Efficient Implementation of Many-Body Quantum Chemical Methods on the Intel® Xeon Phi Coprocessor

This paper presents the implementation and performance of the highly accurate CCSD(T) quantum chemistry method on the Intel® Xeon Phi coprocessor within the context of the NWChem computational chemistry package. The widespread use of highly correlated methods in electronic structure calculations is contingent upon the interplay between advances in theory and the possibility of utilizing the ever-growing computer power of emerging heterogeneous architectures. We discuss the design decisions of our implementation as well as the optimizations applied to the compute kernels and data transfers between host and coprocessor. We show the feasibility of adopting the Intel® Many Integrated Core Architecture and the Intel Xeon Phi coprocessor for developing efficient computational chemistry modeling tools. Remarkable scalability is demonstrated by benchmarks. Our solution scales up to a total of 62560 cores with the concurrent utilization of Intel® Xeon® processors and Intel Xeon Phi coprocessors.

[1]  Andrew G. Taube,et al.  Improving upon CCSD(T): LambdaCCSD(T). II. Stationary formulation and derivatives. , 2008, The Journal of chemical physics.

[2]  R. Bartlett,et al.  The full CCSDT model for molecular electronic structure , 1987 .

[3]  Piotr Piecuch,et al.  Renormalized coupled-cluster methods exploiting left eigenstates of the similarity-transformed Hamiltonian. , 2005, The Journal of chemical physics.

[4]  Message P Forum,et al.  MPI: A Message-Passing Interface Standard , 1994 .

[5]  David,et al.  Gaussian basis sets for use in correlated molecular calculations . Ill . The atoms aluminum through argon , 1999 .

[6]  Oreste Villa,et al.  Noniterative Multireference Coupled Cluster Methods on Heterogeneous CPU-GPU Systems. , 2013, Journal of chemical theory and computation.

[7]  Angela K. Wilson,et al.  Gaussian basis sets for use in correlated molecular calculations. IX. The atoms gallium through krypton , 1993 .

[8]  Martin Head-Gordon,et al.  A second-order correction to singles and doubles coupled-cluster methods based on a perturbative expansion of a similarity-transformed Hamiltonian , 2000 .

[9]  S. J. Cole,et al.  Towards a full CCSDT model for electron correlation , 1985 .

[10]  S. Hirata.  Tensor Contraction Engine: Abstraction and Automated Parallel Implementation of Configuration-Interaction, Coupled-Cluster, and Many-Body Perturbation Theories , 2003 .

[11]  Alistair P. Rendell,et al.  A direct coupled cluster algorithm for massively parallel computers , 1997 .

[12]  Josef Paldus,et al.  Correlation Problems in Atomic and Molecular Systems. IV. Extended Coupled-Pair Many-Electron Theory and Its Application to the B H 3 Molecule , 1972 .

[13]  J. Stanton.  Why CCSD(T) works: a different perspective , 1997 .

[14]  Henry F. Schaefer,et al.  A new implementation of the full CCSDT model for molecular electronic structure , 1988 .

[15]  Martin Head-Gordon,et al.  A perturbative correction to the quadratic coupled-cluster doubles method for higher excitations , 2002 .

[16]  Tjerk P. Straatsma,et al.  NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations , 2010, Comput. Phys. Commun..

[17]  R. Bartlett,et al.  A full coupled‐cluster singles and doubles model: The inclusion of disconnected triples , 1982 .

[18]  James Reinders,et al.  Intel Xeon Phi Coprocessor High Performance Programming , 2013 .

[19]  Karol Kowalski,et al.  The method of moments of coupled-cluster equations and the renormalized CCSD[T], CCSD(T), CCSD(TQ), and CCSDT(Q) approaches , 2000 .

[20]  R. Bartlett,et al.  Coupled-cluster theory in quantum chemistry , 2007 .

[21]  Edoardo Aprà,et al.  Implementation of the multireference Brillouin-Wigner and Mukherjee's coupled cluster methods with non-iterative triple excitations utilizing reference-level parallelism. , 2012, The Journal of chemical physics.

[22]  Rodney J. Bartlett,et al.  Noniterative energy corrections through fifth-order to the coupled cluster singles and doubles method , 1998 .

