The influence of heavy water on boron requirements for neutron capture therapy.

Neutron penetration in tissue is a major limitation of thermal NCT, as such much work has centered upon the epithermal neutron beam in an effort to improve this situation. Further gains in neutron flux penetration, and thus therapeutic ratios, are possible if natural water is replaced with heavy water prior to therapy. Applying MCNP to a heterogeneous ellipsoidal skull/brain model, advantage depth and therapeutic depth parameters are studied as a function of heavy water replacement for a range of tumor to blood boron ratios. Both thermal (0.025 eV) and epithermal (2-7 keV) ideal neutron beams are analyzed. Using 10B ratios in the range of documented human uptake, the thermal advantage depth improved by approximately 0.7 cm for 20% D2O replacement, however, the therapeutic depth increased by less than half this value. For the epithermal beam, both the advantage depth and the therapeutic depth increased by over 1 cm. Effects of heavy water replacement on 10B requirements to therapeutically treat the midline of the brain are also evaluated.

Magnetic repulsion of linear accelerator contaminates.

Neodymium Iron Boron (NdFeB) rare earth permanent magnets have unique properties that enable them to fit easily onto the accessory mount of a clinical linear accelerator to partially sweep away electron contamination produced by the treatment head and block trays and thus increase skin sparing. Using such magnets the central axis entrance surface dose has been reduced by 11% for a 20 x 30 cm field size from 32% to 21% of maximum dose by the magnetic device. A reduction of 14% from 32% to 18% was seen for a 20 x 20 cm field size with a 6 mm perspex block tray positioned above the magnet. The magnetic device is light weight and thus clinically usable.

A new radiotherapy surface dose detector:the MOSFET.

Radiotherapy x-ray and electron beam surface doses are accurately measurable by use of a MOS-FET detector system. The MOSFET (Metal Oxide Semiconductor Field Effect Transistor) is approximately 200-microns in diameter and consists of a 0.5-microns Al electrode on top of a 1-microns SiO2 and 300-microns Si substrate. Results for % surface dose were within +/- 2% compared to the Attix chamber and within +/- 3% of TLD extrapolation results for normally incident beams. Detectors were compared using different energies, field size, and beam modifying devices such as block trays and wedges. Percentage surface dose for 10 x 10-cm and 40 x 40-cm field size for 6-MV x rays at 100-cm SSD using the MOSFET were 16% and 42% of maximum, respectively. Factors such as its small size, immediate retrieval of results, high accuracy attainable from low applied doses, and as the MOSFET records its dose history make it a suitable in vivo dosimeter where surface and skin doses need to be determined. This can be achieved within part of the first fraction of dose (i.e., only 10 cGy is required.)

Monte Carlo calculations of epithermal boron neutron capture therapy with heavy water.

Much work over the past decade has centred upon the development of epithermal neutron beams for boron neutron capture therapy (BNCT) in an effort to increase thermal-neutron flux penetration and dose homogeneity throughout the brain. While heavy water has been used extensively to improve neutron penetration associated with thermal neutron beams, the effects of heavy water with epithermal neutron beams remain largely unexplored. Applying the Monte Carlo code MCNP to a heterogenous ellipsoidal skull/brain model, the effects of heavy-water replacement are studied for the JRC/ECN Petten HFR epithermal neutron beam. Thermal neutron flux and induced gamma depth dose distributions are calculated for 20% D2O replacement in comparison to standard brain and skull materials. Results are presented for both unilateral and bilateral irradiation. With bilateral irradiation, thermal-neutron flux homogeneity is substantially increased with 20% D2O replacement, thus improving the potential to give lethal doses to boron-10-loaded, disseminated cancer cells whilst avoiding local 'hot spots' to healthy tissue. Additionally, the induced gamma dose is reduced by up to 30%, substantially lowering the background dose to healthy tissue. With bilateral irradiation, 20% D2O replacement increases the therapeutic ratio from 2.25 to 2.75 for over 4 cm depth centred at the midline of the brain. These calculations use documented tumour and blood 10B concentrations for boronophenylalanine (BPA) in humans and recently documented neutron relative biological effectiveness (RBE) values.

Teatment planning figures of merit in thermal and epithermal boron neutron capture therapy of brain tumours.

