How to Define Data and Databases for PMI (in ten pieces)
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1 How to Define Data and Databases for PMI (in ten pieces) Predrag Krstić Physics Division, CFADC Oak Ridge National Laboratory Support from: US DOE (OFES and OBES) and ORNL LDRD program for the Department of Energy Improving the Database for Physical And Chemical Sputtering, IAEA, 12/2012
2 Theory: CMD Close collaborators: Mat. PWDFT Stephan Irle, Nagoya U. TBDFT modeling Carlos Reinhold PD, ORNL Steve Stuart Clemson U. Paul Kent ORNL Alain Allouche CNRS, Fr K. Morokuma, Kyoto U. J. Jakowski, NICS H. Witek, Taiwan Experiment: Students Eric (Purdue) Fred Meyer (PD, ORNL) beam Eric Hollmann (UCSD) plasma JP Allain (Purdue) Chase Taylor Purdue) beam and plasma Jae (ORISE) Jonny (UTK) Chris (MTSU) for the 2 Department of Energy Improving the OFES Database Review, for ORNL, Physical March And 02, Chemical 2010 Sputtering, IAEA, 12/2012
3 1. Why PLASMA-MATERIAL INTERFACE is such an important problem? for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
4 All energy from D-T fusion reactions passes through first wall Flux of (particles + heat + 14 MeV neutrons) ~10 MW/m 2 Supercon ducting magnet Schematic magnetic fusion reactor Plasma heating (rf, microwave,...) Turbine generator ITER, DEMO Plasma a Shield Vac. Blanket Unlike nuclear fission where energy is volume-distributed Plasma-material interactions limit performance in present non-dt experiments TORE SUPRA (France) IR image of wall, T max ~ 600 C Visible emission, inner wall for the 4 Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
5 2. Why defining the data for PMI is so difficult problem? 1) Interfacial physics, when the two worlds meet : traditionally the most challenging areas of science 2) It mixes material of the two worlds, creating in between a new entity : P-M DYNAMICAL SURFACE which communicates between the two! 3) Plasma is source of synergistic effects of many energies, angles, particles These are the main causes of the simulation difficulties for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
6 PMI strategy is evolving thru ITER towards DEMO reactor ITER (> 2020) uses multi-matl walls Pulses ~ hundreds of sec ~Be Main chamber wall(700m 2 ) Low Z + oxygen getter ~W Baffle/Dome (100 m 2 ) Funnels exhaust to divertor chamber Low erosion, long lifetime ~ C Divertor Target (50 m 2 ) (Graphite) Minimize high-z impurities (which lead to large radiative losses) Divertor chamber DEMO (> 2030?): Steady-state, power flux ~ 10 MW/m 2 Hot walls (>600 C ) Refractory metals Neutron irradiation 14.1 MeV (> 100 dpa) Parameter range inaccessible in present devices F valid extrapolation needed! for the 6 Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
7 PMI has many fundamental processes & synergies When an ion or neutral arrives at a surface it undergoes a series of elastic and inelastic collisions with the atoms of the solid. elastic reflection trapping/detrapping retention What surface :Chemistry, Mixture, Morphology? diffusion, permeation implantation Drivers: Plasma Material Multi -T, -n, -species, plasma irradiation, re-emission & neutrons sputtering & sheath acceleration chemistry Give rise to synergistic effects Damage Effects: Vacancies, bubbles, blisters, dislocations, voids, neutrons? Erosion Ablation Melting (metals) for the 7 Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012 Re-deposition Co-deposition
8 Example:Chemical Sputtering Function of : -Type (H, H 2, Ar, N, He) - Impinging projectile energy (1-100 ev), angle - Internal state of the projectile - Isotopic effect (D, T) - Flux density ( m -2 s -1 ) Surface microstructure - Crystalline, amorphous a-c, polycrystalline); Doping (Si, B) - Hydrogenation level (H/C ratio) - Hybridization level (sp/sp 2 /sp 3 ratio) - Surface morphology; preparation - Surface temperature ( K) for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
9 number density (a.u.) Normalized Mass 20 signal surface Chemical sputtering creates a dynamic surface Competition between beam induced C=C bond breaking, H passivation, HC precursor formation, and H loss, HC product emission At steady state dynamic equilibrium between H loading and H 2 loss has been reached Time evolution of methane signal 60 ev / D D 3 + incident on ATJ graphite saturated signal Vergara et al., 2006 Steady state methane yield/d Total carbon MD 20 wall contribution to saturated signal: ~ 10 % CD 3 +CD 4 Steady state Beam ON Time (s) background level No yield!! Fluence (10 20 m -2 ) 100 ev / D impact C density saturated signal Evolution of the density profile (a) No impacts (b)1000 impacts Fluence = 1.4 x10 20 D m 2 (c)3000 impacts wall contribution to H density saturated signal: ~ 20 % Beam -5 ON depth (A) for the Department 0 of Energy Time (s) background level Stuart et al, J. Phys. Conf. Ser. 194, (2009) OFES ICOPS/SOFE Review, ORNL, 2011 March Mini 02, Course 2010
