Browsing by Author "Lin, Hong-Ji"

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A Metal-Insulator Transition of the Buried MnO2 Monolayer in Complex Oxide Heterostructure
(2016-11-02)
Liu, Heng-Jui
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Lin, Jheng-Cyuan
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Fang, Yue-Wen
;
Wang, Jing-Ching
;
Huang, Bo-Chao
A novel artificially created MnO2 monolayer system is demonstrated in atomically controlled epitaxial perovskite heterostructures. With careful design of different electrostatic boundary conditions, a magnetic transition as well as a metal-insulator transition of the MnO2 monolayer is unveiled, providing a fundamental understanding of dimensionality-confined strongly correlated electron systems and a direction to design new electronic devices.
Antiferromagnetic Interfacial Coupling and Giant Magnetic Hysteresis in La0.5Ca0.5MnO3-SrRuO3 Superlattices
(2018-10-01)
Kumar, Vandrangi Suresh
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Zhou, Shu-Liang
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Liu, Rui-Rui
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Zhu, Yuan-Min
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Liu, Heng-Jui
Superlattices are of great importance due to their potential as new materials genome to synthesize new functional materials. Thus, tuning of the ground state of superlattices is crucial to further control their physical properties. In this study, superlattices (SLs) consisting of alternating layers of SrRuO3 (SRO) (5 nm) and La0.5Ca0.5MnO3 (LCMO) (5 nm) are epitaxially grown on SrTiO3 (STO) and LaAlO3 (LAO) substrates with 10-unit-cell periods. A variation in the substrate-induced-strain for this choice of SLs triggers observation of remarkable properties, such as magnetic anisotropy and large magnetic hysteresis. The strain states experienced by LCMO and SRO in these SLs result in strong ferromagnetic interlayer coupling and weak antiferromagnetic interlayer coupling at low temperatures in SLs of LCMO-SRO/STO and a strong antiferromagnetic interlayer coupling in SLs of LCMO-SRO/LAO. Besides, a large magnetic hysteresis resulting from the predominant magnetic anisotropy of SRO together with the strength of magnetic coupling is observed in SLs of LCMO-SRO/LAO along the out-of-plane direction of the LAO substrate. These four different magnetic behaviors along four different directions of substrate orientations are interpreted in terms of preferential orbital occupation and competing magnetic exchange coupling together with magnetic anisotropy. This study demonstrates the subtleties in controlling the strength of magnetic coupling at the interface and stands as a model system to realize fascinating magnetic phenomena in layer-by-layer hetero-epitaxial oxide films.
Atomic origin of the spin-polarization of the Co2FeAl Heusler compound
(2016-02-25)
Liang, Jaw-Yeu
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Lam, Tu-Ngoc
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Lin, Yan-Cheng
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Chang, Shu-Jui
;
Lin, Hong-Ji
Using synchrotron x-ray techniques, we studied the Co2FeAl spin-polarization state that generates the half-metallicity of the compound during an A(2) (low-spin) -> B-2 (high-spin) phase transition. Given the advantage of element specificity of x-ray techniques, we could fingerprint the structural and magnetic cross-reactions between Co and Fe within a complex Co2FeAl structure deposited on a MgO (0 0 1) substrate. X-ray diffraction and extended x-ray absorption fine structure investigations determined that the Co atoms preferably populate the (1/4,1/4,1/4) and (3/4,3/4,3/4) sites during the development of the B-2 phase. X-ray magnetic spectroscopy showed that although the two magnetic elements were ferromagnetically coupled, they interacted in a competing manner via a charge-transfer effect, which enhanced Co spin polarization at the expense of Fe spin polarization during the phase transition. This means that the spin-polarization of Co2FeAl was electronically dominated by Fe in A(2) whereas the charge transfer turned the dominance to Co upon B-2 formation. Helicity-dependent x-ray absorption spectra also revealed that only the minority state of Co/Fe was involved in the charge-transfer effect whereas the majority state was independent of it. Despite an overall increase of Co2FeAl magnetization, the charge-transfer effect created an undesired trade-off during the Co-Fe exchange interactions, because of the presence of twice as many X sites (Co) as Y sites (Fe) in the Heusler X(2)YZ formula. This suggests that the spin-polarization of Co2FeAl is unfortunately regulated by compromising the enhanced X (Co) sites and the suppressed Y (Fe) sites, irrespective of the development of the previously known high-spin-polarization phase of B-2. This finding provides a possible cause for the limited half-metallicity of Co2FeAl discovered recently. Electronic tuning between the X and Y sites is necessary to further increase the spin-polarization, and likely the half-metallicity as well, of the compound.
