free energy landscape -evolution of the tdm- takashi odagaki kyushu university iv wnep round table...
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![Page 1: Free Energy Landscape -Evolution of the TDM- Takashi Odagaki Kyushu University IV WNEP Round Table Discussion September 22, 2006 Trapping diffusion Model](https://reader037.vdocument.in/reader037/viewer/2022103005/56649d455503460f94a2226a/html5/thumbnails/1.jpg)
Free Energy Free Energy LandscapeLandscape
-Evolution of the -Evolution of the TDM-TDM-
Takashi Odagaki
Kyushu University
IV WNEP Round Table Discussion September 22, 2006
Trapping diffusion Model
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What do we have to What do we have to understand?understand?
ThermodynamicsThermodynamics What is the transition?What is the transition? Cooling rate dependence?Cooling rate dependence? TTgg? T? TKK??
Slow process
Fast process DynamicsDynamics Slow dynamics? TSlow dynamics? T00?? Fast dynamics?Fast dynamics? TTgg? T? Txx??
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How do we proceed?How do we proceed?
Phenomenological UnderstandingPhenomenological Understanding of Experimentsof Experiments
Fundamental TheoryFundamental Theory
New ParadigmNew Paradigm
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2nd order Phase Transition
Glass transition
Configuration
Fre
e en
ergy gTT
gTT
Degree of quenching (t obs)=
basins of #
visitedbasins of #1
Annealed
quenched
C
gTT
disordered
ordered
C
CTT
doq
T
T
CTT
CTT F waittgTAt
Slow & fast relaxations
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Trapping diffusion model
• Single particle description of the FEL picture
2)( tt
)(
)()(
gcg
gcgc
TsT
TsTTTs
Waiting time distribution
0t1 0T 0)( 0 Tsc
2t xT10 gTt 0D
• Findings
• Gaussian – non-Gaussian Transition at
•
• Characteristic Temperature Equation1
0 )(2 TTTT ggx
gT
0TTK
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Characteristic Temperature Equation
V B Kokshenev & P D Borges, JCP 122, 114510 (2005)
g
C
T
T
0/TTg
g
C
T
T
0/TTg
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• 20 basins:Einstein oscillators
slow
fast
Specific heat
Probability of being in basin a at t
aE
),( tTPa
Energy of basin a
),(),( tTPEtTE aa
a
i
ii TT
tTEtTEttTC
),(),(
),( 00
a
anneale
d
quen
che
d
•Findings
• Annealed to quenched transition
• Cooling rate dependence
• Characteristic behaviors of ac specific heat
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ConclusionConclusion
The FEL picture is the only frame The FEL picture is the only frame work that provides unified work that provides unified understanding of the glass transition.understanding of the glass transition.
The FEL can be constructed by The FEL can be constructed by thethe
density functional approach.density functional approach.
RemarRemarkk
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The 1st order ac specific heat
D
eb
ye
10-2 10-1 100 10110-1
100
101
p
ea
kw
0
(T-T0)/Tg
914.00 )(~ TT
gT
10-2 10-1 100
2
4
6
8
(T-T0)/Tg
)]/(022.0exp[04.1~ 0TTTg
gT
)75.0/( 0 TgT
Real part
0/Wpeak
Imaginary part
10-2
100
102
0
1T/T g=0.85
T/T g=0.85
T/T g=1.0
T/T g=1.0
T/T g=1.25
T/T g=1.25
(C 1()-C quench )/(C aneeal -C quench )~
/w 0
Return
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10−2 100 102
−2
−1
0
1
/w0
(C"2()−C2(∞ )) (C2(0)−C2(∞ ))/~ ~ ~ ~
T/Tg=0.825T/Tg=0.875T/Tg=1.0T/Tg=1.25T/Tg=2.5
10−2 100 102
−2
−1
0
1
/w0
(C'2()−C2(∞ )) (C2(0)−C2(∞ ))/~ ~ ~ ~
T/Tg=0.825T/Tg=0.875T/Tg=1.0T/Tg=1.25T/Tg=2.5
The 2nd order ac specific heat Real part Imaginary part
10−2 10−1 100 101
10−2
100
=0.97
(T−T0)/Tg
Min of real part
Max of imaginary partMin of imaginary part
=1.05=1.01
Tg
)(~ 0TT
Return
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Free energy landscape
)()( tuRtr iii
])(exp[})({ 2 i
iiii RrCRr For practical calculation
dRrrHN
RNVTZ iiii })({})]({exp[!
1}){,,,(
}){,,,(ln}){,,,( iBi RNVTZTkRNVT
ttt 0for )(trR ii where
Separation of microscopic and structural-relaxation time scales
))()()(()(2
1
))(()(
log)(][)]([
212121 ll
ll
l
cdd
dd
rrrrrr
rrr
rrr
: Direct correlation function
)(rc
Ramakrishnan-Yussouff free energy functional for hard spheres
])(exp[)( 2 i
iC Rrr
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Simultaneously and cooperatively rearranging regions
SRR: Difference between two adjacent basins
CRR: Atoms involved in the transition state
108
523.0
N
return
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No of atoms in the core : 32555.0 362
String motion and CRRReturn