10 Materials exposed to plasma are modified, resulting in a dynamical surface Partial count Sputtering Yield/D sp 3 density (1/A 3 ) surface Deuterium impact of carbon Amorphization depends on penetration depth rather than of deposited energy Methane sputtering requires H loading of the surface sp impact sp2 5 ev/d 7.5 ev/d 30 ev/d 15 ev/d 20 ev/d Depth (A) 6 C-CD3 : sp3 z<5 4 C-CD2 : sp2 Plasma 2 irradiation results in a different C-CD surface : sp b) 0 z<15 1x10-2 C 2 D 2 CD 3 CD 4 8x10-3 6x10-3 C 2 D n, n>2 CD 2 CD C 2 D 4x10-3 C 3 D n sp a) E (ev/d) Chemical sputtering of hydrocarbons Surface morphology on tungsten Nano-fuzz on W irradiated with He Sub-surface structure (W) D, H retention Blistering 2x E (ev/d) Krstic et al, New J. of Phys. 9, 219 (2007). for 10 the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/ µm grain ejection
11 3. How to build the data for PMI? Data : Mutiscale probem: At what scale, for what scale, defined? for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
12 Probing the PMI requires integration of many experimental and theoretical techniques spanning orders of magnitude in time, length, and energy scales e.g., quartz crystal microbalance e.g., secondary neutral mass spectrometry e.g., low energy ion scattering, x-ray photoelectron spectroscopy Monte-Carlo techniques Diffusion; transport e.g., Rutherford backscattering, elastic recoil detection Courtesy of J.P. Allain for 12 the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
13 Guiding principle: If Edison had a needle to find in a haystack, he would proceed at once with the diligence of the bee to examine straw after straw until he found the object of his search I was a sorry witness of such doings, knowing that a little theory and calculation would have saved him 90% of his labor. Nikola Tesla, New York Times, October 19, 1931 The traditional trial-and-error approach to PMI for future fusion devices by successively refitting the walls of toroidal plasma devices with different materials and component designs is becoming prohibitively slow and costly for 13 the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
14 MEANING OF THE CUMMULATIVE BOMBARDMENT What does flux of particles/m 2 s mean (ITER) for a typical atomistic (MD) simulation? for the Department of Energy At a box of surface of 3 nm lateral dim? a few thousands atoms (carbon) The flux is 0.01 particle/nm 2 ns 1) 1 particle at the interface surface of the cell of 10 nm 2 each 10 ns. But for deuterium with impact energy less then 100 ev: Penetration is less than 2 nm, typical sputtering process takes up to 50 ps Each impact independent, uncorrelated! In effect interaction of an impact particle with nanosize macromolecule functionalizes it! News is that each particle will change the surface for the subsequent impact! OFES Review, ORNL, March 02, 2010
15 5. How to build atomistic scale data? for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
16 Molecular dynamics (MD): computes pico-to-nano scale Simultaneous evolution of a many-particle system over t ~ ps-ns Equations of motion solved for each particle at series of smaller time steps (energy conservation) t ~ 0.1 fs Potential energy U: predefined function Classical MD 2 nd Newton s law for each particle 1000 s of randomized trajectories repeated: F V Krstic, 2008 Abell-Tersoff-Brenner-Stuart form used for covalent (short range) coupling (like is in amorphous hydrocarbons) for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
17 Classical MD is only as good as the interatomic potential model used Most advanced: hydro-carbon potential developed for chemistry Brenner, 1990, 2002 : REBO, short range, 0.2nm more sophisticated AIREBO (Stuart, 2000, 2004, 1.1 nm) > 400 semi-empirical parameters, bond order, chemistry Adaptive Intermolecular Reactive Bond Order (AIREBO) potential : torsion, dispersion, Van der Waals, EX: MD calc. of reflection coeff. Significant sensitivity to changes in potential model for some processes Experimental validation essential to establish credible MD simulation. Interatomic potentials for W, Be, C exist (talk of Nordlund) Experimental validation? Improvements to CH potentials done (Kent et al, 2010) New Li-C-H-O potentials being developed (Dadras et al, 2010) for 17 the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012 Reinhold et al, J. Stuart, Nuc. Instr. Meth. B 267, 691 (2009).
