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H. Gai

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8 records found

Journal article (2026) - H. Yibole, L. Shanshan, B. Narsu, F. Guillou, B. Detlefs, P. Glatzel, W. Hanggai, A. Kiecana, N. H. Van Dijk, E. Brück
First-order magnetoelastic transitions usually involve mechanisms unique to each family of materials. For (Mn,Fe)2(P,Si) compounds, it is generally predicted that the unit cell distortion occurring at the ferromagnetic transition leads to a strong electronic reconstruction of the Fe d states accompanied by a notable change in magnetic moment. However, there is no experimental consensus on this mechanism. Here, we use x-ray emission spectroscopy (XES) complemented by first-principles calculations, high-energy resolution fluorescence detected x-ray absorption (HERFD-XAS), and resonant inelastic x-ray scattering (RIXS) experiments, to clarify the nature of the first-order transition in a Mn0.74Fe1.23P0.71Si0.32 crystal. HERFD-XAS and RIXS data show a minor evolution of the spectral features in the upper part of the K-edge for Mn and Fe, consistent with the calculated 4p density of states and fingerprinting the transition. In contrast, no significant evolution of the XES spectra is observed when the transition is crossed. In Fe-rich compositions, the calculations indicate that Fe at the 3g site develops a magnetic moment (2.43 μB) that is smaller than that of Mn at the 3g site (2.93 μB), but larger than that of Fe at the 3f site (1.48 μB). Quantitative XES analysis using the IAD method gives a reasonable agreement with the magnetic moments for different (Mn,Fe)2(P,Si) compositions. However, the reduction of the Fe moment predicted by theory (approx. −0.6μB) is not observed around the transition. This study indicates that the Fe moment collapse at the transition may be weaker than the theoretically predicted value or more gradual in temperature, suggesting a secondary role for this moment instability in the giant magnetocaloric effect of (Mn,Fe)2(P,Si) compounds. ...
Journal article (2026) - W. Hanggai, H. Yibole, F. Guillou, C. Kwakernaak, N. H. van Dijk, E. Brück
The (Mn,Fe)2(P,Si) compounds are one of the rare materials systems that exhibit an isostructural first-order ferromagnetic transition (FOMT) near ambient temperature. Since the discovery of its giant magnetocaloric effect (GMCE), this system is garnering ongoing interest, both for its promising performances for applications and for the scientific interest in uncovering the fundamental mechanisms driving the FOMT. This study examines the evolution of the structure, the microstructure, the thermal and magnetic properties in Mn0.60+x Fe1.3-x P0.66-y Si0.34+y (0 ≤ x ≤ 0.08, x = 2y ) compounds prepared by the melt-spun technique. The simultaneous increase in Mn and Si concentrations leads to a 40 % enhancement in the isothermal entropy change (|Δ S max|) compared to parent compound. Furthermore, we propose a method to separate the latent heat ( L ) from the reversible specific heat. This allows us to establish a convincing correlation between two intrinsic quantities, the latent heat ( L ) and the elastic strain energy ( U e). Our results demonstrate that both latent heat ( L ) and thermal hysteresis (Δ T hys) are proportionally linked and vanish simultaneously at a critical end point. ...
