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1.
Synthetic ZrSiO4 and (mildly to strongly radiation-damaged) natural zircon samples were irradiated with 8.8 MeV 4He2+ ions (fluences in the range 1 × 1013–5 × 1016 ions/cm2). For comparison, an additional irradiation experiment was done with 30 MeV 16O6+ ions (fluence 1 × 1015 ions/cm2). The light-ion irradiation resulted in the generation of new (synthetic ZrSiO4) or additional (mildly to strongly metamict natural samples) damage. The maximum extent of the damage is observed in a shallow depth range approximately 32–33 μm (8.8 MeV He) and ~12 μm (30 MeV O) below the sample surface, i.e. near the end of the ion trajectories. These depth values, and the observed damage distribution, correspond well to defect distribution patterns as predicted by Monte Carlo simulations. The irradiation damage is recognised from the notable broadening of Raman-active vibrational modes, lowered interference colours (i.e. decreased birefringence), and changes in the optical activity (i.e. luminescence emission). At very low damage levels, a broad-band yellow emission centre is generated whereas at elevated damage levels, this centre is suppressed and samples experience a general decrease in their emission intensity. Most remarkably, there is no indication of notable structural recovery in pre-damaged natural zircon as induced by the light-ion irradiation, which questions the relevance of alpha-assisted annealing of radiation damage in natural zircon.  相似文献   

2.
Cathodoluminescence (CL) spectra of unirradiated, He+ ion-implanted and electron-irradiated plagioclase minerals contain the following emission bands: (1) below 300 nm due to Pb2+, (2) at ~320 and ~350 nm to Ce3+, (3) at 380–420 nm to Eu2+, Ti4+ and/or Al–O?–Al/Ti defects, (4) at 560–580 nm to Mn2+ and (5) at 720–760 nm to Fe3+. During the implantation of He+ ion, much of their energy may be dissipated by partial destruction and strain of the feldspar framework, resulting in quenching of CL. Deconvolution of CL spectra acquired from albite and oligoclase reveals an emission component at 1.86 eV (666 nm) assigned to a radiation-induced defect center associated with Na+ atoms. As its intensity increases with radiation dose, this emission component has potential for geodosimetry and geochronometry. Electron irradiation causes Na+ migration in plagioclase, and then a considerable reduction in intensity of emissions assigned to impurity centers, which is responsible for an alteration in the energy state or a decrease in luminescence efficiency following the change of activation energy. Emission intensity at 1.86 eV positively correlates with electron irradiation time for unimplanted and He+ ion-implanted albite and oligoclase, but negatively for the implanted albite above 1.07 × 10?4 C/cm2. It implies that radiation halo produced by α-particles should not be measured using CL spectroscopy to estimate β radiation dose on albite in the high radiation level.  相似文献   

3.
In this paper, possibilities and limits of the application of REE3+ luminescence (especially the Nd3+ 4F3/2 → 4I9/2 emission) as structural probe are evaluated. Important factors controlling the Nd3+ luminescence signal are discussed, including effects of the crystal-field, crystal orientation, structural state, and temperature. Particular attention was paid to the study of the accessory minerals zircon (ZrSiO4), xenotime–(Y) (YPO4), monazite–(Ce) (CePO4) and their synthetic analogues. Based on these examples we review in short that (1) REE3+ luminescence can be used as non-destructive phase identification method, (2) the intensities of certain luminescence bands are strongly influenced by crystal orientation effects, and (3) increased widths of REE3+-related emission bands are a strong indicator for structural disorder. We discuss the potential of luminescence spectroscopy, complementary to Raman spectroscopy, for the quantitative estimation of chemical (and potentially also radiation-induced) disorder. For the latter, emissions of Nd3+-related centres are found to be promising candidates.  相似文献   

