Search

Surface-specific sum frequency generation vibrational spectroscopy is applied to study the molecular configuration of short-chain n-alkanethiol self-assembled monolayers (SAMs with n = 2–6) on the Au surface. For monolayers with n ≥ 3, the alkanethiols are upright-oriented, with the CH3 tilt angle varying between ∼33° and ∼46° in clear even–odd dependency. The ethanethiol monolayer (n = 2) is, however, found to exhibit a distinct lying-down configuration with a larger methyl tilt angle (67°–79°) and a smaller CH2 tilt angle (56°–68°). Such a unique configurational transition from n = 2 to n ≥ 3 discloses the steric effect owing to chain–chain interaction among neighboring molecules. Through density functional theory calculations, the transition is further confirmed to be energetically favorable for thiols on a defective reconstructed Au(111) surface but not on the pristine one. Our study highlights the roles of the chain–chain interaction and the substrate surface atomic structure when organizing SAMs, offering a strategic pathway for exploiting their applications. [ABSTRACT FROM AUTHOR]

An economical and stable single-shot pulse picker design without dispersion, nonlinear effect, and limitation on wavelength is proposed. This design is composed of a periodic pulse blocker (PPB), a control unit, and a mechanical shutter. It has successfully been applied to the commercial high-fluence femtosecond laser with 11-mm beam diameter, 2-mJ pulse energy, and 1-kHz repetition rate. Significantly, by incorporating commercial optical choppers equipped with custom-designed chopper blades in the PPB, this design can accommodate lasers with fluences reaching 610 mJ/cm2 and the standard 1 kHz repetition rate typical of high-fluence lasers. Furthermore, the proposed design provides a cost-effective substitute compared to using electro-optic modulators or acousto-optic modulators. [ABSTRACT FROM AUTHOR]

Mesenchymal stem cells (MSCs) play an important role as immune modulator through interaction with several immune cells, including macrophages. In this study, the immunomodulatory potency of human umbilical cord‐derived mesenchymal stem cells (hUC‐MSCs) was demonstrated in the in vivo middle cerebral artery occlusion (MCAo)‐induced brain injury rat model and in vitro THP‐1‐derived macrophages model. At 24 h after induction of MCAo, hUC‐MSCs was administered via tail vein as a single dose. Remarkably, hUC‐MSCs could inhibit M1 polarization and promote M2 polarization of microglia in vivo after 14 days induction of MCAo. Compared with THP‐1‐derived macrophages which had been stimulated by lipopolysaccharide, the secretion of proinflammatory cytokines, tumor necrosis factor‐α (TNF‐α) and interferon‐γ inducible protein (IP‐10), were significantly reduced in the presence of hUC‐MSCs. Moreover, the secretion of anti‐inflammatory cytokine, interleukin‐10 (IL‐10), was significantly increased after cocultured with hUC‐MSCs. Prostaglandins E2 (PGE2), secreted by hUC‐MSCs, is one of the crucial immunomodulatory factors and could be inhibited in the presence of COX2 inhibitor, NS‐398. PGE2 inhibition suppressed hUC‐MSCs immunomodulatory capability, which was restored after addition of synthetic PGE2, establishing the minimum amount of PGE2 required for immunomodulation. In conclusion, our data suggested that PGE2 is a crucial potency marker involved in the therapeutic activity of hUC‐MSCs through macrophages immune response modulation and cytokines regulation. This study provides the model for the development of a surrogate quantitative potency assay of immunomodulation in stem cells production. [ABSTRACT FROM AUTHOR]

Cigarette smoke (CS) has been reported to induce oxidative stress and inflammatory process in the lungs. However, the role of human umbilical cord-derived mesenchymal stem cells (hUC-MSCs) in the regulation of pulmonary inflammation remains unclear. The objective of this study is to investigate the effects of hUC-MSCs on lung inflammation in the acute CS-induced pulmonary inflammation animal model. Eight-week-old male C57BL/6 mice were intravenously administered 3 × 106, 1 × 107, and 3 × 107 cells/kg of hUC-MSCs as well as normal saline alone (control) after 3 days of CS exposure. Mice exposed to high-efficiency particulate air (HEPA)-filtered room air served as the CS control group. High-dose (3 × 107 cells/kg) hUC-MSC administration significantly decreased tumor necrosis factor (TNF)-α in the bronchoalveolar lavage fluid (BALF) of CS-exposed mice (p < 0.05). The chemokine (CXC motif) ligand 1/keratinocyte chemoattractant (CXCL1/KC) in BALF were significantly reduced by low-dose (3 × 106 cells/kg) and high-dose (3 × 107 cells/kg) hUC-MSC (p < 0.05). Medium-dose hUC-MSC administration decreased interleukin (IL)-1β in lung of mice, and TNF-α and caspase-3 were decreased in the lung of CS-exposed mice by medium- and high-dose MSC (p < 0.05). Low-dose hUC-MSCs significantly elevated serum CXCL1/KC and IL-1β in CS-exposed mice (p < 0.05). Our results suggest that high-dose hUC-MSCs reduced pulmonary inflammation and had antiapoptotic effects in acute pulmonary inflammation. [ABSTRACT FROM AUTHOR]

