The method of increments and frozen natural orbital (MI-FNO) framework is introduced to help expedite the application of noisy, intermediate-scale quantum (NISQ) devices for quantum chemistry simulations. The MI-FNO framework provides a systematic reduction of the occupied and virtual orbital spaces for quantum chemistry simulations. The correlation energies of the resulting increments from the MI-FNO reduction can then be solved by various algorithms, including quantum algorithms such as the phase estimation algorithm and the variational quantum eigensolver (VQE). The unitary coupled-cluster singles and doubles VQE framework is used to obtain correlation energies for the case of small molecules (i.e., BeH2, CH4, NH3, H2O, and HF) using the cc-pVDZ basis set. The quantum resource requirements are estimated for a constrained geometry complex catalyst that is utilized in industrial settings for the polymerization of α-olefins. We show that the MI-FNO approach provides a significant reduction in the quantum bit (qubit) requirements relative to the full system simulations. We propose that the MI-FNO framework can create scalable examples of quantum chemistry problems that are appropriate for assessing the progress of NISQ devices.
Scaling up electronic structure calculations on quantum computers: The frozen natural orbital based method of increments
Prakash Verma, Lee Huntington, Marc P. Coons, Yukio Kawashima, Takeshi Yamazaki, Arman Zaribafiyan; Scaling up electronic structure calculations on quantum computers: The frozen natural orbital based method of increments. J. Chem. Phys. 21 July 2021; 155 (3): 034110. https://doi.org/10.1063/5.0054647
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