Input Manual
Version 1.1

Copyright (C) 2019 Nakai group
Department of Chemistry and Biochemistry,
School of Advanced Science and Engineering, Waseda University
All rights reserved.

1

Table of Contents
Input File
Job Options
Molecular Information
Basis Sets
Basis Sets 2
Core Potential$MOA, $MOB, $MOG
Job Options$Run$Wavefunction$Hamiltonian$Mol$Basis$Integral$Guess
$SCF
$MP2
$DFT
$TDDFT$Opt$Property$FCP$TCE
Basis Set Library
Minimal STO-nG Basis Sets
Pople Basis Sets
Sapporo Basis Sets
Correlation-Consistent Basis Sets
Polarization-Consistent Basis Sets
Others2

Input File
The input file in RAQET consists of the following main sections:
1. Job Options

specifies general options for the calculation

2. Molecular Information

specifies molecular structure

3. Basis Sets

specifies atomic basis sets

4. Basis Sets 2

specifies atomic basis sets for initial guess (not required if
GuessMethod=Hcore)

5. Core Potential

specifies options for core potentials (not mandatory)

6. $MOA, $MOB, $MOG

specifies initial MO coefficients when using MO read-in(not mandatory)

Job Options
In this section, the general calculation options are specified. A complete list of the options canbe found in the Job Options section. Each section begins with $[option name], ends with $end,
and can contain several keywords. Each keyword and its parameters have to be specified in a
new line as shown in the following example:$Run
JobType=sp
Mem=1000MB$end

Molecular Information
The molecular structure is specified in this section. Besides the element symbols and therespective Cartesian coordinates (in Å), atom-specific basis sets and those used for the initial
guess can be declared. The molecular structure section is initiated by molecular information in
the first line. All subsequent lines follow the format
Element symbol[basis set][basis set (2)]

x

y

z

Input in [] is not mandatory. The definition of atom-specific basis sets will overwrite the basis
sets defined in the Basis Sets and Basis Sets 2 sections. As separator, spaces have to be used,
not tabs. As an example of a minimal sample input, the molecular structure of the formaldehyde
molecule is shown.
molecular information
C
0.000000 0.000000
O
0.000000 1.219457

0.000000
0.0000003

H
H

0.465617 -0.542208 0.815579
0.465617 -0.542208 -0.815579

In this example, the basis set specified in the Basis Sets section is used. The same molecular
structure with atom-specific basis set input (here for the case of the 6-31G(d,p) basis set) reads
molecular information
C DB:/6-31G(d,p)/C
0.000000 0.000000 0.000000
O DB:/6-31G(d,p)/O
0.000000 1.219457 0.000000
H DB:/6-31G(d,p)/H
0.465617 -0.542208 0.815579
H DB:/6-31G(d,p)/H
0.465617 -0.542208 -0.815579
Note that also a mixture of atom-specific basis sets and global basis sets is possible. In thiscase, atoms without atom-specific basis sets will use the basis sets defined in the sections
Basis Sets and Basis Sets 2, while atom-specific bases will overwrite the global definition for theother atoms.

Basis Sets
In this section, the atomic basis set is specified. The declaration of the global basis set (for all
atoms) follows the format:
basis sets = 6-31G(d,p)
Element-specific basis sets overwriting the global basis set, e.g. for heavy elements, can be
declared bybasis sets = Sapporo-DZP-2012
Rh DB:Sapporo-DKH3-DZP-2012/Rh
Ir DB:Sapporo-DKH3-DZP-2012/Ir
Basis sets can be also specified explicitly, i.e. the angular momentum, basis function exponents,
contraction coefficients, and the number of contracted primitives are given explicitly for eachshell of a specific element. In the following, you can find a sample basis set input for hydrogenand oxygen without declaring a global basis set:basis sets
O
S
6
1.00
5484.6717000
825.2349500
188.0469600
52.9645000

0.0018311
0.0139501
0.0684451
0.2327143
4

SP

SP
D

H
S

S

16.8975700
5.7996353
3
1.00
15.5396160
3.5999336
1.0137618
1
1.00
0.2700058
1
1.00
0.8000000