We report investigations on the elasticity of superconducting FeSe using picosecond ultrasonic technique. The tetragonal (001) FeSe thin film, deposited on a processed SrTiO3 substrate by the pulsed laser deposition, exhibits distinct c-axis preferred orientation and single-crystalline features as a result of the x-ray diffraction. The high-quality crystallinity thus enables quantitative examinations of anisotropic stiffness coefficients (C33) of FeSe, correlating to the interatomic interaction in the simplest iron-based superconductor. Our experiment indicates a room-temperature C33 of 40.9 ± 0.4 GPa and material stiffening of 4.3% at low temperatures, which can be explained by the weakening of anharmonic phonon-phonon interactions. [ABSTRACT FROM AUTHOR]

Ultrafast carrier thermalization in n-type indium nitride (InN) with an electron concentration of 3.8×1018 cm-3 was investigated by femtosecond transient transmission measurements at room temperature with different wavelengths. An extremely fast carrier external thermalization time on the order of 400 fs was observed, which is much faster than all previous reports. This observed femtosecond thermalization time is consistent with a prediction based on a Coulomb screening effect. Through wavelength dependent and power dependent studies, even with a 400 fs thermalization time, we did not observe any evidence of the existence of the hot phonon effect, which agrees with a recent report that a longitudinal optical phonon lifetime could be shorter than 300 fs in specific InN samples. [ABSTRACT FROM AUTHOR]

Picosecond ultrasonic experiments were performed to generate and detect acoustic pulses in piezoelectric (111) epilayers of InxGa(1-x)As, and the longitudinal sound velocities in the [111] direction of InxGa(1-x)As were thus directly determined by controlling the indium content x. We found that the sound velocity exhibits an obvious bowing with different alloy compositions and can be described as a quadratic function of VL(x)=458x2-1451x+5414. This result supports a nonlinear compositional dependence of the elastic constants of InxGa(1-x)As and indicates that the linear-interpolation approximation is inapplicable for estimating sound velocity in this specific case. [ABSTRACT FROM AUTHOR]

Ultrafast carrier thermalization in n-type indium nitride (InN) with an electron concentration is examined by using femtosecond transient transmission measurements at room temperature with different wavelengths. The femtosecond thermalization time is consistent with the prediction based on a Coulomb screening effect, but there is no evidence on the existence of the hot phonon effect.

Summary: Kinetics study on the generation of hydrogen from an Al/water system is performed. The reaction is affected by three major factors such as the concentration of hydroxyl ions (pH values), catalysts, and temperature. However, these factors are interacted and sometimes difficult to separate. This study demonstrates how these factors affect the generation of hydrogen in an Al/water system. Aluminum hydroxide, Al(OH)3 (bayerite phase), synthesized using a chemical solution method, is proved to be a very effective catalyst for the reaction of Al and water. Approximately 95% yield (1300 mL) of hydrogen is produced from 1 g Al in 10 mL water using 3 g Al(OH)3 catalyst at room temperature within 1 minute. The generation rate of hydrogen is accelerated due to the catalyst Al(OH)3 and the exothermic heat. In this report, a ball‐mixing process, the ratio of Al:Al(OH)3:H2O, and the reacting temperatures are investigated to clarify the effect of catalyst Al(OH)3. The synthesized Al(OH)3 catalyst is found to reduce the activation energy of Al/water reaction from 158 kJ/mol to 73.3~76.9 kJ/mol. The roles of hydroxyl ions (ie, pH values), temperature, and catalyst on this phenomenal reaction are explained using a kinetics study and the concept of Fick first law. The 3 factors all improve the flux of hydroxyl ions through the passive Al2O3 layer; therefore, the generation of hydrogen is enhanced. [ABSTRACT FROM AUTHOR]

