Electrochemical promotion of catalysis using solid-state proton-conducting membranes

A solid-state electrochemical reactor with ceramic proton-conducting membrane has been used to study the effect of electrochemically induced hydrogen spillover on the catalytic activity of platinum during ethylene oxidation. Suitable proton-conducting electrolyte membranes (Gd-doped BaPrO ₃ (BPG) and Y-doped BaZrO₃ (BZY)) were fabricated. These materials were chosen because of their protonic conductivity in the operational temperature region of the reaction (400-700 °C). The BZY-based electrochemical cell was used to investigate the open-circuit voltage (OCV) dependence on H₂ partial pressure with comparison being made to the theoretical OCV as predicted by the Nernst equation. Furthermore, the BZY pellets were used to study the effect of proton transfer of the catalytic activity of platinum during ethylene oxidation. The reaction was found to exhibit electrochemical promotion at 400 °C and to be electrophilic in nature, i.e. proton addition to the platinum surface resulted in an increase in reaction rate. At higher temperatures, the rate was not affected, within experimental error, by proton addition or removal. Under similar conditions, AC impedance showed that there was a large overall cell resistance at 400 °C with significantly decreased resistance at higher temperatures. It is possible that there could be a relationship between large cell resistances and the onset of electrochemical promotion in this system but there is, as yet, no conclusive evidence for this. © 2003 Elsevier B.V. All rights reserved.

Variations in the Processing of DNA Double-Strand Breaks Along 60-MeV Therapeutic Proton Beams

PURPOSE: To investigate the variations in induction and repair of DNA damage along the proton path, after a previous report on the increasing biological effectiveness along clinically modulated 60-MeV proton beams.

METHODS AND MATERIALS: Human skin fibroblast (AG01522) cells were irradiated along a monoenergetic and a modulated spread-out Bragg peak (SOBP) proton beam used for treating ocular melanoma at the Douglas Cyclotron, Clatterbridge Centre for Oncology, Wirral, Liverpool, United Kingdom. The DNA damage response was studied using the 53BP1 foci formation assay. The linear energy transfer (LET) dependence was studied by irradiating the cells at depths corresponding to entrance, proximal, middle, and distal positions of SOBP and the entrance and peak position for the pristine beam.

RESULTS: A significant amount of persistent foci was observed at the distal end of the SOBP, suggesting complex residual DNA double-strand break damage induction corresponding to the highest LET values achievable by modulated proton beams. Unlike the directly irradiated, medium-sharing bystander cells did not show any significant increase in residual foci.

CONCLUSIONS: The DNA damage response along the proton beam path was similar to the response of X rays, confirming the low-LET quality of the proton exposure. However, at the distal end of SOBP our data indicate an increased complexity of DNA lesions and slower repair kinetics. A lack of significant induction of 53BP1 foci in the bystander cells suggests a minor role of cell signaling for DNA damage under these conditions.

Proton acceleration enhanced by a plasma jet in expanding foils undergoing relativistic transparency

Ion acceleration driven by the interaction of an ultraintense (2 × 10²⁰ W cm^-2) laser pulse with an ultrathin ( nm) foil target is experimentally and numerically investigated. Protons accelerated by sheath fields and via laser radiation pressure are angularly separated and identified based on their directionality and signature features (e.g. transverse instabilities) in the measured spatial-intensity distribution. A low divergence, high energy proton component is also detected when the heated target electrons expand and the target becomes relativistically transparent during the interaction. 2D and 3D particle-in-cell simulations indicate that under these conditions a plasma jet is formed at the target rear, supported by a self-generated azimuthal magnetic field, which extends into the expanded layer of sheath-accelerated protons. Electrons trapped within this jet are directly accelerated to super-thermal energies by the portion of the laser pulse transmitted through the target. The resulting streaming of the electrons into the ion layers enhances the energy of protons in the vicinity of the jet. Through the addition of a controlled prepulse, the maximum energy of these protons is demonstrated experimentally and numerically to be sensitive to the picosecond rising edge profile of the laser pulse.

Picosecond metrology of laser-driven proton bursts

Tracking primary radiation-induced processes in matter requires ultrafast sources and high precision timing. While compact laser-driven ion accelerators are seeding the development of novel high instantaneous flux applications, combining the ultrashort ion and laser pulse durations with their inherent synchronicity to trace the real-time evolution of initial damage events has yet to be realized. Here we report on the absolute measurement of proton bursts as short as 3.5±0.7 ps from laser solid target interactions for this purpose. Our results verify that laser-driven ion acceleration can deliver interaction times over a factor of hundred shorter than those of state-of-the-art accelerators optimized for high instantaneous flux. Furthermore, these observations draw ion interaction physics into the field of ultrafast science, opening the opportunity for quantitative comparison with both numerical modelling and the adjacent fields of ultrafast electron and photon interactions in matter.

Buffered high charge spectrally-peaked proton beams in the relativistic-transparency regime

Spectrally-peaked proton beams of high charge (E_p ≈ 8 MeV, ΔE ≈ 4 MeV, N ≈ 50 nC ) have been observed from the interaction of an intense laser (>10¹⁹Wcm^-2) with ultrathinCHfoils, as measured by spectrally-resolved full beam profiles. These beams are reproducibly generated for foil thicknesses 5-100 nm, and exhibit narrowing divergence with decreasing target thickness down to ≈8° for 5 nm. Simulations demonstrate that the narrow energy spread feature is a result of buffered acceleration of protons. The radiation pressure at the front of the target results in asymmetric sheath fields which permeate throughout the target, causing preferential forward acceleration. Due to their higher chargeto-mass ratio, the protons outrun a carbon plasma driven in the relativistic transparency regime.

