Modern Approaches to Exact Diagonalization and Selected Configuration Interaction with the Adaptive Sampling CI Method
Norm M. Tubman,Norm M. Tubman,C. Daniel Freeman,C. Daniel Freeman,Daniel S. Levine,Daniel S. Levine,Diptarka Hait,Diptarka Hait,Martin Head-Gordon,Martin Head-Gordon,K. Birgitta Whaley,K. Birgitta Whaley +11 more
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TLDR
This work shows that a useful paradigm for generating efficient selected CI/exact diagonalization algorithms is driven by fast sorting algorithms, much in the same way iterative diagonalization is based on the paradigm of matrix vector multipli- cation.Abstract:
Recent advances in selected configuration interaction methods have made them competitive with the most accurate techniques available and, hence, creating an increasingly powerful tool for solving quantum Hamiltonians. In this work, we build on recent advances from the adaptive sampling configuration interaction (ASCI) algorithm. We show that a useful paradigm for generating efficient selected CI/exact diagonalization algorithms is driven by fast sorting algorithms, much in the same way iterative diagonalization is based on the paradigm of matrix vector multiplication. We present several new algorithms for all parts of performing a selected CI, which includes new ASCI search, dynamic bit masking, fast orbital rotations, fast diagonal matrix elements, and residue arrays. The ASCI search algorithm can be used in several different modes, which includes an integral driven search and a coefficient driven search. The algorithms presented here are fast and scalable, and we find that because they are built on fast sorting algorithms they are more efficient than all other approaches we considered. After introducing these techniques, we present ASCI results applied to a large range of systems and basis sets to demonstrate the types of simulations that can be practically treated at the full-CI level with modern methods and hardware, presenting double- and triple-ζ benchmark data for the G1 data set. The largest of these calculations is Si2H6 which is a simulation of 34 electrons in 152 orbitals. We also present some preliminary results for fast deterministic perturbation theory simulations that use hash functions to maintain high efficiency for treating large basis sets.read more
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Software for the frontiers of quantum chemistry: An overview of developments in the Q-Chem 5 package
Evgeny Epifanovsky,Andrew T.B. Gilbert,Andrew T.B. Gilbert,Xintian Feng,Xintian Feng,Joonho Lee,Yuezhi Mao,Narbe Mardirossian,Narbe Mardirossian,Pavel Pokhilko,Alec F. White,Marc P. Coons,Adrian L. Dempwolff,Zhengting Gan,Diptarka Hait,Paul R. Horn,Leif D. Jacobson,Ilya Kaliman,Jörg Kussmann,Adrian W. Lange,Ka Un Lao,Daniel S. Levine,Jie Liu,Jie Liu,Simon C. McKenzie,Adrian F. Morrison,Kaushik D. Nanda,Felix Plasser,Felix Plasser,Dirk R. Rehn,Marta L. Vidal,Zhi-Qiang You,Zhi-Qiang You,Ying Zhu,Bushra Alam,Benjamin J. Albrecht,Abdulrahman Aldossary,Ethan Alguire,J. Andersen,Vishikh Athavale,Dennis Barton,Khadiza Begam,Andrew Behn,Nicole Bellonzi,Yves A. Bernard,Eric J. Berquist,Hugh G. A. Burton,Abel Carreras,Kevin Carter-Fenk,Romit Chakraborty,Romit Chakraborty,Alan D. Chien,Kristina D. Closser,Vale