Atomistic nucleation sites of Pt nanoparticles on N-doped carbon nanotubes
(2013)
Sun, Chia-Liang
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Pao, Chih-Wen
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Tsai, Huang-Ming
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Chiou, Jau-Wern
;
Ray, Sekhar C.
The atomistic nucleation sites of Pt nanoparticles (Pt NPs) on N-doped carbon nanotubes (N-CNTs) were investigated using C and N K-edge and Pt L-3-edge X-ray absorption near-edge structure (XANES)/extended X-ray absorption fine structure (EXAFS) spectroscopy. Transmission electron microscopy and XANES/EXAFS results revealed that the self-organized Pt NPs on N-CNTs are uniformly distributed because of the relatively high binding energies of the adsorbed Pt atoms at the imperfect sites. During the atomistic nucleation process of Pt NPs on N-CNTs, stable Pt-C and Pt-N bonds are presumably formed, and charge transfer occurs at the surface/interface of the N-CNTs. The findings in this study were consistent with density functional theory calculations performed using cluster models for the undoped, substitutional-N-doped and pyridine-like-N-doped CNTs.
Complex Oxide-Noble Metal Conjugated Nanoparticles
(2013-04-11)
Guo, Jun-Ling
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Chiou, Yao-De
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Liang, Wen-I
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Liu, Heng-Jui
;
Chen, Ying-Jiun
Hybrid nanoparticles (NPs) composed of multiple components offer new opportunities for next-generation materials. In this study, a paradigm for the noble metal/ternary complex oxide hybrid NPs is reported by adopting pulsed laser ablation in liquids. As model hybrids, gold-spinel heterodimer (Au-CoFe2O4) and gold-pervoskite heterodimer (Au-SrTiO3) NPs are investigated. This work has demonstrated the diverse playgroup of NP conjugation enlarged by complex oxides.
Correlation among photoluminescence and the electronic and atomic structures of Sr2SiO4:xEu(3+) phosphors: X-ray absorption and emission studies
(2020-07-29)
Zheng, Shi-Yan
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Chiou, Jau-Wern
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Li, Yueh-Han
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Yang, Cheng-Fu
;
Ray, Sekhar Chandra
A series of Eu3+-activated strontium silicate phosphors, Sr2SiO4:xEu(3+) (SSO:xEu(3+), x=1.0, 2.0 and 5.0%), were synthesized by a sol-gel method, and their crystalline structures, photoluminescence (PL) behaviors, electronic/atomic structures and bandgap properties were studied. The correlation among these characteristics was further established. X-ray powder diffraction analysis revealed the formation of mixed orthorhombic alpha'-SSO and monoclinic beta-SSO phases of the SSO:xEu(3+) phosphors. When SSO:xEu(3+) phosphors are excited under ultraviolet (UV) light (lambda=250 nm,similar to 4.96 eV), they emit yellow (similar to 590 nm), orange (similar to 613 nm) and red (similar to 652 and 703 nm) PL bands. These PL emissions typically correspond to 4f-4f electronic transitions that involve the multiple excited D-5(0)-> F-7(J) levels (J=1, 2, 3 and 4) of Eu3+ activators in the host matrix. This mechanism of PL in the SSO:xEu(3+) phosphors is strongly related to the local electronic/atomic structures of the Eu3+-O2- associations and the bandgap of the host lattice, as verified by Sr K-edge and Eu L-3-edge X-ray absorption near-edge structure (XANES)/extended X-ray absorption fine structure, O K-edge XANES and K-alpha X-ray emission spectroscopy. In the synthesis of SSO:xEu(3+) phosphors, interstitial Eu2O3-like structures are observed in the host matrix that act as donors, providing electrons that are nonradiatively transferred from the Eu 5d and/or O 2p-Eu 4f/5d states (mostly the O 2p-Eu 5d states) to the D-5(0) levels, facilitating the recombination of electrons that have transitioned from the D-5(0) level to the F-7(J) level in the bandgap. This mechanism is primarily responsible for the enhancement of PL emissions in the SSO:xEu(3+) phosphors. This PL-related behavior indicates that SSO:xEu(3+) phosphors are good light-conversion phosphor candidates for use in near-UV chips and can be very effective in UV-based light-emitting diodes.