3
1.00
18.7311370
2.8253937
0.6401217
1
1.00
0.1612778

0.4701930
0.3585209-0.1107775-0.1480263
1.1307670

0.0708743
0.3397528
0.7271586

1.0000000

1.0000000

1.0000000

0.03349460
0.23472695
0.81375733
1.00000000

In general, the definition of the basis set follows the format:
basis sets
element symbol
shell symbol
exponent 1
exponent 2···
shell symbol
exponent 1
exponent 2······

contraction length
scaling factor
contraction coefficient 1.1[1.2 ···]
contraction coefficient 2.1[2.2 ···]
contraction length
scaling factor
contraction coefficient 1.1[1.2 ···]
contraction coefficient 2.1[2.2 ···]← one blank line
element symbol
shell symbol······

contraction length

scaling factor

Basis Sets 2
Apart from the atomic basis set specified in the Basis Sets section, a separate (usually smaller)
basis set for the initial guess method can be declared. In the case of a core Hamiltonian guess5

(GuessMethod = Hcore in job option $Guess), the Basis Set 2 directive is not used and thus notneed to be declared. The input format is equivalent to the atomic basis set input described in theprevious section.

Core Potential
In this section, the frozen core potential (FCP) is specified. Currently, the definition is restricted
to one element. In order to obtain the FCP, one has to perform a calculation with FCPmethod =potential specified by the job option $FCP and copy the section (core potential and below) fromthe punch file (.pun) to the corresponding input file. The number of frozen core orbitals andnon-frozen orbitals can be specified by the options coreRegion and valRegion in the $FCP
directive, respectively. The FCP has the following format:
core potential
DKH3Gen
COR
1S
78-2.98347169E+03-9.99727309E-01 -2.77962103E-03
···
COR
2S
78
-5.31922309E+02
4.04002299E-04 -1.00320737E+00
···
COR
2P
78
···
···
···
COR
4F
78
-3.78970260E+00
1.68980828E-12 -7.43624793E-11···

3.95750145E-03 -7.64787402E-04

4.73374430E-03 -1.09011031E-03

6.00973024E-10 -9.47083392E-10$MOA, $MOB, $MOG
This section describes the format for the input of molecular orbital coefficients used for the initial
guess in the case of GuessMethod = MOread. The directives $MOA, $MOB, and $MOG,
containing the converged MO coefficients of the α, β, or general orbitals for the respective SCF
method, are written to the punch file (.pun) at the end of a calculation. To be used for the initial
guess, the respective directive has to be copied to the input file. Furthermore, one has to ensurethat the employed Basis Set 2 is the same used for the representation of the MOs, i.e. theatomic orbital basis of the SCF calculation. Also, set GuessMethod = MOread.
6

The directive $MOA has the following format (equivalent for $MOB):$MOA
1 MO coeff. 1.1
1 MO coeff. 1.5···
2 MO coeff. 2.1
···
···
$end

MO coeff. 1.2
MO coeff. 1.6

MO coeff. 1.3
MO coeff. 1.7

MO coeff. 1.4
MO coeff. 1.8

MO coeff. 2.2

MO coeff. 2.3

MO coeff. 2.4

The first number in each line represents the number of the molecular orbital. The directive isclosed with $end in the same way as the job options. For general Hartree-Fock and DFT
calculations, i.e. WavefuncType = GHF, the coefficients are specified by the $MOG directive, inwhich real and imaginary parts of the MO coefficients are stored continuously as follows:$MOG
1 coeff. 1.1(real)
1 coeff. 1.5(real)···
2 coeff. 2.1(real)
2 coeff. 2.5(real)
···
$end

coeff. 1.1(imag.)coeff. 1.5(imag.)coeff. 1.2(real)coeff. 1.6(real)

···
···

coeff. 2.1(imag.)coeff. 2.5(imag.)coeff. 2.2(real)coeff. 2.6(real)

···
···

7

Job Options$Run
Basic settings of the calculation
JobTypetype of calculation to be executed
Energy [sp]single-point energy calculation (default)

Gradient [grad]energy gradient calculation

Optimization [opt]geometry optimization

Property [prop]

property calculationMemmaximum amount of memory used in calculation (default: 1024MB)
unit: KB, MB, GB, KW, MW, GW

wayDiag

type of Lapack diagonalization routine
1*syevd (divide-and-conquer algorithm)

2*syev (standard algorithm; default)$Wavefunction
WavefuncType

selection of wavefunction theory or treatment of spin in DFT

DFT

RHF

restricted Hartree-Fock and DFT (default)✓UHF

unrestricted open-shell Hartree-Fock and DFT

✓

ROHF

restricted open-shell Hartree-Fock and DFT✓

GHF

generalized Hartree-Fock and DFT

✓

RMP2

restricted second-order Møller-Plesset
perturbation theory

✕

GMP2

general second-order Møller-Plesset perturbation
theory✕8

$Hamiltonian
Hamiltonian settings
HamilType

Hamiltonian types
Infinite-order Douglas-Kroll-Hess (IODKH) is a synonym ofinfinite-order two-component (IOTC).

