Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical review. B, Condensed matter

Laser-induced instantaneous spectral diffusion in Tb 3 + compounds as observed in photon-echo experiments

G. K. Liu, R. L. Cone

Published Apr 1, 1990• 61 citations
Publisher

Abstract

We have observed a significant ``instantaneous spectral diffusion'' phenomenon in photon-echo experiments on ${\mathrm{Tb}}^{3+}$:${\mathrm{LiYF}}_{4}$. This laser-induced effect makes observed optical dephasing rates intensity dependent and can also contribute a frequency dependence to the measured rates. A change in the magnetic dipole-dipole interaction between ${\mathrm{Tb}}^{3+}$ echo ions and surrounding ${\mathrm{Tb}}^{3+}$ ions occurs when surrounding ions are excited. This causes an instantaneous shift in the optical frequency of the echo ion that lasts for ${\mathit{T}}_{1}$\ensuremath{\sim}1 msec. Frequency shifts caused by the first excitation pulse have no effect on echo rephasing (${\mathit{T}}_{1}$\ensuremath{\gg}${\mathit{T}}_{2}$), but those caused by the second pulse prevent proper echo rephasing. A summary is given of other ion-lattice and ion-ion interactions that can cause similar laser-induced effects in a wide variety of insulating compounds. There is potential for probing the nature of inhomogeneous broadening.

DOI
10.1103/physrevb.41.6193

Related papers

Stimulated-photon-echo spectroscopy. I. Spectral diffusion in Eu3+ : YAlO3

Ryuzi Yano, Masaharu Mitsunaga, Naoshi Uesugi

Systematic measurements of stimulated-photon-echo intensities as a function of the first-to-second (\ensuremath{\tau}) and second-to-third (T) pulse separations allow the investigation of the dynamical properties of the spectral diffusion for the $^{7}$${\mathit{F}}_{0}$${\mathrm{\ensuremath{-}}}^{5}$${\mathit{D}}_{0}$ transition of a cryogenic ${\mathrm{Eu}}^{3+}$:${\mathrm{YAlO}}_{3}$ sample. The existence of spectral diffusion was verified by the significant broadening (from 1.2 to 7.2 kHz) of the homogeneous linewidth (\ensuremath{\Gamma}) as T increases from microseconds to milliseconds, the effect being attributed to the flip flop of nearby aluminum nuclear spins surrounding the ${\mathrm{Eu}}^{3+}$ ion. A similar broadening effect (from 0.61 kHz, to a few kHz) was also observed in the presence of a static magnetic field ${\mathit{H}}_{0}$=137 G, but with a much slower diffusion rate. To explain these observations, we use three theoretical models: the Bai-Fayer model, the diffusion-equation model, and the Monte Carlo model. Each agrees reasonably well with the experimental data and indicates the flip rates of sub-kHz order at ${\mathit{H}}_{0}$=0 and an order of magnitude lower at 137 G.

Physical review. B, Condensed matter•Jun 1, 1992•26 citations

Photon-echo attenuation in rare-earth-ion-doped crystals

Stefan B. Altner, G. Zumofen, Urs P. Wild +1 more

We study the optical properties of rare-earth-ion-doped inorganic crystals with an emphasis on the dependence of two-pulse photon echoes on the excitation density in the system. The experimental investigations concentrate on ${\mathrm{Pr}}^{3+}$:${\mathrm{Nd}}^{3+}$:${\mathrm{Eu}}^{3+}$ codoped ${\mathrm{Y}}_{2}$Si${\mathrm{O}}_{5}$ and YAl${\mathrm{O}}_{3}$ crystals at low temperatures. With two pulses of one laser the echo is induced in one ion species and with a third, "scrambler" pulse of a second laser another species is excited. These scrambler excitations lead to a dephasing and thus to an echo attenuation which depends on the strength, frequency, and time of the scrambler pulse. The spectral sensitivity of the echo attenuation is used for a spectroscopic technique: "photon-echo attenuation spectroscopy." As a function of the delay time ${t}_{s}$ between the scrambler pulse and the onset of the two-pulse echo sequence the attenuation shows a very specific behavior dictated by the excitation-induced frequency shifts (EFS's). For ${t}_{s}$ between the two echo-inducing pulses the echo intensity is partially regained by the "dephasing-rephasing balancing" of the reversible EFS's. For the theoretical description a stochastic model is introduced and the dephasing by excitation-induced lattice vibrations and by EFS's are analyzed in detail. The present results are discussed in the light of previous experimental and theoretical investigations.

