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Transcript of CC and CI in terms that even a Physicist can understand Karol Kowalski William R Wiley Environmental...
![Page 1: CC and CI in terms that even a Physicist can understand Karol Kowalski William R Wiley Environmental Molecular Sciences Laboratory and Chemical Sciences.](https://reader038.fdocuments.us/reader038/viewer/2022110209/56649e2a5503460f94b1865d/html5/thumbnails/1.jpg)
CC and CI in terms that even a Physicist can understand
Karol KowalskiWilliam R Wiley Environmental Molecular Sciences
Laboratory and Chemical Sciences Division,Pacific Northwest National Laboratory
![Page 2: CC and CI in terms that even a Physicist can understand Karol Kowalski William R Wiley Environmental Molecular Sciences Laboratory and Chemical Sciences.](https://reader038.fdocuments.us/reader038/viewer/2022110209/56649e2a5503460f94b1865d/html5/thumbnails/2.jpg)
How it started
Coester & Kummel (1958,1960)Čižek (1966)Paldus & Čižek (1971)Bartlett MonkhorstMukherjeeLindgrenKutzelnigg… and many others
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CC reviews
J. Paldus, X. Li, “A critical assessment of coupled cluster methods in quantum chemistry,” Advances in Chemical Physics 110, 1 (1999).R.J. Bartlett, M. Musial, “Coupled-cluster theory in quantum chemistry,” Reviews of Modern Physics 79, 291 (2007).
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What we want to solve
4
EH
Molecular/Atomic Physics, Quantum Chemistry
(electronic Schrödinger equations)
Nuclear Physics
Solid State Physics
Many Particle Systems
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Exact solution of Schrödinger equation
5
Weyl formula (dimensionality of full configuration interaction space) – exact solution of Schrödinger equation
12/
1
2/
1112),,(
SN
n
SN
nnSSNnf
!!!10 config. FCI#
:orbitals 100 electrons, 12
:molecule C
17
2
n – total number of orbitals
N – total number of correlated electrons
S – spin of a given electronic state
Efficient approximations are needed
![Page 6: CC and CI in terms that even a Physicist can understand Karol Kowalski William R Wiley Environmental Molecular Sciences Laboratory and Chemical Sciences.](https://reader038.fdocuments.us/reader038/viewer/2022110209/56649e2a5503460f94b1865d/html5/thumbnails/6.jpg)
Approximate wavefunction (WF) methods
Hartree-Fock method (single determinant) EHF is used to define the correlation energy E E=E-EHF
In molecules EHF accounts for 99% of total energy but without E making any reliable predictions is
impossibleCorrelated methods (going beyond single determinant description)
Configuration interaction method (linear parametrizaton of WF) Perturbative methods (MBPT-n)Coupled Cluster methodsand many other approaches
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Many-Fermion Systems
Creation/annihilation operators
Second quantized form of the Hamiltonian (welcome to the Fock space)
7
},{
0},{
0},{
aa
aa
aaIndices & designate the one particle states: in chemistry spinorbitals
, ,,,41
0 aaaavaahEH
Annn HHH )...( 1111
n times
F=
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Wick Theorem
The basic tool in deriving CC equations
Commutator of two operators A & B
8
BA, represented by connecteddiagrams only
]...[]...[... 212121 kkk MMMNMMMNMMMM
aa
In normal product of the operator string M (N[M]) all the creations operator are permuted to the left of all annihilation operators, attaching (+/-) phase depending on the parity of the required permutation.
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Particle-hole formalism
Special form of the Bogoliubov-Valatin transformation (choosing a new Fermi Vacuum)
9
aa
iab
if
if
aa
iab
if
if
Slater determinant
i,j,k,… occupied single particle statesa,b,c, …. unoccupied single particle states
0b
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CC and CI methods
CI formalism
10
)...1(
)...(
21
210
N
N
CCC
DDDD
Intermediate normalization
reference function(HF determinant)
1
n
n
nn
n
n
aaii
iiaaaaiin aaaac
nC
......
......2
1
1
11
1
1......
)!(
1
n
nnn
aaiiiiaa aaaa ...
...1
111......
baji
ijabcC2
N stands for the number of electrons
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CC and CI methods
CC method
11
TeNTTTTT ...321
Intermediate normalization 1
n
n
nn
n
n
aaii
iiaaaaiin aaaat
nT
......
......2
1
1
11
1
1......
)!(
1
cluster amplitudes
)...1( !13
!312
!21 N
N TTTT
For fermions the expansion for eT terminates (Pauli principle)
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CI and CC methods
Full CI and full CC expansions are equivalent (and this is the only case when CI=CC)
12
TeC)1(
...
