The demand for advanced multifunctional materials in next-generation electronics requires the integration of diverse, high-performance capabilities into a single, flexible platform. This study details the fabrication of samarium iron garnet-polyvinylidene fluoride (Sm3Fe5O12-PVDF) nanocomposite films via a cost-effective solution casting method. Structural analyses confirm the absence of impure phases via X-ray diffraction with Rietveld refinement, while FESEM demonstrates uniform nanofiller dispersion within the PVDF matrix. Incorporating these nanoparticles enhances the electroactive β-phase from 42% to 57%, increasing the maximum dielectric constant to 19 while maintaining a low leakage current density of 10−5 A/m2 at 160 kV/m. The films exhibit robust multiferroic behavior with a saturation magnetization of 5.2 emu/g and a maximum ferroelectric polarization of 0.267 μC/cm2 at 14.44 kV/cm. Magnetodielectric studies confirm strong magnetoelectric coupling, further demonstrated by a 12.17% polarization enhancement, from 0.2676 μC/cm2 to 0.3001 μC/cm2, during magnetic field-dependent measurements under a 1.75 kG field. As a piezoelectric energy harvester, the optimally loaded film yields an exceptional 160 V, 24.29 μA, and 1982.9 μW/cm2 maximum power density under a 0.186 N force. Furthermore, the giant magnetostriction of Sm3+ ions induce internal strain under 2.57 kG magnetic fields, generating voltage without mechanical stimulation. This establishes the material as a highly sensitive, contactless magneto-mechano-electric energy generator. Simultaneously, the engineered nanocomposite films act as advanced structural absorbers, achieving an outstanding total electromagnetic interference shielding effectiveness of −68.5 dB at 9.4 GHz. This yields 99.999986% attenuation across the 8 to 18 GHz frequency range. This fundamentally novel platform promises significant advancements in self-powered electronics, shielding, and contactless magnetic sensing.
We demonstrate exchange bias-driven large topological Hall effect in epitaxial NiFeMo/NiFeMoO heterostructures fabricated on Al2O3 (0001) substrates. Structural analyses confirm high-quality epitaxial growth with distinct strain states in single-layer NiFeMo and bilayer NiFeMo/NiFeMoO thin films. Magnetometry reveals that NiFeMo remains ferromagnetic over the entire temperature range, whereas NiFeMoO undergoes a suggested paramagnetic-to-antiferromagnetic transition near 175 K, inducing robust exchange bias in field cooled NiFeMo/NiFeMoO heterostructures. Magnetic force microscopy, supported by micromagnetic simulations incorporating Dzyaloshinskii-Moriya interactions, uncovers non-coplanar spin textures at room temperature under moderate magnetic fields. Magnetotransport studies identify a pronounced topological Hall-like signal, strongly enhanced by exchange bias at low temperatures. These results establish that epitaxial strain and interfacial exchange coupling act synergistically to stabilize non-coplanar spin textures and tailor the topological Hall response from 10 to 300 K, offering a promising pathway for oxide/metal interface-based topological spintronic applications.
We report a remarkable bias voltage dependent specific negative capacitance in multidomain La-doped [Pb(Zr0.4Ti0.6)O-3(PLZT)] ferroelectric capacitors. The specific negative capacitance maximizes at a specific bias voltage because of emergence of maximum domain-wall density during "switching" of the domains. Domain configuration changes from such an "optimum" state if higher or lower bias voltage is applied at a much faster or slower rate. Phase-field simulation using time-dependent Ginzburg-Landau equation corroborates the experimental results and shows dependence of the domain-wall length during switching on the bias voltage amplitude and its maximization at a specific bias voltage amplitude. Interestingly, the radius of curvature of the resulting polarization ( P) vs voltage ( V) hysteresis loop at the coercive voltage ( V-C), as well, turns out to be depending on the bias voltage. All these results indicate a close correlation among the bias voltage pulse profile (amplitude and time scale), domain-wall length during switching, shape of the resulting ferroelectric hysteresis loop, and the transient negative capacitance. It may have important ramifications both in the context of physics behind negative capacitance in a multidomain ferroelectric capacitor and devices being developed by exploiting its advantages.
