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Suppressed Triplet Exciton Diffusion Due to Small Orbital Overlap as a Key Design Factor for Ultralong-Lived Room-Temperature Phosphorescence in Molecular Crystals
摘要： Persistent room-temperature phosphorescence (RTP) under ambient conditions is attracting attention due to its strong potential for applications in bioimaging, sensing, or optical recording. Molecular packing leading to a rigid crystalline structure that minimizes nonradiative pathways from triplet state is often investigated for efficient RTP. However, for complex conjugated systems a key strategy to suppress the nonradiative deactivation is not found yet. Here, the origin of small rates of a nonradiative decay process from triplet states of conjugated molecular crystals showing RTP is reported. Optical microscopy analysis showed that, despite a favorable molecular stacking, an aromatic crystal with strong RTP is characterized by small diffusion length and small values of the diffusion coefficient of triplet excitons. Quantum chemical calculations reveal a large overlap between the lowest unoccupied molecular orbitals but very small overlap between the highest occupied molecular orbitals (HOMOs). Inefficient electron exchange caused by the small overlap of HOMOs prevents triplet excitons from diffusing over long distances and consequently from quenching at defect sites inside the crystal or at the crystal surface. These results will allow design of comprehensive molecular structures to obtain molecular solids with more efficient RTP.
关键词： suppressed nonradiative rate,persistent room-temperature phosphorescence,triplet exciton diffusion,molecular orbital overlap,fluorescence microscopy
更新于2025-09-23 15:23:52
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Single Particle Tracking and Super-Resolution Imaging of Membrane-Assisted Stop-and-Go Diffusion and Lattice Assembly of DNA Origami
摘要： DNA nanostructures offer the possibility to mimic functional biological membrane components due to their nanometer-precise shape configurability and versatile biochemical functionality. Here we show that the diffusional behavior of DNA nanostructures and their assembly into higher order membrane-bound lattices can be controlled in a stop-and-go manner and that the process can be monitored with super-resolution imaging. The DNA structures are transiently immobilized on glass-supported lipid bilayers by changing the mono- and divalent cation concentrations of the surrounding buffer. Using DNA-PAINT super-resolution microscopy, we confirm the fixation of DNA origami structures with different shapes. On mica-supported lipid bilayers, in contrast, we observe residual movement. By increasing the concentration of NaCl and depleting MgCl2, a large fraction of DNA structures restarts to diffuse freely on both substrates. After addition of a set of oligonucleotides that enables three Y-shaped monomers to assemble into a three-legged shape (triskelion), the triskelia can be stopped and super-resolved. Exchanging buffer and adding another set of oligonucleotides triggers the triskelia to diffuse and assemble into hexagonal 2D lattices. This stop-and-go imaging technique provides a way to control and observe the diffusional behavior of DNA nanostructures on lipid membranes that could also lead to control of membrane-associated cargos.
关键词： single-particle tracking,DNA origami,diffusion,super-resolution microscopy,lipid membrane,DNA nanotechnology
更新于2025-09-23 15:23:52
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Learning compact q-space representations for multi-shell diffusion-weighted MRI
摘要： Diffusion-weighted MRI measures the direction and scale of the local diffusion process in every voxel through its spectrum in q-space, typically acquired in one or more shells. Recent developments in microstructure imaging and multi-tissue decomposition have sparked renewed attention in the radial b-value dependence of the signal. Applications in motion correction and outlier rejection therefore require a compact linear signal representation that extends over the radial as well as angular domain. Here, we introduce SHARD, a data-driven representation of the q-space signal based on spherical harmonics and a radial decomposition into orthonormal components. This representation provides a complete, orthogonal signal basis, tailored to the spherical geometry of q-space and calibrated to the data at hand. We demonstrate that the rank-reduced decomposition outperforms model-based alternatives in human brain data, whilst faithfully capturing the micro- and meso-structural information in the signal. Furthermore, we validate the potential of joint radial-spherical as compared to single-shell representations. As such, SHARD is optimally suited for applications that require low-rank signal predictions, such as motion correction and outlier rejection. Finally, we illustrate its application for the latter using outlier robust regression.