4124
12
212
1222
13144
316
12133
212
122
11
TTTTTTTC
TTTTC
TTC
TC
CI amplitudes are calculated from the variational principle while the cluster amplitudes are obtained from projective methods
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CC formalism
Working equations:
13
TT EeHe
EHee TT
| Te
CT
TT
He
TTTTHTTTHTTHTHHHee
)(
]}],],],,[[[[]],],,[[[]],,[[],[{ !41
!31
21
From Campbell-Hausdorff formula
...]],],,[[[]],,[[],[ !31
21 BBBABBABAAAee BB
We get
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CC formalism
Separating the equations for cluster amplitudes from the equation for energy
14
P
Nn
aaii
aaii
aaii
n
n
n
n
n
nQ
,...,1...
...
......
......
1
1
1
1
1
1
0)( CTHeQ
CTHeE )(
QP 1
Step1: we solve energy independent equations for cluster amplitudes
Step 2 :having cluster amplitudes we Can calculate the energy
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Approximations: CCD
CC with doubles (CCD):
15
2TT
bajiCTab
ij He ; 0)( 2
bajiCabij HTHTH ;
222
12 0)(
CT
CCD HeE )( 2
CHFCCCD HTETHE )())1(( 22
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Approximations: CCD
16
NNN VFHHH
,
][ aaNfFN
,,,41 ][ aaaaNvVN
||v
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Approximations: CCSD
CC with singles and doubles (CCSD):
17
bajiCTTab
ij He ; 0)( 21
aiCTTa
i He ; 0)( 21
CHF
CTT
CCSD
HTHTE
HeE
)(
)(2
121
2
21
21 TTT
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CCSD and Thouless Theorem
Thouless theorem
CCSD wavefunction
CCSD provides better description of the static correlation effects (than the CCD approach)
18
& two Slater determinants 0
1 Te
21221 1 TTTTTCCSD eeee
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CC approximations: CCSDT
CC with singles, doubles, and triples (CCSDT):
19
321 TTTT
bajiCTTTab
ij He ; 0)( 321
aiCTTTa
i He ; 0)( 321
cbakjiCTTTabc
ijk He ; 0)( 321
CHF
CTT
CCSDT
HTHTE
HeE
)(
)(2
121
2
21
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CC and Perturbation Theory (Linked Cluster Theorem)
Linked Cluster Theorem states:Perturbative expansion for the energy is expressed in terms of closed (having no external lines) connected diagrams onlyPerturbative expansion for the wavefunction is epxressed in terms of linked diagrams (having no disconnected closed part) only
20
E ....
.... .... ....
)1(2T )1(
2T)1(
2T)3(
2T
Cluster operator T is represented by connected diagrams only
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CC and Perturbation Theory
Enable us to categorize the importance of particular cluster amplitudes
Enable us to express higher-order contributions through lower-order contribution (CCSD(T))
21
...
...
...
...
)3(44
)2(33
)1(22
)2(11
TT
TT
TT
TT
2)0(
33 TVRT N
]5[]4[)( EEEE CCSDTCCSD
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CCSD(T) method
Driving force of modern computational chemistry (ground-state problems)Belongs to the class of non-iterative methodsEnable to reduce the cost of the inclusion of triple excitations to no
3nu4 (N7) : required triply excited
amplitudes can be generated on-the-fly.Storage requirements as in the CCSD approach
22
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Size-consistency of the CC energies
23
A BR
BABA HHH
Cluster operator is represented by the connected diagrams only:
BA TTT
BATT BAee
BA EEE
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Numerical cost
24
Method Numerical Complexity
Global MemoryRequirements
CCSD N6 N4
CCSD(T) N7 N4
CCSDT N8 N6
CCSDTQ N10 N8
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Equation-of-Motion Coupled Cluster Methods: Excited-State CC extension
TKK eR
“excitation” operator
reference function (HF determinant) Te0
cluster operator
KKK RERH TTHeeH
KKK RERHsimilarity transformed Hamiltonian
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EOMCCSD: singly-excited states
EOMCCSDT: singly and doubly excited states
Perturbative methods: EOMCCSD(T) formulations
26
Equation-of-Motion Coupled Cluster Methods: Excited-State CC extension
21)( 2,1,,TT
KKoKEOMCCSDK eRRR
321)( 3,2,1,,TTT
KKKoKEOMCCSDTK eRRRR
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CC methods: across the energy and spatial scales
CC methods can be universally applied across energy and spatial scales!