4.
Field Emission SEM (FESEM) textural observations, crystal size distribution (CSD) analyses, UV-excited luminescence imaging, and photoluminescence (PL) microspectroscopy excited by 488 nm laser were conducted on two texturally contrasting samples of carbonado, a kind of natural polycrystalline diamond from the Central African Republic (CAR). The investigated carbonado samples A and B show extremely different textures: sample A is made up of faceted crystals accompanied by abundant, small rectangular pores, whereas sample B has a granular texture with coarser crystals and scarce, large pores. Diamond crystals smaller than 2–3 µm are enriched in sample A but depleted in sample B. These textural features indicate that sample B diamonds were annealed under thermodynamically stable P–T conditions. The pore characteristics indicate that fluid permeability was higher for sample A than sample B. Photoluminescence (PL) spectra indicate that samples A and B correspond to Group A and B carbonados in the classification of Kagi et al. (1994), respectively, so that sample A reveals emissions from the H3 center without any N–V0 derived emission at 575 nm, whereas sample B shows emissions from the 3H center and the N–V0 defect. In addition, UV-excited luminescence images and photoluminescence spectra for sample B indicate that the rims of diamond crystals within several microns of a pore show luminescence features similar to those of Group AB carbonados (Kagi et al., 1994), indicating that this Group AB material was formed from Group B by irradiation from pore-filling, radioactive-element-bearing materials at a low temperature. The extent of the low-temperature irradiation is considered to depend on fluid permeability, and the Group A material was strongly irradiated due to its permeable texture whereas the Group B material was not significantly irradiated due to its less permeable granular texture. These results indicate that Group B carbonados have retained their original PL spectral features produced under high pressures and temperatures at mantle depths.  相似文献   

5.
The paper summarises new data and results referring to the characterization of the nature of luminescence centres in minerals that were published during the last 8 years. Besides well-established luminescence centres, such as Mn2+, Fe3+, Cr3+, divalent and trivalent rare-earth elements, S2 ?, and Pb2+, several other centres were proposed and substantiated, such as Mn3+, Mn4+, V2+, Ni2+, Pb+, Mn3+, Sb3+, Tl+, and radiation-induced centres. Also, a relatively new type of luminescence excitation mechanism is discussed briefly, namely plasma-induced luminescence. Here, the emission takes place when the matrix, where the formation of plasma is caused by irradiation with a beam of laser light, is capable to luminescence and contains luminescence centres.  相似文献   

6.
The luminescence spectra of a suite of natural sodium framework silicates including four different sodalite variants and tugtupite have been collected during X-ray irradiation as a function of temperature between 20 and 673 K. The origin of the emission bands observed in these samples is attributed to F-centres (360 nm), paramagnetic oxygen defects (400 and 450 nm), S2 ? ions (620 nm) and tetrahedral Fe3+ (730 nm). Luminescence in the yellow (550 nm) is tentatively attributed to Mn2+, and red luminescence in Cr-rich pink sodalite is possibly from Cr3+ activation. Sudden reduction in luminescence intensities of emission centres was observed for all minerals in the 60–120 K range. Since it is common to all the sodalite-group minerals, we infer it is a feature of the aluminosilicate framework. Sodalite luminescence has responses from substitutions on the framework (e.g. paramagnetic oxygen defects, Fe3+) which give sodalite properties akin to other framework silicates such as feldspar and quartz. However, the presence of the sodalite cage containing anions (such as F-centres, S2 ? ions) imparts additional properties akin to alkali halides. The possibility of coupling between Fe3+ and S2 ? is discussed. The overall luminescence behaviour of sodalite group can be understood in terms of competition between these centre types.  相似文献   

7.
The photoluminescence (PL) and optical excitation spectra of baratovite in aegirine syenite from Dara-i-Pioz, Tien Shan Mts., Tajikistan and katayamalite in aegirine syenite from Iwagi Islet, Ehime, Japan were obtained at 300 and 80 K. Under short wave (253.7 nm) ultraviolet light, baratovite and katayamalite exhibited bright blue-white luminescence. The PL spectrum of baratovite at 300 K consisted of a wide band with a peak at approximately 406 nm and a full width at half maximum (FWHM) of approximately 6.32k cm−1. The excitation spectrum of the blue-white luminescence from baratovite at 300 K consisted of a prominent band with a peak at approximately 250 nm. The PL and excitation spectra of katayamalite were similar to those of baratovite. The luminescence from these minerals was attributed to the intrinsic luminescence from the TiO6 center.  相似文献   

