Direct spectroscopic observation of quantum jumps of a single molecule

Photon Antibunching and Collective Effects in the Fluorescence of Single Bichromophoric Molecules

“…In particular, the temporal properties of photon emission from single molecules were the subject of numerous studies. Photon antibunching [2,3], stochastic fluorescence off times due to excursions of the molecule to the triplet manifold [4], and quantum jumps [5] have been reported. Recently, SMS has yielded novel insights into the electronic interactions in multichromophoric assemblies such as light-harvesting pigments [6], conjugated polymers [7], donor-acceptor substituted biopolymers [8], and dendrimers carrying a variable number of chromophores [9].…”

Mode-coupling theory for multiple-point and multiple-time correlation functions

“…These new approaches have the potential to provide extremely useful information on how collective motions of the system are correlated to specific statistical features of the dynamics such as the distribution of time scales of fluctuations, the length scale and size-distribution of solid-like clusters, and cage structural relaxation rates. One approach to probe the nature of dynamical heterogeneities is based on single molecule spectroscopy techniques [13][14][15][16] in which the environment of a one molecule is tracked over a period of time. The technique allows the information of not only the distribution of heterogeneous environments but also the explicit reorganization times which are present in the system, since the individual measurements are not statistically averaged.…”

Blinking molecules: Determination of photophysical parameters from the intensity correlation function

“…1(a)). These vibrational states have a life time of about 10 −12 s [5]. On the other hand, a transition from |3 to the vibrational states of |1 occur on a time scale of 10 −8 s and from |3 to the triplet state |2 about every 10 −3 s. Therefore these transitions can be described by effective electronic Einstein coefficients A 31 , A The extremely fast relaxation of the vibrational levels leads to an effective four-level system with two metastable states, |2 (1) and |2 (2) , and effective Einstein coefficients…”

“…Due to the interaction between the magnetic moments of the electron spins the metastable triplet state of terrylene splits into two metastable sub-levels with different population and depopulation rates (zero-field splitting) [5]. Each electronic level is characterized by a host of vibrational degrees of freedom (cf.…”

“…In the presence of metastable triplet levels the molecule can exhibit light and dark periods in its fluorescence ("blinking") [5,6], just as ions in the V or Λ configuration [7,8,9,10,11,12,13,14]. Spectroscopy of single molecules is of fundamental importance both for basic quantum mechanical aspects like antibunching, quantum jumps or the dynamical Stark effect [5,15,16], as well as for applications in chemical and biophysics, cf. e.g.…”