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Creators/Authors contains: "Zhao, Zhibo"

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  1. The ability to accommodate multiple principal cations within a single crystallographic structure makes high entropy oxides (HEOs) ideal systems for exploring new composition–property relationships. In this work, the high-entropy design strategy is extended to strained single-crystal HEO-manganite (HEO-Mn) thin films. Phase-pure orthorhombic films of (Gd0.2La0.2Nd0.2Sm0.2Sr0.2)MnO3 were deposited on three different single-crystal substrates: SrTiO3 (STO) (100), NdGaO3 (110), and LaAlO3 (LAO) (100), each inducing different degrees of epitaxial strain. Fully coherent growth of the thin films is observed in all cases, despite the high degree of lattice mismatch between HEO-Mn and LAO. Magnetometry measurements reveal distinct differences in the magnetic properties between epitaxially strained HEO-Mn thin films and their bulk crystalline HEO counterparts. In particular, the bulk polycrystalline HEO-Mn shows two magnetic transitions as opposed to a single one observed in epitaxial thin films. Moreover, the HEO-Mn film deposited on LAO exhibits a significant reduction in the Curie temperature, which is attributed to the strong variation of the in-plane lattice parameter along the thickness of the film and the resulting changes in the Mn–O–Mn bond geometry. Thus, this preliminary study demonstrates the potential of combining high entropy design with strain engineering to tailor the structure and functionality of perovskite manganites. 
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  2. Abstract High entropy oxides (HEOs), based on the incorporation of multiple‐principal cations into the crystal lattice, offer the possibility to explore previously inaccessible oxide compositions and unconventional properties. Here it is demonstrated that despite the chemical complexity of HEOs external stimuli, such as epitaxial strain, can selectively stabilize certain magneto‐electronic states. Epitaxial (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4‐HEO thin films are grown in three different strain states: tensile, compressive, and relaxed. A unique coexistence of rocksalt and spinel‐HEO phases, which are fully coherent with no detectable chemical segregation, is revealed by transmission electron microscopy. This dual‐phase coexistence appears as a universal phenomenon in (Co0.2Cr0.2Fe0.2Mn0.2Ni0.2)3O4epitaxial films. Prominent changes in the magnetic anisotropy and domain structure highlight the strain‐induced bidirectional control of magnetic properties in HEOs. When the films are relaxed, their magnetization behavior is isotropic, similar to that of bulk materials. However, under tensile strain, the hardness of the out‐of‐plane (OOP) axis increases significantly. On the other hand, compressive straining results in an easy OOP magnetization and a maze‐like magnetic domain structure, indicating the perpendicular magnetic anisotropy. Generally, this study emphasizes the adaptability of the high entropy design strategy, which, when combined with coherent strain engineering, opens additional prospects for fine‐tuning properties in oxides. 
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  3. Abstract Thrombosis in the circulation system can lead to major myocardial infarction and cardiovascular deaths. Understanding thrombosis formation is necessary for developing safe and effective treatments. In this work, using digital light processing (DLP)-based 3D printing, we fabricated sophisticated in vitro models of blood vessels with internal microchannels that can be used for thrombosis studies. In this regard, photoacoustic microscopy (PAM) offers a unique advantage for label-free visualization of the 3D-printed vessel models, with large penetration depth and functional sensitivity. We compared the imaging performances of two PAM implementations: optical-resolution PAM and acoustic-resolution PAM, and investigated 3D-printed vessel structures with different patterns of microchannels. Our results show that PAM can provide clear microchannel structures at depths up to 3.6 mm. We further quantified the blood oxygenation in the 3D-printed vascular models, showing that thrombi had lower oxygenation than the normal blood. We expect that PAM can find broad applications in 3D printing and bioprinting for in vitro studies of various vascular and other diseases. 
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  4. Abstract Three-dimensional (3D) bioprinting has emerged as an enabling tool for various biomedical applications, such as tissue regeneration and tissue model engineering. To this end, the development of bioinks with multiple functions plays a crucial role in the applications of 3D bioprinting technologies. In this study, we propose a new bioink based on two immiscible aqueous phases of gelatin methacryloyl (GelMA) and dextran, further endowed with anti-bacterial and anti-inflammatory properties. This micropore-forming GelMA-dextran (PGelDex) bioink exhibited excellent printability with vat-polymerization, extrusion, and handheld bioprinting methods. The porous structure was confirmed after bioprinting, which promoted the spreading of the encapsulated cells, exhibiting the exceptional cytocompatibility of this bioink formulation. To extend the applications of such a micropore-forming bioink, interleukin-4 (IL-4)-loaded silver-coated gold nanorods (AgGNRs) and human mesenchymal stem cells (MSCs) were simultaneously incorporated, to display synergistic anti-infection behavior and immunomodulatory function. The results revealed the anti-bacterial properties of the AgGNR-loaded PGelDex bioink for both Gram-negative and Gram-positive bacteria. The data also indicated that the presence of IL-4 and MSCs facilitated macrophage M2-phenotype differentiation, suggesting the potential anti-inflammatory feature of the bioink. Overall, this unique anti-bacterial and immunomodulatory micropore-forming bioink offers an effective strategy for the inhibition of bacterial-induced infections as well as the ability of immune-regulation, which is a promising candidate for broadened tissue bioprinting applications. 
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  5. Abstract Digital light processing bioprinting favors biofabrication of tissues with improved structural complexity. However, soft-tissue fabrication with this method remains a challenge to balance the physical performances of the bioinks for high-fidelity bioprinting and suitable microenvironments for the encapsulated cells to thrive. Here, we propose a molecular cleavage approach, where hyaluronic acid methacrylate (HAMA) is mixed with gelatin methacryloyl to achieve high-performance bioprinting, followed by selectively enzymatic digestion of HAMA, resulting in tissue-matching mechanical properties without losing the structural complexity and fidelity. Our method allows cellular morphological and functional improvements across multiple bioprinted tissue types featuring a wide range of mechanical stiffness, from the muscles to the brain, the softest organ of the human body. This platform endows us to biofabricate mechanically precisely tunable constructs to meet the biological function requirements of target tissues, potentially paving the way for broad applications in tissue and tissue model engineering. 
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