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Effects of fabrication and annealing methods on spin relaxation and crystallite quality in rare-earth-ion doped powders studied using spectral hole burning

Thomas Lutz, Lucile Veissier, Charles W. Thiel, Philip J. T. Woodburn, R. L. Cone, Paul E. Barclay, Wolfgang Tittel

Published Sep 25, 2015• 0 citations
OpenAlex

Abstract

High-quality rare-earth-ion (REI) doped materials are a prerequisite for many applications such as quantum memories, ultra-high-resolution optical spectrum analyzers and information processing. Compared to bulk materials, REI doped powders offer low-cost fabrication and a greater range of accessible material systems. Here we show that crystal properties, such as nuclear spin lifetime, are strongly affected by mechanical treatment, and that spectral hole burning can serve as a sensitive method to characterize the quality of REI doped powders. We focus on the specific case of thulium doped Y$_2$Al$_5$O$_{12}$ (Tm:YAG). Different methods for obtaining the powders are compared and the influence of annealing on the spectroscopic quality of powders is investigated. We conclude that annealing can reverse some detrimental effects of powder fabrication and, in certain cases, the properties of the bulk material can be reached. Our results may be applicable to other impurities and other crystals, including color centres in nano-structured diamond.

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Effects of fabrication methods on spin relaxation and crystallite quality in Tm-doped Y3Al5O12 powders studied using spectral hole burning

Thomas Lutz, Lucile Veissier, Charles W. Thiel +4 more

High-quality rare-earth-ion (REI) doped materials are a prerequisite for many applications such as quantum memories, ultra-high-resolution optical spectrum analyzers and information processing. Compared to bulk materials, REI doped powders offer low-cost fabrication and a greater range of accessible material systems. Here we show that crystal properties, such as nuclear spin lifetime, are strongly affected by mechanical treatment, and that spectral hole burning can serve as a sensitive method to characterize the quality of REI doped powders. We focus on the specific case of thulium doped Y3Al5O12 (Tm:YAG). Different methods for obtaining the powders are compared and the influence of annealing on the spectroscopic quality of powders is investigated on a few examples. We conclude that annealing can reverse some detrimental effects of powder fabrication and, in certain cases, the properties of the bulk material can be reached. Our results may be applicable to other impurities and other crystals, including color centers in nano-structured diamond.

arXiv:1509.07862•Science and Technology of Advanced Materials•Mar 16, 2016•13 citations

Rare-earth-doped materials with application to optical signal processing, quantum information science, and medical imaging technology

R. L. Cone, Charles W. Thiel, Yazhou Sun +2 more

Unique spectroscopic properties of isolated rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms and enable a variety of recent applications. We design rare-earth-doped crystals, ceramics, and fibers with persistent or transient "spectral hole" recording properties for applications including high-bandwidth optical signal processing where light and our solids replace the high-bandwidth portion of the electronics; quantum cryptography and information science including the goal of storage and recall of single photons; and medical imaging technology for the 700-900 nm therapeutic window. Ease of optically manipulating rare-earth ions in solids enables capturing complex spectral information in 105 to 108 frequency bins. Combining spatial holography and spectral hole burning provides a capability for processing high-bandwidth RF and optical signals with sub-MHz spectral resolution and bandwidths of tens to hundreds of GHz for applications including range-Doppler radar and high bandwidth RF spectral analysis. Simply stated, one can think of these crystals as holographic recording media capable of distinguishing up to 108 different colors. Ultra-narrow spectral holes also serve as a vibration-insensitive sub-kHz frequency reference for laser frequency stabilization to a part in 1013 over tens of milliseconds. The unusual properties and applications of spectral hole burning of rare earth ions in optical materials are reviewed. Experimental results on the promising Tm3+:LiNbO3 material system are presented and discussed for medical imaging applications. Finally, a new application of these materials as dynamic optical filters for laser noise suppression is discussed along with experimental demonstrations and theoretical modeling of the process.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Feb 9, 2012•16 citations