关键词： Diffusion-weighted imaging,Blind source separation,Multi-shell HARDI,Dimensionality reduction
更新于2025-09-23 15:23:52
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Understanding Spatiotemporal Photocarrier Dynamics in Monolayer and Bulk MoTe <sub/>2</sub> for Optimized Optoelectronic Devices
摘要： Semiconducting molybdenum ditelluride has emerged as a promising transition-metal dichalcogenide with a number of novel properties. In particular, its bandgap in infrared range makes it an attractive candidate for ultrathin and high-performance infrared optoelectronic applications. Dynamical properties of photocarriers play a key role in determining performance of such devices. We report an experimental study on spatiotemporal dynamics of photocarriers in both monolayer and bulk MoTe2. Transient absorption measurement in reflection geometry revealed ultrafast thermalization and relaxation processes of photocarriers and lifetimes of about 60 and 80 ps in monolayer and bulk MoTe2, respectively. By spatially resolved transient absorption measurements on monolayer, we obtained an exciton diffusion coefficient of 20 ± 10 cm2 s?1, a mean free time of 200 fs, a mean free path of 20 nm, and a diffusion length of 350 nm. The corresponding values for the bulk sample are 40 ± 10 cm2 s?1, 400 fs, 40 nm, and 570 nm, respectively. These results provide fundamental information for understanding and optimizing performance of MoTe2-based optoelectronic devices.
关键词： two-dimensional material,exciton,transient absorption,molybdenum ditelluride,transition-metal dichalcogenide,diffusion,photocarrier dynamics
更新于2025-09-23 15:23:52
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heterostructures: Examination of spin relaxation mechanism
摘要： The thickness, temperature, and composition studies of spin diffusion length (SDL) and spin Hall angle (SHA) are performed by measuring the spin Hall magnetoresistance in Pd1?xPtx/Y3Fe5O12 (=YIG) heterostructures. The SDL is found to be invariant to changes in the electron momentum relaxation time by varying the temperature, the normal metal (NM) thickness, or the alloy composition, while the SHA exhibits a nonmonotonic dependence on temperature. These findings suggest the appearance of D’yakonov-Perel’ spin relaxation mechanism and phonon skew scattering in our heterostructures that is associated with strong interfacial Rashba spin-orbit coupling (IRSOC). At last, we employ the ab initio calculations to quantify the IRSOC at the inversion-symmetry-broken NM/YIG interface.
关键词： spin diffusion length,spin relaxation mechanism,spin Hall angle,interfacial Rashba spin-orbit coupling,PdPt/YIG heterostructures
更新于2025-09-23 15:23:52
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Controlling the emission and absorption spectrum of a quantum emitter in a dynamic environment
摘要： We study the emission spectrum and absorption spectrum of a quantum emitter when it is driven by various pulse sequences. We consider the Uhrig sequence of nonequidistant πx pulses, the periodic sequence of πxπy pulses and the periodic sequence of πz pulses (phase kicks). We find that, similar to the periodic sequence of πx pulses, the Uhrig sequence of πx pulses has emission and absorption that are, with small variations, analogous to those of the resonance fluorescence spectrum. In addition, while the periodic sequence of πz pulses produces a spectrum that is dependent on the detuning between the emitter and the pulse carrier frequency, the Uhrig sequence of nonequidistant πx pulses and the periodic sequence of πxπy pulses have spectra with little dependence on the detuning as long as it stays moderate along with the number of pulses. This implies that they can also, similar to the previously studied periodic sequence of πx pulses, be used to tune the emission or absorption of quantum emitters to specific frequencies, to mitigate inhomogeneous broadening and to enhance the production of indistinguishable photons from emitters in the solid state.
关键词： spectral diffusion,emission/absorption spectrum,solid state emitter,pulse-driven emitter
更新于2025-09-23 15:23:52
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Influence of fuel nature on dye adsorption efficiency of solution combustion derived zinc oxide nanoparticles: A comparative study
摘要： The present work demonstrates the use of coffee husk extract as a fuel (otherwise an agro waste) for the synthesis of nano zinc oxide (ZnO) by one step solution combustion synthesis. We also show the comparative studies of coffee husk extract (green fuel) derived nano ZnO (CHZnO) and sugar (chemical fuel) derived nano ZnO (SZnO) as an adsorbent for Congo red dye removal. The adsorption characteristics were investigated with respect to changes in pH, temperature, initial dye concentration, adsorbent dose and contact time. CHZnO exhibited higher adsorption capacity (76 mg/g) compared to SZnO (56 mg/g). The equilibrium adsorption data were analyzed using various isotherm models (Langmuir, Freundlich, Temkin, and Dubinin-Radushkevith) and thermodynamic parameters. Among the models studied, Langmuir isotherm fitted well with experimental equilibrium data (R2>0.99). Adsorption kinetics was found to follow pseudo-second order with the highest R2 value. Intraparticle or pore diffusion was the major rate controlling step in the adsorption process. The present study demonstrates the potential application of agro-based bio-waste as a novel fuel in the synthesis of nanomaterials for use as efficient adsorbents in water treatment.
