The Localized Active Space Method with Unitary Selective Coupled Cluster

IF 5.7 1区化学 Q2 CHEMISTRY, PHYSICAL

Journal of Chemical Theory and Computation Pub Date : 2024-09-10 DOI:10.1021/acs.jctc.4c0052810.1021/acs.jctc.4c00528

Abhishek Mitra, Ruhee D’Cunha, Qiaohong Wang, Matthew R. Hermes, Yuri Alexeev, Stephen K. Gray*, Matthew Otten* and Laura Gagliardi*,

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Abstract

We introduce a hybrid quantum-classical algorithm, the localized active space unitary selective coupled cluster singles and doubles (LAS-USCCSD) method. Derived from the localized active space unitary coupled cluster (LAS-UCCSD) method, LAS-USCCSD first performs a classical LASSCF calculation, then selectively identifies the most important parameters (cluster amplitudes used to build the multireference UCC ansatz) for restoring interfragment interaction energy using this reduced set of parameters with the variational quantum eigensolver method. We benchmark LAS-USCCSD against LAS-UCCSD by calculating the total energies of (H₂)₂, (H₂)₄, and trans-butadiene, and the magnetic coupling constant for a bimetallic compound [Cr₂(OH)₃(NH₃)₆]³⁺. For these systems, we find that LAS-USCCSD reduces the number of required parameters and thus the circuit depth by at least 1 order of magnitude, an aspect which is important for the practical implementation of multireference hybrid quantum-classical algorithms like LAS-UCCSD on near-term quantum computers.

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具有单元选择性耦合簇的局部主动空间法

我们介绍了一种量子-古典混合算法--局部有源空间单元选择性耦合簇单倍和双倍（LAS-USCCSD）方法。LAS-USCCSD 源自局部有源空间单元耦合簇（LAS-UCCSD）方法，它首先执行经典的 LASSCF 计算，然后利用变异量子等价求解器方法，选择性地确定最重要的参数（用于建立多参考 UCC 方解的簇振幅），以利用这组减少的参数恢复碎片间的相互作用能。我们通过计算 (H2)2、(H2)4 和反式丁二烯的总能量以及双金属化合物 [Cr2(OH)3(NH3)6]3+ 的磁耦合常数，将 LAS-USCCSD 与 LAS-UCCSD 进行了比较。对于这些系统，我们发现 LAS-USCCSD 减少了所需参数的数量，从而将电路深度降低了至少 1 个数量级，这对于在近期量子计算机上实际应用像 LAS-UCCSD 这样的多参考混合量子-经典算法非常重要。

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来源期刊

Journal of Chemical Theory and Computation 化学-物理：原子、分子和化学物理

CiteScore

9.90

自引率

16.40%

发文量

568

审稿时长

1 months

期刊介绍： The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.