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  • 高橋開人 博士
    Journal of Physical Chemistry A, 123, 5300-5308.
    Unsaturated carbon cluster chains often have chemical properties depending on the cluster size. While carbon cluster cation chains show odd−even variation in the reactivity with hydrogen, thechemistry of the carbon anion chain has been poorly understood even for the bimolecular reaction with hydrogen. We present a systematic theoretical study based on transition state calculations and molecular dynamics trajectory simulations for the reaction of Cn (n = 2−8) + H2. We show that carbon cluster chain anion also has an odd−even variation in reactivity where the even ones are more reactive. In addition, dynamics trajectory shows that while odd n only resulted in the CnH2 product with direct H insertion similar to the static reaction pathway, even  ...
  • 賴品光 博士
    Nucleic Acids Research, doi: 10.1093/nar/gkaa669 (2020).
    Tracking DNA double strand break (DSB) repair is paramount for the understanding and therapeutic development of various diseases including cancers. Herein, we describe a multiplexed bioluminescent repair reporter (BLRR) for non-invasive monitoring of DSB repair pathways in living cells and animals. The BLRR approach employs secreted Gaussia and Vargula luciferases to simultaneously detect homology-directed repair (HDR) and non-homologous end joining (NHEJ), respectively. BLRR data are consistent with next-generation sequencing results for reporting HDR (R2 = 0.9722) and NHEJ (R2 = 0.919) events. Moreover, BLRR analysis allows longitudinal tracking of HDR and NHEJ activities in cells, and enables detection of DSB repairs in xenografted tumours in vivo. Using the BLRR system, we observed a significant difference in the efficienc ...
  • 謝佳龍 博士
    ACS Nano 13(10), 10918-10928 (2019)
    Single-molecule tracking is a powerful method to study molecular dynamics in living systems including biological membranes. High-resolution single-molecule tracking requires a bright and stable signal, which has typically been facilitated by nanoparticles due to their superb optical properties. However, there are concerns about using a nanoparticle to label a single molecule because of its relatively large size and the possibility of cross-linking multiple target molecules, both of which could affect the original molecular dynamics. In this work, using various labeling schemes, we investigate the effects using nanoparticles to measure the diffusion of single-membrane molecules. We demonstrate a simple and robust strategy for the monovalent and oriented labeling of a single lipid molecule with a AuNP by using naturally dimeric rhizavidin (rAv) as a  ...
  • 汪治平 博士
    Nature Communication 11, 2787 (2020)
    Availability of relativistically intense, single-cycle, tunable infrared sources will open up newareas of relativistic nonlinear optics of plasmas, impulse IR spectroscopy and pump-probeexperiments in the molecular fingerprint region. However, generation of such pulses is still achallenge by current methods. Recently, it has been proposed that time dependent refractiveindex associated with laser-produced nonlinear wakes in a suitably designed plasma densitystructure rapidly frequency down-converts photons. The longest wavelength photons slipbackwards relative to the evolving laser pulse to form a single-cycle pulse within the nearlyevacuated wake cavity. This process is called photon deceleration. Here, we demonstrate thisscheme for generating high-power (~100 GW), near single-cycle, wavelength tunable(3–20 μm), infrared pulses using an 81 ...
  • 陳貴賢 博士
    Nature Commmunictions 11, 4233 (2020).
    Nonnoble metal catalysts are low-cost alternatives to Pt for the oxygen reduction reactions (ORRs), which have been studied for various applications in electrocatalytic systems. Among them, transition metal complexes, characterized by a redox-active single-metal-atom with biomimetic ligands, such as pyrolyzed cobalt–nitrogen–carbon (Co–N x /C), have attracted considerable attention. Therefore, we reported the ORR mechanism of pyrolyzed Vitamin B12 using operando X-ray absorption spectroscopy coupled with electrochemical impedance spectroscopy, which enables operando monitoring of the oxygen binding site on the metal center. material design strategies for high-performance electrocatalysts for fuel cell applications. Furthermore, the charge transfer mechanism between the catalyst and reactant enables further Co–O species  ...
  • 張煥正 博士
    ACS Appl. Mater. Interfaces 12, 3847−3853 (2020).
