Lanthanide-doped upconversion nanoparticles enable upconversion stimulated emission depletion microscopy with high photostability and low-intensity near-infrared continuous-wave lasers.Controlling energy transfer dyna...Lanthanide-doped upconversion nanoparticles enable upconversion stimulated emission depletion microscopy with high photostability and low-intensity near-infrared continuous-wave lasers.Controlling energy transfer dynamics in these nanoparticles is crucial for super-resolution microscopy with minimal laser intensities and high photon budgets.However,traditional methods neglect the spatial distribution of lanthanide ions and its effect on energy transfer dynamics.Here,we introduce topology-driven energy transfer networks in lanthanide-doped upconversion nanoparticles for upconversion stimulated emission depletion microscopy with reduced laser intensities,maintaining a high photon budget.Spatial separation of Yb^(3+)sensitizers and Tm^(3+)emitters in 50-nm core-shell nanoparticles enhance energy transfer dynamics for super-resolution microscopy.Topology-dependent energy migration produces strong 450-nm upconversion luminescence under low-power 980-nm excitation.Enhanced cross-relaxation improves optical switching efficiency,achieving a saturation intensity of 0.06 MW cm^(−2) under excitation at 980 nm and depletion at 808 nm.Super-resolution imaging with a 65-nm lateral resolution is achieved using intensities of 0.03 MW cm^(−2) for a Gaussian-shaped excitation laser at 980 nm and 1 MW cm^(−2) for a donut-shaped depletion laser at 808 nm,representing a 10-fold reduction in excitation intensity and a 3-fold reduction in depletion intensity compared to conventional methods.These findings demonstrate the potential of harnessing topology-dependent energy transfer dynamics in upconversion nanoparticles for advancing low-power super-resolution applications.展开更多
Energy-intensive technologies and high-precision research require energy-efficient techniques and materials.Lensbased optical microscopy technology is useful for low-energy applications in the life sciences and other ...Energy-intensive technologies and high-precision research require energy-efficient techniques and materials.Lensbased optical microscopy technology is useful for low-energy applications in the life sciences and other fields of technology,but standard techniques cannot achieve applications at the nanoscale because of light diffraction.Farfield super-resolution techniques have broken beyond the light diffraction limit,enabling 3D applications down to the molecular scale and striving to reduce energy use.Typically targeted super-resolution techniques have achieved high resolution,but the high light intensity needed to outperform competing optical transitions in nanomaterials may result in photo-damage and high energy consumption.Great efforts have been made in the development of nanomaterials to improve the resolution and efficiency of these techniques toward low-energy super-resolution applications.Lanthanide ion-doped upconversion nanoparticles that exhibit multiple long-lived excited energy states and emit upconversion luminescence have enabled the development of targeted super-resolution techniques that need low-intensity light.The use of lanthanide ion-doped upconversion nanoparticles in these techniques for emerging low-energy super-resolution applications will have a significant impact on life sciences and other areas of technology.In this review,we describe the dynamics of lanthanide ion-doped upconversion nanoparticles for superresolution under low-intensity light and their use in targeted super-resolution techniques.We highlight low-energy super-resolution applications of lanthanide ion-doped upconversion nanoparticles,as well as the related research directions and challenges.Our aim is to analyze targeted super-resolution techniques using lanthanide ion-doped upconversion nanoparticles,emphasizing fundamental mechanisms governing transitions in lanthanide ions to surpass the diffraction limit with low-intensity light,and exploring their implications for low-energy nanoscale applications.展开更多
基金supported by the National Key Research and Development program of China(Grant No.2022YFB2804301 and Grant No.2021YFB2802000)the Science and Technology Commission of Shanghai Municipality(Grant No.21DZ1100500)+3 种基金the Shanghai Municipal Science and Technology Major Project,the Shanghai Frontiers Science Center Program(2021-2025 No.20)the National Natural Science Foundation of China(Grant No.61975123 and Grant No.62205208)the China Postdoctoral Science Foundation(3722904001,3722904006)the Shanghai Super Postdoctoral Incentive Scheme(5B22904002,5B22904006).
