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Applied Physics Letters

Laser-induced absorption line narrowing for ions in crystals: Application to the hyperfine structure of the 6011-Å Pr3+ : LaCl3 line

Christian Delsart, Nicole Pelletier-Allard, R. Pelletier

Published Oct 1, 1977• 6 citations
Publisher

Abstract

We report on the observation of absorption line narrowing in a crystal. A saturating cw single-mode dye laser leads to hole burning over a homogeneous width according to the site selection, while a second tunable cw single-mode dye laser probes the perturbed profile. Two-level and three-level resonances corresponding to the Pr3+ : LaCl3 6011-Å line hyperfine structure are obtained with very high spectral resolution (σ/Δσ≃6×107).

DOI
10.1063/1.89734

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A technique involving the laser-induced narrowing of a fluorescence line is used to obtain high-resolution spectra of Pr3+:LaCl3. The second-order effects caused by Zeeman and nuclear interactions are systematically investigated in the 3H4E2 to or from 1D2A1 transition. A non-zero perpendicular Zeeman splitting of the ground level, proportional to the square of the magnetic field, is measured and interpreted as being caused by the perturbation by the four upper Stark levels belonging to the 3H4 multiplet. The variation of the number and of the relative intensities of the hyperfine lines is demonstrated to be closely related to the angle between the external magnetic field direction and the crystal axis. It is unambiguously attributed to an angular dependence, with regard to the magnetic field direction, of the hyperfine states of the excited level. The importance of the effect, caused by a very distant perturbing level, is shown to be a result of the quasidegeneracy of the mu =0 excited level.

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Remarkably narrow optical homogeneous linewidths of the order of 1 kHz have now been observed in low temperature zero‐phonon transitions of dilute impurity ion crystals, such as Pr3+ in LaF3. Novel nonlinear optical resonance techniques have been devised for this purpose using ultrastable phase locked cw dye lasers where the measurements are performed either in the frequency domain (hole burning) or in the time domain (coherent optical transients). These studies effectively bring the Mossbauer effect into the optical region. Hence, the observed linewidths are no longer limited by inhomogeneous strain broadening (∼5 GHz) or even by static local fields due to neighboring spins (∼100 kHz). However, weak magnetic field fluctuations from local spins are readily detected. As an example, spin decoupling and line narrowing, which are well known in NMR, are observed in an optical transition of Pr3+:LaF3 at 2 K where the 19F– 19F dipolar interaction is quenched and the optical linewidth drops from 10 to 2 kHz, clearly demonstrating the spin broadening mechanism. Results will be discussed in terms of a Monte Carlo line broadening theory.

Laser Chemistry•Jan 1, 1983•5 citations
We report on the observation of absorption line narrowing in a crystal. A saturating cw single-mode dye laser leads to hole burning over a homogeneous width according to the site selection, while a second tunable cw single-mode dye laser probes the perturbed profile. Two-level and three-level resonances corresponding to the Pr3+ : LaCl3 6011-Å line hyperfine structure are obtained with very high spectral resolution (σ/Δσ≃6×107).
A technique involving the laser-induced narrowing of a fluorescence line is used to obtain high-resolution spectra of Pr3+:LaCl3. The second-order effects caused by Zeeman and nuclear interactions are systematically investigated in the 3H4E2 to or from 1D2A1 transition. A non-zero perpendicular Zeeman splitting of the ground level, proportional to the square of the magnetic field, is measured and interpreted as being caused by the perturbation by the four upper Stark levels belonging to the 3H4 multiplet. The variation of the number and of the relative intensities of the hyperfine lines is demonstrated to be closely related to the angle between the external magnetic field direction and the crystal axis. It is unambiguously attributed to an angular dependence, with regard to the magnetic field direction, of the hyperfine states of the excited level. The importance of the effect, caused by a very distant perturbing level, is shown to be a result of the quasidegeneracy of the mu =0 excited level.
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 $^{3}H_{4}\text{\ensuremath{-}}^{1}D_{2}$ 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.
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 have observed kilohertz and sub-kilohertz resonance structures in RF-optical double resonance experiments of rare-earth-doped solids, when the frequency of the RF field is scanned across the hyperfine transitions while monitoring the resonant optical absorption of a CW laser. The effect is observed only when the laser spectral width is broad compared to the hyperfine structure. The observed line widths are apparently free of the inhomogeneous widths of hyperfine levels and the line shape has peculiar double peak structure. The effect is modelled with a resonance involving three atomic levels interacting with three electromagnetic fields, two optical and one RF, in a triangular or “delta’ configuration. While the ordinary optical-RF two-field resonance is limited by spin inhomogeneous width, the simultaneous excitation of three coupled transitions leads to narrow and highly nonlinear resonance structures that are not averaged by the inhomogeneous distribution of hyperfine transition.
Abstract An experiment on the saturated absorption spectroscopy (SAS) of 87Rb-D2 line is performed using the Laguerre–Gaussian (LG) beam as structured light. The theoretical simulation of which is done by considering a four-level atom-laser coupled system. The theoretically simulated spectra fairly match with the experimentally observed spectra. The line-width narrowing behavior of both the observed hyperfine and crossover resonances in the Doppler-broadened probe absorption spectra is attributed by the spatially dependent Rabi frequency of the pump LG beam irrespective of the characteristics of the probe beam. The results also illustrated that the narrowing behavior of the line shapes of the hyperfine structure using the LG beam is universal in nature, i.e. irrespective of hyperfine or crossover transitions. This structured light-induced narrowing of line-width of the sub-Doppler hyperfine and crossover resonances can be utilized for high-precision laser frequency locking at a particular hyperfine or crossover transition. Moreover, a significant narrowing of hyperfine and crossover resonances with the variation of the orbital angular momentum (OAM) number of the LG beam shows that the generated SAS signal can be manipulated by using the OAM of the structured light as a control knob.
Remarkably narrow optical homogeneous linewidths of the order of 1 kHz have now been observed in low temperature zero‐phonon transitions of dilute impurity ion crystals, such as Pr3+ in LaF3. Novel nonlinear optical resonance techniques have been devised for this purpose using ultrastable phase locked cw dye lasers where the measurements are performed either in the frequency domain (hole burning) or in the time domain (coherent optical transients). These studies effectively bring the Mossbauer effect into the optical region. Hence, the observed linewidths are no longer limited by inhomogeneous strain broadening (∼5 GHz) or even by static local fields due to neighboring spins (∼100 kHz). However, weak magnetic field fluctuations from local spins are readily detected. As an example, spin decoupling and line narrowing, which are well known in NMR, are observed in an optical transition of Pr3+:LaF3 at 2 K where the 19F– 19F dipolar interaction is quenched and the optical linewidth drops from 10 to 2 kHz, clearly demonstrating the spin broadening mechanism. Results will be discussed in terms of a Monte Carlo line broadening theory.