[molpro-user] Unreasonable T2 norm for CCSD(T) calculation with cc-pCVTZ but not for cc-pCVDZ

Tatiana Korona tania at tiger.chem.uw.edu.pl
Thu Feb 5 15:18:36 GMT 2015


Hi,

If you put

CC_NORM_MAX=100.0 ! some large number

somewhere in your input, it will force CCSD to assume that your T2 norm is 
"reasonable", but of course your CCSD should converge in order to get sensible 
results.

Best wishes,

Tatiana

On Thu, 5 Feb 2015, Paul Jerabek wrote:

> Dear all,
>
> I'm trying to calculate the core electron ionization energy for CO with
> CCSD(T) including core-valence correlation. The problem arises with the
> singly 1s(C) core-electron ionized CO molecule.
>
> With a cc-pCVDT basis I get a nicely converged CCSD(T) result.  When
> using the larger basis cc-pCVTZ, the calculation stops with the
> "unreasonable norm" error and a large value for the t2 norm vector.
>
> Also: The MP2 part of the CCSD(T) calculation won't converge with the
> cc-pCVTZ basis as well, although I overcame this obstacle by playing
> around with the DIIS options: "diis, 1,1,6,1" worked for me.
>
> Do you have any idea what exactly causes the problem at the cc-pCVTZ
> level and how to deal with it this? I'd really like to get the energies
> at the  CCSD(T)/cc-pCVTZ level of theory.
>
> Thank you very much for your help!!
>
> 	Paul
>
>
>
> - Inputs and outputs:
>
>
> My cc-pCVTZ input:
>
>
> basis=cc-pCVTZ
> angstrom
>
> geometry={
> 2
>
> C         0.0000000000        0.0000000000        0.0000000
> O          0.0000000000        0.000000000       -1.12800000
> }
>
> {hf;
> WF, elec=13, sym=1, spin=1;
> }
>
> ! The following creates the 1s(C) core hole:
> {hf,nitord=1;
> WF, elec=13, sym=1, spin=1;
> rotate, 2.1,5.1,0;
> open, 2.1;
> }
>
> {uccsd(t);core;}
>
>
>
> Generating this output for the CCSD(T) part:
>
>
> ____________________________________________
> 1PROGRAM * CCSD (Unrestricted open-shell coupled cluster)     Authors:
> C. Hampel, H.-J. Werner, 1991, M. Deegan, P.J. Knowles, 1992
>
>
> Convergence thresholds:  THRVAR = 1.00D-08  THRDEN = 1.00D-06
>
> CCSD(T)     terms to be evaluated (factor= 1.000)
>
>
> Number of closed-shell orbitals:   6 (   4   1   1   0 )
> Number of active  orbitals:        1 (   1   0   0   0 )
> Number of external orbitals:      79 (  33  19  19   8 )
>
> Memory could be reduced to 2.50 Mwords without degradation in triples
>
> Number of N-1 electron functions:              13
> Number of N-2 electron functions:              78
> Number of singly external CSFs:               382
> Number of doubly external CSFs:            108930
> Total number of CSFs:                      109312
>
> Molecular orbitals read from record     2101.2  Type=RHF/CANONICAL
> (state 1.1)
>
> Integral transformation finished. Total CPU:   0.03 sec, npass=  1
> Memory used:   0.30 MW
>
> Starting RMP2 calculation
>
> ITER.      SQ.NORM     CORR.ENERGY   TOTAL ENERGY   ENERGY CHANGE
>  DEN1      VAR(S)    VAR(P)  DIIS     TIME
>   1      1.26767668    -0.49403951  -102.35576095    -0.49403951
> -0.00556325  0.11D-04  0.88D-01  1  1     0.04
>   2      1.24402423    -0.49386440  -102.35558584     0.00017510
> -0.00474534  0.12D-04  0.75D-01  2  2     0.05
>   3      1.17062309    -0.49303741  -102.35475885     0.00082700
> -0.00214434  0.47D-05  0.19D-01  3  3     0.05
>   4      1.19163131    -0.49336773  -102.35508917    -0.00033032
> -0.00280304  0.37D-05  0.29D-01  4  4     0.06
>   5      1.14022363    -0.49331910  -102.35504054     0.00004862
> -0.00008010  0.35D-06  0.78D-03  5  5     0.07
>   6      1.14287798    -0.49347226  -102.35519370    -0.00015315
> -0.00016096  0.11D-06  0.15D-02  6  6     0.07
>   7      1.13954710    -0.49342221  -102.35514365     0.00005005
