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Despite significant advances toward accurate tuning of the size and shape of colloidal nanoparticles, the precise control of the surface chemistry thereof remains a grand challenge. It is desirable to conjugate functional bio-molecules onto the selected facets of nanoparticles owing to the versatile capabilities rendered by the molecules. We report here facet-selective conjugation of DNA molecules onto upconversion nanoparticles via ligand competition reaction. Different binding strengths of phosphodiester bonds and phosphate groups on DNA and the surfactant molecules al low one to create heterogeneous bio-chemistry surface for upconversion nanoparticles. The tailored surface properties lead to the formation of distinct self-assembly structures. Our findings provide insight into the interactions between biomolecules and nanoparticles, unveiling the potential of using nanoparticles as fundamental building blocks for creating self-assembled nano-architectures.

Despite significant advances toward accurate tuning of the size and shape of colloidal nanoparticles, the precise control of the surface chemistry thereof remains a grand challenge. It is desirable to conjugate functional bio-molecules onto the selected facets of nanoparticles owing to the versatile capabilities rendered by the molecules. We report here facet-selective conjugation of DNA molecules onto upconversion nanoparticles via ligand competition reaction. Different binding strengths of phosphodiester bonds and phosphate groups on DNA and the surfactant molecules al low one to create heterogeneous bio-chemistry surface for upconversion nanoparticles. The tailored surface properties lead to the formation of distinct self-assembly structures. Our findings provide insight into the interactions between biomolecules and nanoparticles, unveiling the potential of using nanoparticles as fundamental building blocks for creating self-assembled nano-architectures.

Despite significant advances toward accurate tuning of the size and shape of colloidal nanoparticles, the precise control of the surface chemistry thereof remains a grand challenge. It is desirable to conjugate functional bio-molecules onto the selected facets of nanoparticles owing to the versatile capabilities rendered by the molecules. We report here facet-selective conjugation of DNA molecules onto upconversion nanoparticles via ligand competition reaction. Different binding strengths of phosphodiester bonds and phosphate groups on DNA and the surfactant molecules al low one to create heterogeneous bio-chemistry surface for upconversion nanoparticles. The tailored surface properties lead to the formation of distinct self-assembly structures. Our findings provide insight into the interactions between biomolecules and nanoparticles, unveiling the potential of using nanoparticles as fundamental building blocks for creating self-assembled nano-architectures.

The key to produce inorganic heterogeneous nanostructures, and to integrate multiple functionalities, is to enhance or at least retain the functionalities of different components of materials. However, this ideal scenario is often deteriorated at the interface of the heterogeneous nanostructures due to lattice mismatches, resulting in downgraded performance in most hybrid nanomaterials. Here, we report that there is a narrow window in controlling temperature in a Lewis acid-base reaction process to facilitate epitaxial alignment during the synthesis of hybrid nanomaterials. We demonstrate a perfectly fused NaYF 4 :Yb,Tm@ZnO heterogeneous nanostructure, in which the semiconductor ZnO shell can be epitaxially grown onto lanthanide-doped upconversion nanoparticles. By achieving a matched crystal lattice, the interface defects and crystalline grain boundaries are minimized to enable more efficient energy transfer from the upconversion nanoparticles to the semiconductor, resulting in both enhanced upconversion luminescence intensity and superior photoelectrochemical properties. This strategy provides an outstanding approach to endow lanthanide-doped upconversion nanoparticles with versatile properties.

The key to produce inorganic heterogeneous nanostructures, and to integrate multiple functionalities, is to enhance or at least retain the functionalities of different components of materials. However, this ideal scenario is often deteriorated at the interface of the heterogeneous nanostructures due to lattice mismatches, resulting in downgraded performance in most hybrid nanomaterials. Here, we report that there is a narrow window in controlling temperature in a Lewis acid-base reaction process to facilitate epitaxial alignment during the synthesis of hybrid nanomaterials. We demonstrate a perfectly fused NaYF 4 :Yb,Tm@ZnO heterogeneous nanostructure, in which the semiconductor ZnO shell can be epitaxially grown onto lanthanide-doped upconversion nanoparticles. By achieving a matched crystal lattice, the interface defects and crystalline grain boundaries are minimized to enable more efficient energy transfer from the upconversion nanoparticles to the semiconductor, resulting in both enhanced upconversion luminescence intensity and superior photoelectrochemical properties. This strategy provides an outstanding approach to endow lanthanide-doped upconversion nanoparticles with versatile properties.

