Divergences in classical and quantum linear response and equation of motion formulations
Divergences in classical and quantum linear response and equation of motion formulations
Calculating molecular properties using quantum devices can be performed through the quantum linear response (qLR) or, equivalently, the quantum equation of motion (qEOM) formulations. Different parameterizations of qLR and qEOM are available, namely naïve, projected, self-consistent, and state-transfer. In the naïve and projected parameterizations, the metric is not the identity, and we show that it depends on redundant orbital rotations. This dependency may lead to divergences in the excitation energies for certain choices of the redundant orbital rotation parameters in an idealized noiseless setting. Furthermore, this leads to a significant variance when calculations include statistical noise from finite quantum sampling.
computational chemistry, Quantum Chemistry, quantum computing, Theoretical Chemistry
Kjellgren, Erik Rosendahl
c05eb9d4-e87e-43da-800a-1828d8d7f95f
Reinholdt, Peter
ddb08ed1-8804-437d-816d-d9e7ee558022
Ziems, Karl Michael
6d346238-2471-47c7-b89f-590059caf037
Sauer, Stephan P.A.
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Coriani, Sonia
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Kongsted, Jacob
460ce016-8491-4084-8934-a439c16105c5
25 September 2024
Kjellgren, Erik Rosendahl
c05eb9d4-e87e-43da-800a-1828d8d7f95f
Reinholdt, Peter
ddb08ed1-8804-437d-816d-d9e7ee558022
Ziems, Karl Michael
6d346238-2471-47c7-b89f-590059caf037
Sauer, Stephan P.A.
7a0e1312-165e-4670-ac1c-a0f3541e4181
Coriani, Sonia
a1d68d22-6db5-4c02-9971-097ff3f7bc71
Kongsted, Jacob
460ce016-8491-4084-8934-a439c16105c5
Kjellgren, Erik Rosendahl, Reinholdt, Peter, Ziems, Karl Michael, Sauer, Stephan P.A., Coriani, Sonia and Kongsted, Jacob
(2024)
Divergences in classical and quantum linear response and equation of motion formulations.
Journal of Chemical Physics, 161 (12), [124112].
(doi:10.1063/5.0225409).
Abstract
Calculating molecular properties using quantum devices can be performed through the quantum linear response (qLR) or, equivalently, the quantum equation of motion (qEOM) formulations. Different parameterizations of qLR and qEOM are available, namely naïve, projected, self-consistent, and state-transfer. In the naïve and projected parameterizations, the metric is not the identity, and we show that it depends on redundant orbital rotations. This dependency may lead to divergences in the excitation energies for certain choices of the redundant orbital rotation parameters in an idealized noiseless setting. Furthermore, this leads to a significant variance when calculations include statistical noise from finite quantum sampling.
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Accepted/In Press date: 10 September 2024
Published date: 25 September 2024
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Publisher Copyright:
© 2024 Author(s).
Keywords:
computational chemistry, Quantum Chemistry, quantum computing, Theoretical Chemistry
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Local EPrints ID: 498222
URI: http://eprints.soton.ac.uk/id/eprint/498222
ISSN: 0021-9606
PURE UUID: 938058ee-8e1c-465c-8ffa-d3504797df49
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Date deposited: 12 Feb 2025 17:48
Last modified: 13 Feb 2025 03:16
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Contributors
Author:
Erik Rosendahl Kjellgren
Author:
Peter Reinholdt
Author:
Karl Michael Ziems
Author:
Stephan P.A. Sauer
Author:
Sonia Coriani
Author:
Jacob Kongsted
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