18 What to do with Lithium dynamics: Problem to study theoretically because Li polarizing features when interacting with other elements Electronegativity is chemical property of an element defining its tendency to attract electrons: Li has it exceptionally low in comparison to H, C, O, Mo, W. Consequence: Bonding between Li and other atoms covalent and polar; Long-range nonbonding: Coulomb :1/R Lennard-Jones :1/R 6, 1/R 12 Electronegativity and size of atoms related! for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
19 Charging changes at each simulation step: Quantum-Classical Molecular dynamics a must Potential energy calculated at each time step by solving Schrödinger equation for electrons with adiabatic instantaneous Hamiltonian Current DOE capabilities: Jaguar, Kraken, Titan: Hundreds of thousands of processors, GPUs Electrons: Quantum mechanically at each step, resulting in charges and forces Nuclei: Classical motion Employed the Self-Consistent-Charge Density-Functional Tight-Binding (SCC-DFTB) method (developed by Bremen Center for Computational Materials Science, Germany) It is an approximation to the DFT method in which only valence orbitals are considered, and difficult Integrals parameterized in advance. In comparison to other TB methods: Improved self-consistent interaction of electronic charges This enables computational efficiency about 1,000 time faster than ab initio quantum methods (and about 1,000 time slower than Classical Molecular Dynamics) for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
20 H impact Who are the users of the data? example: Monte Carlo trajectory approach Macroscopic master equation for the long-time evolution Boltzmann like collisional relaxation operator (rates form MD) desorption Conversion to CH 4 sp 2 diffusion H sp x H H sp 3 H H diffusion carbon CH 3 is created for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
21 6. How to validate theory with experiments (and vv)?! How do we learn that our results are real? Without mutual validation of experiment and theory in this area chances very slim to have believable results! for the Department of Energy OFES Review, ORNL, March 02, 2010
22 Sputtering yield (/D) What have we learned from the next door beam-surface experiments? Beam-surface exp t: precision control of projectiles & targets enabled development & validation of MD approach total C hydrocarbon CD 3 +CD 4 Remarkable agreement of theory & exp t when simulation mimics exp t. No fitting parameters! Key: simulation prepares surface by bombardment! Fluence (not flux) like that in experiment Type, internal state, energy, angle as in exp t 10-3 MD with D 2 (*) MD with D MD with D(g) 2 exp with D 2 + exp with D + exp with D Impact energy (ev/d) Reaching steady state Meyer et al, Physica Scripta T128, 50 (2007). for 22 the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
23 7. Can modeling provide believable data that are not available from experiment! Who are users of data? Some examples highlights for the Department of Energy OFES Review, ORNL, March 02, 2010
24 Counts Yield/D (%) E s (ev) Yield More examples include even more parameters!!! 1) Total hydrogen yield as a measure of stationarity 2) Sputtering with (ro)vibrationally excited projectiles has significant effects D gs) D(1s ) D ( ~ 6) D 2 ( 2 E=10 ev/d C CD y Krstic et al, New J. of Phys. 9, 219 (2007). for the Department of Energy C 2 Dy E=7.5 ev/d CD y C 2 D y E=10 ev/d CD y C 2 D y C 3 D y C 4 D y C 2 D y C 3 D y C4 D y C 5 D y E=20 ev/d E= 30 ev/d M s (amu) Amplitude (Angtroms) OFES Review, ORNL, March 02, 2010 CD 3 +CD 4 C 2 D 2 Krstic et al, Europhys. Lett. 77, (2007). Mass/energy spectra of sputtered hydrocarbons: 1)Heavier species at higher energies 2) Hot hydrocarbon ejects (kinetic desorption) 150 e -E s(ev)/0.6) E=20 ev/amu E s (ev) CD y C 2D y E=7.5 ev/d E=20 ev/d E=10 ev/d E=30 ev/d C3Dy C 4D y M s (amu) Ejected mass spectra