> -0.00003111  0.15D-06  0.22D-03  6  1     0.08
>   8      1.13958229    -0.49353959  -102.35526103    -0.00011738
> -0.00000080  0.92D-08  0.13D-03  6  6     0.08
>   9      1.14034754    -0.49350265  -102.35522409     0.00003694
> -0.00001444  0.15D-08  0.25D-03  6  5     0.09
>  10      1.13949383    -0.49358308  -102.35530452    -0.00008043
> -0.00000358  0.15D-08  0.20D-04  6  4     0.09
>  11      1.13948118    -0.49359562  -102.35531706    -0.00001254
> -0.00000445  0.53D-09  0.35D-04  6  2     0.10
>  12      1.13955524    -0.49358821  -102.35530965     0.00000741
> -0.00000303  0.18D-09  0.20D-04  6  3     0.10
>  13      1.13954808    -0.49359154  -102.35531298    -0.00000333
> -0.00000306  0.97D-10  0.22D-04  6  1     0.11
>  14      1.13956163    -0.49358927  -102.35531071     0.00000227
> -0.00000303  0.88D-10  0.23D-04  6  6     0.11
>  15      1.13954749    -0.49359911  -102.35532055    -0.00000983
> -0.00000350  0.66D-10  0.33D-04  6  5     0.11
>  16      1.13957530    -0.49359128  -102.35531272     0.00000783
> -0.00000292  0.40D-10  0.21D-04  6  4     0.12
>  17      1.13975404    -0.49356581  -102.35528725     0.00002547
> -0.00000226  0.53D-10  0.90D-05  6  3     0.12
>  18      1.13969374    -0.49357987  -102.35530131    -0.00001406
> -0.00000223  0.18D-10  0.13D-04  6  2     0.13
>  19      1.13981644    -0.49357693  -102.35529837     0.00000293
> -0.00000248  0.11D-10  0.20D-04  6  4     0.14
>  20      1.13985209    -0.49356639  -102.35528782     0.00001055
> -0.00000197  0.22D-10  0.70D-05  6  2     0.15
>  21      1.13967732    -0.49359340  -102.35531484    -0.00002702
> -0.00000330  0.14D-10  0.37D-04  6  3     0.16
>  22      1.13978183    -0.49358187  -102.35530331     0.00001154
> -0.00000266  0.18D-10  0.24D-04  6  2     0.16
>  23      1.13985227    -0.49356499  -102.35528643     0.00001688
> -0.00000212  0.20D-10  0.72D-05  6  3     0.17
>  24      1.13968904    -0.49359119  -102.35531263    -0.00002620
> -0.00000296  0.15D-10  0.30D-04  6  2     0.17
>  25      1.13977038    -0.49358362  -102.35530506     0.00000757
> -0.00000278  0.17D-10  0.27D-04  6  3     0.18
>  26      1.13982646    -0.49356695  -102.35528839     0.00001667
> -0.00000200  0.19D-10  0.69D-05  6  2     0.19
>  27      1.13969005    -0.49359153  -102.35531297    -0.00002458
> -0.00000303  0.15D-10  0.32D-04  6  3     0.19
>  28      1.13976301    -0.49358524  -102.35530668     0.00000629
> -0.00000296  0.17D-10  0.30D-04  6  2     0.20
>  29      1.13978672    -0.49357212  -102.35529356     0.00001313
> -0.00000181  0.17D-10  0.60D-05  6  3     0.21
>
> ?CONVERGENCE NOT REACHED AFTER MAX. ITERATIONS
>
> Spin contamination <S**2-Sz**2-Sz>     0.01026906
>  Reference energy                   -101.861721439818
>  RHF-RMP2 correlation energy          -0.493572115599
> !RHF-RMP2 energy                    -102.355293555417
>
> Starting UCCSD calculation
>
> ITER.      SQ.NORM     CORR.ENERGY   TOTAL ENERGY   ENERGY CHANGE
>  DEN1      VAR(S)    VAR(P)  DIIS     TIME
>   1      7.56966322    -0.48016065  -102.34188209    -0.48016065
> -0.31678089  0.58D-02  0.61D+01  1  1     0.36
>
> UNREASONABLE NORM. CALCULATION STOPPED
>
> Norm of t1 vector:      0.09135834      S-energy:    -0.00521914
> T1 diagnostic:  0.01443667
>
> D1 diagnostic:  0.03480135
> Norm of t2 vector:      2.56150676      P-energy:    -0.47494151
>                                         Alpha-Beta:  -0.37116672
>                                         Alpha-Alpha: -0.04996811
>                                         Beta-Beta:   -0.05380668
>
> Doubles amplitudes (print threshold =  0.500E-01):
>
>         I         J         SYM. A    SYM. B    A         B      T(IJ,