8.
It is proved that blue luminescence from benitoite is connected with intrinsic luminescence centers, namely isolated TiO6 octahedra. The metastable level 3T1u is the emitting level at low temperatures with a long decay time of 1.1 ms. At higher temperatures an energy level with higher radiation probability must be involved in the emission process, and this level is situated at 0.06 eV higher than the lowest level. These two levels may be connected with 3T1u level splitting or with closely spaced 3T1u and 3T2u levels. Decay time shortening and thermal quenching are connected with nonradiative decay within the TiO6 luminescence center, while energy migration does not take place at least up to room temperature.  相似文献   

9.
A comparative study of damage accumulation in magnesium aluminate spinel (MgAl2O4) has been conducted using ionoluminescence (IL), cathodoluminescence (CL) and Rutherford Backscattering Spectrometry/channeling (RBS/C) techniques. MgAl2O4 single crystal and polycrystalline samples were irradiated with 320 keV Ar+ ions at fluencies ranging from 1 × 1012 to 2 × 1016 cm?2 in order to create various levels of radiation damage. RBS/C measurements provided quantitative data about damage concentration in the samples. These values were then compared to the luminescence measurements. The results obtained by IL and RBS/C methods demonstrate a two-step character of damage buildup process. The CL data analysis points to the three-step damage accumulation mechanism involving the first defect transformation at fluencies of about 1013 cm?2 and second at about 1015 cm?2. The rate of changes resulting from the formation of nonluminescent recombination centers is clearly nonlinear and cannot be described in terms of continuous accumulation of point defects. Both, IL and CL techniques, appear as new, complementary tools bringing new possibilities in the damage accumulation studies in single- and polycrystalline materials.  相似文献   

10.
We have undertaken a study of the common green or orange-brown spots at the surface of rough diamond specimens, which are caused by alpha particles emanating from radioactive sources outside the diamond. Richly coloured haloes represent elevated levels of structural damage, indicated by strong broadening of the main Raman band of diamond, intense strain birefringence, and up-doming of spots due to their extensive volume expansion. Green radio-colouration was analogously generated through the irradiation of diamond with 8.8 MeV helium ions. The generation of readily visible radio-colouration was observed after irradiating diamond with ≥1015 He ions per cm2. The accumulation of such a high number of alpha particles requires irradiation of the diamond from a radioactive source over long periods of time, presumably hundreds of millions of years in many cases. In the samples irradiated with He ions, amorphisation was observed in volume areas where the defect density exceeded 5 × 10?3 Å?3 (or 0.03 dpa; displacements per target atom). In contrast, graphitisation as a direct result of the ion irradiation was not observed. The green colouration transformed to brown at moderate annealing temperatures (here 450 °C). The colour transformation is associated with only partial recovery of the radiation damage. The colour change is mainly due to the destruction of the GR1 centre, explained by trapping of vacancies at A defects to form the H3 centre. An activation energy of ~2.4 ± 0.2 eV was determined for the GR1 reduction. The H3 centre, in turn, causes intense yellowish-green photoluminescence under ultraviolet illumination. Radio-colouration and associated H3 photoluminescence are due to point defects created by the ions irradiated, whereas lattice ionisation is of minor importance. This is concluded from the depth distribution of the colouration and the photoluminescence intensity (which corresponds to the defect density but not the ionisation distribution pattern). The effect of the implanted He ions themselves on the colour and photoluminescence seems to be negligible, as radio-colouration and H3 emission were analogously produced through irradiation of diamond with C ions. The photoluminescence emission becomes observable at extremely low defect densities on the order of 10?6 Å?3 (or 0.000006 dpa) and is suppressed at moderate defect densities of ~5 × 10?4 Å?3 (or ~0.003 dpa). Intensely brown-coloured diamond hence does not show the H3 emission anymore. Anneals up to 1,600 °C has reduced considerably irradiation damage and radio-colouration, but the structural reconstitution of the diamond (and its de-colouration) was still incomplete.  相似文献   