The boron neutron capture therapy (BNCT) figures of merit of advantage depth, therapeutic depth, modified advantage depth and maximum therapeutic depth have been studied as functions of 10B tumour to blood ratios and absolute levels. These relationships were examined using the Monte Carlo neutron photon transport code, MCNP, with an ideal 18.4 cm diameter neutron beam incident laterally upon all ellipsoidal neutron photon brain-equivalent model. Mono-energetic beams of 0.025 eV (thermal) and 35 eV (epithermal) were simulated. Increasing the tumour to blood 10B ratio predictably increases all figures of merit. concentration was also shown to have a strong bearing on the figures of merit when low levels were present in the system. This is the result of a non-10B dependent background dose. At higher levels however, the concentration of 10B has a diminishing influence. For boron sulphydryl (BSH), little advantage is gained by extending the blood 10B level beyond 30 ppm, whilst for D,L,-p-boronophenylalanine (BPA) this limit is 10 ppm. To achieve a therapeutic depth of 6 cm (brain mid-line from brain surface) using the thermal beam, a tumour to blood ratio of 25 with 10 ppm 10B in the blood is required for BPA. Similarly, a tumour to blood ratio of 8.5 with 30 ppm blood 10B is required for the maximum therapeutic depth of BSH to reach the brain mid-line. These requirements are five times above current values for these compounds in humans. Applying the epithermal beam under identical conditions, the therapeutic depth reaches the brain mid-line with a tumour to blood 10B ratio of only 5.7 for BPA. For BSH, the maximum therapeutic depth reaches the brain mid-line with a tumour to blood ratio of only 1.9 with 30 ppm in the blood. Human data for these compounds are very close to these requirements.

Radiochromic film as a radiotherapy surface-dose detector.

Radiochromic film is shown to be a useful surface-dose detector for radiotherapy x-ray beams. Central-axis percentage surface-dose results as measured by Gafchromic film for a 6 MVp x-ray beam produced by a Varian 2100C Linac at 100 cm SSD are 16%, 25%, 35%, 41% for 10, 20, 30 and 40 cm square field sizes, respectively. Using a simple, uniform light source and a CCD camera connected to an image analysis system, quantitative 3D surface doses are accurately attainable in real time as either numerical data, a black-and-white image or a colour-enhanced image.

Effect of interaction of thenoyltrifluoroacetone with neutral oxo-donors in the synergistic extraction of tervalent actinides.

The interaction of HTTA with TBP, DOSO, DBBP and TOPO in xylene has been studied by a spectrophotometric method. The complex species formed is HTTA. S (where S is a neutral donor) and the equilibrium constants for the formation of the species follow the order TOPO > DBBP > DOSO > TBP. After application of a correction for the HTTA-S interaction, the free HTTA and S concentrations in the organic phase were calculated. Plots of log D vs. log [HTTA] for the tervalent actinides Am, Cm, Bk and Cf gave straight lines with a slope of 3 only after application of the interaction correction, otherwise curves with slopes varying from 3 to 2 were found. The equilibrium constants of the organic phase synergistic reactions of the tervalent actinides are found to be approximately 10% higher after application of the HTTA-S interaction correction.

ICP-AES determination of silver after chemical separation from uranium matrix.

The separation of silver from a uranium matrix has been carried out using Cyanex-471X (triisobutylphosphine sulphide) in xylene. The effects of various parameters such as the Cyanex-471X concentration, the nitric acid molarity, the contact time and the nitrate ion concentration on the extraction of silver have been studied. The silver metal ion species extracted into the organic phase was found to be Ag(NO(3)).2S (where S is Cyanex-471X). The stripping of silver into an aqueous medium was carried out with 5% NaHSO(3), followed by its determination using ICP-AES.

Extraction of actinides and fission products by octyl(phenyl)-N,N-diisobutylcarbamoylmethyl-phosphine oxide from nitric acid media.

Extraction of promethium(III), uranium(VI), plutonium(IV), americium(III), zirconium(IV), ruthenium(III), iron(III) and palladium(II) has been carried out with a mixture of octyl(phenyl)-N,N-diisobutylcarbamoylmethylphosphine oxide (CMPO) and tributyl phosphate (TBP) in dodecane. The effects of nitric acid, TBP and CMPO concentrations on the extraction of these metal ions have been studied. The nature of the species of the above metal ions extracted into the organic phase has been suggested.

Determination of trace impurities in uranium, thorium and plutonium matrices by solvent extraction and inductively coupled plasma atomic emission spectrometry.

