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Background Perturbation of gut microbiota has been linked to chronic kidney disease (CKD), which was correlated with a sophisticated milieu of metabolic and immune dysregulation. Methods To clarify the underlying host–microbe interaction in CKD, we performed multi-omics measurements, including systems-level gut microbiome, targeted serum metabolome and deep immunotyping, in a cohort of patients and non-CKD controls. Results Our analyses on functional profiles of the gut microbiome showed a decrease in the diversity and abundance of carbohydrate-active enzyme (CAZyme) genes but an increase in the abundance of antibiotic resistance, nitrogen cycling enzyme and virulence factor genes in CKD. Moreover, models generated using measurements of serum metabolites (amino acids, bile acids and short-chain fatty acids) or immunotypes were predictive of renal impairment but less so than many of the functional profiles derived from gut microbiota, with the CAZyme genes being the top-performing model to accurately predict the early stage of diseases. In addition, co-occurrence analyses revealed coordinated host–microbe relationships in CKD. Specifically, the highest fractions of significant correlations were identified with circulating metabolites by several taxonomic and functional profiles of gut microbiome, while immunotype features were moderately associated with the abundance of microbiome-encoded metabolic pathways and serum levels of amino acids (e.g. B cell cluster tryptophan and B cell cluster tryptophan metabolism). Conclusion Overall, our multi-omics integration revealed several signatures of systems-level gut microbiome in robust associations with host–microbe co-metabolites and renal function, which may have aetiological and diagnostic implications in CKD. [ABSTRACT FROM AUTHOR]

We present experimental and theoretical evidence demonstrating the Mie resonance effect in the terahertz (THz) range, utilizing Fe3O4/Kerosene ferrofluid. Our findings indicate a significant and rapid change in the complex refractive indices at 0.5 THz with an increase in the magnetic field strength. Moreover, we observed a prominent absorption peak at 0.5 THz in transmittance and absorption coefficient measurements, corresponding to a magnetic field intensity of 178.0 mT. This phenomenon occurs due to the adjustment of particle spacing, leading to resonance under different magnetic field conditions. These research results hold immense potential in advancing the development of magneto-optical THz modulators for imaging and communication applications. [ABSTRACT FROM AUTHOR]

A recent experiment on the 267 nm photolysis of gaseous acetaldehyde reveals that the molecular products (CO + CH4) present product state distributions with computation –experiment discrepancy. This work aims to provide solution to such issue. The direct dynamics simulation of classical trajectories and the generalized multi‐center impulsive model (GMCIM) are both utilized to predict the product state distributions of CO and CH4 from 267 nm photolysis of acetaldehyde. Comparison with the experimental observation provides an assessment of the conventional approach of minimum energy path within the framework of three‐center transition state (TS) and CH3‐roaming pathways. The result shows that the high‐speed products observed in experiment are likely formed via the three‐center TS pathway. The reasons that lead to the discrepancy between computation and experiments in previous studies are also investigated. A better agreement between computational and state‐resolved experimental results can be achieved by selecting specific internal states of CO product from the computational data. [ABSTRACT FROM AUTHOR]

This work aims to introduce a generalized impulsive model for unimolecular dissociation processes. This model allows us to take into account the curvature of the reaction path explicitly. It is a generalization of the previously developed multi-center impulsive model [P.-Y. Tsai and K.-C. Lin, J. Phys. Chem. A 119, 29 (2015)]. Several limitations of conventional impulsive models are eliminated by this study: (1) Unlike conventional impulsive models, in which a single molecular geometry is responsible for the impulse determination, the gradients on the whole dissociation path are taken into account. The model can treat dissociation pathways with large curvatures and loose saddle points. (2) The method can describe the vibrational excitation of polyatomic fragments due to the bond formation by multi-center impulse. (3) The available energy in conventional impulsive models is separated into uncoupled statistical and impulsive energy reservoirs, while the interplay between these reservoirs is allowed in the new model. (4) The quantum state correlation between fragments can be preserved in analysis. Dissociations of several molecular systems including the roaming pathways of formaldehyde, nitrate radical, acetaldehyde, and glyoxal are chosen as benchmarks. The predicted photofragment energy and vector distributions are consistent with the experimental results reported previously. In these examples, the capability of the new model to treat the curved dissociation path, loose saddle points, polyatomic fragments, and multiple-body dissociation is verified. As a cheaper computational tool with respect to ab initio on-the-fly direct dynamic simulations, this model can provide detailed information on the energy disposal, quantum state correlation, and stereodynamics in unimolecular dissociation processes. [ABSTRACT FROM AUTHOR]

The dissociation dynamics of CO-forming channel on the ground state (S0) of methyl formate has been studied by direct dynamics simulations and Generalised Multi-Centre Impulsive Model (GMCIM) under photon energy of 193 nm. Comparison of the simulated product-state distribution with experimental results permits us to conclude that the major forming channel of primary CO is through the conventional three-centre saddle point (TS1), which leads to CO (X1∑+) + CH3OH ( X ~ 1 A ′ ) products. Besides, the photolysis wavelength dependence of product state distribution via TS1 is successfully interpreted by GMCIM, whereas the excess energy above the barrier top is treated by sudden approximation. In addition, the possibility to produce secondary CO is also considered. With the aid of phase-space theory simulation, it turns out that the most probable route to form secondary CO is via the sequential triple fragmentation due to the further decomposition of energetic HCO( X ~ 2 A ′ ), which takes place on the S0 surface of methyl formate. [ABSTRACT FROM AUTHOR]

