005 Keiji Morokuma

1
Density-Functional Tight-Binding Molecular

Dynamics Simulation of Growth of Single-Walled
Carbon Nanotubes from Metal Cluster
1
Kyoto University
2
Nagoya University
http://kmweb.fukui.kyoto-u.ac.jp/nano http://qc.chem.nagoya-u.ac.jp
The Fourth NASA-Rice-AFOSR Workshop on Nucleation and Growth
Mechanisms of Single Wall Carbon Nanotubes
Tierra Sagrada, TX April 17-21, 2009
Yasuhito

Ohta,

Yoshiko

Okamoto, Alister

J . Page, Ying

Wang,

Stephan Irle,

Keiji Morokuma
1
Fukui Institute for Fundamental Chemistry, Kyoto University
2
Institute for Advanced Chemistry and Department of Chemistry, Nagoya University
3
Cherry L. Emerson Center for Scientific Computation and Department of Chemistry, Emory University
3
Emory University
2
Outline

Motivation

Review: state of the art SWNT growth control and
theoretical modeling

Density-functional tight-binding (DFTB) method and its
application in molecular dynamics simulations

Continued growth simulations of armchair SWNTs,
temperature dependence; zigzag SWNTs

Surface diffusion, cap formation and cap growth on
transition metal cluster, acetylene decomposition

Summary and outlook
3
Outline

Motivation
Motivation





Summary and outlook
Motivation A Nobelists Perspective
4
Sir Harry Kroto in D. J. Palmer, Where nano is going,

Nano Today 3, 46 (2008)
They [nanotubes and
nanowires] have to have
reproducible properties, and
we're not in that situation at the
present time; you can make
various types of nanotubes and
study the properties of them but
at the moment we don't have
the control to produce the
nanotubes with accurately
specified diameter, structure,
chirality, you name it.
5
Outline

Motivation





Summary and outlook
6
Review SWNT Growth Control
Recent advancements in SWNT growth control
Diameter control:
C. Lu and J. Liu, Controlling the Diameter
of Carbon Nanotubes in Chemical Vapor
Deposition Method by Carbon Feeding, J.
Phys. Chem. B 110, 20254 (2006)
H. Shinohara and coworkers: Synthesis of
single-wall carbon nanotubes grown from
size-controlled Rh/Pd nanoparticles by
catalyst-supported chemical vapor
deposition, Chem. Phys. Lett. 458, 346
(2008)
Chirality control:
D. E. Resasco, R. B. Weisman, and
coworkers, Narrow (n,m)-Distribution of
Single-Walled Carbon Nanotubes Grown
Using a Solid Support Catalyst, J. Am. Chem.
Soc. 125, 11186 (2003)
Many others ...
T=800

C
C
2

H
6

feedstock
Red: 4200 ppm
Green: 14,400 ppm
CoMoCAT

:
Co-Mo
catalyst
7
Other improvements
High yield:
K. Hata, D. Futaba, et al. Water-Assisted
Highly Efficient Synthesis of Impurity-Free
Single-Walled Carbon Nanotubes, Science
306, 1362 (2004)
Defect control:
S. Maruyama et al., Low-temperature
synthesis of

high-purity single-walled carbon
nanotubes from alcohol, Chem. Phys. Lett.
360, 229 (2002)
Length control:
L. X. Zheng et al., Ultralong single-wall
carbon nanotubes, Nature Mater. 3, 673
(2004)
Many other groups and improvements
so-called supergrowth
Low Raman D/G
ratio = high purity
when using
alcohols as
feedstock
(ACCVD)
8
But How to put the puzzle pieces together?
(5,5) SWNT
high yield, desired length, defect-free, eventually catalyst-free
ACCVD etc
Selection of
appropriate

growth
conditions
9
Review Experimental Growth Studies
Look here in situ environmental TEM studies of
SWNT nucleation and growth
H. Yoshida, et al. Atomic-Scale In-situ
Observation of Carbon Nanotube
Growth from Solid State Carbide
Nanoparticles, Nano Lett. 8, 2082 (2008)
Fe/SiO
2

C
2

H
2

:H
2

T=600

C
Fluctuating solid Fe
3
C
S. Hofmann, et al. In-situ Observations of
Catalyst Dynamics during Surface-Bound
Carbon Nanotube Nucleation, Nano Lett. 7,
602 (2007)
Ni/SiO
2

