Dolgounitcheva, O.; Zakrzewski, V. G.; Streit, L.; Ortiz, J. V.
Ab initio electron propagator calculations in the partial third order (P3) and P3+ approximations were performed to obtain vertical electron detachment energies (VEDEs) of fluoride and chloride clusters with one through three molecules of water. Larger clusters of F- and Cl- with six water molecules were also treated with and without the polarisable continuum model (PCM). For the smaller clusters, good agreement between calculated VEDEs and peak positions in photoelectron spectra is achieved. Large shifts in VEDEs are observed for both hexameric fluoride-water and chloride-water complexes when the PCM is applied. Significant changes in coordination geometries about the chloride anion also occur in this model. In all fluoride complexes, Dyson orbitals for the lowest VEDEs are delocalised over oxygen atoms. On the contrary, for the case of chloride-water clusters, the Dyson orbitals corresponding to the lowest VEDEs are localised on the anion.
Moses, Gregory; Chenhall, Jeffrey; Cao, Duc; Delettrez, Jacques
Four electron thermal transport models are compared for their ability to accurately and efficiently model non-local behavior in ICF simulations. Goncharov's transport model has accurately predicted shock timing in implosion simulations but is computationally slow and limited to 1D. The iSNB (implicit Schurtz Nicolai Busquet electron thermal transport method of Cao et al. uses multigroup diffusion to speed up the calculation. Chenhall has expanded upon the iSNB diffusion model to a higher order simplified P3 approximation and a Monte Carlo transport model, to bridge the gap between the iSNB and Goncharov models while maintaining computational efficiency. Comparisons of the above models for several test problems will be presented. This work was supported by Sandia National Laboratory - Albuquerque and the University of Rochester Laboratory for Laser Energetics.
Vukanic, J.; Davidovic, D. M.
Reflection of electrons from solids is treated by the approximate analytic solution of the linearized transport equation. Scattering of electrons on target atoms is determined by the screened Coulomb interaction and the energy loss due to interaction with target electrons is defined by Bethe- Bloch formula. The anisotropic P_3 approximation of the collision integral is utilized and the Bolzmann transport equation is Laplace transformed in relative path length and solved by applying the DP0 technique. The approach is applicable in a wide range of electron energy --from several tens of keV to several MeV- and for materials where the mean number of collisions of an electron with target atoms during slowing down is large. Analytic expressions for energy distribution of backscattered electrons as well as for the particle and energy reflection coefficients were derived. Comparison of our results with data of the computational bipartition model is presented.
Chin, Lee C L; Worthington, Arthur E; Whelan, William M; Vitkin, I Alex
Interstitial quantification of the optical properties of tissue is important in biomedicine for both treatment planning of minimally invasive laser therapies and optical spectroscopic characterization of tissues, for example, prostate cancer. In a previous study, we analyzed a method first demonstrated by Dickey et al., [Phys. Med. Biol. 46, 2359 (2001)] to utilize relative interstitial steady-state radiance measurements for recovering the optical properties of turbid media. The uniqueness of point radiance measurements were demonstrated in a forward sense, and strategies were suggested for improving performance under noisy experimental conditions. In this work, we test our previous conclusions by fitting the P3 approximation for radiance to Monte Carlo predictions and experimental data in tissue-simulating phantoms. Fits are performed at: 1. a single sensor position (0.5 or 1 cm), 2. two sensor positions (0.5 and 1 cm), and 3. a single sensor position (0.5 or 1 cm) with input knowledge of the sample's effective attenuation coefficient. The results demonstrate that single sensor radiance measurements can be used to retrieve optical properties to within approximately 20%, provided the transport albedo is greater than approximately 0.9. Furthermore, compared to the single sensor fits, employing radiance data at two sensor positions did not significantly improve the accuracy of recovered optical properties. However, with knowledge of the effective attenuation coefficient of the medium, optical properties can be retrieved experimentally to within approximately 10% for an albedo greater or equal to 0.5. PMID:18163843
Faris, Gregory W
Presented here are expressions for the P(N) approximation for light propagation in scattering media in the frequency domain. To elucidate parametric dependencies, the derivation uses normalization of the resulting expressions to either the total interaction coefficient or the reduced total interaction coefficient. For the latter case, a set of reduced phase function coefficients are introduced. Expression of the P(N) approximation as a conventional eigenvalue problem facilitates computation of the eigenvalues or attenuation coefficients. This approach is used to determine the attenuation coefficients in the asymptotic regime over the full values of the scattering albedo and reduced scattering albedo (0 to 1) and all positive values of the asymmetry factor (0 to 1). Frequency-domain measurements yield a sensitivity to turbid media optical properties for reduced scattering albedos as small as 0.2. P(N) calculations are used to assess the magnitude of errors associated with the P1 and P3 approximations over a range of scattering albedo, phase function, and modulation frequency. PMID:15835355
Joint derivation method for determining optical properties based on steady-state spatially resolved diffuse reflectance measurement at small source-detector separations and large reduced albedo range: theory and simulation.
