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Quantum chemistry simulation of ground- and excited-state properties of the sulfonium cation on a superconducting quantum processor
- Source :
- Chemical Science. 14:2915-2927
- Publication Year :
- 2023
- Publisher :
- Royal Society of Chemistry (RSC), 2023.
-
Abstract
- The computational description of correlated electronic structure, and particularly of excited states of many-electron systems, is an anticipated application for quantum devices. An important ramification is to determine the dominant molecular fragmentation pathways in photo-dissociation experiments of light-sensitive compounds, like sulfonium-based photo-acid generators used in photolithography. Here we simulate the static and dynamical electronic structure of the H$_3$S$^+$ molecule, taken as a minimal model of a triply-bonded sulfur cation, on a superconducting quantum processor of the IBM Falcon architecture. To this end, we generalize a qubit reduction technique termed entanglement forging or EF [A. Eddins et al., Phys. Rev. X Quantum, 2022, 3, 010309], currently restricted to the evaluation of ground-state energies, to the treatment of molecular properties. While in a conventional quantum simulation a qubit represents a spin-orbital, within EF a qubit represents a spatial orbital, reducing the number of required qubits by half. We combine the generalized EF with quantum subspace expansion [W. Colless et al, Phys. Rev. X, 2018, 8, 011021], a technique used to project the time-independent Schrodinger equation for ground and excited states in a subspace. To enable experimental demonstration of this algorithmic workflow, we deploy a sequence of error-mitigation techniques. We compute dipole structure factors and partial atomic charges along the ground- and excited-state potential energy curves, revealing the occurrence of homo- and heterolytic fragmentation. This study is an important step towards the computational description of photo-dissociation on near-term quantum devices, as it can be generalized to other photodissociation processes and naturally extended in different ways to achieve more realistic simulations.<br />13 pages, 7 figures
- Subjects :
- Quantum Physics
FOS: Physical sciences
General Chemistry
Quantum Physics (quant-ph)
Subjects
Details
- ISSN :
- 20416539 and 20416520
- Volume :
- 14
- Database :
- OpenAIRE
- Journal :
- Chemical Science
- Accession number :
- edsair.doi.dedup.....ef74d4c63e730f20543c5ee50842f866