C
2

H
2

:NH
3

T=480 to 700

C
Fluctuating solid pure nickel
F. Ding, et al.
Appl. Phys. Lett.
88, 133110
(2006)
Fe
2000

, T=1007

C
REBO/MD
L
i
n
d
e
m
a
n
n

i
n
d
e
x

(
a
.
u
.
)
10
Review Experimental Growth Studies
SWNT Growth N-dimensional Parameter Space
catalyst size [nm]
catalyst composition
T [

C]
Fe
Co
Ni
Co/Mo
Rh/Pd
600
1000
1 4 10
feedstock species
feeding rate/
pressure
substrate
etching agent
Fill all space with blocks/scan full

parameter space
Evaluate interdependence relations
perfect

(n,m)-specific synthesis
Systematic Investigation of
SWNT growth mechanism(s):
Can only construct ~1 machine/year
Let Theory Do It!! (computer time is
cheap )
Experimentalist:
J.-Y. Raty et al, Growth of Carbon Nanotubes on Metal Nanoparticles: A Microscopic

Mechanism from Ab Initio Molecular Dynamics Simulations, Phys. Rev, Lett. 95, 096103 (2005)
Nano-diamond: Inappropriate model!
Change from diamond structure (sp
3
) to
fullerene cap (sp
2
) immediately!
simulation time~10 ps
Too short

to demonstrate
self-assembly
Review Previous CPMD
11
Previous Car-Parrinello Molecular Dynamics (CPMD)
J. Gavillet et al, Root-Growth Mechanism for SWNTs, Phys. Rev, Lett. 87, 275504 (2001)
Carbon precipitation on Co carbide
particle, 51 Co & 102 C atoms, 25
ps 1 hexagon, 2 pentagons
C
30

+44C on Co surface at 1500 K, 15
ps 5 carbon atoms diffused to cap
Heroic efforts on supercomputers, one-shot simulations!
12
F. Ding et al., J. Phys. Chem. B 108, 17369 (2004)
Bond order potential allows bond breaking

via potential switching functions, but
does not include effects of -conjugation or charge transfer
Y. Shibuta & S.
Maruyama, Chem. Phys.
Lett. 382, 381 (2003)
Review Previous REBO MD
Reactive Empirical Bond Order (REBO) MD
Feeding
carbon
atoms from
center of Fe
clusters:
Fe50 + nC,
T=627

C
500 C atoms +nC,
Ni
108

, T=2227

C
(20 nm)
3

PBC
Classical potential, cheaper, many long simulations!
Y. Shibuta & S. Maruyama, Chem.
Phys. Lett. 437, 218 (2003)
500 C atoms
+nC, Ni
256

on
LJ support
T=2227

C
(20 nm)
3

PBC
F. Ding et al., J. Chem. Phys. 121, 2775
(2004)
Fe
m

+ nC, T=527

C to 627

C
Many more studies
Review Previous REBO MD
13
Review REBO/MD Simulations
Specific problems of REBO MD for SWNT growth
Problem 1: large number of non-hexagon rings!
REBO does not discriminate between
aromatic or antiaromatic rings
\Unrealistically many 4- and 8-
membered rings (formally antiaromatic)
F. Ding et al., J. Phys. Chem.
B, 108, 17369 (2004)
\Amorphous structure formation
Problem 3: sp
3
defects overestimated
N. A. Marks N. A. Marks et al et al., ., Phys. Rev. B Phys. Rev. B 65 65, 075411 (2002) , 075411 (2002)
SI, G. Zheng, Z. Wang, K. Morokuma, SI, G. Zheng, Z. Wang, K. Morokuma, J. Phys. Chem. J. Phys. Chem.
B B 110 110, 14531 (2006) , 14531 (2006)
Important for self-healing of graphitic sheets
\Very slow transformation processes
G. G. Zheng Zheng, SI, M. , SI, M. Elstner Elstner, K. , K. Morokuma Morokuma, , J. Phys. Chem. A J. Phys. Chem. A
108 108, 3182 (2004) , 3182 (2004)
Problem 2: polyynes are underrepresented
14
Dilemma of theoretical simulations for
scanning SWNT growth parameter space
Review MD Problems
-Conventional quantum chemical MD (like CPMD) is too expensive
-Classical REBO MD is qualitatively incorrect: too long time scale,
unrealistic events
Target MD
Quantum mechanics
??
Then: scan of
parameter space
15
Outline

