ترغب بنشر مسار تعليمي؟ اضغط هنا

Isoelectronic series of oxygen deficient centers in silica: experimental estimation of homogeneous and inhomogeneous spectral widths

428   0   0.0 ( 0 )
 نشر من قبل Michele D'Amico
 تاريخ النشر 2008
  مجال البحث فيزياء
والبحث باللغة English




اسأل ChatGPT حول البحث

We report nanosecond time-resolved photoluminescence measurements on the isoelectronic series of oxygen deficient centers in amorphous silica, Si-ODC(II), Ge-ODC(II) and Sn-ODC(II) which are responsible of fluorescence activities at $sim$4 eV under excitation at $sim$5 eV. The dependence of the first moment of their emission band on time, and that of the radiative decay lifetime on emission energy are analyzed within a theoretical model able to describe the effects introduced by disorder on the optical properties of the defects. We obtain separate estimates of the homogeneous and inhomogeneous contributions to the measured emission linewidth and we derive homogeneous spectroscopic features of the investigated point defects (Huangh-Rhys factor, homogeneous width, oscillator strength, vibrational frequency). The results point to a picture in which an oxygen deficient center localized on a heavier atom features a higher degree of inhomogeneity due to stronger local distortion of the surrounding matrix. For Si, Ge, Sn related defects the parameter $lambda$, able to quantify inhomogeneity, results to be 65, 78 and 90$%, respectively.

قيم البحث

اقرأ أيضاً

The article describes an experimental method that allows to estimate the inhomogeneous and homogeneous linewidths of the photoluminescence band of a point defect in an amorphous solid. We performed low temperature time-resolved luminescence measureme nts on two defects chosen as model systems for our analysis: extrinsic Oxygen Deficient Centers (ODC(II)) in amorphous silica and F+ 3 centers in crystalline Lithium Fluoride. Measurements evidence that only defects embedded in the amorphous matrix feature a dependence of the radiative decay lifetime on the emission energy and a time dependence of the first moment of the emission band. A theoretical model is developed to link these properties to the structural disorder typical of amorphous solids. Specifically, the observations on ODC(II) are interpreted by introducing a gaussian statistical distribution of the zero phonon line energy position. Comparison with the results obtained on F+ 3 crystalline defects strongly confirms the validity of the model. By analyzing experimental data within this frame, we obtain separate estimations of the homogenous and inhomogeneous contributions to the measured total linewidth of ODC(II), which results to be mostly inhomogeneous.
New temperature dependent inelastic x-ray (IXS) and Raman (RS) scattering data are compared to each other and with existing inelastic neutron scattering data in vitreous silica (v-SiO_2), in the 300 - 1775 K region. The IXS data show collective propa gating excitations up to Q=3.5 nm^-1. The temperature behaviour of the excitations at Q=1.6 nm^-1 matches that of the boson peak found in INS and RS. This supports the acoustic origin of the excess of vibrational states giving rise to the boson peak in this glass.
We report time-resolved photoluminescence spectra of point defects in amorphous silicon dioxide (silica), in particular the decay kinetics of the emission signals of extrinsic Oxygen Deficient Centres of the second type from singlet and directly-exci ted triplet states are measured and used as a probe of structural inhomogeneity. Luminescence activity in sapphire ($alpha$-Al$_2$O$_3$) is studied as well and used as a model system to compare the optical properties of defects in silica with those of defects embedded in a crystalline matrix. Only for defects in silica, we observe a variation of the decay lifetimes with emission energy and a time dependence of the first moment of the emission bands. These features are analyzed within a theoretical model with explicit hypothesis about the effect introduced by the disorder of vitreous systems. Separate estimations of the homogenous and inhomogeneous contributions to the measured emission linewidth are obtained: it is found that inhomogeneous effects strongly condition both the triplet and singlet luminescence activities of oxygen deficient centres in silica, although the degree of inhomogeneity of the triplet emission turns out to be lower than that of the singlet emission. Inhomogeneous effects appear to be negligible in sapphire.
We computer model a free-standing vitreous silica bilayer which has recently been synthesized and characterized experimentally in landmark work. Here we model the bilayer using a computer assembly procedure that starts from a single layer of amorphou s graphene, generated using a bond switching algorithm from an initially crystalline graphene structure. Next each bond is decorated with an oxygen atom and the carbon atoms are relabeled as silicon. This monolayer can be now thought of as a two dimensional network of corner sharing triangles. Next each triangle is made into a tetrahedron, by raising the silicon atom above each triangle and adding an additional singly coordinated oxygen atom at the apex. The final step is to mirror reflect this layer to form a second layer and then attach the two layers together to form the bilayer. We show that this vitreous silica bilayer has the additional macroscopic degrees of freedom to easily form a network of identical corner sharing tetrahedra if there is a symmetry plane through the center of the bilayer going through the layer of oxygen ions that join the upper and lower layers. This has the consequence that the upper rings lie exactly above the lower rings, which are tilted in general. The assumption of a network of perfect corner sharing tetrahedra leads to a range of possible densities that we have previously characterized in three dimensional zeolites as a flexibility window. Finally, using a realistic potential, we have relaxed the bilayer to determine the density, and other structural characteristics such as the Si-Si pair distribution functions and the Si-O-Si bond angle distribution, which are compared to the experimental results obtained by direct imaging.
86 - R. DellAnna 1998
We report a molecular dynamics simulation study of the sound waves in vitreous silica in the mesoscopic exchanged momentum range. The calculated dynamical structure factors are in quantitative agreement with recent experimental inelastic neutron and x-ray scattering data. The analysis of the longitudinal and transverse current spectra allows to discriminate between opposite interpretations of the existing experimental data in favour of the propagating nature of the high frequency sound waves.
التعليقات
جاري جلب التعليقات جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
mircosoft-partner

هل ترغب بارسال اشعارات عن اخر التحديثات في شمرا-اكاديميا