1. Introduction
The exploitation of Brillouin scattering in silica-based optical fibers has attracted much interest in temperature and strain monitoring in harsh environments such as those encountered in the nuclear industry [
1,
2]. Measuring the fiber Brillouin signature with a reflectometer (either in the time or frequency domain [
3,
4]) opens the way to distributed temperature and strain in situ measurement along the fiber length over long distances of tens of kilometers [
5]. This work investigates the sensing possibilities offered by Brillouin-based optical fiber sensors in harsh environments with combined radiation and temperature constraints. In the literature, this approach to combined temperature/irradiation effects via Brillouin sensing has never been systematically studied.
This study investigates both losses and Brillouin signature behaviors under X-rays on Germanium-doped (Ge-doped) and Fluorine-doped (F-doped) single-mode (SM) optical fibers. Ge-doped single-mode fibers (SMFs) are commonly employed for such applications, constituting the majority of deployed single-mode fibers in the telecommunications industry. F-doped optical fibers are nowadays considered as radiation-hard SMFs for environments associated with steady-state irradiation and doses exceeding 10 kGy [
6], for which they present the lowest degradation due to the Radiation-Induced Attenuation (RIA) phenomenon at Telecom wavelengths. This work is performed using a Stimulated Brillouin Scattering (SBS) interrogator known as Brillouin Optical Time Domain Analyzer (BOTDA) at 1550 nm. The counter-propagation of the two-pump pulse and continuous probe along the waveguide allows Brillouin backscattering, containing the Brillouin spectrum signature, when the two counter-propagative waves match the Brillouin frequency. In fact, through the electrostriction effect [
7], the stimulation of acoustic waves in the fiber core and cladding allows Brillouin spectrum measurement along the fiber length. Brillouin frequencies of the fibers (their specific and intrinsic responses) (
) are dependent on both temperature and stress applied and present a cross-sensitivity of both temperature (
) and strain (
) coefficients for the standard types of fibers of 1 MHz/°C and 0.05 MHz/
[
8,
9], respectively, originating from the silica core glass density and refractive index profile of the fiber, which are both temperature (T) and strain (ε) dependent. The central Brillouin Frequency Shift follows relation (1):
The frequency shifts due to temperature and strain variations according to the fiber sensitivities. The central Brillouin Frequency Shift
follows relation (1), where
and
are temperature and strain variations [
10].
However, when irradiated, point defects are generated in the fiber glass matrix, leading to the creation of additional spectral absorption bands in the fiber transmission window responsible for an excess of optical losses called Radiation-Induced Attenuation (RIA) [
11]. Depending on the nature of the involved optically active defects, RIA usually grows with the total ionizing dose and can decay after irradiation as some defects recover [
12]. RIA also leads to a decrease in the Brillouin spectrum signal amplitude. Moreover, the Brillouin spectrum is also subjected to radiation-induced modification of its spectrum through Radiation-Induced Brillouin Frequency Shift (RI-BFS) [
13]. RI-BFS leads to systematic temperature and strain errors when measuring Brillouin central frequency in a harsh environment as the BFS is used to monitor those parameters. RIA and Brillouin spectrum modifications under irradiation have been shown to depend on the fiber composition (dopant and concentration), on the operating wavelength and on environmental conditions such as the irradiation temperature [
2].
The irradiation effect on Brillouin signature has been studied [
14] on both Ge-doped and F-doped fibers under γ-rays at room temperature up to 10 MGy, exhibiting an RI-BFS of 4 MHz and 2.3 MHz, respectively. These frequency shifts can be interpreted as variations of 4 °C or 80 µε for the Ge fiber, which results in errors being induced in the measurements by the irradiations. In our case, no significant radiation effect on
was pointed out for the tested fibers, and a decrease of 6% was noted in
after a 10 MGy accumulated dose for the F-doped fiber. Online SBS measurements were conducted during γ-rays exposure up to a cumulative dose of 1 MGy in Ge-doped single-mode fibers (SMF) at room temperature, +80 °C, +100 °C and +120 °C. This first combined thermal and radiation effect study on Brillouin sensing revealed a dependence of the Brillouin peak amplitude decrease on the irradiation temperature.; lower losses were observed at higher temperatures [
15] and showed an RI-BFS of 4 MHz, experiencing a sublinear trend. It was then not obvious that the irradiation temperature had an impact on the RI-BFS considering the uncertainties of the measurement. This phenomenon needs a deeper investigation.