GradientNR

non-relativistic Hamiltonian (default)✓

FW[DKH1]

Foldy-Wouthuysen transformation for
one-electron Hamiltonian + non-relativistic
two-electron Hamiltonian✕

IOTC[IODKH]infinite-order two-component one-electron
Hamiltonian + non-relativistic two-electron
Hamiltonian✕

LUT-IOTC[LUT-IODKH]

infinite-order two-component one-electron
Hamiltonian with local unitary transformation +non-relativistic two-electron Hamiltonian✓

IOTC-IOTC[IODKH-IODKH]

infinite-order two-component Hamiltonian

✕

SD1e

calculation of one-electron spin-dependent terms to incorporate spin-orbit
coupling (default: false)
effective for WavefuncType=GHF
Analytic gradient is available for the Hartree-Fock calculation with the LUT-IOTC
Hamiltonian.

ConvY

convergence threshold for the iterative determination of the decoupling matrix in
IOTC calculations (default: 1.0d-09)

tolHess

threshold for linear dependency screening in calculation of Hess’ transformation
matrix (default: 1.0d-10)

tolLUTtau

cutoff radius in the local unitary transformation (default: 3.5 Å)

tolRelTEI

cutoff value for relativistic transformation of two-electron integrals(default: 1.0d-10)

Nucleusmodel of nuclei
point

point-charge model (default)

finitefinite-size nucleus based on the Gaussian model
parametrized by Visscher and Dyall
applied to the electron-nucleus attraction in energy
9calculations, meaning that the nuclear repulsion is calculated
based on the point-charge model$Mol
Additional molecular information
mchargemolecular charge (default: 0)

multiplicity

spin multiplicity (default: 1)$BasisAdditional basis set settings
BasType

BasTypeSmall

OrbitalShapeformat conversion of the atomic basis set
None

no conversion

GC

conversion to general contraction (default)SC

conversion to segmented contractionUC

conversion to uncontracted basis

format conversion of the basis set specified in the Basis Sets 2 section (ifnot specified, same as BasType)None

no conversion

GC

conversion to general contraction (default)SC

conversion to segmented contractionUC

conversion to uncontracted basis

shape of the orbitals
Cartesian[xyz]

Cartesian basis functions (default)

Spherical[SH]

spherical harmonic basis functions (only for energy
calculations of Hartree-Fock and MP2 methods)10$Integral
Molecular integral settings
Method_TEI

algorithm for two-electron integral calculation
Note that direct SCF is performed based on “Hybrid” algorithm.
Gauss-Rys

Gauss-Rys quadrature

PHMD

combination of the Pople-Hehre andMcMurchie-Davidson methods

ACE-TRR[SC-ACE-TRR]

accompanying coordinate expansion and recurrence
relation method

GC-ACE-TRR

general contraction accompanying coordinate expansion
and recurrence relation method

Hybridcombination of the above methods (default)

Cutoff_OEI

one-electron integral cutoff (default: 1.0d-20)

Cutoff_TEI

two-electron integral cutoff (default: 1.0d-20)

Cutoff_TEIout

cutoff for two-electron integrals to be saved on disk, not used in direct SCF(default: 1.0d-12)

Cutoff_preExp

integral cutoff based on exponents of basis functions(default: 20.0 * log(10.0))

isSchwarz

use Schwarz inequality to reduce computational cost of two-electron
integrals (default: true)

Method_DTEI

algorithm for two-electron integral gradients
Gauss-Rys

Gauss-Rys quadrature

ACE-TRR[SC-ACE-TRR]

accompanying coordinate expansion and recurrence
relation method

GC-ACE-TRR

general contraction accompanying coordinate expansion
and recurrence relation method

Hybridcombination of the above methods (default)

Cutoff_DOEI

cutoff for one-electron integral gradient (default: 1.0d-15)

Cutoff_DTEI

cutoff for two-electron integral gradient (default: 1.0d-10)

11$Guess
Settings for the initial guess method
GuessMethod

GuessWavefuncType

GuessMix

initial guess method
Hcore

core Hamiltonian guess

Huckelextended-Hückel guess with basis set 2 (definition isrequired; default)
available up to atom number 103
DKH3minimal is recommended as basis set 2.

