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Quantum defects are atomic defects in materials that provide resources to construct quantum information devices such as single-photon emitters and spin qubits. Recently, two-dimensional (2D) materials gained prominence as a host of quantum defects with many attractive features derived from their atomically thin and layered material formfactor. In this Perspective, we discuss first-principles computational methods and challenges to predict the spin and electronic properties of quantum defects in 2D materials. We focus on the open quantum system nature of the defects and their interaction with external parameters such as electric field, magnetic field, and lattice strain. We also discuss how such prediction and understanding can be used to guide experimental studies, ranging from defect identification to tuning of their spin and optical properties. This Perspective provides significant insights into the interplay between the defect, the host material, and the environment, which will be essential in the pursuit of ideal two-dimensional quantum defect platforms.
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Lessons Learned from Catalysis to Qubits: General Strategies to Build Accessible and Accurate First-Principles Models of Point Defects
Defects and dopants play critical roles in defining the properties of a material. Achieving a mechanistic understanding of how such properties arise is challenging with current experimental methods, and computational approaches suffer from significant modeling limitations that frequently require a posteriori fitting. Consequently, the pace of dopant discovery as a means of tuning material properties for a particular application has been slow. However, recent advances in computation have enabled researchers to move away from semiempirical schemes to reposition density functional theory as a predictive tool and improve the accessibility of highly accurate first-principles methods to all researchers. This Perspective discusses some of these recent achievements that provide more accurate first-principles geometric, thermodynamic, optical, and electronic properties simultaneously. Advancements related to supercells, basis sets, functionals, and optimization protocols, as well as suggestions for evaluating the quality of a computational model through comparison to experimental data, are discussed. Moreover, recent computational results in the fields of energy materials, heterogeneous catalysis, and quantum informatics are reviewed along with an evaluation of current frontiers and opportunities in the field of computational materials chemistry.
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- Award ID(s):
- 2310205
- PAR ID:
- 10530832
- Publisher / Repository:
- ACS
- Date Published:
- Journal Name:
- The Journal of Physical Chemistry C
- Volume:
- 127
- Issue:
- 45
- ISSN:
- 1932-7447
- Page Range / eLocation ID:
- 21930 to 21939
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acs.jpcc.3c06267
