Molpro is a comprehensive system of ab initio programs for advanced molecular electronic structure calculations, designed and maintained by H.-J. Werner and P. J. Knowles, and containing contributions from many other authors.
The emphasis of MOLPRO is on highly accurate computations, with extensive treatment of the electron correlation problem through the CASPT2-F12, MRCI-F12, CCSD(T)-F12 and associated methods. These efficient explicitly correlated methods make it possible to obtain results with near complete basis set (CBS) limit accuracy using triple-zeta basis sets. Well parallelised and explicitly correlated local coupled-cluster methods [PNO-LCCSD(T)-F12] allow to easily compute highly accurate energies for molecules with 100-200 atoms.
Efficient DFT and TD-DFT methods with a very large number of density functionals are also available. Analytical gradient techniques and many molecular properties are implemented for a wide range of closed- and open-shell methods, both for ground and electronically excited states. Relativistic effects can be accounted for by using Douglas-Kroll-Hess and Breit-Pauli approaches or effective core potentials.
The reviews in doi:10.1002/wcms.82 and doi:10.1063/5.0005081 summarise with examples the capabilities of the package, and full details can be found in the users' manual.Molpro runs on all modern computing platforms, and is supported by graphical front-ends iMolpro and gmolpro. It is very easy to use for standard applications, but also includes many advanced options for expert applications. Molpro can also be used as a platform for development.
Molpro version 2024.2 has been released in September 2024. It contains new features and improvements, and the changes are summarised here. Any feedback regarding improvements of this version will be appreciated. Introductory licence discounts are available until 30/11/2024 for anyone who has not held a Molpro licence in the last 6 months, with 20% being discounted from the licence fee for the first year of any non-commercial group, site or service licence.
The graphical user input program, iMolpro, has now been ported to Windows, and provides a complete platform for using Molpro on Windows, MacOS and Linux, including the running of jobs both locally and on remote servers. iMolpro is open source and freely available, but requires Molpro to be installed locally. For further details, see here; Self-contained binaries for MacOS, Linux and Windows can be downloaded from here.
Version 2.4.0 of the graphical user interface gmolpro was released in March 2024.