Cofer-Shabica,Saswata Dasgupta,Marc de Wergifosse,Jia Deng,Michael Diedenhofen,Hainam Do,Sebastian Ehlert,Po Tung Fang,Shervin Fatehi,Shervin Fatehi,Shervin Fatehi,Qingguo Feng,Triet Friedhoff,James R. Gayvert,Qinghui Ge,Gergely Gidofalvi,Matthew Goldey,Joseph Gomes,Cristina E. González-Espinoza,Sahil Gulania,Anastasia O. Gunina,Magnus W. D. Hanson-Heine,Phillip H.P. Harbach,Andreas W. Hauser,Michael F. Herbst,Michael F. Herbst,Mario Hernández Vera,Manuel Hodecker,Zachary C. Holden,Shannon E. Houck,Xunkun Huang,Kerwin Hui,Bang C. Huynh,Maxim V. Ivanov,Ádám Jász,Hyunjun Ji,Hanjie Jiang,Benjamin Kaduk,Sven Kähler,Kirill Khistyaev,Jae-Hoon Kim,Gergely Kis,Phil Klunzinger,Zsuzsanna Koczor-Benda,Joong Hoon Koh,Dimitri Kosenkov,Laura Koulias,Tim Kowalczyk,Tim Kowalczyk,Caroline M. Krauter,Karl Y Kue,Alexander A. Kunitsa,Thomas Kus,István Ladjánszki,Arie Landau,Keith V. Lawler,Daniel Lefrancois,Susi Lehtola,Susi Lehtola,Run R. Li,Yi-Pei Li,Jiashu Liang,Marcus Liebenthal,Hung Hsuan Lin,You Sheng Lin,Fenglai Liu,Kuan-Yu Liu,Matthias Loipersberger,Arne Luenser,Aaditya Manjanath,Prashant Uday Manohar,Erum Mansoor,Sam F. Manzer,Shan Ping Mao,Aleksandr V. Marenich,Thomas Markovich,Stephen E. Mason,Simon A. Maurer,Peter F. McLaughlin,Maximilian F. S. J. Menger,Jan-Michael Mewes,Stefanie A. Mewes,Pierpaolo Morgante,J. Wayne Mullinax,Katherine J. Oosterbaan,Katherine J. Oosterbaan,Garrette Paran,Garrette Paran,Alexander C. Paul,Suranjan K. Paul,Fabijan Pavošević,Zheng Pei,Stefan Prager,Emil Proynov,Ádám Rák,Eloy Ramos-Cordoba,Bhaskar Rana,Alan E. Rask,Adam Rettig,Ryan M. Richard,Fazle Rob,Elliot Rossomme,Tarek Scheele,Maximilian Scheurer,Matthias Schneider,Nickolai Sergueev,Shaama Mallikarjun Sharada,Wojciech Skomorowski,David W. Small,Christopher J. Stein,Yu-Chuan Su,Eric J. Sundstrom,Zhen Tao,Jonathan Thirman,Gábor János Tornai,Takashi Tsuchimochi,Norm M. Tubman,Srimukh Prasad Veccham,Oleg A. Vydrov,Jan Wenzel,Jon Witte,Atsushi Yamada,Kun Yao,Sina Yeganeh,Shane R. Yost,Alexander Zech,Igor Ying Zhang,Xing Zhang,Yu Zhang,Dmitry Zuev,Alán Aspuru-Guzik,Alexis T. Bell,Nicholas A. Besley,Ksenia B. Bravaya,Bernard R. Brooks,David Casanova,Jeng-Da Chai,Sonia Coriani,Christopher J. Cramer,György Cserey,A. Eugene DePrince,Robert A. DiStasio,Andreas Dreuw,Barry D. Dunietz,Thomas R. Furlani,William A. Goddard,Sharon Hammes-Schiffer,Teresa Head-Gordon,Warren J. Hehre,Chao-Ping Hsu,Chao-Ping Hsu,Thomas-C. Jagau,Thomas-C. Jagau,Yousung Jung,Andreas Klamt,Jing Kong,Daniel S. Lambrecht,WanZhen Liang,WanZhen Liang,Nicholas J. Mayhall,C. William McCurdy,Jeffrey B. Neaton,Christian Ochsenfeld,John Parkhill,Roberto Peverati,Vitaly A. Rassolov,Yihan Shao,Lyudmila V. Slipchenko,Tim Stauch,Tim Stauch,Ryan P. Steele,Joseph E. Subotnik,Alex J. W. Thom,Alexandre Tkatchenko,Donald G. Truhlar,Troy Van Voorhis,Tomasz Adam Wesolowski,K. Birgitta Whaley,H. Lee Woodcock,Paul M. Zimmerman,Shirin Faraji,Peter Gill,Peter Gill,Martin Head-Gordon,John M. Herbert,Anna I. Krylov +238 more
TL;DR: The Q-Chem quantum chemistry program package as discussed by the authors provides a suite of tools for modeling core-level spectroscopy, methods for describing metastable resonances, and methods for computing vibronic spectra, the nuclear-electronic orbital method, and several different energy decomposition analysis techniques.
