Recently, all-$d$-metal Ni(Co)-Mn-Ti Heusler systems have become the research hotspot due to their magnetoresponsive properties associated with a tunable first-order magnetostructural transformation (MST) and excellent mechanical stability for potential applications. However, the presence of large thermal hysteresis acts as an obstacle to the cyclic operation of this novel material. In this present paper, we investigate a large reversible magnetocaloric effect (MCE) and magnetoresistance (MR) in ${\mathrm{Ni}}_{37-x}{\mathrm{Co}}_{13+x}{\mathrm{Mn}}_{34.5}{\mathrm{Ti}}_{15.5}$ all-$d$-metal Heusler alloys that undergo a first-order MST accompanied by a large magnetization change between ferromagnetic austenite and antiferromagnetic martensite phases. Tuning the small at.% of Co doping in ${\mathrm{Ni}}_{37-x}{\mathrm{Co}}_{13+x}{\mathrm{Mn}}_{34.5}{\mathrm{Ti}}_{15.5}$ systems, we achieved an optimum composition with $x$ = 1 where low thermal hysteresis of $\sim 4.7$ K, a narrow transformation interval of $\sim 11.2$ K, and improved sensitivity of transformation temperature $\sim 2.8$ K/T is observed. In addition, the origin of small hysteresis is studied based on geometric compatibility between cubic austenite and monoclinic martensite phases, calculated from the powder x-ray diffraction data. These optimized parameters lead to a reversible magnetic field-induced inverse martensitic transition under the field cycling, yielding a large reversible magnetic entropy change ($\mathrm{\Delta }{\mathrm{S}}_M$) of $\sim 17.78$ J ${\mathrm{kg}}^{-1}{\mathrm{K}}^{-1}$ at 277 K in a field change of 5 T. Moreover, a large reversible magnetoresistance (MR) of $\sim 14\%$ out of 32.6% is also obtained under 5-T magnetic field for $x$ = 1 sample in all-$d$-metal Heusler alloys. These reversible magnetoresponsive properties are comparable to other Ni-Mn-based Heusler alloys and have not been reported so far in the all-$d$-metal Heusler system. Therefore our present work demonstrates a pathway to design new cyclically stable multifunctional materials in all-$d$-metal Heusler systems for solid-state cooling devices and magnetic recording applications.

• Received 26 May 2022
• Accepted 12 September 2022

DOI:https://doi.org/10.1103/PhysRevMaterials.6.094411