25 v y (10 7 m/s) ) Angular distributions dn/dω total hydrocarbon E=30 ev/d 4) Isotope effects increase with the mass of the projectile Bond-breaking threshold are nearly mass independent and are dominated by associative-dissociative reactions vx (10 7 m/s) Angular moments L sin law or isotropic CM velocities follow cos-law Krstic et al, J. Appl. Phys. 104, (2008). Reinhold et al,j. Nucl. Mat. 401, 1 (2010). for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
26 Counts Ejection energy (ev) 5) Rovibrational energy distributions: Ejected Hydrocarbons rotational distribution of ejecta Fit based on Maxwell of 0.34 ev D 2 with D impact (10 ev) H 2 with D impact (10 ev) energy (ev) Hydrocarbon ejection CD 3 ejection Translational Rovibrational Rotational Vibrational D Impact energy (ev) Ejection energy Approximate thermalization indicated Functions of hydrocarbon mass and impacting D energy for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012 (a) (b) Ejection temperature Krstic et al, J. Appl. Phys. 104, (2008).
27 8. What information cannot atomistic modeling provide? This is multiscale problem: One theoretical approach cannot cover all scales Example: Tungsten fuzz for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
28 Carbon yield (C/D) Example : Where MD fails? Thermal processes!!!! Dependence of Carbon erosion on the surface temperature 0.1 Time scale of thermal D-release longer than ps-ns scale ev D impact at deuterated a-c Legend MD C yield Exp Balden MD C yield with red D Temperature (K) J. Dadras et al, NIMB 269, 1280 (2010) for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
29 Challenges with carbon surfaces: Long standing problems? Do we need better potentials? Do we need direct line of sight experiments? Open problem: simulations overestimates the yield of large molecules ->Erosion of carbon oversized at higher energies Krstic et al, Nuc. Instr. Meth. B 267, 704 (2009). for the Department of Energy OFES ICOPS/SOFE Review, ORNL, 2011 March Mini 02, Course 2010
30 9. Is the PMI phenomenology with plasma irradiation different than with a beam irradiation? Can we derive plasma-irradiated PMI from the beam-pmi? Can we model plasma irradiation at all? Do we need data from plasma and from beam? Answer is: Yes, No, Yes, Yes for the Department of Energy OFES Review, ORNL, March 02, 2010
31 Goal: Study synergy in the evolution of surface irradiated by plasma Experiments with Ar+ and H: Sputtering = (chemical) + (physical) Surface preparation by H impact for chemical sputtering Impurity atoms in plasma are efficient precursors for erosion PM processes very dependent on inventory of H in the material Exposure of pyrolytic graphite to 5 MeV C+ simulates NEUTRON DAMAGE: more nucleation enhanced erosion sites for H retention increased HC density? increased ejection probability? Ion flux = 3.5 * cm -2 s -1 H flux = 1.4 * cm -2 s -1 H and Ar + physical H alone Ar + alone Hopf & von Keudell, 2003 B.I. Khripunov et al for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
32 Synergies in tungsten!!! Fuzz nanostructures on W irradiated by He high W temperatures (>1000K) He suppresses H retention He penetrates deeper than H Strong dependence on energy He bubbles: barrier to H diffusion? He: 0.1% He: 0% Baldwin, 2008 Blistering related to D, H retention Sparser for T > 600 K H implantation(2-20 nm) T=653 K H grain boundaries > 1 µm Dome-like blisters grain ejection Ueda et al,2008 for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
33 Counts Yield Simulations of the plasma irradiation (D atom impact) V Z T=10,000K sqrt(e) exp(-e/kt) E (ev) T=10,000K All V Z >0 changed sign uniform V X HOW? Maxwell Impact distributions V Y 0.8 D ejected plasma beam D 2 sputtered Impact energy of D (ev) Krstic et al, 2009 With plasma irradiation: Reflection significantly higher, sputtering suppresed!!! Krstic et al, AIP Conf. Proc. 1161, 75 (2009). for 33 the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