Coupled microstructural and magnetic transition in Co-doped Ni nano-arrays
(2011-10-01)
Yang, Chao-Yao
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Huang, Chun-Chao
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Tseng, Yuan-Chieh
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Liu, Chien-Min
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Chen, Chih
A superparamagnetic (SM) to ferromagnetic (FM) phase transition was investigated in Co-doped (similar to 6%) electroless plated Ni arrays. The introduction of Co altered the microstructure of the Ni arrays from nanocrystalline to polycrystalline, resulting in a SM -> FM transition. This Co-induced magnetic phase transition is similar to that observed after heat treatment of undoped samples [C. M. Liu, Y. C. Tseng, C. Chen, M. C. Hsu, T. Y. Chao, and Y. T. Cheng, Nanotechnology 20, 415703 (2009); C. C. Huang, C. C. Lo, Y. C. Tseng, C. M. Liu, and C. Chen, J. Appl. Phys. 109, 113905 (2011)]. The role of Co dopant was identified electronically using x-ray magnetic spectroscopy, revealing that the transition modified the Ni host's electronic structure and enhanced its moment by effectively spin-polarizing the Ni 3d conduction band. This was distinctly different than in the heat treatment case, which underwent an electronically independent phase transition. The element-specific magnetic hysteresis of Co and Ni was also probed, which showed that the two elements were magnetically coupled. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3647753]
Defect induced ferromagnetic ordering in epitaxial Zn0.95Mn0.05O films on sapphire (0001)
(2019-12-04)
Liu, Wei-Rein
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Pao, Chih-Wen
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Yu, Doris Weijyun
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Chin, Yi-Ying
;
Wu, Wen-Bin
We report the influence of Mn dopant on magnetic properties of Zn0.95Mn0.05O (ZMO)/Al2O3(0001) hetero-epitaxial systems grown by using pulsed-laser deposition. The room temperature (RT) intrinsic ferromagnetic (FM) ordering verified by superconducting quantum interference device magnetometer and x-ray magnetic circular dichroism spectrum of Mn L-2(,3) edges is ascribed to the substitutional Mn atoms in the Zn site of ZnO. Mn in ZMO has a tetrahedral local symmetry instead of the octahedral symmetry of MnO, after verifying the absence of the Mn-related impurities or clusters in ZMO epitaxial film by Mn K-edge and Zn K-edge x-ray absorption spectroscopy spectrum, as well as the analysis of long-range structural ordering on Renninger scan of forbidden (0005) reflection in x-ray diffraction, transmission electron microscopy and Raman spectrum. Comparison of x-ray absorption spectra of ZMO with those of ZnO epilayers at O K-, Zn K-, and L-3-edges indicates that the substitution of the Zn site with Mn enhances the charge-transfer (CT) transition and the presence of Zn vacancies (V-Zn) also dominate the photoluminescence (PL) spectrum, implying that the formation of numerous V-Zn defects plays an important role in activating FM interactions. The strong CT effect and the existence of high-density V-Zn suggest that the intrinsic RT FM ordering of insulating ZMO is a result of the formation of the bound magnetic polarons (BMPs) that interact with each other via intermediate magnetic impurities.
Effectiveness of organic molecules for spin filtering in an organic spin valve: Reaction-induced spin polarization for Co atop Alq(3)
(2015-01-21)
Tu-Ngoc Lam
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Lai, Yu-Ling
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Chen, Chih-Han
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Chen, Po-Hung
;
Chan, Yuet-Loy
The spin polarization of organic-ferromagnetic interfaces in an organic spin valve critically affects the efficiency of spin injection or detection. We examined the chemical and electronic properties of ferromagnetic Co deposited on organic Alq(3) and the interfacial spin-polarized capability of the electronic states. Our x-ray photoemission spectra and calculations with density-functional theory indicate a sequential and unequal distribution of charge from Co clusters to N and then to O atoms in Alq(3). The preferential orbital hybridization at specific functional sites produces efficient spin polarization of organic molecules. Element-specific measurements of x-ray magnetic circular dichroism demonstrate the preferential spin polarization in the lowest unoccupied molecular orbital state of N atoms at the complex interface for Co atop Alq(3), which agrees satisfactorily with calculation. Our results indicate that an induced interfacial spin polarization on engineering the dominant reaction of Co with mainly N and O atoms in Alq(3) might pave a way for effective spin filtering in organic spintronics.