Neuromorphic computing demands artificial synaptic devices capable of mimicking biological synaptic behaviors with high efficiency. In this study, we demonstrate stable and reliable resistive switching (RS) characteristics in a memristor consisting of layered thin films of the ferroelectric perovskite PbZr0.52Ti0.48O3 (PZT) and the ferromagnetic half-metal La0.65Sr0.35MnO3 (LSMO). A high quality epitaxial PZT/LSMO thin film was deposited on single crystal MgO (100) substrate using the pulsed laser deposition technique; forming a robust Ag/PZT/LSMO memristor. The device exhibits forming-free and compliance-free highly stable RS behaviour under DC voltage sweeps, implying reliability and low power consumptions. Furthermore, under pulse voltage stimulation, the memristor successfully emulates key synaptic functions, including potentiation, depression, spike-time-dependent plasticity (STDP), paired-pulse facilitation/depression (PPF)/(PPD), and short-term memory (STM) to long-term memory (LTM) transition. These results establish a strong foundation for the integration of PZT-based memristors into next-generation neuromorphic computing systems, enabling efficient and scalable artificial intelligence hardware.
Using a combined experimental and first-principles theoretical approach, we demonstrate interface engineering of the anomalous Hall effect in Ni-based epitaxial thin-film heterostructures. Ferromagnetic Ni thin films are grown on (001)-oriented single-crystal LaAlO_3, SrTiO_3, and MgO substrates, which impose different biaxial tensile strains of 0.3
We demonstrate room temperature electric field control of the anomalous Hall effect in epitaxial Ni80Fe20 (Py) BaTiO3 (BTO) La0.7Sr0.3MnO3 (LSMO) thin film heterostructures grown on MgO and LaAlO3 substrates. Substrate induced strain states generate distinct magnetic anisotropies, enabling voltage driven tuning between anomalous and topological Hall contributions. Robust ferroelectric polarization in BTO, confirmed by piezoresponse force microscopy, couples strongly to interfacial orbital reconstruction and carrier redistribution. As a result, Hall resistivity exhibits giant low voltage tunability, with up to nearly 93 percent modulation at operating voltages of only 0.5 tand 2 V. Density functional theory calculations further reveal polarization controlled Rashba spin splitting, establishing a direct link between ferroelectric order and emergent quantum transport. These findings establish Py/BTO/LSMO heterostructures as promising candidates for low-power multifunctional spintronic devices, where substrate engineering enables control over emergent quantum transport phenomena.
The emergence of new physical properties at the interfaces between complex oxides has always been of both fundamental and practical importance. Here, we report the observation of a giant topological Hall resistivity of ∼ 2.8 μΩ cm at room temperature in an epitaxial thin-film heterostructure of permalloy (Py, Ni_80Fe_20) and the half-metallic ferromagnet La_0.65Sr_0.35MnO_3 (LSMO). This large magnitude of the topological Hall effect in the Py/LSMO heterostructure, compared to a single-layer Py thin film, is attributed to the optimized combination of ferromagnetism in LSMO and the strong spin-orbit-coupling-driven Rashba interaction at the interface. The introduction of a ferroelectric BaTiO_3 (BTO) sandwich layer in the Py/LSMO heterostructure also leads to an enhanced topological Hall resistivity compared to the single-layer Py thin film. Interestingly, magnetic force microscopy measurements reveal skyrmion-like features, suggesting the origin of the topological Hall effect. Our theoretical model calculations for the skyrmion lattice further indicate that the Rashba interaction, driven by the broken inversion symmetry in the Py/LSMO films, can account for the observed changes in the topological Hall effect at the interface. Our work opens the door for the potential use of Py/LSMO thin films in spintronic applications.
We have investigated the critical behavior and underlying magnetic interactions in Mn-intercalated TaS2 through a critical scaling analysis of isothermal magnetization across the ferromagnetic-paramagnetic transition. This compound shows a ferromagnetic (FM) order below TC similar to 30 K and exhibits magnetic anisotropy with a large ab-plane moment and a small moment along the c-axis. The critical scaling analysis of isothermal magnetization yields the critical exponents beta = 0.377 +/- 0.002, gamma = 1.345 +/- 0.003, delta = 4.682 +/- 0.003. The exponent beta is close to the 3D Heisenberg model but gamma lies between the 3D Heisenberg and 3D XY models, suggesting the presence of complex magnetic interactions arising from the competition between Heisenberg exchange and Dzyaloshinskii-Moriya (DM) interactions.
