Variance and width of absorption lines of single molecules in low temperature glasses

We consider the line shapes of single molecules in low temperature glasses due to dipole–dipole interaction between the molecules and other particles of the system. Motivated by computer simulations, we employ a simplified formula for the absorption lines and derive an analytic expression for the distribution of the variance of such absorption lines. The simplest version of this distribution—derived for pointlike particles without cutoff of the interaction at small distances—already accounts for the qualitative features of width histograms measured experimentally or gained by computer simulation. We further analyze the effect of the minimal approach distance between the chromophore and the perturbing particles and employ an approximate relation between the variance and the full width at half maximum of the absorption lines. We find that the main characteristics of the histogram of widths stem from the (homogeneous) distribution of interactions in space and do not reflect the distribution of the internal p...

[1]  J. Skinner,et al.  Theory of photon echoes and hole burning in low temperature glasses: How good are the standard approximations? , 1997 .

[2]  J. Skinner,et al.  THEORY OF SINGLE-MOLECULE OPTICAL LINE-SHAPE DISTRIBUTIONS IN LOW-TEMPERATURE GLASSES , 1997 .

[3]  H. Nakatsuka,et al.  Inhomogeneous and single molecule line broadening of terrylene in a series of crystalline n-alkanes , 1997 .

[4]  J. Skinner,et al.  Spectral Dynamics of Individual Molecules in Glasses and Crystals , 1996 .

[5]  W. Moerner,et al.  Structure and Dynamics in Solids As Probed by Optical Spectroscopy , 1996 .

[6]  C. Bräuchle,et al.  Single molecule spectroscopy in solids: Quantum optics and spectral dynamics , 1996 .

[7]  R. Silbey,et al.  Time and temperature dependence of optical linewidths in glasses at low temperature: Spectral diffusion , 1996 .

[8]  James H. Jett,et al.  Single-Molecule Fluorescence Analysis in Solution , 1996 .

[9]  D. Cahill,et al.  Elastic properties of several amorphous solids and disordered crystals below 100 K , 1996 .

[10]  L. Kador Recent Results of Single‐Molecule Spectroscopy in Solids , 1995 .

[11]  J. Skinner,et al.  Spectral diffusion of individual pentacene molecules in P‐terphenyl crystal: Stochastic theoretical model and analysis of experimental data , 1995 .

[12]  M. Orrit,et al.  Single molecule lines and spectral hole burning of terrylene in different matrices , 1994 .

[13]  J. Skinner,et al.  Spectroscopy of a chromophore coupled to a lattice of dynamic two‐level systems. I. Absorption line shape , 1994 .

[14]  A. Renn,et al.  Single molecule spectroscopy : Stark-, pressure-, polarization-effects and fluorescence lifetime measurements , 1994 .

[15]  W. Moerner Fundamentals of single-molecule spectroscopy in solids , 1994 .

[16]  Joseph Klafter,et al.  Spectral random walk of a single molecule , 1994 .

[17]  R. Silbey,et al.  Low-temperature dynamics in glasses and the stochastic sudden-jump model , 1994 .

[18]  M. Orrit,et al.  Spectral diffusion and individual two-level systems probed by fluorescence of single terrylene molecules in a polyethylene matrix , 1993 .

[19]  M. Orrit,et al.  High-resolution spectroscopy of organic molecules in solids: from fluorescence line narrowing and hole burning to single molecule spectroscopy , 1993 .

[20]  Heuer,et al.  Microscopic description of tunneling systems in a structural model glass. , 1993, Physical review letters.

[21]  Thomas Basché,et al.  Optical Spectroscopy Of Single Impurity Molecules In Solids , 1993, Laser Applications to Chemical Analysis.

[22]  M. Orrit,et al.  Single pentacene molecules detected by fluorescence excitation in a p-terphenyl crystal. , 1990, Physical review letters.

[23]  R. Silbey,et al.  Hole‐Burning Spectroscopy of Glasses , 1990 .

[24]  W. Moerner,et al.  Optical detection and spectroscopy of single molecules in a solid. , 1989, Physical review letters.

[25]  J. Skinner,et al.  Proton transfer in benzoic acid crystals: A chemical spin–boson problem. Theoretical analysis of nuclear magnetic resonance, neutron scattering, and optical experiments , 1988 .

[26]  M. Meissner,et al.  How universal are the low temperature acoustic properties of glasses? , 1988 .

[27]  A. C. Anderson,et al.  Amorphous Solids: Low-Temperature Properties , 1981 .

[28]  B. Halperin,et al.  Spectral diffusion, phonon echoes, and saturation recovery in glasses at low temperatures , 1977 .

[29]  W. A. Phillips,et al.  Tunneling states in amorphous solids , 1972 .

[30]  Philip W. Anderson,et al.  Spectral Diffusion Decay in Spin Resonance Experiments , 1962 .

[31]  Ryogo Kubo,et al.  Note on the Stochastic Theory of Resonance Absorption , 1954 .

[32]  P. W. Anderson,et al.  A Mathematical Model for the Narrowing of Spectral Lines by Exchange or Motion , 1954 .

[33]  Thomas Basché,et al.  Single-molecule optical detection, imaging and spectroscopy , 1997 .

[34]  Roger M. Macfarlane,et al.  Homogeneous line broadening of optical transitions of ions and molecules in glasses , 1987 .

[35]  P. Anderson,et al.  Anomalous low-temperature thermal properties of glasses and spin glasses , 1972 .

[36]  Am Stoneham,et al.  Shapes of Inhomogeneously Broadened Resonance Lines in Solids (Invited Talk) , 1969 .