> AB) [Alpha-Alpha]
>
>         7         6         2         3         1         1      0.05116033
>         7         6         3         2         1         1     -0.05116033
>
>         I         J         SYM. A    SYM. B    A         B      T(IJ,
> AB) [Beta-Beta]
>
>         3         2         1         1         1        21      0.11558142
>         3         2         1         1        21         1     -0.11558142
>         4         2         1         1         1        21      0.09454732
>         4         2         1         1         1        22      2.11412607
>         4         2         1         1        21         1     -0.09454732
>         4         2         1         1        22         1     -2.11412607
>
>         I         J         SYM. A    SYM. B    A         B      T(IJ,
> AB) [Alpha-Beta]
>
>         3         2         1         1        21         1      0.21097982
>         3         2         1         1        22         1      0.05146041
>         2         3         1         1        21         1      0.29802902
>         2         3         1         1        22         1      0.07194777
>         4         2         1         1        22         1      0.26354643
>         2         4         1         1        21         1      0.06646343
>         2         4         1         1        22         1      1.31945707
>         6         6         2         2         1         1     -0.09221865
>         7         7         3         3         1         1     -0.09221865
>         7         6         3         2         1         1     -0.06479562
>         6         7         2         3         1         1     -0.06479562
>
> ?ERROR: NO CONVERGENCE. TRIPLES WILL NOT BE DONE. THIS CAN BE AVOIDED
> USING THE NOCHECK OPTION.
>
> Spin contamination <S**2-Sz**2-Sz>     0.08566146
>
>
>  Correlated core orbitals:             1.1       2.1
>  Orbital energies:                   -21.2251   -2.0818
>
>  UCCSD core-core energy               -0.055641118427
>  UCCSD core-valence energy            -0.112063864274
>  UCCSD valence correlation energy     -0.312455667665
>
>
> RESULTS
> =======
>
>  Reference energy                   -101.861721439818
>  UCCSD singles energy                 -0.005219140527
>  UCCSD pair energy                    -0.474941509839
>  UCCSD correlation energy             -0.480160650366
>
> !RHF-UCCSD energy                   -102.341882090184
>
> Program statistics:
>
> Available memory in ccsd:               799999438
> Min. memory needed in ccsd:                363878
> Max. memory used in ccsd:                  491028
> Max. memory used in cckext:                437954 ( 1 integral passes)
> Max. memory used in cckint:                302473 ( 1 integral passes)
>
>
> ? Error
> ? No convergence. This error exit can be avoided using the NOCHECK option
> ? The problem occurs in ccsd
> ____________________________________________
>
>
>
> My cc-pCVDZ input is as follows:
>
>
>
> basis=cc-pCVDZ
> angstrom
>
> geometry={
> 2
>
> C         0.0000000000        0.0000000000        0.0000000
> O          0.0000000000        0.000000000       -1.12800000
> }
>
> {hf;
> WF, elec=13, sym=1, spin=1;
> }
>
> ! The following creates the 1s(C) core hole:
> {hf,nitord=1;
> WF, elec=13, sym=1, spin=1;
> rotate, 2.1,5.1,0;
> open, 2.1;
> }
>
> {uccsd(t);core;}
>
>
>
>
> Generating this output for the CCSD(T) part:
>
> ____________________________________________
> 1PROGRAM * CCSD (Unrestricted open-shell coupled cluster)     Authors:
> C. Hampel, H.-J. Werner, 1991, M. Deegan, P.J. Knowles, 1992
>
>
> Convergence thresholds:  THRVAR = 1.00D-08  THRDEN = 1.00D-06