    Fluorescent nanodiamond (FND) containing nitrogen-vacancy (NV) centers as built-in fluorophores exhibits a nearly constant emission profile over 550 – 750 nm upon excitation by vacuum-ultraviolet (VUV), extreme ultraviolet (EUV), and X- radiations from a synchrotron source over the energy (wavelength) range of 6.2 – 1450 eV (0.86 – 200 nm).  The photoluminescence (PL) quantum yield of FND increases steadily with the increasing excitation energy, attaining a value as great as 1700% at 700 eV (1.77 nm).  Notably, the yield curve is continuous, having no gap in the VUV to X-ray region.  In addition, no significant PL intensity decreases were observed for hours.  Applying the FND sensor to measure the absorption cross sections of gaseous O2 over 110 – 200 nm and comparing the measurements with ...
  • 林志民 博士
    Angew. Chem. Int. Ed. (DOI: 10.1002/anie.201900711, 2019).
    Recent reports [Jara‐Toro et al., Angew. Chem. Int. Ed. 2017, 56, 2166 and PCCP 2018, 20, 27885] suggest that the rate coefficient of OH reactions with alcohols would increase by up to two times in going from dry to high humidity. This finding would have an impact on the budget of alcohols in the atmosphere and it may explain differences in measured and modeled methanol concentrations. The results were based on a relative technique carried out in a small Teflon bag, which might suffer from wall reactions. The effect was reinvestigated using a direct fluorescence probe of OH radicals, and no catalytic effect of H2O could be found. Experiments in a Teflon bag were also carried out, but the results of Jara‐Toro et al. were not reproducible. Further theoretical calculations show that the water‐mediated reactions have negligible rates compared to  ...
  • 賴品光 博士
    Advanced Science, doi:/10.1002/advs.202001467 (2020).
    Extracellular particles (EPs) including extracellular vesicles (EVs) and exomeres play significant roles in diseases and therapeutic applications. However, their spatiotemporal dynamics in vivo have remained largely unresolved in detail due to the lack of a suitable method. Therefore, a bioluminescence resonance energy transfer (BRET)‐based reporter, PalmGRET, is created to enable pan‐EP labeling ranging from exomeres (<50 nm) to small (<200 nm) and medium and large (>200 nm) EVs. PalmGRET emits robust, sustained signals and allows the visualization, tracking, and quantification of the EPs from whole animal to nanoscopic resolutions under different imaging modalities, including bioluminescence, BRET, and fluorescence. Using PalmGRET, it is shown that EPs released by lung metastatic hepatocellular carcinoma (HCC) exhibit lung tropism wi ...
  • 廖仲麒 博士
    eLife 9, e53580 (2020).
    Subdistal appendages (sDAPs) are centriolar elements observed proximal to the distal appendages (DAPs) in vertebrates. Despite their obvious presence, structural and functional understanding of sDAPs remains elusive. Here, by combining super-resolved localization analysis and CRISPR-Cas9 genetic perturbation, we find that, although DAPs and sDAPs are primarily responsible for distinct functions in ciliogenesis and microtubule anchoring respectively, the presence of one element actually affects the positioning of the other. Specifically, we find dual layers of both ODF2 and CEP89, where their localizations are differentially regulated by DAP and sDAP integrity. DAP depletion relaxes longitudinal occupancy of sDAP protein ninein to cover the DAP region, implying a role of DAPs in sDAP positioning. Removing sDAPs alter the distal border of centrosomal ...
  • 許良彥 博士
    J. Phys. Chem. Lett. 11, 15, 5948–5955 (2020).
    We investigate the coherent-to-incoherent transition of molecular fluorescence of a chromophore above a silver surface (including bulk and thin-film systems) and explore the distance dependence of fluorescence rate enhancement. In the framework of macroscopic quantum electrodynamics, we generalize our previous theory to include multiple vibrational modes. The present theory can accurately describe quantum dynamics from the coherent limit to the incoherent limit. Moreover, we introduce a new concept Incoherent Index to quantify the degree of quantum coherence and demonstrate that the coherent-to-incoherent transition can be controlled by the dielectric environment and the molecule–silver distance. In addition, our theory indicates that strong molecule–photon (polariton) coupling can be achieved by virtue of small Huang–Rhys factors ...
  • 曾文碧 博士
    Physical Chemistry Chemical Physics, 21, 9665-9671 (2019).
