Impact of a charged neighboring particle on Förster resonance energy transfer (FRET)

Förster resonance energy transfer (FRET) is an important physical phenomenon which demands precise control over the FRET rate for its wide range of applications. Hence, enhancing the FRET rate using different techniques has been extensively studied in the literature. Research indicates that introducing additional particles to a system consisting of a donor-acceptor pair can change the behaviour of FRET in the system. One such technique is to utilize the collective oscillations of the surface electrons of a neighboring electrically-neutral metal nanoparticle (MNP). However, the perceived changes on the FRET rate between the donor and the acceptor, when the MNP carries excess electrical charges are yet unknown. In this paper, we study these changes by introducing a charged MNP, in the proximity of an excited donor and a ground state acceptor. We deploy the classical Green's tensor to express the FRET rate in the system. We consider an effective dielectric response for the MNP, which accounts for the extraneous surface charge effects. We analyze the electrical potential at the acceptor position due to the changed dipole moment of the donor molecule as a result of the electric field induced at the donor position, and obtain the FRET rate of the system. This model considers arbitrary locations and orientations of the two molecular dipole moments with regard to the position of the spherical MNP. We present the enhancement of the FRET rate, predominantly caused by both the surface plasmon excitations and the extraneous surface electrical charges carried by the neighboring MNP. We obtain the results by varying the separation distance between the molecules and the MNP, the transition frequency of the donor-acceptor pair and the size of the metallic sphere. Specifically, we demonstrate that a donor-acceptor pair placed in the vicinity of an electrically-charged Silver MNP exhibits a remarkable improvement in the FRET rate. Furthermore, the aggregate FRET enhancement is determined by other characteristics such as the location of the donor, transition frequency, separation distances and the radius of the MNP. In essence, these findings reveal an approach to realize the enhanced FRET rate in a larger span in a more controlled manner that is desirable in many FRET-based applications including spectroscopic measurements

Designer Gene Delivery Vectors: Molecular Engineering and Evolution of Adeno-Associated Viral Vectors for Enhanced Gene Transfer

Gene delivery vectors based on adeno-associated virus (AAV) are highly promising due to several desirable features of this parent virus, including a lack of pathogenicity, efficient infection of dividing and non-dividing cells, and sustained maintenance of the viral genome. However, several problems should be addressed to enhance the utility of AAV vectors, particularly those based on AAV2, the best characterized AAV serotype. First, altering viral tropism would be advantageous for broadening its utility in various tissue or cell types. In response to this need, vector pseudotyping, mosaic capsids, and targeting ligand insertion into the capsid have shown promise for altering AAV specificity. In addition, library selection and directed evolution have recently emerged as promising approaches to modulate AAV tropism despite limited knowledge of viral structure–function relationships. Second, pre-existing immunity to AAV must be addressed for successful clinical application of AAV vectors. “Shielding” polymers, site-directed mutagenesis, and alternative AAV serotypes have shown success in avoiding immune neutralization. Furthermore, directed evolution of the AAV capsid is a high throughput approach that has yielded vectors with substantial resistance to neutralizing antibodies. Molecular engineering and directed evolution of AAV vectors therefore offer promise for generating ‘designer’ gene delivery vectors with enhanced properties

Mouse Chromosome 11

Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/46996/1/335_2004_Article_BF00648429.pd

Selective hydrogen production at Pt(111) investigated by Quantum Monte Carlo methods for metal catalysis

This rapid communication gives the salient points and results of the theoretical investigation of a chemical reaction for efficient selective hydrogen production. The clean fuel produced is a sustainable energy source. Accurate methods based on quantum theory are used because the changing electronic structure is a probe that monitors reactions. The reaction between water and carbon monoxide is used industrially with metal catalysts, usually platinum. There is a considerable economic and environmental challenge underpinning this fundamental investigation where bond dissociation plays an essential role. A bond dissociation process is often the limiting step of reaction rates for industrial catalysis. Most mainstream quantum approaches fail to a greater or lesser degree in the description of this process. The present work advocates a promising alternative: the initial analysis of statistical data generated by the Quantum Monte Carlo (QMC) method demonstrated very stringent statistical accuracy for essential information on hydrogen production via the water-gas shift reaction with platinum catalyst. The transition state structure is obtained from QMC force constants and illustrated here. It corresponds to water OH-stretch concerted with Pt-H bond formation, whilst the OH oxygen atom begins to interact with the CO carbon. The present QMC evaluation of the corresponding activation barrier is low: 17.0 ± 0.2 kcal/mol. It is close to the experimental apparent activation energy of 17.05 kcal/mol. This method is applicable to a wide range of similar systems.acceptedVersionPeer reviewe

Quantum Monte Carlo Approach for Determining the Activation Barrier of Water Addition to Carbon Monoxide Adsorbed on Pt(111) within 1 kJ/mol

Quantum Monte Carlo (QMC) methods offer ab initio calculations of remarkable accuracy for reaction activation barriers (to 1 kJ/mol or 0.01 eV), even at solid surfaces. Chemical reactions generally involve bond dissociation that is poorly described by Hartree-Fock and density functional theory (DFT) methods. However, such processes are often the key to rate-limiting reaction steps at solid surfaces. In this work, a novel QMC methodology is demonstrated as a solution. Carbon monoxide (CO) on platinum reacts with water, first giving the addition products. QMC methods are used here to investigate addition at close-packed Pt(111). The CO is preadsorbed on Pt(111). First, an approaching water molecule is only partially dissociated. At the same time, its oxygen atom binds to CO giving an adsorbed formate moiety (COOH) and Pt-H. This concerted addition is rate-limiting. The QMC activation barrier (in kJ/mol) is 71.0 ± 0.7, and its apparent measured value is 71.4. This showcases QMC as a method to investigate related catalytic systems.acceptedVersionPeer reviewe

Biodegradation of the herbicide mesotrione in soil from batch to microcosm experiments

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