Motivation


Density
Density
-
-
functional tight
functional tight
-
-
binding (DFTB) method and its
binding (DFTB) method and its



Summary and outlook
16
Self-consistent-charge density-functional tight-
binding (SCC-DFTB)
1
2
2
tot i i rep
i
E f E q q
o| o |
o|
c = + + A A

D. Porezag, Th. Frauenheim, T. Khler, G. Seifert, R. Kaschner, Phys. Rev. B 51, 12947 (1995)
M. Elstner et al., Phys. Rev. B 58, 7260 (1998)
( )
0
vi i
v
c H S
v v
c =
Second order-expansion of DFT total energy with respect to charge fluctuation

TB-eigenvalue equation
~100 atoms
~100s ps
DFTB Energy, Mermin, gradient
Single-zeta
STO basis set
Conjugation explicit
Finite temperature approach (Mermin

free energy E
Mermin
)
( )
1
exp / 1
i
i B e
f
k T c
=
+ (

( ) ( )
2 ln 1 ln 1
e B i i i i
i
S k f f f f
= +
T
e
: electronic temperature
S
e
: electronic entropy
0 1
2
N
rep
i i i i
i
E H H S
F f c c q q
S R R R R
v v v o
o v o
v
v o o o o
c
(
| |
c c c c
= A A
( |
|
c c c c
(
\ .

0 1
i
f s s
Atomic force
E
2f
i
0 1 2
M. Weinert, J. W. Davenport, Phys. Rev. B 45, 13709 (1992)

E
Mermin
= E
tot
- T
e
S
e
Openshellness
explicit
17
Fullerene Isomer Geometries and Energies vs B3LYP/6-31G(d)
G. Zheng, SI, M.
Elstner, K. Morokuma,
Chem. Phys. Lett. 412,
210 (2005)
DFTB Performance
Vibrational IR and Raman Spectra
H. A. Witek, SI, G.
Zheng, W. A. de Jong,
K. Morokuma, J. Chem.
Phys. 125, 214706
(2005)
RMS [ ] NCC-DFTB SCC-DFTB AM1 PM3
C20-C36 0.025 0.019 0.035 0.030
C60-C86 0.014 0.014 0.016 0.015
R
2
(lin. reg.) NCC-DFTB SCC-DFTB AM1 PM3
C20-C36 0.88 0.93 0.77 0.73
C60-C86 0.97 0.98 0.86 0.84
Geometries
Energetics
102 Fullerene Isomers
small cage non-IPR C
20

-C
36

(35), large cage IPR C
70

-C
86

(67)
R
2
: linear regression coefficient between AE(Method) and AE(B3LYP)
I
h
-C
60
D
5h
-C
70
D
2
-C
28
18
A B C
DFT:PW91
[1]
-6.24 -5.63 -1.82
SCC-DFTB
[2]
-5.17 -4.68 -1.86
Adhesion energies (eV/atom)
A
B
C
PW91: An ultrasoft pseudopotential with a plane-wave cutoff of 290 eV for the single metal and the
projector augmented wave method with a plane-wave cutoff of 400 eV for the metal cluster
Fe-Fe and Fe-C DFTB parameters from: G. Zheng et al., J. Chem. Theor. Comput. 3, 1349 (2007)
[1] Phys. Rev. B 75, 115419 (2007) [2] Fermi broadening=0.13 eV
H
10

C
60

Fe
H
10

C
60

Fe
H
10

C
60

Fe
55
Fe
55

icosahedron
(5,5) armchair SWNT (H
10
C
60
) + Fe / Fe
55
DFTB Performance
Y. Ohta, Y. Okamoto, SI, K. Morokuma, Phys. Rev. B, in press
DFTB/MD simulations of carbon nanostructure formation
SI,G.Zheng,Z.Wang,K.Morokuma,J.Phys.

Chem.B110,14531(2006)andothers
Fullereneformation
ShrinkingHotGiant

Road
2000K
+108ps
+SiC

Si
SI,Z.Wang,G.Zheng,K.Morokuma,M.

Kusunoki,J.Chem.Phys.125,044702(2006)
Z.Wang,SI,G.Zheng,M.Kusunok,K.