Effects of strain on the electronic structure and magnetic properties in SrMn0.5Fe0.5O3
(2016-09-01)
Mi, Chun-Wei
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Chin, Yi-Ying
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Hsiao, Yen-Fu
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Fang, Hau-Wei
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Luo, Chih-Wei
The electronic structure and magnetic properties of SrMn0.5Fe0.5O3 powder and films grown on (100)-SrTiO3 (STO) and (100)-LaAlO3 (LAO) substrates by pulsed laser deposition (PLD) were investigated by temperature dependent magnetization and soft x-ray absorption. The results exhibit characteristics of 3d(5) Fe3+, 3d(5) (L) under bar Fe4+, and 3d(3) + 3d(4) (L) under bar Mn4+ at room temperature in all samples. However, the features of 3d(5) Fe3+ and 3d(3) Mn4+ increased significantly for SMFO/LAO at 35 K, which also displayed substantial competition between antiferromagnetic and ferromagnetic order well-above the Neel temperature of SrFeO3 (T-N similar to 134 K). We attributed this to being caused by charge disproportionation resulting from ligand-hole localization, which is more favorable to take place when the sample is under compressive strain.
Electrically enhanced magnetization in highly strained BiFeO3 films
(2016-05)
Yang, Jan-Chi
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Kuo, Chang-Yang
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Liu, Heng-Jui
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Ding, Hang-Chen
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Duan, Chun-Gang
The control of magnetism via an electric field has attracted substantial attention because of potential applications in magnetoelectronics, spintronics and high-frequency devices. In this study, we demonstrate a new approach to enhance and control the magnetization of multiferroic thin film by an electric stimulus. First, to reduce the strength of the antiferromagnetic superexchange interaction in BiFeO3, we applied strain engineering to stabilize a highly strained phase. Second, the direction of the ferroelectric polarization was controlled by an electric field to enhance the Dzyaloshinskii-Moriya interaction in the highly strained BiFeO3 phase. Because of the magnetoelectric coupling in BiFeO3, a strong correlation between the modulated ferroelectricity and enhanced magnetization was observed. The tunability of this strong correlation by an electric field provides an intriguing route to control ferromagnetism in a single-phase multiferroic.
Element-specific study of the coupled magneto-structural and magneto-electronic properties of CoNi nanoarrays
(2013-04-01)
Yang, Chao-Yao
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Tseng, Yuan-Chieh
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Lin, Hong-Ji
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材料科學與工程學系
;
Department of Materials Science and Engineering
The magneto-structural (MS) and magneto-electronic (ME) effects, as well as their coupling relationship, were investigated in electroless-plated (EL) Co0.5Ni0.5 arrays treated by post N-2 annealing and in situ field plating. Separately and combined, these two treatments have been widely employed to improve the properties of magnetic nanostructures. This work aimed to discriminate between treatments with respect to electronic and structural properties, and magnetic degrees of freedom of Co0.5Ni0.5 nanostructures. The field-plated sample exhibited a strong MS-ME coupling due to magneto-crystalline anisotropy (MCA), arising from a FCC (111) preferred orientation with lattice planes stacking orthogonally to the long axial direction of the arrays. A large coercivity was observed in this structure, arising from high magnetic stability. X-ray magnetic circular dichroism revealed that magnetization was enhanced primarily by Co magnetism, while the field-plated sample underwent a MS/ME transition with corresponding increase of the plating field. Conversely, the heat-treated sample comprised isotropically oriented nanocrystals approximately 20 +/- 3 nm in diameter, coated with an oxidation layer (approximately 5 +/- 2 nm thick). The absence of MCA in these samples ensured a weak MS-ME coupling. Although the Ni magnetization of heat-treated samples remained close to that of the field-plated sample, the Co constituent exhibited CoO and Co3O4 phases in addition to the metallic state. By contrast, the Co constituent of the field-plated sample was mainly metallic. The lack of MCA, combined with a complex Co magnetic state, appears responsible for the divergent macroscopic magnetic behaviors of the heat-treated and the field-plated samples. By isolating changes in local magnetic moments of Ni and Co, we gained a fundamental understanding of the effects of post-N-2 annealing and field plating on CoNi. Such knowledge may assist researches in improving the magnetic properties of bimetallic nanostructures.
