“…Inclusion of the dynamic Jahn-Teller effect, known to occur for Fe 2+ , results in nonmagnetic, ground vibronic levels. 8,9 At the lowest temperatures, only the nondegenerate electronic ground state is occupied, so that Fe 2+ has no permanent magnetic moment in the crystal. Under application of an external magnetic field H, however, the Zeeman interaction H Z = B B · ͑L +2S͒ mixes ⌫ 1 with the higher-lying levels, inducing a magnetic moment along H. This behavior has been referred to as Van Vleck paramagnetism.…”
The Van Vleck paramagnetism of Cd 1−x Fe x Te, a diluted magnetic semiconductor, is explored with electronic Raman spectroscopy of an internal transition of Fe 2+ , on the one hand, and the spin-flip Raman scattering ͑SFRS͒ from donor-bound electrons, on the other. Zeeman splitting of the Raman transition from the nonmagnetic ground state to the first excited state displays patterns consistent with energy levels responsible for the Van Vleck paramagnetism. SFRS, in turn, delineates characteristic features of the Van Vleck magnetization, as expected from s-d exchange interaction. The combination of SFRS and magnetization measurements yielded the s-d exchange constant in Cd 1−x Fe x Te, ␣N 0 = 244± 10 meV.
“…Inclusion of the dynamic Jahn-Teller effect, known to occur for Fe 2+ , results in nonmagnetic, ground vibronic levels. 8,9 At the lowest temperatures, only the nondegenerate electronic ground state is occupied, so that Fe 2+ has no permanent magnetic moment in the crystal. Under application of an external magnetic field H, however, the Zeeman interaction H Z = B B · ͑L +2S͒ mixes ⌫ 1 with the higher-lying levels, inducing a magnetic moment along H. This behavior has been referred to as Van Vleck paramagnetism.…”
The Van Vleck paramagnetism of Cd 1−x Fe x Te, a diluted magnetic semiconductor, is explored with electronic Raman spectroscopy of an internal transition of Fe 2+ , on the one hand, and the spin-flip Raman scattering ͑SFRS͒ from donor-bound electrons, on the other. Zeeman splitting of the Raman transition from the nonmagnetic ground state to the first excited state displays patterns consistent with energy levels responsible for the Van Vleck paramagnetism. SFRS, in turn, delineates characteristic features of the Van Vleck magnetization, as expected from s-d exchange interaction. The combination of SFRS and magnetization measurements yielded the s-d exchange constant in Cd 1−x Fe x Te, ␣N 0 = 244± 10 meV.
“…The theoretical formalism used to treat the Jahn-Teller interaction is similar to that described in detail in Ref. [28] where a study was made of the vibronic states of Fe 2+ in a tetrahedral environment taking into account a weak Jahn-Teller coupling of the orbital ground state multiplet with a phonon of symmetry Γ 3 and a strong interaction of the excited orbital triplet 5 Γ 5 with a phonon of symmetry Γ 5 . The model was successfully applied to explain with high accuracy the positions and intensities of the absorption and emission lines of CdTe:Fe 2+ in the near and far infrared.…”
A theoretical study of the isotopic-mass dependence of the internal transitions of Fe 2+ at a cation site in a cubic zinc-blende semiconductor is presented. The model used is based on crystal-field theory and includes the spinorbit interaction and a weak dynamic Jahn-Teller coupling between the 5 Γ 5 excited manifold of Fe 2+ and a local vibrational mode (LVM) of Γ 5 symmetry. The mass dependence of the LVM frequency is described, in the harmonic approximation, within two different limits: the rigid-cage model and a molecular model. In the rigidcage model, the Fe 2+ ion undergoes a displacement but the rest of the lattice is fixed. In this case, a simple M -1l2 dependence of the frequency is obtained and the Jahn-Teller energy, E JT is independent of the mass. In the molecular model, the four nearest neighbors of the magnetic ion are allowed to move and the LVM then behaves as the Γ 5 mode of a MX 4 tetrahedral molecule leading to a more complicated dependence of the frequency on the isotopic mass and to a mass-dependence of E JT . The theoretical results obtained with these two models are compared with the observed isotopic shifts of the zero-phonon lines in InP:Fe and GaP:Fe corresponding to an optical transition between the vibronic Γ 1 ground state and the lowest Γ 5 state originating from the 5 Γ 5 excited orbital multiplet. A prediction of the isotopic shifts of the zero-phonon line in GaAs:Fe is also presented.
“…are electronic operators whose elements are given by group theoretical considerations [16] and are proportional to E (3) JT or E (5) JT , the JT energies for the 3 and 5 phonons, respectively. The phonon states and their overtones are classified according to the irreducible representations of the group T d and are listed in references [16,18].…”
Abstract.A theoretical study of optical absorption and emission measurements of Fe 2+ as a substitutional impurity in InP and GaP is presented. A new interpretation of the low-temperature absorption spectrum is proposed based on a weak Jahn-Teller interaction between the electronic excited states and a local gap mode of 5 symmetry. The model also includes the crystal potential, hybridization with the orbitals of the ligands of the host crystal, spin-orbit interaction and a weak dynamic Jahn-Teller coupling of the orbital ground state of Fe 2+ with transverse acoustic phonons of 3 symmetry. The theoretical model describes with good accuracy the measured positions and relative intensities of the spectral lines. In addition, the mass dependence of the local gap mode of 5 symmetry reproduces the general features of the fine structures associated with the isotopic shifts of the zero-phonon line and the contribution to the isotopic shifts arising from the difference in zero-point energy between the initial and final states of the transition is evaluated.
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