Doctoral thesis (2025) - H. Gai, E.H. Brück, N.H. van Dijk
Efficient energy utilization has been central to human progress, with each new energy source driving societal and technological advancements. While fossil fuels like coal, oil, and natural gas currently dominate, their environmental impact and finite availability underscore the urgent need for sustainable alternatives. Developing environmentally friendly and efficient energy conversion processes is vital to addressing the challenges of resource scarcity and climate change. Magnetocaloric materials (MCMs) are at the forefront of research in advanced cooling technologies due to their ability to exhibit a magnetocaloric effect (MCE). This area of study holds both significant fundamental scientific interest and critical application potential. From a scientific point of view, MCMs are highly intriguing due to their ability to exhibit a giant magnetocaloric effect (GMCE). Uncovering the underlying mechanisms of first-order magnetic transitions (FOMT) plays a pivotal role in advancing research and development in this field [1–6]. From an application perspective, related research primarily focuses on developing 3D-printed bulk materials to achieve gradient composites manufacturing of MCMs with enhanced heat transfer coefficients [7]. This approach is particularly relevant given the narrow operating range of FOMTs, which necessitates multiple material layers to achieve optimal efficiency [8]. However, for the successful commercialization of magnetic cooling and heat pump technologies, the primary future challenge lies in ensuring mechanical stability of GMCMs, which is a critical prerequisite. This thesis explores the unique structure and thermomagnetic properties of Fe2Pbased and potential novel MCM systems using techniques such as magnetization, heat capacity, Mössbauer spectroscopy, Density Functional Theory (DFT), X-ray and neutron diffraction. ...
Journal article (2025) - P. Uliss, H. Gai, F. Kahler, E. Aprea, Q. Jia, Vasiliki Gkouzioti, Jean-Philippe Frimat, E.H. Brück, C.M. Boutry
Magnetothermal stimulation is key in biomedical applications like tumor ablation, drug delivery, and regenerative therapies. A common method involves injecting magnetic particles that heat under an alternating magnetic field (AMF). However, uncontrolled heating can damage healthy tissues. Maintaining temperatures below 45 °C is critical. Using materials with a Curie temperature (Tc) near this limit offers a self-regulating solution, as magnetization—and thus heating—drops sharply at Tc. This study explores Mn0.65Fe1.30P0.65Si0.37 (MCM), a magnetocaloric material composed of non-toxic elements and featuring a tunable Tc. It is engineered to exhibit a Tc of 43 °C, close to the safe physiological threshold. MCM particles are encapsulated in a wax matrix to form a composite that responds to AMF exposure. Heat generated by MCM particles triggers the wax phase transition, while the obtained Tc enables the composite to achieve self-limiting thermal regulation under magnetic field exposure. Biocompatibility tests using human umbilical vein endothelial cells (HUVECs) show over 90% cell viability in direct and indirect contact. Stability tests in phosphate buffers at 37 °C confirm controlled degradation over 28 days. These results demonstrate that MCM is a promising, burn-free magnetic material for safe, localized heating, supporting its use in self-regulating, temperature-responsive biomedical systems. ...
Review (2024) - Na Ta, Jing Yi Huang, Shuai He, W. Hanggai, Luo Meng Chao
The increasing energy consumption in buildings due to cooling and heating, accounting for over one-third of the total energy consumption in society, has become a growing concern. Therefore, reducing building energy consumption has become an urgent issue for countries worldwide. Windows serve as the primary channel for energy exchange between the indoor and the outdoor environments. While providing natural lighting for occupants, windows are also the weakest link in terms of energy consumption. In recent years, there have been some new and superior coating glass technologies compared to traditional low-emissivity glass. These coatings utilize various optical functional materials to regulate the incident sunlight, aiming to save cooling and heating energy consumption. Materials, such as tungsten-based compounds, vanadium dioxide, lanthanum hexaboride, or copper monosulfide, can absorb near-infrared light to effectively control solar radiation by leveraging the localized surface plasmon resonance (LSPR) effect of nanoparticles. This paper mainly introduces the micro-mechanisms of these materials and provides a detailed summary of the latest advancements in coating materials. The application and effects of these coatings in building energy conservation are emphasized. Finally, the challenges and prospects of LSPR-based smart windows are discussed. It is expected that this review will provide new insights into the application of smart windows in green buildings. ...