Engineered impurity-doped materials for Quantum Information Processing applications - nano-structures and disordered materials

Lutz, Thomas

In this thesis we explore various ways to extend population lifetimes and coherence times of solid-state emitters. We focus on rare-earth-ion doped host materials and silicon vacancy centers in diamond, both of which are used for applications in quantum information processing and quantum communications. Enhanced lifetimes and coherence times would improve the performance of these applications. One approach investigates the possibility to suppress lattice vibrations that cause decoherence and population relaxation by engineering the phonon density of states through nano-structuring of the emitter's host material. Towards this end we study different materials and methods to obtain the desired nano-materials. Using various optical spectroscopic methods, we show that population dynamics can indeed be influenced by modifying the structure of the surrounding host material. However, we also find that the employed fabrication and synthesis methods often induce crystal damage that, in turn, degrades spectroscopic properties. As a second approach, we study rare-earth-ions in disordered host materials. Detailed spectroscopic characterizations are presented and we show with the example of an erbium doped fiber that such materials can indeed feature better properties, specifically longer population lifetimes, than the commonly used bulk crystals. We found optimal operation parameters for the erbium doped fiber which made it possible to use this medium for successful proof of principle experiments demonstrating a multimode quantum memory that operates within the convenient telecom band (around 1550 nm wavelength). Besides increasing the fundamental knowledge, the results of the studies presented in this thesis are highly relevant for the fields of quantum communications and quantum information processing since nano-structured materials are beginning to be investigated for on-chip implementations of various applications such as quantum memories and quantum gates. In addition, we found that population dynamics driven by detrimental lattice vibrations can indeed be modified in small powder materials and thus, with improved fabrication techniques, the complete suppression of lattice vibrations should be possible, benefiting a plethora of applications.

•Jan 1, 2017•0 citations

Month-long-lifetime microwave spectral holes in an erbium-doped scheelite crystal at millikelvin temperature

Zhiren Wang, Sen Lin, Marianne Le Dantec +9 more

Rare-earth-ion (REI) ensembles in crystals have remarkable optical and spin properties characterized by narrow homogeneous linewidths relative to the inhomogeneous ensemble broadening. This makes it possible to precisely tailor the ensemble spectral density and therefore the absorption profile by applying narrow-linewidth radiation to transfer population into auxiliary levels, a process broadly known as spectral hole burning (SHB). REI-doped crystals find applications in information processing, both classical (pattern recognition, filtering, spectral analysis) and quantum (photon storage), all protocols requiring suitable ensemble preparation by SHB as a first step. In Er$^{3+}$-doped materials, the longest reported hole lifetime is one minute, and longer lifetimes are desirable. Here, we report SHB and accumulated echo measurements in a scheelite crystal of CaWO$_4$ by pumping the electron spin transition of Er$^{3+}$ ions at microwave frequencies and millikelvin temperatures, with nuclear spin states of neighboring $^{183}$W atoms serving as the auxiliary levels. The lifetime of the holes and accumulated echoes rises steeply as the sample temperature is decreased, exceeding a month at 10 mK. Our results demonstrate that millikelvin temperatures can be beneficial for signal processing applications requiring long spectral hole lifetimes.

arXiv:2408.12758•Aug 22, 2024•0 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

Quadratic Zeeman spectral diffusion of thulium ion population in an yttrium gallium garnet crystal