Atomicatomic Hartree-Fock calculation with basis set 2(definition is required) and projection to basis set

Small

full Hartree-Fock calculation with basis set 2 (definition
required) and projection to basis set

MOreadread MO coefficients from directives $MOA, $MOB, or$MOG

wavefunction type for initial guess(default: WavefuncType)
RHF

restricted Hartree-Fock (default)UHF

unrestricted open-shell Hartree-Fock

ROHF

restricted open-shell Hartree-Fock

GHF

generalized Hartree-Fockfor open-shell singlet UHF and UDFT calculations: mix HOMO andLUMO of α- and β- spin (default: false)

12

$SCF
Settings for self-consistent-field (SCF) calculations
maxSCFcycle

maximum number of SCF iterations (default: 50)

convSCFSCF energy convergence threshold (default: 1.0d-09)

convDen

SCF density matrix convergence threshold (default: 1.0d-05)

convTech

SCF convergence acceleration technique (different methods can be
combined by using ‘+’ as separator)
C1-DIIS[DIIS, C-DIIS]

direct inversion in the iterative subspace (DIIS) method

C2-DIIS

C2-DIIS method, valid for large values of maxDIIS

EDIIS

energy-based DIIS method

EDIIS+DIIS

combination of DIIS and EDIIS (default)

SOSCF

approximate second-order SCF (SOSCF) methodsDampstatic damping

FON

non-integer occupation numbers during SCF based on
Fermi distribution function, integer occupation forconverged orbitals, known as Fermi smearing

QmtE_Cutoff

threshold for determination of linear dependencies in canonicalorthogonalization of atomic orbitals (default: 1.0d-06)

isDirectSCF

switch off storage of two-electron integrals on disc, i.e. recalculation of
integrals for each SCF step, known as direct SCF (default: false)

isFockDiff

use difference density matrix algorithm in direct-SCF calculations(default: true)

Couplecoupling coefficients used for linear combination of Fock matrix in ROHF
calculations, where FXX = A XX × Fα + BXX × Fβ (X = C, O, V)
Davidson

ACC=1/2, A OO=1, A VV=1, BCC=1/2, BOO=0, BVV=0(default)

C2006

Plakhutin et al (2006), which fulfills Koopmans’ theorem(ACC=0, A OO=1, A VV=1, BCC=1, BOO=0, BVV=0)

ManualAcc, Aoo, Avv, Bcc, Boo, Bvv are specified in $SCF
13

[Man, Input]
maxDIIS

number of previous iterations used in DIIS (default: 10)iDIISerrVec

method for calculation of DIIS error vector
1conventional (default)

2

Anderson type (default for complex MO coefficients)

maxEDIIS

number of previous iterations used in EDIIS (default: 10)

maxIterEDIIS

maximum number of iterations in EDIIS method (default: 200)

maxSOSCF

number of previous iterations used in SOSCF (default: 20)

tolSOSCFinithreshold for slope, below which SOSCF is started (default: 0.25)

tolSOSCFgradthreshold for convergence of SOSCF gradient (default: 1.0d-8)

SCFdampFac

static damping coefficient in sDamp, weight of previous density matrix
between 0.0 and 1.0 (default: 0.75)$MP2
Settings for second-order Møller-Plesset (MP2) calculations
nFrzA

number of frozen inner-shell α electrons in RMP2 calculations (default: 0)

nFrz

number of frozen inner-shell electrons in GMP2 calculations (default: 0)

SCSFacS

coefficient for antiparallel spin term used in SCS-MP2 calculations (default:
1.2d+00)

SCSFacT

coefficient for parallel spin term used in SCS-MP2 calculations (default:
0.3333333333d+00)

Cutoff_MP2

molecular integral threshold for MP2 calculations (default: 1.0d-09)

14

$DFT
Settings for density functional theory (DFT) calculations
DensfuncType

type of exchange-correlation functionalNone

wavefunction theory (default)

exchange only
SlaterSlater-Dirac (LDA) exchange

Becke88B88 exchange by Becke

PBEX

Perdew-Burke-Ernzerhof (PBE) exchange

Hartree-Fock + DFT correlation
VWN

Vosko-Wilk-Nusair (VWN) LDA correlation
VWN5 parameterization

VWN3

VWN3 parameterization

PW92

Perdew-Wang (PW92) LDA correlation

LYP

Lee-Yang-Parr (LYP) correlation

PBEC

Perdew-Burke-Ernzerhof (PBE) correlation

Pure (semi-)local density functionals
SVWN

Slater + VWN5SVWN3Slater + VWN3SPW92Slater + PW92

BLYP

Becke88 + LYP

PBE

PBEX + PBEC

revPBE

revised PBEX + PBEC

VS98

meta-GGA by van Voorhis and Scuseria

M06-L

meta-GGA by Zhao and Truhlar (2006)
15

Global hybrid functionals
B3LYP

three-parameter hybrid functional by Becke
20% exact exchange (EXX)B3LYP3B3LYP with VWN3 parameterization