Physical review. B, Condensed matter•Dec 15, 1996•22 citations

Intensity-dependent photon-echo relaxation in rare-earth-doped crystals

Stefan Kröll, E. Y. Xu, M. K. Kim +2 more

Photon-echo-relaxation measurements made on the $^{3}\mathrm{H}_{4}$${\mathrm{\ensuremath{-}}}^{3}$${\mathrm{P}}_{0}$ transition of 0.01 at. % ${\mathrm{Pr}}^{3+}$:YAG (where YAG represents yttrium aluminum garnet), $^{3}\mathrm{H}_{4}$${\mathrm{\ensuremath{-}}}^{1}$${\mathrm{D}}_{2}$ transition in 0.1 at. % ${\mathrm{Pr}}^{3+}$:${\mathrm{YAlO}}_{3}$, and $^{7}\mathrm{F}_{0}$${\mathrm{\ensuremath{-}}}^{5}$${\mathrm{D}}_{0}$ transition in 0.25 at. % ${\mathrm{Eu}}^{3+}$:${\mathrm{YAlO}}_{3}$ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in ${\mathrm{Pr}}^{3+}$:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring ${\mathrm{Pr}}^{3+}$ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.

Physical review. B, Condensed matter•Jun 1, 1990•33 citations

Optically induced shifts in the frequency of the 3 H4 −1 D2 transition of Pr3+ in LaF3

Jiamin Zhang, THOMAS W. MOSSBERG

Photon-echo techniques were employed to measure the homogeneous dephasing rate of the 592.5-nm, $^{3}$${\mathit{H}}_{4\mathrm{\ensuremath{-}}}^{1}$${\mathit{D}}_{2}$, transition of ${\mathrm{Pr}}^{3+}$ as experimental parameters affecting the number of ${\mathrm{Pr}}^{3+}$ ions optically excited were varied. These parameters include the dopant concentration and the intensity, carrier frequency, and bandwidth of the excitation pulses. Dephasing rates are found to contain a background contribution whose magnitude is dependent upon the specific crystal sample studied and a second contribution whose magnitude increases with the number of ${\mathrm{Pr}}^{3+}$ ions changing state in the course of the echo excitation sequence. The second contribution to the dephasing rate is attributed to the presence of optical instantaneous diffusion, i.e., the redistribution of ionic transition frequencies consequent to optical excitation, in the samples.

Physical review. B, Condensed matter•Sep 1, 1993•8 citations

Dephasing-Rephasing Balancing in Photon Echoes by Excitation Induced Frequency Shifts

Stefan B. Altner, Masaharu Mitsunaga, G. Zumofen +1 more

The excitation dephasing in solids resulting from the interaction with neighboring species' excitations is investigated. The frequency shifts due to these interactions are identified by the observation of partial dephasing-rephasing balancing in bichromatic photon-echo experiments applied to rare-earth ion doped crystals. The experimental observations are in good agreement with the predictions obtained from a model which accounts for the disorder in the crystal and for the stochastic nature of the excitations.

Physical Review Letters•Mar 4, 1996•24 citations

Effects of spectral diffusion in incoherent photon-echo experiments

Yue Bai, M. D. Fayer

The application of the incoherent photon-echo experiment to complex systems is analyzed. In systems in which spectral diffusion occurs, incoherent echo measurements do not yield the same optical dephasing rate as conventional two-pulse photon-echo measurements. The difference can be of major significance. To make the calculations explicit, optical dephasing in a glass is considered using the tunneling two-level system model.