We demonstrate a beam-scanning nonlinear light endoscope based on a flexible fiber bundle. Excited with a femtosecond Cr:Forsterite laser, the degradation in multiphoton multiharmonic excitation efficiency due to the pulse-broadening effect is significantly reduced without utilizing any external devices. The system resolution has been characterized to be 5.4 μm in the two-photon fluorescence endoscope, limited by the sampling theory. Finally, several image examples have been given. Microsc. Res. Tech., 2008. © 2008 Wiley-Liss, Inc. [ABSTRACT FROM AUTHOR]

We report ultra-broadband ultrasonic spectroscopy with an impedance-matched piezoelectric nanolayer, which enables optical generation and detection of a 730-fs acoustic pulse (the width of ten lattice constants). The bandwidth improvement facilitates THz laser ultrasonics to bridge the spectral gap between inelastic light and x-ray scatterings (0.1-1 THz) in the studies of lattice dynamics. As a demonstration, this method is applied to measure sound attenuation α in a vitreous SiO2 thin film. Our results extend the existing low-frequency data obtained by ultrasonic-based and light scattering methods and also show a α∝ f2 behavior for frequencies f up to 650 GHz. [ABSTRACT FROM AUTHOR]

By using femtosecond laser-ultrasonic, we demonstrate an approach to study the surface plasmon field optically excited in the interface between metal and a semiconductor thin film. By femtosecond impulsive excitation on gallium-nitride (GaN), different optical probe signals were observed when the impulse-excited nanoacoustic pulse propagated through the metal film and metal nanoslits. By analyzing the shape and temporal response of thus induced acousto-optical signals, our femtosecond laser-ultrasonic study not only reveals the plasmonic field distribution optically excited in the metal/substrate interface but also confirms that the penetration depth of surface plasmon field into the substrate agrees well with a simulation result. [ABSTRACT FROM AUTHOR]

The authors demonstrated that the piezoelectric superlattice, can serve as narrow-band detectors for propagating coherent longitudinal acoustic phonons at multiple frequencies corresponding to the spatial frequency of the superlattice and its higher harmonics, and its detection bandwidth is determined by the total structure width. By optically exciting a broadband propagating longitudinal acoustic pulse from a thin Ni film, the authors studied the acoustic spectral sensitivity function of a ten-period In0.12Ga0.88N/GaN multiple quantum well. Because the barriers (19 nm) and wells (3.6 nm) are of different widths, the second detection band, corresponding to the second harmonic of the fundamental frequency, can be resolved. [ABSTRACT FROM AUTHOR]

The authors demonstrate the generation of coherent acoustic phonons in (111)-strained InGaAs/GaAs multiple quantum wells through piezoelectric coupling by an optical pump-probe technique. Dependence of the induced strain amplitude on the photocarrier density reveals that coherent acoustic phonons can be efficiently excited by the piezoelectric effect with an unscreened built-in electric field. Under high fluence excitation, the generation of coherent acoustic phonons saturates. The experimental results are supported by a macroscopic theoretical model. No backward Raman signal and no zone-folded phonon modes were observed in this low impedance-mismatch and finite-period heterostructure. [ABSTRACT FROM AUTHOR]

Carrier thermalization dynamics in heavily doped n-type InN was investigated at room temperature with a femtosecond transient transmission measurement. The dependence of hot carrier cooling time on the total electron density indicates that the plasma screening of electron-LO phonon interactions is responsible for the reduction in energy-loss rate. Under low excitation, the carriers with different excess energies can be found to cool down with a fixed thermalization time of 1.4 ps. Intensity dependent study suggests that this relatively slow carrier cooling time could be attributed to the screening effect by high-background-doping plasma rather than the hot phonon effect. [ABSTRACT FROM AUTHOR]

By coinciding the plasmon frequency with the third-harmonic frequency of the excitation light, the authors determined the plasmon-resonance enhanced optical third-harmonic-generation (THG) susceptibility of a polyvinylpyrrolidone-coated Ag nanoparticle with a 5–7 nm diameter. With dispersed Ag nanoparticles on a quartz surface and through measuring the frequency dependent THG intensities, interface THG showed evident enhancement when the third harmonic of excitation matched the Ag-nanoparticle’s plasmon-resonant frequency. According to the effective medium theory and by analyzing the interface THG under focused Gaussian beams, the ensemble-averaged χ(3)(3ω:ω,ω,ω) of a Ag nanoparticle can be estimated to be on the order of 2×10-11 esu. [ABSTRACT FROM AUTHOR]