BHHLYP

50% Becke88 + 50% EXX + LYP

PBE0

75% PBEX + 25% EXX ＋ PBEC

M05

hybrid meta-GGA by Zhao, Schultz and Truhlar(2005, 28% EXX)

M05-2Xhybrid meta-GGA by Zhao, Schultz and Truhlar(2005, 56% EXX)

M06

hybrid meta-GGA by Zhao and Truhlar (2006, 27% EXX)

M06-2Xhybrid meta-GGA by Zhao and Truhlar (2006, 54% EXX)

M06-HFhybrid meta-GGA by Zhao and Truhlar (2006, 100% EXX)

Double hybrid functionals
B2PLYP

47% Becke88 + 53% EXX + 73% LYP + 27% MP2

B2GPPLYP

35% Becke88 + 65% EXX ＋ 64% LYP + 36% MP2

PBE0-DH

50% PBEX + 50% EXX + 87.5% PBEC + 12.5% MP2

PBE0-220.6299% PBEX + 79.3701% EXX + 50% PBEC + 50%
MP2

nRad

number of radial grid points in molecular integration grid (default: 96)nLeb

number of spherical grid points in molecular integration grid
(Gauss-Lebedev quadrature)
allowed values: 6, 14, 26, 38, 50, 74, 86, 110, 146, 170, 194, 230, 266,
302, 350, 434, 590, 770, 974, 1202, 1454 (default: 302)

sdCol

axis of collinear spin density in spin-dependent calculationXx axisYy axis16

Zz axisNoneno specific axis, meaning DFT calculation with
non-collinear spin density (default)isRelPC

picture-change correction based on IOTC (IODKH) transformation for
exchange-correlation terms in relativistic DFT and TDDFT (default: false)available for WavefuncType=RHF, UHF, ROHF with
HamilType=IOTC-IOTC

isRelFun

replace Slater-Dirac and Becke 88 exchange functional with relativistic
counterparts (default: false)
effective for DensfuncType=SVWN, BLYP, B3LYP, B2PLYP, etc.
HamilType=IOTC-IOTC and isRelPC=.true. is recommended.
valid for ground-state calculations, meaning that coupling matrix of
TDDFT is calculated using a non-relativistic functional

17

$TDDFT
Settings for excited-state calculation based on linear-response time-dependent DFT
isExcitedperform an excited-state calculation based on linear-response TDDFT
using the exchange-correlation functional specified by DensfuncType in$DFT (default: false)available for WavefuncType=RHF and GHF

isTDA

Tamm-Dancoff approximation (default: false)
For WavefuncType=GHF, this keyword is forced to be true.

wayDiagdiagonalization method (eigenvalue solver)DavidsonDavidson method (for few eigenvalues; default)

QR

all eigenvalues by QR method

nEigennumber of eigenvalues (excitation energies) with the Davidson method(default: 10)

maxVeckeyword regarding the maximum value of the subspace extension with
the Davidson method (default: 100)
maximum size of subspace = nEigen × maxVec

TDmultispin multiplicity of excited states for WavefuncType=RHF
1singlet excited states (default)

3

triplet excited states

TDnRadnumber of radial grid points in molecular integration grid (default: 48)

TDnLebnumber of spherical grid points in molecular integration grid
(Gauss-Lebedev quadrature)
allowed values: 6, 14, 26, 38, 50, 74, 86, 110, 146, 170, 194, 230, 266,
302, 350, 434, 590, 770, 974, 1202, 1454 (default: 110)

18

$DFT (new routine)
Settings for density functional theory (DFT) calculations using newly implemented routine
isExCorDM

switch on newly implemented density-matrix-based routine forexchange-correlation energy and potential (default: false)

isRelPC

picture-change transformation based on the IOTC (IODKH) method for
Coulomb repulsion and exchange-correlation terms in relativistic DFT(default: false)available for WavefuncType=RHF, UHF, ROHF with
HamilType=IOTC-IOTC

isRelFun

replace Slater-Dirac and Becke 88 exchange functional with relativistic
counterparts (default: false)
effective for DensfuncType=SVWN, BLYP, B3LYP, B2PLYP, etc and local
hybrid functionals listed below
HamilType=IOTC-IOTC and isRelPC=.true. is recommended.

