Quantum control of laser induced dynamics of diatomic molecular ions using shaped intense ultrafast laser pulses

The beauty of ultrafast science lies inherently in the ability to induce and image dynamics on a timescale comparable to the fastest nuclear motion, In recent years, a plethora of rich and fascinating phenomena involving the interaction of diatomic molecules with intense femtosecond laser pulse has been unveiled, Such research is motivated by the ambition to understand and optically drive chemical reactions to the highest degree of specificity, In this work, the strategy employed toward achieving this goal relies ., on the interaction of Hydrogenic ions and analytically shaped and well characterized pulses, The ability to manipulate photodissociation dynamics using the instantaneous frequency and temporal profile of pulses shaped with quadratic (ψ") and cubic (ψ’") spectral phase functions was studied, A three-dimensional (3D) momentum imaging technique was used to measure the kinetic energy release (KER) and angular distribution of the dissociation fragments, A significant enhancement in the dissociation probability of non-resonant transitions from the low lying vibrational levels using the sign and magnitude of the applied phase function as a control tool was demonstrated, Furthermore, the tractability of Hydrogenic ions means a mechanistic explanation for these observations can be theoretically determined, Investigating the behavior of ions more complex than H+2 in strong laser fields can present many theoretical and experimental challenges, Laser-induced fragmentation of CD+ was explored using the 3D momentum imaging technique in the longitudinal field imaging mode, The high mass ratio (12:2) hinders the simultaneous measurement of the two constituents, at all angles and kinetic energies, Alternatively, the recently developed longitudinal and transverse field imaging technique was used to perform a piecewise dissociation measurement, This allowed the branching ratio of the dissociation channels to be obtained, Furthermore, the fragmentation channels of CD+ were identified and studied as a function of laser intensity and wavelength,EThOS - Electronic Theses Online ServiceGBUnited Kingdo