Defects, Diffusion, Deformation and Thermal Conductivity in the Lower Mantle and D
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1 Defects, Diffusion, Deformation and Thermal Conductivity in the Lower Mantle and D John Brodholt UCL Thanks to: Michael Ammann, Simon Hunt, James Wookey, Kai Wang, Andrew Walker and David Dobson College de France,
2 Defects and Diffusion is important: Controls chemical exchange between crystalline, melt and fluid phases Degree of composition zoning in minerals Kinetics of phase transitions Rate at which minerals grow and their grain sizes Has a central role in controlling rheology (Deformation) High P & T experiments on diffusion are hard. So our approach is to use a theoretical approach (ab initio or first principles). College de France,
3 Forces are calculated either from First principles - quantum mechanics - or from empirical potentials. College de France,
4 He diffusion in perovskite - the exception. College de France,
5 He diffusion in perovskite - the exception. College de France,
6 Self Diffusion: D sd = AN V e S H k e kt All energies and frequencies obtained from DFT calculations Migration enthalpy: H = E saddlepoint E initial N Attempt frequency and migration entropy (Vineyard Theory) e S k = f i n=1 N 1 f i n=1 College de France,
7 Migration enthalpy of Si diffusion in MgSiO3 perovskite Theory: Wright & Price (1993) = 9.4 ev (empirical potentials) Experiments: Yamazaki et al., (2000) = 3.6 ev Theory: Karki and Khanduja (2007) = 9 ev (DFT) Experiments: Dobson et al, (2008) = 3.7 ev Text College de France,
8 Si Diffusion in Perovskite College de France,
9 Si diffusion in MgSiO3 perovksite Energy [ev] Reaction Coordinate [A] Agreement with experiment (3.6 ev) is better than previous estimates (9 ev) but still not great! College de France,
10 1 6 Six-jump cycle for Si diffusion in MgSiO3 Perovskite College de France,
11 Si diffusion in perovksite does not seem to occur via a simple vacancy hoping mechanism. 4 Silicon Six-Jump Cycle in Perovskite 3 E (ev) Mg1->V Si Si->V Mg Mg2->V Si Mg1 Si ->V Mg Si Mg ->V Si Mg2 Si ->V Mg Apparent activation energy for the total cycle is 3.6 ev. This agrees well with 3.61 ev and 3.5 ev found by Dobson et al. (2008) and Yamazaki et al (2000). College de France,
12 PEROVSKITE DIFFUSION RATES College de France,
13 Absolute Diffusion Rates in MgO LDA GGA College de France,
14 What about other components? Fe2+, Fe3+, Al3+ etc. And in particular the effect of spin transition in Fe. High Spin Low Spin eg eg 0 0 t2g t2g Pressure College de France,
15 High - Low Spin Transition in Ferropericlase College de France, 2012 Wentzcovitch et al. PNAS 2009, 14
16 Low Pressure Saddle point Saddle point HLS Low Spin HHS HLS High Spin HHS Initial state Final state Initial state Final state HLS ~ HHS HLS < HHS College de France,
17 Low Pressure High Pressure Saddle point Saddle point HLS HHS HHS HLS Initial state Final state Initial state Final state HLS < HHS HLS > HHS College de France,
18 = = G2 kt D (Nabbaro-Herring Creep) College de France,
19 Diffusion in post-perovskite College de France,
20 Diffusion in post-perovskite is extremely anisotropic. Si and Mg diffusion in the <100> direction is very fast College de France,
21 Deformation Map for Olivine Don t know deformation map for PPV, but... If diffusion creep, PPV could be several orders of magnitude more viscous that PV. If dislocation creep, PPV could be up to four orders of magnitude weaker than PV - if climb controlled. Katayama, Geology (2012) College de France,
22 What about dislocation creep? Dislocation creep is generally controlled by climb - and this is also a diffusion controlled mechanism. So the much faster diffusion of Si in the [100] direction in postperovskite relative to post-perovskite should make it creep faster too - i.e., post-perovskite should be up to 4 orders of magnitude weaker than perovskite. College de France, 2012
23 Experimental creep rates in transforming CaIrO3 D-DIA X-rays 800 COMPRES beamline at the NSLS Hunt et al, Nature Geoscience 2009 length (pixels) MgO CaIrO Time (s) College de France,
24 Other implications for weak post-perovskite: Cadek and Fleitout (2005) College de France,
25 Is the phase transition too wide to be consistent with a sharp seismic refector? Akber-Knutson et al, (2005) Catalli et al (2009) College de France,
26 College de France, 2012 Ammann, Brodholt, Wookey and Dobson, Nature (2010)
27 Thermal conductivity (k) Energy added Energy removed College de France,
28 College de France,
29 College de France,
30 Flow model Anisotropy (LPO) Conductive heat flow Implications? College de France,
31 Flow Model from Walker et al, 2011 and Simmons et al (2007,2008) College de France,
32 Anisotropy Walker et al (2011) College de France,
33 Total heat flow = 3.5, 4.9, 4.8 TW for three models College de France,
34 Isotropic Anisotropic Does this matter? College de France,
35 College de France,
36 Conclusions Can use ab initio methods to calculate diffusion rates of minerals difficult to measure experimentally Ferro-periclase is much weaker than perovskite throughout the mantle. Spin transition slightly weakens it further. Lower mantle viscosity could be controlled by ferropericlase in areas of high strains. Post-perovskite has very anisotropic diffusion rates and is probably much weaker than perovksite Post-perovskite has somewhat anisotropic conductivity, which may help stabilise plumes. College de France,
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