4fn ⇒ 4fn transitions of trivalent rare earth ions doped in crystals frequently give sharp spectral lines. The transitions associated with the higher levels of a multiplet can be relatively sharp, 10-1000 GHz, where the width is determined by the decay rate of the levels by spontaneous phonon emission to lower levels. The transitions and their linewidth can be determined using conventional absorption or excitation techniques. On the other hand the transitions associated with the meta-stable lower levels typically give much sharper features with linewidths of 1 - 100 GHz and the widths are determined by the inhomogeneities of the crystal field. These inhomogeneous linewdths can be obtained by conventional spectroscopic techniques but the homogeneous linewidth requires more innovative techniques such as optical holeburning or photon echoes. The time domain photon echo measurements do not requiring a high resolution source and have frequently been used to establish that the homogeneous linewidth of such transitions. The lines can be very narrow down to the kHz regime [1,2]. Should complimentary measurements be attempted in the frequency domain utilising holeburning a special frequency stabilised lasers is required and one has been developed in association with the current work [3].
4fn ⇒ 4fn transitions of trivalent rare earth ions doped in crystals frequently give sharp spectral lines. The transitions associated with the higher levels of a multiplet can be relatively sharp, 10-1000 GHz, where the width is determined by the decay rate of the levels by spontaneous phonon emission to lower levels. The transitions and their linewidth can be determined using conventional absorption or excitation techniques. On the other hand the transitions associated with the meta-stable lower levels typically give much sharper features with linewidths of 1 - 100 GHz and the widths are determined by the inhomogeneities of the crystal field. These inhomogeneous linewdths can be obtained by conventional spectroscopic techniques but the homogeneous linewidth requires more innovative techniques such as optical holeburning or photon echoes. The time domain photon echo measurements do not requiring a high resolution source and have frequently been used to establish that the homogeneous linewidth of such transitions. The lines can be very narrow down to the kHz regime [1,2]. Should complimentary measurements be attempted in the frequency domain utilising holeburning a special frequency stabilised lasers is required and one has been developed in association with the current work [3].
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,
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.
We propose a novel, wideband spectrum analyzer based on spectral hole burning (SHB) technology. SHB crystals contain rare earth ions doped into a host lattice, and are cooled to cryogenic temperatures to allow sub-MHz hole burning linewidths. The signal spectrum is recorded in an SHB crystal by illuminating the crystal with an optical beam modulated by the RF signal of interest. The signal's spectral components excite those rare earth ions whose resonance frequencies coincide with the spectral component frequencies, engraving the RF spectrum into the crystal's absorption profile. Probing this altered absorption profile with a low power, chirped laser while measuring the transmitted intensity results in a time-domain readout of the accumulated RF signal spectrum. The resolution of the spectrum analyzer is limited only by the homogeneous linewidth of the rare earth ions (< 1 MHz when the SHB crystal is cooled to cryogenic temperatures). The spectrum analyzer bandwidth is limited by the inhomogeneous linewidth and by the electro-optic modulator bandwidth, both of which can be > 20 GHz.
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+ in Y2SiO5. Information on the hyperfine structure and relative transition strengths of the $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ hyperfine transitions in Pr3+:Y2SiO5 has been obtained from frequency-resolved absorption measurements, in combination with coherent and incoherent driving of the transitions.
We demonstrate a 20 GHz spectrum analyzer with 1 MHz resolution and >40 dB dynamic range using spectral-hole-burning (SHB) crystals, which are cryogenically cooled crystal hosts lightly doped with rare-earth ions. We modulate a rf signal onto an optical carrier using an electro-optic intensity modulator to produce a signal beam modulated with upper and lower rf sidebands. Illuminating SHB crystals with modulated beams excites only those ions resonant with corresponding modulation frequencies, leaving holes in the crystal's absorption profile that mimic the modulation power spectrum and persist for up to 10 ms. We determine the spectral hole locations by probing the crystal with a chirped laser and detecting the transmitted intensity. The transmitted intensity is a blurred-out copy of the power spectrum of the original illumination as mapped into a time-varying signal. Scaling the time series associated with the transmitted intensity by the instantaneous chirp rate yields the modulated beam's rf power spectrum. The homogeneous linewidth of the rare-earth ions, which can be <100 kHz at cryogenic temperatures, limits the fundamental spectral resolution, while the medium's inhomogeneous linewidth, which can be >20 GHz, determines the spectral bandwidth.
We report the optical study of europium nitrate hexahydrate crystals Eu(NO 3 ) ⋅ 3 6H 2 O and their deuterated version Eu(NO 3 ) ⋅ 3 6D 2 O conducted at 50 mK. The crystals show sub-GHz inhomogeneous linewidths for the F 0 7 ↔ 5 D 0 transition and optical coherence times up to 136 μs for the non-deuterated crystal and 750 μs for the deuterated one. In addition, using the spectral hole burning technique, the hyperfine splittings in the absence of an external field have been estimated for the ground and optical levels. These results suggest that rare-earth nitrate crystals could represent a promising class of materials for quantum information applications as well as for fundamental physics experiments requiring narrow optical transitions and good coherence properties. • Deuterated and non-deuterated europium nitrate crystals were grown using the slow-cooling method. • Optical coherence times up to 0.75 ms were measured at 50 mK using the photon echo technique. • Sub-GHz optical inhomogeneous linewidths were observed. • The hyperfine splittings of the ground and optical states were assessed via spectral hole burning.