TY - JOUR

T1 - Inter-Kramers electric quadrupole transitions in high-spin systems induced by resonant alternating inhomogeneous electric field

AU - Maryasov, Alexander G.

AU - Melnikov, Anatoly R.

AU - Fedin, Matvey V.

AU - Veber, Sergey L.

N1 - This work was funded by the Russian Science Foundation, Grant No. 23-73-00042. A.R.M., M.V.F., and S.L.V. acknowledge the Ministry of Science and Higher Education of the Russian Federation for granting access to the equipment for numerical modeling of the powder spectra. A.G.M. acknowledges the Ministry of Science and Higher Education of the Russian Federation for providing a possibility to develop the theoretical methodology for quadrupole transitions (Contract No. 075-00365-25-00). Inter-Kramers electric quadrupole transitions in high-spin systems induced by resonant alternating inhomogeneous electric field / A. G. Maryasov, A. R. Melnikov, M. V. Fedin, S. L. Veber // Journal of Applied Physics. - 2025. - Т. 138. № 12. № 123906. DOI 10.1063/5.0293954

PY - 2025/9/24

Y1 - 2025/9/24

N2 - This study presents a theoretical analysis of the interaction of high-spin systems with inhomogeneous alternating electric field and homogeneous alternating magnetic field that induce electric quadrupole (QT, E2) and magnetic dipole transitions (MT, M1), respectively. In order to distinguish QTs from MTs, an analytical expression for the intensities and selection rules for a model system with a half-integer total spin S = 3 / 2 was derived using the spin Hamiltonian and operator-equivalent approaches. The direct comparison of the absorption patterns for the QT and MT of a model high-spin Co(II) system was performed in a frequency domain corresponding to Frequency Domain Fourier Transform Terahertz Electron Paramagnetic Resonance spectroscopy. This type of systems often exhibits the properties of a single molecular magnet at helium temperatures and is characterized by a large zero field splitting. Despite more flexible selection rules for electric quadrupole transitions, the powder spectra of QT and MT were shown to be similar, emphasizing the need for precise spectral measurements to determine the dominant transition type in high-spin systems. The approach developed in the paper not only solves a rather complex quantum mechanical problem that includes the estimation of the quadrupole moment of unpaired electrons, but also demonstrates a possible way for advanced manipulation of spin states, a capability crucial for the development of quantum computing and information storage technologies.

AB - This study presents a theoretical analysis of the interaction of high-spin systems with inhomogeneous alternating electric field and homogeneous alternating magnetic field that induce electric quadrupole (QT, E2) and magnetic dipole transitions (MT, M1), respectively. In order to distinguish QTs from MTs, an analytical expression for the intensities and selection rules for a model system with a half-integer total spin S = 3 / 2 was derived using the spin Hamiltonian and operator-equivalent approaches. The direct comparison of the absorption patterns for the QT and MT of a model high-spin Co(II) system was performed in a frequency domain corresponding to Frequency Domain Fourier Transform Terahertz Electron Paramagnetic Resonance spectroscopy. This type of systems often exhibits the properties of a single molecular magnet at helium temperatures and is characterized by a large zero field splitting. Despite more flexible selection rules for electric quadrupole transitions, the powder spectra of QT and MT were shown to be similar, emphasizing the need for precise spectral measurements to determine the dominant transition type in high-spin systems. The approach developed in the paper not only solves a rather complex quantum mechanical problem that includes the estimation of the quadrupole moment of unpaired electrons, but also demonstrates a possible way for advanced manipulation of spin states, a capability crucial for the development of quantum computing and information storage technologies.

UR - https://www.mendeley.com/catalogue/6933bfe7-6388-3a71-9a1e-18f82dec4ead/

UR - https://www.scopus.com/inward/record.uri?partnerID=HzOxMe3b&scp=105016992263&origin=inward

U2 - 10.1063/5.0293954

DO - 10.1063/5.0293954

M3 - Article

VL - 138

JO - Journal of Applied Physics

JF - Journal of Applied Physics

SN - 0021-8979

IS - 12

M1 - 123906

ER -