>
> CCSD(T)     terms to be evaluated (factor= 1.000)
>
>
> Number of closed-shell orbitals:   6 (   4   1   1   0 )
> Number of active  orbitals:        1 (   1   0   0   0 )
> Number of external orbitals:      29 (  13   7   7   2 )
>
> Memory could be reduced to 0.46 Mwords without degradation in triples
>
> Number of N-1 electron functions:              13
> Number of N-2 electron functions:              78
> Number of singly external CSFs:               154
> Number of doubly external CSFs:             16890
> Total number of CSFs:                       17044
>
> Molecular orbitals read from record     2101.2  Type=RHF/CANONICAL
> (state 1.1)
>
> Integral transformation finished. Total CPU:   0.01 sec, npass=  1
> Memory used:   0.10 MW
>
> Starting RMP2 calculation
>
> ITER.      SQ.NORM     CORR.ENERGY   TOTAL ENERGY   ENERGY CHANGE
>  DEN1      VAR(S)    VAR(P)  DIIS     TIME
>   1      1.12409217    -0.38855487  -102.17840478    -0.38855487
> -0.00170845  0.11D-04  0.75D-03  1  1     0.01
>   2      1.12590721    -0.39038223  -102.18023214    -0.00182737
> -0.00000500  0.11D-06  0.21D-05  2  2     0.01
>   3      1.12598549    -0.39044480  -102.18029471    -0.00006257
> -0.00000003  0.15D-08  0.19D-07  3  3     0.01
>   4      1.12599306    -0.39045144  -102.18030135    -0.00000664
> -0.00000000  0.21D-10  0.16D-09  4  4     0.01
>   5      1.12599334    -0.39045148  -102.18030139    -0.00000003
> -0.00000000  0.21D-12  0.11D-11  5  5     0.01
>
> Norm of t1 vector:      0.03516262      S-energy:    -0.00321409
> T1 diagnostic:  0.00027154
> Norm of t2 vector:      0.35320947      P-energy:    -0.38723739
>                                         Alpha-Beta:  -0.29058556
>                                         Alpha-Alpha: -0.04917439
>                                         Beta-Beta:   -0.04747745
>
> Spin contamination <S**2-Sz**2-Sz>     0.00993509
>  Reference energy                   -101.789849910161
>  RHF-RMP2 correlation energy          -0.390451477943
> !RHF-RMP2 energy                    -102.180301388104
>
> Starting UCCSD calculation
>
> ITER.      SQ.NORM     CORR.ENERGY   TOTAL ENERGY   ENERGY CHANGE
>  DEN1      VAR(S)    VAR(P)  DIIS     TIME
>   1      1.11229466    -0.36958544  -102.15943535    -0.36958544
> -0.01717517  0.42D-02  0.36D-02  1  1     0.03
>   2      1.12851095    -0.38441097  -102.17426088    -0.01482553
> -0.00248284  0.26D-03  0.81D-03  2  2     0.06
>   3      1.13880762    -0.38898714  -102.17883705    -0.00457618
> -0.00050990  0.11D-03  0.12D-03  3  3     0.08
>   4      1.14645710    -0.39199507  -102.18184498    -0.00300793
> -0.00018231  0.27D-04  0.36D-04  4  4     0.10
>   5      1.15013310    -0.39273917  -102.18258908    -0.00074409
> -0.00008220  0.32D-05  0.20D-04  5  5     0.12
>   6      1.15221476    -0.39315130  -102.18300121    -0.00041214
> -0.00004124  0.21D-05  0.11D-04  6  6     0.15
>   7      1.15307829    -0.39342898  -102.18327889    -0.00027767
> -0.00002168  0.40D-05  0.50D-05  6  1     0.18
>   8      1.15336241    -0.39346566  -102.18331557    -0.00003668
> -0.00001331  0.32D-05  0.28D-05  6  3     0.20
>   9      1.15401855    -0.39372727  -102.18357718    -0.00026161
> -0.00000572  0.67D-06  0.16D-05  6  2     0.22
>  10      1.15437935    -0.39378095  -102.18363086    -0.00005368
> -0.00000179  0.11D-06  0.60D-06  6  5     0.24
>  11      1.15480576    -0.39385868  -102.18370859    -0.00007773
> -0.00000043  0.98D-07  0.95D-07  6  4     0.26
>  12      1.15491062    -0.39385889  -102.18370881    -0.00000022
> -0.00000019  0.48D-07  0.43D-07  6  6     0.29
>  13      1.15498805    -0.39386528  -102.18371519    -0.00000638
> -0.00000006  0.75D-08  0.18D-07  6  1     0.31