DensfuncType

type of exchange-correlation functional
In addition to the same functionals implemented in the old routine except
meta-GGA, local hybrid functionals are available.
local hybrid functional
Lh07t-SVWN

local mixing of exact exchange and Slater exchangewith mixing function of kinetic energy density and
VWN correlation

Lh07s-SVWN

local mixing of exact exchange and Slater exchangewith mixing function of dimensionless density
gradient and VWN correlation

Lh12ct-SVWN

local mixing of exact exchange and Slater exchangewith mixing function of kinetic energy density and
VWN correlation

Lh12ct-SsirPW92

local hybrid functional with self-interaction-reduced
PW92 correlation

Lh12ct-SsifPW92

local hybrid functional with self-interaction-free PW92
correlation19

Lh14t-calPBE

GridType

local mixing of exact exchange and PBE exchangewith mixing function of kinetic energy density,
calibration function, and PBE correlation

type of grid used in computation of exchange-correlation terms
SMASH

conventional Lebedev grid implemented in the
SMASH program (default)

Ahlrichs

standard grid for efficient calculation proposed by
AhlrichsnRad

number of radial grid points in molecular integration grid for
GridType=SMASH (default: 96)nLeb

number of spherical grid points in molecular integration grid
(Gauss-Lebedev quadrature) for GridType=SMASH
allowed values: 6, 14, 26, 38, 50, 74, 86, 110, 146, 170, 194, 230, 266,
302, 350, 434, 590, 770, 974, 1202, 1454 (default: 302)

GridSizepredefined grid sizes for Ahlrichs grids
1very small test grid2

small standard grid for fast calculation

3

medium standard grid for standard calculation(default)

4large standard grid5large standard grid with higher accuracy

6

small reference grid7

accurate reference grid8highly accurate reference grid9‘cheap’ reference grid for accurate atomic
calculations

42

meaninglessly large grid for almost exact results,
reference only

20

Junc

thresholds for screening in seminumerical integration of exact exchange
energy density (default: 12,12,12)“Junc=s,d,f” means thresholds of 10^-s, 10^-p, and 10^-f for S-junction(overlap screening), P-junction (density matrix screening), andF-junctions (screening before Fock matrix build), respectively.

21

$Opt
Settings for molecular structure optimization
Coord

coordinates used for optimization
Redundant[RD, Redun]

redundant internal coordinates (default)

Cartesian[Cart]

Cartesian coordinates

maxOptCycle

maximum number of optimization steps (default: 50)

convOpt

convergence threshold wrt the gradient in hartree/bohr (default: 1.0d-04)

wayDTEI

method for calculating two-electron integral gradients
Gauss-Rys

Gauss-Rys quadrature

ACE-TRR

accompanying coordinate expansion and recurrence
relation method

GC-ACE-TRR

general contraction accompanying coordinate expansion
and recurrence relation method

Hybridcombination of ACE-TRR, PHMD, and Gauss-Rys (default)

Numerical

numerical differentiation of total energy to calculate gradient (default: false)

StepSizedisplacement for numerical gradient in angstrom (default: 1.0d-04)

numPoint

number of points for numerical differentiation
3

three-point formula (default)

5five-point formula7

seven-point formula9

nine-point formula

22

$FCP
Settings for frozen core potential (FCP)
FCPmethod

FCP creation/calculation settings
None

no FCP (default)

Potential

creating an FCP

FCP

execution of calculation using FCP

nCoreOut(n)number of core shells of FCP (n = 1, 2, 3, 4 corresponds to s, p, d and forbitals)

CoreRegion(1)number of shells treated as core shells

ValRegion(1)number of shells treated as valence shells

isUcorecore potential obtained with UHF (default: false)

isCorePotEx

presence of exchange integration in core potential generation(default: true)

isValPotEx

presence of exchange integration in valence potential generation(default: true)

doCVint

core-valence electron integration to create potential (default: true)
requires false for OrbitalShape = Spherical

23

$TCE
Settings for post-HF calculations implemented using tensor contraction engine (TCE)
TCEmethodelectron correlation methodNone

do not utilize the TCE routine (default)

MP2second-order Møller-Plesset perturbation theory

MP2.5

average of MP2 & MP3

MP3

third-order Møller-Plesset perturbation theory

LCCD

linearized coupled cluster doubles

CCD

coupled cluster doubles

LCCSD

linearized coupled cluster singles and doubles

CCSD

coupled cluster singles and doubles

CCSD[T]

coupled cluster singles and doubles with non-iterative
connected triples

CCSD(T)

coupled cluster singles and doubles with non-iterative
connected triples

CCSDT

coupled cluster singles, doubles, and triples

CCSDTQ

coupled cluster singles, doubles, triples, and quadruples

nFrzA

number of frozen inner-shell α electrons (default: 0)

nFrzVirA

number of frozen virtual α orbitals (default: 0)