RIA in Ge- and F-doped fibers has been extensively investigated under X-rays at room temperature [
11]. RIA in F-doped fibers exhibits low levels and low irradiation temperature dependence [
6] from −80 °C to +80 °C at 1550 nm. Similar studies have been conducted on Ge-doped fibers, exhibiting higher RIA levels and a high sensitivity to the temperature of irradiation in the same temperature range [
16]. In fact, RIA and its temperature sensitivity also depend on the Ge dopant concentration [
17], demonstrating a reduced sensitivity to temperature with an increase in germanium dopant concentration (>7 mol%).
This work aims to study both radiation and temperature contributions to Brillouin sensing capabilities for different fiber compositions in a large temperature range. Three types of fibers were tested in this work: a low GeO2 dopant concentration (4 wt%) (SMF28e+), a higher GeO2 concentration (10 wt%) and a radiation-hardened F-doped fiber (1 wt%). Samples were X-ray irradiated up to a cumulated dose of 108 kGy(SiO2) at a dose rate of 6 Gy/s from −80 °C to +80 °C, providing optical fiber Brillouin-based sensing capabilities in a harsh environment to adapt the fiber type to the desired application.
3. Results
In this section, we present for all the studied samples the measured RIA dependence at different temperatures of irradiation. In addition, BGS behavior under irradiation at different temperatures was monitored, providing results on the BGS attenuation and BFS, as well as Brillouin temperature and strain sensitivities.
3.1. Radiation-Induced Attenuation
In this section, we present the measured RIA dependence on temperature of irradiation for SMF28e+, CMS and F-doped fibers obtained at the unique dose rate of 6 Gy (SiO
2)/s and accumulated dose of 108 kGy(SiO
2). Each fiber type was irradiated at −80 °C, −40 °C, +20 °C and +80 °C. The online measurements were carried out with an OTDR at three probe wavelengths (1310 nm, 1550 nm and 1625 nm) according to the irradiation configuration shown in
Figure 2. The evolution of the RIA both during the irradiation run (5 h) and recovery phase (1 h) is presented in
Figure 4 for all the studied fibers and at the three wavelengths.
RIA corresponds to the increase in the fiber attenuation caused by point defects. The F-doped fiber exhibited the lowest RIA levels at any measured wavelength, with a maximum of 30 dB/km, 17 dB/km and 5 dB/km at −80 °C, −40 °C, +20 °C and +80 °C, respectively, at 1550 nm. We can highlight that for all our samples and at all probed wavelengths, RIA levels decreased versus temperature. It is known that pure-silica-core and fluorine-doped fibers are radiation-hardened fibers exhibiting low RIA levels [
24] in the NIR (Near-Infra-Red) domain. The RIA difference between −80 °C and +80 °C is about 48 dB/km, 24 dB/km and 17 dBm at 1310 nm, 1550 nm and 1625 nm, respectively. According to RIA spectral studies conducted on both pure-silica-core fiber and F-doped fibers [
24,
25], RIA levels increase when decreasing the wavelength in the NIR domain for a lower temperature of irradiation. Similar results were obtained from −80 °C to +80 °C, with losses equal to 43 dB/km and 6 dB/km, respectively, at 1550 nm up to an accumulated dose of 100 kGy [
6]. In this same study, the limited RIA temperature dependence of the F-doped fiber is explained by the invariance of the defect generation rate with temperature. The main defect contributors are identified as two precursor sites from the drawing processes and one from the matrix [
6].
The SMF28e+ fiber exhibited the highest RIA temperature sensitivity [
6], with RIA level differences of 2055 dB/km at 1310 nm, 878 dB/km at 1550 nm and 736 dB/km at 1625 nm between +80 °C and −80 °C. This high RIA vulnerability increased at lower wavelengths. In fact, in the NIR region, Kashaykin et al. [
17] suggested that the GeY color center is the main defect responsible for the absorption of low-Ge-dopant-concentration optical fibers such as SMF28e+. Even though this defect structure remains unknown, its concentration behavior with the temperature of irradiation has been identified in [
17], showing an increase in the GeY-related attenuation with decreasing temperature. In addition, it is known that the GeY absorption band is centered at 1.38 eV (~898 nm) with a Full-Width Half Maximum (FWHM) of 0.71 eV [
24]. In the NIR domain, for low-Ge-doped fibers such as the SMF28e+, RIA levels and kinetics mainly depend on the GeY defect concentration behavior, having a high sensitivity to temperature and being responsible for the high RIA temperature sensitivity. In addition, both RIA levels and their temperature sensitivities decrease at higher wavelengths due to the reduction in the GeY center contribution.
