A novel coupled RPL/OSL system to understand the dynamics of the metastable states

Metastable states form by charge (electron and hole) capture in defects in a solid. They play an important role in dosimetry, information storage, and many medical and industrial applications of photonics. Despite many decades of research, the exact mechanisms resulting in luminescence signals such as optically/thermally stimulated luminescence (OSL or TL) or long persistent luminescence through charge transfer across the metastable states remain poorly understood. Our lack of understanding owes to the fact that such luminescence signals arise from a convolution of several steps such as charge (de)trapping, transport and recombination, which are not possible to track individually. Here we present a novel coupled RPL(radio-photoluminescence)/OSL system based on an electron trap in a ubiquitous, natural, geophotonic mineral called feldspar (aluminosilicate). RPL/OSL allows understanding the dynamics of the trapped electrons and trapped holes individually. We elucidate for the first time trap distribution, thermal eviction, and radiation-induced growth of trapped electron and holes. The new methods and insights provided here are crucial for next generation model-based applications of luminescence dating in Earth and environmental sciences, e.g. thermochronometry and photochronometry.Comment: Manuscript accepted in Scientific Reports (https://www.nature.com/srep/

Optical dating in a new light: A direct, non-destructive probe of trapped electrons

Abstract Optical dating has revolutionized our understanding of Global climate change, Earth surface processes, and human evolution and dispersal over the last ~500 ka. Optical dating is based on an anti-Stokes photon emission generated by electron-hole recombination within quartz or feldspar; it relies, by default, on destructive read-out of the stored chronometric information. We present here a fundamentally new method of optical read-out of the trapped electron population in feldspar. The new signal termed as Infra-Red Photo-Luminescence (IRPL) is a Stokes emission (~1.30 eV) derived from NIR excitation (~1.40 eV) on samples previously exposed to ionizing radiation. Low temperature (7–295 K) spectroscopic and time-resolved investigations suggest that IRPL is generated from excited-to-ground state relaxation within the principal (dosimetry) trap. Since IRPL can be induced even in traps remote from recombination centers, it is likely to contain a stable (non-fading), steady-state component. While IRPL is a powerful tool to understand details of the electron-trapping center, it provides a novel, alternative approach to trapped-charge dating based on direct, non-destructive probing of chronometric information. The possibility of repeated readout of IRPL from individual traps will open opportunities for dating at sub-micron spatial resolution, thus, marking a step change in the optical dating technology

OSL-thermochronometry of feldspar from the KTB borehole, Germany

The reconstruction of thermal histories of rocks (thermochronometry) is a fundamental tool both in Earth science and in geological exploration. However, few methods are currently capable of resolving the low-temperature thermal evolution of the upper ∼2 km of the Earth's crust. Here we introduce a new thermochronometer based on the infrared stimulated luminescence (IRSL) from feldspar, and validate the extrapolation of its response to artificial radiation and heat in the laboratory to natural environmental conditions. Specifically, we present a new detailed Na-feldspar IRSL thermochronology from a well-documented thermally-stable crustal environment at the German Continental Deep Drilling Program (KTB). There, the natural luminescence of Na-feldspar extracted from twelve borehole samples (0.1–2.3 km depth, corresponding to 10–70 °C) can be either (i) predicted within uncertainties from the current geothermal gradient, or (ii) inverted into a geothermal palaeogradient of 29±2 °C km−1, integrating natural thermal conditions over the last ∼65 ka. The demonstrated ability to invert a depth–luminescence dataset into a meaningful geothermal palaeogradient opens new venues for reconstructing recent ambient temperatures of the shallow crust (200 °C Ma−1 range). Although Na-feldspar IRSL is prone to field saturation in colder or slower environments, the method's primary relevance appears to be for borehole and tunnel studies, where it may offer remarkably recent (<0.3 Ma) information on the thermal structure and history of hydrothermal fields, nuclear waste repositories and hydrocarbon reservoirs

Testing the performance of an EMCCD camera in measuring single-grain feldspar (thermo)luminescence in comparison to a laser-based single-grain system

