Next Generation Supercomputer Project(GFlops)

Next
NextGeneration
GenerationSuperSuper Computer
Computer

1.0E+08
Todai
1st in TOP500
10th in TOP500

1.0E+07
1.0E+06

Earth Simulator
35.6 TFLOPS, 5120 nodes

Peta

1.0E+05
1.0E+04
1.0E+03Tera

1.0E+02
1.0E+01

Earth Simulatorより280倍の計算速度
Earth Simulatorより10倍以上の並列度

1.0E+00

Giga201320
112009

2007

2005

2003

2001

1999

1997

1995

1993

1991

1989

1987

1985

1983

1.0E-01(Year)

Nano-Bio Simulation
With the emergence of petascale computing platforms
computational chemistry is on the verge of entering a new era ofmodeling. It will enable us to tackle scientific problems that larger
and more complex, more realistic than ever before, and to include
more of the complex dynamical behavior of nature. Petascalecomputing should be science driven.

Biomolecules

Nano-scale molecules• Simulations for larger and more complex,
more realistic systems• Very Accurate results• Chemistry at periodic interfaces• Coupling multiple scales• Benchmarking abilities• Heavy element chemistry

大規模分子系への理論化学の展開¾ 波動関数法（ab initio MO法）
体系的理論、近似を上げれば厳密解に収束小さな系では極めて精度の高い結果を与える
計算時間の系の大きさ(N)依存性が大きい（計算時間がかかりすぎる）

N依存性を下げる理論、アルゴリズムの開発¾ 電子密度法（密度汎関数法）
簡潔で概念的、精度は汎関数に依存
半定量的理論であり、大きな系に適用可能
2次の分子物性、van der Waals力や励起状態の記述は悪い

より良い汎関数の開発

Gaussian and FE Coulomb Approach
CPU timehourO(N2.9)75
5025O(N2.4)
O(N1.1)O(N0.9)# of basis functions
1D Alanine α-helix chain/ SVP

Gaussian and FE Coulomb Approach
CPU timehour

O(N2.9)125O(N2.5)100
7550O(N2.6)
25962 atoms
10,660 basis functions
Total cpu 198 hours
on IBM Power 5O(N1.2)# of basis functions
3D diamond/ SVPEnergy Gradient
Gaussian and FE Coulomb Approach
CPU timehour
48
Analytical
GFC

36O(N3.2)

2412O(N1.3)
001000

2000
3000# ofäÓíÍä÷êîÇÃêî
basis functions

3D diamond/ SVP

4000

長距離補正の汎関数 (LC-DFT)
電子間反発 1/r12 をEwald分割法を利用して長距離、短距離部分に分け、短距離部はDFT汎関数、長距離部はHartree-Fock交換で表現⎞⎛ 1
1= L(r12 ) + ⎜⎜ − L(r12 ) ⎟⎟r12⎠⎝ r12⎛
erf (μr12 )⎜⎜ L(r12 ) =,r12⎝

erf (μr12 ) 2 μ −(1 / a ) μ 2 r12 2 ⎞e, L⎟⎟−r12π⎠

651 erf (μr12 ) 1 − erf (μr12 )=+r12r12r124

1 − erf ( μr12 )r1231r12erf ( μr12 )r122
1

HF exchange GGA exchange

0.5

1

1.5

2

2次の分子物性の改善
励起エネルギー計算の平均誤差(eV)Hyperpolarizabilityの改善

27 valence excitations (N2, CO, H2CO, C2H4, C6H6)

B3LYP

BLYP
B3LYP
LC-BLYP
SAC-CI

41 Rydberg excitations (N2, CO, H2CO, C2H4, C6H6)

MP2
LC-BOP
HF

ω CT (R ) - ω CT (5.0 Å ) (eV)

2.0

LC-BOP
BOP
AC-BOPLC-PBEOPPBEOPLC-BLYPBLYP
B3LYP
SVWNSAC-CI

1.5

1.0

0.36
0.37
0.32
0.37

BLYP
B3LYP
LC-BLYP
SAC-CI

1.54
0.89
0.41
0.19

CT励起状態の記述
C2F4R
C2H4ΔECT(eV)

0.50.05678

Intramolecule distance R (Å)

910

BLYP
B3LYP
LC-BLYP
Exptl.

5.40
7.49
12.49
12.5

van der Waals分子の記述
Naphthalene Dimer

ClF…He

これまでのGGA汎関数はすべてrepulsive

これまでの汎関数はLinear structuresのみを与える
Our DFT with aug-cc-pVQZ

HeCollinear minimum : -76.43 cm-1
(Re = 3.41Å）

Our DFT with 6-31+G**

R8PC
TPD
P CCSD(T)C CCSD(T)T CCSD(T)PD CCSD(T)

6E (kcal/mol)

42Cl

Ө

T-shaped minimum:-46.53 cm-1
(Re=3.19Å,θe=70.0°)

Antilinear minimum:-30.04 cm-1
(Re=3.91Å）

FCCSD(T) with aug-cc-pVQZ+BF(3s3p2d2f1g)

0
Collinear minimum : -63.53 cm-1
(Re = 3.54Å）-2

T-shaped minimum:-41.09 cm-1
(Re=3.23Å,θe=70.1°)-4
Antilinear minimum:-33.80 cm-1
(Re=3.95Å)

-6-8

2.8

3.4

4

4.6
5.2
R (Angstrom)

5.8

6.4

Our DFT
6.16 kcal/mol
CBS CCSD(T) 5.73 kcal/mol7in cm-1

5 0 .0
4 5 .0)mo
ta 4 0 .0/Ve 3 5 .0m(ygre 3 0 .0nenoit 2 5 .0ailo
f 2 0 .0xE
1 5 .0Exfoliation energies per C-atom in polycyclic aromatichydrocarbon trimers (LC-BOP/6-31++G**)
Experimental data 35, 43, 52 meVPrevious calculation 8 ~170 meV

37.3
36.1

34.0
34.1

29.5

35.2

32.3 (69.0)
28.5 (49.1)

Present (MP2)17.9

d im e rt r im e r

17.4 (34.4)

1 0 .0(C6H6)3 (C24H12)3 (C54H18)3(C96H24)3(C150H30)3

UTChemプロジェクト - 理論の実用化
理論化学のソフトウエアは物質科学の共通基盤
ソフトウエアの研究開発は欧米に大きく遅れをとる
世界の分子軌道プログラム・パッケージ
••••
••
•

DALTON
Gaussian (Gaussian, Inc.)GAMESS (Iowa State Univ.)
MolproMolcas (Lund Univ.)
NWChem (PNNL)
Q-Chem (Q-Chem, Inc.)

なぜ新しいソフトウェアが必要か(1) 既存のプログラムを使うことで，多くの恩恵を受けてきた。しかし、プログラムの制限で真のブレークスルーは成し難い。
(2) 既存のプログラムでは取り扱うことができない重要で強力な方法論が多く存在する。

Ab initio MO, DFT, and Dynamics
非相対論、相対論(2成分、4成分相対論理論)
CISD, CISDT, CISDTQ,CCSD, CCSDT, CCSDTQ,
MP2, MP3, and MP4,パラレル版も用意

http://utchem.qcl.t.u-tokyo.ac.jp/

Conclusions
With the emergence of petascale computing platforms
computational quantum chemistry is on the verge ofentering a new era of modeling. It will enable us totackle scientific problems that larger and more realistic
than ever before, and to include more of the complex
dynamical behavior of nature. Of course much moreremains to be achieved but

Let’s Do More Chemistry with Computers!