11.
The orientation dependence of the luminescence of a well-characterized plagioclase crystal at room temperature and 40 K is reported. A beam of H + ions was used to provide the excitation. Ion beam luminescence provides emissions effectively from the bulk of the material, and therefore minimizes the contribution to the luminescence from atypical regions. The intensity of the luminescence is strongly orientation-dependent. The intensity and photon energy, particularly of the red/infrared and yellow emission bands, vary significantly. We interpreted this as resulting from Fe 3+ and Mn 2+ activator ions, respectively, on crystallographic sites with low point symmetry. An emission at 860 nm was also significantly orientation-dependent. The blue luminescence showed the least variability. At room temperature, a 350 nm near-UV emission was noted, whereas at 40 K, emissions were at 240, 260, 300 and 340 nm. UV emissions may result from Na + diffusion along interfaces within the plagioclase, notably albite-law (010) twins. This variability has significant consequences for the use of single-crystal quantitative luminescence techniques. We have also studied the dependence of the peak intensities and profiles during prolonged ion beam bombardment with heavier (He +) ions. Broadening of the red-infrared emission is interpreted as reflecting growing amorphization of the sample.  相似文献   

12.
Chromium-doped titanite and malayaite samples, which were synthesised to evaluate their performance as ceramic pigments, show remarkable photoluminescence behaviour. Emissions of centres related to traces of trivalent rare-earth elements (REE) are observed exclusively from chromium-free samples. Their Cr-doped analogues (containing the same REEs on the same concentration levels), in contrast, only show broad-band Cr3+ emission whereas all REE emissions are suppressed. This behaviour is assigned to quenching of REE emissions by chromium centres (i.e., REE3+ → Cr3+ energy transfer).  相似文献   

13.
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14.
For the first time, the luminescence properties of Pr3+, Nd3+ and Tm3+ and Yb3+ ions in fluorite crystal have been obtained by steady-state measurements. In addition, the luminescence spectra of Ce3+, Sm2+, Sm3+, Dy3+, Er3+ and Yb3+ were measured. It was pointed out that λexc.?=?415?nm is most suitable for measuring the Ho3+ emission beside the Er3+. The emission of trivalent holmium and erbium ions was measured independently using time-resolved measurements and tentative assignment of luminescence lines to C 3v and C 4v symmetry sites was proposed. Besides for natural fluorite crystal, the transitions between Stark energy levels of lanthanide ions were presented.  相似文献   

15.
The study of radiation of intrinsic and impurity excitations in natural barite showed that the patterns of BaSO4 luminescence were mostly controlled by the presence of the [SO4] anion complex. Several types of self-radiation were registered including those at the expense of the presence of O2– ions of the axial and nonaxial configurations of the anionic group (emission bands within the wavelength ranges of 209–213 and 330–350 nm, respectively). Exitons located near the impurity and intrinsic defects largely participate in emission. Impurity defects participating in the luminescent centers of barite from the Ore Altai include Pb2+, Gd3+, Eu2+, Eu3+, Cu+, and Ag+ (under X-ray excitation). Variations in the spectral composition of barite indicate the different conditions of its formation.  相似文献   

16.
Irradiation techniques are often applied to gem minerals for color enhancement purposes. Natural green, blue and colorless specimens of rare gemological quality euclase, BeAlSiO4(OH), from Brazil were irradiated with gamma rays in the dose range from 10 to 500 kGy. Although the colors of the different specimens were not strongly influenced, two different irradiation-induced paramagnetic defect centers were found by electron paramagnetic resonance (EPR). The first one is an O− hole center interacting with one Al neighbor and the second is a Ti3+ electron center. The EPR angular rotation patterns of both irradiation-induced defects were measured and analyzed. The results suggest that O− hole centers are formed by dissociation of the hydroxyl ions, similar as in topaz crystals. In euclase the OH− ions interconnect distorted Al octahedra and Be tetrahedra in O5 positions. During irradiation, the electrons are captured by titanium ions (Ti4+ + e−), leading to the formation of paramagnetic Ti3+ ions. From the EPR rotation patterns it is clear that these ions substitute for Al ions. The spin Hamiltonian parameters of the irradiation-induced defects are analyzed and compared to similar defect centers in other mineral specimens. Thermal annealing experiments show that the O− hole centers and Ti3+ electron centers are directly connected through the radiation process.  相似文献   

