ترغب بنشر مسار تعليمي؟ اضغط هنا

A general moment NRIXS approach to the determination of equilibrium Fe isotopic fractionation factors: application to goethite and jarosite

117   0   0.0 ( 0 )
 نشر من قبل Nicolas Dauphas
 تاريخ النشر 2012
  مجال البحث فيزياء
والبحث باللغة English




اسأل ChatGPT حول البحث

We measured the reduced partition function ratios for iron isotopes in goethite FeO(OH), potassium-jarosite KFe3(SO4)2(OH)6, and hydronium-jarosite (H3O)Fe3(SO4)2(OH)6, by Nuclear Resonant Inelastic X-Ray Scattering (NRIXS, also known as Nuclear Resonance Vibrational Spectroscopy -NRVS- or Nuclear Inelastic Scattering -NIS) at the Advanced Photon Source. These measurements were made on synthetic minerals enriched in 57Fe. A new method (i.e., the general moment approach) is presented to calculate {beta}-factors from the moments of the NRIXS spectrum S(E). The first term in the moment expansion controls iron isotopic fractionation at high temperature and corresponds to the mean force constant of the iron bonds, a quantity that is readily measured and often reported in NRIXS studies.



قيم البحث

اقرأ أيضاً

A new experimental method of determination of equilibrium isotopic properties of substances based on Inelastic Neutron Scattering (INS) is proposed. We present mathematical formalism allowing calculation of beta-factor of single-element solids based on INS-derived Phonon Density of States (PDOS). PDOS data for nanodiamonds of widely different sizes and of macroscopic diamond were determined from Inelastic Neutron Scattering experiment. This allowed determination of heat capacities and, for the first time, b{eta}-factors for the diamond nanoparticles. We demonstrate considerable size-dependent increase of the heat capacities and decrease of the beta-factors for nanodiamonds relative to bulk diamond. Contributions of surface impurities/phases and phonon confinement to the size effects are evaluated. Applications to formation of diamond nanoparticles in nature are briefly discussed.
We introduce an approach to exploit the existence of multiple levels of description of a physical system to radically accelerate the determination of thermodynamic quantities. We first give a proof of principle of the method using two empirical inter atomic potential functions. We then apply the technique to feed information from an interatomic potential into otherwise inaccessible quantum mechanical tight-binding calculations of the reconstruction of partial dislocations in silicon at finite temperature. With this approach, comprehensive ab initio studies at finite temperature will now be possible.
We present a method to compute optical spectra and exciton binding energies of molecules and solids based on the solution of the Bethe-Salpeter equation (BSE) and the calculation of the screened Coulomb interaction in finite field. The method does no t require the explicit evaluation of dielectric matrices nor of virtual electronic states, and can be easily applied without resorting to the random phase approximation. In addition it utilizes localized orbitals obtained from Bloch states using bisection techniques, thus greatly reducing the complexity of the calculation and enabling the efficient use of hybrid functionals to obtain single particle wavefunctions. We report exciton binding energies of several molecules and absorption spectra of condensed systems of unprecedented size, including water and ice samples with hundreds of atoms.
We review a series of works where the fundamental master equation is used to develop a microscopical description of evolution of non-equilibrium atomic distributions in alloys. We describe exact equations for temporal evolution of local concentration s and their correlators as well as approximate methods to treat these equations, such as the kinetic mean-field and the kinetic cluster methods. We also describe an application of these methods to studies of kinetics of L1_0 type orderings in FCC alloys which reveal a number of peculiar microstructural effects, many of them agreeing well with experimental observations.
410 - Fujun Du , Berengere Parise 2011
[Context] The stochasticity of grain chemistry requires special care in modeling. Previously methods based on the modified rate equation, the master equation, the moment equation, and Monte Carlo simulations have been used. [Aims] We attempt to devel op a systematic and efficient way to model the gas-grain chemistry with a large reaction network as accurately as possible. [Methods] We present a hybrid moment equation approach which is a general and automatic method where the generating function is used to generate the moment equations. For large reaction networks, the moment equation is cut off at the second order, and a switch scheme is used when the average population of certain species reaches 1. For small networks, the third order moments can also be utilized to achieve a higher accuracy. [Results] For physical conditions in which the surface reactions are important, our method provides a major improvement over the rate equation approach, when benchmarked against the rigorous Monte Carlo results. For either very low or very high temperatures, or large grain radii, results from the rate equation are similar to those from our new approach. Our method is faster than the Monte Carlo approach, but slower than the rate equation approach. [Conclusions] The hybrid moment equation approach with a cutoff and switch scheme is applicable to large gas-grain networks, and is accurate enough to be used for astrochemistry studies. The layered structure of the grain mantle could also be incorporated into this approach, although a full implementation of the grain micro-physics appears to be difficult.
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