National Synchrotron Light Source Workshop

aharacterization of Advanced Materials under Extreme Environments

for Next Generation Energy Systems
Brookhaven National Laboratory, September 25, 2009

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Nuclear Science and Engineering and Materials Science and Engineering

Massachusetts Institute of Technology
 u E Workshop on
Basic Research Needs for Advanced Nuclear Energy Systems, July 2006

Identify new, emerging, and scientifically challenging areas in materials and chemical sciences
that have the potential for significant impact on advanced nuclear energy systems

The fundamental challenge:

Understand and control chemical and physical phenomena in multi-component systems from femto
seconds to millennia, temperatures to 1000ºa, and radiation doses to hundreds of displacements per atom.

Enormous and broad implications in the materials science and chemistry of complex systems:
New understanding is required for microstructural evolution and phase stability under extreme chemical
and physical conditions, chemistry and structural evolution at interfaces, chemical behavior of actinide and
fission-product solutions, and nuclear and thermo-mechanical phenomena in fuels and waste forms.

First-principles approaches are needed to describe ˜-electron systems, design molecules for separations,
and explain materials failure mechanisms. Nanoscale synthesis and characterization methods are needed to
understand and design materials and interfaces with radiation, temperature, and corrosion resistance.

New multiscale approaches are needed to integrate this knowledge into accurate models of relevant
phenomena and complex systems across multiple length and time scales.
 The fundamental challenge:

Understand and control chemical and physical phenomena

in multi-component systems

from femto seconds to millennia,

temperatures to 1000ºa,

and radiation doses to hundreds of displacements per atom.

u
Workshop on Basic Research Needs ˜or Advanced Nuclear
nergy Systems, July 2006
 Structure ± Property aorrelation

Unit Process to Functional Behavior

aoncept Materials

Role of Experiments
 Modeling and Simulation across length/time
scales, from electrons, atoms to the continuum

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uynamics of Metals ± a large multiscale modeling ASaI
program at the Lawrence Livermore National Laboratory

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 Unit Process in Mechanical behavior

ideal shear strength (nano-indentation)

tensile failure (soft mode instability )
charge density redistribution (affine shear deformation)
water-silica reaction (hydrolytic weakening)
dislocation nucleation (crack tip plasticity)

J. Li, ³Physics and Mechanics of uefect Nucleation´,

MRS Bulletin w, 151 (2007)

many properties (structural, thermal, transport, etc.) can be studied

 !


 


 
 
  !  

0 ( w, k ) ! (Cijkl wi wk  X jl ) k j kl ! 0
soft phonons
Nonlocal instability criterion for homogenous nucleation of a dislocation
J. Li et al., Nature ", 307 (2002)
aharge density redistributions in affine shear Al



#$#
au
S. gata et al, Science 298, 807 (2002)

au Al
attack of water molecule on quartz (Si 2)

Transition state pathway

sampling (NEB)

Molecular orbital theory

Stress-dependent
activation barrier

minimum energy path

T. Zhu et al., J. Mech. Phys

Solids 0w, 1597 (2005)
ü2 + Si- -Si 2Si ü
 from unit processes at the atomistic level to
systems behavior at the meso/macro-scale
__________________________

µaoncept Materials¶

virtual prototypes -- all-atom models capable of

predicting functional behavior in extreme conditions

Transform existing technology

from empirical practice to science based
 xidation resistance of a UüTa (ZrB2) depends critically
on oxygen transport across a protective complex oxide layer

Borosilicate
glass layer

Zr 2

unreacted ZrB2
Sia

Monteverde and Bellosi,

J. Electrochem. Soc. 0 (2003) B552
 Understanding the kinetics of hardening in cement paste

Mechanism ?

Shear modulus of slurry (water-cement =0.80 w/w) measured by ultrasonic

attenuation showing coagulation and setting stages [Lootens et al. (2004)]
 Molecular Model of aement?
Schematic of cement paste showing dissolution of
a3S and precipitation of a-S-ü platelets in a solution
of aa( ü)2 and aa2+ and other ions [Jönsson et al.
(2005)]

a
a 
a
 a





Mu model of mineral-solution interface,

aan such a model describe cement hardening ? 30 A aqueous layer with al-, Si 42-, and Na+
[Kalinichev et al. (2006)]
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