Effects of Measurement Temperature on Radioluminescence Processes in Cerium-Activated Silica Glasses for Dosimetry Applications.

Cerium-doped-silica glasses are widely used as ionizing radiation sensing materials. However, their response needs to be characterized as a function of measurement temperature for application in various environments, such as in vivo dosimetry, space and particle accelerators. In this paper, the temperature effect on the radioluminescence (RL) response of Cerium-doped glassy rods was investigated in the 193-353 K range under different X-ray dose rates. The doped silica rods were prepared using the sol-gel technique and spliced into an optical fiber to guide the RL signal to a detector. Then, the experimental RL levels and kinetics measurements during and after irradiation were compared with their simulation counterparts. This simulation is based on a standard system of coupled non-linear differential equations to describe the processes of electron-hole pairs generation, trapping-detrapping and recombination in order to shed light on the temperature effect on the RL signal dynamics and intensity.

Properties of Gd-Doped Sol-Gel Silica Glass Radioluminescence under Electron Beams.

The radiation-induced emission (RIE) of Gd3+-doped sol-gel silica glass has been shown to have suitable properties for use in the dosimetry of beams of ionizing radiation in applications such as radiotherapy. Linear electron accelerators are commonly used as clinical radiotherapy beams, and in this paper, the RIE properties were investigated under electron irradiation. A monochromator setup was used to investigate the light properties in selected narrow wavelength regions, and a spectrometer setup was used to measure the optical emission spectra in various test configurations. The RIE output as a function of depth in acrylic was measured and compared with a reference dosimeter system for various electron energies, since the dose-depth measuring abilities of dosimeters in radiotherapy is of key interest. The intensity of the main radiation-induced luminescence (RIL) of the Gd3+-ions at 314 nm was found to well represent the dose as a function of depth, and was possible to separate from the Cherenkov light that was also induced in the measurement setup. After an initial suppression of the luminescence following the electron bunch, which is ascribed to a transient radiation-induced attenuation from self-trapped excitons (STEX), the 314 nm component was found to have a decay time of approximately 1.3 ms. An additional luminescence was also observed in the region 400 nm to 600 nm originating from the decay of the STEX centers, likely exhibiting an increasing luminescence with a dose history in the tested sample.

Radiation Effects on Fiber Bragg Gratings: Vulnerability and Hardening Studies.

Fiber Bragg gratings (FBGs) are point optical fiber sensors that allow the monitoring of a diversity of environmental parameters, e.g., temperature or strain. Several research groups have studied radiation effects on the grating response, as they are implemented in harsh environments: high energy physics, space, and nuclear facilities. We report here the advances made to date in studies regarding the vulnerability and hardening of this sensor under radiation. First, we introduce its principle of operation. Second, the different grating inscription techniques are briefly illustrated as well as the differences among the various types. Then, we focus on the radiation effects induced on different FBGs. Radiation induces a shift in their Bragg wavelengths, which is a property serving to measure environmental parameters. This radiation-induced Bragg wavelength shift (RI-BWS) leads to a measurement error, whose amplitude and kinetics depend on many parameters: inscription conditions, fiber type, pre- or post-treatments, and irradiation conditions (nature, dose, dose rate, and temperature). Indeed, the radiation hardness of an FBG is not directly related to that of the fiber where it has been photo-inscribed by a laser. We review the influence of all these parameters and discuss how it is possible to manufacture FBGs with limited RI-BWS, opening the way to their implementation in radiation-rich environments.

Monitoring of Ultra-High Dose Rate Pulsed X-ray Facilities with Radioluminescent Nitrogen-Doped Optical Fiber.

