On the interactions between molecules in an off-resonant laser beam:Evaluating the response to energy migration and optically induced pair forces

Electronically excited molecules interact with their neighbors differently from their ground-state counterparts. Any migration of the excitation between molecules can modify intermolecular forces, reflecting changes to a local potential energy landscape. It emerges that throughput off-resonant radiation can also produce significant additional effects. The context for the present analysis of the mechanisms is a range of chemical and physical processes that fundamentally depend on intermolecular interactions resulting from second and fourth-order electric-dipole couplings. The most familiar are static dipole-dipole interactions, resonance energy transfer (both second-order interactions), and dispersion forces (fourth order). For neighboring molecules subjected to off-resonant light, additional forms of intermolecular interaction arise in the fourth order, including radiation-induced energy transfer and optical binding. Here, in a quantum electrodynamical formulation, these phenomena are cast in a unified description that establishes their inter-relationship and connectivity at a fundamental level. Theory is then developed for systems in which the interplay of these forms of interaction can be readily identified and analyzed in terms of dynamical behavior. The results are potentially significant in Förster measurements of conformational change and in the operation of microelectromechanical and nanoelectromechanical devices. © 2009 American Institute of Physics

A molecular theory for two-photon and three-photon fluorescence polarization

In the analysis of molecular structure and local order in heterogeneous samples, multiphoton excitation of fluorescence affords chemically specific information and high-resolution imaging. This report presents the results of an investigation that secures a detailed theoretical representation of the fluorescence polarization produced by one-, two-, and three-photon excitations, with orientational averaging procedures being deployed to deliver the fully disordered limits. The equations determining multiphoton fluorescence response prove to be expressible in a relatively simple, generic form, and graphs exhibit the functional form of the multiphoton fluorescence polarization. Amongst other features, the results lead to the identification of a condition under which the fluorescence produced through the concerted absorption of any number of photons becomes completely unpolarized. It is also shown that the angular variation of fluorescence intensities is reliable indicator of orientational disorder

Quantum Monte Carlo calculations of H2_2 dissociation on Si(001)

We present quantum Monte Carlo calculations for various reaction pathways of H$_2$ with Si(001), using large model clusters of the surface. We obtain reaction energies and energy barriers noticeably higher than those from approximate exchange-correlation functionals. In improvement over previous studies, our adsorption barriers closely agree with experimental data. For desorption, the calculations give barriers for conventional pathways in excess of the presently accepted experimental value, and pinpoint the role of coverage effects and desorption from steps.Comment: 4 pages, 1 figur

Using Intervention Mapping to Develop an Efficacious Multicomponent Systems-Based Intervention to Increase Human Papillomavirus (HPV) Vaccination in a Large Urban Pediatric Clinic Network

Background: The CDC recommends HPV vaccine for all adolescents to prevent cervical, anal, oropharyngeal, vaginal, vulvar, and penile cancers, and genital warts. HPV vaccine rates currently fall short of national vaccination goals. Despite evidence-based strategies with demonstrated efficacy to increase HPV vaccination rates, adoption and implementation of these strategies within clinics is lacking. The Adolescent Vaccination Program (AVP) is a multicomponent systems-based intervention designed to implement five evidence-based strategies within primary care pediatric practices. The AVP has demonstrated efficacy in increasing HPV vaccine initiation and completion among adolescents 10-17 years of age. The purpose of this paper is to describe the application of Intervention Mapping (IM) toward the development, implementation, and formative evaluation of the clinic-based AVP prototype. Methods: Intervention Mapping (IM) guided the development of the Adolescent Vaccination Program (AVP). Deliverables comprised: a logic model of the problem (IM Step 1); matrices of behavior change objectives (IM Step 2); a program planning document comprising scope, sequence, theory-based methods, and practical strategies (IM Step 3); functional AVP component prototypes (IM Step 4); and plans for implementation (IM Step 5) and evaluation (IM Step 6). Results: The AVP consists of six evidence-based strategies implemented in a successful sequenced roll-out that (1) established immunization champions in each clinic, (2) disseminated provider assessment and feedback reports with data-informed vaccination goals, (3) provided continued medical and nursing education (with ethics credit) on HPV, HPV vaccination, message bundling, and responding to parent hesitancy, (4) electronic health record cues to providers on patient eligibility, and (5) patient reminders for HPV vaccine initiation and completion. Conclusions: IM provided a logical and systematic approach to developing and evaluating a multicomponent systems-based intervention to increase HPV vaccination rates among adolescents in pediatric clinics

A photonic basis for deriving nonlinear optical response

Nonlinear optics is generally first presented as an extension of conventional optics. Typically the subject is introduced with reference to a classical oscillatory electric polarization, accommodating correction terms that become significant at high intensities. The material parameters that quantify the extent of the nonlinear response are cast as coefficients in a power series - nonlinear optical susceptibilities signifying a propensity to generate optical harmonics, for example. Taking the subject to a deeper level requires a more detailed knowledge of the structure and properties of each nonlinear susceptibility tensor, the latter differing in form according to the process under investigation. Typically, the derivations involve intricate development based on time-dependent perturbation theory, assisted by recourse to a set of Feynman diagrams. This paper presents a more direct route to the required results, based on photonic rather than semiclassical principles, and offers a significantly clearer perspective on the photophysics underlying nonlinear optical response. The method, here illustrated by specific application to harmonic generation and down-conversion processes, is simple, intuitive and readily amenable for processes of arbitrary photonic order. © 2009 IOP Publishing Ltd

Associations of sitting accumulation patterns with cardio-metabolic risk biomarkers in Australian adults

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