Transform-Limited Pulses Are Not Optimal for Resonant Multiphoton Transitions
- 1 January 2001
- journal article
- research article
- Published by American Physical Society (APS) in Physical Review Letters
- Vol. 86 (1), 47-50
- https://doi.org/10.1103/physrevlett.86.47
Abstract
Maximizing nonlinear light-matter interactions is a primary motive for compressing laser pulses to achieve ultrashort transform limited pulses. Here we show how, by appropriately shaping the pulses, resonant multiphoton transitions can be enhanced significantly beyond the level achieved by maximizing the pulse's peak intensity. We demonstrate the counterintuitive nature of this effect with an experiment in a resonant two-photon absorption, in which, by selectively removing certain spectral bands, the peak intensity of the pulse is reduced by a factor of 40, yet the absorption rate is doubled. Furthermore, by suitably designing the spectral phase of the pulse, we increase the absorption rate by a factor of 7.Keywords
This publication has 20 references indexed in Scilit:
- Laser Control of Chemical ReactionsScience, 1998
- Quantum Theory of Chemical Reaction DynamicsScience, 1998
- Observation of Coherently Controlled Photocurrent in Unbiased, Bulk GaAsPhysical Review Letters, 1997
- Quantum Control of Wave Packet Evolution with Tailored Femtosecond PulsesPhysical Review Letters, 1995
- Coherent Control of Quantum Dynamics: The Dream Is AliveScience, 1993
- New Ideas for Guiding the Evolution of a Quantum SystemScience, 1992
- Femtosecond laser control of a chemical reactionNature, 1992
- Coherent pulse sequence induced control of selectivity of reactions: Exact quantum mechanical calculationsThe Journal of Chemical Physics, 1986
- Laser control of product quantum state populations in unimolecular reactionsThe Journal of Chemical Physics, 1986
- Control of selectivity of chemical reaction via control of wave packet evolutionThe Journal of Chemical Physics, 1985