Teplukhin Alexander, Kendrick Brian K, Mniszewski Susan M, Zhang Yu, Kumar Ashutosh, Negre Christian F A, Anisimov Petr M, Tretiak Sergei, Dub Pavel A
Theoretical Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA.
Computer, Computational and Statistical Sciences Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA.
Sci Rep. 2021 Sep 22;11(1):18796. doi: 10.1038/s41598-021-98331-y.
The possibility of using quantum computers for electronic structure calculations has opened up a promising avenue for computational chemistry. Towards this direction, numerous algorithmic advances have been made in the last five years. The potential of quantum annealers, which are the prototypes of adiabatic quantum computers, is yet to be fully explored. In this work, we demonstrate the use of a D-Wave quantum annealer for the calculation of excited electronic states of molecular systems. These simulations play an important role in a number of areas, such as photovoltaics, semiconductor technology and nanoscience. The excited states are treated using two methods, time-dependent Hartree-Fock (TDHF) and time-dependent density-functional theory (TDDFT), both within a commonly used Tamm-Dancoff approximation (TDA). The resulting TDA eigenvalue equations are solved on a D-Wave quantum annealer using the Quantum Annealer Eigensolver (QAE), developed previously. The method is shown to reproduce a typical basis set convergence on the example [Formula: see text] molecule and is also applied to several other molecular species. Characteristic properties such as transition dipole moments and oscillator strengths are computed as well. Three potential energy profiles for excited states are computed for [Formula: see text] as a function of the molecular geometry. Similar to previous studies, the accuracy of the method is dependent on the accuracy of the intermediate meta-heuristic software called qbsolv.
将量子计算机用于电子结构计算的可能性为计算化学开辟了一条充满希望的道路。朝着这个方向，在过去五年中已经取得了许多算法上的进展。绝热量子计算机的原型——量子退火器的潜力尚未得到充分探索。在这项工作中，我们展示了使用D-Wave量子退火器来计算分子系统的激发电子态。这些模拟在许多领域发挥着重要作用，如光伏、半导体技术和纳米科学。使用两种方法处理激发态，即含时哈特里-福克（TDHF）和含时密度泛函理论（TDDFT），均在常用的塔姆-丹科夫近似（TDA）范围内。由此产生的TDA本征值方程在D-Wave量子退火器上使用先前开发的量子退火器本征解算器（QAE）求解。该方法在示例[公式：见正文]分子上被证明能重现典型的基组收敛情况，并且还应用于其他几种分子物种。还计算了诸如跃迁偶极矩和振子强度等特征性质。针对[公式：见正文]作为分子几何结构的函数计算了激发态的三个势能曲线。与先前的研究类似，该方法的准确性取决于名为qbsolv的中间元启发式软件的准确性。
