Distribution of variances of single molecules in a disordered lattice

被引:5
作者
Barkai, E
Silbey, R [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
[2] MIT, Ctr Mat Sci & Engn, Cambridge, MA 02139 USA
关键词
D O I
10.1021/jp9924880
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Single molecule spectroscopy in disordered lattice is investigated from a theoretical point of view. We consider energy fluctuations of the molecule due to dipolar interactions with two level system (TLS) defects distributed randomly on a three-dimensional cubic lattice. Each independent TLS is randomly nipping so the energy of the molecule is time dependent. We investigate the probability distribution g(W) of the variance of the energy fluctuations. The exact solution, found for finite systems, exhibits peaks, peaks within peaks, etc., corresponding to interaction with nearest neighbors, next-nearest neighbors, etc. For an infinite crystal at high defect density, the distribution of W is shown to depend strongly on the interaction with nearest neighbors and hence on lattice symmetry. At low defect density, g(W) exhibits several peaks separated by large gaps in which g(W) similar to 0. We explain these peaks in terms of contributions from single defects located on discrete distances from the molecule. For the continuum version of our model, g(W) is a Levy stable nonsymmetrical probability density function, decaying according to g(W) similar to W-3/2. We discuss the relation between the continuum and lattice models.
引用
收藏
页码:342 / 353
页数:12
相关论文
共 37 条
[1]  
Abramovitz M., 1970, HDB MATH FUNCTIONS
[2]   DETECTION AND SPECTROSCOPY OF SINGLE PENTACENE MOLECULES IN A PARA-TERPHENYL CRYSTAL BY MEANS OF FLUORESCENCE EXCITATION [J].
AMBROSE, WP ;
BASCHE, T ;
MOERNER, WE .
JOURNAL OF CHEMICAL PHYSICS, 1991, 95 (10) :7150-7163
[3]  
BACHE T, 1996, SINGLE MOL OPTICAL D
[4]   Distribution of single-molecule line widths [J].
Barkai, E ;
Silbey, R .
CHEMICAL PHYSICS LETTERS, 1999, 310 (3-4) :287-295
[5]   An investigation of the effects of two level system coupling on single molecule lineshapes in low temperature glasses [J].
Brown, FLH ;
Silbey, RJ .
JOURNAL OF CHEMICAL PHYSICS, 1998, 108 (17) :7434-7450
[6]  
Feller W., 1970, INTRO PROBABILITY TH, V2
[7]   SPECTRAL DIFFUSION AND INDIVIDUAL 2-LEVEL SYSTEMS PROBED BY FLUORESCENCE OF SINGLE TERRYLENE MOLECULES IN A POLYETHYLENE MATRIX [J].
FLEURY, L ;
ZUMBUSCH, A ;
ORRIT, M ;
BROWN, R ;
BERNARD, J .
JOURNAL OF LUMINESCENCE, 1993, 56 (1-6) :15-28
[8]  
FLEURY L, 1995, THESIS U BORDEAUX BR
[9]   STABLE DISTRIBUTION ANALYSIS OF INTERNAL FIELD DISTRIBUTION IN AU(FE) SPIN-GLASS SYSTEM .1. VARIATION OF THE DISTRIBUTION WITH CONCENTRATION [J].
FURUKAWA, Y ;
NAKAI, Y ;
KUNITOMI, N .
JOURNAL OF THE PHYSICAL SOCIETY OF JAPAN, 1993, 62 (01) :306-313
[10]   Single molecule spectral trajectories in low-temperature glasses [J].
Geva, E ;
Skinner, JL .
CHEMICAL PHYSICS LETTERS, 1998, 287 (1-2) :125-130