skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.

Explore Research Products in the PAR
It may take a few hours for recently added research products to appear in PAR search results.


Title: Structural coupling and magnetic tuning in Mn2− x Co x P magnetocalorics for thermomagnetic power generation
Promising materials for magnetic refrigeration and thermomagnetic power generation often display strong coupling between magnetism and structure. It has been previously proposed that MnCoP exhibits this strong coupling, contributing to its substantial magnetocaloric effect near TC = 578K. Here, we show from temperature-dependent synchrotron x-ray diffraction that MnCoP displays a discontinuity in the thermal expansion at TC, with spontaneous magnetostriction that is positive in the a direction and negative in the b direction, highlighting the anisotropic nature of the magnetostructural coupling. Varying the Mn:Co ratio of Mn2−xCoxP within the range of 0.6 ≤ x ≤ 1.4 allows the magnetic properties to be tuned. TC decreases as the composition deviates from stoichiometric MnCoP, as does the saturation magnetization. The magnitude of the magnetocaloric effect, |ΔSM|, decreases as well, due to broadening of the magnetic transition. The large reversible change in magnetization ΔM accessible over a small temperature range under moderate magnetic fields makes these materials promising for thermomagnetic power generation from waste heat.  more » « less
Award ID(s):
1710638
PAR ID:
10594602
Author(s) / Creator(s):
; ; ; ; ; ;
Publisher / Repository:
American Institute of Physics
Date Published:
Journal Name:
APL Materials
Volume:
8
Issue:
4
ISSN:
2166-532X
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. ; ; ; (, Advanced Electronic Materials)
    Abstract The highest ambient‐pressure Tc among binary compounds is 40 K (MgB2). Higher Tc is achieved in high‐pressure hydrides or multielement cuprates. Alternatively, are explored superconducting properties of binary, metastable sub‐oxides, that may emerge under extremely low oxygen partial pressure. The emphasis is on the rock‐salt structure, which is known to promote superconductivity, and exploring AlO, ScO, TiO, and NbO. Dynamic lattice stability is achieved by introducing metal and oxygen vacancies in the fashion of Nb1−xO1−x‐type structure (x = ¼). The electron‐phonon (e‐ph) coupling is remarkably large in Al1−xO1−xand Ti1−xO1−x(λ ≈ 2 at x = ¼), with Tc ≈ 35 K according to the Allen–Dynes equation. Significantly, the coupling strength is comparable to that in high‐pressure hydrides, yet, in contrast to hydrides and MgB2, the coupling is largely driven by low frequency phonons. Sc1−xO1−xand Nb1−xO1−xshow significantly smaller λ and Tc. Further, hydrogen intercalation to boost λ and Tc is investigated. Only Ti1−x(O1−xHx) and Nb1−x(O1−xHx) are dynamically stable upon intercalation, where H, respectively, decreases and increases Tc. The effect of H doping on electronic structure and Tc is discussed. Altogether, the study suggests that metal sub‐oxides are promising compounds to achieve strong e‐ph coupling at ambient pressure. 
    more » « less
  2. ; ; ; ; ; (, Journal of Materials Chemistry C)
    The ternary manganese pnictide phases, MnAs 1− x Sb x , are of interest for magnetic refrigeration and waste heat recovery due to their magnetocaloric properties, maximized at the Curie temperature ( T C ), which varies from 580–240 K, depending on composition. Nanoparticles potentially enable application in microelectronics (cooling) or graded composites that can operate over a wide temperature range, but manganese pnictides are synthetically challenging to realize as discrete nanoparticles and their fundamental magnetic properties have not been extensively studied. Accordingly, colloidal synthesis methods were employed to target discrete MnAs x Sb 1− x nanoparticles ( x = 0.1–0.9) by arrested precipitation reactions of Mn 2 (CO) 10 with (C 6 H 5 ) 3 AsO and (C 6 H 5 ) 3 Sb in coordinating solvents. The MnAs x Sb 1− x particles are spherical in morphology with average diameters 10–13 nm (standard deviations <20% based on transmission electron microscopy analysis). X-Ray fluorescence spectroscopy measurements on ensembles showed that all phases had an excess of Sb relative to the targeted composition, whereas energy dispersive spectroscopic mapping data of single particles revealed that the nanoparticles are inhomogeneous, adopting a core–shell structure, with the amorphous shell rich in Mn and O (and sometimes Sb) while the crystalline core is rich in Mn, As, and Sb. Magnetization measurements of the nanoparticle ensemble demonstrated the presence of both ferromagnetic and paramagnetic phases. By combining the magnetization measurements with precision chemical mapping and simple modeling, we were able to unambiguously attribute ferromagnetism to the MnAs x Sb 1− x crystalline core, whereas paramagnetism was attributed to the amorphous shell. Magnetization measurements at variable temperatures were used to determine the superparamagnetic transition of the nanoparticles, although for some compositions and particle sizes the blocking temperature exceeded room temperature. Preliminary magnetic studies also revealed a conventional dependence between core size and coercivity, in spite of variable compositions of the nanoparticles, an unexpected result. 