Shi, Zhenzhi; Fan, Ying; Zhao, Huijuan; Xu, Kexin
Accurate determination of the optical properties (the absorption coefficient μ(a) and the reduced scattering coefficient μ(s) (')) of tissues is very important in a variety of diagnostic and therapeutic procedures. Optical diffusion theory is frequently used as the forward model for describing the photon transfer in media with large reduced albedos (a(')) and in large source-detector separations (SDS). Several other methods (PN approximation, hybrid diffusion-P3 approximation) have also been published that describe photon transfer in media with low a(') or small SDSs. We studied the theoretical models for the steady-state spatially resolved diffuse reflectance measurement to accurately determine μ(a) and μ(s) (') at large a(') range but small SDSs. Instead of using a single model, a joint derivation method is proposed. The developed method uses one of the best aforementioned theoretical methods separately in five ranges of a(') determined from several forward models. In the region of small SDSs (the range between 0.4 and 8 mm) and large a(') range (between 0.5 and 0.99), the best theoretical derivation model was determined. The results indicate that the joint derivation method can improve the derivation accuracy and that a(') range can be determined by the steady-state spatially resolved diffuse reflectance measurement. PMID:22734782
Übeyli, Mustafa; Yapıcı, Hüseyin
ARIES-RS is one of the major magnetic fusion energy reactor designs that uses a blanket having vanadium alloy structure cooled by lithium [1, 2]. It is a deuterium-tritium (DT) fusion driven reactor, having a fusion power of 2170 MW [1, 2]. This study presents the neutronic analysis of the ARIES-RS fusion reactor using heavy metal molten salts in which Li2BeF4 as the main constituent was mixed with increased mole fractions of heavy metal salt (ThF4 or UF4) starting by 2 mol.% up to 12 mol.%. Neutron transport calculations were carried out with the help of the SCALE 4.3 system by solving the Boltzmann transport equation with the XSDRNPM code in 238 neutron groups and a S 8- P 3 approximation. According to the numerical results, tritium self-sufficiency was attained for the coolants, Flibe with 2% UF4 or ThF4 and 4% UF4. In addition, higher energy multiplication values were found for the salt with UF4 compared to that with ThF4. Furthermore, significant amount of high quality nuclear fuel was produced to be used in external reactors.
Kulkarni, M.R.; Peck, R.E.
A theoretical study of the heating effectiveness of a composite porous radiant burner (PRB) is conducted. A one-dimensional laminar premixed flame model incorporating a radiatively participating inert porous medium consisting of two layers of different properties is used to describe the heat release/transfer processes. Combined conductive, convective, and radiative heat transfer is considered. The spherical harmonics method with the P-3 approximation is used to model the radiation part. A multistep reaction mechanism for premixed methane-air combustion is employed. A parametric study is carried out to determine the effect of the radiative properties of the two porous layers on burner performance. Calculations indicate that a significant improvement in the radiative output of a PRB can be attained by optimizing the burner properties upstream and downstream of the flame. Generally, the upstream layer should be of lower porosity, shorter length, and higher optical thickness than the downstream layer. Also, the upstream layer should be highly scattering, while the downstream layer should be nonscattering.
