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arXiv:cond-mat/0408515 · Physical Review B

Hole-burning techniques for isolation and study of individual hyperfine transitions in inhomogeneously broadened solids demonstrated in Pr3+:Y2SiO5

Mattias Nilsson, Lars Rippe, Stefan Kröll, Robert Klieber, Dieter Suter

Published Dec 30, 2004• 201 citations
arXivHTMLPDF

Abstract

Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in ${\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.

DOI
10.1103/physrevb.70.214116

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Hyperfine structure, optical dephasing, and spectral-hole lifetime of single-crystalline Pr3+:La2(WO4)3

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Most of the experiments related to quantum information applications, involving rare-earth doped inorganic crystals, are performed on yttrium orthosilicate single crystals. The work presented here is motivated by the search of new compounds which can be used in the field of quantum computing and/or quantum storage. Relaxation times and hyperfine structure of the $^{3}H_{4}(0)\ensuremath{\rightarrow}^{1}D_{2}(0)$ transition in 1.4% ${\mathrm{Pr}}^{3+}:{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}$ at $4\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ have been measured by photon-echo and spectral-hole-burning techniques. The hyperfine splittings of the ground $^{3}H_{4}(0)$ and the excited $^{1}D_{2}(0)$ states are $14.9\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $24.6\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ and $5.0\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $7.3\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, respectively. An inhomogeneous linewidth of $18.8\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ was measured. A homogeneous linewidth of $25.3\ifmmode\pm\else\textpm\fi{}2.0\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ was obtained with or without an external magnetic field of about $14\phantom{\rule{0.3em}{0ex}}\mathrm{mT}$. The fluorescence dynamics of the $^{1}D_{2}$ level obtained by a direct excitation in the $^{3}H_{4}\ensuremath{\rightarrow}^{1}D_{2}$ transition gives a nonexponential decay which indicates energy-transfer processes. This decay can be accurately fitted by the Inokuti-Hirayama model [J. Chem. Phys. 43, 1978 (1965)] with a radiative lifetime of $61\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ giving a minimal homogeneous linewidth of $2.6\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$. The spectral-hole lifetime due to population redistribution within the ground hyperfine levels is $16\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\mathrm{s}$. The results obtained for the ${\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}$ compound make this crystal an interesting host for quantum applications.

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Rare-earth ion-doped crystals are promising systems for quantum communication and quantum information processing. In particular, paramagnetic rare-earth centers can be utilized to realize quantum coherent interfaces simultaneously for optical and microwave photons. In this paper, we study hyperfine and magnetic properties of a ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal doped with $^{171}\mathrm{Yb}^{3+}$ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin $S=\frac{1}{2}$ and nuclear spin $I=\frac{1}{2}$, which results in the simplest possible hyperfine level structure. In this work, we determine the hyperfine tensors for the ground and excited states on the optical $^{2}\mathrm{F}_{7/2}(0)\ensuremath{\longleftrightarrow}^{2}\mathrm{F}_{5/2}(0)$ transition by combining spectral hole burning and optically detected magnetic resonance techniques. The resulting spin Hamiltonians correctly predict the magnetic-field dependence of all observed optical-hyperfine transitions, from zero applied field up to fields where the Zeeman interaction is dominating the hyperfine interaction. Using the optical absorption spectrum, we can also determine the order of the hyperfine levels in both states. These results pave the way for realizing solid-state optical and microwave quantum memories based on a $^{171}\mathrm{Yb}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal.

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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,

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Persistent spectral hole-burning is extensively studied in many materials. In inorganic materials doped with rare earth ions, we have mainly two mechanisms for hole-burning; one is optical pumping to hyperfine sublevels in rare earth ions, and the other is optically induced rearrangement of local structure around optical centers. In crystals we often observe the hole due to the former mechanism while the hole due to the latter is reported mainly in glasses. Up to now, there seems to be only little study about the correlation between the mechanism of hole-burning and sample-quality or defects. Recently we reported that the character of holes in Y2O3:Pr3+ depends on the quality of samples [1]. In this paper we study the origin of these holes in Y2O3 with a well-controlled manner. For this purpose, we applied hole-burning spectroscopy to various Y2O3:Pr3+(0.2mol%) samples doped with other metallic ions.