The rising need for energy-efficient data processing has sparked increased attention towards neuromorphic computing which seems to replicate the human brain-like functions. This innovative method enables faster and more cost-efficient parallel data processing, overcoming the constraints of traditional von Neumann systems. A crucial component in this process is the advancement of memristors which functions like biological synapses. Recently researchers have concentrated on integrating nociceptors-sensory neurons that detect external stimuli-into memristors, enhancing their use in robotics and artificial intelligence (AI). This combination allows memristors to adjust to different conditions while maintaining affordability. Hence, this study provides a detailed investigation into mimicking bio-synaptic and bio-nociceptive functions on a single ZnO-based flexible artificial synaptic memristor, aiming at on-receptor computing applications. The Ag/ZnO/ITO memristors were fabricated on both glass and flexible polyethylene terephthalate (PET) substrates using the pulsed laser deposition (PLD) techniques under varying ambient oxygen flow rates. The optimized device exhibited stable, forming-free, and bipolar resistive switching with low operating voltages (within +/- 0.7 V), a modest ON/OFF ratio of 102, and endurance exceeding 500 cycles. The memristor effectively mimicked key features of bio-nociceptor such as threshold, relaxation, sensitization characteristics, and recovery under varying stimuli, emphasizing its strong sensing properties. It also exhibited versatile bio-synaptic behaviours, such as potentiation, depression, spike- timing dependent plasticity (SRDP), paired-pulse facilitation/depression (PPF/PPD), and transitions from short to long-term plasticity (STP to LTP) highlighting its potential for learning-enabled sensor platforms, i.e. on- receptor computing application. Additionally, the synaptic and nociceptive functions of the flexible ZnO-based device, fabricated under optimized growth conditions exhibiting excellent stability and reliability under different bending conditions. These results suggest that the multifunctional ZnO-based memristor could play a significant role in advancing neuromorphic artificial intelligence, brain-computer interfaces, wearable electronics, and other sensor-based systems, paving the way for innovative future applications in on-receptor computing.
The emergence of new physical properties at the interfaces between complex oxides has always been of both fundamental and practical importance. Here, we report the observation of a giant topological Hall resistivity of similar to 2.8 mu S2 cm at room temperature in an epitaxial thin-film heterostructure of permalloy (Py, Ni80Fe20) and the half-metallic ferromagnet La0.65Sr0.35MnO3 (LSMO). This large magnitude of the topological Hall effect in the Py/LSMO heterostructure, compared to single-layer Py and LSMO thin films, is attributed to the optimized combination of ferromagnetism in LSMO and the strong spin-orbit-coupling-driven Rashba interaction at the interface. The introduction of a ferroelectric BaTiO3 sandwich layer in the Py/LSMO heterostructure also leads to an enhanced topological Hall resistivity compared to the single-layer Py thin film. Interestingly, magnetic force microscopy measurements reveal skyrmionlike features, suggesting the origin of the topological Hall effect. Our theoretical model calculations for the skyrmion lattice further indicate that the Rashba interaction, driven by the broken inversion symmetry in the Py/LSMO films, can account for the observed changes in the topological Hall effect at the interface. Our work opens the door for the potential use of Py/LSMO thin films in spintronic
The emergence of new physical properties at the interfaces between complex oxides has always been of both fundamental and practical importance. Here, we report the observation of a giant topological Hall resistivity of $\sim 2.8 \mu \Omega$ \text{cm} at room temperature in an epitaxial thin-film heterostructure of permalloy (Py, Ni$_{80}$Fe$_{20}$) and the half-metallic ferromagnet La$_{0.65}$Sr$_{0.35}$MnO$_3$ (LSMO). This large magnitude of the topological Hall effect in the Py/LSMO heterostructure, compared to a single-layer Py thin film, is attributed to the optimized combination of ferromagnetism in LSMO and the strong spin-orbit-coupling-driven Rashba interaction at the interface. The introduction of a ferroelectric BaTiO$_3$ (BTO) sandwich layer in the Py/LSMO heterostructure also leads to an enhanced topological Hall resistivity compared to the single-layer Py thin film. Interestingly, magnetic force microscopy measurements reveal skyrmion-like features, suggesting the origin of the topological Hall effect. Our theoretical model calculations for the skyrmion lattice further indicate that the Rashba interaction, driven by the broken inversion symmetry in the Py/LSMO films, can account for the observed changes in the topological Hall effect at the interface. Our work opens the door for the potential use of Py/LSMO thin films in spintronic applications.
