This document provides an introduction to the Vienna Ab Initio Simulation Package (VASP) software for performing density functional theory (DFT) calculations. It describes key aspects of DFT and the plane wave basis used in VASP, including exchange-correlation functionals, pseudopotentials, and common input/output files like INCAR, POSCAR, POTCAR and KPOINTS. Online resources for learning more about VASP and DFT are also listed.

1. INL/CON-20-59245
Introduction to the
Vienna Ab Initio Simulation Package
(VASP)
Idaho National Laboratory

2. INL/CON-20-59245
Online Resources for VASP
• John Kitchin’s book: “Modeling materials using density functional
theory” (2012)
– http://kitchingroup.cheme.cmu.edu/dft-book/dft.html
• VASP Workshop Lectures:
– https://www.vasp.at/documentation/
• VASP Wiki:
– https://www.vasp.at/wiki/index.php/The_VASP_Manual
• NERSC VASP Tutorial
– https://www.nersc.gov/assets/Uploads/VASP-lecture-Basics.pdf
• NERSC Examples for VASP:
– https://www.nersc.gov/assets/Uploads/VASP-tutorial-
AtomsMoleculesBulk.pdf
• Atomic Simulation Environment
– https://wiki.fysik.dtu.dk/ase/tutorials/tutorials.html

3. INL/CON-20-59245
Density Functional Theory -- Resources
DFT from a chemistry perspective: A chemical and theoretical way to look at
bonding on surfaces
By Ronald Hoffmann
https://journals.aps.org/rmp/pdf/10.1103/RevModPhys.60.601
DFT Review Article: Density Functional Theory as a Major Tool in
Computational Materials Science
By Arthur Freeman
https://www.annualreviews.org/doi/10.1146/annurev.ms.25.080195.000255
DFT Implementation details for VASP: Efficiency of ab-initio total energy
calculations for metals and semiconductors using a plane-wave basis set
By Kresse and Furthmüller
https://doi.org/10.1016/0927-0256(96)00008-0

4. INL/CON-20-59245
Density Functional Theory -- Background
1926:
For a time-independent n-body system:
where
is the wave function for an n-body system
For systems with small number of electrons ( ~O(10) ), solving this is doable.
But for larger systems, this becomes too complicated to solve.

5. INL/CON-20-59245
Density Functional Theory -- Background
Solution: The Hohenberg-Kohn-Sham theory: a systematic way to map
the many-body problem onto a single-body problem
(Courtesy NERSC)
Why is solving the Schrödinger equation for the many-body problem too
difficult for anything but a relatively small number of electrons?
Storage for example…

6. INL/CON-20-59245
Density Functional Theory -- Background
What is a functional?
Suppose f(x) = x2 ; we call f(x) a function since when we give it a
number, it returns a number.
A functional returns a number when we give it a function: e.g.
g(f(x) is a functional; if I give it f(x) = sin(x), g(f(x)) returns 2.

7. INL/CON-20-59245
Density Functional Theory -- Background
Walter Kohn (Nobel Prize in Chemistry 1998)
The key idea:
Don’t rely on the wave function; express material properties
(ground state) as a functional of the charge density
Why is this important? The charge density is only 3 dimension
regardless of the number of electrons!
The Hohenberg – Kohn theorems (1964) ensure that the functional exists but
doesn’t say how to find it!
So the ground state energy of system can be written as:
where is some functional of
Nobel Lecture: Electronic structure of matter—wave functions and
density functionals by W. Kohn
https://journals.aps.org/rmp/abstract/10.1103/RevModPhys.71.1253

8. INL/CON-20-59245
Density Functional Theory -- Background
What is an exchange correlation functional?
Generally written in this form:
where is the exchange correlation
energy density (it represents the energy per
electron )
and is the charge density (or number of
electrons per unit volume)

9. INL/CON-20-59245
Density Functional Theory -- Background
There are several types of exchange-correlation
functionals:
Local Density Approximation (LDA)
-- Assumes that the exchange-correlation
energy density at every position in space is the
same as a uniform electron gas

10. INL/CON-20-59245
Density Functional Theory -- Background
There are several types of exchange-correlation functionals:
Generalized Gradient Approximation (GGA)
-- Incorporates the gradients of the charge density at a point as well
as the value, i.e.
GGA functionals are generally constructed as a correction term, e.g.