We exploited the potential of radiation-induced emissions (RIEs) in the visible domain of a nitrogen-doped, silica-based, multimode optical fiber to monitor the very high dose rates associated with experiments at different pulsed X-ray facilities. We also tested this sensor at lower dose rates associated with steady-state X-ray irradiation machines (up to 100 keV photon energy, mean energy of 40 keV). For transient exposures, dedicated experimental campaigns were performed at ELSA (Electron et Laser, Source X et Applications) and ASTERIX facilities from CEA (Commissariat à l'Energie Atomique-France) to characterize the RIE of this fiber when exposed to X-ray pulses with durations of a few µs or ns. These facilities provide very large dose rates: in the order of MGy(SiO2)/s for the ELSA facility (up to 19 MeV photon energy) and GGy(SiO2)/s for the ASTERIX facility (up to 1 MeV). In both cases, the RIE intensities, mostly explained by the fiber radioluminescence (RIL) around 550 nm, with a contribution from Cerenkov at higher fluxes, linearly depend on the dose rates normalized to the pulse duration delivered by the facilities. By comparing these high dose rate results and those acquired under low-dose rate steady-state X-rays (only RIL was present), we showed that the RIE of this multimode optical fiber linearly depends on the dose rate over an ultra-wide dose rate range from 10-2 Gy(SiO2)/s to a few 109 Gy(SiO2)/s and photons with energy in the range from 40 keV to 19 MeV. These results demonstrate the high potential of this class of radiation monitors for beam monitoring at very high dose rates in a very large variety of facilities as future FLASH therapy facilities.

Radioluminescence Response of Ce-, Cu-, and Gd-Doped Silica Glasses for Dosimetry of Pulsed Electron Beams.

Radiation-induced emission of doped sol-gel silica glass samples was investigated under a pulsed 20-MeV electron beam. The studied samples were drawn rods doped with cerium, copper, or gadolinium ions, which were connected to multimode pure-silica core fibers to transport the induced luminescence from the irradiation area to a signal readout system. The luminescence pulses in the samples induced by the electron bunches were studied as a function of deposited dose per electron bunch. All the investigated samples were found to have a linear response in terms of luminescence as a function of electron bunch sizes between 10-5 Gy/bunch and 1.5×10-2 Gy/bunch. The presented results show that these types of doped silica rods can be used for monitoring a pulsed electron beam, as well as to evaluate the dose deposited by the individual electron bunches. The electron accelerator used in the experiment was a medical type used for radiation therapy treatments, and these silica rod samples show high potential for dosimetry in radiotherapy contexts.

Impact of γ-rays Irradiation on Hybrid TiO2-SiO2 Sol-Gel Films Doped with RHODAMINE 6G.

In the present paper, we investigate how the optical and structural properties, in particular the observed photoluminescence (PL) of photocurable and organic-inorganic TiO2-SiO2 sol-gel films doped with Rhodamine 6G (R6G) are affected by γ-rays. For this, four luminescent films, firstly polymerized with UV photons (365 nm), were submitted to different accumulated doses of 50 kGy, 200 kGy, 500 kGy and 1 MGy while one sample was kept as a reference and unirradiated. The PL, recorded under excitations at 365 nm, 442 nm and 488 nm clearly evidences that a strong signal peaking at 564 nm is still largely present in the γ-irradiated samples. In addition, M-lines and Fourier-transform infrared (FTIR) spectroscopies are used to quantify the radiation induced refractive index variation and the chemical changes, respectively. Results show that a refractive index decrease of 7 × 10-3 at 633 nm is achieved at a 1 MGy accumulated dose while a photo-induced polymerization occurs, related to the consumption of CH=C, Si-OH and Si-O-CH3 groups to form Ti-O and Si-O bonds. All these results confirm that the host matrix (TiO2-SiO2) and R6G fluorophores successfully withstand the hard γ-ray exposure, opening the way to the use of this material for sensing applications in radiation-rich environments.

Investigation of the Incorporation of Cerium Ions in MCVD-Silica Glass Preforms for Remote Optical Fiber Radiation Dosimetry.