CutoffTransInt

molecular integral threshold for correlation calculation (default: 1.0d-09)

maxTCEcycle

maximum number of iterations for iterative methods (default: 100)

TCEtolconvergence threshold wrt. the amplitudes (default: 1.0d-08)

24

$PropSetting for property evaluations
In addition to Mulliken atomic charge, Mulliken atomic spin density (WavefuncType=UHF,ROHF) and Mulliken atomic spin vector (WavefuncType=GHF) are obtained by a single-point
calculation. For WavefuncType=RHF, UHF, and ROHF, other properties are calculated by
RunType=prop and the following options:
isContactcalculate contact density, which is electron density and spin density at theposition of nuclear coordinate (default: false)isGridProperty

calculate atomic charge, dipole moment, and electric field gradient tensor
using grid routine (default: false)
Atomic charges are calculated using Becke's partition function and the valuesof covalent radii, which are also used in DFT and TDDFT routines.

isPCC

perform picture-change transformation of the density operator (default: true)
valid for HamilType=IOTC, IOTC-IOTC, LUT-IOTC

25

Basis Set Library
RAQET provides the user with a comprehensive basis set library containing a large number ofpredefined common Gaussian basis sets. Each basis set is stored in a separate subdirectory of
the library. Addition of new basis sets can be done by the following procedure:
1. Create a new directory for the basis set, e.g. basis/MyDZP.
2. Create basis set files for the desired elements. The format can be adapted from theexisting basis set files and is similar to the format described in the section Basis Sets.
3. Different basis set names can be used by creating symbolic links.
The initially provided basis set library contains the following basis sets:

STO-nG Basis Sets
Elements
STO-2G

H-Ca, Sr

STO-3G

H-Cd

STO-6G

H-Zn

Remarks

Pople Basis Sets
Alias

Elements

3-21G
3-21G(d)H-Cs
3-21G*

Na-Ar

3-21++G
3-21++G(d)H-Ca
3-21++G*

Na-Ar

4-31G

H-Ne, P-Cl

6-31G

H-Zn

6-31G(d)6-31G*

H-Zn

6-31G(d,p)

6-31G**

H-Zn

6-31+G
6-31+G(d)H-Ar
6-31+G*

H-Ca

6-31++G

H-Ca
26

Remarks

6-31++G(d)6-31++G*

H-Ca

6-31++G(d,p)

6-31++G**

H-Ar

6-311G

H-Ca, Ga-Kr, I

6-311G(d)6-311G*

H-Ca, Ga-Kr, I

6-311G(d,p)

6-311G**

H-Ca, Ga-Kr, I

6-311G(2df,2pd)

H-Ne, K-Ca

6-311+G(d)6-311+G*

H-Ca

6-311++G(d,p)

6-311++G**

H-Ca

6-311++G(2d,2p)

H-Ca

6-311++G(3df,3pd)

