Minnesota OpenMolcas Homepage


Mar. 21, 2020

1. OpenMolcas General Information

1.1. OpenMolcas Website

    OpenMolcas is a quantum chemistry package available at
    https://gitlab.com/Molcas/OpenMolcas

    The OpenMolcas online manual is available at
     https://molcas.gitlab.io/OpenMolcas/sphinx

1.2. Reference

    The citation for OpenMolcas is the following [this will be updated when the article is accepted and online]:

"OpenMolcas: From Source Code to Insight," I. F. Galván, M. Vacher, A. Alavi, C. Angeli, J. Autschbach, J. J. Bao, S. I. Bokarev, N. A. Bogdanov, R. K. Carlson, L. F. Chibotaru, J. Creutzberg, N. Dattani, M. G. Delcey, S. S. Dong, A. Dreuw, L. Freitag, L. M. Frutos, L. Gagliardi, F. Gendron, A. Giussani, L. González, G. Grell, M. Guo, C. E. Hoyer , M. Johansson, E. Källman, S. Keller, S. Knecht, G. Kovacevic, G. Li Manni, M. Lundberg, Y. Ma, S. Mai, J. P. Malhado, P. Å. Malmqvist, P. Marquetand, S. A. Mewes, J. Norell, M. Olivucci, , M. Oppel, Q. M. Phung, K. Pierloot, F. Plasser, M. Reiher, A. M. Sand, I. Schapiro, P. Sharma, L. K. Sørensen, C. Stein, D. G. Truhlar, M. Ugandi, L. Ungur, A. Valentini, S. Vancoillie, V. Veryazov, P.-O. Widmark, S. Wouters, J. P. Zobel, and R. Lindh, Journal of Chemical Theory and Computation, Journal of Computational Chemistry 15, 5925-5964 (2019). doi.org/10.1021/acs.jctc.9b00532

    OpenMolcas evolved from Molcas. The final version of Molcas was 8.2, and it was described in the following article:

"Molcas 8: New Capabilities for Multiconfigurational Quantum Chemical Calculations across the Periodic Table," F. Aquilante, J. Autschbach, R. K. Carlson, L. Chibotaru, M. G. Delcey, L. De Vico, I. F. Galván, N. Ferré, L. M. Frutos, L. Gagliardi, M. Garavelli, A. Giussani, C. E. Hoyer, G. Li Manni, H. Lischka, D. Ma, P.-Å. Malmqvist, T. Müller, A. Nenov, M. Olivucci, T. B. Pedersen , D. Peng, F. Plasser, B. Pritchard, M. Reiher, I. Rivalta, I. Schapiro, J. Segarra-Martí, M. Stenrup, D. G. Truhlar, L. Ungur, A. Valentini, S. Vancoillie, V. Veryazov, V. P. Vysotskiy, O. Weingart, F. Zapata, R. Lindh, Journal of Computational Chemistry 37, 506-541 (2016). doi.org/10.1002/jcc.24221

*Minnesota coauthors (at Minnesota at the time the work was done) of Molcas 8.2 are R. K. Carlson, L. Gagliardi, M. Hermes, C. E. Hoyer, G. Li Manni, D. Ma, and D. G. Truhlar.


2. OpenMolcas Enhancements at Minnesota

    OpenMolcas has all or most of the capabilites described in that article plus several new ones contributed by many workers at many institutions. At Minnesota we have made several enhancements beyond what is in version 8.2.
    We list the Minnesota enhancements of OpenMolcas that are fully available from the Gitlab site.
    In the near future, more of our added capabilities will be added to the Gitlab repository, and the present web page will be updated to give more information about the Minnesota-added capabilities of OpenMolcas.

2.1. Multiconfiguration Pair-Density Functional Theory (MC-PDFT)

2.1.1. Introduction to Theory

    Multiconfiguration pair-density functional theory (MC-PDFT) is a post-MCSCF method that evaluates the energy of a state with on-top pair-density function theory.
    Readers may refer to the two following references for the details of the theory.