Morokuma,J.Phys.Chem.C111,12960

(2007)
NoncatalyticCNTgrowth
19
DFTB DFTB/MD Applications
Ar/O
2
Fullerenesinbenzenecombustion
C>~170
Giantfullerenes
Metallofullerene
formation
Fe/Co/Ni

catalyzedCNT

nucleation
3000K
3000K
0.1ps 25.0ps 64.2ps
NDtoSpiroidtoOnion

Transformationupon

Heating
B.Saha,S.Shindo,SI,K.Morokuma,submitted
F u l l e r e n e

f or med onl y

a f t e r a l l H

atoms are gone.
20
Outline

Motivation





Summary and outlook
Model system and carbon supply
R.E. Smalley et al. JACS 128, 15824 (2006)
fcc Fe
38
(5,5) armchair SWNT
length = 6.2

diameter = 7.5
Silicon-oxide
Diameter: ~1nm
Fe particle
Total: 108 atoms
Y. Ohta, Y. Okamoto, SI, K. Morokuma,
ACS Nano 2, 1437 (2008)
Armchair SWNT Growth Experiment & Model System
21
Simulation Flow Chart
T
n

= 1500 K = 1227

C
At=1 fs
Nose-Hoover chain
Equilibrated for 10 ps
10 geometries are
randomly sampled
between 5 and 10 ps
One C atom is supplied around
the C-Fe interface every 0.5 ps,
incident velocity corresponding
to T
n
velocity Verlet
45 ps, 90 Cs are added
ACS Nano 2, 1437 (2008) &
J. Phys. Chem. C, 113, 159-169, (2009).
Armchair SWNT Growth Methodology
22
catalyst composition
T [

C]
Fe
Co
Ni
feedstock
C C
2
C
2

H
4
750
1227
Smalleys experiment
DFTB/MD
simulation
List of theoretical crutches :
Targeted C atom shooting to Fe/C region
Small Fe nanoparticle (~0.7 nm)
Very fast C atom supply
Armchair SWNT Growth DFTB/MD
10 Trajectories after 45 ps C supply
T
u
b
e

l
e
n
g
t
h

[
]
Time [ps]
23
Schematic depiction of C atom insertion events
Trajectory F
new 5-, 6-, 7-membered rings
ACS Nano 2, 1437 (2008)
Growth rate: ~10 pm/ps
24
Self-healing process of sidewall (annealing)
Fe-Carbon mobility at interface important!
Trajectory 6: T
n

= 1500 K, T
e

= 10k K, C
int

=1500 K
24.5 ps -

27.5 ps
Armchair SWNT Growth Sidewall Annealing
Movie
F. Ding, et al. Appl. Phys.
Lett. 88, 133110 (2006)
Fe
2000

, T=1007

C
REBO/MD
L
i
n
d
e
m
a
n
n

i
n
d
e
x

(
a
.
u
.
)
25
SCC-DFTB Mulliken atomic partial charges
Carbon
Iron
C
2

and C
3

on the surface of Fe
cluster are negatively charged
Negatively charged
C atoms penetrate
into the Fe cluster
Charge transfer near
metal-carbon boundary
Armchair SWNT Growth SCC-DFTB Charges
Slow
carbide
formation
26
Armchair SWNT Growth Behavior of Fe Particle
2 4 6 8 10
0
1
2
3
4
5
6
r []
g
F
e
-
F
e
5 ps
20 ps
30 ps
45 ps
Fe-Fe radial distribution function
data sampling in 5 ps intervals
Snapshot at 45 ps
Trajectory 2: Tn=1500K, Te=10kK, C
int

=

500K
Slow Fe-carbide formation
Short polyyne chains such as C
2

,C
3
, C

form on the surface of Fe cluster
C atoms penetrate into
the Fe cluster
0 10 20 30 40
0
5
10
15
20
25
30
0 10 20 30 40
0
5
10
15
20
25
30
0 10 20 30 40
7
8
9
10
11
Time [ps]
T
u
b
e

l
e
n
g
t
h

[
]
N
u
m
b
e
r

o
f

r
i
n
g
s
0 10 20 30 40
7
8
9
10
11
Time [ps]
F
H
T
u
b
e

l
e
n
g
t
h

[
]
N
u
m
b
e
r

o
f

r
i
n
g
s
27
Armchair SWNT Growth Length and Ring Statistics
Relationship between ring type and length
10 trajectories, T
n
= 1500 K
28
Armchair SWNT Growth Length and Ring Statistics
For comparison: Fullerene formation from C
2
w/o Fe catalyst
S3
0
5
10
15
20
25
30
35
40
45
50
0 5 10 15 20 25 30 35 40 45
Time [ps]
Pentagon# in MD geom.
Hexagon# in MD geom.
Heptagon# in MD geom.
Pentagon# in Opt. geom.
Hextagon# in Opt. geom.
Heptagon# in Opt. geom.
2000K
SI, G. Zheng, Z. Wang, K. Morokuma, J.
Phys. Chem. B 110, 14531 (2006)
Note: No 4- or 8-
membered rings
as in REBO/MD
29
T=1500K T=2000K T=1000K
Continued SWNT growth as function of
temperature
10 Trajectories for 3 temperatures
727