Materials exhibiting topological transport properties, such as a large topological Hall resistivity, are crucial for next-generation spintronic devices. Here, we report large topological Hall resistivities in epitaxial supermalloy (NiFeMo) thin films with [100] and [111] orientations grown on single-crystal MgO (100) and Al2O3 (0001) substrates, respectively. While X-ray reciprocal maps confirmed the epitaxial growth of the films, X-ray stress analyses revealed large residual strains in the films, inducing tetragonal distortions of the cubic NiFeMo unit cells. Magnetic force microscopy showed the presence of skyrmion-like features, which may arise from strain-induced spin texturing in the films. Magneto-optic Kerr effect confirmed a 4-fold magnetic anisotropy in the NiFeMo/MgO (100) film which exhibited a more pronounced topological Hall effect compared to that in the NiFeMo/Al2O3 (0001) film. We envisage that the strain-induced disruption of the centrosymmetry in the NiFeMo films possibly leads to Dzyaloshinskii-Moriya (DM) interactions within the spins. This gives rise to the skyrmion-like spin textures and notable topological Hall effects near room temperature hitherto unobserved in NiFeMo thin films. Theoretical simulations based on DM interactions strongly correlate the experimental results and corroborate with the presence of skyrmion-like spin textures in the films. The modulation of topology and magnetism in NiFeMo thin films through strain engineering may provide useful direction for the pursuit of quantum Hall effect based spintronic devices.
In this study, tunable bipolar magnetization reversal with an inverse exchange bias effect and magnetically switched magnetocaloric effect are reported in the hetero-tri-spin of a 3d-5d-4f based Gd2NiIrO6 (GNIO) polycrystalline sample. The sample was prepared using a conventional solid-state reaction method. Temperature (T)- dependent direct current (DC) and alternating current (AC) magnetic susceptibility studies revealed that GNIO exhibits ferrimagnetic (FiM) behavior below the transition temperature T-N similar to 164 K owing to the Ni2+- O2- - Ir4+ superexchange interactions. With the application of 500 Oe, low-field-cooled (HFC) induced magnetization reversal (MR) below the compensation temperature (T-comp) similar to 28 K, and a spin re-orientation (SR) like behavior at T-SR similar to 96 K were observed in FC mode within the temperature region of T-comp < T-SR < T-N. T he observed negative magnetization across the magnetic compensation could be attributed to the competing magnetic interactions arising from the thermal variations in the magnetic moments of the Gd and Ni-Ir sublattices. An inverse exchange bias effect was observed from isothermal magnetization measurements, where the M(H) loop shifted after field- cooling (H-FC). The H-assisted magnetization switching confirmed the spin reversal phenomenon, and temperature-dependent magnetic entropy changes complemented both the conventional and inverse magneto- caloric effects. Density functional theory (DFT) calculations employing the generalized gradient approximation (GGA) and the Hubbard U model along with spin-orbit coupling confirmed that the FiM phase is the most stable magnetic state for GNIO. This finding is in good agreement with the experimental observations. Interestingly, the calculated spin-polarized density of states revealed a dominant contribution of Ird over Nid near the Fermi level, confirming the Mott-insulating behavior of GNIO.
Rare-earth molybdates have drawn tremendous attention due to their magnetoelectric nature, including type-II multiferroicity and structural phase transitions linked to displacive type ferroelectricity, making them well-suited for multicaloric effect in solid-state refrigeration phenomena. This study focuses on the synthesis and crystal structure analysis, temperature and field-dependent magnetic susceptibility, and magnetocaloric properties of TbGd(MoO4)3 (TGMO) polycrystals. The magnetic field and temperature variation of magnetization and specific heat capacity were conducted to evaluate the spin contributed magnetic entropy changes (-GSM) and temperature change under adiabatic (GTad) conditions in the synthesised sample. The investigated compound exhibits no obvious long-range order with in the measured low-temperature limit. The calculated-GSM shows a maximum value of 13.6 Jkg-1K-1 at 3.5 K for 70 kOe. Moreover, the estimated temperature change under adiabatic conditions for TGMO was found to be 8.5 K. These characteristics, including a significant magneto-caloric effect with magnetic field and the absence of thermal and magnetic hysteresis loss, is comparable to good magnetic refrigerants near liquid helium temperatures.