Physical review. B, Condensed matter•Jun 15, 1988•21 citations
We have observed a significant ``instantaneous spectral diffusion'' phenomenon in photon-echo experiments on Tb3+{\mathrm{Tb}}^{3+}Tb3+:LiYF4{\mathrm{LiYF}}_{4}LiYF4​. This laser-induced effect makes observed optical dephasing rates intensity dependent and can also contribute a frequency dependence to the measured rates. A change in the magnetic dipole-dipole interaction between Tb3+{\mathrm{Tb}}^{3+}Tb3+ echo ions and surrounding Tb3+{\mathrm{Tb}}^{3+}Tb3+ ions occurs when surrounding ions are excited. This causes an instantaneous shift in the optical frequency of the echo ion that lasts for T1{\mathit{T}}_{1}T1​\ensuremath{\sim}1 msec. Frequency shifts caused by the first excitation pulse have no effect on echo rephasing (T1{\mathit{T}}_{1}T1​\ensuremath{\gg}T2{\mathit{T}}_{2}T2​), but those caused by the second pulse prevent proper echo rephasing. A summary is given of other ion-lattice and ion-ion interactions that can cause similar laser-induced effects in a wide variety of insulating compounds. There is potential for probing the nature of inhomogeneous broadening.
Systematic measurements of stimulated-photon-echo intensities as a function of the first-to-second (\ensuremath{\tau}) and second-to-third (T) pulse separations allow the investigation of the dynamical properties of the spectral diffusion for the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathit{D}}_{0}D0​ transition of a cryogenic Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ sample. The existence of spectral diffusion was verified by the significant broadening (from 1.2 to 7.2 kHz) of the homogeneous linewidth (\ensuremath{\Gamma}) as T increases from microseconds to milliseconds, the effect being attributed to the flip flop of nearby aluminum nuclear spins surrounding the Eu3+{\mathrm{Eu}}^{3+}Eu3+ ion. A similar broadening effect (from 0.61 kHz, to a few kHz) was also observed in the presence of a static magnetic field H0{\mathit{H}}_{0}H0​=137 G, but with a much slower diffusion rate. To explain these observations, we use three theoretical models: the Bai-Fayer model, the diffusion-equation model, and the Monte Carlo model. Each agrees reasonably well with the experimental data and indicates the flip rates of sub-kHz order at H0{\mathit{H}}_{0}H0​=0 and an order of magnitude lower at 137 G.
We study the optical properties of rare-earth-ion-doped inorganic crystals with an emphasis on the dependence of two-pulse photon echoes on the excitation density in the system. The experimental investigations concentrate on Pr3+{\mathrm{Pr}}^{3+}Pr3+:Nd3+{\mathrm{Nd}}^{3+}Nd3+:Eu3+{\mathrm{Eu}}^{3+}Eu3+ codoped Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{O}}_{5}O5​ and YAlO3{\mathrm{O}}_{3}O3​ crystals at low temperatures. With two pulses of one laser the echo is induced in one ion species and with a third, "scrambler" pulse of a second laser another species is excited. These scrambler excitations lead to a dephasing and thus to an echo attenuation which depends on the strength, frequency, and time of the scrambler pulse. The spectral sensitivity of the echo attenuation is used for a spectroscopic technique: "photon-echo attenuation spectroscopy." As a function of the delay time ts{t}_{s}ts​ between the scrambler pulse and the onset of the two-pulse echo sequence the attenuation shows a very specific behavior dictated by the excitation-induced frequency shifts (EFS's). For ts{t}_{s}ts​ between the two echo-inducing pulses the echo intensity is partially regained by the "dephasing-rephasing balancing" of the reversible EFS's. For the theoretical description a stochastic model is introduced and the dephasing by excitation-induced lattice vibrations and by EFS's are analyzed in detail. The present results are discussed in the light of previous experimental and theoretical investigations.
Photon-echo-relaxation measurements made on the 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{3}$P0{\mathrm{P}}_{0}P0​ transition of 0.01 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (where YAG represents yttrium aluminum garnet), 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathrm{D}}_{2}D2​ transition in 0.1 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​, and 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition in 0.25 at. % Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.
Photon-echo techniques were employed to measure the homogeneous dephasing rate of the 592.5-nm, 3^{3}3${\mathit{H}}_{4\mathrm{\ensuremath{-}}}^{1}$D2{\mathit{D}}_{2}D2​, transition of Pr3+{\mathrm{Pr}}^{3+}Pr3+ as experimental parameters affecting the number of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions optically excited were varied. These parameters include the dopant concentration and the intensity, carrier frequency, and bandwidth of the excitation pulses. Dephasing rates are found to contain a background contribution whose magnitude is dependent upon the specific crystal sample studied and a second contribution whose magnitude increases with the number of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions changing state in the course of the echo excitation sequence. The second contribution to the dephasing rate is attributed to the presence of optical instantaneous diffusion, i.e., the redistribution of ionic transition frequencies consequent to optical excitation, in the samples.
The excitation dephasing in solids resulting from the interaction with neighboring species' excitations is investigated. The frequency shifts due to these interactions are identified by the observation of partial dephasing-rephasing balancing in bichromatic photon-echo experiments applied to rare-earth ion doped crystals. The experimental observations are in good agreement with the predictions obtained from a model which accounts for the disorder in the crystal and for the stochastic nature of the excitations.