We present a case study on Eu 3+ -doped Y 2 O 3 transparent ceramics in which high-resolution laser spectroscopy is used as a material characterization tool. By comparing the results from coherent and incoherent optical spectroscopy with other characterization methods, we show that optical techniques can deliver supplementary information about the local environment of the activator ions in materials. Thus, high-resolution spectroscopy may be of interest for the investigation of a wider range of rare earth doped optical materials beyond materials studied for quantum information technology. The refinement of optical spectroscopy for the study of narrow optical transitions in rare earth ion single crystals has demonstrated that these techniques are extremely sensitive tools for probing the local environment of the rare earth ion. These techniques, such as photon echo experiments, have been important in developing materials for quantum information technology and spectral filtering applications. Here, we apply these techniques to transparent ceramic samples and compare the results with information gained from conventional material characterization techniques. Our present study demonstrates the high sensitivity of laser spectroscopic methods to microstructural strain and the presence of defects. In particular, the sensitivity is sufficient to detect small changes introduced by different thermal treatments in nominally equivalent materials. The results of our work show that it is possible to relate high-resolution optical measurements to defects and microstructural strain.
We present a case study on Eu 3+ -doped Y 2 O 3 transparent ceramics in which high-resolution laser spectroscopy is used as a material characterization tool. By comparing the results from coherent and incoherent optical spectroscopy with other characterization methods, we show that optical techniques can deliver supplementary information about the local environment of the activator ions in materials. Thus, high-resolution spectroscopy may be of interest for the investigation of a wider range of rare earth doped optical materials beyond materials studied for quantum information technology. The refinement of optical spectroscopy for the study of narrow optical transitions in rare earth ion single crystals has demonstrated that these techniques are extremely sensitive tools for probing the local environment of the rare earth ion. These techniques, such as photon echo experiments, have been important in developing materials for quantum information technology and spectral filtering applications. Here, we apply these techniques to transparent ceramic samples and compare the results with information gained from conventional material characterization techniques. Our present study demonstrates the high sensitivity of laser spectroscopic methods to microstructural strain and the presence of defects. In particular, the sensitivity is sufficient to detect small changes introduced by different thermal treatments in nominally equivalent materials. The results of our work show that it is possible to relate high-resolution optical measurements to defects and microstructural strain.
Inhomogeneous and homogeneous linewidth are reported in a Eu3+ doped transparent Y2O3 ceramic for the 7F0-5D0 transition, using high-resolution coherent spectroscopy. The 8.7-GHz inhomogeneous linewidth is close to that of single crystals, as is the 59-kHz homogeneous linewidth at 3 K (T2= 5.4 $\ensuremath{\mu}$s). The homogeneous linewidth exhibits a temperature dependence that is typical of a crystalline environment, and additional dephasing observed in the ceramic is attributed to magnetic impurities or defects introduced during the synthesis process. The absence of Eu3+segregation at the grain boundaries, evidenced through confocal microfluorescence, further indicates that the majority of Eu3+ions in the ceramic experience an environment comparable to a single crystal. The obtained results suggest that ceramic materials can be competitive with single crystals for applications in quantum information and spectral hole burning devices, beyond their current applications in lasers and scintillators.
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,
We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of Eu3+ dopants in a series of Y2O3 ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and Zr4+ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.
Homogeneous linewidths below 10 kHz are reported for the first time in high-quality Eu3+ doped Y 2O3 transparent ceramics. This result is obtained on the 7F0→5D0 transition in Eu3+ doped Y 2O3 ceramics and corresponds to an improvement of nearly one order of magnitude compared to previously reported values in transparent ceramics. Furthermore, we observed spectral hole lifetimes of ∼15 min that are long enough to enable efficient optical pumping of the nuclear hyperfine levels. Additionally, different Eu3+ concentrations (up to 1.0%) were studied, resulting in an increase of up to a factor of three in the peak absorption coefficient. These results suggest that transparent ceramics can be useful in applications where narrow and deep spectral holes can be burned into highly absorbing lines, such as quantum information processing and spectral filtering.
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.
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.