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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Hole-Burning and External Field Effects: Principles, Recent Results and New Systems (Superfine Films)

Roman I. Personov

Published Jan 1, 1991• 0 citations
Publisher

Abstract

The possibility to investigate the influence of external electric and magnetic fields on complex molecules in amorphous solids is essentially limited by a large width of their spectral bands (Δν=102-103 cm−1 even at liquid helium temperature). Hole-burning opens up new excellent opportunities for using the Stark and Zeeman effects in spectroscopy of molecules and solids and their different applications [1]. Owing to the small hole width (Δν=10−1-10−2 cm−1 at 2-5 K) the sensitivity of measurements increases by several orders of magnitude.

DOI
10.1364/pshb.1991.thd2

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The possibility to investigate the influence of external electric and magnetic fields on complex molecules in amorphous solids is essentially limited by a large width of their spectral bands (Δν=102-103 cm−1 even at liquid helium temperature). Hole-burning opens up new excellent opportunities for using the Stark and Zeeman effects in spectroscopy of molecules and solids and their different applications [1]. Owing to the small hole width (Δν=10−1-10−2 cm−1 at 2-5 K) the sensitivity of measurements increases by several orders of magnitude.
Persistent spectral hole-burning (PSHB) is a versatile tool to study Stark effect in solids where impurity spectra is strongly inhomogeneously broadened. At liquid helium temperatures impurity homogeneous zero-phonon line widths are small (γhom~10–2-10–4cm–1) and narrow holes can be burnt in the inhomogeneous distribution by illumination with narrow band laser(Δνlaser < γhom) U1- Stark effect alters the shape of narrow spectral holes depending on the Stark shift (splitting) of impurity energy levels, orientation of the impurities, strength and orientation of the electric field, as well as on the properties of the matrix [2].
The dependence of spectral holes of dye molecules in amorphous solids on the following parameters has been calculated: the electric field strength, the angles between the hole-burning and probing laser light fields and the external electric field, the electric dipole moment difference Δμm between the excited and ground state of the guest molecule, the contribution Δμ* of the host matrix to the electric dipole moment difference, and the angle γ, between Δμm and the transition dipole moment μge. When the molecular dipole moment difference Δμm dominates the spectral hole broadens or splits into two holes by the application of the electric field, depending on the angle γ and the directions of the laser light fields and the external field. With increasing values of the host-induced electric dipole moment difference Δμ* the spectral hole shape in the electric field changes significantly if appropriate directions of the light fields and the external field are chosen. The material parameters γ, Δμm, and Δμ* can be determined unequivocally by comparing the calculated holes both in the frequency dimension and the electric field dimension with experimental results.
The photoselection of impurity molecules caused by spectral hole burning produces a specific spectral angular distribution of the molecules in low-temperature amorphous matrices: All the molecules, whose zero-phonon absorption lines lie within a selected narrow spectral interval, have a specified distribution of their orientations relative to the laboratory coordinate system. In this paper, the possibility of application of known methods of hole burning in this spectral interval is studied and the outlook for combination of these methods with preliminary photoselection is demonstrated by the example of the Stark effect.
At very low temperatures, the spread in the different environments of matrix embedded dye molecules results in an inhomogeneously broadened S1 ← S0 band. Spectroscopic techniques based on the appearence of optical zero phonon lines, such as fluorescence line narrowing, spectral hole-burning, and single molecule spectroscopy provide an experimental resolution limited by the homogeneous linewidth. From the investigation of the homogeneous line width as a function of different parameters (time, temperature) information on the guest host interactions responsible for the observed linewidth is obtained. Spectrally narrow features are extremely sensitive probes for external perturbations, such as electric fields, magnetic fields, or hydrostatic pressure.
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.