The incorporation of Ce3+ ions in silicate glasses is a crucial issue for luminescence-based sensing applications. In this article, we report on silica glass preforms doped with cerium ions fabricated by modified chemical vapor deposition (MCVD) under different atmospheres in order to favor the Ce3+ oxidation state. Structural analysis and photophysical investigations are performed on the obtained glass rods. The preform fabricated under reducing atmosphere presents the highest photoluminescence (PL) quantum yield (QY). This preform drawn into a 125 µm-optical fiber, with a Ce-doped core diameter of about 40 µm, is characterized to confirm the presence of Ce3+ ions inside this optical fiber core. The fiber is then tested in an all-fibered X-ray dosimeter configuration. We demonstrate that this fiber allows the remote monitoring of the X-ray dose rate (flux) through a radioluminescence (RL) signal generated around 460 nm. The response dependence of RL versus dose rate exhibits a linear behavior over five decades, at least from 330 µGy(SiO2)/s up to 22.6 Gy(SiO2)/s. These results attest the potentialities of the MCVD-made Ce-doped material, obtained under reducing atmosphere, for real-time remote ionizing radiation dosimetry.

Transient absorption with a femtosecond tunable excitation pump reveals the emission kinetics of color centers in amorphous silica.

We report a set of femtosecond (fs) transient absorption (TA) measurements following the dynamics of the so-called nonbridging oxygen hole center in silica, a model color center in wide bandgap amorphous solids, characterized by a very large Stokes shift between the UV excitation and its associated red emission at 1.9 eV. The changes in the TA spectrum were probed in the UV-visible range at various delays after photoexcitation and analyzed as a function of the UV excitation energy, in single-photon absorption conditions. The combination of the experiments helps to clarify the defect photocycle, highlighting how TA measurements with tunable UV excitation could represent a powerful tool to investigate the dynamics of color centers embedded in transparent materials.

Extreme Radiation Sensitivity of Ultra-Low Loss Pure-Silica-Core Optical Fibers at Low Dose Levels and Infrared Wavelengths.

We report here the response of a commercial ultra-low loss (ULL) single-mode (SM) pure silica core (PSC) fiber, the Vascade EX1000 fiber from Corning, associated with 0.16 dB/km losses at 1.55 µm to 40 keV X-rays at room temperature. Today, among all fiber types, the PSC or F-doped ones have been demonstrated to be the most tolerant to the radiation induced attenuation (RIA) phenomenon and are usually used to design radiation-hardened data links or fiber-based point or distributed sensors. The here investigated ULL-PSC showed, instead, surprisingly high RIA levels of ~3000 dB/km at 1310 nm and ~2000 dB/km at 1550 nm at a limited dose of 2 kGy(SiO2), exceeding the RIA measured in the P-doped SM fibers used for dosimetry for doses of ~500 Gy. Moreover, its RIA increased as a function of the dose with a saturation tendency at larger doses and quickly recovered after irradiation. Our study on the silica structure suggests that the very specific manufacturing process of the ULL-PSC fibers applied to reduce their intrinsic attenuation makes them highly vulnerable to radiations even at low doses. From the application point of view, this fiber cannot be used for data transfer or sensing in harsh environments, except as a very efficient radiation detector or beam monitor.

In-situ regeneration of P-doped optical fiber dosimeter.

We demonstrate the feasibility of resetting and reusing dosimeters exploiting the measurement of the infrared radiation-induced attenuation (IR-RIA) in phosphosilicate optical fibers (OFs) to provide point or distributed dose measurements in radiation environments. To bleach the room temperature stable IR-RIA, we used the photobleaching (PB) phenomenon. The PB efficiency was evaluated for different wavelengths in the [400-1100] nm range. The best identified PB resetting condition consists in using a continuous-wave Argon-ion laser at 514 nm. This treatment successfully bleached ∼97% of the IR-RIA at 1550 nm of a 30 m-long P-doped single mode optical fiber X-ray irradiated at a dose of 100 Gy. Successive re-irradiations of the same OF sample, regenerated after each run, confirm that the dosimeter keeps the same calibration curve during the whole process.

Atmospheric Neutron Monitoring through Optical Fiber-Based Sensing.