11. INL/CON-20-59245
Density Functional Theory -- Background
There are several types of exchange-correlation functionals:
Meta-Generalized Gradient Approximation (GGA)
-- Incorporates the Laplacian of the density
Hybrid functionals (or Adiabatic Connection Method functionals)
-- Include fractions of exact Hartree-Fock exchange energy

12. INL/CON-20-59245
Density Functional Theory -- Background
Specific exchange-correlation functionals can be selected by setting the
GGA flag in the INCAR file of VASP:
GGA default is the type of exchange-correlation specified in the POTCAR file
Many functionals contains empirical parameters with values fitted to
reproduce experiments. Others have no empirically determined
parameters (e.g. PW91).

13. INL/CON-20-59245
Density Functional Theory -- Background
Example: Geometry optimization of water using different exchange
correlation functionals
From C.K. Skylaris

14. INL/CON-20-59245
Density Functional Theory -- Background
In VASP the time independent Schrödinger equation becomes
where is the eigenvector dependent exchange correlation functional
replacing the Hamiltonian operator
are the eigenvalues as a function of the eigenvectors or energy
bands
and the wavefunction is replaced by a radial density expansion that is a
superposition of plane waves:
where are constants.

15. INL/CON-20-59245
Density Functional Theory -- Background
Why plane waves?
1. Good choice for systems with repeating
structure because it enables a periodic density
expansion
2. We can use FFT’s to evaluate the action of the
Hamiltonian on the orbitals. FFT’s are O(N log N)
and so this approach is computationally
compelling.
Is VASP the only DFT software that uses plane waves?
No. CASTEP also does, among others.

16. INL/CON-20-59245
The VASP ENCUT parameter can be used to control this
Density Functional Theory -- Background
Do we need an infinite number of plane waves?
The coefficients of the planewaves ( ) go to zero for high energy planewaves.
So we can truncate above a cutoff energy. But the cutoff energy is element
dependent!
Cutoff energies (eV) for two different elements
and two different precision levels. (from John
Kitchin)

17. INL/CON-20-59245
History of VASP
• Based on code written by Mike Payne (then @ MIT)
– VASP is similar to CASTEP code because of this
(CASTEP = Cambridge Serial Total Energy Package)
• 1989 Jürgen Hafner brought the code to U. Vienna
• 1993 VASP written by J. Furthmüller and G. Kresse
• Development continues under G. Kresse
• Stable Releases over the past 10 years:
– V6.1.0 28 Jan 2020
– V5.4.4 18 April 2017
– V5.3.3 18 Dec 2012
– V5.2.11 Dec 2010

18. INL/CON-20-59245
Pseudopotentials
• The core electrons of an atom are computationally expensive with
planewave basis sets
– Large number of planewaves are required to expand their
wavefunctions
– Contributions of core electrons versus valence electrons to
bonding is usually negligible
• To address this, we replace the atomic potential due the to core
electrons with a pseudopotential which has the same effect on valence
electrons: (see also “Efficient pseudopotentials for plane-wave
calculations by Troullier and Martins:
– https://journals.aps.org/prb/abstract/10.1103/PhysRevB.43.1993)
• VASP provides a database of pseudopotentials based on the Project
Augmented-Wave (PAW) method. These are called PAW potentials.
– https://journals.aps.org/prb/abstract/10.1103/PhysRevB.50.17953
– https://journals.aps.org/prb/abstract/10.1103/PhysRevB.59.1758

19. INL/CON-20-59245
Pseudopotentials
• PAW potentials come in two varieties:
– Norm-conserving soft pseudopotentials
– Vanderbilt ultrasoft potentials (requires fewer plane waves to
expand by a factor of 2-3 times):
https://journals.aps.org/prb/abstract/10.1103/PhysRevB.41.7892
• Pseudopoentials are not unique!
• Predicted properties do depend on them!
(From G. Kresse)
Wavefunction for different angular
momentum quantum numbers

20. INL/CON-20-59245
CAR Files
• Input and output data in VASP are read from or written to “CAR” files ( a
reference to “CARDS” when I/O on computers was done by punchcards
• VASP requires at least four CAR files to run: INCAR, POSCAR,
POTCAR, and KPOINTS
• VASP may also read in: CHGCAR, WAVECAR
• VASP will detect the presence of a STOPCAR file
• Some VASP output files include: CHG, CHGCAR, CONTCAR,
DOSCAR, EIGENVAL, ELFCAR, IBZKPT, LOCPOT, OSZICAR,
OUTCAR, PARCHG, PCDAT, PROCAR, WAVECAR,XDATCAR
INPUT
OUTPUT

