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Final Report

Laser Hole Burning Spectroscopy: A High Resolution Probe of Molecular Environments.

R. M. Macfarlane, Robert M. Shelby

Published Jun 1, 1981• 0 citations
OpenAlex

Abstract

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.

Related papers

Hole-Burning of Rare Earth Ions with kHz Resolution

Neil B. Manson, Matthew J. Sellars, Peter Fisk +1 more

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].

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations

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 +2 more

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.

arXiv:cond-mat/0408515•Physical Review B•Dec 30, 2004•201 citations

New Host Lattices for Optical Hole Burning: Materials of Low Nuclear Spin Densities

A. Caprez, P. Meyer, J. Hulliger

Optical hole burning (OHB) on rare earth ions has so far been performed mainly on single crystals which have been developed as a laser host material. However, an essential drawback of most of these lattices is the high nuclear spin density s of the constituting ions, giving rise to a broadening of the homogeneous width of the absorption of individual rare earth ions [1]. As a result of a limited number of elements providing a high natural abundance of isotopes with zero nuclear spin I or small nuclear momentum µ, there are not too many existing or possible new host lattices to work on. Further restrictions arise in the case of heterogeneous doping as well as from a given site symmetry.

Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)•Jan 1, 1996•0 citations

Observation of persistent spectral hole–burning in semiconductor nanocrystals

Yasuaki Masumoto, Lev Zimin, Kazuhiko Naoe

So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations

Spectral Hole Burning for Ultra-stable Lasers

Shuo Zhang, Nemanja Lučić, Nicolas Galland +6 more

Spectral hole burning in rare earth doped crystal can provide frequency references based on the optical transition of the dopant ions [1] . The narrow spectral patterns can be used to improve laser frequency stabilization [2] , [3] and provide a new generation of ultra-stable lasers with lower thermal noise benefiting from the cryogenic environment and better quality factor of the crystal than the amorphous glass typically used in the Fabry-Perot cavity. We utilize Europium doped yttrium silicon oxide (Eu:YSO) in our experiments, which allow realization of long lived (hours or more depending on temperature) narrow spectral holes ( kHz or less) well suited for high precision experiment applications. We will describe our novel double-heterodyne detection method [4] , used to decrease the detection noise, as well as experiments assessing quantitatively the sensitivity of the spectral pattern to crystal deformation [5] , [6] , application of electric field [7] and temperature fluctuations. We currently demonstrate a state-of-the-art laser frequency stability at 1.7 × 10 − 15 at 1s [4] , limited by the latter effect, for which improvement strategies have been demonstrated elsewhere [2] and which we are currently implementing. The other effects which we have quantitatively studied are compatible with a few 10 − 18 frequency stability at 1s time scale. This work is particularly promising in the context of optical frequency lattice clocks, for which the ultra-stable laser used for probing the clock transition is a strong limiting factor of the frequency stability.

Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)•Jun 21, 2021•1 citation

The role of divalent ions in persistent hole-burning mechanism in Y2O3:Pr3+ crystals

Tsuyoshi Okuno, Kōichiro Tanaka, Tohru Suemoto

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.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations
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.
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].
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.
Optical hole burning (OHB) on rare earth ions has so far been performed mainly on single crystals which have been developed as a laser host material. However, an essential drawback of most of these lattices is the high nuclear spin density s of the constituting ions, giving rise to a broadening of the homogeneous width of the absorption of individual rare earth ions [1]. As a result of a limited number of elements providing a high natural abundance of isotopes with zero nuclear spin I or small nuclear momentum µ, there are not too many existing or possible new host lattices to work on. Further restrictions arise in the case of heterogeneous doping as well as from a given site symmetry.
So far, persistent spectral hole-burning (PSHB) phenomenon has been observed in a number of materials. They are molecules in glasses, crystals and polymers, color centers in alkali halide crystals, and rare earth and transition metal ions in glasses and crystals. They are molecular or ionic guests embedded in glass, crystal or polymer hosts. Basic requirements for the PSHB are summarized as follows: (1) The optical absorption of guests embedded in hosts must be broadened inhomogeneously. (2) There must exist more than one ground state configurations of the total system consisting of guests and hosts. (3) The relaxation among the ground states must be slower than the decay rate of any excited state. In fact, this set of requirements is satisfied in many kinds of molecular or ionic guests in hosts, such as glasses, crystals and polymers, at low temperatures. We can naturally understand that guests consisting of small number of atoms are greatly influenced by the surrounding hosts and that the energy levels of the guests are inhomogeneously broadened.
Spectral hole burning in rare earth doped crystal can provide frequency references based on the optical transition of the dopant ions [1] . The narrow spectral patterns can be used to improve laser frequency stabilization [2] , [3] and provide a new generation of ultra-stable lasers with lower thermal noise benefiting from the cryogenic environment and better quality factor of the crystal than the amorphous glass typically used in the Fabry-Perot cavity. We utilize Europium doped yttrium silicon oxide (Eu:YSO) in our experiments, which allow realization of long lived (hours or more depending on temperature) narrow spectral holes ( kHz or less) well suited for high precision experiment applications. We will describe our novel double-heterodyne detection method [4] , used to decrease the detection noise, as well as experiments assessing quantitatively the sensitivity of the spectral pattern to crystal deformation [5] , [6] , application of electric field [7] and temperature fluctuations. We currently demonstrate a state-of-the-art laser frequency stability at 1.7 × 10 − 15 at 1s [4] , limited by the latter effect, for which improvement strategies have been demonstrated elsewhere [2] and which we are currently implementing. The other effects which we have quantitatively studied are compatible with a few 10 − 18 frequency stability at 1s time scale. This work is particularly promising in the context of optical frequency lattice clocks, for which the ultra-stable laser used for probing the clock transition is a strong limiting factor of the frequency stability.
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.