Jacob H. Davidson, Antariksha Das, Nir Alfasi +3 more

The creation of well-understood structures using spectral hole burning is an important task in the use of technologies based on rare-earth ion-doped crystals. We apply a series of different techniques to model and improve the frequency dependent population change in the atomic level structure of thulium yttrium gallium garnet (Tm:YGG). In particular we demonstrate that, at zero applied magnetic field, numerical solutions to frequency-dependent three-level rate equations show good agreement with spectral hole-burning results. This allows us to predict spectral structures given a specific hole-burning sequence, the underpinning spectroscopic material properties, and the relevant laser parameters. This enables us to largely eliminate power-dependent hole broadening through the use of adiabatic hole-burning pulses. Although this system of rate equations shows good agreement at zero field, the addition of a magnetic field results in unexpected spectral diffusion proportional to the induced Tm ion magnetic-dipole moment and average magnetic-field strength, which, through the quadratic Zeeman effect, dominates the optical spectrum over long timescales. Our results allow optimization of the preparation process for spectral structures in a large variety of rare-earth ion-doped materials for quantum memories and other applications.

arXiv:2210.05005•Physical review. B./Physical review. B•Mar 9, 2023•4 citations
High-quality rare-earth-ion (REI) doped materials are a prerequisite for many applications such as quantum memories, ultra-high-resolution optical spectrum analyzers and information processing. Compared to bulk materials, REI doped powders offer low-cost fabrication and a greater range of accessible material systems. Here we show that crystal properties, such as nuclear spin lifetime, are strongly affected by mechanical treatment, and that spectral hole burning can serve as a sensitive method to characterize the quality of REI doped powders. We focus on the specific case of thulium doped Y2_22​Al5_55​O12_{12}12​ (Tm:YAG). Different methods for obtaining the powders are compared and the influence of annealing on the spectroscopic quality of powders is investigated. We conclude that annealing can reverse some detrimental effects of powder fabrication and, in certain cases, the properties of the bulk material can be reached. Our results may be applicable to other impurities and other crystals, including color centres in nano-structured diamond.
High-quality rare-earth-ion (REI) doped materials are a prerequisite for many applications such as quantum memories, ultra-high-resolution optical spectrum analyzers and information processing. Compared to bulk materials, REI doped powders offer low-cost fabrication and a greater range of accessible material systems. Here we show that crystal properties, such as nuclear spin lifetime, are strongly affected by mechanical treatment, and that spectral hole burning can serve as a sensitive method to characterize the quality of REI doped powders. We focus on the specific case of thulium doped Y3Al5O12 (Tm:YAG). Different methods for obtaining the powders are compared and the influence of annealing on the spectroscopic quality of powders is investigated on a few examples. We conclude that annealing can reverse some detrimental effects of powder fabrication and, in certain cases, the properties of the bulk material can be reached. Our results may be applicable to other impurities and other crystals, including color centers in nano-structured diamond.
Unique spectroscopic properties of isolated rare earth ions in solids offer optical linewidths rivaling those of trapped single atoms and enable a variety of recent applications. We design rare-earth-doped crystals, ceramics, and fibers with persistent or transient "spectral hole" recording properties for applications including high-bandwidth optical signal processing where light and our solids replace the high-bandwidth portion of the electronics; quantum cryptography and information science including the goal of storage and recall of single photons; and medical imaging technology for the 700-900 nm therapeutic window. Ease of optically manipulating rare-earth ions in solids enables capturing complex spectral information in 105 to 108 frequency bins. Combining spatial holography and spectral hole burning provides a capability for processing high-bandwidth RF and optical signals with sub-MHz spectral resolution and bandwidths of tens to hundreds of GHz for applications including range-Doppler radar and high bandwidth RF spectral analysis. Simply stated, one can think of these crystals as holographic recording media capable of distinguishing up to 108 different colors. Ultra-narrow spectral holes also serve as a vibration-insensitive sub-kHz frequency reference for laser frequency stabilization to a part in 1013 over tens of milliseconds. The unusual properties and applications of spectral hole burning of rare earth ions in optical materials are reviewed. Experimental results on the promising Tm3+:LiNbO3 material system are presented and discussed for medical imaging applications. Finally, a new application of these materials as dynamic optical filters for laser noise suppression is discussed along with experimental demonstrations and theoretical modeling of the process.