Enhanced Magnetic Anisotropy via Quasi-Molecular Magnet at Organic-Ferromagnetic Contact
(2013-01-17)
Hsu, Yao-Jane
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Lai, Yu-Ling
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Chen, Chih-Han
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Lin, Ying-Chang
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Chien, Hsiu-Yun
To realize the origin of efficient spin injection at organic-ferromagnetic contact in organic spintronics, we have implemented the formation of quasi-molecular magnet via surface restructuring of a strong organic acceptor, tetrafluoro-tetracyanoquinodimethane (F4-TCNQ), in contact with ferromagnetic cobalt. Our results demonstrate a spin-polarized F4-TCNQ layer and a remarkably enhanced magnetic anisotropy of the Co film. The novel magnetic properties are contributed from strong magnetic coupling caused by the molecular restructuring that displays an angular anchoring conformation of CN and upwardly protruding fluorine atoms. We conclude that the pi bonds of CN, instead of the lone-pair electrons of N atoms, contribute to the hybridization-induced magnetic coupling between CN and Co and generate a superior magnetic order on the surface.
Enhanced Magnetocaloric Effect Driven by Interfacial Magnetic Coupling in Self-Assembled Mn3O4-La0.7Sr0.3MnO3 Nanocomposites
(2015-12-09)
Vandrangi, Suresh K.
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Yang, Jan-Chi
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Zhu, Yuan-Min
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Chin, Yi-Ying
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Lin, Hong-Ji
Magnetic refrigeration, resulting from the magneto caloric effect of a material around the magnetic phase-transition temperature, is a topic of great interest as it is considered to be an alternate energy solution to conventional vapor-compression refrigeration. The viability of a magnetic refrigeration system for magnetic cooling can be tested by exploiting materials in various forms, from bulk to nanostrucutres. In this study, magnetocaloric properties of self-assembled Mn3O4-La0.7Sr0.3MnO3 nanocomposites, with varying doping concentrations of Mn3O4 in the form of nanocrystals embedded in the La0.7Sr0.3MnO3 matrix, are investigated. The temperatures corresponding to the paramagnetic-to-ferromagnetic transitions are higher, and the values of change in magnetic entropy under a magnetic field of 2 T show an enhancement (highest being similar to 130%) for the nanocomposites with low doping concentrations of Mn3O4, compared to that of pure La0.7Sr0.3MnO3 thin films. Relative cooling power remain close to those of La0.7Sr0.3MnO3. The enhanced magnetic phase-transition temperature and magnetocaloric effect are interpreted and evidenced in the framework of interfacial coupling between Mn3O4 and La0.7Sr0.3MnO3. This work demonstrates the potentiality of self-assembled nanostructures for magnetic cooling near room temperature under low magnetic fields.
Enhancing the magnetic moment of ferrimagnetic NiCo2O4 via ion irradiation driven oxygen vacancies
(2018-06-01)
Pandey, Parul
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Bitla, Yugandhar
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Zschornak, Matthias
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Wang, Mao
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Xu, Chi
Ion irradiation has emerged as a powerful tool for the efficient control of uniaxial lattice expansion to fine tune and modulate the otherwise inaccessible complex correlated phases in oxide thin-films. We report the fine tuning of the magnetic moment, ferromagnetic-paramagnetic and metal-insulator transition temperatures in the NiCo2O4 inverse-spinel oxide by creating oxygen deficiencies, employing high energy He-ion irradiation. Tailoring of oxygen vacancies and consequently a uniaxial lattice expansion in the out-of-plane direction drives the system toward the increase of the magnetic moment by two-times in magnitude. The magnetic moment increases with the He-ion irradiation fluence up to 2.5 x 10(16)/cm(2) . Our results are corroborated well by spin-polarized electronic structure calculations with density functional theory and X-ray absorption spectroscopic data, which show peak-height change and energy shift of Co-L-2,L-3 and Ni-L-2,L-3 edges driven by the oxygen vacancies. These results demonstrate a new pathway of tailoring oxygen vacancies via He-ion irradiation, useful for designing new functionalities in other complex oxide thin-films. (C) 2018 Author(s).