Studies on the determination of trace metallic impurities in nuclear materials such as uranium, thorium and plutonium are described. The bulk of the matrix is separated by batch extraction from their nitric acid solutions using 2-ethylhexyl hydrogen 2-ethylhexyl phosphonate (KSM-17, equivalent to PC88-A). The final aqueous phase containing the metallic impurities is fed to a high-temperature source inductively coupled plasma and the analysis is carried out employing a computer-controlled multichannel direct-reading spectrometer. The studies also included the recovery of impurities at various acidities and spectral interferences of the above matrices over the analyte elements. Based on the above studies, methods were standardized for the determination of 19 elements, viz. Al, B, Be, Ca, Cd, Cr, Cu, Fe, Mg, Mn, Ni, Pb, Si, Zn, Ce, Dy, Eu, Gd and Sm, in U/Th/Pu solutions. The relative standard deviation for various elements is in the range 1-5%.

Recovery of plutonium and americium from laboratory acidic waste solutions using tri-n-octylamine and octylphenyl-N-N- diisobutylcarbamoylmethylphosphine oxide.

Plutonium from acidic waste solutions has been recovered quantitatively using tri-n-octylamine (TnOA) in xylene and americium using a mixture of octylphenyl-N-N- diisobutylcarbamoylmethylphosphine oxide (CMPO) and TBP in dodecane by extraction and extraction chromatographic methods. The Pu ( IV ) TnOA species extracted into the organic phase from higher nitric acid concentrations has been confirmed as (R(3)NH)(2)Pu(NO(3))(6) (where R(3)N = TnOA by employing slope analysis as well as spectrophotometric studies.

An analytical representation of equivalent square field size in relation to surface dose.

Analytical representation of the build up characteristics of megavoltage photon beams is achievable, producing accurate percentage dose results in the build up region for typical patient treatments. This approach requires conversion of an irregular shaped field to a equivalent square field for mathematical analysis. Surface dose for rectangular fields is expressed by an extension to Stirling's 4A/P formula while irregular shaped fields follow an area integration technique. The equivalent square for a typical irregular treatment field is modelled within +/- 0.5 cm2 for all measured fields.

Effect of block trays on skin dose in radiotherapy.

Percentage dose at the surface and at 1 mm depth for megavoltage photon beams are increased through the influence of block trays. This represents a decrease in skin sparing properties for both the epidermal and dermal layers. The increase in percentage dose varies with type and thickness of block tray material. At 6MVp, 20cm x 20cm field size, the percentage surface dose is 26%, 26.5%, 33% and 35% for open, steel honeycomb tray, 6mm perspex and 10 mm perspex block trays respectively. At 1 mm depth these values are 52%, 52.5%, 61%, 60% respectively. A similar effect is seen at higher energies. Results show that care should be taken when selecting an appropriate block tray if skin sparing is of importance.

6MV x-ray dose in the build up region: empirical model and the incident angle effect.

A simple and fast empirical model has been developed which accurately predicts central axis surface and build up dose for a 6MV radiotherapy x-ray beam. The model is based on fits to experimental data and accounts for open fields, block trays and wedges at normal incidence and at angle. The model separates the beam into components produced by primary photon interactions which have only interacted in the phantom at normal and oblique incidence and head scattered photons/electrons generated in the treatment head. The model quantifies these components for open unwedged fields and then the effect on each component by introducing beam modifying devices/ accessories or changing the angle of incidence is determined. Dose results at oblique incidence for Monte Carlo (electron contamination free) and experimental (electron contamination present) are sufficiently close to imply that the increase in build up dose with beam angle is mainly due to changes in photon interactions within the phantom and only a slight increase with angle is due to changes in the electron contamination. Electron contamination/ head scatter component was found to be measurable by three methods. These being TLD extrapolation in air, ionisation chamber measurements in air and Monte Carlo pure photon methods. These methods produced comparable electron contamination/head scatter dose results at all field sizes.

Conversion of an infrared densitometer for radiochromic film analysis.

By the simple incorporation of a high intensity red LED into a typical infrared film densitometer, radiochromic film can be analysed using existing detectors and scanning software. Results show an accurate dose measurement using radiochromic film and this system compared to conventional detectors for percentage depth dose and penumbral measurements in high and low energy x-ray beams. A small circuit including a red Light Emitting Diode (LED) was positioned inside the film densitometer which does not obscure the infrared source. The red and infrared diodes work independently. For 6 MV x-rays, the 80%/20% penumbral width at 15 mm depth for a 10 x 10 cm field at 100 cm SSD was measured to be 3.5 mm with radiochromic film as compared to 3.3 with corrected diode measurements. Percentage depth doses were measured to within +/- 3% of ionisation chamber data at 6MV and within +/- 2% for 250 kVp x-ray with the film placed parallel to the beam direction in both cases.

Skin dose reduction by a clinically viable magnetic deflector.