Increasing the GeO
2 dopant percentage in the fiber core has been shown to increase the GeX and decrease the GeY concentrations during the irradiation [
17]. For highly Ge-doped fibers, such as our CMS fiber, the RIA depends on both GeY and GeX defects in the NIR domain. This same study showed that GeX-related RIA contribution decreases with temperature. In addition, the contribution of GeY reduces for a higher dopant concentration in the fiber core. We observed a drastic diminution of the RIA temperature sensitivity for the CMS samples in the NIR domain due to the increase in the GeX concentration and the reduced contribution of the GeY center. Results exhibited no major RIA temperature dependency on CMS samples but a higher sensitivity for higher wavelengths. In fact, at higher wavelengths, the contribution of the GeX spectral band, centered at 2.6 eV (~477 nm) with a FWHM of 0.71 eV, decreased, and the GeY band became preponderant, inducing a higher temperature sensitivity in the NIR domain.
3.2. Brillouin Gain Attenuation
BGS was acquired using a conventional BOTDA in order to perform online measurement as described in
Section 2.2. The procedure outlined in
Section 2.4 enables monitoring of the peak amplitude evolution throughout both the irradiation and recovery phases.
Figure 5 presents the Brillouin peak amplitude over accumulated dose and time for the three tested fibers at −80 °C, −40 °C, +20 °C and +80 °C. Brillouin spectrum measurements were conducted under identical conditions to the RIA experiments, although during separate irradiation runs.
The Brillouin spectrum’s amplitude decreases with the accumulated dose. As for the RIA procedure, radiation-induced absorption bands are generated in the fiber core and cladding due to X-rays exposure. Consequently, the counter-propagating pump pulse, CW probe of the BOTDA interrogator and the backscattered signal from the sample are affected by RIA. This process results in a decrease in the BGS amplitude over the accumulated dose. The fiber composition changes the sensitivity of the sample to BGS attenuation due to the dopant-related defects’ absorption bands in the fiber core and cladding. All three tested fibers with different dopant types and concentrations presented different Brillouin gain attenuation behaviors under the same irradiation conditions. The evolution of the Brillouin peak amplitude under irradiation depends on both linear losses due to RIA effects and Brillouin central gain (
). The latter depends on both the refractive index profile (RIP) and Acoustic Velocity Profile (AVP) along the fiber core and cladding [
26], defined as:
where
and
are the effective refractive index of the guided mode and the effective acoustic velocity in the core, respectively,
is the pump wavelength,
is the density of the fiber core, E is Young’s modulus,
is the Poisson number and
is the electro-strictive constant in the core. The modification of the fiber matrix under irradiation by the introduction of point defects in the core and cladding results in a change of the acoustic velocity and the refractive index [
27,
28].
Figure 5 shows the combined effects of the dopant nature and the temperature of irradiation for the three tested fibers, which exhibited a similar behavior with RIA. The Brillouin gain of the slightly Ge-doped fiber (SMF28e+) exhibited a high temperature dependence, experiencing a gain attenuation of 32% at +80 °C and 90% loss at −80 °C compared to non-irradiated samples. The gain of the highly Ge-doped CMS fiber showed no temperature dependence up to 108 kGy(SiO
2), experiencing 50% gain attenuation for all tested temperatures. Given that the primary factor contributing to Brillouin gain loss is RIA, similar behaviors were observed such as: the loss increases at lower temperature, the stabilization effect of the temperature dependence for the highly Ge-doped fiber core, as described in
Section 3.1, and the effect of the dopant nature. In fact, Ge-doped fibers exhibited higher gain losses than F-doped fibers due to their spectral absorption bands in the NIR domain, inducing greater RIA. The F-doped fiber exhibited low Brillouin gain irradiation temperature sensitivity from 12% losses at +80 °C to 20% losses at −80 °C compared to pristine samples. As the temperature decreases, the efficiency of thermal annealing diminishes and the Brillouin gain exhibits higher attenuation at −80 °C. Since the Brillouin gain attenuation is subjected to RIA, refractive index and acoustic velocity changes, it is not possible yet to decorrelate the contribution of each phenomenon to Brillouin gain attenuation.