The potential of fiber-based sensors to monitor the fluence of atmospheric neutrons is evaluated through accelerated tests at the TRIUMF Neutron Facility (TNF) (BC, Canada), offering a flux approximatively 109 higher than the reference spectrum observed under standard conditions in New York City, USA. The radiation-induced attenuation (RIA) at 1625 nm of a phosphorus-doped radiation sensitive optical fiber is shown to linearly increase with neutron fluence, allowing an in situ and easy monitoring of the neutron flux and fluence at this facility. Furthermore, our experiments show that the fiber response remains sensitive to the ionization processes, at least up to a fluence of 7.1 × 1011 n cm-², as its radiation sensitivity coefficient (~3.36 dB km-1 Gy-1) under neutron exposure remains very similar to the one measured under X-rays (~3.8 dB km-1 Gy-1) at the same wavelength. The presented results open the way to the development of a point-like or even a distributed dosimeter for natural or man-made neutron-rich environments. The feasibility to measure the dose caused by the neutron exposure during stratospheric balloon experiments, or during outer space missions, is presented as a case study of a potential future application.

Comparison between the UV and X-ray Photosensitivities of Hybrid TiO2-SiO2 Thin Layers.

The photo-induced effects on sol-gel-based organo TiO2-SiO2 thin layers deposited by the dip-coating technique have been investigated using two very different light sources: A light-emitting diode (LED) emitting in the UV (at 365 nm, 3.4 eV) and an X-ray tube producing 40 keV mean-energy photons. The impact of adding a photo-initiator (2,2-dimethoxy-2-phenylacetophenone-DMPA) on the sol-gel photosensitivity is characterized namely in terms of the photo-induced refractive index measured through M-line spectroscopy. Results show that both silica-titania sol-gel films with or without the photo-initiator are photosensitive to both photon sources. The induced refractive index values reveal several features where slightly higher refractive indexes are obtained for the sol-gel containing the photo-initiator. UV and X-ray-induced polymerization degrees are discussed using Fourier-transform infrared (FTIR) spectroscopy where the densification of hybrid TiO2-SiO2 layers is related to the consumption of the CH=C groups and to the decomposition of Si-OH and Si-O-CH3 bonds. X-rays are more efficient at densifying the TiO2-SiO2 inorganic and organic network with respect to the UV photons. Hard X-ray photolithography, where no cracks or damages are observed after intense exposition, can be a promising technique to design submicronic-structure patterns on TiO2-SiO2 thin layers for the building of optical sensors.

Cu/Ce-co-Doped Silica Glass as Radioluminescent Material for Ionizing Radiation Dosimetry.

Optically activated glasses are essential to the development of new radiation detection systems. In this study, a bulk glassy rod co-doped with Cu and Ce ions, was prepared via the sol-gel technique and was drawn at about 2000 °C into a cylindrical capillary rod to evaluate its optical and radioluminescence properties. The sample showed optical absorption and photoluminescence (PL) bands attributed to Cu+ and Ce3+ ions. The presence of these two ions inside the host silica glass matrix was also confirmed using PL kinetics measurements. The X-ray dose rate was remotely monitored via the radioluminescence (RL) signal emitted by the Cu/Ce scintillating sensor. In order to transport the optical signal from the irradiation zone to the detection located in the instrumentation zone, an optical transport fiber was spliced to the sample under test. This RL signal exhibited a linear behavior regarding the dose rate in the range at least between 1.1 mGy(SiO2)/s and 34 Gy(SiO2)/s. In addition, a spectroscopic analysis of this RL signal at different dose rates revealed that the same energy levels attributed to Cu+ and Ce3+ ions are involved in both the RL mechanism and the PL phenomenon. Moreover, integrated intensities of the RL sub-bands related to both Cu+ and Ce3+ ions depend linearly on the dose rate at least in the investigated range from 102 mGy(SiO2)/s up to 4725 mGy(SiO2)/s. The presence of Ce3+ ions also reduces the formation of HC1 color centers after X-ray irradiation.

Study of silica-based intrinsically emitting nanoparticles produced by an excimer laser.