Blagoĭ, Iu P; Kornilova, S V; Leont'ev, V S; Sorokin, V A; Gladchenko, G O; Valeev, V A; Grigor'ev, D N; Kapinos, L E; Bondarenko, V N; Kolod, V Ia
The properties of animal DNAs exposed to prolonged irradiation in the Chernobyl zone, have been studied by the methods of viscometry, thermal denaturation, IR-spectroscopy, and electrophoresis. High content of low-molecular fractions have been observed in the preparations of DNA from liver and spleen, their quantities increasing with age and generation of animals. This effect is especially strong in DNA from liver. Low-molecular fraction of DNA is shown to be enriched with G-C pairs and to consist of the following four fractions: 1) approximately 500 base pairs (B.p.), 2) approximately 1.5 divided by 2 thousand B.p., 3) approximately 4 divided by 5 thousand B.p. and 4) a mixture of approximately 20 thousand B.p. fragments. Further, it has been observed that the DNA preparations from the tissues of experimental animals contain about ten times higher contents of Fe, Zn, Se and other elements as compared to the control preparations. PMID:7981273
Finlay, Jarod C.; Zhu, Timothy C.; Dimofte, Andreea; Friedberg, Joseph S.; Cengel, Keith A.; Hahn, Stephen M.
We present the results of a series of spectroscopic measurements made in vivo in patients undergoing photodynamic therapy (PDT). The patients studied here were enrolled in Phase II clinical trials of Photofrin-mediated PDT for the treatment of non-small cell lung cancer and cancers with pleural effusion. Patients were given Photofrin at dose of 2 mg per kg body weight 24 hours prior to treatment. Each patient received surgical debulking of the tumor followed by intracavity PDT at 630nm to a dose of 60 J/cm2. Dose was monitored continuously using implanted isotropic fiber-based light detectors. We measured the diffuse reflectance spectra before and after PDT in various positions within the cavity, including tumor, diaphragm, pericardium, skin, and chest wall muscle in 10 patients. The measurements were acquired using a specially designed fiber optic-based probe consisting of one fluorescence excitation fiber, one white light delivery fiber, and 9 detection fibers spaced at distances from 0.36 to 7.8 mm from the source, all of which are imaged via a spectrograph onto a CCD, allowing measurement of radially-resolved diffuse reflectance and fluorescence spectra. The absorption spectra were analyzed using an analytical model of light propagation in diffuse media based on the P3 approximation to radiative transport, assuming a known basis set of absorbers including hemoglobin in its oxygenated and deoxygenated forms and Photofrin. We find significant variation in hemodynamics and sensitizer concentration among patients and within tissues in a single patient.
Chin, Lee C. L.; Lloyd, Brendan; Whelan, William M.; Vitkin, I. Alex
We present an optical technique, point radiance spectroscopy, to directly recover chromophore concentrations and the reduced optical scattering coefficient spectrum from continuous wave interstitial point radiance measurements at a single-source-detector separation in turbid, tissuelike media. The method employs a spectral algorithm to fit the relative radiance data, using the P3 approximation, at only two detection angles (0° and 90°). The spectral fitting algorithm is applied to simulated data of relative point fluence and relative point radiance data with added 1% noise and shows that even under realistic experimental conditions, only point radiance information is able to provide quantitative information regarding chromophore concentrations and scattering power at distances greater than two to three mean free paths from the source. Furthermore, experimental measurements in tissue-simulating phantoms demonstrate that dye concentrations and scattering parameters can be recovered to within ˜10%. The developed point radiance technique bridges a technological gap between local surface reflectance and spatially resolved interstitial fluence methods in optical assessment of random media such as biological tissue.