Heteroepitaxy of Co-Based Heusler Compound/Muscovite for Flexible Spintronics
(2019-09-25)
Chen, Yi-Cheng
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Yen, Min
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Lai, Yu-Hong
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Markou, Anastasios
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Zhang, Liguo
Materials with high spin-polarization play an important role in the development of spintronics. Co-based Heusler compounds are a promising candidate for practical applications because of their high Curie temperature and tunable half-metallicity. However, it is a challenge to integrate Heusler compounds into thin film heterostructures because of the lack of control on crystallinity and chemical disorder, critical factors of novel behaviors. Here, muscovite is introduced as a growth substrate to fabricate epitaxial Co2MnGa films with mechanical flexibility. The feature of heteroepitaxy is evidenced by the results of X-ray diffraction and transmission electron microscopy. Moreover, high chemical ordering with superior properties is delivered according to the observation of large Hall conductivity (680 Omega(-1) cm(-1)) and highly saturated magnetic moment (similar to 3.93 mu(B)/f.u.), matching well with bulk crystals. Furthermore, the excellence of magnetic and electrical properties is retained under the various mechanical bending conditions. Such a result suggests that the development of Co2MnGa/muscovite heteroepitaxy provides not only a pathway to the thin film heterostructure based on high-quality Heusler compounds but also a new aspect of spintronic applications on flexible substrates.
Interfacial symmetry of Co-Alq(3)-Co hybrid structures for effective spin filtering
(2015-11-01)
Lam, Tu-Ngoc
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Lai, Yu-Ling
;
Chen, Chih-Han
;
Chen, Po-Hung
;
Wei, Der-Hsin
Understanding the interfacial behavior at FM-OSC-FM hybrid structures for both the bottom contact (Alq(3) adsorption on Co, Co/Alq(3)) and the top contact (Co atop Alq(3), Alq(3)/Co) is crucial for efficient spin filtering with transport of spin-polarized charge carriers through these interfaces. X-ray photoelectron spectroscopy (XPS) spectra indicate a symmetry of charge transfer from Co to Alq(3) and the corresponding orbital hybridization to a certain extent at both contacts. The alignment of energy levels at both Alq(3)/Co and Co/Alq(3) heterostructures is depicted with ultraviolet photoelectron spectroscopy (UPS). Through magnetic images acquired with a X-ray photoemission electron microscope (XPEEM), the strong hybridization of the top contact presents no micromagnetic domain but still shows magnetic coupling, to some extent, to the bottom contact in the Co-Alq(3)-Co trilayer structure. Measurements of X-ray magnetic circular dichroism (XMCD) demonstrate the induced spin-polarization of non-magnetic Alq(3) at both contacts, proving Alq(3) a unique and promising organic material for spin filtering in OSV. (C) 2015 Elsevier B.V. All rights reserved.
Interfacial symmetry of Co-Alq(3)-Co hybrid structures for effective spin filtering (vol 354, pg 90, 2015)
(2018-05-31)
Tu-Ngoc Lam
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Lai, Yu-Ling
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Chen, Chih-Han
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Chen, Po-Hung
;
Wei, Der-Hsin
Large Magnetoresistance in Magnetically Coupled SrRuO3-CoFe2O4 Self-Assembled Nanostructures
(2013-09-14)
Liu, Heng-Jui
;
Vu-Thanh Tra
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Chen, Ying-Jiun
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Huang, Rong
;
Duan, Chun-Gang
Magnetic Mesocrystal-Assisted Magnetoresistance in Manganite
(2014-11-01)
Yang, Jan-Chi
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He, Qing
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Zhu, Yuan-Min
;
Lin, Jheng-Cyuan
;
Liu, Heng-Jui
Mesocrystal, a new class of crystals as compared to conventional and well-known single crystals and polycrystalline systems, has captured significant attention in the past decade. Recent studies have been focused on the advance of synthesis mechanisms as well as the potential on device applications. In order to create further opportunities upon functional mesocrystals, we fabricated a self-assembled nanocomposite composed of magnetic CoFe2O4 mesocrystal in Sr-doped manganites. This combination exhibits intriguing structural and magnetic tunabilities. Furthermore, the antiferromagnetic coupling of the mesocrystal and matrix has induced an additional magnetic perturbation to spin-polarized electrons, resulting in a significantly enhanced magnetoresistance in the nanocomposite. Our work demonstrates a new thought toward the enhancement of intrinsic functionalities assisted by mesocrystals and advanced design of novel mesocrystal-embedded nanocomposites.