We report an experimental study demonstrating the feasibility to produce both pure and Ge-doped silica nanoparticles (size ranging from tens up to hundreds of nanometers) using nanosecond pulsed KrF laser ablation of bulk glass. In particular, pure silica nanoparticles were produced using a laser pulse energy of 400 mJ on pure silica, whereas Ge-doped nanoparticles were obtained using 33 and 165 mJ per pulse on germanosilicate glass. The difference in the required energy is attributed to the Ge doping, which modifies the optical properties of the silica by facilitating energy absorption processes such as multiphoton absorption or by introducing absorbing point defects. Defect generation in bulk pure silica before nanoparticle production starts is also suggested by our results. Regarding the Ge-doped samples, scanning electron microscopy (SEM) and cathodoluminescence (CL) investigations revealed a good correspondence between the morphology of the generated particles and their emission signal due to the germanium lone pair center (GLPC), regardless of the energy per pulse used for their production. This suggests a reasonable homogeneity of the emission features of the samples. Similarly, energy dispersive X-ray spectroscopy (EDX) data showed that the O, Ge and Si signals qualitatively correspond to the particle morphology, suggesting a generally uniform chemical composition of the Ge-doped samples. No significant CL signal could be detected in pure silica nanoparticles, evidencing the positive impact of Ge for the development of intrinsically emitting nanoparticles. Transmission electron microscope (TEM) data suggested that the Ge-doped silica nanoparticles are amorphous. SEM and TEM data evidenced that the produced nanoparticles tend to be slightly more spherical in shape for a higher energy per pulse. Scanning transmission electron microscope (STEM) data have shown that, regardless of size and applied energy per pulse, in each nanoparticle, some inhomogeneity is present in the form of brighter (i.e., more dense) features of a few nanometers.

How transparent film applied on dermatologic imaging devices in order to prevent infections affects image quality?

BACKGROUND: In the clinical practice, transparent films are used as sterile interfaces in in vivo dermatologic imaging in order to prevent the transmissions of infections. However, in our experience, the use of a transparent film can alter skin images. Our study aimed to compare the optical quality of a series of different plastic films used as interfaces in order to understand if some might be more suitable for imaging. MATERIALS AND METHODS: We tested the optical properties of 11 different protective transparent films that are marketed in France with a transparency meter and a spectrophotometer. RESULTS: Transmission, minimal diffusion, amount of gray, and contrast were obtained for each transparent film. Transmission ranged from 93.24% to 96.88% (mean 95.36; standard deviation SD 1.02), minimal diffusion from 88.28% to 123.87% (mean 101.04; standard deviation SD 10.02) and contrast from 11.01 to 15.88 (mean 13.93 and SD 1.3). For some films, the transmission was lower at lower wavelengths. CONCLUSION: All tested films had excellent optical properties. However, some of them had better optical qualities and seemed more suitable for their use in dermatologic imaging.

Radiation hardened high-power Er3+/Yb3+-codoped fiber amplifiers for free-space optical communications.

The radiation responses of different high-power erbium/ytterbium-codoped fiber amplifiers (HP-EYDFA) have been investigated up to 100 krad (SiO2) dose levels. These devices are able to deliver 20 W of signal output power at 1565 nm by pumping at 915 nm (43 W) radiation tolerant (Er/Yb) or radiation hardened (ErYbCe) active few mode fibers; these performances are needed for free-space communications between low-orbit satellites and ground transceivers. X-ray irradiation results show that, thanks to a positive influence of the photo- and thermal-bleaching phenomena associated with such high-power operating conditions, the gain degradation levels of HP-EYDFA based on radiation hardened fibers remain below 6% after 100 krad at an accelerated dose rate of 3.4 rad/s.

France's State of the Art Distributed Optical Fibre Sensors Qualified for the Monitoring of the French Underground Repository for High Level and Intermediate Level Long Lived Radioactive Wastes.

This paper presents the state of the art distributed sensing systems, based on optical fibres, developed and qualified for the French Cigéo project, the underground repository for high level and intermediate level long-lived radioactive wastes. Four main parameters, namely strain, temperature, radiation and hydrogen concentration are currently investigated by optical fibre sensors, as well as the tolerances of selected technologies to the unique constraints of the Cigéo's severe environment. Using fluorine-doped silica optical fibre surrounded by a carbon layer and polyimide coating, it is possible to exploit its Raman, Brillouin and Rayleigh scattering signatures to achieve the distributed sensing of the temperature and the strain inside the repository cells of radioactive wastes. Regarding the dose measurement, promising solutions are proposed based on Radiation Induced Attenuation (RIA) responses of sensitive fibres such as the P-doped ones. While for hydrogen measurements, the potential of specialty optical fibres with Pd particles embedded in their silica matrix is currently studied for this gas monitoring through its impact on the fibre Brillouin signature evolution.

