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AIP conference proceedings

Single-Ion-Induced Magnon Sideband in the Optical Absorption Spectrum of GdCl[sub 3]

Richard S. Meltzer, Hugh C. Wolfe, C. D. Graham, James Jennings Rhyne

Published Jan 1, 1973• 1 citation
Publisher

Abstract

We report the observation of a magnon sideband in the 6P7/2 ⇐ 8S7/2 optical absorption spectrum of Gd+3 in the ferromagnetic insulator GdCl3. The transition energy and its dependence on magnetic field demonstrate this to arise from the simultaneous excitation of a magnon and optical exciton. The decrease in its intensity with increasing magnetic field suggest the source of its intensity is directly connected with the zero‐point spin deviations which occur in a ferromagnet possessing significant magnetic dipolar interactions. The magnitude of the intensity is shown to be consistent with a single‐ion transition mechanism which because of the zero‐point spin deviations allows a small probability for a double‐excitation process. This transition mechanism is distinct from that responsible for the previously observed magnon sidebands in the transition‐metal magnetic insulators.

DOI
10.1063/1.2946879

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Dispersion of the Magnon and Optical-Exciton States of Gd Cl3 and Gd (OH)3 and Their Effect upon the Single-Ion-Induced Absorption Line Shapes

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The high-resolution optical-absorption spectra of the magnetic insulators Gd${\mathrm{Cl}}_{3}$ and Gd${(\mathrm{OH})}_{3}$ in a 35-kG magnetic field are used to demonstrate, for the first time, the influence of the magnon dispersion on the line shapes of single-ion-induced optical transitions. The absorption line shapes for transitions from the first thermally populated spin state to several single-ion states of the $^{6}P_{\frac{7}{2}}$ and $^{6}P_{\frac{5}{2}}$ manifolds of the ${\mathrm{Gd}}^{+3}$ ion are calculated. The initial and final states are properly treated as a magnon and exciton, respectively, including the dispersion of both states. The single-ion transition-moment operator is transformed to a basis in the crystal eigenstates and the resulting absorption line shape is shown to depend on a $\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}$-dependent transition-moment operator weighted by a combined exciton-magnon density of states and the magnon occupation number. The magnon dispersion is calculated from the known ground-state exchange interactions while the exciton dispersion is varied to give a best fit to the observed line shapes. The resulting excited-state exchange parameters are shown to be reasonable. The exciton dispersion is found to be quite significant (up to 2 ${\mathrm{cm}}^{\ensuremath{-}1}$) for one of the excited states. These two materials thus represent the first examples for which the exciton dispersion of the electronically excited states of a rare-earth salt have been directly observed.

Physical review. B, Solid state•Jul 1, 1972•40 citations

EXCITON DYNAMICS FOLLOWING TWO PHOTON ABSORPTION IN GdCl3

Rachid Mahiou, B. Jacquier, R. L. Cone

Observation by fluorescence of direct two photon absorption within the 8S7/2→6P7/2 transition of the Gd3+ ion following excitation with a pulse dye laser is reported. The whole fluorescence spectra correlate well with the ones obtained from the one UV photon absorption. However excitation spectra exhibits a linenarrowing compare to the OPA and an observable shift when decreasing the temperature from 4.4 K down to the ferromagnetic order below Tc = 2.2 K. At these temperatures, exciton decay exhibits a non exponential behaviour which can be only treated as a sum of two expoentials in disagreament with the OPA measurements.