H-Ar

Sapporo Basis Sets
Elements

Remarks

Sapporo-DZP

H-Xe

Sapporo-DZP+d

H-Xe

Sapporo-DZP-2012

H-Xe

Sapporo-DZP-2012+d

H-Xe

Sapporo-TZP

H-Xe

Sapporo-TZP+d

H-Xe

Sapporo-TZP-2012

H-Xe

Sapporo-TZP-2012+d

H-Xe

Sapporo-QZP

H-Xe

Sapporo-QZP+d

H-Xe

Sapporo-QZP-2012

H-Xe

Sapporo-QZP-2012+d

H-Xe

Sapporo-DKH3-DZP

K-Xe

for relativistic calculations

Sapporo-DKH3-DZP+d

K-Xe

for relativistic calculations

27

Sapporo-DKH3-DZP-2012

K-Rn

for relativistic calculations

Sapporo-DKH3-DZP-2012+d

K-Rn

for relativistic calculations

Sapporo-DKH3-TZP

K-Xefor relativistic calculations

Sapporo-DKH3-TZP+d

K-Xe

for relativistic calculations

Sapporo-DKH3-TZP-2012

K-Rn

for relativistic calculations

Sapporo-DKH3-TZP-2012+d

K-Rn

for relativistic calculations

Sapporo-DKH3-QZP

K-Xe

for relativistic calculations

Sapporo-DKH3-QZP+d

K-Xe

for relativistic calculations

Sapporo-DKH3-QZP-2012

K-Rn

for relativistic calculations

Sapporo-DKH3-QZP-2012+d

K-Rn

for relativistic calculations

Correlation-Consistent Basis Sets
Elements
cc-pVDZ

H-Ar, Ca-Kr

cc-pVTZ

H-Ar, Ca-Kr

cc-pVQZ

H-Ar, Ca-Kr

cc-pV5Z

H-Ar, Ca-Kr

cc-pV6Z

H-He, B-Ne, Al-Ar

Remarks

cc-pVDZ-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

cc-pVTZ-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

cc-pVQZ-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

cc-pV5Z-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

cc-pCVDZ

H-He, B-Ar, Ca

cc-pCVTZ

H-He, B-Ar, Ca

28

cc-pCVQZ

H-He, B-Ar, Ca

cc-pCV5Z

H-He, B-Ne

cc-pwCVDZ

H-He, B-Ne, Al-Ar

cc-pwCVTZ

H-He, B-Ne, Al-Ar, Sc-Zn

cc-pwCVQZ

H-He, B-Ne, Al-Ar, Sc-Zn

cc-pwCV5Z

H-He, B-Ne, Al-Ar, Sc-Zn

cc-pwCVTZ-DK

B-Ne, Al-Ar, Sc-Zn

contractions optimized for
relativistic calculations

cc-pwCVQZ-DK

B-Ne, Al-Ar, Sc-Zn

contractions optimized for
relativistic calculations

cc-pwCV5Z-DK

B-Ne, Al-Ar, Sc-Zn

contractions optimized for
relativistic calculations

cc-pV(D+d)Z

Al-Ar

cc-pV(T+d)Z

Al-Ar

cc-pV(Q+d)Z

Al-Ar

cc-pV(5+d)Z

Al-Ar

cc-pV(6+d)ZAl-Ar

aug-cc-pVDZ

H-Ar, Sc-Kr

aug-cc-pVTZ

H-Ar, Sc-Kr

aug-cc-pVQZ

H-Ar, Sc-Kr

aug-cc-pV5Z

H-He, B-Be, Al-Ar, Sc-Kr

aug-cc-pV6Z

H-He, B-Ne, Al-Ar

aug-cc-pVDZ-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

aug-cc-pVTZ-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

aug-cc-pVQZ-DK

H-He, B-Ne, Al-Ar, Sc-Kr

contractions optimized for
relativistic calculations

29

aug-cc-pV5Z-DK

H-He, B-Ne, Al-Ar, Sc-Kr

aug-cc-pCVDZ

H-Ar

aug-cc-pCVTZ

H-Ar

aug-cc-pCVQZ

H-Ar

aug-cc-pCV5Z

H-He, B-Ne, Al-Ar

aug-cc-pV(D+d)Z

Al-Ar

aug-cc-pV(T+d)Z

Al-Ar

aug-cc-pV(Q+d)Z

Al-Ar

aug-cc-pV(5+d)ZAl-Ar

aug-cc-pV(6+d)Z

Al-Ar

cc-pVQZdenfit

H, B-F, Al-Cl

aug-pV7Z

H, C-F, S

aug-cc-pCVTZ-CTOCDuc

H, C-F

aug-cc-pVTZ-J

H, C-F, S

contractions optimized for
relativistic calculations

Polarization-Consistent Basis Sets
Elements

Remarks

pc-0

H-Ca, Ga-Kr

general contractions

pc-1

H-Kr

general contractions

pc-2

H-Kr

general contractions

pc-3

H-Kr

general contractions

pc-4

H-Kr

general contractions

pcseg-0H-Kr

pcseg-1

H-Kr

pcseg-2H-Kr

30

pcseg-3

H-Kr

pcseg-4

H-Kr

OthersElements

Remarks

ANO-RCC

H-Cm

general contractions for
relativistic calculations

DKH3minimal

H-Lr

general contractions for
relativistic calculations

SARC-DKH

La-Rn, Ac-Lr

contractions for relativistic
calculations

Sadlej-pol

H-Ca, Cu-Sr, Ag-Ba, Au-Fr

for polarizability calculations

Sadlej-pol-DK

H-Ca, Cu-Sr, Ag-Ba, Pt-Fr

for relativistic polarizability
calculations

UGBS

H-Th, Pu-Am, Cf-Lr

General purpose minimalbasis set

WTBS

He-Rn

Nuclear Basis Set

N1G-VD97

Elements

Remarks

H-Rn

Gaussian nucleus model
parameterized by Visscher
and Dyall, used with
Nucleus=finite31