RESUMEN
The analysis of a chemical reaction along the ground-state potential energy surface in conjunction with an unknown spin state is challenging because electronic states must be separately computed several times using different spin multiplicities to find the lowest energy state. However, in principle, the ground state could be obtained with just a single calculation using a quantum computer without specifying the spin multiplicity in advance. In the present work, ground-state potential energy curves for PtCO were calculated as a proof-of-concept using a variational quantum eigensolver (VQE) algorithm. This system exhibits a singlet-triplet crossover as a consequence of the interaction between Pt and CO. VQE calculations using a statevector simulator were found to converge to a singlet state in the bonding region, while a triplet state was obtained at the dissociation limit. Calculations performed using an actual quantum device provided potential energies within ±2 kcal/mol of the simulated energies after error mitigation techniques were adopted. The spin multiplicities in the bonding and dissociation regions could be clearly distinguished even in the case of a small number of shots. The results of this study suggest that quantum computing can be a powerful tool for the analysis of the chemical reactions of systems for which the spin multiplicity of the ground state and variations in this parameter are not known in advance.
RESUMEN
A new concept of the molecular structure optimization method based on quantum dynamics computations is presented. Nuclei are treated as quantum mechanical particles, as are electrons, and the many-body wave function of the system is optimized by the imaginary time evolution method. The numerical demonstrations with a two-dimensional H2 + system and a H-C-N system exemplify two possible advantages of our proposed method: (1) the optimized nuclear positions can be specified with a small number of observations (quantum measurements) and (2) the global minimum structure of nuclei can be obtained without starting from any sophisticated initial structure and getting stuck in the local minima. This method is considered to be suitable for quantum computers, the development of which will realize its application as a powerful method.
RESUMEN
The possibility of performing quantum-chemical calculations using quantum computers has attracted much interest. Variational quantum deflation (VQD) is a quantum-classical hybrid algorithm for the calculation of excited states with noisy intermediate-scale quantum devices. Although the validity of this method has been demonstrated, there have been few practical applications, primarily because of the uncertain effect of calculation conditions on the results. In the present study, calculations of the core-excited and core-ionized states for common molecules based on the VQD method were examined using a classical computer, focusing on the effects of the weighting coefficients applied in the penalty terms of the cost function. Adopting a simplified procedure for estimating the weighting coefficients based on molecular orbital levels allowed these core-level states to be successfully calculated. The O 1s core-ionized state for a water molecule was calculated with various weighting coefficients, and the resulting ansatz states were systematically examined. The application of this technique to functional materials was demonstrated by calculating the core-level states for titanium dioxide (TiO2) and nitrogen-doped TiO2 models. The results demonstrate that VQD calculations employing an appropriate cost function can be applied to the analysis of functional materials in conjunction with an experimental approach.