Le Journal de Physique Colloques•Oct 1, 1985•1 citation

One-dimensional energy transfer in GdCl3

Rachid Mahiou, B. Jacquier, Christine Madej

We report the observation of the intrinsic fluorescence of anydrous gadolinium trichloride GdCl3 when laser light is absorbed into the first excited state 6P7/2. With the aid of a frequency doubled pulsed dye laser, we are able to analyze carefully the excitation and emission spectra as well as the decay times over a range of temperatures including that at which the material undergoes a ferromagnetic transition at 2.2 K. At 4.4 K and above, experiments at low excitation density (N0<1014 excited ions/cm3) show that the intrinsic and the impurity induced trap fluorescence dynamics are well described in terms of a fast diffusion and trapping model. When the excitation density is increased anti-Stokes fluorescences appear efficiently; they are assigned to the 6D9/2, 6I7/2→8S7/2 transitions. High excitation density effect on the intrinsic decay as well as the decay of the anti-Stokes fluorescence are nicely reproduced by a theoretical model involving mainly an exciton–exciton annihilation process. Moreover, an excited state absorption mechanism contributes notably to the anti-Stokes fluorescence intensity at t=0 with increasing the excitation density. In the ferromagnetic phase of GdCl3, at 1.5 K, the one-dimensional nature of the exciton diffusion (8S7/2↔6P7/2) is confirmed by the ‘‘incoherent’’ exciton decay analysis using an appropriate model recently developed by Cibert et al. Finally a diffusion length spreading over 2500 visited Gd3+ normal sites is evaluated, knowing the hopping time as a function of the nearest neighbor interactions (nn) in the crude approximation of an ideal two level system in a linear chain of atoms.

The Journal of Chemical Physics•Nov 1, 1988•19 citations

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The authors report a detailed analysis of the intensity and polarisation dependence of the 8 S 7/2 to 6 P 7/2 two-photon transition Stark components of Gd 3+ in the concentrated magnetic insulator Gd(OH) 3 under an applied magnetic field (up to 3.5 T) at very low temperature (2 K). The experimental technique consisted of detecting the ultraviolet 6 P 7/2 to 8 S 7/2 one-photon fluorescent emission resulting from two-photon excitation in the 6 P 7/2 states, using a single pulsed dye-laser beam. The standard second-order theory of Axe is shown to fail in explaining the relative intensities of the Stark components. This is especially true in the case of the Delta M=0 transitions for which strong disagreements are observed. It is shown that the introduction of the third-order contribution involving the spin-orbit interaction within the 4f 6 5d states allows the experimental spectra to be reproduced in a correct way. Finally the effects of ion-ion interactions on the two-photon line profiles are discussed.

Journal of Physics Condensed Matter•Oct 9, 1989•8 citations

Exciton-assisted low-energy magnetic excitations in a photoexcited Mott insulator on a square lattice

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Abstract Photoexcitation of a Mott insulator on a square lattice has weakened the intensity of both single- and two-magnon as observed in time-resolved resonant-inelastic x-ray scattering and time-resolved Raman scattering. However, the spectral change in low-energy regions below the magnons has not been clarified so far. To uncover the nature of photoinduced low-energy magnetic excitations of the Mott insulator, we numerically investigate transient magnetic dynamics in a photoexcited half-filled Hubbard model on the square lattice. After turning off a pump pulse tuned for an absorption edge, new magnetic signals clearly emerge well below magnon energy in both single- and two-magnon excitations. We find that the low-energy excitations are predominantly created via excitonic states at the absorption edge. These exciton-assisted magnetic excitations may provide a possible explanation for low-energy spectral weight in a recent time-resolved two-magnon Raman scattering experiment for insulating YBa2Cu3O6.1.

arXiv:2207.03141•Communications Physics•Mar 5, 2023•2 citations

Optical spectroscopy of single- and two-ion transitions in an antiferromagnetic stoichiometric rare-earth crystal

