig. 2. HR-TEM images and electron diffraction patterns for (a, b) x = 0.0 along [001] (c) x = 0.1 along [110] and (d) x = 0.3 along [0-11] specimens, the electron diffraction dot patterns are inserted in (c, d) respectively.

Fig. 3. HR-TEM images of PSMO series for which (a) x = 0.0 (b) x = 0.1 (c) x = 0.3 and (d) x = 0.5. The stripes images shown in the lower panels were obtained through inverse fast Fourier transform (FFT), the lattice dislocations are clearly visible in each FFT images indicated with yellow. Inset of (b) is the local magnified view from the region in white square, here the lattice faults are noticeable in the form of dark stripes indicated with yellow arrows. The bilayer atomic arrangement is illustrated such that the bright dots are assigned to Pr atoms (marked as purple) and less intense dots to Sr atoms (marked as green) respectively.

Fig. 4. Schematic illustration of sintering mechanism and involvement of the three phases during the sintering process. The FESEM image corresponds to x = 0.3 compositions, here the parasitic PrO2 particles are shown through a local magnification from the top surface. In the below scheme the unit cells correspond to tetragonal (double layer), orthorhombic (single perovskite), cubic (PrO2) lattice structures.

Fig. 5. (a) The variation in the FC magnetization of the sintered compounds against the variable temperature under the presence of an applied field of 0.1 T. (b) The temperature dependency of FC-ZFC magnetization for x = 0.0, 0.2, 0.3, 0.5 samples with the presence of a 0.1T magnetic field. (c) The illustration of ZFC-FC process involving the magnetic phases of variable spin functionalities which are possibly present in/onto the microstructure.

Fig. 6. The variation in the temperature-dependent magnetoelastic Landau coefficients: (a) C1, (b) C3 and (c) C5. (d) The local magnification of C3 parameter indicating the variation from negative to positive values.

Fig. 7. The change in isothermal entropy curves derived by implementing the Maxwell equations from isothermal magnetization plots, the dotted curves in the background representing the magnetic entropy calculated from the Landau Theory. The entropy values calculated at magnetic field values 0.0 T, 0.5 T 1 T, 1.5 T, 2 T, 2.5 T for (a) x = 0.0 (b) 0.1, (c) 0.2, (d) 0.3, (e) 0.4, and (f) 0.5 samples, respectively.

Fig. 8. Comparison of the various figure of merits to assess the magnetocaloric performance of the compounds (a) variation in the magnetic entropy against the temperature and Pr-concentrations under an applied field of 2.5 T, (b) change in adiabatic temperature at 2.5 T magnetic field plotted against the variable temperature and Pr-concentrations, (c) TEC values compared at ΔTH-C = 10 K, for x = 0.0, 0.1, 0.2, 0.3, 0.4, 0.5, compounds under the magnetic field from 0.0 T up to 2.5 T, (d) Relative cooling power of the prepared compounds upon the application of various magnetic field strength.

Table 2. Comparison of various magnetocaloric figure of merits of the compounds prepared in this work with the MC performance of other compounds reported in literature.

Composition	T_C (K)	\|ΔS_M\|^max (J kg^-1 K ^{- 1})	µ₀H (T)	RCP (J kg^-1)	Ref.
Pr_1.4Sr_1.6Mn₂O₇	304	0.27	2.5	27	This work
Pr_1.5Sr_1.5Mn₂O₇	305	0.41	2.5	35	This work
Pr_1.6Sr_1.4Mn₂O₇	306	0.60	2.5	50	This work
Pr_1.7Sr_1.3Mn₂O₇	306	0.78	2.5	65	This work
Pr_1.8Sr_1.2Mn₂O₇	307	0.86	2.5	73	This work
Pr_1.9Sr_1.1Mn₂O₇	308	0.96	2.5	78	This work
Pr_0.6Sr_0.4Mn₂O₃	320	2.3	2.5	34.5	[40]
(1-x)PSMO/xBTO composites	273	1.86-2.89	2	38-63	[25]
LSMO/Ta₂O₅ Composites	309-318	0.200-0.295	0.5	18-36	[26]
La_0.7(Ba,Sr)_0.3(Mn,Ga)₁O₃	300-316	1.02-1.27	2	71-75	[59]
(Cu-Zn)₁Fe₂O₄	143-373	0.77-1.27	3	36.7-37.8	[60]
La_0.8Ca_0.2MnO₃/La_0.8K_0.2MnO₃	247	1.51	2	60	[61]
R₂NiMnO₆ (R = rare-earths)	86-191	1.1-3.1	2	24-59	[62]

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Chemically inducing room temperature spin-crossover in double layered magnetic refrigerants Pr_1.4+_xSr_1.6-_xMn₂O₇ (0.0 ≤ x ≤ 0.5)

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