The double perovskite Eu2CoMnO6 (ECMO), known for its complicated metamagnetic behavior, was studied in this report to examine how postannealing synthesis affects its crystal structure and magnetic and electronic behavior. The slow-cooling, Argon treatment, and quenching procedure during the sample synthesis indicated the important significance of antisite disorder (ASD) in influencing the material's magnetic response. The magnetic study revealed diverse transitions, including two low-temperature antiferromagnetic (AFM)-like transitions at similar to 51 and similar to 10 K in the slow-cooled sample and vibronic ferromagnetic (FM) superexchange interactions at similar to 105 K in the argon (Ar)-treated sample, while the quenched sample displayed an AFM behavior at low temperatures. The XPS analysis indicated the presence of diverse concentrations of Co and Mn in multiple valence states, specifically (2+, 3+) and (3+, 4+) respectively, across the samples subjected to different annealing processes. The Griffiths phase was particularly noticeable in the quenched sample, highlighting the role of disorder with Griffith's disorder exponent (lambda) = 0.81. The M(H) data at 2.5 K under zero-field-cooled mode revealed that the Ar-treated sample had a smooth, saturating-like loop, while the quenched sample had the hysteresis loop shifted toward the positive field axis with a reduced magnetic moment of 2.2 mu B/f.u., and the slow-cooled sample exhibited sharp metamagnetic jumps with an unsaturated magnetic moment of 3.3 mu B/f.u. While M(H) data recorded under a field-cooled protocol altered the position of critical fields (H C) for the slow-cooled sample, the evolution of an extra magnetization jump was noticed in the case of the Ar-annealed sample, and the quenched sample showed the loop shifting completely toward the negative field axis. The loop shift and varying H C values were explained in terms of an exchange bias-like spin-pinning mechanism. Additionally, DFT calculations corroborate the experimental results, revealing an increased likelihood of antisite disorders in the presence of oxygen vacancies, as well as altered behavior of Co and Mn spin states in relation to the disorders and oxygen vacancies. The effect of the disorder and oxygen vacancies on the electrical and magnetic ground states was also investigated, and the results were complemented with the experimentally observed magnetic behavior. This study demonstrates how postannealing conditions may be carefully controlled to regulate the disorder and, thus, magnetic behavior, including valence states, Griffiths phase, and metamagnetic behavior of ECMO, opening up new avenues for developing materials with desired functional properties.
Layered thin films of the ferroelectric perovskite Ba0.85Ca0.15Ti0.9Zr0.1O3 (BCZT) and the ferromagnetic half-metal La0.80Sr0.20MnO3 (LSMO) are well-known multiferroic systems that show promise for spintronic applications. In this work, the structure–property relationships are explored in novel BCZT/LSMO thin film heterostructures with optimized ferroic properties. Epitaxial BCZT/LSMO thin film heterostructures are grown by varying the lattice mismatch strains on single crystal LaAlO3 (LAO) (100) and MgO (100) substrates using the pulsed laser deposition technique. The epitaxial strain in the films gives rise to a tetragonal distortion of the BCZT and LSMO unit cells and significantly affects their magnetotransport and magnetodielectric properties. The BCZT/LSMO/LAO heterostructure exhibits a colossal magnetoresistance effect due to a large out-of-plane tensile strain, which induces enhanced carrier hopping in the LSMO layer as compared to the BCZT/LSMO/MgO film. The larger tetragonal distortion of the BCZT unit cell in BCZT/LSMO/MgO contributes to higher dielectric permittivity, with a greater dielectric maxima temperature and freezing temperature. Magnetodielectric measurements reveal a hitherto unobserved giant magnetodielectric effect in the BCZT/LSMO/MgO film, attributed to a large in-plane strain, which induces interfacial polarization distortion at the interfacial layer. Overall, this work elucidates the unique strain and charge-mediated cross-coupled phenomena of magnetic and electric orders in multiferroic thin film heterostructures, which are critical for their technological applications.
We investigated the magnetic transitions in BiFeO3 at low temperature (5-300 K) and observed nearly 90 degrees rotation of magnetic domains (imaged by vertical magnetic force microscopy) across 150 K in an epitaxial thin film of thickness similar to 36 nm. It offers a clear evidence of spin reorientation transition. It also corroborates the transition observed below similar to 150 K in the zero-field-cooled and field-cooled magnetization versus temperature data. The field-driven 180 degrees domain switching at room temperature, on the other hand, signifies presence of ferromagnetism. Since bulk antiferromagnetic BiFeO3 does not exhibit such a transition, this observation in ferromagnetic thin film of BiFeO3 indicates a radical effect because of epitaxial strain. Density functional theory-based first-principles calculations also reveal that combined in- and out-of-plane epitaxial strain induces magnetic transition from G- to C-type structure in BiFeO3.
