Title: Description of reaction and vibrational energetics of CO₂–NH₃ interaction using quantum computing algorithms

Abstract

CO₂ capture is critical to solving global warming. Amine-based solvents are extensively used to chemically absorb CO₂. Thus, it is crucial to study the chemical absorption of CO₂ by amine-based solvents to better understand and optimize CO₂ capture processes. Here, we use quantum computing algorithms to quantify molecular vibrational energies and reaction pathways between CO₂ and a simplified amine-based solvent model—NH₃. Molecular vibrational properties are important to understanding kinetics of reactions. However, the molecule size correlates with the strength of anharmonicity effect on vibrational properties, which can be challenging to address using classical computing. Quantum computing can help enhance molecular vibrational calculations by including anharmonicity. We implement a variational quantum eigensolver (VQE) algorithm in a quantum simulator to calculate ground state vibrational energies of reactants and products of the CO₂ and NH₃ reaction. The VQE calculations yield ground vibrational energies of CO₂ and NH₃ with similar accuracy to classical computing. In the presence of hardware noise, Compact Heuristic for Chemistry (CHC) ansatz with shallower circuit depth performs better than Unitary Vibrational Coupled Cluster. The “Zero Noise Extrapolation” error-mitigation approach in combination with CHC ansatz improves the vibrational calculation accuracy. Excited vibrational states are accessed with quantum equation of motion methodmore » for CO₂ and NH₃. Using quantum Hartree–Fock (HF) embedding algorithm to calculate electronic energies, the corresponding reaction profile compares favorably with Coupled Cluster Singles and Doubles while being more accurate than HF. Our research showcases quantum computing applications in the study of CO₂ capture reactions.« less

Authors:

Nguyen, Manh Tien  ^[1];

• Search DOE PAGES for author "Nguyen, Manh Tien"
• Search DOE PAGES for ORCID "0000-0001-5264-3583"

Lee, Yueh-Lin  ^[2];

• Search DOE PAGES for author "Lee, Yueh-Lin"
• Search DOE PAGES for ORCID "0000-0003-2477-6412"

Alfonso, Dominic  ^[2];

• Search DOE PAGES for author "Alfonso, Dominic"
• Search DOE PAGES for ORCID "0000-0002-2886-2433"

Shao, Qing  ^[3];

• Search DOE PAGES for author "Shao, Qing"
• Search DOE PAGES for ORCID "0000-0001-9433-1131"

Duan, Yuhua  ^[2]

• Search DOE PAGES for author "Duan, Yuhua"
• Search DOE PAGES for ORCID "0000-0001-7447-0142"

---

+ Show Author Affiliations

1. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States); Univ. of Kentucky, Lexington, KY (United States)
2. National Energy Technology Lab. (NETL), Pittsburgh, PA (United States)
3. Univ. of Kentucky, Lexington, KY (United States)

Publication Date:

Tue Mar 14 00:00:00 EDT 2023

Research Org.:

National Energy Technology Laboratory (NETL), Pittsburgh, PA, Morgantown, WV, and Albany, OR (United States)

Sponsoring Org.:

USDOE Office of Fossil Energy (FE); USDOE Laboratory Directed Research and Development (LDRD) Program

OSTI Identifier:

1962424

Alternate Identifier(s):

OSTI ID: 1961480

Grant/Contract Number:  

1024903; 89243318CFE000003; LDRD #1024903

Resource Type:

Accepted Manuscript

Journal Name:

AVS Quantum Science

Additional Journal Information:

Journal Volume: 5; Journal Issue: 1; Journal ID: ISSN 2639-0213

Publisher:

American Institute of Physics (AIP) - American Vacuum Society

Country of Publication:

United States

Language:

English

Subject:

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Quantum computing; Self consistent field methods; Energy economics; Global warming; Potential energy surfaces; Vibrational properties; Algorithms and data structure; Quantum simulators; Coupled-cluster methods; Reaction mechanisms