The key to produce inorganic heterogeneous nanostructures, and to integrate multiple functionalities, is to enhance or at least retain the functionalities of different components of materials. However, this ideal scenario is often deteriorated at the interface of the heterogeneous nanostructures due to lattice mismatches, resulting in downgraded performance in most hybrid nanomaterials. Here, we report that there is a narrow window in controlling temperature in a Lewis acid-base reaction process to facilitate epitaxial alignment during the synthesis of hybrid nanomaterials. We demonstrate a perfectly fused NaYF 4 :Yb,Tm@ZnO heterogeneous nanostructure, in which the semiconductor ZnO shell can be epitaxially grown onto lanthanide-doped upconversion nanoparticles. By achieving a matched crystal lattice, the interface defects and crystalline grain boundaries are minimized to enable more efficient energy transfer from the upconversion nanoparticles to the semiconductor, resulting in both enhanced upconversion luminescence intensity and superior photoelectrochemical properties. This strategy provides an outstanding approach to endow lanthanide-doped upconversion nanoparticles with versatile properties.

The key to produce inorganic heterogeneous nanostructures, and to integrate multiple functionalities, is to enhance or at least retain the functionalities of different components of materials. However, this ideal scenario is often deteriorated at the interface of the heterogeneous nanostructures due to lattice mismatches, resulting in downgraded performance in most hybrid nanomaterials. Here, we report that there is a narrow window in controlling temperature in a Lewis acid-base reaction process to facilitate epitaxial alignment during the synthesis of hybrid nanomaterials. We demonstrate a perfectly fused NaYF 4 :Yb,Tm@ZnO heterogeneous nanostructure, in which the semiconductor ZnO shell can be epitaxially grown onto lanthanide-doped upconversion nanoparticles. By achieving a matched crystal lattice, the interface defects and crystalline grain boundaries are minimized to enable more efficient energy transfer from the upconversion nanoparticles to the semiconductor, resulting in both enhanced upconversion luminescence intensity and superior photoelectrochemical properties. This strategy provides an outstanding approach to endow lanthanide-doped upconversion nanoparticles with versatile properties.

The key to produce inorganic heterogeneous nanostructures, and to integrate multiple functionalities, is to enhance or at least retain the functionalities of different components of materials. However, this ideal scenario is often deteriorated at the interface of the heterogeneous nanostructures due to lattice mismatches, resulting in downgraded performance in most hybrid nanomaterials. Here, we report that there is a narrow window in controlling temperature in a Lewis acid-base reaction process to facilitate epitaxial alignment during the synthesis of hybrid nanomaterials. We demonstrate a perfectly fused NaYF 4 :Yb,Tm@ZnO heterogeneous nanostructure, in which the semiconductor ZnO shell can be epitaxially grown onto lanthanide-doped upconversion nanoparticles. By achieving a matched crystal lattice, the interface defects and crystalline grain boundaries are minimized to enable more efficient energy transfer from the upconversion nanoparticles to the semiconductor, resulting in both enhanced upconversion luminescence intensity and superior photoelectrochemical properties. This strategy provides an outstanding approach to endow lanthanide-doped upconversion nanoparticles with versatile properties.

The rapid development of a variety of molecular contrast agents makes the multimodality bioimaging highly attractive towards higher resolution, more sensitive, informative diagnosis. The key lies in the development of facile material synthesis that allows the integration of multiple contrast agents, ideally in a way that each of the components should be logically assembled to maximize their performances. Here, we report the one-pot programmable growth of multifunctional heterogeneous nanocrystal with tunable size, shape, composition, and properties. We demonstrated a facile one-pot hot-injection method to enable the highly selectively controlled growth of different sodium lanthanide fluoride nanomaterials in either longitudinal or transversal directions with atomic scale precision. This technique allows the upconversion luminescence signal, MRI signal and x-ray signal logically integrated and optimized within one single versatile nanoplatform for multimode bioimaging. These findings suggest that the facile strategy developed here have the promising to get the desired heterogeneous nanocrystals as an all-in-one contrast agent for integrated and self-correlative multimodal bioimaging.

The rapid development of a variety of molecular contrast agents makes the multimodality bioimaging highly attractive towards higher resolution, more sensitive, informative diagnosis. The key lies in the development of facile material synthesis that allows the integration of multiple contrast agents, ideally in a way that each of the components should be logically assembled to maximize their performances. Here, we report the one-pot programmable growth of multifunctional heterogeneous nanocrystal with tunable size, shape, composition, and properties. We demonstrated a facile one-pot hot-injection method to enable the highly selectively controlled growth of different sodium lanthanide fluoride nanomaterials in either longitudinal or transversal directions with atomic scale precision. This technique allows the upconversion luminescence signal, MRI signal and x-ray signal logically integrated and optimized within one single versatile nanoplatform for multimode bioimaging. These findings suggest that the facile strategy developed here have the promising to get the desired heterogeneous nanocrystals as an all-in-one contrast agent for integrated and self-correlative multimodal bioimaging.

