Breaking the exascale barrier for the electronic structure problem in <i>ab-initio</i> molecular dynamics

Schade, Robert; Kenter, Tobias; Elgabarty, Hossam; Lass, Michael; Kühne, Thomas D.; Plessl, Christian

doi:10.1177/10943420231177631

Cited by 9 publications

(3 citation statements)

References 38 publications

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“…Owing to recent progress in electronic structure calculations [12][13][14] and quantum mechanics/molecular mechanics approaches, 15 the development of reactive force fields, 16 and the emergence of neural network potentials, 17 chemical reactions will increasingly be modeled through simulations rather than through Eyring TST. Thus, models of chemical reactions in large molecular systems with complex environments come within reach.…”

Section: Introductionmentioning

confidence: 99%

Thermal isomerization rates in retinal analogues using Ab‐Initio molecular dynamics

Ghysbrecht,

Keller

2024

J Comput Chem

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For a detailed understanding of chemical processes in nature and industry, we need accurate models of chemical reactions in complex environments. While Eyring transition state theory is commonly used for modeling chemical reactions, it is most accurate for small molecules in the gas phase. A wide range of alternative rate theories exist that can better capture reactions involving complex molecules and environmental effects. However, they require that the chemical reaction is sampled by molecular dynamics simulations. This is a formidable challenge since the accessible simulation timescales are many orders of magnitude smaller than typical timescales of chemical reactions. To overcome these limitations, rare event methods involving enhanced molecular dynamics sampling are employed. In this work, thermal isomerization of retinal is studied using tight‐binding density functional theory. Results from transition state theory are compared to those obtained from enhanced sampling. Rates obtained from dynamical reweighting using infrequent metadynamics simulations were in close agreement with those from transition state theory. Meanwhile, rates obtained from application of Kramers' rate equation to a sampled free energy profile along a torsional dihedral reaction coordinate were found to be up to three orders of magnitude higher. This discrepancy raises concerns about applying rate methods to one‐dimensional reaction coordinates in chemical reactions.

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Section: Introductionmentioning

confidence: 99%

Thermal isomerization rates in retinal analogues using Ab‐Initio molecular dynamics

Ghysbrecht,

Keller

2024

J Comput Chem

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“…The whole calculation was finished in 7 minutes on Frontier using 12 288 AMD GPUs. 26 In the field of density functional theory (DFT), HPC has significantly extended the simulation scale, 27–34 from simulating 1000 atoms with 1200 CPUs at a parallel efficiency of ∼20% in the early stage 27 to simulating SARS-CoV-2 spike proteins with up to 83 million atoms on a high performance platform with 70 400 CPUs plus 4400 GPUs. 34 Overall, HPC is a leading tool to push the electronic structure theory to the limit on modern supercomputers.…”

Section: Introductionmentioning

confidence: 99%

Quantum-centric high performance computing for quantum chemistry

Liu,

Ma,

Shang

et al. 2024

Phys. Chem. Chem. Phys.

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“…Theoretical chemistry has always been one of the main drivers of the development of high-performance computing and computers (HPC) 1 , 2 and is now aiming at saturating the resources of exascale computers. 3 , 4 Since the calculation of electronic structure and dynamics is ultimately NP-hard, this means that classical computing may soon face an exponential wall, not the least when it comes to energy consumption, information is physical. 5 Here, quantum computers may in principle provide exponential advantage for quantum chemistry through quantum superposition and entanglement.…”

Section: Introductionmentioning

confidence: 99%

Complete Active Space Methods for NISQ Devices: The Importance of Canonical Orbital Optimization for Accuracy and Noise Resilience

Triviño

Delcey

Wendin

2023

J. Chem. Theory Comput.

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To avoid the scaling of the number of qubits with the size of the basis set, one can divide the molecular space into active and inactive regions, which is also known as complete active space methods. However, selecting the active space alone is not enough to accurately describe quantum mechanical effects such as correlation. This study emphasizes the importance of optimizing the active space orbitals to describe correlation and improve the basis-dependent Hartree−Fock energies. We will explore classical and quantum computation methods for orbital optimization and compare the chemically inspired ansatz, UCCSD, with the classical full CI approach for describing the active space in both weakly and strongly correlated molecules. Finally, we will investigate the practical implementation of a quantum CASSCF, where hardware-efficient circuits must be used and noise can interfere with accuracy and convergence. Additionally, we will examine the impact of using canonical and noncanonical active orbitals on the convergence of the quantum CASSCF routine in the presence of noise.

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Breaking the exascale barrier for the electronic structure problem in ab-initio molecular dynamics

Cited by 9 publications

References 38 publications

Thermal isomerization rates in retinal analogues using Ab‐Initio molecular dynamics

Thermal isomerization rates in retinal analogues using Ab‐Initio molecular dynamics

Quantum-centric high performance computing for quantum chemistry

Complete Active Space Methods for NISQ Devices: The Importance of Canonical Orbital Optimization for Accuracy and Noise Resilience

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