C 1227

C 1727

C
T[

C] 727 1227 1727
Growth rate

[pm/ps]
a
3.48 5.07 4.13
Chain carbons
a
3.9 0.3 0.2
SWNT C atoms
a
112.9 110.1 102.7
( (5,5) armchair SWNT)
Y. Ohta, Y. Okamoto, SI, K. Morokuma, J.
Phys. Chem. C, 113, 159-169, (2009).
Growth T-dependence DFTB/MD Growth Rates
a
averaged over 10 trajectories/T
30
J. Phys. Chem. C, 113, 159-169, (2009).
Growth T-dependence DFTB/MD Growth Rates
T=727

C
10 Trajectories after 45 ps
Encapsulation of Fe by polyyne
Trajectory C
A B C D E
F G H
I J
(a)
8.60 ps 7.40 ps 8.32 ps
(b) Dissociation of C
2

from Fe/C
T=1727

C
10 Trajectories after 45 ps
Trajectory G
31
H
10

C
62

Fe
38
(8,0) zigzag
length = 7.1
diameter = 6.3
Equilibrated at 1500 K
Zigzag SWNT Growth DFTB/MD
1C
0.0 ps
0.5 ps
59C
30.0 ps 50.0 ps
40C
52C
76.0 ps
Using (8,0) seed SWNT
fcc Fe
38
32
Outline

Motivation





Summary and outlook
Cap Growth DFTB/MD
C
20
cluster
H
10

C
20

Fe
38
H. Yoshida et al, Nano Lett. (2008).
1 C 32 Cs
33 Cs
20 ps 40 ps
t = 0 0.5 ps
Nanotube 10 long
was formed.
Y. Ohta, Y. Okamoto, S. Irle, and K. Morokuma, Phys. Rev. B, in press
(2009)
Side
Top
Experimental snaphots
0 10 20 30 40
0
2
4
6
8
10
12
3- ring
4- ring
5- ring
6- ring
7- ring
During growth, non-hexagonal rings and polyyne chains frequently formed
and then rearrangement of sp
2
network occurs to construct carbon sidewall.
Surface Diffusion DFTB/MD Annealing
t = 0 20 ps
180 ps
40 Cs
0 20 40 60 80 100 120 140 160
8.0
8.5
9.0
9.5
10.0
10.5
0 20 40 60 80 100 120 140 160
0
2
4
6
8
10
12
14
16
pentagon
hexagon
0 20 40 60 80 100 120 140 160
5
6
7
10
11
12
pentagon
hexagon
Time variation of the
averaged number of rings
Lift-off of cap cluster
was observed
C
40
cluster
H
10

C
40

Fe
38
Annealed at
1500 K
Only pentagons
and hexagons
were formed
Y. Ohta, Y. Okamoto, S. Irle, and K. Morokuma
Carbon 47, 1270-1275 (2009).
Annealed at
1500 K
Annealed at
1500 K
Cap Fragment Formation DFTB/MD Annealing
35
Y. Ohta, Y. Okamoto, A. J. Page, S. Irle, and K. Morokuma, submitted
1 3 4 5
8 6 7 9 10
2
1 3 4 5
8 6 7 9 10
2
10 geometries are
randomly sampled
between 5 and 10 ps
for ten trajectories.
Initial model: Fe
38
Annealed at
1500 K
10 ps
410 ps
t = 0 ps
30 C
2
s
30 ps
t = 410 ps
A
t = 0
100 ps 410 ps
0 5 0 1 0 0 1 5 0 2 0 0 2 5 0 3 0 0 3 5 0 4 0 0
0
1
2
3
4
5
6
7
8

N
u
m
b
e
r

o
f

p
o
l
y
g
o
n
a
l

r
i
n
g
s
T i m e [ p s ]
f i v e - m e m b e r e d r i n g
s i x - m e m b e r e d r i n g
s e v e n - m e m b e r e d r i n g
200 ps 300 ps
0 5 0 1 0 0 1 5 0 2 0 0 2 5 0 3 0 0 3 5 0 4 0 0
0
1
2
3
4
5
6
7
8

