Biomedical subjects
Publications and source records attributed to Frantisek Sanda.
The stochastic Liouville equations are employed to investigate the combined signatures of chemical exchange (two-state jump) and spectral diffusion (coupling to an overdamped Brownian oscillator) in the coherent response of an anharmonic vibration to three femtosecond infrared pulses. Simulations reproduce the main features recently observed in the OD stretch of phenol in benzene.
The two-point fluorescence intensity correlation function g(2)t and the Mandel parameter Mt are calculated for a strongly pumped dimer of two-level molecules undergoing Gaussian-Markovian frequency fluctuations. The effects of detuning and saturation are examined. All fluctuation time scale regimes are explored using a continued fraction solution of the stochastic Liouville equation for the generating function. Bunching and antibunching are observed for slow and fast fluctuations, respectively. The short-time antibunching dip in g(2) and its variation with intermolecular coupling, the exciton annihilation rate, and laser detuning are studied.
Quantum effects on multitime distributions and correlation functions of single objects, stemming from both the dynamics and repeated measurements, are calculated for a driven harmonic system using a superoperator generating functional formalism. Marked differences between multipoint observables associated with classical and quantum measurements are identified. The effects of quantum collapse and measurement resolution are discussed.
Recursive relations are derived for nonlinear optical response functions of a two-level chromophore with stochastic frequency fluctuations described by a continuous-time random walk. Stationary ensembles are constructed and signatures of anomalous relaxation in the photon echo signal are discussed for a two state jump modulation with a power law waiting time density function psi(t) approximately t(-alpha-1). Stretched exponential decay of the photon echo signal is predicted for 0<alpha<1 and power law asymptotics for 1<alpha<2.
Recursive relations are developed for computing the multipoint correlation functions of a particle undergoing a biased continuous-time random walk (CTRW) in an external potential. Two- and three-point correlation functions are calculated for waiting-time distributions with an anomalous power-law profile t(-alpha-1), 0 < alpha < 1, on intermediate time scales with a crossover to an exponential long time decay. Comparison of the CTRW with the Brownian harmonic oscillator model (Gaussian process) illustrates how higher-order correlation functions may be used to distinguish between dynamical models that have the same two-point correlation function.