The primary elimination channel of bromine molecule in one-photon dissociation of CH2BrC(O)Br at 248 nm is investigated using cavity ring-down absorption spectroscopy. By means of spectral simulation, the ratio of nascent vibrational population in v = 0, 1, and 2 levels is evaluated to be 1:(0.5 ± 0.1):(0.2 ± 0.1), corresponding to a Boltzmann vibrational temperature of 581 ± 45 K. The quantum yield of the ground state Br2 elimination reaction is determined to be 0.24 ± 0.08. With the aid of ab initio potential energy calculations, the obtained Br2 fragments are anticipated to dissociate on the electronic ground state, yielding vibrationally hot Br2 products. The temperature-dependence measurements support the proposed pathway via internal conversion. For comparison, the Br2 yields are obtained analogously from CH3CHBrC(O)Br and (CH3)2CBrC(O)Br to be 0.03 and 0.06, respectively. The trend of Br2 yields among the three compounds is consistent with the branching ratio evaluation by Rice-Ramsperger-Kassel-Marcus method. However, the latter result for each molecule is smaller by an order of magnitude than the yield findings. A non-statistical pathway so-called roaming process might be an alternative to the Br2 production, and its contribution might account for the underestimate of the branching ratio calculations. [ABSTRACT FROM AUTHOR]

By using time-resolved Fourier-transform infrared emission spectroscopy, the fragments of HCN(v = 1, 2) and CO(v = 1-3) are detected in one-photon dissociation of acetyl cyanide (CH3COCN) at 308 nm. The S1(A″), 1(nO, π*CO) state at 308 nm has a radiative lifetime of 0.46 ± 0.01 μs, long enough to allow for Ar collisions that induce internal conversion and enhance the fragment yields. The rate constant of Ar collision-induced internal conversion is estimated to be (1-7) × 10-12 cm3 molecule-1 s-1. The measurements of O2 dependence exclude the production possibility of these fragments via intersystem crossing. The high-resolution spectra of HCN and CO are analyzed to determine the ro-vibrational energy deposition of 81 ± 7 and 32 ± 3 kJ/mol, respectively. With the aid of ab initio calculations, a two-body dissociation on the energetic ground state is favored leading to HCN + CH2CO, in which the CH2CO moiety may further undergo secondary dissociation to release CO. The production of CO2 in the reaction with O2 confirms existence of CH2 and a secondary reaction product of CO. The HNC fragment is identified but cannot be assigned, as restricted to a poor signal-to-noise ratio. Because of insufficient excitation energy at 308 nm, the CN and CH3 fragments that dominate the dissociation products at 193 nm are not detected. [ABSTRACT FROM AUTHOR]

A primary dissociation channel of Br2 elimination is detected following a single-photon absorption of (COBr)2 at 248 nm by using cavity ring-down absorption spectroscopy. The technique contains two laser beams propagating in a perpendicular configuration. The tunable laser beam along the axis of the ring-down cell probes the Br2 fragment in the B3Πou+-X1Σg+ transition. The measurements of laser energy- and pressure-dependence and addition of a Br scavenger are further carried out to rule out the probability of Br2 contribution from a secondary reaction. By means of spectral simulation, the ratio of nascent vibrational population for v = 0, 1, and 2 levels is evaluated to be 1:(0.65 ± 0.09):(0.34 ± 0.07), corresponding to a Boltzmann vibrational temperature of 893 ± 31 K. The quantum yield of the ground state Br2 elimination reaction is determined to be 0.11 ± 0.06. With the aid of ab initio potential energy calculations, the pathway of molecular elimination is proposed on the energetic ground state (COBr)2 via internal conversion. A four-center dissociation mechanism is followed synchronously or sequentially yielding three fragments of Br2 + 2CO. The resulting Br2 is anticipated to be vibrationally hot. The measurement of a positive temperature effect supports the proposed mechanism. [ABSTRACT FROM AUTHOR]

Following single-photon dissociation of CH2I2 at 248 nm, I2 molecular elimination is detected by using cavity ring-down absorption spectroscopy. The technique comprises two laser beams propagating in a perpendicular configuration, in which a tunable laser beam along the axis of the ring-down cell probes the I2 fragment in the B 3Πou+ - X 1Σg+ transition. The nascent vibrational populations for v = 0, 1, and 2 levels are obtained with a population ratio of 1:(0.65 ± 0.10):(0.30 ± 0.05), corresponding to a Boltzmann-like vibrational temperature of 544 ± 73 K. The quantum yield of the ground state I2 elimination reaction is determined to be 0.0040 ± 0.0025. With the aid of ab initio potential energy calculations, the pathway of molecular elimination is proposed on the energetic ground state CH2I2 via internal conversion, followed by asynchronous three-center dissociation. A positive temperature effect supports the proposed mechanism. [ABSTRACT FROM AUTHOR]

Quasi-classical trajectory (QCT) calculations are performed on the molecular products CO + CH4via the tight transition state (TS) and global minimum configurations. With the aid of this theoretical evidence, we have re-examined the experimental results published previously to clarify the controversial issue of photodissociation dynamics of CH3CHO at 248 nm. For the CO (v = 0 and 1) bimodal rotational distributions obtained previously [K.-C. Hung, P.-Y. Tsai, H.-K. Li, and K.-C. Lin, J. Chem. Phys., 2014, 140, 064313], the low-rotational (J) component is re-assigned to the contribution of triple fragmentation (H + CO + CH3), whereas the high-J component is ascribed to the CH3-roaming pathway. The H-roaming pathway is not found in the calculations. Further, the QCT results have confirmed that the CO vibrational population especially at higher states and the low-energy component of CH4 vibrational bimodality obtained experimentally are mainly produced following the TS pathway, which has never been identified before. While taking into account both the theoretical and experimental results, the ratio of the molecular products (CO(v = 1) + CH4) obtained by the triple fragmentation/roaming/TS processes is evaluated to be 0.23 : 1 : 0.29. [ABSTRACT FROM AUTHOR]