[23]  Robert J. Harrison,et al.  Liquid water: obtaining the right answer for the right reasons , 2009, Proceedings of the Conference on High Performance Computing Networking, Storage and Analysis.

[24]  J. Demmel,et al.  Sun Microsystems , 1996 .

[25]  Piotr Piecuch,et al.  Single-reference, size-extensive, non-iterative coupled-cluster approaches to bond breaking and biradicals , 2006 .

[26]  Mihály Kállay,et al.  Coupled-cluster methods including noniterative corrections for quadruple excitations. , 2005, The Journal of chemical physics.

[27]  F. Coester,et al.  Short-range correlations in nuclear wave functions , 1960 .

[28]  So Hirata,et al.  Perturbative corrections to coupled-cluster and equation-of-motion coupled-cluster energies: A determinantal analysis , 2001 .

[29]  Iain Bethune,et al.  Optimising CP2K for the Intel Xeon Phi , 2013 .

[30]  T. H. Dunning.  Gaussian basis sets for use in correlated molecular calculations. I. The atoms boron through neon and hydrogen , 1989 .

[31]  T. Dunning,et al.  Electron affinities of the first‐row atoms revisited. Systematic basis sets and wave functions , 1992 .

[32]  Andrew G. Taube,et al.  Improving upon CCSD(T): LambdaCCSD(T). I. Potential energy surfaces. , 2008, The Journal of chemical physics.

[33]  Jeffrey Goldstone,et al.  Derivation of the Brueckner many-body theory , 1957, Proceedings of the Royal Society of London. Series A. Mathematical and Physical Sciences.

[34]  Sriram Krishnamoorthy,et al.  GPU-Based Implementations of the Noniterative Regularized-CCSD(T) Corrections: Applications to Strongly Correlated Systems. , 2011, Journal of chemical theory and computation.

[35]  F. Coester,et al.  Bound states of a many-particle system , 1958 .

[36]  Anna I. Krylov,et al.  Second order perturbation corrections to singles and doubles coupled-cluster methods: General theory and application to the valence optimized doubles model , 2000 .

[37]  Message Passing Interface Forum.  MPI: A message - passing interface standard , 1994 .

[38]  Mihály Kállay,et al.  Approximate treatment of higher excitations in coupled-cluster theory. , 2005, The Journal of chemical physics.

[39]  Pradeep Dubey,et al.  Improving Communication Performance and Scalability of Native Applications on Intel Xeon Phi Coprocessor Clusters , 2014, 2014 IEEE 28th International Parallel and Distributed Processing Symposium.

[40]  J. Cizek.  On the Correlation Problem in Atomic and Molecular Systems. Calculation of Wavefunction Components in Ursell-Type Expansion Using Quantum-Field Theoretical Methods , 1966 .

[41]  Karol Kowalski,et al.  New coupled-cluster methods with singles, doubles, and noniterative triples for high accuracy calculations of excited electronic states. , 2004, The Journal of chemical physics.

[42]  Sriram Krishnamoorthy,et al.  Scalable implementations of accurate excited-state coupled cluster theories: Application of high-level methods to porphyrin-based systems , 2011, 2011 International Conference for High Performance Computing, Networking, Storage and Analysis (SC).

[43]  M. Head‐Gordon,et al.  A fifth-order perturbation comparison of electron correlation theories , 1989 .

[44]  Karol Kowalski,et al.  Generating functionals based formulation of the method of moments of coupled cluster equations. , 2009, The Journal of chemical physics.

[45]  Marat Valiev,et al.  Extensive regularization of the coupled cluster methods based on the generating functional formalism: application to gas-phase benchmarks and to the SN2 reaction of CHCl3 and OH- in water. , 2009, The Journal of chemical physics.

[46]  John F. Stanton,et al.  INVESTIGATION OF AN ASYMMETRIC TRIPLE-EXCITATION CORRECTION FOR COUPLED-CLUSTER ENERGIES , 1998 .

[47]  David E. Woon,et al.  Gaussian basis sets for use in correlated molecular calculations. IV. Calculation of static electrical response properties , 1994 .