We report on the synthesis, structural, DC magnetic susceptibility studies on Gd-2(MoO4)(3) and Tb-2(MoO4)(3) polycrystals, prepared by conventional solid-state reaction method. Temperature and magnetic field (H) dependent magnetization and heat capacity measurements have been carried out to estimate the isothermal magnetic-entropy change (-Delta S-m) and adiabatic temperature change (Delta T-adi) in both rare-earth molybdates. No obvious long-range magnetic ordering can be found down to 2 K in both studied compounds. The estimated maximum value of -Delta S-m at 3.5 K for 70 kOe is 31.1 J kg(-1) K-1 and 16.7 J kg(-1) K-1 in Gd-2(MoO4)(3) and Tb-2(MoO4)(3), respectively. Further, the calculated total-adiabatic temperature change for Gd-2(MoO4)(3) was 12.8 K, and Tb-2(MoO4)(3) has shown 9.8 K. The difference in the observed magnetocaloric and adiabatic temperature responses of Tb-2(MoO4)(3) compared to Gd-2(MoO4)(3) could be attributed to the presence of orbital angular moment of Tb3+ ions and relatively low-value of magnetization. Both the systems show a large magnetocaloric effect (MCE) (-Delta S-m similar to 12 J kg(-1) K-1) even in low applied H (<20 kOe) attainable by a permanent magnet. Large magnetocaloric behaviour of Gd-2(MoO4)(3) and Tb-2(MoO4)(3) systems at a moderate field change along with very low electrical conductivity and the absence of thermal and magnetic field hysteresis in magnetization make them conducive to their use as promising magnetic refrigerants in the vicinity of liquid-helium temperatures.
Structural, dielectric, and electrocaloric properties were investigated in Pb-free ceramic (Ba0.88Ca0.12) (Ti0.94Sn0.06)O-3 (BCST), synthesized using solid-state sintering method. Rietveld refinement of room temperature XRD data revealed the existence of pure perovskite tetragonal (P4mm) phase. Temperature -dependent XRD analyses confirmed a structural transition from tetragonal to cubic phase near 380 K. Temperature -dependent dielectric constant (epsilon(r)) and specific heat capacity (C-p) confirmed the presence of thermal hysteresis in two phase transitions near 233 +/- 10 K and 254 +/- 10 K, and a non -hysteretic behavior at the Curie temperature (T-C similar to 373 +/- 10 K). A comprehensive Raman study corroborated the existence of phase transitions. Electrocaloric properties were determined using indirect method utilizing the non -hysteretic nature across T C . A large adiabatic temperature change of |Delta T| = 0.52 K, isotropic entropy change |Delta S| = 0.68 J/kg.K, electrocaloric coefficients, |Delta T/ Delta E| = 0.311 K.mm/kV and |Delta S/Delta E| = 0.41 J.mm/K.kg.kV were obtained at 380 K for an electric field of 16.7 kV/cm. Obtained value of |Delta T/Delta E| is relatively good, reported among other BaTiO3-based ceramics.
Electrocaloric effects of adiabatic temperature change via the application of external electric fields are explored for energy-efficient solid-state refrigeration. These effects are typically estimated from the thermodynamic analyses of polarization and field in electrocaloric materials, which implies that higher field application gives larger temperature changes. However, this may not be always true. Here, using both indirect and direct methods, we report an anomalous effect where larger thermal changes occur by applications of lower fields in a multi-domain BaTiO3 (001) single crystal. A large temperature change of 1.9 K under a low field change of 8 kV/cm at 404 K is observed in a multi-domain BaTiO3 (001) single crystal in comparison to that of 1.4 K at a high field change of 30 kV/cm. We attribute this counterintuitive effect to the interplay of the c- and a-domains in the BaTiO3 (001) single crystal under the influence of temperature and field changes. This work provides a fundamental understanding of the complex role of domains in governing the electrocaloric response of ferroelectric materials which is often overlooked but critical for their practical applications.