Solvent‐induced nonadiabatic transitions in iodine: An ultrafast pump–probe computational study

1996 ◽  
Vol 105 (8) ◽  
pp. 3035-3056 ◽  
Author(s):  
M. Ben‐Nun ◽  
R. D. Levine ◽  
Graham R. Fleming
Keyword(s):  
Computational Study ◽  
Pump Probe ◽  
Nonadiabatic Transitions

scholarly journals Coherent Exciton Dynamics in Ensembles of Size-Dispersed CdSe Quantum Dot Dimers Probed via Ultrafast Spectroscopy: A Quantum Computational Study

2020 ◽  
Vol 10 (4) ◽  
pp. 1328 ◽  
Author(s):  
Hugo Gattuso ◽  
Barbara Fresch ◽  
Raphael D. Levine ◽  
Françoise Remacle
Keyword(s):  
Transient Absorption ◽  
Computational Study ◽  
Laser Pulses ◽  
Transient Absorption Spectroscopy ◽  
Basis Set ◽  
Charge Migration ◽  
Pump Probe ◽  
Electronic Response ◽  
Charge Transfer Excitons ◽  
Interdot Coupling

Interdot coherent excitonic dynamics in nanometric colloidal CdSe quantum dots (QD) dimers lead to interdot charge migration and energy transfer. We show by electronic quantum dynamical simulations that the interdot coherent response to ultrashort fs laser pulses can be characterized by pump-probe transient absorption spectroscopy in spite of the inevitable inherent size dispersion of colloidal QDs. The latter, leading to a broadening of the excitonic bands, induce accidental resonances that actually increase the efficiency of the interdot coupling. The optical electronic response is computed by solving the time-dependent Schrodinger equation including the interaction with the oscillating electric field of the pulses for an ensemble of dimers that differ by their size. The excitonic Hamiltonian of each dimer is parameterized by the QD size and interdot distance, using an effective mass approximation. Local and charge transfer excitons are included in the dimer basis set. By tailoring the QD size, the excitonic bands can be tuned to overlap and thus favor interdot coupling. Computed pump-probe transient absorption maps averaged over the ensemble show that the coherence of excitons in QD dimers that lead to interdot charge migration can survive size disorder and could be observed in fs pump-probe, four-wave mixing, or covariance spectroscopy.

Pump-Probe Measurements Using Silicon Nanocrystal Waveguides

2003 ◽  
Vol 770 ◽  
Author(s):  
Nathanael Smith ◽  
Max J. Lederer ◽  
Marek Samoc ◽  
Barry Luther-Davies ◽  
Robert G. Elliman
Keyword(s):  
Probe Beam ◽  
Time Resolution ◽  
Pump Beam ◽  
Silicon Nanocrystals ◽  
Continuous Wave ◽  
Optical Gain ◽  
Optical Pump ◽  
Time Resolved ◽  
Pump Probe ◽  
Probe Measurements

AbstractOptical pump-probe measurements were performed on planar slab waveguides containing silicon nanocrystals in an attempt to measure optical gain from photo-excited silicon nanocrystals. Two experiments were performed, one with a continuous-wave probe beam and a pulsed pump beam, giving a time resolution of approximately 25 ns, and the other with a pulsed pump and probe beam, giving a time resolution of approximately 10 ps. In both cases the intensity of the probe beam was found to be attenuated by the pump beam, with the attenuation increasing monotonically with increasing pump power. Time-resolved measurements using the first experimental arrangement showed that the probe signal recovered its initial intensity on a time scale of 45-70 μs, a value comparable to the exciton lifetime in Si nanocrystals. These data are shown to be consistent with an induced absorption process such as confined carrier absorption. No evidence for optical gain was observed.

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