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<p>The combinatorial growth of configuration interaction (CI) has long limited this formally exact quantum chemistry method to only the smallest molecules. Here, we report a numerically exact CI calculation exceeding one quadrillion (10<sup>15</sup>) determinants, made possible by a lossless categorical compression strategy within the small-tensor-product distributed active space (STP-DAS) framework. This approach overcomes the traditional memory bottlenecks of CI by a numerically exact compression of the wavefunction representation and reformulating the most computationally demanding matrix–vector operations. Using this method, we performed a fully relativistic CI calculation of the ground state of HBrTe with over 10<sup>15</sup> complex-valued determinants in just 34.5 h on 1000 computing nodes—the largest CI calculation ever reported. We further achieved fast computation for systems with hundreds of billions of determinants on only a few compute nodes. Extensive benchmarks confirm that the method retains full numerical exactness while cutting memory and computational cost by orders of magnitude. Compared to previous state-of-the-art CI calculations, this work achieves a 1000 times increase in CI space, a 10<sup>6</sup>-fold increase in floating-point operations performed, and a 10<sup>6</sup>-fold improvement in computational speed.</p>

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Numerically exact configuration interaction at quadrillion-determinant scale

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月10日

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  • Agam Shayit,
  • Can Liao,
  • Shiv Upadhyay,
  • Hang Hu,
  • Tianyuan Zhang,
  • A. Eugene DePrince III,
  • Chao Yang,
  • Xiaosong Li

摘要

The combinatorial growth of configuration interaction (CI) has long limited this formally exact quantum chemistry method to only the smallest molecules. Here, we report a numerically exact CI calculation exceeding one quadrillion (1015) determinants, made possible by a lossless categorical compression strategy within the small-tensor-product distributed active space (STP-DAS) framework. This approach overcomes the traditional memory bottlenecks of CI by a numerically exact compression of the wavefunction representation and reformulating the most computationally demanding matrix–vector operations. Using this method, we performed a fully relativistic CI calculation of the ground state of HBrTe with over 1015 complex-valued determinants in just 34.5 h on 1000 computing nodes—the largest CI calculation ever reported. We further achieved fast computation for systems with hundreds of billions of determinants on only a few compute nodes. Extensive benchmarks confirm that the method retains full numerical exactness while cutting memory and computational cost by orders of magnitude. Compared to previous state-of-the-art CI calculations, this work achieves a 1000 times increase in CI space, a 106-fold increase in floating-point operations performed, and a 106-fold improvement in computational speed.