Electric dipole spin resonance
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This article may be too technical for most readers to understand. (August 2015) |
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Theory
Electron spin resonance, also known as electron paramagnetic resonance, is due to the coupling of electron magnetic moment to the external magnetic field through the Hamiltonian describing its Larmor precession. Magnetic moment is related to electron angular momentum as , where is a Landé g-factor. For a free electron in vacuum . Larmor interaction quantizes electron spin energy levels in a dc magnetic field as , and a resonant ac magnetic field of a frequency results in electron paramagnetic resonance.Coupling electron spin to electric fields in vacuum and atoms
An electron moving in vacuum in an ac electric field sees, according to the Lorentz transformation, an ac magnetic field in its center of mass system. However, for slow electrons with this field is so weak that its effect can be neglected. In atoms, electron orbital and spin dynamics are coupled because of the electric field of nuclei as it follows from the Dirac equation. This coupling, known as spin-orbit interaction, is small in the fine-structure constant . However, this constant appears in a combination with the atomic number as ,[1] and this product is of the order of unity already in the middle of the periodic table. This enhancement of the coupling between the orbital and spin dynamics originates from strong electric fields and electron velocities near nuclei. While this mechanism is also expected to couple electron spin to ac electric fields, such an effect has been probably never observed in atomic spectroscopy.Basic mechanisms of Electric Dipole Spin Resonance in crystals
Most important, this enhanced spin-orbit coupling in atoms translates into spin-orbit coupling in crystals formed from such atoms or ions that may be strong even for slow electrons. It becomes an essential part of the band structure of their energy spectrum. The ratio of the spin-orbit splitting of the bands to the forbidden gap becomes a parameter that evaluates the effect of spin-orbit coupling, and it is generically of the order of unity.As a result, even slow electrons in solids experience strong spin-orbit coupling. This means that the Hamiltonian of a free electron in a crystal includes, side by side with the electron quasimomentum also Pauli matrices , and the terms including both of them are not small. Coupling of electron spin to the external electromagnetic field can be found by the substitution as is required by the gauge invariance of the theory, here is the vector potential, and the substitution is known as Peierls substitution. And because the electric field , it becomes coupled to the electron spin and can produce spin-flip transitions.
Electric Dipole Spin Resonance (EDSR) is the electron spin resonance driven by a resonant ac electric field . Because the Compton length cm entering into the Bohr magneton and controlling the coupling of electron spin to ac magnetic field is much shorter than all characteristic lengths of solid state physics, EDSR can be by orders of magnitude stronger than the electron paramagnetic resonance driven by ac magnetic field. EDSR was proposed by Rashba.[2]
EDSR is usually strongest in materials without the inversion center where the two-fold degeneracy of the energy spectrum is lifted and time-symmetric Hamiltonians include products of Pauli matrices and odd powers of the quasimomemtum . In such cases electron spin is coupled to the vector-potential of electromagnetic field. Remarkably, EDSR on free electrons can be observed not only at the spin-resonance frequency but also at its linear combinations with the cyclotron resonance frequency . In narrow-gap semiconductors with inversion center EDSR can emerge due direct coupling of electric field to the anomalous coordinate , see Spin-orbit interaction.
EDSR is allowed both with free carriers and with electrons bound at defects. However, for transitions between Kramers conjugate bound states its intensity is suppressed by a factor where is the separation between adjacent levels of the orbital motion.
Origin of high intensity of EDSR: Simplified theory and physical mechanism
As stated above, various mechanisms of EDSR operate in different crystals. The mechanism of its generically high efficiency is illustrated below as applied to electrons in direct-gap semiconductors of the InSb type. If spin-orbit splitting of energy levels is comparable to the forbidden gap , the effective mass of an electron and its g-factor can be evaluated in the framework of the Kane scheme,[3][4] see [[ perturbation theory]],
where is a coupling parameter between the electron an valence bands, and is the electron mass in vacuum.
Choosing the spin-orbit coupling mechanism based on the anomalous coordinate (see spin-orbit coupling) under the condition , we have
where is electron quasimomentum. Then energy of an electron in a ac electric field is
An electron moving in vacuum with a velocity in an ac electric field sees, according to the Lorentz transformation ab effective magnetic field . Its energy in this field
where is the Bohr magneton and is the speed of light. The ratio of these energies
.
This expression shows explicitly where the dominance of EDSR over the electron paramagnetic resonance comes from. The numerator 0.5MeV of the second factor is a half of the Dirac gap while is of atomic scale, 1eV. The physical mechanism behind the enhancement is based on the fact that inside crystals electrons move in strong field of nuclei, and in the middle of the periodic table the product of the atomic number and the fine-structure constant is of the order of unity, and it is this product that plays the role of the effective coupling constant, cf. spin-orbit coupling. However, one should bear in mind that the above arguments based on effective mass approximation are not applicable to electrons localized in deep centers of the atomic scale. For them the electron paramagnetic resonance is usually the dominant mechanism.
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