The coupling of plasmonic resonances with the multiple phonon modes of a plasmonic supracrystal is studied. Ultrafast optical pump-probe spectroscopy with variable wavelength allows the selective detection of the breathing mode, the interparticle vibrations, and the vibration of the whole structure. Thanks to this selectivity, the characterization of the bonding strength between nanoparticles in different directions of the supracrystal is possible. The observation of these vibrations could be useful for the realization of future phonon modulated photonic and plasmonic devices. [ABSTRACT FROM AUTHOR]

Interface-specific hydrogen (H)-bonding network of water directly controls the energy transfer and chemical reaction pathway at many charged aqueous interfaces, yet to characterize these bonded water layer structures remains a challenge. We now develop a sum-frequency spectroscopic scheme with varying photon momenta as an all-optic solution for retrieving the vibrational spectra of the bonded water layer and the ion diffuse layer and, hence, microscopic structural and charging information about an interface. Application of the method to a model surfactant-water interface reveals a hidden weakly donor H-bonded water species, suggesting an asymmetric hydration-shell structure of fully solvated surfactant headgroups. In another application to a zwitterionic phosphatidylcholine lipid monolayer-water interface, we find a highly polarized bonded water layer structure associating to the phosphatidylcholine headgroup, while the diffuse layer contribution is experimentally proven to be negligible. Our all-optic method offers an in situ microscopic probe of electrochemical and biological interfaces and the route toward future imaging and ultrafast dynamics studies.

Human umbilical cord-derived mesenchymal stem cells (hUC-MSCs) were shown to have potential for immunoregulation and tissue repair. The objective of this study was to investigate the effects of hUC-MSCs on emphysema in chronic obstructive pulmonary disease (COPD). The C57BL/6JNarl mice were exposed to cigarette smoke (CS) for 4 months followed by administration of hUC-MSCs at 3 × 10 6 (low dose), 1 × 10 7 (medium dose), and 3 × 10 7 cells/kg body weight (high dose). The hUC-MSCs caused significant decreases in emphysema severity by measuring the mean linear intercept (MLI) and destructive index (DI). A decrease in neutrophils (%) and an increase in lymphocytes (%) in bronchoalveolar lavage fluid (BALF) were observed in emphysematous mice after hUC-MSC treatment. Lung levels of interleukin (IL)-1β, C-X-C motif chemokine ligand 1 (CXCL1)/keratinocyte chemoattractant (KC), and matrix metalloproteinase (MMP)-12 significantly decreased after hUC-MSC administration. Significant reductions in tumor necrosis factor (TNF)-α, IL-1β, and IL-17A in serum occurred after hUC-MSC administration. Notably, the cell viability of lung fibroblasts improved with hUC-MSCs after being treated with CS extract (CSE). Furthermore, the hUC-MSCs-conditioned medium (hUC-MSCs-CM) restored the contractile force, and increased messenger RNA expressions of elastin and fibronectin by lung fibroblasts. In conclusion, hUC-MSCs reduced inflammatory responses and emphysema severity in CS-induced emphysematous mice., Competing Interests: WL, C-HC, and Y-CW are employed by Meridigen Biotech Co., Ltd. The remaining authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2021 Chen, Chen, Lin, Chen, Wen, Hsiao, Chou, Chung and Chuang.)

We develop a new, to the best of our knowledge, optical scheme based on second-harmonic generation (SHG) at multiple wavelengths for unequivocal separation of the second-order and the electric-field-induced third-order nonlinear optical contributions from aqueous interfaces. The third-order SHG originating from the field-induced reorientation order of water molecules in the electrical double layer offers an optical label-free and inherent probe to the surface charge density and surface potential in the absolute scales. We verify this wavelength-scanning SHG scheme both theoretically and experimentally, and show that the approach is applicable to water interfaces with bulk ionic strength below 500 µM and can achieve a detection sensitivity for a surface charge density of ∼10 -4 C / m 2 .

Protons at the water/vapor interface are relevant for atmospheric and environmental processes, yet characterizing their surface affinity on the quantitative level is still challenging. Here we utilize phase-sensitive sum-frequency vibrational spectroscopy to quantify the surface density of protons (or their hydronium form) at the intrinsic water/vapor interface through inspecting the surface-field-induced alignment of water molecules in the electrical double layer of ions. With hydrogen halides in water, the surface adsorption of protons is found to be independent of specific proton-halide anion interactions and to follow a constant adsorption free energy, Δ G ≈ -3.76 (±0.79) kJ/mol, corresponding to a partitioning coefficient of the surface with respect to bulk water by 3.3∼6.2, for bulk ion concentrations up to 0.3 M. Our spectroscopic study not only is of importance in atmospheric chemistry but also offers a microscopic-level basis to develop advanced quantum-mechanical models for molecular simulations.