关键词： Adsorption,Intraparticle diffusion,Coffee husk extract,nano ZnO,Congo Red
更新于2025-09-23 15:23:52
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A study of surface diffusion of ternary (Cu-Ag-Zr) adatoms clusters for applications in thin film formation
摘要： This study presents the diffusion of heterogeneous ternary (Cu‐Ag‐Zr) adatoms clusters on Ag(111) using molecular dynamics techniques which could be important for the surface phenomena's and helpful for the ternary cluster's growth and formation of ternary alloy‐based thin films. The mechanism of nanoscale surface diffusion is investigated for 1Cu‐1Ag‐1Zr, 2Cu‐2Ag‐2Zr, 3Cu‐3Ag‐3Zr, and 4Cu‐4Ag‐4Zr clusters at temperatures 300, 500, and 700 K. The diffusion mechanism displays that the diffusion of trimer cluster exhibits hopping, sliding, and shearing at 300 K, whereas for hexamer, nonamer, and decamer, the diffusion rate is low; however, breathing, anchoring, and concentrated motion dominates. At 500 K, trimer and hexamer show the process of atomic exchange; however, the atomic exchange is not observed in the case of nonamer and decamer diffusion. The atomic exchange mechanism of Cu and Zr adatoms dominates at 700 K for all size clusters, except Ag adatoms, where Zr adatoms show a relatively more tendency. Separation and rejoining of the one and two adatoms (likely Zr adatom) are also witnessed at high temperature. The pop‐up of Ag adatoms also occurs in very short intervals over the remaining adatoms of clusters. Interestingly, during trimer diffusion, the adsorption of the Zr‐ or Cu‐adatom among the trimer cluster into the substitutional site is found. At 700 K, vacancy generation, filling of vacancies, and migration of vacancy, in the neighborhood of the adatoms cluster, also observed. Moreover, the rate of diffusion decreases with the size increase of the clusters and increases with the increase in temperature.
关键词： molecular dynamics,adatoms clusters,vacancy diffusion,surface diffusion
更新于2025-09-23 15:22:29
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Comparison of basis functions and q-space sampling schemes for robust compressed sensing reconstruction accelerating diffusion spectrum imaging
摘要： Time constraints placed on magnetic resonance imaging often restrict the application of advanced diffusion MRI (dMRI) protocols in clinical practice and in high throughput research studies. Therefore, acquisition strategies for accelerated dMRI have been investigated to allow for the collection of versatile and high quality imaging data, even if stringent scan time limits are imposed. Diffusion spectrum imaging (DSI), an advanced acquisition strategy that allows for a high resolution of intra-voxel microstructure, can be sufficiently accelerated by means of compressed sensing (CS) theory. CS theory describes a framework for the efficient collection of fewer samples of a data set than conventionally required followed by robust reconstruction to recover the full data set from sparse measurements. For an accurate recovery of DSI data, a suitable acquisition scheme for sparse q-space sampling and the sensing and sparsifying bases for CS reconstruction need to be selected. In this work we explore three different types of q-space undersampling schemes and two frameworks for CS reconstruction based on either Fourier or SHORE basis functions. After CS recovery, diffusion and microstructural parameters and orientational information are estimated from the reconstructed data by means of state-of-the-art processing techniques for dMRI analysis. By means of simulation, diffusion phantom and in vivo DSI data, an isotropic distribution of q-space samples was found to be optimal for sparse DSI. The CS reconstruction results indicate superior performance of Fourier-based CS-DSI compared to the SHORE-based approach. Based on these findings we outline an experimental design for accelerated DSI and robust CS reconstruction of the sparse measurements that is suitable for the application within time-limited studies.
关键词： diffusion MRI,sparse acquisition,q-space undersampling,microstructure,compressed sensing,basis functions,diffusion spectrum imaging
更新于2025-09-23 15:22:29
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[IEEE 2018 International Conference on Simulation of Semiconductor Processes and Devices (SISPAD) - Austin, TX, USA (2018.9.24-2018.9.26)] 2018 International Conference on Simulation of Semiconductor Processes and Devices (SISPAD) - The Impact of Dopant Diffusion on Random Dopant Fluctuation in Si Nanowire FETs: A Quantum Transport Study
摘要： In this work, we perform statistical quantum transport simulations with 3×3 nm2 Si nanowire (NW) field-effect transistors (FETs) to investigate the impact of dopant diffusion on random dopant fluctuation. First, we use an effective mass Hamiltonian for the transport where the confinement and transport effective masses are extracted from the tight-binding band structure calculations. The dopant diffusion along the transport direction from the source/drain regions to the channel region is modeled by the Gaussian doping profile. To generate random discrete dopants, we adopt a rejection scheme considering the 3-dimensional atomic arrangement of the NW structures. Our statistical simulation results show that the diffused dopants into the channel region cause large variability problems in Si NW FETs.
关键词： non-equilibrium Green's function,tight-binding,dopant diffusion,random discrete dopants,silicon nanowire
更新于2025-09-23 15:22:29