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O. Guillot-Noël, Philippe Goldner, Florian Beaudoux +6 more

We studied the hyperfine structure and hyperfine coherent properties of the ${^{3}\text{H}}_{4}(0)\ensuremath{\rightarrow}{^{1}\text{D}}_{2}(0)$ transition of ${\text{Pr}}^{3+}$ ions in a tungstate single crystal ${\text{La}}_{2}{({\text{WO}}_{4})}_{3}$ by hole-burning and photon-echo techniques. This work is motivated by the search of an efficient three level $\ensuremath{\Lambda}$ system in this new compound with which we could build up a quantum memory. By nonconventional hole-burning experiments, the ordering of the hyperfine splittings in the ${^{3}\text{H}}_{4}(0)$ ground state and in the ${^{1}\text{D}}_{2}(0)$ excited state is obtained. The hyperfine splittings are thus ordered: 24.6 and 14.9 MHz for the ${^{3}\text{H}}_{4}(0)$ level and 5.0 and 7.3 MHz for the ${^{1}\text{D}}_{2}(0)$ level. The relative and absolute transition strengths of individual hyperfine transitions are determined by comparing absorption strengths and by measuring the Rabi flopping frequency as the transition is coherently driven. Free induction and Raman echo decays give inhomogeneous and homogeneous hyperfine linewidths of $57\ifmmode\pm\else\textpm\fi{}2$ and $1.25\ifmmode\pm\else\textpm\fi{}0.1\text{ }\text{kHz}$, respectively.

