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  • 詹楊皓 博士
    Proceedings of National Academy of Sciences
    Shift current is a direct current generated from nonlinear light–matter interaction in a noncentrosymmetric crystal and is considered a promising candidate for next-generation photovoltaic devices. The mechanism for shift currents in real materials is, however, still not well understood, especially if electron–hole interactions are included. Here, we employ a first-principles interacting Green’s-function approach on the Keldysh contour with real-time propagation to study photocurrents generated by nonlinear optical processes under continuous wave illumination in real materials. We demonstrate a strong direct current shift current at subbandgap excitation frequencies in monolayer GeS due to strongly bound excitons, as well as a giant excitonic enhancement in the shift current coefficients at above bandgap photon frequencies. Our re ...
  • 郭哲來 博士
    The Journal of Physical Chemistry Letters 11, 10067 (2020); https://doi.org/10.1021/acs.jpclett.0c03059.
    Complex vibrational features of solvated hydronium ion, H3O+, in 3 μm enable us to look into the vibrational coupling among O-H stretching modes and other degrees of freedom. Two anharmonic coupling schemes have often been engaged to explain observed spectra: coupling with OH bending overtone, known as Fermi resonance (FR), has been proposed to account for the splitting of the OH stretch band at ~3300 cm-1 in H3O+…Ar3, but an additional peak in H3O+…(N2)3 at the similar frequency region has been assigned to a combination band (CB) with the low-frequency intermolecular stretches. While even stronger vibrational coupling is expected in H3O+…(H2O)3, such pronounced peaks are a ...
  • 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.
  • 謝雅萍 博士
    Nano Lett., https://doi.org/10.1021/acs.nanolett.1c02331 (2021).
    We here demonstrate the multifunctional properties of atomically thin heterojunctions that are enabled by strong interfacial interactions and their integration into ultra-high performance, self-powered sensors. Epitaxial alignment between tin diselenide and graphene through direct growth produces thermoelectric and mechanoelectric properties beyond the ability of either component. An unprecedented ZT of 2.43 originated from the synergistic combination of graphene’s high carrier conductivity and SnSe2 mediated thermal conductivity lowering. Moreover, strong interaction at the SnSe2/graphene interface produces stress localization that results in a novel 2D-crack-assisted strain sensing mechanism whose sensitivity (GF=450) is superior to all other 2D materials. Finally, the graphene-assisted growth process, permits the formation of hi ...
  • 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  ...
  • 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 ...
  • 陳貴賢 博士
    Nature Commmunictions 11, 3682 (2020).
    In this study, a self-capping vaporliquid-solid reaction is proposed to fabricate large-grain, continuous MoS2 films. An intermediate liquid phase-Na2Mo2O7 is formed through a eutectic reaction of MoO3 and NaF,followed by being sulfurized into MoS2. The as-formed MoS2 seeds function as a capping layer that reduces the nucleation density and promotes lateral growth. By tuning the driving force of the reaction, large mono/bilayer (1.1 mm/200 μm) flakes or full-coverage films (with a record-high average grain size of 450 μm) can be grown on centimeter-scale substrates. The field-effect transistors fabricated from the full-coverage films show high mobility (33 and 49 cm2V-1s-1 for the mono and bilayer regions) and on/off ratio (1 ~ 5 × 108) across a 1.5 cm × 1.5 cm region.
  • 郭哲來 博士
    Angewandte Chemie International Edition, https://doi.org/10.1002/anie.202012665 (2020).
    Experimental infrared spectra between 2600 to 3800 cm-1 for a series of asymmetric proton bound dimers with protonated trimethylamine (TMA–H+) as the proton donor were recorded and analyzed. Based on conventional wisdom, the frequency of the N-H+ stretching mode is expected to red shift as the proton affinity of proton acceptors (Ar, N2, CO, C2H2, H2O, CH3OH, and C2H5OH) increases. The observed band, however, shows a peculiar splitting of ≈300 cm-1 with the intensity shifting pattern resembling a two-level system. Theoretical investigation based on ab initio anharmonic algorithms reveals that the observed band splitting and its extraordinarily large gap of ≈300 cm-1 is a result of strong coupling betw ...