Risø laser-based luminescence readers (XY) are well-established in measuring single-grain luminescence for dating and tracing purposes. The use of novel EMCCD cameras is upcoming within the luminescence community, but not common practice yet. In this study we optimize Risø EMCCD camera system settings for detecting single-grain feldspar luminescence and compare system performance to the XY system. We suggest approaches to avoid quartz window staining (which may cause blurred EMCCD images), and to remove Bremsstrahlung-induced spikes from EMCCD-derived decay curves. We show that aperture size has little effect on signal intensity and crosstalk, and that a signal integration Region Of Interest (ROI) of 450 μm diameter provides a good trade-off regarding signal intensity and crosstalk. Our comparison of the XY and EMCCD systems shows that the detection sensitivity and grain acceptance of both systems is similar in measuring feldspar grains. Furthermore, we demonstrate that the EMCCD system allows automated detection of single-grain feldspar thermoluminescence signals, providing new opportunities for sediment tracing and mineral identification.</p

Passive atomic-scale optical sensors for mapping light flux in ultra-small cavities

Abstract Understanding light propagation and attenuation in cavities is limited by lack of applicable light sensing technologies. Here we demonstrate the use of light-sensitive metastable states in wide bandgap aluminosilicates (feldspar) as passive optical sensors for high-resolution mapping of light flux. We develop non-destructive, infrared photoluminescence (IRPL) imaging of trapped electrons in cracks as thin as 50 µm width to determine the spatio-temporal evolution of light sensitive metastable states in response to light exposure. Modelling of these data yields estimates of relative light flux at different depths along the crack surfaces. Contrary to expectation, the measured light flux does not scale with the crack width, and it is independent of crack orientation suggesting the dominance of diffused light propagation within the cracks. This work paves way for understanding of how light attenuates in the minutest of cavities for applications in areas as diverse as geomorphology, biology/ecology and civil engineering

Do attenuation coefficients based on luminescence bleaching fronts reflect true light attenuation in rocks?

The emerging technique of rock surface luminescence dating employs a double-exponential fitting dating model based on the Bouguer-Lambert law. The accuracy of exposure age determination is sensitive to the light attenuation coefficient, μ, which is usually derived from fitting the luminescence profile as a function of depth into the rock. Alternatively, μ might be determined by direct measurement using a spectrophotometer. However, their directly measured values of μ were significantly larger than those estimated from field luminescence bleaching data. Here, we aim to confirm these previous results by measuring the luminescence-depth profiles of both IRSL and IRPL signals from granite rock exposed to different light sources, including sunlight, SOL2 and IR LEDs under controlled conditions. We also measured monochromatic light (blue LED: (470 ± 30) nm, green LED: (520 ± 30) nm, and infrared LED: (850 ± 30) nm) attenuation in granite rock slices of varying thickness (0.62–2.60 mm) using a high-sensitivity photodiode. Finally, we use a camera-based measurement system and a Risø Luminescence Imager to investigate spatial variation in transmitted light as a function of slice thickness. The spatial correlation between direct light transmission and luminescence emission is then investigated, to investigate the underlying reasons for the difference between direct measurement and luminescence-based estimates of μ. We find that light attenuation through a granite rock slice is very heterogeneous; most light penetrates through localized low attenuation light paths corresponding to transmission through the most transparent grains, presumably quartz. The light penetration and escape into the surrounding matrix are assumed to be influenced by the surface area of quartz grains. As a result, transmissive light paths result in a significant area of feldspar grains at depth in the slice being exposed to more light than might be expected from average attenuation measurement. When the incident light predominantly travels through feldspar minerals, simultaneously stimulating luminescence from within any potassium feldspar (K-feldspar), the attenuation coefficients derived from the luminescence-depth profiles tend to be smaller than the average of 1.18 ± 0.07 (n = 79) irrespective of the kinetic model used for fitting. Thus, luminescence-based attenuation coefficient estimates appear to be affected by the distribution of light attenuation across and within the rock slice, making such estimates preferable to directly measured (average) estimates of light attenuation coefficients. These insights are important for our understanding of the significance of light attenuation coefficients in rock samples; they contribute to the reassessment of parameters and measurement methods in dating models and so to improvements in accuracy of rock surface luminescence dating techniques.</p