Lineshape theory and photon counting statistics for blinking quantum dots: a Levy walk process

被引:107
作者
Jung, Y [1 ]
Barkai, E [1 ]
Silbey, RJ [1 ]
机构
[1] MIT, Dept Chem, Cambridge, MA 02139 USA
基金
美国国家科学基金会;
关键词
D O I
10.1016/S0301-0104(02)00547-5
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
Motivated by recent experimental observations of power-law statistics both in spectral diffusion process and fluorescence intermittency of individual semiconductor nanocrystals (quantum dots), we consider two different but related problems: (a) a stochastic lineshape theory for the Kubo-Anderson oscillator whose frequency modulation follows power-law statistics and (b) photon counting statistics of quantum dots whose intensity fluctuation is characterized by power-law kinetics. In the first problem, we derive an analytical expression for the lineshape formula and find rich type of behaviors when compared with the standard theory. For example, new type of resonances and narrowing behavior have been found. We show that the lineshape is extremely sensitive to the way the system is prepared at time t = 0 and discuss the problem of stationarity. In the second problem, we use semiclassical photon counting statistics to characterize the fluctuation of the photon counts emitted from quantum dots. We show that the photon counting statistics problem can be mapped onto a Levy walk process. We find unusually large fluctuations in the photon counts that have not been encountered previously. In particular, we show that Mandel's Q parameter may increase in time even in the long time limit. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:181 / 194
页数:14
相关论文
共 61 条
  • [1] FLUORESCENCE SPECTROSCOPY AND SPECTRAL DIFFUSION OF SINGLE IMPURITY MOLECULES IN A CRYSTAL
    AMBROSE, WP
    MOERNER, WE
    [J]. NATURE, 1991, 349 (6306) : 225 - 227
  • [2] DETECTION AND SPECTROSCOPY OF SINGLE PENTACENE MOLECULES IN A PARA-TERPHENYL CRYSTAL BY MEANS OF FLUORESCENCE EXCITATION
    AMBROSE, WP
    BASCHE, T
    MOERNER, WE
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1991, 95 (10) : 7150 - 7163
  • [4] Exciton dynamics probed by single molecule spectroscopy
    Bach, H
    Renn, A
    Zumofen, G
    Wild, UP
    [J]. PHYSICAL REVIEW LETTERS, 1999, 82 (10) : 2195 - 2198
  • [5] Statistics of persistent events:: An exactly soluble model
    Baldassarri, A
    Bouchaud, JP
    Dornic, I
    Godrèche, C
    [J]. PHYSICAL REVIEW E, 1999, 59 (01): : R20 - R23
  • [6] Evidence for a thermal contribution to emission intermittency in single CdSe/CdS core/shell nanocrystals
    Banin, U
    Bruchez, M
    Alivisatos, AP
    Ha, T
    Weiss, S
    Chemla, DS
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1999, 110 (02) : 1195 - 1201
  • [7] One-dimensional stochastic Levy-Lorentz gas
    Barkai, E
    Fleurov, V
    Klafter, J
    [J]. PHYSICAL REVIEW E, 2000, 61 (02) : 1164 - 1169
  • [8] Levy distribution of single molecule line shape cumulants in glasses
    Barkai, E
    Silbey, R
    Zumofen, G
    [J]. PHYSICAL REVIEW LETTERS, 2000, 84 (23) : 5339 - 5342
  • [9] Time-dependent fluctuations in single molecule spectroscopy: A generalized Wiener-Khintchine approach
    Barkai, E
    Jung, Y
    Silbey, R
    [J]. PHYSICAL REVIEW LETTERS, 2001, 87 (20) : 207403 - 1
  • [10] DIRECT SPECTROSCOPIC OBSERVATION OF QUANTUM JUMPS OF A SINGLE-MOLECULE
    BASCHE, T
    KUMMER, S
    BRAUCHLE, C
    [J]. NATURE, 1995, 373 (6510) : 132 - 134