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Condensed Matter > Materials Science
Title: Interpreting X-ray absorption spectra of Vanadyl Phthalocyanines Spin Qubit Candidates using a Machine Learning-Assisted Approach
(Submitted on 28 Sep 2023 (v1), last revised 22 Mar 2024 (this version, v5))
Abstract: The magnetic dilution of Vanadyl phthalocyanine (VOPc) within the isostructural diamagnetic Titanyl phthalocyanine (TiOPc) affords promising molecular spin qubit platforms for solid-state quantum computing. The development of quantitative methods for determining how the interactions with a supporting substrate impact the electronic structure of the system are fundamental to determine their potential integration in physical devices. In this work we propose a combined approach based on X-ray absorption spectroscopy (XAS), atomic multiplet calculations, and density functional theory (DFT) to investigate the 3d orbital level structure of VOPc on TiOPc/Ag(100). We characterize VOPc in different molecular environments realized by changing the thickness of TiOPc interlayer and adsorption configuration on Ag(100). Depending on the molecular film structure, we find characteristic XAS features that we analyze using atomic multiplet calculations. We use a Bayesian optimization algorithm to accelerate the parameter search process in the multiplet calculations and identify the ground state properties, such as the 3d orbital occupancy and splitting, as well as intra-atomic interactions. Our analysis indicates that VOPc retains its spin S = 1/2 character in all configurations. Conversely, the energy separation and sequence of the unoccupied V 3d orbitals sensitively depend on the interaction with the surface and TiOPc interlayer. We validate the atomic orbital picture obtained from the multiplet model by comparison with DFT, which further allows us to understand the VOPc electronic properties using a molecular orbital description.
Submission history
From: Fabio Donati [view email][v1] Thu, 28 Sep 2023 13:08:32 GMT (1401kb)
[v2] Thu, 5 Oct 2023 07:34:11 GMT (1655kb)
[v3] Mon, 18 Dec 2023 07:56:58 GMT (2125kb)
[v4] Mon, 19 Feb 2024 08:39:04 GMT (3804kb)
[v5] Fri, 22 Mar 2024 14:15:25 GMT (2768kb)
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