3.3. Radiation-Induced Brillouin Frequency Shift
X-ray irradiation not only affects losses in the fiber and Brillouin gain losses, but also induces a BFS. The Lorentz–Lorenz equation for molecular refractivity links the refractive index change to the density change [
27,
29], showing a linear increase in the refractive index change with the density. On the other hand, the Kramers–Kronig equation links an increase in the refractive index change to an increase in the RIA. For X-rays exposure up to 108 kGy(SiO
2) absorbed dose, no significant densification or dilatation are expected [
11]. No particular relation between X-ray irradiation and a silica-based glass compaction has been demonstrated, but a significant effect from γ-rays on Ge-doped fibers irradiated at 13 MGy(H
2O) [
30] has been reported, showing a positive refractive index change of
.
A significant RI-BFS at this dose level can then be seen as a multi-contribution of the refractive index change due to RIA, a change in the acoustic velocity due to Young’s modulus or a change in the Poisson coefficient respective to relations (3) and (4).
where
is the Brillouin central peak frequency depending on the effective refractive index, the effective acoustic velocity and the pump wavelength.
Figure 6 shows the RI-BFS evolution as a function of the accumulated dose up to 108 kGy(SiO
2) at −80 °C, −40 °C, +20 °C and +80 °C for the three tested fiber samples. The presented results have to be considered with a ±0.4 MHz uncertainty margin resulting from temperature variations inside the irradiation chamber, which can become critical when differentiating low RI-BFS levels. The sole contribution of X-rays to BFS was obtained from the measured BFS temperature correction procedure described in
Section 2.4. The overall behavior was similar to the RIA and Brillouin gain loss behaviors. Larger BFS were found at lower temperatures for all tested fibers. SMF28e+ demonstrated the highest RI-BFS at −80 °C, reaching up to 6.8 MHz, and, at +80 °C, it achieved 0.6 MHz. For a higher Ge dopant concentration, the CMS fiber exhibited a lower temperature of irradiation sensitivity, experiencing a 4.2 MHz RI-BFS at −80 °C and a 1.4 MHz RI-BFS at +80 °C. Concerning the F-doped fiber, no RI-BFS could be seen from +80 °C to −40 °C, whereas, as for the RIA and BGS losses, the F-doped fiber exhibited a particular temperature sensitivity, experiencing an RI-BFS of 1.8 MHz at −80 °C only. For low temperatures, the known radiation-hardened F-doped fiber reaches equivalent RI-BFS levels to a Ge-doped fiber at room temperature.
The radiation-induced frequency shift temperature sensitivity was reduced for a higher GeO2 dopant concentration between the SMF28e+ and CMS samples. Having a more major contribution of the RIA to the refractive index change than the density has to both the refractive index and acoustic velocity, the main contribution to the RI-BFS is the RIA through the Kramers–Kronig dispersion relation. The RI-BFS did not present any particular recovery after irradiation for all tested temperature from −80 °C to +80 °C.
A systematic frequency measurement error is induced under irradiation due to RI-BFS, leading to temperature and strain systematic errors when used as a sensor. This systematic error depends on both the fiber composition and the temperature of irradiation, as shown in
Figure 6. After the 108 kGy(SiO
2) accumulated dose, temperature- and strain-related radiation-induced errors from −80 °C to +80 °C were as presented in
Table 2. The F-doped fiber exhibited the lowest temperature and strain radiation-induced errors with no errors for temperatures higher than −40 °C.
3.4. Post Mortem Results
Post-irradiation temperature and strain Brillouin sensitivity measurements were performed for the three tested fibers irradiated up to 108 kGy(SiO
2) at −80 °C, −40 °C, +20 °C and +80 °C. Temperature and strain measurements were performed following the procedure described in
Section 2.3.
