doi: 10.1021/acs.jctc.6b00508.
Epub 2016 Jul 13.
An Efficient Variational Principle for the Direct Optimization of Excited States
Affiliations
- PMID: 27379468
- DOI: 10.1021/acs.jctc.6b00508
Item in Clipboard
An Efficient Variational Principle for the Direct Optimization of Excited States
J Chem Theory Comput.
.
Abstract
We present a variational principle that enables systematically improvable predictions for individual excited states through an efficient Monte Carlo evaluation. We demonstrate its compatibility with different ansatzes and with both real space and Fock space sampling and discuss its potential for use in the solid state. In numerical demonstrations for challenging molecular excitations, the method rivals or surpasses the accuracy of very high level methods using drastically more compact wave function approximations.
Similar articles
-
A Blocked Linear Method for Optimizing Large Parameter Sets in Variational Monte Carlo.J Chem Theory Comput. 2017 Jun 13;13(6):2604-2611. doi: 10.1021/acs.jctc.7b00119. Epub 2017 Jun 1. J Chem Theory Comput. 2017. PMID: 28514597
-
A Generalized Variational Principle with Applications to Excited State Mean Field Theory.J Chem Theory Comput. 2020 Mar 10;16(3):1526-1540. doi: 10.1021/acs.jctc.9b01105. Epub 2020 Feb 22. J Chem Theory Comput. 2020. PMID: 32017562
-
Charge-transfer excited states: Seeking a balanced and efficient wave function ansatz in variational Monte Carlo.J Chem Phys. 2017 Nov 21;147(19):194101. doi: 10.1063/1.4998197. J Chem Phys. 2017. PMID: 29166112
-
Multiple-Resonance Local Wave Functions for Accurate Excited States in Quantum Monte Carlo.J Chem Theory Comput. 2016 Mar 8;12(3):1157-68. doi: 10.1021/acs.jctc.5b01077. Epub 2016 Feb 3. J Chem Theory Comput. 2016. PMID: 26761421
-
Discovery of a general method of solving the Schrödinger and dirac equations that opens a way to accurately predictive quantum chemistry.Acc Chem Res. 2012 Sep 18;45(9):1480-90. doi: 10.1021/ar200340j. Epub 2012 Jun 11. Acc Chem Res. 2012. PMID: 22686372 Review.
Cited by
-
Fighting Noise with Noise: A Stochastic Projective Quantum Eigensolver.J Chem Theory Comput. 2024 Jul 23;20(14):5964-5981. doi: 10.1021/acs.jctc.4c00295. Epub 2024 Jul 2. J Chem Theory Comput. 2024. PMID: 38954827 Free PMC article.
-
Ab initio quantum chemistry with neural-network wavefunctions.Nat Rev Chem. 2023 Oct;7(10):692-709. doi: 10.1038/s41570-023-00516-8. Epub 2023 Aug 9. Nat Rev Chem. 2023. PMID: 37558761 Review.
-
Electronic excited states in deep variational Monte Carlo.Nat Commun. 2023 Jan 17;14(1):274. doi: 10.1038/s41467-022-35534-5. Nat Commun. 2023. PMID: 36650151 Free PMC article.
LinkOut - more resources
Other Literature Sources