Journal ArticleDOI
The Ground State Electronic Energy of Benzene.
Janus J. Eriksen,Tyler A. Anderson,J. Emiliano Deustua,Khaldoon Ghanem,Diptarka Hait,Diptarka Hait,Mark R. Hoffmann,Seung-Hoon Lee,Daniel S. Levine,Ilias Magoulas,Jun Shen,Norm M. Tubman,K. Birgitta Whaley,Enhua Xu,Yuan Yao,Ning Zhang,Ali Alavi,Ali Alavi,Garnet Kin-Lic Chan,Martin Head-Gordon,Martin Head-Gordon,Wenjian Liu,Piotr Piecuch,Sandeep Sharma,Seiichiro Ten-no,Cyrus Umrigar,Jürgen Gauss +26 more
TL;DR: In this study, the findings of a blind challenge devoted to determining the frozen-core, full configuration interaction (FCI) ground-state energy of the benzene molecule in a standard correlation-consistent basis set of double-ζ quality are reported.
Journal ArticleDOI
CASSCF with Extremely Large Active Spaces Using the Adaptive Sampling Configuration Interaction Method
Daniel S. Levine,Daniel S. Levine,Diptarka Hait,Diptarka Hait,Norm M. Tubman,Susi Lehtola,K. Birgitta Whaley,K. Birgitta Whaley,Martin Head-Gordon,Martin Head-Gordon +9 more
TL;DR: In this article, the adaptive sampling configuration interaction (ASCI) method is used as an approximate full active space self-consistent field solver in the active space to solve the orbital optimization problem.
Journal ArticleDOI
Iterative Configuration Interaction with Selection
TL;DR: The iCIPT2 as discussed by the authors algorithm is based on the Epstein-Nesbet second-order perturbation theory (PT2) and is shown to achieve state-of-the-art performance on the C2, O2, Cr2 and C6H6.
Journal ArticleDOI
The Variational Quantum Eigensolver: A review of methods and best practices
TL;DR: The variational quantum eigensolver (or VQE) as mentioned in this paper was proposed to compute the ground state energy of a Hamiltonian, a problem that is central to quantum chemistry and condensed matter physics.
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TL;DR: A summary of the technical advances that are incorporated in the fourth major release of the Q-Chem quantum chemistry program is provided in this paper, covering approximately the last seven years, including developments in density functional theory and algorithms, nuclear magnetic resonance (NMR) property evaluation, coupled cluster and perturbation theories, methods for electronically excited and open-shell species, tools for treating extended environments, algorithms for walking on potential surfaces, analysis tools, energy and electron transfer modelling, parallel computing capabilities, and graphical user interfaces.
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RESEARCH ARTICLE Advances in molecular quantum chemistry contained in the Q-Chem 4 program package
Yihan Shao,Zhengting Gan,Evgeny Epifanovsky,Michael Wormit,Joerg Kussmann,Adrian W. Lange,Andrew Behn,Jia Deng,Xintian Feng,Debashree Ghosh,Matthew Goldey,Paul R. Horn,L eif,J ie Liu,I. Proynov,Ryan M. Richard,Mary A. Rohrdanz,Ryan P. Steele,Eric J. Sundstrom,H. Lee Woodcock,Dmitry Zuev,Ben Albrecht,Ethan Alguire,Brian Austin,Gregory J. O. Beran,Yves A. Bernard,Eric Berquist,Kai Brandhorst,Ksenia B. Bravaya,Shawn T. Brown,David Casanova,Chun-Min Chang,Yunqing Chen,Siu Hung Chien,Kristina D. Closser,Deborah L. Crittenden,Hainam Do,Anthony D. Dutoi,Richard G. Edgar r,Laszlo Fusti-Molnar,Anna Golubeva-Zadorozhnaya,Joseph Gomes,Andreas W. Hauser,Edward G. Hohenstein,Zachary C. Holden +44 more
TL;DR: Detailed benchmarks of the comparative accuracy of modern density functionals for bonded and non-bonded interactions, tests of attenuated second order Møller–Plesset methods for intermolecular interactions, and tests of the accuracy of implicit solvation models are provided.