In this thesis we explore various ways to extend population lifetimes and coherence times of solid-state emitters. We focus on rare-earth-ion doped host materials and silicon vacancy centers in diamond, both of which are used for applications in quantum information processing and quantum communications. Enhanced lifetimes and coherence times would improve the performance of these applications. One approach investigates the possibility to suppress lattice vibrations that cause decoherence and population relaxation by engineering the phonon density of states through nano-structuring of the emitter's host material. Towards this end we study different materials and methods to obtain the desired nano-materials. Using various optical spectroscopic methods, we show that population dynamics can indeed be influenced by modifying the structure of the surrounding host material. However, we also find that the employed fabrication and synthesis methods often induce crystal damage that, in turn, degrades spectroscopic properties. As a second approach, we study rare-earth-ions in disordered host materials. Detailed spectroscopic characterizations are presented and we show with the example of an erbium doped fiber that such materials can indeed feature better properties, specifically longer population lifetimes, than the commonly used bulk crystals. We found optimal operation parameters for the erbium doped fiber which made it possible to use this medium for successful proof of principle experiments demonstrating a multimode quantum memory that operates within the convenient telecom band (around 1550 nm wavelength). Besides increasing the fundamental knowledge, the results of the studies presented in this thesis are highly relevant for the fields of quantum communications and quantum information processing since nano-structured materials are beginning to be investigated for on-chip implementations of various applications such as quantum memories and quantum gates. In addition, we found that population dynamics driven by detrimental lattice vibrations can indeed be modified in small powder materials and thus, with improved fabrication techniques, the complete suppression of lattice vibrations should be possible, benefiting a plethora of applications.
Rare-earth-ion (REI) ensembles in crystals have remarkable optical and spin properties characterized by narrow homogeneous linewidths relative to the inhomogeneous ensemble broadening. This makes it possible to precisely tailor the ensemble spectral density and therefore the absorption profile by applying narrow-linewidth radiation to transfer population into auxiliary levels, a process broadly known as spectral hole burning (SHB). REI-doped crystals find applications in information processing, both classical (pattern recognition, filtering, spectral analysis) and quantum (photon storage), all protocols requiring suitable ensemble preparation by SHB as a first step. In Er3+^{3+}3+-doped materials, the longest reported hole lifetime is one minute, and longer lifetimes are desirable. Here, we report SHB and accumulated echo measurements in a scheelite crystal of CaWO4_44​ by pumping the electron spin transition of Er3+^{3+}3+ ions at microwave frequencies and millikelvin temperatures, with nuclear spin states of neighboring 183^{183}183W atoms serving as the auxiliary levels. The lifetime of the holes and accumulated echoes rises steeply as the sample temperature is decreased, exceeding a month at 10 mK. Our results demonstrate that millikelvin temperatures can be beneficial for signal processing applications requiring long spectral hole lifetimes.
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,
The creation of well-understood structures using spectral hole burning is an important task in the use of technologies based on rare-earth ion-doped crystals. We apply a series of different techniques to model and improve the frequency dependent population change in the atomic level structure of thulium yttrium gallium garnet (Tm:YGG). In particular we demonstrate that, at zero applied magnetic field, numerical solutions to frequency-dependent three-level rate equations show good agreement with spectral hole-burning results. This allows us to predict spectral structures given a specific hole-burning sequence, the underpinning spectroscopic material properties, and the relevant laser parameters. This enables us to largely eliminate power-dependent hole broadening through the use of adiabatic hole-burning pulses. Although this system of rate equations shows good agreement at zero field, the addition of a magnetic field results in unexpected spectral diffusion proportional to the induced Tm ion magnetic-dipole moment and average magnetic-field strength, which, through the quadratic Zeeman effect, dominates the optical spectrum over long timescales. Our results allow optimization of the preparation process for spectral structures in a large variety of rare-earth ion-doped materials for quantum memories and other applications.