21. INL/CON-20-59245
INCAR
• This is the central input file of VASP. Tip: tabs in this file cause
problems with VASP – avoid tabs!
Simple Example:
IBRION = 2
ISIF = 3
NSW = 100
POTIM = 0.5
ENCUT = 400
PREC = Accurate
NBANDS = 20

22. INL/CON-20-59245
POSCAR
• The “position” card. Contains the lattice geometry and the ion positions.
• The first line is a comment line (put your system name here!)
• The second line is a scaling factor.
• The next three lines are vectors describing the unit cell of the system
• Line 6 tells the elements in the system (in order of appearance in the POTCAR file)
• Line 7 tells the number of atoms for each atom type
• Line 8: May either say “Selective Dynamics” or “Cartesian” or “Direct” coordinates
• Next line: positions of the atoms
Simple Example:

23. INL/CON-20-59245
KPOINTS
• The “K” comes from reciprocal space (or k-space). This file specifies
the reciprocal lattice for integration in k-space over the first Brillouin
zone.
Example: the first Brillouin
zone of a square lattice

24. INL/CON-20-59245
POTCAR
• The “Potential” CAR holding the pseudopotentials. Each element has
one or more PAW dataset; they can be concatenated together.
• VASP comes with a library of PAW datasets.
• When you have more than one type of atom, you have to concatenate
the PAW datasets IN THE SAME ORDER as atomic species is
specified in the POSCAR file.
• Each individual PAW data set starts with a descriptive section,
specifying amongst other things:
– Parameters that were required to generate the dataset:
– Number of valence electrons
– Atomic mass
– Default energy cutoffs

25. INL/CON-20-59245
OUTPUT Files
Coutesy NERSC

26. INL/CON-20-59245
Compiling VASP
• Most of the time VASP will already be compiled for you, but it is
distributed in source code form so it is likely at some point you will
need to compile it.
• Compiling VASP requires manual modification of the makefile.include
file.
• The core computations of VASP are FFT’s and dense linear algebra
including eigenvector and eigenvalue computations; hence, the better
the BLAS and FFT support you have, the better the performance.
• Compiling VASP against OpenBLAS, LAPACK, ScaLAPACK, and
FFTW (all open source libraries) is possible and easily done; however,
performance is about 3X worse compared with linking against Intel’s
MKL libraries (closed, proprietary).
• VASP will also compile on ARM architectures; benchmarks show it
about 20% slower than Broadwell 22c

27. INL/CON-20-59245
VASP on ARM
• Cray User 2018 Study on VASP on ARM by Simon McIntosh-Smith:
https://uob-hpc.github.io/assets/cug-2018.pdf
Calculations by VASP are dominated by floating-point intensive routines which favors x86
processors. ARM gives higher core counts to compensate but benchmarks show VASP about
20% slower than Broadwell and half the speed of Skylake

28. INL/CON-20-59245
Profiling VASP
• VASP is already fully instrumented for profiling
• Add the –DPROFILING flag to the CPP_OPTIONS in makefile.include
• Profiling output will be written to the OUTCAR
• Profile includes both a flat profile and Cumulative profile

29. INL/CON-20-59245
Profiling VASP
• You can add custom profiling by encapsulating routines of interest with
the API call: PROFILING_START and PROFILING_STOP, e.g.
PROFILING_START(‘my_profile_check’)
…
PROFILING_STOP(‘my_profile_check’)

30. INL/CON-20-59245
VASP Executables
• There are three executables associated with VASP:
– VASP_STD
• This is the standard version – for general k-point meshes with
collinear spins
– VASP_GAM
• The “Gamma Point only” version – typical for large unit cells
– VASP_NCL
• The “non-collinear” version
• For general k-point meshes
• Used for magnetic structure calculations OR to include spin-
orbit interactions in a calculation
• Runs 3-D FFT’s on mesh twice the size of VASP_STD