Laser driven MeV proton beam focussing by auto-charged electrostatic lens configuration

Significant reduction of inherent large divergence of the laser driven MeV proton beams is achieved by strong (of the order of 10^9 V/m ) electrostatic focussing field generated in the confined region of a suitably shaped structure attached to the proton generating foil. The scheme exploits the positively charging of the target following an intense laser interaction. Reduction in the proton beam divergence, and commensurate increase in proton flux is observed while preserving the beam laminarity. The underlying mechanism has been established by the help of particle tracing simulations. Dynamic focussing power of the lens, mainly due to the target discharging, can also be exploited in order to bring up the desired chromaticity of the lens for the proton beams of broad energy range.

Investigating the Implications of a Variable RBE on Proton Dose Fractionation Across a Clinical Pencil Beam Scanned Spread-Out Bragg Peak

Purpose: To investigate the clinical implications of a variable relative biological effectiveness (RBE) on proton dose fractionation. Using acute exposures, the current clinical adoption of a generic, constant cell killing RBE has been shown to underestimate the effect of the sharp increase in linear energy transfer (LET) in the distal regions of the spread-out Bragg peak (SOBP). However, experimental data for the impact of dose fractionation in such scenarios are still limited.

Methods and Materials: Human fibroblasts (AG01522) at 4 key depth positions on a clinical SOBP of maximum energy 219.65 MeV were subjected to various fractionation regimens with an interfraction period of 24 hours at Proton Therapy Center in Prague, Czech Republic. Cell killing RBE variations were measured using standard clonogenic assays and were further validated using Monte Carlo simulations and parameterized using a linear quadratic formalism.

Results: Significant variations in the cell killing RBE for fractionated exposures along the proton dose profile were observed. RBE increased sharply toward the distal position, corresponding to a reduction in cell sparing effectiveness of fractionated proton exposures at higher LET. The effect was more pronounced at smaller doses per fraction. Experimental survival fractions were adequately predicted using a linear quadratic formalism assuming full repair between fractions. Data were also used to validate a parameterized variable RBE model based on linear α parameter response with LET that showed considerable deviations from clinically predicted isoeffective fractionation regimens.

Conclusions: The RBE-weighted absorbed dose calculated using the clinically adopted generic RBE of 1.1 significantly underestimates the biological effective dose from variable RBE, particularly in fractionation regimens with low doses per fraction. Coupled with an increase in effective range in fractionated exposures, our study provides an RBE dataset that can be used by the modeling community for the optimization of fractionated proton therapy.

Dynamic control of laser driven proton beams by exploiting self-generated, ultrashort electromagnetic pulses

As part of the ultrafast charge dynamics initiated by high intensity laser irradiations of solid targets,high amplitude EM pulses propagate away from the interaction point and are transported along anystalks and wires attached to the target. The propagation of these high amplitude pulses along a thinwire connected to a laser irradiated target was diagnosed via the proton radiography technique,measuring a pulse duration of 20 ps and a pulse velocity close to the speed of light. The strongelectric field associated with the EM pulse can be exploited for controlling dynamically the protonbeams produced from a laser-driven source. Chromatic divergence control of broadband laser drivenprotons (upto 75% reduction in divergence of >5 MeV protons) was obtained by winding the supportingwire around the proton beam axis to create a helical coil structure. In addition to providingfocussing and energy selection, the technique has the potential to post-accelerate the transiting protonsby the longitudinal component of the curved electric field lines produced by the helical coil lens.

Direct spun aligned carbon nanotube web-reinforced proton exchange membranes for fuel cells

A new method combining electrospinning of SPEEK and direct spinning of CNT forests has been used to prepare sulfonated poly(ether ether ketone) (SPEEK)/directly spinnable carbon nanotube (dsCNT) composite proton exchange membranes. The SPEEK/dsCNT membrane is more robust than SPEEK alone, and in a fuel cell significantly outperforms both SPEEK and the commercial Nafion 212 membranes.

A transport beamline solution to control optically accelerated proton beams

Laser-target interaction represents a very promising field for several potential applications,
from the nuclear physics to the radiobiology. However optically accelerated particle beams are
characterized by some extreme features, not suitable for many applications. Therefore, beyond
the improvements at the laser-target interaction level, many researchers are spending their efforts
for the development of specific beam transport devices in order to obtain controlled and
reproducible output beams.In this background, the ELIMED (ELI-Beamlines MEDical applications)
project was born. Within 2017, a dedicated transport beam-line coupled with dosimetric
systems, named ELIMED, will be installed at the Extreme Light Infrastructure Beamlines
(ELI-Beamlines) facility in Prague (CZ),as a part of the ELIMAIA (ELI Multidisciplinary Applications
of laserâA ¸SIon Acceleration) beamline

Towards optical polarization control of laser-driven proton acceleration in foils undergoing relativistic transparency

Control of the collective response of plasma particles to intense laser light is intrinsic to relativistic optics, the development of compact laser-driven particle and radiation sources, as well as investigations of some laboratory astrophysics phenomena. We recently demonstrated that a relativistic plasma aperture produced in an ultra-thin foil at the focus of intense laser radiation can induce diffraction, enabling polarization-based control of the collective motion of plasma electrons. Here we show that under these conditions the electron dynamics are mapped into the beam of protons accelerated via strong charge-separation-induced electrostatic fields. It is demonstrated experimentally and numerically via 3D particle-in-cell simulations that the degree of ellipticity of the laser polarization strongly influences the spatial-intensity distribution of the beam of multi-MeV protons. The influence on both sheath-accelerated and radiation pressure-accelerated protons is investigated. This approach opens up a potential new route to control laser-driven ion sources.