Nguyenmcdonald3533

First, we showed that inducing transitions to both the electronic excited state and triplet state can effectively diminish the SRS peaks. Second, we revealed that the epr-SRS signals can be effectively switched off in red-absorbing organic molecules through light-facilitated transitions to a reduced state. Third, we identified that photoswitchable proteins with near-infrared photoswitchable absorbance, whose states are modulable with their electronic resonances detunable toward and away from the pump photon energy, can function as the photoswitchable epr-SRS probes with desirable sensitivity (40 cycles). These photophysical characterizations and proof-of-concept demonstrations should advance the development of novel photoswitchable Raman probes and open up the unexplored Raman imaging capabilities.Using a particle swarm optimization algorithm and finite-difference in time-domain simulations, we optimize the coupling strength between excitons in poly(3-hexylthiophene-2,5-diyl) (P3HT) and surface lattice resonances in open cavities defined by arrays of aluminum nanoparticles. Strong light-matter coupling and the formation of exciton-polaritons are demonstrated. Nanoparticle arrays with optimal dimensions have been fabricated and measured, validating the predictions by the numerical method. P3HT is a regioregular semiconducting polymer used as a donor material in acceptor-donor blends for organic photovoltaic applications. Our results demonstrate the efficacy of the proposed method for the optimization of light-matter coupling and its potential application for the enhanced performance of optoelectronic devices.Because of the sophisticated error cancellation in the density functional theory (DFT)-based calculations, a theoretically more accurate input would not guarantee a better output. In this work, our first-principles GW plus Bethe-Salpeter equation calculations using pseudopotentials show that cuprous halides (CuCl and CuBr) are such extreme cases for which a better one-electron band is not accompanied with a better exciton binding energy. Moreover, we find that the exchange interaction of Cu core electrons plays a crucial role in their ground-state electronic properties, especially in the energy gap and macroscopic dielectric constant. Our work provides new insights into the understanding of the electronic structure of cuprous halides from the DFT perspective.Properties of solid-liquid interfaces and surface charge characteristics mediate ionic and molecular transport through porous systems, affecting many processes such as separations. Herein, we report experiments designed to probe the electrochemical properties of solid-liquid interfaces using a model system of a single polyethylene terephthalate (PET) pore in contact with aqueous and propylene carbonate solutions of LiClO4. First, the existence and polarity of surface charges were inferred from current-voltage curves recorded when a pore was placed in contact with a LiClO4 concentration gradient. Second, the electro-osmotic transport of uncharged polystyrene particles through the PET pore provided information on the polarity and the magnitude of the pore walls' zeta potential. Our experiments show that the PET pores become effectively positively charged when in contact with LiClO4 solutions in propylene carbonate, even though in aqueous LiClO4, the same pores are negatively charged. Additionally, the electro-osmotic velocity of the particles revealed a significantly higher magnitude of the positive zeta potential of the pores in propylene carbonate compared to the magnitude of the negative zeta potential in water. The presented methods of probing the properties of solid-liquid interfaces are expected to be applicable to a wide variety of solid and liquid systems.A scalable, stochastic algorithm evaluating the fourth-order many-body perturbation (MP4) correction to energy is proposed. Three hundred Goldstone diagrams representing the MP4 correction are computer generated and then converted into algebraic formulas expressed in terms of Green's functions in real space and imaginary time. Sunitinib solubility dmso They are evaluated by the direct (i.e., non-Markov, non-Metropolis) Monte Carlo (MC) integration accelerated by the redundant-walker and control-variate algorithms. The resulting MC-MP4 method is efficiently parallelized and is shown to display O(n5.3) size-dependence of cost, which is nearly two ranks lower than the O(n7) dependence of the deterministic MP4 algorithm. It evaluates the MP4/aug-cc-pVDZ energy for benzene, naphthalene, phenanthrene, and corannulene with the statistical uncertainty of 10 mEh (1.1% of the total basis-set correlation energy), 38 mEh (2.6%), 110 mEh (5.5%), and 280 mEh (9.0%), respectively, after about 109 MC steps.Dynamical or spatial properties of charged species can be obtained using electrostatic lenses by velocity map imaging (VMI) or spatial map imaging (SMI), respectively. Here, we report an approach for extracting dynamical and spatial information from patterns in SMI images that map the initial coordinates, velocity vectors, and angular distributions of charged particles onto the detector, using the same apparatus as in VMI. Deciphering these patterns required analysis and modeling, involving both their predictions from convolved spatial and velocity distributions and fitting observed images to kinetic energies (KEs) and anisotropy parameters (βs). As the first demonstration of this capability of SMI, the ensuing photoelectrons resulting from (2 + 1) resonant ionization of water in a selected rotational state were chosen to provide a rigorous basis for comparison to VMI. Operation with low acceleration voltages led to a measured SMI pattern with a unique vertical intensity profile that could be least-squares fitted to yield KE and β, in good agreement with VMI measurement. Due to the potential for improved resolution and the extended KE range achievable by this new technique, we expect that it might augment VMI in applications that require the analysis of charged particles and particularly in processes with high KE release.Elemental copper and potassium are immiscible under ambient conditions. It is known that pressure is a useful tool to promote the reaction between two different elements by modifying their electronic structure significantly. Here, we predict the formation of four K-Cu compounds (K3Cu2, K2Cu, K5Cu2, and K3Cu) under moderate pressure through unbiased structure search and first-principles calculations. Among all predicted structures, the simulated x-ray diffraction pattern of K3Cu2 perfectly matches a K-Cu compound synthesized in 2004. Further simulations indicate that the K-Cu compounds exhibit diverse structural features with novel forms of Cu aggregations, including Cu dimers, linear and zigzag Cu chains, and Cu-centered polyhedrons. Analysis of the electronic structure reveals that Cu atoms behave as anions to accept electrons from K atoms through fully filling 4s orbitals and partially extending 4p orbitals. Covalent Cu-Cu interaction is found in these compounds, which is associated with the sp hybridizations.