The rapid development of a variety of molecular contrast agents makes the multimodality bioimaging highly attractive towards higher resolution, more sensitive, informative diagnosis. The key lies in the development of facile material synthesis that allows the integration of multiple contrast agents, ideally in a way that each of the components should be logically assembled to maximize their performances. Here, we report the one-pot programmable growth of multifunctional heterogeneous nanocrystal with tunable size, shape, composition, and properties. We demonstrated a facile one-pot hot-injection method to enable the highly selectively controlled growth of different sodium lanthanide fluoride nanomaterials in either longitudinal or transversal directions with atomic scale precision. This technique allows the upconversion luminescence signal, MRI signal and x-ray signal logically integrated and optimized within one single versatile nanoplatform for multimode bioimaging. These findings suggest that the facile strategy developed here have the promising to get the desired heterogeneous nanocrystals as an all-in-one contrast agent for integrated and self-correlative multimodal bioimaging.

The rapid development of a variety of molecular contrast agents makes the multimodality bioimaging highly attractive towards higher resolution, more sensitive, informative diagnosis. The key lies in the development of facile material synthesis that allows the integration of multiple contrast agents, ideally in a way that each of the components should be logically assembled to maximize their performances. Here, we report the one-pot programmable growth of multifunctional heterogeneous nanocrystal with tunable size, shape, composition, and properties. We demonstrated a facile one-pot hot-injection method to enable the highly selectively controlled growth of different sodium lanthanide fluoride nanomaterials in either longitudinal or transversal directions with atomic scale precision. This technique allows the upconversion luminescence signal, MRI signal and x-ray signal logically integrated and optimized within one single versatile nanoplatform for multimode bioimaging. These findings suggest that the facile strategy developed here have the promising to get the desired heterogeneous nanocrystals as an all-in-one contrast agent for integrated and self-correlative multimodal bioimaging.

The ultimate frontier in nanomaterials engineering is to realize their composition control with atomic scale precision to enable fabrication of nanoparticles with desirable size, shape and surface properties. Such control becomes even more useful when growing hybrid nanocrystals designed to integrate multiple functionalities. Here we report achieving such degree of control in a family of rare-earth-doped nanomaterials. We experimentally verify the co-existence and different roles of oleate anions (OA-) and molecules (OAH) in the crystal formation. We identify that the control over the ratio of OA- to OAH can be used to directionally inhibit, promote or etch the crystallographic facets of the nanoparticles. This control enables selective grafting of shells with complex morphologies grown over nanocrystal cores, thus allowing the fabrication of a diverse library of monodisperse sub-50 nm nanoparticles. With such programmable additive and subtractive engineering a variety of three-dimensional shapes can be implemented using a bottom-up scalable approach.

The ultimate frontier in nanomaterials engineering is to realize their composition control with atomic scale precision to enable fabrication of nanoparticles with desirable size, shape and surface properties. Such control becomes even more useful when growing hybrid nanocrystals designed to integrate multiple functionalities. Here we report achieving such degree of control in a family of rare-earth-doped nanomaterials. We experimentally verify the co-existence and different roles of oleate anions (OA-) and molecules (OAH) in the crystal formation. We identify that the control over the ratio of OA- to OAH can be used to directionally inhibit, promote or etch the crystallographic facets of the nanoparticles. This control enables selective grafting of shells with complex morphologies grown over nanocrystal cores, thus allowing the fabrication of a diverse library of monodisperse sub-50 nm nanoparticles. With such programmable additive and subtractive engineering a variety of three-dimensional shapes can be implemented using a bottom-up scalable approach.

The ultimate frontier in nanomaterials engineering is to realize their composition control with atomic scale precision to enable fabrication of nanoparticles with desirable size, shape and surface properties. Such control becomes even more useful when growing hybrid nanocrystals designed to integrate multiple functionalities. Here we report achieving such degree of control in a family of rare-earth-doped nanomaterials. We experimentally verify the co-existence and different roles of oleate anions (OA-) and molecules (OAH) in the crystal formation. We identify that the control over the ratio of OA- to OAH can be used to directionally inhibit, promote or etch the crystallographic facets of the nanoparticles. This control enables selective grafting of shells with complex morphologies grown over nanocrystal cores, thus allowing the fabrication of a diverse library of monodisperse sub-50 nm nanoparticles. With such programmable additive and subtractive engineering a variety of three-dimensional shapes can be implemented using a bottom-up scalable approach.

The ultimate frontier in nanomaterials engineering is to realize their composition control with atomic scale precision to enable fabrication of nanoparticles with desirable size, shape and surface properties. Such control becomes even more useful when growing hybrid nanocrystals designed to integrate multiple functionalities. Here we report achieving such degree of control in a family of rare-earth-doped nanomaterials. We experimentally verify the co-existence and different roles of oleate anions (OA-) and molecules (OAH) in the crystal formation. We identify that the control over the ratio of OA- to OAH can be used to directionally inhibit, promote or etch the crystallographic facets of the nanoparticles. This control enables selective grafting of shells with complex morphologies grown over nanocrystal cores, thus allowing the fabrication of a diverse library of monodisperse sub-50 nm nanoparticles. With such programmable additive and subtractive engineering a variety of three-dimensional shapes can be implemented using a bottom-up scalable approach.