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Condens. Matter 2022, 7, 4 4 of 7 0.2 0.15 0.1 0.05 0 0 0.2 0.4 0.6 0.8 1 1.2 Lithium concentration, x !"#$%&$' ()*%+ SQUID Magnetic ,&$%&$'-()*%+ Compton Figure 2. Magnetic moments for various lithium concentrations x obtained by SQUID magnetometry (black circles) and magnetic Compton profile measurements (red circles). Background colors mark regions of cationic and anionic redox. In order to extract atomic features driving the magnetic behavior in Figure 2, we have carried out a curve-fitting analysis of the magnetic Compton profiles, as illustrated in Figure 3b–d. Figure 3a shows radial distributions of the orphaned O 2p orbital and Mn 3d orbitals. The areas under the radial distributions are normalized to the same value. The magnetic Compton profiles are normalized by the spin magnetic moment for each Li concentration. The curve-fitting is performed by using: ∞∞∞ m = Jmag(pz)dpz = a −JO2p(pz)dpz + b JMn3d(pz)dpz, (5) −∞ −∞ −∞ where a and b are weight parameters, and JO2p(pz) and JMn3d(pz) are the Compton profiles of O 2p [3] and Mn 3d [24] orbitals, respectively. Our analysis is based on DFT simulations [3], which show that electrons on the orphaned O 2p, which occupies the B site of rock-salt-type structure, and Mn 3d states, which partially occupy the A site of rock-salt-type structure, couple antiferromagnetically and that the magnetic contribution from Ti can be neglected. Table 1 summarizes the results of our fit. Table 1. O 2p and Mn 3d contributions to the spin magnetic moments for various lithium concentra- tions. The error bars are based on the number of measured scattered photons. Lithium Concentration 0.4 0.8 1.2 Spin Magnetic Moment 0.157 ± 0.002 0.140 ± 0.002 0.080 ± 0.002 O 2p 0.027 0.022 0.010 Mn 3d 0.184 0.162 0.090 Magnetic moment ( B/f.u.)PDF Image | Magnetic Compton Scattering Study of Li-Rich Battery Materials
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