Journal article (2024) - H. Gai, N.H. van Dijk, E.H. Brück
The transition-metal based alloy system YNi 4-xCo xSi shows a second-order ferromagnetic-to-paramagnetic transition near room temperature. Here, the magnetic structure, the magnetocaloric properties and the magnetic anisotropy of YNi 4-xCo xSi (x = 0–4) are investigated. For x = 3.5, 3.75 and 4.0 a Curie temperature near room temperature is observed with T C = 250, 283 and 310 K, respectively. In orientated YNi 4-xCo xSi powder samples the c axis of the hexagonal crystal structure is found to be the easy magnetic axis, with a large dominant K 2 anisotropy constant (K 2 > K 1 > 0). The magnetic structure and the preferred atomic position for Ni are demonstrated by neutron diffraction measurements. We have found a dramatic decrease in the magnetic moment at the 3 g site in the CaCu 5-type structure (space group P6/mmm), the saturation magnetization and the Curie temperature with increasing Ni concentration. ...
Journal article (2022) - Balnude Nuendute, Wuliji Hanggai, Hargen Yibole, Bao Tana, Ojiyed Tegus, Francois Guillou
Mn compounds presenting magneto-structural phase transitions are currently intensively studied for their giant magnetocaloric effect; nevertheless, several parameters remain to be further optimized. Here, we explore the Mn(Fe,Ni)(Si,Al) series, which presents two advantages. The Mn content is fixed to unity ensuring a large saturation magnetization, and it is based on non-critical Si and Al elements instead of the more commonly employed Ge. Structural and magnetic properties of MnFe0.6 Ni0.4 Si1-x Alx compounds are investigated using powder X-ray diffraction, SEM, EDX, DSC, and magnetic measurements. We demonstrate that a magneto-structural coupling leading to transformation from ferromagnetic with orthorhombic TiNiSi-type structure to a paramagnetic hexagonal Ni2 In-type phase can be realized for 0.06 < x ≤ 0.08. Unfortunately, the first-order transition is relatively broad and incomplete, likely as the result of insufficient sample homogeneity. A comparison between samples synthesized in different conditions (as-cast, quenched from 900 C, or quenched from 1100 C) reveals that Mn(Fe,Ni)(Si,Al) samples decompose into a Mn5 Si3-type phase at intermediate temperatures, preventing the synthesis of high-quality samples by conventional methods such as arc-melting followed by solid-state reaction. By identifying promising MnFe0.6 Ni0.4 Si1-x Alx compositions, this study paves the way toward the realization of a giant magnetocaloric effect in these compounds using alternative synthesis techniques. ...

From macroscopic single crystals to submicron-sized particles

Journal article (2021) - H. Yibole, B. Lingling-Bao, J. Y. Xu, H. Alata, O. Tegus, W. Hanggai, N. H. van Dijk, E. Brück, F. Guillou
While rare-earth magnets exhibit unchallenged hard-magnetic properties, looking for alternatives based on inexpensive elements of non-critical supply remains of utmost interest. Here, we demonstrate that (Fe,Co)2(P,Si) single crystals combine a large magnetocrystalline anisotropy (K1 ≈ 0.9 MJ m−3 at 300 K), high Curie temperatures (TC up to 560 K) and an appreciable saturation specific magnetization (101 A m2 kg−1) leading to a theoretical |BH|max ≈ 165 kJ m-3, making them promising candidate materials as rare-earth-free permanent magnets. Our comparison between (Fe,Co)2P and (Fe,Co)2(P,Si) single crystals highlights that Si substitution reduces the low-temperature magnetocrystalline anisotropy, but strongly enhances TC, making the latter quaternary alloys most favorable for room temperature applications. Submicron-sized particles of Fe1.75Co0.20P0.75Si0.25 were prepared by a top-down ball-milling approach. While the energy products of bonded particles are to this point modest, they demonstrate that permanent magnetic properties can be achieved in (Fe,Co)2(P,Si) quaternary alloys. This work correlates the development of permanent magnetic properties to a control of the microstructure. It paves the way toward the realization of permanent magnetic properties in (Fe,Co)2(P,Si) alloys made of economically competitive Fe, P and Si elements, making these materials desirable for applications. ...