Quantum Chemistry on Quantum Computers: A Method for Preparation of Multiconfigurational Wave Functions on Quantum Computers without Performing Post-Hartree–Fock Calculations,ACS Central Science

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Quantum Chemistry on Quantum Computers: A Method for Preparation of Multiconfigurational Wave Functions on Quantum Computers without Performing Post-Hartree–Fock Calculations
ACS Central Science ( IF 12.7 ) Pub Date : 2018-12-31 00:00:00 , DOI: 10.1021/acscentsci.8b00788
Kenji Sugisaki ₁ , Shigeaki Nakazawa ₁ , Kazuo Toyota ₁ , Kazunobu Sato ₁ , Daisuke Shiomi ₁ , Takeji Takui _{1,

2}

Affiliation

The full configuration interaction (full-CI) method is capable of providing the numerically best wave functions and energies of atoms and molecules within basis sets being used, although it is intractable for classical computers. Quantum computers can perform full-CI calculations in polynomial time against the system size by adopting a quantum phase estimation algorithm (QPEA). In the QPEA, the preparation of initial guess wave functions having sufficiently large overlap with the exact wave function is recommended. The Hartree–Fock (HF) wave function is a good initial guess only for closed shell singlet molecules and high-spin molecules carrying no spin-β unpaired electrons, around their equilibrium geometry, and thus, the construction of multiconfigurational wave functions without performing post-HF calculations on classical computers is highly desired for applying the method to a wide variety of chemistries and physics. In this work, we propose a method to construct multiconfigurational initial guess wave functions suitable for QPEA-based full-CI calculations on quantum computers, by utilizing diradical characters computed from spin-projected UHF wave functions. The proposed approach drastically improves the wave function overlap, particularly in molecules with intermediate diradical characters.

中文翻译：

量子计算机上的量子化学：一种无需执行后哈特里-福克计算即可在量子计算机上制备多构型波函数的方法

全构型相互作用（full-CI）方法能够提供所使用的基组内原子和分子的数值最佳波函数和能量，尽管这对于经典计算机来说是棘手的。量子计算机可以通过采用量子相位估计算法（QPEA）在多项式时间内针对系统规模执行全CI计算。在 QPEA 中，建议准备与精确波函数具有足够大重叠的初始猜测波函数。 Hartree-Fock (HF) 波函数是一个很好的初始猜测，仅适用于闭壳单线态分子和在其平衡几何结构周围不携带自旋 β 不成对电子的高自旋分子，因此，无需执行后处理即可构建多构型波函数。 - 非常需要在经典计算机上进行高频计算，以便将该方法应用于各种化学和物理领域。在这项工作中，我们提出了一种方法，通过利用自旋投影 UHF 波函数计算出的双根特征来构造适合量子计算机上基于 QPEA 的全 CI 计算的多配置初始猜测波函数。所提出的方法极大地改善了波函数重叠，特别是在具有中间双自由基特征的分子中。

更新日期：2018-12-31

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