文摘Lanthanide-doped upconversion nanoparticles enable upconversion stimulated emission depletion microscopy with high photostability and low-intensity near-infrared continuous-wave lasers.Controlling energy transfer dynamics in these nanoparticles is crucial for super-resolution microscopy with minimal laser intensities and high photon budgets.However,traditional methods neglect the spatial distribution of lanthanide ions and its effect on energy transfer dynamics.Here,we introduce topology-driven energy transfer networks in lanthanide-doped upconversion nanoparticles for upconversion stimulated emission depletion microscopy with reduced laser intensities,maintaining a high photon budget.Spatial separation of Yb^(3+)sensitizers and Tm^(3+)emitters in 50-nm core-shell nanoparticles enhance energy transfer dynamics for super-resolution microscopy.Topology-dependent energy migration produces strong 450-nm upconversion luminescence under low-power 980-nm excitation.Enhanced cross-relaxation improves optical switching efficiency,achieving a saturation intensity of 0.06 MW cm^(−2) under excitation at 980 nm and depletion at 808 nm.Super-resolution imaging with a 65-nm lateral resolution is achieved using intensities of 0.03 MW cm^(−2) for a Gaussian-shaped excitation laser at 980 nm and 1 MW cm^(−2) for a donut-shaped depletion laser at 808 nm,representing a 10-fold reduction in excitation intensity and a 3-fold reduction in depletion intensity compared to conventional methods.These findings demonstrate the potential of harnessing topology-dependent energy transfer dynamics in upconversion nanoparticles for advancing low-power super-resolution applications.
基金The National Key Research and Development program of China(Grant No.2021YFB2802000 and Grant Nos.2022YFB2804301)the Science and Technology Commission of Shanghai Municipality(Grant No.21DZ1100500)+3 种基金the Shanghai Municipal Science and Technology Major Project,the Shanghai Frontiers Science Center Program(2021-2025 No.20)the National Natural Science Foundation of China(Grant No.61975123 and Grant No.62205208)the China Postdoctoral Science Foundation(3722904001,3722904006)the Shanghai Super Postdoctoral Incentive Scheme(5B22904002,5B22904006).
文摘Energy-intensive technologies and high-precision research require energy-efficient techniques and materials.Lensbased optical microscopy technology is useful for low-energy applications in the life sciences and other fields of technology,but standard techniques cannot achieve applications at the nanoscale because of light diffraction.Farfield super-resolution techniques have broken beyond the light diffraction limit,enabling 3D applications down to the molecular scale and striving to reduce energy use.Typically targeted super-resolution techniques have achieved high resolution,but the high light intensity needed to outperform competing optical transitions in nanomaterials may result in photo-damage and high energy consumption.Great efforts have been made in the development of nanomaterials to improve the resolution and efficiency of these techniques toward low-energy super-resolution applications.Lanthanide ion-doped upconversion nanoparticles that exhibit multiple long-lived excited energy states and emit upconversion luminescence have enabled the development of targeted super-resolution techniques that need low-intensity light.The use of lanthanide ion-doped upconversion nanoparticles in these techniques for emerging low-energy super-resolution applications will have a significant impact on life sciences and other areas of technology.In this review,we describe the dynamics of lanthanide ion-doped upconversion nanoparticles for superresolution under low-intensity light and their use in targeted super-resolution techniques.We highlight low-energy super-resolution applications of lanthanide ion-doped upconversion nanoparticles,as well as the related research directions and challenges.Our aim is to analyze targeted super-resolution techniques using lanthanide ion-doped upconversion nanoparticles,emphasizing fundamental mechanisms governing transitions in lanthanide ions to surpass the diffraction limit with low-intensity light,and exploring their implications for low-energy nanoscale applications.