17.
Recent work [Shuster D. L., Flowers R. M. and Farley K. A. (2006) The influence of natural radiation damage on helium diffusion kinetics in apatite. Earth Planet. Sci. Lett.249(3-4), 148-161] revealing a correlation between radiogenic 4He concentration and He diffusivity in natural apatites suggests that helium migration is retarded by radiation-induced damage to the crystal structure. If so, the He diffusion kinetics of an apatite is an evolving function of time and the effective uranium concentration in a cooling sample, a fact which must be considered when interpreting apatite (U-Th)/He ages. Here we report the results of experiments designed to investigate and quantify this phenomenon by determining He diffusivities in apatites after systematically adding or removing radiation damage.Radiation damage was added to a suite of synthetic and natural apatites by exposure to between 1 and 100 h of neutron irradiation in a nuclear reactor. The samples were then irradiated with a 220 MeV proton beam and the resulting spallogenic 3He used as a diffusant in step-heating diffusion experiments. In every sample, irradiation increased the activation energy (Ea) and the frequency factor (Do/a2) of diffusion and yielded a higher He closure temperature (Tc) than the starting material. For example, 100 h in the reactor caused the He closure temperature to increase by as much as 36 °C. For a given neutron fluence the magnitude of increase in closure temperature scales negatively with the initial closure temperature. This is consistent with a logarithmic response in which the neutron damage is additive to the initial damage present. In detail, the irradiations introduce correlated increases in Ea and ln(Do/a2) that lie on the same array as found in natural apatites. This strongly suggests that neutron-induced damage mimics the damage produced by U and Th decay in natural apatites.To investigate the potential consequences of annealing of radiation damage, samples of Durango apatite were heated in vacuum to temperatures up to 550 °C for between 1 and 350 h. After this treatment the samples were step-heated using the remaining natural 4He as the diffusant. At temperatures above 290 °C a systematic change in Tc was observed, with values becoming lower with increasing temperature and time. For example, reduction of Tc from the starting value of 71 to ∼52 °C occurred in 1 h at 375 °C or 10 h at 330 °C. The observed variations in Tc are strongly correlated with the fission track length reduction predicted from the initial holding time and temperature. Furthermore, like the neutron irradiated apatites, these samples plot on the same Ea − ln(Do/a2) array as natural samples, suggesting that damage annealing is simply undoing the consequences of damage accumulation in terms of He diffusivity.Taken together these data provide unequivocal evidence that at these levels, radiation damage acts to retard He diffusion in apatite, and that thermal annealing reverses the process. The data provide support for the previously described radiation damage trapping kinetic model of Shuster et al. (2006) and can be used to define a model which fully accommodates damage production and annealing.  相似文献   