    The resonance-enhanced multiphoton ionization (REMPI) of a mixed sandwich complex has been achieved for the first time when exciting (η7-C7H7)(η5-C5H5)Cr via the Rydberg 4pz state. The REMPI spectrum is indicative of unexpectedly small changes of the sandwich geometry on excitation. Time- dependent DFT calculations reveal fine effects of the ligand nature on the molecular and electronic structure variations accompanying electronic excitation. Different trends are predicted for the sandwich geometry transformations in the mixed sandwich complex and its symmetric isomer, (η6-C6H6)2Cr, both on Rydberg excitation and ionization.
  • 羅佩凌 博士
    Communications Chemistry, 3, 95 (2020)
    Quantitative determination of multiple transient species is critical in investigating reaction mechanisms and kinetics under various conditions. Dual-comb spectroscopy, a comb-laser-based multi-heterodyne interferometric technique that enables simultaneous achievement of broadband, high-resolution, and rapid spectral acquisition, opens a new era of time-resolved spectroscopic measurements. Employing an electro-optic dual-comb spectrometer with central wavelength near 3 µm coupled with a Herriott multipass absorption cell, here we demonstrate simultaneous determination of multiple species, including methanol, formaldehyde, HO2 and OH radicals, and investigate the reaction kinetics. In addition to quantitative spectral analyses of high-resolution and tens of microsecond time-resolved spectra recorded upon flash photolysis of precurso ...
  • 謝雅萍 博士
    Nature Materials, 19, 745–751 (2020).
    Carrier transport processes in assemblies of nanostructures rely on morphology-dependent and hierarchical conduction mechanisms, whose complexity cannot be captured by current modelling approaches. Here we apply the concept of complex networks to modelling carrier conduction in such systems. The approach permits assignment of arbitrary connectivity and connection strength between assembly constituents and is thus ideal for nanostructured films, composites and other geometries. Modelling of simplified rod-like nanostructures is consistent with analytical solutions, whereas results for more realistic nanostructure assemblies agree with experimental data and reveal conduction behaviour not captured by previous models. Fitting of ensemble measurements also allows the conduction properties of individual constituents to be extracted, which are subsequent ...
  • 余慈顏 博士
    Annals of Clinical and Translational Neurology, DOI:10.1002/acn3.50887
    Objective: Ala97Ser (A97S) is the major transthyretin (TTR) mutation in Taiwanese patients of familial amyloid polyneuropathy (FAP), characterized by a late-onset but rapidly deteriorated neuropathy. Tafamidis can restore the stability of some mutant TTR tetramers and slow down the progression of TTR-FAP. However, there is little understanding of the biophysical features of A97S-TTR mutant and the pharmacological modulation effect of tafamidis on it. This study aims to delineate the biophysical characteristics of A97S-TTR and the pharmacological modulation effect of tafamidis on this mutant.Method: The stability of TTR tetramers was assessed by urea denaturation and differential scanning calorimetry. Isothermal titration calorimetry (ITC) was used to measure the binding constant of tafamidis to TTR. Nuclear magnetic resonance spectroscopy (NMR) tit ...

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演講資訊

Sep
24
2020
How Chemistry Facilitates 3D Super-Resolution Imaging of Brain
陳壁彰副研究員, 本院應用科學研究中心
2020-09-24 下午 03:30  浦大邦紀念講堂
Oct
08
2020
Hydrogenation-Induced Effects on Magnetism of Pd-Alloy Thin Films
林文欽教授, 國立臺灣師範大學物理學系
2020-10-08 下午 03:30  浦大邦紀念講堂
Oct
15
2020
Quantum Tomography with Machine Learning
李瑞光教授, 國立清華大學光電工程研究所
2020-10-15 下午 03:30  浦大邦紀念講堂
Oct
22
2020
Glycoproteomic Identification of Novel Tumor Biomarkers and Viral Receptors
張權發教授, 國立成功大學醫學檢驗生物技術學系
2020-10-22 下午 03:30  浦大邦紀念講堂
Oct
29
2020
Multifunctional Nanocarriers for Efficient Cancer Immunotherapy
陳韻晶副教授, 國立清華大學生物醫學工程研究所
2020-10-29 下午 03:30  浦大邦紀念講堂

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