    more » « less
  3. ; ; ; (, AIP Advances)
    Stability of cobalt-doped lanthanum iron silicide, La(FexCoySi1-x-y)13 have been investigated under conditions required for magnetocaloric refrigeration. The XRD analysis revealed that both milled and non-milled samples stored in water loose a few Bragg peaks corresponding to the NaZn13 phase of La(FexCoySi1-x-y)13. Samples stored in air show well-defined Bragg peaks similar to that of pristine material. The SEM-EDS of the milled and non-milled samples stored in water and air show an increased concentration of oxygen in the samples, particularly those treated with water. The course non-milled powders stored in air and water show sharp transitions at the Curie temperature TC = 300K without large magnetization above the TC. The milled, fine-particulate sample stored in air shows a slightly broadened transition at TC, and that stored in deionized water for 14 days shows significantly broadened transition from 300K and retains large magnetizations above 400 K. This is indicative of relatively fast hydrolysis and removal of some or all of La, likely as hydroxide, from fine powders, leaving behind La-poor or, potentially, La-free Fe-Co-Si containing ferromagnetic residue with much higher Curie temperature. The non-milled course sample stored in water has sharper magnetic transition and higher magnetization hence it shows the highest entropy change among all 4 type of samples. 
    more » « less
  4. ; ; ; ; ; (, Magnetochemistry)
    The magnetocaloric effect (MCE) in iron (Fe) nanoparticles incorporated within a titanium nitride (TiN) thin-film matrix grown using pulsed laser deposition (PLD) is investigated in this study. The study demonstrates the ability to control the entropy change across the magnetic phase transition by varying the size of the Fe nanoparticles. The structural characterization carried out using X-ray diffraction (XRD), scanning electron microscopy (SEM), atomic force microscopy (AFM), and scanning transmission electron (TEM) showed that TiN films are (111) textured, while the Fe-particles are mostly spherical in shapes, are single-crystalline, and have a coherent structure with the surrounding TiN thin-film matrix. The TiN thin-film matrix was chosen as a spacer layer since it is nonmagnetic, is highly corrosion-resistive, and can serve as an excellent conduit for extracting heat due to its high thermal conductivity (11 W/m K). The magnetic properties of Fe–TiN systems were investigated using a superconducting quantum interference device (SQUID) magnetometer. In-plane magnetic fields were applied to record magnetization versus field (M–H) and magnetization versus temperature (M–T) curves. The results showed that the Fe–TiN heterostructure system exhibits a substantial isothermal entropy change (ΔS) over a wide temperature range, encompassing room temperature to the blocking temperature of the Fe nanoparticles. Using Maxwell’s relation and analyzing magnetization–temperature data under different magnetic fields, quantitative insights into the isothermal entropy change (ΔS) and magnetocaloric effect (MCE) were obtained for the Fe–TiN heterostructure system. The study points out a considerable negative change in ΔS that reaches up to 0.2 J/kg K at 0.2 T and 300 K for the samples with a nanoparticle size on the order of 7 nm. Comparative analysis revealed that Fe nanoparticle samples demonstrate higher refrigeration capacity (RC) in comparison to Fe thin-film multilayer samples, with the RC increasing as the Fe particle size decreases. These findings provide valuable insights into the potential application of Fe–TiN heterostructures in solid-state cooling technologies, highlighting their enhanced magnetocaloric properties. 
    more » « less
  5. ; ; ; ; ; ; ; ; ; (, APL Materials)
    Tuning the properties of magnetic topological materials is of interest to realize exotic physical phenomena, new quantum phases and quasiparticles, and topological spintronic devices. However, current topological materials exhibit Curie temperature (TC) values far below those needed for practical applications. In recent years, significant progress has been made to control and optimize TC, particularly through defect-engineering of these structures. Most recently, we reported TC values up to 80 K for (MnSb2Te4)x(Sb2Te3)1−x when 0.7 ≤ x ≤ 0.85 by controlling the composition x and the Mn content in these structures during molecular beam epitaxy growth. In this study, we show further enhancement of the TC, as high as 100 K, by maintaining high Mn content and reducing the growth rate from 0.9 nm/min to 0.5 nm/min. Derivative curves of the Hall resistance and the magnetization reveal the presence of two TC components contributing to the overall value and suggest TC1 and TC2 have distinct origins: excess Mn in MnSb2Te4 septuple layers (SLs) and high Mn content in Sb2−yMnyTe3 quintuple layer (QL) alloys, respectively. To elucidate the mechanisms promoting higher TC values in this system, we show evidence of enhanced structural disorder due to the excess Mn that occupies not only Sb sites but also Te sites, leading to the formation of a new crystal structure for these materials. Learning to control defects that enhance desired magnetic properties and understanding the mechanisms that promote high TC in magnetic topological materials such as (Mn1+ySb2−yTe4)x(Sb2−yMnyTe3)1−x is of great importance to achieve practical quantum devices. 
    more » « less
  • Citation Formats
  • MLA
  • APA
  • Chicago
  • BibTeX
  • Save / Share this Record
  • Send to Email