18.
Summary Investigations of natural and synthetic quartz specimens by cathodoluminescence (CL) microscopy and spectroscopy, electron paramagnetic resonance (EPR) and trace-element analysis showed that various luminescence colours and emission bands can be ascribed to different intrinsic and extrinsic defects. The perceived visible luminescence colours in quartz depend on the relative intensities of the dominant emission bands between 380 and 700 nm. Some of the CL emissions of quartz from the UV to the yellow spectral region (175 nm, 290 nm, 340 nm, 420 nm, 450 nm, 580 nm) can be related to intrinsic lattice defects. Extrinsic defects such as the alkali (or hydrogen)-compensated [AlO4/M+] centre have been suggested as being responsible for the transient emission band at 380–390 nm and the short-lived blue-green CL centered around 500 nm. CL emissions between 620 and 650 nm in the red spectral region are attributed to the nonbridging oxygen hole centre (NBOHC) with several precursors. The weak but highly variable CL colours and emission spectra of quartz can be related to genetic conditions of quartz formation. Hence, both luminescence microscopy and spectroscopy can be used widely in various applications in geosciences and techniques. One of the most important fields of application of quartz CL is the ability to reveal internal structures, growth zoning and lattice defects in quartz crystals not discernible by means of other analytical techniques. Other fields of investigations are the modal analysis of rocks, the provenance evaluation of clastic sediments, diagenetic studies, the reconstruction of alteration processes and fluid flow, the detection of radiation damage or investigations of ultra-pure quartz and silica glass in technical applications. Zusammenfassung Ursachen, spektrale Charakteristika und praktische Anwendungen der Kathodolumineszenz (KL) von Quarz – eine Revision Untersuchungen von natürlichen und synthetischen Quarzproben mittels Kathodolumineszenz (KL) Mikroskopie und -spektroskopie, Elektron Paramagnetischer Resonanz (EPR) und Spurenelementanalysen zeigen verschiedene Lumineszenzfarben und Emissionsbanden, die unterschiedlichen intrinsischen und extrinsischen Defekten zugeordnet werden k?nnen. Die sichtbaren Lumineszenzfarben von Quarz werden durch unterschiedliche Intensit?tsverh?ltnisse der dominierenden Emissionsbanden zwischen 380 und 700 nm verursacht. Einige der KL Emissionen vom UV bis zum gelben Spektralbereich (175 nm, 290 nm, 340 nm, 420 nm, 450 nm, 580 nm) stehen im Zusammenhang mit intrinsischen Defekten. Die kurzlebigen Lumineszenzemissionen bei 380–390 nm sowie 500 nm werden mit kompensierten [AlO4/M+]-Zentren in Verbindung gebracht. Die KL-Emissionen im roten Spektralbereich bei 620 bis 650 nm haben ihre Ursache im “nonbridging oxygen hole centre” (NBOHC) mit verschiedenen Vorl?uferzentren. Die unterschiedlichen KL-Farben und Emissionsspektren von Quarz k?nnen oft bestimmten genetischen Bildungsbedingungen zugeordnet werden und erm?glichen deshalb vielf?ltige Anwendungen in den Geowissenschaften und in der Technik. Eine der gravierendsten Einsatzm?glichkeiten ist die Sichtbarmachung von Internstrukturen, Wachstumszonierungen und Defekten im Quarz, die mit anderen Analysenmethoden nicht oder nur schwer nachweisbar sind. Weitere wesentliche Untersuchungsschwerpunkte sind die Modalanalyse von Gesteinen, die Eduktanalyse klastischer Sedimente, Diageneseuntersuchungen, die Rekonstruktion von Alterationsprozessen und Fluidmigrationen, der Nachweis von Strahlungssch?den oder die Untersuchung von ultrareinem Quarz und Silikaglas für technische Anwendungen. Received March 29, 2000 Accepted October 27, 2000  相似文献   

19.
This work explores the potential of laser excited luminescence for the study of type and concentration of rare-earth (RE) luminescence centres in CaF2. A comparison with X-ray excited luminescence is made. The luminescence spectra of several natural and synthetic samples are obtained at low and room temperatures using different Ar+ and Kr+ laser lines for excitation. Tentative assignment of the luminescent lines to different RE2+ and RE3+ ions is made. The excitation is shown to take place predominantly through the emission of one phonon. The possibilities for concentration measurements of luminescent centres are discussed.  相似文献   

20.
The stability of synthetic REE-aluminate garnets irradiated by accelerated Kr2+ ions and affected by alpha decay of 244Cm (T1/2 = 18.1 yr) has been studied. The dose of irradiation sufficient for the complete disordering of the aluminate garnet structure is 0.40–0.55 displacements per atom. This value increases with rising temperature due to the increasing intensity of recovery from radiation damage to the lattice by heating. The critical temperature above which the structure of REE-aluminate is not damaged by radiation is 550°C. The amorphization dose for aluminates with garnet structure is two to three times higher than of that previously studied ferrites; the critical temperature of both is similar. In resistance to radiation, aluminate garnets do not yield to zirconolite and exceed titanate pyrochlore. Heating to 250°C does not lead to substantial recovery from radiation defects in the garnet structure. The radiation impact on matrices of real actinide (An) wastes is lower than that related to ion irradiation and 244Cm doping, and this facilitates a higher radiation resistance of garnets containing HLW.  相似文献   

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