>  14      1.15500282    -0.39386034  -102.18371025     0.00000494
> -0.00000002  0.13D-08  0.47D-08  6  3     0.33
>  15      1.15500066    -0.39385580  -102.18370571     0.00000454
> -0.00000001  0.34D-09  0.20D-08  6  2     0.36
>  16      1.15499853    -0.39385514  -102.18370505     0.00000066
> -0.00000001  0.49D-09  0.18D-08  6  5     0.38
>
> Norm of t1 vector:      0.12340148      S-energy:    -0.00480873
> T1 diagnostic:  0.01684129
>
> D1 diagnostic:  0.03924278
> Norm of t2 vector:      0.37385907      P-energy:    -0.38904641
>                                         Alpha-Beta:  -0.31570541
>                                         Alpha-Alpha: -0.03770254
>                                         Beta-Beta:   -0.03563847
>
> Singles amplitudes (print threshold =  0.500E-01):
>
>         I         SYM. A    A   T(IA) [Alpha-Alpha]
>
>         6         2         1      0.06824784
>         7         3         1      0.06824784
>
> Doubles amplitudes (print threshold =  0.500E-01):
>
>         I         J         SYM. A    SYM. B    A         B      T(IJ,
> AB) [Alpha-Beta]
>
>         4         4         2         2         1         1     -0.05458637
>         4         4         3         3         1         1     -0.05458637
>         6         6         2         2         1         1     -0.12357167
>         7         7         3         3         1         1     -0.12357167
>         5         6         2         1         1         1     -0.05688095
>         5         7         3         1         1         1     -0.05688095
>         7         6         3         2         1         1     -0.07404280
>         6         7         2         3         1         1     -0.07404280
>
> Spin contamination <S**2-Sz**2-Sz>     0.00671828
>
> Memory could be reduced to 0.51 Mwords without degradation in triples
>
>
>  Correlated core orbitals:             1.1       2.1
>  Orbital energies:                   -21.2420   -2.0950
>
>  UCCSD core-core energy               -0.044277318985
>  UCCSD core-valence energy            -0.067552227320
>  UCCSD valence correlation energy     -0.282025593229
>
>
> RESULTS
> =======
>
>  Reference energy                   -101.789849910161
>  UCCSD singles energy                 -0.004808728256
>  UCCSD pair energy                    -0.389046411278
>  UCCSD correlation energy             -0.393855139534
>  Triples (T) contribution             -0.014392247539
>  Total correlation energy             -0.408247387073
>
>  RHF-UCCSD energy                   -102.183705049695
>  RHF-UCCSD[T] energy                -102.199882100889
>  RHF-UCCSD-T energy                 -102.197637602862
> !RHF-UCCSD(T) energy                -102.198097297234
>
> Program statistics:
>
> Available memory in ccsd:               799999438
> Min. memory needed in ccsd:                 61788
> Max. memory used in ccsd:                   81128
> Max. memory used in cckext:                112394 (16 integral passes)
> Max. memory used in cckint:                 98436 ( 1 integral passes)
> ____________________________________________
>
>
>
> -- 
> Dr. Paul Jerabek
> Fachbereich Chemie, AK Berger, Theoretische Chemie
> Philipps-Universität Marburg
> Hans-Meerwein-Strasse
> D-35032 Marburg
> Germany
>
> Phone: +49-(0)6421-28-27001
>
> _______________________________________________
> Molpro-user mailing list
> Molpro-user at molpro.net
> http://www.molpro.net/mailman/listinfo/molpro-user
>

Dr. Tatiana Korona http://tiger.chem.uw.edu.pl/staff/tania/index.html
Quantum Chemistry Laboratory, University of Warsaw, Pasteura 1, PL-02-093 Warsaw, POLAND


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