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Physical Review Letters

Persistent Holes in the Spectra of Localized Vibrational Modes in Crystalline Solids

W. E. Moerner, Albert J. Sievers, Robert H. Silsbee, ANDREW R. CHRAPLYVY, D. K. Lambert

Published Aug 9, 1982• 20 citations
Publisher

Abstract

Persistent nonphotochemical spectral holes have been burnt at low laser intensity in the vibrational absorption line of a spherical-top molecule in alkali halide crystals. These observations complement earlier studies on electronic transitions in organic crystals and glasses and demonstrate that persistent hole burning is a general solid-state phenomenon.

DOI
10.1103/physrevlett.49.398

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Persistent nonphotochemical spectral holes have been burnt at low laser intensity in the vibrational absorption line of a spherical-top molecule in alkali halide crystals. These observations complement earlier studies on electronic transitions in organic crystals and glasses and demonstrate that persistent hole burning is a general solid-state phenomenon.
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.
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.
The persistent spectral hole-burning (PSHB) phenomenon was observed in semiconductor quantum dots, CdSe , CuCl , and CuBr , embedded in glass and crystal. In inhomogeneously broadened exciton absorption spectra of these dots, the narrow bleaching hole and its associated structure are made by the narrowband laser excitation and are conserved for more than several hours at 2 K after the laser irradiation. The observation of the PSHB phenomenon in these four kinds of samples shows the generality of the phenomenon in semiconductor quantum dots and requires the existence of more than one ground-state configurations of the total system consisting of quantum dots and surrounding matrix. It means that not only the size distribution but also these ground-state configurations give inhomoge-neous broadening to semiconductor quantum dots. Thermally annealing and light-induced hole-filling phenomena were observed. Hole-burning and hole-filling mechanisms are discussed. Quantum dots consisting of 103–104 atoms behave like molecules or ions in matrix to give the PSHB phenomenon.
Persistent spectral hole-burning phenomenon in CuBr quantum dots embedded in glass was observed. The spectral hole and the sideband holes were made together with the redshift of the absorption spectrum in proportion to the logarithm of the laser fluence and were preserved for more than 8 h at 2 K. They were erasable by the temperature rise or by the light exposure. Electron trapping at the surface of the dots and hole tunneling into traps in the glass host is the most probable origin of the persistent spectral hole-burning phenomenon in CuBr quantum dots.