Steady γ-Ray Effects on the Performance of PPP-BOTDA and TW-COTDR Fiber Sensing.

We investigated the evolution of the performances of Pulse Pre Pump-Brillouin Time Domain Analysis (PPP-BOTDA) and Tunable Wavelength Coherent Optical Time Domain Reflectometry (TW-COTDR) fiber-based temperature and strain sensors when the sensing optical fiber is exposed to two γ-ray irradiation conditions: (i) at room temperature and a dose rate of 370 Gy(SiO2)/h up to a total ionizing dose (TID) of 56 kGy; (ii) at room temperature and a dose rate of 25 kGy(SiO2)/h up to a TID of 10 MGy. Two main different classes of single-mode optical fibers have been tested in situ, radiation-tolerant ones: fluorine-doped or nitrogen-doped core fibers, as well as Telecom-grade germanosilicate ones. Brillouin and Rayleigh Sensitivities of N-Doped fibers were not reported yet, and these characterizations pave the way for a novel and alternative sensing scheme. Moreover, in these harsh conditions, our results showed that the main parameter affecting the sensor sensitivity remains the Radiation Induced Attenuation (RIA) at its operation wavelength of 1550 nm. RIA limits the maximal sensing range but does not influence the measurement uncertainty. F-doped fiber is the most tolerant against RIA with induced losses below 8 dB/km after a 56 kGy accumulated dose whereas the excess losses of other fibers exceed 22 dB/km. Both Rayleigh and Brillouin signatures that are exploited by the PPP-BOTDA and the TW-COTDR remain unchanged (within our experimental uncertainties). The strain and temperature coefficients of the various fibers under test are not modified by radiations, at these dose/dose rate levels. Consequently, this enables the design of a robust strain and temperature sensing architecture for the monitoring of radioactive waste disposals.

Influence of photo-inscription conditions on the radiation-response of fiber Bragg gratings.

We compared the sensitivity to X-rays of several fiber Bragg gratings (FBGs) written in the standard telecommunication fiber Corning SMF28 with different techniques. Standard gratings were manufactured with phase-mask and UV lasers, continuum wave (cw) at 244 nm or pulsed in the nanosecond domain at 248 nm, in a pre-hydrogenated fiber. Others gratings were written by exposures to a femtosecond IR-laser (800 nm), with both phase-mask and point by point techniques. The response of these FBGs was studied under X-rays at room temperature and 100°C, by highlighting their similarities and differences. Independently of the inscription technique, the two types of fs-FBGs have showed no big difference up to 1 MGy(SiO(2)) dose. A discussion on the causes of the radiation-induced peak change is also reported.

Optical diagnosis of a metabolic disease: cystinosis.

Nephropathic cystinosis (NC) is a rare autosomal recessive storage disease characterized by the lysosomal accumulation of cystine crystals throughout the body, particularly in blood cells, the cornea, skin, kidneys, the central nervous system, and the muscles. The skin and the cornea are the most accessible sites to explore, and in vivo reflectance confocal microscopy (IVCM) helps identify crystals in both but does not provide any information to help define their composition. Raman spectroscopy (RS) allows cystine to be easily recognized thanks to its characteristic signature with a band at 499 cm⁻¹. Two dermatology confocal microscopes were used to visualize crystals in both the skin and the ocular surface of a cystinosis patient, and an ex vivo Raman examination of a skin biopsy and of the cornea was performed and removed during a corneal graft to confirm the cystine composition of the crystals. Recently, RS has been performed in vivo and coupled with IVCM. In the future, it is suggested that crystals in NC and other deposits in storage diseases could be identified with this noninvasive in vivo technique that combines IVCM to recognize the deposits and RS to confirm their chemical nature.