Modeling Singlet Fission on a Quantum Computer

Daniel Claudino; Bo Peng; Karol Kowalski; Travis S. Humble

doi:10.1021/acs.jpclett.3c01106

Modeling Singlet Fission on a Quantum Computer

Daniel Claudino, Bo Peng, Karol Kowalski, Travis S. Humble

Research output: Contribution to journal › Article › peer-review

5 Scopus citations

Abstract

We demonstrate a practical application of quantum computing by using it to investigate the linear H₄ molecule as a simple model for singlet fission. We use the Peeters-Devreese-Soldatov energy functional to calculate the necessary energetics based on the moments of the Hamiltonian estimated on the quantum computer. To reduce the number of required measurements, we use several independent strategies: 1) reduction of the size of the relevant Hilbert space by tapering off qubits; 2) measurement optimization via rotations to eigenbases shared by groups of qubit-wise commuting Pauli strings; and 3) parallel execution of multiple state preparation and measurement operations using all 20 qubits available on the Quantinuum H1-1 quantum hardware. Our results meet the energetic requirements for singlet fission, are in excellent agreement with exact transition energies (for the chosen one-particle basis), and outperform classical methods considered computationally feasible for singlet fission candidates.

Original language	English
Pages (from-to)	5511-5516
Number of pages	6
Journal	Journal of Physical Chemistry Letters
Volume	14
Issue number	24
DOIs	https://doi.org/10.1021/acs.jpclett.3c01106
State	Published - Jun 22 2023

Funding

This work was supported by the “Embedding Quantum Computing into Many-body Frameworks for Strongly Correlated Molecular and Materials Systems” project, which is funded by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, the Division of Chemical Sciences, Geosciences, and Biosciences. This research used resources of the Oak Ridge Leadership Computing Facility at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. This research used resources of the Compute and Data Environment for Science (CADES) at the Oak Ridge National Laboratory, which is supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC05-00OR22725. This manuscript has been authored by UT-Battelle, LLC, under Contract DE-AC0500OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for the United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan.

Funders	Funder number
CADES
Data Environment for Science
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Chemical Sciences, Geosciences, and Biosciences Division	DE-AC05-00OR22725

Access to Document

10.1021/acs.jpclett.3c01106

Cite this

@article{246b423c3e0a40aaa87dd5a623b40d84,

title = "Modeling Singlet Fission on a Quantum Computer",

abstract = "We demonstrate a practical application of quantum computing by using it to investigate the linear H4 molecule as a simple model for singlet fission. We use the Peeters-Devreese-Soldatov energy functional to calculate the necessary energetics based on the moments of the Hamiltonian estimated on the quantum computer. To reduce the number of required measurements, we use several independent strategies: 1) reduction of the size of the relevant Hilbert space by tapering off qubits; 2) measurement optimization via rotations to eigenbases shared by groups of qubit-wise commuting Pauli strings; and 3) parallel execution of multiple state preparation and measurement operations using all 20 qubits available on the Quantinuum H1-1 quantum hardware. Our results meet the energetic requirements for singlet fission, are in excellent agreement with exact transition energies (for the chosen one-particle basis), and outperform classical methods considered computationally feasible for singlet fission candidates.",

author = "Daniel Claudino and Bo Peng and Karol Kowalski and Humble, {Travis S.}",

note = "Publisher Copyright: {\textcopyright} 2023 American Chemical Society.",

year = "2023",

month = jun,

day = "22",

doi = "10.1021/acs.jpclett.3c01106",

language = "English",

volume = "14",

pages = "5511--5516",

journal = "Journal of Physical Chemistry Letters",

issn = "1948-7185",

publisher = "American Chemical Society",

number = "24",

}

TY - JOUR

T1 - Modeling Singlet Fission on a Quantum Computer

AU - Claudino, Daniel

AU - Peng, Bo

AU - Kowalski, Karol

AU - Humble, Travis S.

PY - 2023/6/22

Y1 - 2023/6/22

N2 - We demonstrate a practical application of quantum computing by using it to investigate the linear H4 molecule as a simple model for singlet fission. We use the Peeters-Devreese-Soldatov energy functional to calculate the necessary energetics based on the moments of the Hamiltonian estimated on the quantum computer. To reduce the number of required measurements, we use several independent strategies: 1) reduction of the size of the relevant Hilbert space by tapering off qubits; 2) measurement optimization via rotations to eigenbases shared by groups of qubit-wise commuting Pauli strings; and 3) parallel execution of multiple state preparation and measurement operations using all 20 qubits available on the Quantinuum H1-1 quantum hardware. Our results meet the energetic requirements for singlet fission, are in excellent agreement with exact transition energies (for the chosen one-particle basis), and outperform classical methods considered computationally feasible for singlet fission candidates.

AB - We demonstrate a practical application of quantum computing by using it to investigate the linear H4 molecule as a simple model for singlet fission. We use the Peeters-Devreese-Soldatov energy functional to calculate the necessary energetics based on the moments of the Hamiltonian estimated on the quantum computer. To reduce the number of required measurements, we use several independent strategies: 1) reduction of the size of the relevant Hilbert space by tapering off qubits; 2) measurement optimization via rotations to eigenbases shared by groups of qubit-wise commuting Pauli strings; and 3) parallel execution of multiple state preparation and measurement operations using all 20 qubits available on the Quantinuum H1-1 quantum hardware. Our results meet the energetic requirements for singlet fission, are in excellent agreement with exact transition energies (for the chosen one-particle basis), and outperform classical methods considered computationally feasible for singlet fission candidates.

UR - http://www.scopus.com/inward/record.url?scp=85163568686&partnerID=8YFLogxK

U2 - 10.1021/acs.jpclett.3c01106

DO - 10.1021/acs.jpclett.3c01106

M3 - Article

C2 - 37289995

AN - SCOPUS:85163568686

SN - 1948-7185

VL - 14

SP - 5511

EP - 5516

JO - Journal of Physical Chemistry Letters

JF - Journal of Physical Chemistry Letters

IS - 24

ER -

Modeling Singlet Fission on a Quantum Computer

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this