Disentangling multidimensional femtosecond spectra of excitons by pulse shaping with coherent control.
Sequences of carefully timed and shaped optical pulses provide femtosecond snapshots of molecular structure as well as electronic and vibrational dynamical processes, in analogy with multidimensional NMR. We apply a genetic learning algorithm towards the design of pulse sequences which simplify the multidimensional signals by controlling the relative intensities of various peaks. Numerical simulations demonstrate how poorly resolved weak features may be amplified and observed by using optimized optical pulses, specifically shaped to achieve a desired spectroscopic target.
Abramavicius
Darius
D
Department of Chemistry, University of California, Irvine, California 92697, USA.
Mukamel
Shaul
S
D000465:Algorithms; D002627:Chemistry, Physical / Q000379:methods*; D003627:Data Interpretation, Statistical; D005828:Genetics, Population; D009682:Magnetic Resonance Spectroscopy / Q000379:methods*; D008957:Models, Genetic; D015233:Models, Statistical; D008962:Models, Theoretical; D009154:Mutation; D013997:Time Factors