  • 余慈顏 博士
    Annals of Clinical and Translational Neurology, 2019 Oct;6(10):1961-1970. 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 ...
  • 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 ...
  • 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
    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 ...
  • 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  ...
  • 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  ...
  • 許良彥 博士
    Chem, 2020, 6, 3396-3408.
    Large-scale inhomogeneous plasmonic metal chips have been demonstrated as a promisingplatform for biochemical sensing, but the origin of their strong fluorescence enhancementsand average gap dependence is a challenging issue due to the complexity of modelingtremendous molecules within inhomogeneous gaps. To address this issue, we bridgedmicroscopic mechanisms and macroscopic observations, developed a kinetic model, andexperimentally investigated the fluorescence enhancement factors of IR800-streptavidinimmobilized on metal nanoisland films (NIFs). Inspired by the kinetic model, we controlledthe distribution of IR800-streptavidin within the valleys of NIFs by regioselectivemodification and achieved the fluorescence intensity enhancement up to 488-fold. Thekinetic model allows us to qualitatively explain the mechanism of fluorescence intensityenhance ...
  • 許良彥 博士
    Journal of Chemical Physics 155, 074101 (2021); https://doi.org/10.1063/5.0057018
    Our previous study [S. Wang et al., J. Chem. Phys. 153, 184102 (2020)] has shown that in a complex dielectric environment, molecular emission power spectra can be expressed as the product of the lineshape function and the electromagnetic environment factor (EEF). In this work, we focus on EEFs in a vacuum–NaCl–silver system and investigate molecular emission power spectra in the strong exciton–polariton coupling regime. A numerical method based on computational electrodynamics is presented to calculate the EEFs of single-molecule emitters in a dispersive and lossy dielectric environment with arbitrary shapes. The EEFs in the far-field region depend on the detector position, emission frequency, and molecular orientation. We quantitatively analyze the asymptotic behavior of the EFFs in the far-field region and qualitatively provide  ...
  • 謝雅萍 博士
    Advanced Functional Materials, 2004370 (2020).
    Atomic‐precision patterning at large scale is a central requirement for nanotechnology and future electronics that is hindered by the limitations of lithographical techniques. Historically, imperfections of the fabrication tools have been compensated by multi‐patterning using sequential lithography processes. The realization of nanometer‐scale features from much larger patterns through offset stacking of atomically thin masks is demonstrated. A unique mutual stabilization effect between two graphene layers produces atomically abrupt transitions that selectively expose single‐layer covered regions. Bilayer regions, on the other hand, protect the underlying substrate from removal for several hours permitting transfer of atomic thickness variations into lateral features in various semiconductors. Nanoscopic offsets between two 2D materials lay ...
  • 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 ...
  • 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 ...
  • 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 ...

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演講資訊

Nov
04
2021
Cooperative micro-excitation and structural rearrangement in cold dusty plasma liquids around freezing
伊林教授, 國立中央大學物理學系
2021-11-04 下午 03:30  浦大邦紀念講堂
Nov
11
2021
(To be announced)
林俊成主任, 國立清華大學化學系
2021-11-11 下午 03:30  浦大邦紀念講堂
Nov
18
2021
Characterization of multiphoton states in boson sampling systems
吳俊毅助理教授, 淡江大學物理學系
2021-11-18 下午 03:30  浦大邦紀念講堂
Nov
25
2021
Game of spikes: effects of mutations on the structure and function of SARS-CoV-2 spike variants
徐尚德副研究員, 中央研究院生物化學研究所
2021-11-25 下午 02:00  浦大邦紀念講堂
Dec
09
2021
Rydberg-based quantum sensors using atomic vapors
陳易馨助理教授, 國立中山大學物理系
2021-12-09 下午 03:30  浦大邦紀念講堂

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