MULTICONFIGURATION PAIR-DENSITY FUNCTIONAL THEORY FOR MAGNETIC SYSTEMS
Abstract
We propose a fundamental research program that accurately describes magnetic systems. Magnetism is one of the most basic phenomena in chemical physics that underlies many important chemical and technological applications, including switching and sensing. Historically, magnetism was originally studied in bulk metal and bulk inorganic compounds containing metals. However, in the design of magnetic applications, molecular magnets allow greater flexibility and functionality, but their vast promise for important applications is still mainly untapped. To take greater advantage of the opportunities afforded by molecular magnetism, design efforts need to be guided by a deeper understanding of the electronic structure underlying magnetic effects. This can be greatly aided by advances in the fundamental theory that will address some of the following challenges: (i) Molecular magnets are open-shell systems, usually with more than one unpaired electron. Furthermore, molecular magnets are usually strongly correlated, that is, they are inherently multiconfiguration and thus cannot be treated reliably by many methods that can be used successfully for the treatment of weakly correlated closed-shell singlets, such as most organic molecules. It will therefore be important to further develop and to use multireference methods that are affordable for complex systems. (ii) Many of the most promising magnetic molecules contain heavy metals such as 4d and 5d transition metals, lanthanoids, and actinoids, and such materials require relativistic quantum mechanics for their accurate treatment, including spin-orbit coupling. (iii) Magnetism is ultimately a bulk property, and quantitative treatments cannot be confined to isolated small molecules. (iv) The magnetic properties of materials are often dominated by structural defects, and theoretical methods aimed at studying these systems have to be able to describe defects as well.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Aug 12, 2021
- Source ID
- FA95502010360
Entities
People
- Laura Gagliardi
Organizations
- Air Force Office of Scientific Research
- Regents of the University of Minnesota
- United States Air Force