31. INL/CON-20-59245
VASP GPU
Not all INCAR options are supported in the GPU version
(e.g. LREAL = .FALSE. is not supported)
• Benchmark comparison (siHugeShort) on Sawtooth:
– vasp_gpu on 4 GPUs (one node): 3 min 0 secs
– vasp_std on 48 cores (one node): 4 min 32 secs

32. INL/CON-20-59245
VASP on Sawtooth @ INL
• Sawtooth has a CPU version and a GPU version of VASP
• CPU Executable names are: vasp_std, vasp_gam, and vasp_ncl
• GPU Executable names: vasp_gpu
Note: Not all INCAR options are supported in the GPU version
(e.g. LREAL = .FALSE. is not supported)
• Benchmark comparison (siHugeShort):
– vasp_gpu on 4 GPUs (one node): 3 min 0 secs
– vasp_std on 48 cores (one node): 4 min 32 secs

33. INL/CON-20-59245
Running VASP in parallel:
ways to extract concurrency
• VASP has 3 levels of parallelism
– Over k-points
– Over bands
– Over plane-wave coefficients
• Related fundamentals:
– The number of k-points
– The number of bands (determined indirectly by the number of
atoms and electrons)
– The number of plane waves (which gives the number of grid points
in the FFTs)

34. INL/CON-20-59245
The Number of Bands
• Parallelization over bands is controlled by the NPAR parameter
• NPAR determines the number of bands that are treated in parallel
• Extreme limit is 1 band per core; this is usually too little work to get
good efficiency.
• Good rule of thumb: number of bands per core equal to the average
number of valence electrons (4-8).
• Make sure NPAR evenly divides the number of cores available on a
node, e.g.:
– On Sawtooth (48 cores/node), best efficiency for NPAR is 6
– On Lemhi (40 cores/node), best efficiency for NPAR is 8
– On Falcon (36 cores/node), best efficiency for NPAR is 6

35. INL/CON-20-59245
The Number of K-points
• VASP can treat each k-point independently
• The number of k-point groups that run concurrently is set by the KPAR
parameter
• The upper limit for KPAR is the total number of k-points
• Larger KPAR values increase the memory overhead
• It rarely makes sense to have KPAR larger than the number of
compute nodes requested

36. INL/CON-20-59245
Basis Set Size
• This determines the grid size of the FFTs
• 3-D FFT’s in VASP are computed in a plane-wise manner by default
(to reduce communication between ranks)
• Each of the NPAR groups works on a 2D plane
• NGZ is the number of grid points in the Z direction for the FFT
• Generally you want NGZ to be evenly divisible by NPAR for best load
balancing
• You can tune NGZ by adjusting ENCUT or explicitly setting NGZ

37. INL/CON-20-59245
Simple Example: Molecular Dynamics run on
32-atom cell
• INCAR:
# electronic degrees
ENCUT = 300
LREAL = A # real space projection
PREC = Normal # chose Low only after tests
EDIFF = 1E-5 # do not use default (too large drift)
ISMEAR = 1 ; SIGMA = 0.1 # Fermi smearing: 2000 K 0.086 10-3
ALGO = Very Fast # recommended for MD (fall back ALGO = Fast)
MAXMIX = 40 # reuse mixer from one MD step to next
NCORE= 4 # one orbital on 4 cores
ISYM = 0 # no symmetry
NELMIN = 4 # minimum 4 steps per time step, avoid breaking after 2 steps
# MD (do little writing to save disc space)
IBRION = 0 ; NSW = 100000 ; NWRITE = 0 ; LCHARG = .FALSE. ; LWAVE = .FALSE.
TEBEG = 3063 ; TEEND = 3063
# canonic (Nose) MD with XDATCAR updated every 50 steps

38. INL/CON-20-59245
Simple Example: Molecular Dynamics run on
32-atom cell
• POSCAR:
AgPd (50% Pd) -3% Volume
4.11171
0.00000000 2.00000000 0.00000000
0.00000000 0.00000000 2.00000000
2.00000000 0.00000000 0.00000000
16 16
D
0.00000000 0.00000000 0.00000000
0.25000000 0.00000000 0.25000000
0.25000000 0.25000000 0.00000000
0.00000000 0.50000000 0.00000000
0.25000000 0.50000000 0.25000000
0.75000000 0.25000000 0.00000000
0.00000000 0.00000000 0.50000000
0.25000000 0.25000000 0.50000000
0.00000000 0.75000000 0.75000000
0.25000000 0.75000000 0.50000000