Masaya Hiraishi, Gabrielle A. Hunter-Smith, Gavin G. G. King +5 more

We characterise optical transitions of neodymium ions (Nd3+) in antiferromagnetic neodymium gallate (NdGaO3) with applied fields up to 3 T. The magnetic phase of this material has not previously been studied with the field along its magnetisation axis. The measured optical spectra indicate three magnetic phases -- antiferromagnetic, intermediate, and paramagnetic -- where the intermediate phase likely forms a different magnetic structure from typical spin-flop phases. The observed absorptions were classified into two distinct families of optical transitions: single-Nd and two-Nd absorptions. We demonstrate that the optical transitions in the antiferromagnetic and paramagnetic phases can be modelled using a standard single-ion crystal-field Hamiltonian that interacts with a mean magnetisation from the rest of the lattice, and we expand that model to encompass pairs of ions, explaining the origins of the two-Nd transitions. This study offers a deeper understanding of the optical transitions in rare-earth antiferromagnetic crystals, which have been recently attracting significant interest for microwave-to-optical quantum transduction, despite being relatively unexplored to date.

quant-pharXiv:2511.07747•Nov 12, 2025
We report the observation of a magnon sideband in the 6P7/2 ⇐ 8S7/2 optical absorption spectrum of Gd+3 in the ferromagnetic insulator GdCl3. The transition energy and its dependence on magnetic field demonstrate this to arise from the simultaneous excitation of a magnon and optical exciton. The decrease in its intensity with increasing magnetic field suggest the source of its intensity is directly connected with the zero‐point spin deviations which occur in a ferromagnet possessing significant magnetic dipolar interactions. The magnitude of the intensity is shown to be consistent with a single‐ion transition mechanism which because of the zero‐point spin deviations allows a small probability for a double‐excitation process. This transition mechanism is distinct from that responsible for the previously observed magnon sidebands in the transition‐metal magnetic insulators.
The high-resolution optical-absorption spectra of the magnetic insulators GdCl3{\mathrm{Cl}}_{3}Cl3​ and Gd(OH)3{(\mathrm{OH})}_{3}(OH)3​ in a 35-kG magnetic field are used to demonstrate, for the first time, the influence of the magnon dispersion on the line shapes of single-ion-induced optical transitions. The absorption line shapes for transitions from the first thermally populated spin state to several single-ion states of the 6P72^{6}P_{\frac{7}{2}}6P27​​ and 6P52^{6}P_{\frac{5}{2}}6P25​​ manifolds of the Gd+3{\mathrm{Gd}}^{+3}Gd+3 ion are calculated. The initial and final states are properly treated as a magnon and exciton, respectively, including the dispersion of both states. The single-ion transition-moment operator is transformed to a basis in the crystal eigenstates and the resulting absorption line shape is shown to depend on a $\stackrel{\ensuremath{\rightarrow}}{\mathrm{k}}$-dependent transition-moment operator weighted by a combined exciton-magnon density of states and the magnon occupation number. The magnon dispersion is calculated from the known ground-state exchange interactions while the exciton dispersion is varied to give a best fit to the observed line shapes. The resulting excited-state exchange parameters are shown to be reasonable. The exciton dispersion is found to be quite significant (up to 2 ${\mathrm{cm}}^{\ensuremath{-}1}$) for one of the excited states. These two materials thus represent the first examples for which the exciton dispersion of the electronically excited states of a rare-earth salt have been directly observed.
Observation by fluorescence of direct two photon absorption within the 8S7/2→6P7/2 transition of the Gd3+ ion following excitation with a pulse dye laser is reported. The whole fluorescence spectra correlate well with the ones obtained from the one UV photon absorption. However excitation spectra exhibits a linenarrowing compare to the OPA and an observable shift when decreasing the temperature from 4.4 K down to the ferromagnetic order below Tc = 2.2 K. At these temperatures, exciton decay exhibits a non exponential behaviour which can be only treated as a sum of two expoentials in disagreament with the OPA measurements.