"Multiconfiguration Pair-Density Functional Theory," G. Li Manni, R. K. Carlson, S. Luo, D. Ma, J. Olsen, D. G. Truhlar, and L. Gagliardi, Journal of Chemical Theory and Computation 10, 3669-3680 (2014). doi.org/10.1021/ct500483t
"Multiconfiguration Pair-Density Functional Theory: A New Way to Treat Strongly Correlated Systems," L. Gagliardi, D. G. Truhlar, G. Li Manni, R. K. Carlson, C. E. Hoyer, and J. L. Bao, Accounts of Chemical Research 50, 66-73 (2017). doi.org/10.1021/acs.accounts.6b00471

    In addition, we provide a description of MC-PDFT capabilities in OpenMolcas (as of 2018 November 9) and some input examples.

2.1.2. MC-PDFT Reference Wave Functions

    The reference wave function for a MC-PDFT calculation include state-averaged or state-specific CASSCF, RASSCF, GASSCF, CAS-CI, RAS-CI, and GAS-CI wave functions.     MC-PDFT can be used in conjunction with density matrix renormalization group (DMRG) method. For DMRG-PDFT calculations, an interface between OpenMolcas and QCMaquis (https://gitlab.com/qc-maquis/) is required. A sample input file for N2 molecule with symmetry is shown here.

2.1.3. MC-PDFT On-Top Functionals

    The following on-top density functionals are available for MC-PDFT: tLSDA, ftLSDA, tPBE, ftPBE, trevPBE, ftrevPBE, tBLYP, ftBLYP, tOPBE, and ftOPBE.

2.2. MC-PDFT Analytic Gradients

2.2.1.State-Specific MC-PDFT Analytic Gradients

    State-specific CASSCF-PDFT analytic gradients as described in:

"Analytic Gradients for Complete Active Space Pair-Density Functional Theory," A. M. Sand, C. E. Hoyer, K. Sharkas, K. M. Kidder, R. Lindh, D. G. Truhlar, and L. Gagliardi, Journal of Chemical Theory and Computation 14, 126-138 (2018). doi.org/10.1021/acs.jctc.7b00967

2.3. Multi-State Pair-Density Functional Theory

2.3.1 State-Interaction Pair-Density Functional Theory (SI-PDFT)

    The SI-PDFT method is described in the following reference:

"State-Interaction Pair-Density Functional Theory," A. M. Sand, C. E. Hoyer, D. G. Truhlar, and L. Gagliardi, The Journal of Chemical Physics 149, 024106 (2018). doi.org/10.1063/1.5036727

2.3.2 Extended Multi-State Pair-Density Functional Theory (XMS-PDFT)

    The manual of the XMS-PDFT method can be found here.

2.4. Natural Transition Orbital (NTO) in RASSI

    The user can run a natural transition orbital calculation in the RASSI module in OpenMolcas (by Jie J. Bao).
    For methodology, usage, keywords and examples, one may refer to the manual for the NTO calculation in the RASSI module.

2.5. Scaling Exchange and Correlation in Density Functionals

2.5.1. Introduction

    The user can scale the exchange terms (by a factor of f_exch) and/or the correlation term (by a factor of f_corr) for a density functionals. This scaling works for KS-DFT calculations and MC-PDFT calculations that use translated or fully translated functionals. (by Sijia S. Dong)

2.5.2. Keyword and Usage

     Keyword:   DFCF
     Usage:        DFCF=f_exch f_corr
     Default:      DFCF=1.0 1.0

    *Note: By setting f_exch as 1.25 and f_corr as 0.5 one can get a High Local Exchange (HLE) density functional

2.5.3. Examples

    Example 1:

&SCF;
KSDFT=BLYP;
DFCF=1.0 0.9

    Example 2:

&MCPDFT;
KSDFT=TPBE;
DFCF=1.25 0.5

2.6. Orbital Contributions

    Orbital contributions of properties can be calculated by the SEWARD module for all orbitals (including virtuals), such as orbital moments. Controlled by the new keyword ORBAll in &SEWARD. (by Sijia S. Dong)

2.7. Energy Decomposition in MC-PDFT

    The MC-PDFT module prints out individual energy components of the MC-PDFT total energy by default. (by Prachi Sharma)


3. Contributors

    J. J. Bao, S. S. Dong, L. Gagliardi, C. E. Hoyer, K. M. Kidder, A. Sand, T. Scott, K. Sharkas, P. Sharma, and D. G. Truhlar.


4. Links to Other Pages of Interest:


This document last modified  by Software Manager