34 Counts Impact plasma distributions (D atom) : Examples Counts T=10,000K T=200,000 K Maxwell-Boltzmann sqrt(e) exp(-e/kt) ~sqrt(e) exp(-e/kt) E (ev) E (ev) T=10,000K All V Z >0 changed sign T=200,000 K All V Z >0 inverted sign V Z V Z V X V Y V X V Y for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
35 Counts Counts Output (reflected) distributions of D T p =50,000 K exp(-e/0.6ev) sputtered Boltzmann distributions exp(-e/2.9ev) inelastically reflected Energy of re-emitted D (ev) V X V Y V Z T p =100,000 K exp(-e/0.8ev) sputtered Boltzmann distributions exp(-e/6ev) inelastically reflected V Z VY V Z Energy of re-emitted D (ev) for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
36 Counts Counts Distributions of sputtered hydrocarbons T p =200,000 K exp(-e/1.9ev) c.m. energy E c.m. (ev) V x VY V Z T p = 200,000 K exp(-e/0.45ev) rotational energy L X L Y L Z E rot (ev) Angular momentum distributions for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
37 Sputtering Yield/D Total carbon sputtering yield /D Hydrocarbon sputtering with beam and plasma (Comparison) 1x10-2 C 2 D 2 CD 4 CD 3 8x10-3 6x10-3 4x10-3 2x10-3 beam plasma Impact energy (ev/d) Spectra of typical sputtered hydrocarbons qualitatively the same behavior with beam and plasma irradiations 10-1 MD simulation of chemical sputtering plasma MD with D 2 (*) MD with D 2 diss. MD with D MD with D 2 (g) total hydrocarbon with D 2 (*) Exp. with D 2 + Exp. with D 3 + beam Impact energy (ev/d) Under the same conditions less erosion with plasma than with a beam for the Department of Energy Improving the OFES Database Review, for ORNL, Phys March And Chem 02, 2010 Sputtering, IAEA, 12/2012
38 10. What is outreach of the PMI science data at the fusion plasma facilities? How to build an integrated theoreticalexperimental approach? How to design the plasma-facing materials upon required specification? Difficult to study PMI in thoroidal facilities! Importance of the dedicated PMI facilities Pisces-B, Magnum, ) = Bridge!!! for the Department of Energy OFES Review, ORNL, March 02, 2010
39 QuickTime and a Vision for integrated experimental and theoretical PMI research Ion-surface scattering experiments: Ions on high-dpa, high temp W Simulation of additional fast n & heat load, damage Molecular Dynamics (MD) & Monte Carlo (MC) simulation Material Science High-flux linear PMI experiment: Plasma on high-dpa, high temp W When available MD and MC with plasma synergy Potential models Quantum-classical MD Increases in computational power Toroidal confinement experiments decompressor are needed to see this picture. 39 for the U.S. Department of Energy PMI Design & Validation Predictive science!!! FNSF, DEMO
40 CONCLUSIONS: PMI extremely difficult interfacial problem (Material mixing create SURFACE entity; scale depends on impact energy; What data? PMI data can be built from bottom-up recognizing its multiscale character and building from shortest time/spatial scales (fs/angstrom) up. Theory&modeling of PMI MUST be validated by experiment (and v.v.), (at least to explain phenomenology, is this then the data??) Irradiation create dynamical surface, changing interface, data must come form the steady state, cumulative bombardment!!!! Surface responds to synergy in plasma irradiation (angles, energies, particles), data do not NOT follow linear superposition principle; NEED plasma irradiation modeling and experiments; dedicated plasma devices a must for data validation Inclusion polarization effects in potentials (Li-C-H, Be-C-H(?), ) and extension to quantum-classical approaches an essential step forward, currently allowed by computer developments Categorization of PMI data with respect to surface and projectile states, to time-space scales, to environment, to type of users and to format EXTREMELY DIFFICULT for the Department of Energy WHAT ACCURACY? OFES Review, ORNL, March 02, 2010
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