N
u
m
b
e
r

o
f

p
o
l
y
g
o
n
a
l

r
i
n
g
s
T i m e [ p s ]
5
Average 5-

and 6-ring
counts over 10 annealing
trajectories
C C
C
C
C
C
C
C
C
C
C
C
C C
C
C
C
C
C
C
C
C
C
C
C C
C
C
C
C
C
C
C
C
C
C
C C
C
C
C
C
C
C
C
C
C
C
C C
C
C
C
C
C
C
C
C
C
Formation of first
condensed 2-ring
system (5/5 or 5/6)
Always pentagon first!
Hollow in Fe is
required
A
100 ps 410 ps
0 5 0 1 0 0 1 5 0 2 0 0 2 5 0 3 0 0 3 5 0 4 0 0
0
1
2
3
4
5
6
7
8

N
u
m
b
e
r

o
f

p
o
l
y
g
o
n
a
l

r
i
n
g
s
T i m e [ p s ]
200 ps 300 ps
5
Movie, 5
ot(frames)=2ps
38
Typical sp
2
-carbon network nucleation and annealing
(A)polyyne chains formed on the metal surface attached to each
other creating a Y-shaped structure which preferentially formed

a pentagon;
(B) polyyne chains on a pentagon formed a pentagon or
hexagon fused to the pentagon;
(C) pentagon-to-hexagon self-healing rearrangement took place
with the help of short-lived polyyne chains stabilized by the
metal.
The nucleation process resembles fullerene cage formation.
The metal particle (catalyst) differentiates the two processes.
In particular, the metal particle:
1. holds carbon fragments on the surface (Saturation of
dangling bonds);
2. slows down diffusion;
3. makes the Fe-C bond the most reactive;
4. slows down bond rearrangement processes;
5. prevents closure of the curved open-ended carbon structure.
Polyacetylene formation, largest carbon cluster: C
6
H
x
Acetylene Decomposition DFTB/MD
Initial model: Fe
38
Annealed at
1500 K
10 ps
10 geometries are
randomly sampled
between 5 and 10 ps
for ten trajectories.
t = 0 ps
30 C
2
H
2
s
30 ps
1 2 3 4 5
6 7 8 9 10
Annealed at
1500 K
15 ps
1 2 3 4 5
6 7 8 9 10
40
Outline

Motivation

Review: state of the art SWNT growth control
(experiment and theory)




Summary and outlook
Summary and outlook
41

DFTB/MD method very useful to probe SWNT growth parameter
space

by more realistic simulations of SWNT growth on metal particle.

Carbon atom supply in Fe/C interface region leads to development
of short polyyne chains that grow into 5/6/7 rings, some temperature
dependence of growth.
Summary

SWNT (n,m) chirality NOT preserved! Chirality should be
preserved if carbon addition is slower than defect annealing (10s
of picoseconds)
Summary & Outlook

Pentagon-hexagon-only growth achieved by slower surface
diffusion.

First-ever cap nucleation from C
2

molecules observed by slow
surface diffusion.

Cap nucleation very similar to fullerene cage nucleation,
slowed down by presence of Fe cluster (immobility of C
2

and
polyynes)
42
Extension of DFTB/MD time scale is needed:
Faster alternatives to BOMD but with similar time step
Different type of MD?
Faster computer?
Summary & Outlook Outlook
Future Studies:
What is the role of carbide formation for nucleation?
Different carbon feedstock and different metals
Finally: scan of
parameter space
43
Research Center for Computational Science
(RCCS), Okazaki Research Facilities, National
Institutes for Natural Sciences.
Computer resources :
CREST grant in the Area of High Performance
Computing for Multi-scale and Multi-physics
Phenomena from JST
Academic Center for Computing and Media
Studies (ACCMS), Kyoto University
Funding :
JST Tenure Track Funding by MEXT MSCF (to SI)
Acknowledgements
Center for Nanophase

Materials Sciences
(CNMS),

Oak Ridge National Laboratory

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1

Density-Functional Tight-Binding Molecular

Fill all space with blocks/scan full

Second order-expansion of DFT total energy with respect to charge fluctuation

M. Weinert, J. W. Davenport, Phys. Rev. B 45, 13709 (1992)

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