We report the observation of the intrinsic fluorescence of anydrous gadolinium trichloride GdCl3 when laser light is absorbed into the first excited state 6P7/2. With the aid of a frequency doubled pulsed dye laser, we are able to analyze carefully the excitation and emission spectra as well as the decay times over a range of temperatures including that at which the material undergoes a ferromagnetic transition at 2.2 K. At 4.4 K and above, experiments at low excitation density (N0<1014 excited ions/cm3) show that the intrinsic and the impurity induced trap fluorescence dynamics are well described in terms of a fast diffusion and trapping model. When the excitation density is increased anti-Stokes fluorescences appear efficiently; they are assigned to the 6D9/2, 6I7/2→8S7/2 transitions. High excitation density effect on the intrinsic decay as well as the decay of the anti-Stokes fluorescence are nicely reproduced by a theoretical model involving mainly an exciton–exciton annihilation process. Moreover, an excited state absorption mechanism contributes notably to the anti-Stokes fluorescence intensity at t=0 with increasing the excitation density. In the ferromagnetic phase of GdCl3, at 1.5 K, the one-dimensional nature of the exciton diffusion (8S7/2↔6P7/2) is confirmed by the ‘‘incoherent’’ exciton decay analysis using an appropriate model recently developed by Cibert et al. Finally a diffusion length spreading over 2500 visited Gd3+ normal sites is evaluated, knowing the hopping time as a function of the nearest neighbor interactions (nn) in the crude approximation of an ideal two level system in a linear chain of atoms.
The authors report a detailed analysis of the intensity and polarisation dependence of the 8 S 7/2 to 6 P 7/2 two-photon transition Stark components of Gd 3+ in the concentrated magnetic insulator Gd(OH) 3 under an applied magnetic field (up to 3.5 T) at very low temperature (2 K). The experimental technique consisted of detecting the ultraviolet 6 P 7/2 to 8 S 7/2 one-photon fluorescent emission resulting from two-photon excitation in the 6 P 7/2 states, using a single pulsed dye-laser beam. The standard second-order theory of Axe is shown to fail in explaining the relative intensities of the Stark components. This is especially true in the case of the Delta M=0 transitions for which strong disagreements are observed. It is shown that the introduction of the third-order contribution involving the spin-orbit interaction within the 4f 6 5d states allows the experimental spectra to be reproduced in a correct way. Finally the effects of ion-ion interactions on the two-photon line profiles are discussed.
Abstract Photoexcitation of a Mott insulator on a square lattice has weakened the intensity of both single- and two-magnon as observed in time-resolved resonant-inelastic x-ray scattering and time-resolved Raman scattering. However, the spectral change in low-energy regions below the magnons has not been clarified so far. To uncover the nature of photoinduced low-energy magnetic excitations of the Mott insulator, we numerically investigate transient magnetic dynamics in a photoexcited half-filled Hubbard model on the square lattice. After turning off a pump pulse tuned for an absorption edge, new magnetic signals clearly emerge well below magnon energy in both single- and two-magnon excitations. We find that the low-energy excitations are predominantly created via excitonic states at the absorption edge. These exciton-assisted magnetic excitations may provide a possible explanation for low-energy spectral weight in a recent time-resolved two-magnon Raman scattering experiment for insulating YBa2Cu3O6.1.
We characterise optical transitions of neodymium ions (Nd3+) in antiferromagnetic neodymium gallate (NdGaO3) with applied fields up to 3 T. The magnetic phase of this material has not previously been studied with the field along its magnetisation axis. The measured optical spectra indicate three magnetic phases -- antiferromagnetic, intermediate, and paramagnetic -- where the intermediate phase likely forms a different magnetic structure from typical spin-flop phases. The observed absorptions were classified into two distinct families of optical transitions: single-Nd and two-Nd absorptions. We demonstrate that the optical transitions in the antiferromagnetic and paramagnetic phases can be modelled using a standard single-ion crystal-field Hamiltonian that interacts with a mean magnetisation from the rest of the lattice, and we expand that model to encompass pairs of ions, explaining the origins of the two-Nd transitions. This study offers a deeper understanding of the optical transitions in rare-earth antiferromagnetic crystals, which have been recently attracting significant interest for microwave-to-optical quantum transduction, despite being relatively unexplored to date.