Bartlett, Musial Rev. Mod. Phys. (2007)Dean, Hjorth-Jensen, Phys. Rev. B (2004)
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Performance of the CC methods
28
K. Kowalski,D.J. Dean, M. Hjorth-Jensen,T. Papenbrock, P. Piecuch, PRL 92, 132501 (2004)
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Performance of the CC method
29
R.J. Bartlett Mol. Phys. 108, 2905 (2010).
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Performance of the CC methods
30
Bartlett & Musial, Rev. Mod. Phys.
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Illustrative examples of large-scale excited-state calculations – components of light harvesting systems
1 2 3 4 5 6 71.5
2
2.5
3
3.5
4
4.5
5
5.5
1La state POL1 basis set
Expt.
EOMCCSD
CR-EOMCCSD(T)
Number of rings
Exc
itat
ion
en
erg
y (e
V)
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32
Functionalization of porphyrines
System Leading excitations CR-EOMCCSD(T) (eV)
H L, H-1L+1
H-1L, HL+1
2.32 (Expt. 2.27 eV)
1.86 (Expt. 1.91 eV)
HL, H-1L+1,H-2L+2, H-3L+3
1.91 (Expt. 1.84 eV)
H L 1.78
H L 1.36
K. Kowalski, S. Krishnamoorthy, O. Villa, J.R. Hammond, N. Govind, J. Chem. Phys. 132, 154103 (2010); K. Kowalski, R.M. Olson, S. Krishnamoorthy, V. Tipparaju, E. Apra, J. Chem. Theory Comput. 7, 2200 (2011)
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Multiscale Approaches: localized excited states in extended systems
33
Visible Light Photoresponse of pure and N-doped TiO2 (active-space EOMCCSD calculations, 400 correlated electrons):TiO2 EOMCCSd 3.84 eVN-doped TiO2 EOMCCSd 2.79 eV
N. Govind, K. Lopata, R. Rousseau, A. Andersen, K. Kowalski, J. Phys. Chem. Lett. “Visible Light Absorption of N-Doped TiO2 Rutile Using (LR/RT)-TDDFT and Active Space EOMCCSD Calculations,” J. Phys. Chem. Lett. 2, 2696 (2011).
Localized excited-states in materials
catalysisphotocatalytic decomposition of organic pollutantsphotolysis of watersolar energy conversion
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Why CC method is so popular in computational chemistry (and less popular in
physics)???Simpler form of the interactions (1/r)CC functionalities are available in many quantum chemistry packages
ACES III (parallel)CFOUR (some pieces in parallel)
DALTON (serial)
GAMESS (CCSD/CCSD(T) – parallel)Gaussian (serial)
MOLPRO (parallel)
NWCHEM (parallel)
PQS (CCSD/CCSD(T) – parallel)
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Tensor Contraction Engine (TCE)
Highly parallel codes are needed in order to apply the CC theories to larger molecular systems Symbolic algebra systems for coding complicated tensor expressions: Tensor Contraction Engine (TCE)
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Parallel performance
Parallel structure of the TCE CC codes
Tile structure:
Occupied spinorbitals
unccupied spinorbitals
S1 S2 … S1 S2 … S1 S2 ………. S1 S2 ……….
Tensor structure:
][][m
n
hp
ia TT
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An example of the scalability of the triples part of the CR-EOMCCSD(T) approach for GFPC described by the cc-pVTZ basis set (648 basis set functions). Timings were determined from calculations on the Franklin Cray-XT4 computer at NERSC using 1024, 16384, 20000, 24572, and 34008 cores).
Parallel performance
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38
Scalability of the triples part of the CR- EOMCCSD(T) approach for the FBP-f-coronene system in the AVTZ basis set. Timings were determined from calculations on the Jaguar Cray XT5 computer system at NCCS.
Scalability of the non-iterative EOMCC code
94 %parallel efficiency using 210,000 cores
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Scalability of the iterative EOMCC methods
39
Alternative task schedulers
use “global task pool” improve load balancing reduce the number of synchronization steps to absolute minimumlarger tiles can be effectively used
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Towards future computer architectures
speed
up
The CCSD(T)/Reg-CCSD(T) codes have been rewritten in order to take advantage of GPGPU acceleratorsPreliminary tests show very good scalability of the most expensive N7 part of the CCSD(T) approach
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Concluding remark
If you know the nature of the interactions in your system there is a good chance that the CC methods will give you the right results for the right reasons (assuming you have an access to a large computer)
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42
THANK YOU