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Journal of Physics C Solid State Physics

Two-photon spectroscopy of a resonant three-level spin system

R. Boscaino, A Tripo

Published Jan 28, 1978• 5 citations
Publisher

Abstract

Two-photon transitions in a nearly resonant three-level spin system are experimentally investigated at microwave frequencies by detecting the second harmonic (SH) wave emitted by a resonant paramagnetic spin sample. The dependence of the SH intensity and lineshape on the detuning of the intermediate level from the resonance is measured in a dilute ruby sample (Cr 3+ :Al 2 O 3 ). It is shown that the SH output is the coherent superposition of two different contributions which come, respectively, from processes which involve all three levels and from Raman-like processes to which the intermediate level does not take part. The dependence on the intensity and polarisation of the input radiation is measured for each one of the two kinds of processes and interference effects between them are detected.

DOI
10.1088/0022-3719/11/2/019

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Two-photon spectroscopy of a resonant three-level spin system. II. Resonance shift

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Physical Review B•May 17, 2011•3 citations
Two-photon transitions in a nearly resonant three-level spin system are experimentally investigated at microwave frequencies by detecting the second harmonic (SH) wave emitted by a resonant paramagnetic spin sample. The dependence of the SH intensity and lineshape on the detuning of the intermediate level from the resonance is measured in a dilute ruby sample (Cr 3+ :Al 2 O 3 ). It is shown that the SH output is the coherent superposition of two different contributions which come, respectively, from processes which involve all three levels and from Raman-like processes to which the intermediate level does not take part. The dependence on the intensity and polarisation of the input radiation is measured for each one of the two kinds of processes and interference effects between them are detected.
Laser and microwave fields can be mixed in paramagnetic samples in a coherent Raman process. The radiation scattered in the forward direction contains frequency components at the sum and difference frequency. We consider the details of this scattering process in a static magnetic field, where two types of signals appear: magnetic-resonance transitions give rise to signals at fixed magnetic fields, independent of the laser frequency. Another set of resonances is determined by the optical transition frequencies. These resonances are particularly prominent in samples with narrow optical absorption lines. We derive a comprehensive theory that describes both contributions and compare it with experimental data from the R lines of ruby.
Second-harmonic (SH) generation by paramagnetic samples at microwave frequency is considered, and the dependence of its intensity on the total number NNN of active centers is experimentally investigated. The reported results show a N2{N}^{2}N2 dependence of the SH intensity near the resonance condition and a higher NNN dependence in the far wings of the SH line. A qualitative explanation is suggested in which the observed effect is related to the internal correlations established among the spins during the SH generation process, as theoretically investigated in the following paper by Persico.
Doubly resonant Raman electron paramagnetic transitions in ruby (Al2{}_{2}2​O3{}_{3}3​:Cr3+{}^{3+}3+) have been investigated using dye laser excitation tuned across the range of the Zeeman components of its well-known R1{R}_{1}R1​ emission line. With magnetic field B normal to c, the optic axis of ruby, it is seen that the Raman electron paramagnetic resonance (EPR) lines exhibit significant intensity enhancements due to the simultaneous occurrence of ``in resonance'' and ``out resonance,'' as visualized in the Kramers-Heisenberg formalism of inelastic light scattering. The specific Raman EPR features observed in the present study, together with their resonances, however, differ markedly from those observed in our previous investigation with $\mathbf{B}\ensuremath{\parallel}\mathbf{c}$. These differences can be traced to level mixing effects within the Zeeman multiplet of the 4A2{}^{4}{A}_{2}4A2​ (ground) state on the one hand, and the negligible value of ${g}_{\ensuremath{\perp}}$ for the $\mathrm{E\ifmmode \bar{}\else \={}\fi{}}$ (excited) state of the R1{R}_{1}R1​ emission line on the other. Furthermore, we note that with B\ensuremath{\perp}c and under resonant conditions, the experimentally observed \ensuremath{\Delta}mmm === \ifmmode\pm\else\textpm\fi{}1 pair of Stokes and anti-Stokes Raman lines are not connected by time-reversal symmetry.