KEIO RESEARCHERS INFORMATION SYSTEM

Papers 【 Display / hide 】

Papers 【 Display / hide 】

• Excited state calculations using variational quantum eigensolver with spin-restricted ansätze and automatically-adjusted constraints

  Gocho S., Nakamura H., Kanno S., Gao Q., Kobayashi T., Inagaki T., Hatanaka M.

  npj Computational Materials （npj Computational Materials)  9 （ 1 ）  2023.12

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  The ground and excited state calculations at key geometries, such as the Frank–Condon (FC) and the conical intersection (CI) geometries, are essential for understanding photophysical properties. To compute these geometries on noisy intermediate-scale quantum devices, we proposed a strategy that combined a chemistry-inspired spin-restricted ansatz and a new excited state calculation method called the variational quantum eigensolver under automatically-adjusted constraints (VQE/AC). Unlike the conventional excited state calculation method, called the variational quantum deflation, the VQE/AC does not require the pre-determination of constraint weights and has the potential to describe smooth potential energy surfaces. To validate this strategy, we performed the excited state calculations at the FC and CI geometries of ethylene and phenol blue at the complete active space self-consistent field (CASSCF) level of theory, and found that the energy errors were at most 2 kcal mol−1 even on the ibm_kawasaki device.

  • Access to Document (DOI)

• A New Pathway for CO<inf>2</inf>Reduction Relying on the Self-Activation Mechanism of Boron-Doped Diamond Cathode

  Du J., Fiorani A., Inagaki T., Otake A., Murata M., Hatanaka M., Einaga Y.

  JACS Au （JACS Au)  2 （ 6 ） 1375 - 1382 2022.06

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  By means of an initial electrochemical carbon dioxide reduction reaction (eCO2RR), both the reaction current and Faradaic efficiency of the eCO2RR on boron-doped diamond (BDD) electrodes were significantly improved. Here, this effect is referred to as the self-activation of BDD. Generally, the generation of carbon dioxide radical anions (CO2•-) is the most recognized pathway leading to the formation of hydrocarbons and oxygenated products. However, the self-activation process enabled the eCO2RR to take place at a low potential, that is, a low energy, where CO2•- is hardly produced. In this work, we found that unidentate carbonate and carboxylic groups were identified as intermediates during self-activation. Increasing the amount of these intermediates via the self-activation process enhances the performance of eCO2RR. We further evaluated this effect in long-term experiments using a CO2 electrolyzer for formic acid production and found that the electrical-to-chemical energy conversion efficiency reached 50.2% after the BDD self-activation process.

  • Access to Document (DOI)

• Hybrid Monte Carlo method with potential scaling for sampling from the canonical multimodal distribution and imitating the relaxation process

  Inagaki T., Saito S.

  Journal of Chemical Physics （Journal of Chemical Physics)  156 （ 10 ）  2022.03

  ISSN  00219606

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  Hybrid methods that combine molecular dynamics methods capable of analyzing dynamics with Monte Carlo (MC) methods that can efficiently treat thermodynamically stable states are valuable for understanding complex chemical processes in which an equilibrium state is reached through many elementary processes. The hybrid MC (HMC) method is one such promising method; however, it often fails to sample configurations properly from the canonical multimodal distribution due to the rugged potential energy surfaces. In this paper, we extend the HMC method to overcome this difficulty. The new method, which is termed potential scaling HMC (PS-HMC), makes use of an artificially modulated trajectory to propose a new configuration. The trajectory is generated from Hamilton's equations, but the potential energy surface is scaled to be gradually flattened and then recovered to the original surface, which facilitates barrier-crossing processes. We apply the PS-HMC method to three kinds of molecular processes: the thermal motion of argon particles, butane isomerization, and an atom transfer chemical reaction. These applications demonstrate that the PS-HMC method is capable of correctly constructing the canonical ensemble with a multimodal distribution. The sampling efficiency and accepted trajectories are examined to clarify the features of the PS-HMC method. Despite the potential scaling, many reactive atom transfer trajectories (elementary processes) pass through the vicinity of the minimum energy path. Furthermore, we demonstrate that the method can properly imitate the relaxation process owing to the inherent configurational continuity. By comparing the PS-HMC method with other relevant methods, we can conclude that the new method is a unique approach for studying both the dynamic and thermodynamic aspects of chemical processes.

  • Access to Document (DOI)

Research Projects of Competitive Funds, etc. 【 Display / hide 】

Research Projects of Competitive Funds, etc. 【 Display / hide 】

• 分子シミュレーションで探る化学蓄熱の分子論的な律速過程と反応性向上への道

  2021.04

  -

  2025.03

  MEXT,JSPS, Grant-in-Aid for Scientific Research, Grant-in-Aid for Early-Career Scientists , Principal investigator

Courses Taught 【 Display / hide 】

Courses Taught 【 Display / hide 】

• LABORATORIES IN CHEMISTRY 1

  2023

• LABORATORIES IN BASIC CHEMISTRY

  2023

• LABORATORIES IN CHEMISTRY 1

  2022

• LABORATORIES IN BASIC CHEMISTRY

  2022

• LABORATORIES IN CHEMISTRY 1

  2021

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