Physical Review B•Apr 27, 2009•30 citations
Due to their narrow homogeneous linewidths, rare-earth ions in inorganic crystals at low temperatures have recently been given considerable attention as test materials for experiments in coherent quantum optics. Because these narrow linewidth transitions have been buried in a wide inhomogeneous line, the scope of experiments that could be carried out in these materials has been limited. However, here we present spectroscopic techniques, based on spectral hole burning and optical pumping, which allow hyperfine transitions that are initially buried within an inhomogeneously broadened absorption line to be studied with no background absorption from other transitions. A sequence of hole-burning pulses is used to isolate selected transitions between hyperfine levels, which makes it possible to directly study properties of the transitions, e.g., transition strengths, and gives access to information that is difficult to obtain in standard hole-burning spectroscopy, such as the ordering of hyperfine levels. The techniques introduced are applicable to absorbers in a solid with long-lived sublevels in the ground state and where the homogeneous linewidth and sublevel separations are smaller than the inhomogeneous broadening of the optical transition. In particular, this includes rare-earth ions doped into inorganic crystals and in the present work the techniques are demonstrated in spectroscopy of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​. Information on the hyperfine structure and relative transition strengths of the 3H4\ensuremath-1D2^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}3H4​\ensuremath-1D2​ hyperfine transitions in Pr3+:Y2SiO5{\mathrm{Pr}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Pr3+:Y2​SiO5​ has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.
Most of the experiments related to quantum information applications, involving rare-earth doped inorganic crystals, are performed on yttrium orthosilicate single crystals. The work presented here is motivated by the search of new compounds which can be used in the field of quantum computing and/or quantum storage. Relaxation times and hyperfine structure of the $^{3}H_{4}(0)\ensuremath{\rightarrow}^{1}D_{2}(0)$ transition in 1.4% Pr3+:La2(WO4)3{\mathrm{Pr}}^{3+}:{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}Pr3+:La2​(WO4​)3​ at 4K4\phantom{\rule{0.3em}{0ex}}\mathrm{K}4K have been measured by photon-echo and spectral-hole-burning techniques. The hyperfine splittings of the ground 3H4(0)^{3}H_{4}(0)3H4​(0) and the excited 1D2(0)^{1}D_{2}(0)1D2​(0) states are $14.9\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $24.6\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ and $5.0\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $7.3\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, respectively. An inhomogeneous linewidth of $18.8\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ was measured. A homogeneous linewidth of $25.3\ifmmode\pm\else\textpm\fi{}2.0\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ was obtained with or without an external magnetic field of about 14mT14\phantom{\rule{0.3em}{0ex}}\mathrm{mT}14mT. The fluorescence dynamics of the 1D2^{1}D_{2}1D2​ level obtained by a direct excitation in the $^{3}H_{4}\ensuremath{\rightarrow}^{1}D_{2}$ transition gives a nonexponential decay which indicates energy-transfer processes. This decay can be accurately fitted by the Inokuti-Hirayama model [J. Chem. Phys. 43, 1978 (1965)] with a radiative lifetime of $61\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ giving a minimal homogeneous linewidth of 2.6kHz2.6\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}2.6kHz. The spectral-hole lifetime due to population redistribution within the ground hyperfine levels is $16\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\mathrm{s}$. The results obtained for the La2(WO4)3{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}La2​(WO4​)3​ compound make this crystal an interesting host for quantum applications.
Laser induced hole burning in optical absorption bands of low temperature solids has been investigated with emphasis on mechanisms for population hole burning, the interactions with the environment which limit the hole widths and the use of hole burning for ultra high resolution spectroscopy. Hole burning was observed in a wide range of solids including organic and organometallic molecules in crystals and rare earth ions in crystals and glasses. The mechanisms for hole burning also varied widely and a new mechanism involving optically induced nuclear spin flips of near neighbor nuclei was discovered. Examples of hole burning in new classes of materials are presented here for the first time, namely inorganic glasses (silicate glasses containing Nd(3+), Pr(3+) or Eu(3+)) and undoped stoichiometric compounds (e.g., EuP5O14). Hole recovery was used to determine nuclear spin lattice relaxation rates in praseodymium doped crystals. For allowed optical transitions (e.g., singlet states of zinc porphyrin, dibromoindigo and color centers in alkali halides) the hole widths at 2K are limited by population decay to approximately 50 MHz. For longer lived optical levels in crystalline materials, e.g., those containing rare earth ions, the hole widths are narrower (less than 10 MHz) and are limited by dynamical interactions with surrounding nuclei. In amorphous materials such as europium doped silicate glass, hole widths are much broader, being limited by low frequency tunneling motions. Hole burning measurements were complemented by time domain coherent transient (photon echo, and optical free decay) measurements of homogeneous linewidths which enabled us to measure optical resonances as narrow as 760 Hz in Eu(3+):Y2O3.
Rare-earth ion-doped crystals are promising systems for quantum communication and quantum information processing. In particular, paramagnetic rare-earth centers can be utilized to realize quantum coherent interfaces simultaneously for optical and microwave photons. In this paper, we study hyperfine and magnetic properties of a Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ crystal doped with 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin S=12S=\frac{1}{2}S=21​ and nuclear spin I=12I=\frac{1}{2}I=21​, which results in the simplest possible hyperfine level structure. In this work, we determine the hyperfine tensors for the ground and excited states on the optical $^{2}\mathrm{F}_{7/2}(0)\ensuremath{\longleftrightarrow}^{2}\mathrm{F}_{5/2}(0)$ transition by combining spectral hole burning and optically detected magnetic resonance techniques. The resulting spin Hamiltonians correctly predict the magnetic-field dependence of all observed optical-hyperfine transitions, from zero applied field up to fields where the Zeeman interaction is dominating the hyperfine interaction. Using the optical absorption spectrum, we can also determine the order of the hyperfine levels in both states. These results pave the way for realizing solid-state optical and microwave quantum memories based on a 171Yb3+:Y2SiO5^{171}\mathrm{Yb}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}171Yb3+:Y2​SiO5​ crystal.
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,
Persistent spectral hole-burning is extensively studied in many materials. In inorganic materials doped with rare earth ions, we have mainly two mechanisms for hole-burning; one is optical pumping to hyperfine sublevels in rare earth ions, and the other is optically induced rearrangement of local structure around optical centers. In crystals we often observe the hole due to the former mechanism while the hole due to the latter is reported mainly in glasses. Up to now, there seems to be only little study about the correlation between the mechanism of hole-burning and sample-quality or defects. Recently we reported that the character of holes in Y2O3:Pr3+ depends on the quality of samples [1]. In this paper we study the origin of these holes in Y2O3 with a well-controlled manner. For this purpose, we applied hole-burning spectroscopy to various Y2O3:Pr3+(0.2mol%) samples doped with other metallic ions.
We studied the hyperfine structure and hyperfine coherent properties of the ${^{3}\text{H}}_{4}(0)\ensuremath{\rightarrow}{^{1}\text{D}}_{2}(0)$ transition of Pr3+{\text{Pr}}^{3+}Pr3+ ions in a tungstate single crystal La2(WO4)3{\text{La}}_{2}{({\text{WO}}_{4})}_{3}La2​(WO4​)3​ by hole-burning and photon-echo techniques. This work is motivated by the search of an efficient three level $\ensuremath{\Lambda}$ system in this new compound with which we could build up a quantum memory. By nonconventional hole-burning experiments, the ordering of the hyperfine splittings in the 3H4(0){^{3}\text{H}}_{4}(0)3H4​(0) ground state and in the 1D2(0){^{1}\text{D}}_{2}(0)1D2​(0) excited state is obtained. The hyperfine splittings are thus ordered: 24.6 and 14.9 MHz for the 3H4(0){^{3}\text{H}}_{4}(0)3H4​(0) level and 5.0 and 7.3 MHz for the 1D2(0){^{1}\text{D}}_{2}(0)1D2​(0) level. The relative and absolute transition strengths of individual hyperfine transitions are determined by comparing absorption strengths and by measuring the Rabi flopping frequency as the transition is coherently driven. Free induction and Raman echo decays give inhomogeneous and homogeneous hyperfine linewidths of $57\ifmmode\pm\else\textpm\fi{}2$ and $1.25\ifmmode\pm\else\textpm\fi{}0.1\text{ }\text{kHz}$, respectively.