Multiple spin state analysis applied to graphite-like carbon-based ferromagnetism

TL;DR

This study uses first-principles calculations to analyze multiple spin states in graphene molecules, revealing stable high-spin states linked to room-temperature ferromagnetism in carbon-based materials.

Contribution

It introduces a multiple spin state analysis approach to identify stable high-spin configurations in graphene molecules, advancing understanding of ferromagnetism in carbon materials.

Findings

High-spin states are most stable in dihydrogenated zigzag edge molecules.

Energy differences suggest stability of room-temperature ferromagnetism.

Nitrogen substitution favors low-spin stable states.

Abstract

Recent experiments indicate room-temperature ferromagnetism in graphite like materials. This paper offers an multiple spin state analysis to find out the origine of ferromagnetism in case of nano meter size graphene molecule.First principle density function theory calculation (DFT-GGA with 631-G basis set) is applied to nano meter size asymmetric graphene fifteen molecules. Major results are,(1) Dihydrogenated zigzag edge molecule like C64H27 show that the most stable (lowest molecular energy) spin state is the highest one as Sz=5/2. Examples for spin density map of Sz=1/2,3/2 and 5/2 is shown in Fig.1. In other molecules like C56H24, C64H25, C64H22 and C64H23 also show the highest spin state most stable as shown in Fig.2. Energy difference between most stable spin state and next one overcome temperature difference 1000K,which suggests a stability of room temperature ferromagnetism. (2) Radical carbon zigzag edge molecules are also analysed. As illustrated in Fig.3, in every five molecule, also the highest spin state is most stable. (3) In contrast, nitrogen substituted molecules like C59N5H22, C61N3H22 etc. show opposite result,that is, the lowest spin state is most stable as shown in Fig.4. There are following three key issues to bring those results. (A) Edge specified localized spin arrangement. (B) Up-Up (also Down-Down) complex spin pairs inside of molecule. (C) Optimized atom position rearrangement depend on the spin state. Detailed mechanism will be discussed in the Symposium. Multiple spin state analysis is very useful to design carbon based ferro-magnet and also to design new spintronic devices.