It has been shown that increasing the GeO
2 dopant weight percentage in the fiber core reduced the fiber Brillouin central peak temperature and strain sensitivities [
31], reaching about a −1.48% and −1.61% decrease for 1 mol% of dopant measured on a 3 mol% and 8 mol% GeO
2-doped fiber, respectively [
32]. It was also reported that the Brillouin central frequency depends on the molar concentration, with shifts of −87.3 MHz/mol% at 1550 nm [
32] and −97 MHz/wt% at 1320 nm [
31].
Results are presented in
Figure 7 and corroborate the behaviors of both
and
from the previous studies presented above concerning GeO
2 doping effects.
Figure 7 reveals no particular temperature of irradiation dependency after X-ray exposure from −80 °C to +80 °C for either F-doped or CMS samples within the measurement uncertainties. A higher temperature dependence of the
radiation response can be seen for the SMF28e+ sample, exhibiting a decrease of 3.6% between +80 °C and −80 °C. Knowing that
decreases with the absorbed doses for slightly GeO
2-doped fibers [
22], a tendency for lower temperatures can be seen where the thermal annealing is less efficient. However, this last result is very close to the measurement uncertainties.
Post-irradiation measurements showed no particular irradiation temperature dependence for all three tested fiber types from −80 °C to +80 °C, after 108 kGy(SiO2) X-rays exposure, within our measurement uncertainties. Both and are not affected by the irradiation temperature in the investigated range and uncertainties associated with our experimental setup. Compared to pristine fibers, no significant modification of either sensitivity was found for the irradiated tested samples considering uncertainty margins.
4. Discussion
The presented results show and explain the RIA behavior between −80 °C to +80 °C on a F-doped fiber and two differently doped germanosilicate optical fibers. This work explains the origin of the discrepancies between the tested samples in terms of their temperature of irradiation sensitivity, with the help of previous studies, focusing on spectral analysis of defect creation under irradiation and their contributions to RIA. The same procedure is applied to the BGS amplitude decrease, exhibiting the same temperature of irradiation sensitivity response as RIA for all tested fibers. According to this study, the temperature of irradiation differently impacts the sensing capabilities in terms of RIA and BGS losses, showing a dependence on the fiber dopant in terms of nature and concentration. The irradiation temperature sensitivity is reduced, increasing the Ge dopant concentration, its effect being negligible for the highly Ge-doped fiber between +80 °C and −40 °C.
The Brillouin central peak attenuation due to radiation exposure can lead to a drastic reduction in the sensing length from several tens of kilometers for pristine to ten meters for the most sensitive fiber SMF28e+ at −80 °C after 108 kGy accumulated dose. The temperature of irradiation is a hot topic when designing Brillouin sensing techniques to ensure an accurate measurement during the entire exposure preponderant for two-ended Brillouin sensing techniques. Even though BGS losses and RIA exhibit the same behavior, the combined temperature and irradiation effects on the gain (relation (2)) should not be neglected for high accumulated doses. In fact, the RIA impacts the gain as well as the radiation-induced refractive index change and acoustic velocity. RIA mainly contributes to both Brillouin gain losses (through light propagation of both pump and signals) and the refractive index change (through the Kramers–Kronig dispersion relation [
29]). Moreover, the densification of the fiber matrix can contribute to a refractive index change through the Lorentz–Lorenz relation [
29], but a significant effect would require higher accumulated doses (especially under neutron irradiation).
Desensitizing an optical fiber to its temperature of irradiation in a certain temperature range, as for the CMS fiber, can improve the calibration phase, regulating the expected losses for RIA and Brillouin responses. In addition, using an irradiation-temperature-desensitized fiber helps to correct the systematic temperature or strain measurement errors induced by the RI-BFS, which remains unchanged for any considered temperature of irradiation. In the context of nuclear-waste-monitoring Brillouin-based sensing [
1], this type of fiber would present many advantages in terms of calibration of systematic errors and losses for a long exposure period in a temperature-varying environment. For such an application, an interesting procedure would be to design an irradiation-temperature-immune optical fiber. The F-doped fiber would satisfy these requirements concerning Brillouin sensing in the temperature range from −40 °C to +80 °C and +20 °C to +80 °C in terms of RIA control in a temperature-varying environment.
Deeper investigations into the origin of the RI-BFS and contributions to Brillouin gain losses during irradiation require accurate measurements of acoustic velocities before and after irradiation as well as the refractive index profile.