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Physical Review B

Investigation of the femtosecond inverse Faraday effect using paramagnetic Dy3Al5O12

Alexander H. Reid, Alexey V. Kimel, Andrei I. Kirilyuk, J. F. Gregg, Th. Rasing

Published Mar 8, 2010• 38 citations
Publisher

Abstract

Pump-probe experiments on the rare-earth paramagnet ${\text{Dy}}_{3}{\text{Al}}_{5}{\text{O}}_{12}$ demonstrate that coupling between light and magnetism on the subpicosecond time scale cannot be adequately described by the thermodynamic model of the inverse Faraday effect but instead must be described microscopically by stimulated magneto-Raman scattering. Light-induced paramagnetic resonance, predicted by the thermodynamic theory, is not observed in ${\text{Dy}}_{3}{\text{Al}}_{5}{\text{O}}_{12}$, however, the formation of a coherent superposition between other magnetic sublevels of the ${\text{Dy}}^{3+}$-ion's ground-state multiplet is measured. It is shown that coherence can only be induced between magnetic levels which are connected by the Raman selection rules.

DOI
10.1103/physrevb.81.104404

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Pump-probe experiments on the rare-earth paramagnet Dy3Al5O12{\text{Dy}}_{3}{\text{Al}}_{5}{\text{O}}_{12}Dy3​Al5​O12​ demonstrate that coupling between light and magnetism on the subpicosecond time scale cannot be adequately described by the thermodynamic model of the inverse Faraday effect but instead must be described microscopically by stimulated magneto-Raman scattering. Light-induced paramagnetic resonance, predicted by the thermodynamic theory, is not observed in Dy3Al5O12{\text{Dy}}_{3}{\text{Al}}_{5}{\text{O}}_{12}Dy3​Al5​O12​, however, the formation of a coherent superposition between other magnetic sublevels of the Dy3+{\text{Dy}}^{3+}Dy3+-ion's ground-state multiplet is measured. It is shown that coherence can only be induced between magnetic levels which are connected by the Raman selection rules.
The spin relaxation dynamics of Ce3+{\mathrm{Ce}}^{3+}Ce3+ ions in heavily cerium-doped YAG crystals is studied using pulse-electron paramagnetic resonance and time-resolved pump-probe Faraday rotation. Both techniques address the 4f4f4f ground state, while pump-probe Faraday rotation also provides access to the excited 5d5d5d state. We measure a millisecond spin-lattice relaxation time T1{T}_{1}T1​, a microsecond spin coherence time T2{T}_{2}T2​, and a $\ensuremath{\sim}10$ ns inhomogeneous spin dephasing time T2∗{T}_{2}^{*}T2∗​ for the Ce3+{\mathrm{Ce}}^{3+}Ce3+ ground state at low temperatures. The spin-lattice relaxation of Ce3+{\mathrm{Ce}}^{3+}Ce3+ ions is due to modified Raman processes involving the optical phonon mode at $\ensuremath{\sim}\phantom{\rule{0.16em}{0ex}}125\phantom{\rule{0.16em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The relaxation at higher temperature goes through a first excited level of the 2F52^{2}\mathrm{F}_{\frac{5}{2}}2F25​​ term at about $\ensuremath{\hbar}\ensuremath{\omega}\ensuremath{\approx}228\phantom{\rule{4pt}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. Effects provided by the hyperfine interaction of the Ce3+{\mathrm{Ce}}^{3+}Ce3+ with the 27Al^{27}\mathrm{Al}27Al nuclei are observed.
We report on experimental and theoretical study of the nonlinear Faraday effect under conditions of electromagnetically induced transparency at the $5{S}_{1/2}\ensuremath{\rightarrow}5{P}_{3/2}\ensuremath{\rightarrow}5{D}_{5/2}$ two-photon transition in rubidium vapor. These transitions realize the inverted YYY model which combines the $\ensuremath{\Lambda}$ and ladder systems. Strong nonlinearity allowing for large rotation angles of a probe beam tuned to the $S\ensuremath{\rightarrow}P$ transition was obtained by creation of quantum superpositions of magnetic sublevels (Zeeman coherences) in the rubidium ground state ($\ensuremath{\Lambda}$ scheme). Additionally, electromagnetically induced transparency was accomplished in a ladder scheme by acting with a second strong coupling laser on the $P\ensuremath{\rightarrow}D$ transition. Under conditions of a two-photon resonance the rotation was significantly reduced, which is interpreted as a competition between the coherent processes. The effect was observed in sub-Gauss magnetic fields and could be used for efficient coherent control of generation of the ground-state coherences, e.g., for controlling the polarization state of the probe light.
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.
The inverse Faraday effect (IFE), where a static magnetization is induced by circularly polarized light, offers a promising route to ultrafast control of spin states. Here we study the IFE in Mott insulators using the Floquet theory. We find two distinct IFE behavior governed by the inversion symmetry. In the Mott insulators with inversion symmetry, we find that the effective magnetic field induced by the IFE couples ferromagnetically to the neighboring spins. While for the Mott insulators without inversion symmetry, the effective magnetic field due to IFE couples antiferromagnetically to the neighboring spins. We apply the theory to the spin-orbit coupled single- and multiorbital Hubbard model that is relevant for the Kitaev quantum spin liquid material and demonstrate that the magnetic interactions can be tuned by light.
We report the observation of paramagnetic behavior of an optical lattice operating on the ${F}_{g}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}4\ensuremath{\rightarrow}{F}_{e}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}5$ resonance of cesium. This paramagnetism results from the transfer of population between optical potential wells associated with different magnetic sublevels. The populations are deduced from the amplitudes of stimulated Raman resonances observed in the transmission spectra of probe beams with ${\ensuremath{\sigma}}^{+}$ and ${\ensuremath{\sigma}}^{\ensuremath{-}}$ circular polarizations.
Results of a fairly straightforward experiment on resonant magneto-optical rotation by rubidium-87 atoms revealed strong time-dependence of the polarization plane of light emerging from atomic vapors following a sudden irradiation with a laser beam. The rotation of the plane appears as a not direct consequence of the influence of the magnetic field on atoms. Reported measurements conducted using a vapor cell without any buffer gas or an anti-relaxation wall coating show that transmitted light has initially the same (linear) polarization as the incident one. Rotation of the polarization plane caused by an axial magnetic field develops in time scales similar to the pace of establishing the optical pumping/relaxation equilibrium in the atomic ensemble. The traditional passive Faraday rotation picture providing working description for the resonant magneto-optical effects in steady-state conditions does not explain the observed sequence of evolution of the polarization. The picture has to be augmented with analysis of time dependence in the spatial distribution of relevant quantum states within the atomic ensemble as well as longitudinal and transversal intensity profiles of the light beam. Isolation of external effects caused by the optical pumping and relaxation processes from consequences of internal atomic coherences should uncover more details of mechanisms of the latter in the presence of magnetic field. Plentitude of data available from time-dependent polarization measurements provides strong incentives for further development and tests of comprehensive models of coherent interactions of atomic ensembles with radiation and possibly a base for additional advance in understanding and applications of these phenomena.