39. INL/CON-20-59245
Simple Example: Molecular Dynamics run on
32-atom cell
• KPOINTS:
Gamma-point only
1 ! one k-point
rec ! in units of the reciprocal lattice vector
0 0 0 1 ! 3 coordinates and weight

40. INL/CON-20-59245
Some Use Cases for VASP
• Calculating surface energies
• Calculating formation energies
• Calculating reaction energies
• Calculating energy barriers
– Generally done using the Nudged Elastic Band (NEB) method
– VASP Transition State Tools (VTST) assists this
• Vibrational Frequency Calculations
• Calculating Density of States (DOS)
• Calculating band structures
-5 -4 -3 -2 -1 0
total
s
p
t2g
eg
DOS (Courtesy Zongtang Fang)

41. INL/CON-20-59245
Tools for VASP
VASP Transition State Tools (VTST): http://theory.cm.utexas.edu/vtsttools/
• Provides nudged elastic band (NEB) method implementation for finding
saddle points and minimum energy paths
• Comes as source code that is added to VASP and then VASP is
recompiled

42. INL/CON-20-59245
Tools for VASP
• Pymatgen (Python Materials Genomics)
• I/O support for VASP, Gaussian, ABINT
• Python based
• Is the analysis engine for https://www.materialsproject.org/
• Works in Jupyter notebook (already available on INL HPC systems)
(From Germain Vallverdu)

43. INL/CON-20-59245
Tools for VASP
• Atomic Simulation Environment (https://wiki.fysik.dtu.dk/ase/index.html)
• Python Based
• Used VASP as a calculator
• NEB calculations

44. INL/CON-20-59245
Tools for VASP
• Enumlib (optionally included in pymatgen): https://github.com/msg-
byu/enumlib
• Generates derivative superstructures – deals with combinatorial explosion
when supercells are large

45. INL/CON-20-59245
VASP6: What’s new?
• On-the-fly machine learning for force fields via Bayesian inference
• Demonstrated for predicting melting points:
– https://journals.aps.org/prb/abstract/10.1103/PhysRevB.100.014105
Large number of machine learning force field (ML
FF) parameters added for INCAR, i.e.

46. INL/CON-20-59245
VASP6: What’s New?
• Faster performance for hybrid DFT calculation
• Hybrid OpenMP and MPI parallelization
• OpenACC support for GPUs
• HDF5 support
• Libxc support for gradient correct functionals
• Time evolution support for frequency dependent response
functions

47. INL/CON-20-59245
Machine Learning Opportunities for VASP
• Neural network architectures for modeling atomic systems
– Quantum-chemical insights from deep tensor neural networks
https://www.nature.com/articles/ncomms13890
– A deep learning Toolbox for atomistic systems
https://pubs.acs.org/doi/10.1021/acs.jctc.8b00908
– Transfer Learning for material properties
https://arxiv.org/pdf/2006.16420.pdf
• Databases from high-throughput ab initio calculations for training like
AFLOWLIB: https://doi.org/10.1016/j.commatsci.2012.02.002
• On-the-fly Learning: On-the-fly machine learning force field generation:
Application to melting points
– https://journals.aps.org/prb/abstract/10.1103/PhysRevB.100.014105

48. INL/CON-20-59245
Some Resources for VASP
• VEST: http://jp-minerals.org/vesta/en/
– Free crystal structure viewer and building. Can read and write
POSCAR and CONTCAR files; can read CHGCAR, PARCHG,
LOCPOT, and ELFCAR.
• RINGS: http://rings-code.sourceforge.net/
– Extracts pair distribution functions
• VTST Tools: http://theory.cm.utexas.edu/vtsttools/
– Transition state tools for finding saddle points.
• VMD: http://www.uni-due.de/~hp0058/?file=vmdplugins.html&lang=en.
– Used to visualize structures and trajectories
• CIF2Cell: http://sourceforge.net/projects/cif2cell
– Tool to generate a POSCAR from a Crystallographic Information
Framework (CIF) file.
• Atomic Simulation Environment: https://wiki.fysik.dtu.dk/ase/
• Pymatgen: https://pymatgen.org/index.html
• Others: https://www.vasp.at/index.php/resources