In this study, a neutronic performance of the Laser Inertial Confinement Fusion Fission Energy (LIFE) molten salt blanket is investigated. Neutronic calculations are performed by using XSDRNPM/SCALE5 codes in S8-P3 approximation. The thorium molten salt composition considered in this calculation is 75 % LiF—25 % ThF4, 75 % LiF—24 % ThF4—1 % 233UF4, 75 % LiF—23 % ThF4—2 % 233UF4. Also, effects of the 6Li enrichment in molten salt are performed for all heavy metal salt. The radiation damage behaviors of SS-304 structural material with respect to higher fissionable fuel content and 6Li enrichment are computed. By higher fissionable fuel content in molten salt and with 6Li enrichment (20 and 50 %) in the coolant in form of 75 % LiF—23 % ThF4—2 % 233UF4, an initial TBR >1.05 can be realized. On the other hand, the 75 % LiF—25 % ThF4 or 75 % LiF—24 % ThF4—1 % 233UF4 molten salt fuel as regards maintained tritium self-sufficiency is not suitable as regards improving neutronic performance of LIFE engine. A high quality fissile fuel with a rate of ~2,850 kg/year of 233U can be produced with 75 % LiF—23 % ThF4—2 % 233UF4. The energy multiplication factor is increased with high rate fission reactions of 233U occurring in the molten salt zone. Major damage mechanisms in SS-304 first wall stell have been computed as DPA = 48 and He = 132 appm per year with 75 % LiF—23 % ThF4—2 % 233UF4. This implies a replacement of the SS-304 first wall stell of every between 3 and 4 years.
Corzo, H H; Galano, Annia; Dolgounitcheva, O; Zakrzewski, V G; Ortiz, J V
Two accurate and computationally efficient electron-propagator (EP) methods for calculating the valence, vertical ionization energies (VIEs) of closed-shell molecules have been identified through comparisons with related approximations. VIEs of a representative set of closed-shell molecules were calculated with EP methods using 10 basis sets. The most easily executed method, the diagonal, second-order (D2) EP approximation, produces results that steadily rise as basis sets are improved toward values based on extrapolated coupled-cluster singles and doubles plus perturbative triples calculations, but its mean errors remain unacceptably large. The outer valence Green function, partial third-order and renormalized partial third-order methods (P3+), which employ the diagonal self-energy approximation, produce markedly better results but have a greater tendency to overestimate VIEs with larger basis sets. The best combination of accuracy and efficiency with a diagonal self-energy matrix is the P3+ approximation, which exhibits the best trends with respect to basis-set saturation. Several renormalized methods with more flexible nondiagonal self-energies also have been examined: the two-particle, one-hole Tamm-Dancoff approximation (2ph-TDA), the third-order algebraic diagrammatic construction or ADC(3), the renormalized third-order (3+) method, and the nondiagonal second-order renormalized (NR2) approximation. Like D2, 2ph-TDA produces steady improvements with basis set augmentation, but its average errors are too large. Errors obtained with 3+ and ADC(3) are smaller on average than those of 2ph-TDA. These methods also have a greater tendency to overestimate VIEs with larger basis sets. The smallest average errors occur for the NR2 approximation; these errors decrease steadily with basis augmentations. As basis sets approach saturation, NR2 becomes the most accurate and efficient method with a nondiagonal self-energy. PMID:26226061
Marin, Nena Maribel
Fluorescence and diffuse reflectance spectroscopy are two new optical technologies, which have shown promise to aid in the real time, non-invasive identification of cancers and precancers. Spectral patterns carry a fingerprint of scattering, absorption and fluorescence properties in tissue. Scattering, absorption and fluorescence in tissue are directly affected by biological features that are diagnostically significant, such as nuclear size, micro-vessel density, volume fraction of collagen fibers, tissue oxygenation and cell metabolism. Thus, analysis of spectral patterns can unlock a wealth of information directly related with the onset and progression of disease. Data from a Phase II clinical trial to assess the technical efficacy of fluorescence and diffuse reflectance spectroscopy acquired from 850 women at three clinical locations with two research grade optical devices is calibrated and analyzed. Tools to process and standardize spectra so that data from multiple spectrometers can be combined and analyzed are presented. Methodologies for calibration and quality assurance of optical systems are established to simplify design issues and ensure validity of data for future clinical trials. Empirically based algorithms, using multivariate statistical approaches are applied to spectra and evaluated as a clinical diagnostic tool. Physically based algorithms, using mathematical models of light propagation in tissue are presented. The presented mathematical model combines a diffusion theory in P3 approximation reflectance model and a 2-layer fluorescence model using exponential attenuation and diffusion theory. The resulting adjoint fluorescence and reflectance model extracts twelve optical properties characterizing fluorescence efficiency of cervical epithelium and stroma fluorophores, stromal hemoglobin and collagen absorption, oxygen saturation, and stromal scattering strength and shape. Validations with Monte Carlo simulations show that adjoint model extracted