A variable magnetic deflector which attaches onto the treatment head of a linear accelerator has reduced skin dose by as much as 65% for 6MV x-rays. The magnetic deflector is constructed from Neodymium Iron Boron (NdFeB) rare earth magnets. It weighs approximately 15 kg and is designed to easily fit onto the accessory mount of a clinical linear accelerator. All field sizes are attainable up to 35 cm x 35 cm at 100 cm SSD. The gap between the magnetic poles can be adjusted, providing the highest field strength for each field size. Magnetic field strengths up to 0.55 Tesla are attainable. For a 6MV x-ray beam with a 10 mm perspex block tray, surface dose is reduced from 29% to 14% and from 59% to 37% for a 20 cm x 20 cm and 35 cm x 35 cm field size, respectively. Results at varying SSD's have shown at least 10 cm of space must be allowed between the magnets and patient for adequate reduction of skin dose through removal of electron contaminants.

Coordination modes in the formation of the ternary Am(III), Cm(III), and Eu(III) complexes with EDTA and NTA: TRLFS, 13C NMR, EXAFS, and thermodynamics of the complexation.

The formation and the structure of the ternary complexes of trivalent Am, Cm, and Eu with mixtures of EDTA+NTA (ethylenediamine tetraacetate and nitrilotriacetate) have been studied by time-resolved laser fluorescence spectroscopy, 13C NMR, extended X-ray absorption fine structure, and two-phase metal ion equilibrium distribution at 6.60 m (NaClO4) and a hydrogen ion concentration value (pcH) between 3.60 and 11.50. In the ternary complexes, EDTA binds via four carboxylates and two nitrogens, while the binding of the NTA varies with the hydrogen ion concentration, pcH, and the concentration ratios of the metal ion and the ligand. When the concentration ratios of the metal to ligand is low (1:1:1-1:1:2), two ternary complexes, M(EDTA)(NTAH)(3-) and M(EDTA)(NTA)(4-), are formed at pcH ca. 9.00 in which NTA binds via three carboxylates, via two carboxylates and one nitrogen, or via two carboxylates and a H2O. At higher ratios (1:1:20 and 1:10:10) and pcH's of ca. 9.00 and 11.50, one ternary complex, M(EDTA)(NTA)(4-), is formed in which NTA binds via three carboxylates and not via nitrogen. The two-phase equilibrium distribution studies at tracer concentrations of Am, Cm, and Eu have also confirmed the formation of the ternary complex M(EDTA)(NTA)(4-) at temperatures between 0 and 60 degrees C. The stability constants (log beta111) for these metal ions increase with increasing temperature. The endothermic enthalpy and positive entropy indicated a significant effect of cation dehydration in the formation of the ternary complexes at high ionic strength.

Skin dose from radiotherapy X-ray beams: the influence of energy.

Skin-sparing properties of megavoltage photon beams are compromised by electron contamination. Higher energy beams do not necessarily produce lower surface and basal cell layer doses due to this electron contamination. For a 5 x 5 cm field size the surface doses for 6 MVp and 18 MVp X-ray beams are 10% and 7% of their respective maxima. However, at a field size of 40 x 40 cm the percentage surface dose is 42% for both 6 MVp and 18 MVp beams. The introduction of beam modifying devices such block trays can further reduce the skin-sparing advantages of high energy photon beams. Using a 10 mm perspex block tray, the surface doses for 6 MVp and 18 MVp beams with a 5 x 5 cm field size are 10% and 8%, respectively. At 40 x 40 cm, surface doses are 61% and 63% for 6 MVp and 18 MVp beams, respectively. This trend is followed at the basal cell layer depth. At a depth of 1 mm, 18 MVp beam doses are always at least 5% smaller than 6 MVp doses for the same depth at all field sizes when normalized to their respective Dmax values. Results have shown that higher energy photon beams produce a negligible reduction of the delivered dose to the basal cell layer (0.1 mm). Only a small increase in skin sparing is seen at the dermal layer (1 mm), which can be negated by the increased exit dose from an opposing field.

Chemical separation and ICP-AES determination of 22 metallic elements in U and Pu matrices using cyanex-923 extractant and studies on stripping of U and Pu.

Comprehensive studies have been carried out on the extraction behavior of uranium and plutonium matrices using cyanex-923 extractant. The near total extraction of U/Pu and quantitative separation of 22 metallic elements at trace levels has been established using inductively coupled plasma-atomic emission spectrometry (ICP-AES). The studies carried out on back extraction of U/Pu from organic phase have established the near total recovery of these matrices into the aqueous phase using 1 M Na(2)CO(3) and saturated oxalic acid, respectively.