Objective: Previous study has demonstrated that EphA2 is a biomarker of mesenchymal stem cells (MSCs) from human placenta or umbilical cord and is able to distinguish MSCs from fibroblasts. In this study, we further examine the potential efficacy of EphA2 + human umbilical cord-derived MSCs (hUC-MSCs)., Materials and Methods: MSCs specific markers, EphA2 and CD146 expression on the surface of hUC-MSCs were determined by flow cytometry analysis. Quantitative real time polymerase chain reaction was used to examine pro-fibrotic gene expression of TGF-β1-stimulated lung fibroblast (MRC-5 cells). On the other hand, ELISA was used to analyze the content of pro-inflammatory cytokines (TNF-ɑ; and IP-10) in the LPS-activated macrophages culture supernatant., Results: The pro-fibrotic gene (TGF-β1, CTGF, fibronectin, collagen I and TIMP-1) expression in TGF-β1-activated MRC-5 cells and the pro-inflammatory cytokines (TNF-ɑ and IP-10) in the LPS-activated macrophages culture supernatant were both attenuated when in present of EphA2 + hUC-MSCs. Moreover, once EphA2 + hUC-MSCs treated with prostaglandin E2 specific inhibitor NS-398, both anti-fibrotic and anti-inflammatory effects of EphA2 + hUC-MSCs were abolished., Conclusion: EphA2 + hUC-MSCs possess immunomodulatory and anti-fibrotic properties, and PGE2 plays an important role in these activities. This implies that EphA2 + hUC-MSCs have potentially effectiveness for treatment of acute inflammatory and chronic fibrotic lung diseases., (Copyright © 2018. Published by Elsevier B.V.)

A sum-frequency spectroscopy scheme is developed that allows the measurement of vibrational spectra of the interfacial molecular structure of charged water interfaces. The application of this scheme to a prototype lipid-aqueous interface as a demonstration reveals an interfacial hydrogen-bonding water layer structure that responds sensitively to the charge state of the lipid headgroup and its interaction with specific ions. This novel technique provides unique opportunities to search for better understanding of electrochemistry and biological aqueous interfaces at a deeper molecular level.

Despite the numerous devoted studies, water at solid interfaces remains puzzling. An ongoing debate concerns the nature of interfacial water at a hydrophilic surface, whether it is more solid-like, ice-like, or liquid-like. To answer this question, a complete picture of the distribution of the water molecule structure and molecular interactions has to be obtained in a non-invasive way and on an ultrafast time scale. We developed a new experimental technique that extends the classical acoustic technique to the molecular level. Using nanoacoustic waves with a femtosecond pulsewidth and an ångström resolution to noninvasively diagnose the hydration structure distribution at ambient solid/water interface, we performed a complete mapping of the viscoelastic properties and of the density in the whole interfacial water region at hydrophilic surfaces. Our results suggest that water in the interfacial region possesses mixed properties and that the different pictures obtained up to now can be unified. Moreover, we discuss the effect of the interfacial water structure on the abnormal thermal transport properties of solid/liquid interfaces.

A phonon nanoscopy method, based on the picosecond ultrasonics technique, capable of studying the complex acoustic reflection coefficient at frequency up to 1 THz is proposed and demonstrated. By measuring the reflection coefficient at the same surface location at the interface between GaN and air, and between GaN and the material to characterize, we get access to the THz amplitude and phase spectra of the acoustic phonon reflection. The retrieval of both these pieces of information then allows the calculation of the attenuation in a wide range of frequency and gives new insight into the Kapitza anomaly. This method is then applied to cubic ice, and the measurements of the elastic properties, the phonon anharmonic decay spectrum up to 1 THz, as well as the measurements of the thermal phonon lifetime at 150 K are all achieved.

We report a direct determination of the specular scattering probability of acoustic phonons at a crystal boundary by observing the escape of incident coherent phonons from the coherent state during reflection. In the sub-THz frequency range where the phonon wavelength is much longer than the lattice constant, the acoustic phonon-interface interaction is found to agree well with the macroscopic theory on wave scattering from rough surfaces. This examination thus quantitatively verifies the dominant role of atomic-scale corrugations in the Kapitza anomaly observed at 1-10 K and further opens a new path to nondestructively estimate subnanoscale roughness of buried interfaces.