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

Photon-echo attenuation by dynamical processes in rare-earth-ion-doped crystals

Felix R. Graf, Alois Renn, G. Zumofen, Urs P. Wild

Published Sep 1, 1998• 58 citations
Publisher

Abstract

We study the photon-echo attenuation by various dynamical processes in rare-earth-ion-doped crystals. The experimental investigations concentrate on a ${\mathrm{Pr}}^{3+}:{\mathrm{Eu}}^{3+}:{\mathrm{Nd}}^{3+}$ codoped ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal at low temperatures. Two-pulse photon-echo intensities are measured as a function of the pulse intensities when either the ${\mathrm{Pr}}^{3+}$ or the ${\mathrm{Eu}}^{3+}$ ions are excited. For the quantitative interpretation we consider primarily excitation-induced frequency shifts (EFS) by diagonal and off-diagonal interactions and show that for the systems under consideration EFS are dominated by diagonal interactions. The observed echo attenuation by EFS is compared with the predictions calculated from independent Stark-field measurements and reasonable agreement is obtained. The broadening by spin-ion interactions, by nonequilibrium phonons and the dependence of the echo attenuation on the frequency position in the inhomogeneously broadened band are further investigated.

DOI
10.1103/physrevb.58.5462

Related papers

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

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

Investigations of spectral dynamics in rare earth ion doped crystals using high resolution laser techniques

Graf, Felix R.

Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,

•Jan 1, 1998•5 citations

Quantum Optics and Quantum Information Processing in Rare-Earth-Ion-Doped Crystals

Nicklas Ohlsson

In this thesis, aspects of the use of cryogenically cooled rare-earth-ion-doped crystals in the fields of quantum optics and quantum information processing are addressed. The experiments and theoretical considerations referred to in this thesis are based on the coherent transient interaction between light and the ions in the crystals. A photon echo experiment has been performed where faint optical pulses were accumulated in the crystal. In this experiment, the possibility of single photons acting as two of the optical fields in the photon echo process was investigated. Different aspects on the experiment, which can be viewed as delayed self-interference of a single photon, are discussed in this thesis. A scheme for the possible implementation of quantum information processing in rare-earth-ion-doped crystals is presented. A key feature in this scheme is that small groups of ions, which can be optically manipulated and which interact in a controlled way, can be extracted from a collection of randomly positioned ions in the crystal host. Initial experimental investigations of the scheme, indicating the possibility of implementing quantum gates, are also presented in this thesis. In another experiment, the application of magnetic fields of up to 5 T was seen to increase the lifetime of information stored as frequency-dependent modulation of the population of thulium ions doped into a YAG crystal by several orders of magnitude. This mechanism might be useful in data storage and information processing applications. An experiment in which the same type of crystal was used as the active medium in a photon-echo-based pulse compression experiment, where microsecond long pulses were compressed to nanosecond duration using frequency-chirped light pulses, is also reported in this thesis.

Lund reports on atomic physics•Jan 1, 2003•3 citations

Site interference in Stark-modulated photon echoes

Felix R. Graf, Alois Renn, Urs P. Wild +1 more

We show that Stark-pulse-modulated photon echoes in an impurity-ion-doped crystal are generally characterized by a complex oscillatory behavior with two or more frequency components which results from the interference of the static dipole moment differences of ions located at inequivalent sites. We analyze this phenomenon using group theory and present experimental evidence for a ${\mathrm{Pr}}^{3+}$- and ${\mathrm{Eu}}^{3+}$-codoped ${\mathrm{YAlO}}_{3}$ and a ${\mathrm{Pr}}^{3+}$-doped ${\mathrm{Y}}_{2}$${\mathrm{SiO}}_{5}$ crystal. It is demonstrated that the orientations of the dipole moments and of the crystal axes can be determined with subdegree accuracy.

Physical review. B, Condensed matter•May 1, 1997•27 citations
We study the photon-echo attenuation by various dynamical processes in rare-earth-ion-doped crystals. The experimental investigations concentrate on a Pr3+:Eu3+:Nd3+{\mathrm{Pr}}^{3+}:{\mathrm{Eu}}^{3+}:{\mathrm{Nd}}^{3+}Pr3+:Eu3+:Nd3+ codoped Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ crystal at low temperatures. Two-pulse photon-echo intensities are measured as a function of the pulse intensities when either the Pr3+{\mathrm{Pr}}^{3+}Pr3+ or the Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions are excited. For the quantitative interpretation we consider primarily excitation-induced frequency shifts (EFS) by diagonal and off-diagonal interactions and show that for the systems under consideration EFS are dominated by diagonal interactions. The observed echo attenuation by EFS is compared with the predictions calculated from independent Stark-field measurements and reasonable agreement is obtained. The broadening by spin-ion interactions, by nonequilibrium phonons and the dependence of the echo attenuation on the frequency position in the inhomogeneously broadened band are further investigated.
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.
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.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,
In this thesis, aspects of the use of cryogenically cooled rare-earth-ion-doped crystals in the fields of quantum optics and quantum information processing are addressed. The experiments and theoretical considerations referred to in this thesis are based on the coherent transient interaction between light and the ions in the crystals. A photon echo experiment has been performed where faint optical pulses were accumulated in the crystal. In this experiment, the possibility of single photons acting as two of the optical fields in the photon echo process was investigated. Different aspects on the experiment, which can be viewed as delayed self-interference of a single photon, are discussed in this thesis. A scheme for the possible implementation of quantum information processing in rare-earth-ion-doped crystals is presented. A key feature in this scheme is that small groups of ions, which can be optically manipulated and which interact in a controlled way, can be extracted from a collection of randomly positioned ions in the crystal host. Initial experimental investigations of the scheme, indicating the possibility of implementing quantum gates, are also presented in this thesis. In another experiment, the application of magnetic fields of up to 5 T was seen to increase the lifetime of information stored as frequency-dependent modulation of the population of thulium ions doped into a YAG crystal by several orders of magnitude. This mechanism might be useful in data storage and information processing applications. An experiment in which the same type of crystal was used as the active medium in a photon-echo-based pulse compression experiment, where microsecond long pulses were compressed to nanosecond duration using frequency-chirped light pulses, is also reported in this thesis.
We show that Stark-pulse-modulated photon echoes in an impurity-ion-doped crystal are generally characterized by a complex oscillatory behavior with two or more frequency components which results from the interference of the static dipole moment differences of ions located at inequivalent sites. We analyze this phenomenon using group theory and present experimental evidence for a Pr3+{\mathrm{Pr}}^{3+}Pr3+- and Eu3+{\mathrm{Eu}}^{3+}Eu3+-codoped YAlO3{\mathrm{YAlO}}_{3}YAlO3​ and a Pr3+{\mathrm{Pr}}^{3+}Pr3+-doped Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{SiO}}_{5}SiO5​ crystal. It is demonstrated that the orientations of the dipole moments and of the crystal axes can be determined with subdegree accuracy.