超快光学-第16章-相干控制.pptVIP

Coherent Control Coherent Control attempts to control a chemical reaction with light, usually a cleverly shaped ultrashort laser pulse. Why it’s hard: IVR. Using shaped pulses and  an iterative approach. Coherent Control Chemical reactions proceed in a manner determined by the molecular Hamiltonian. What if we’d like to change this and make different products? Bring in a light frequency to excite a bond we’d like to break. But it’s not so easy! There’s a lot more to it. A long-held dream of chemists. It’s now coming true. Shaped ultrashort pulses are the key. Intramolecular Vibrational Redistribution Coherent control: Using shaped ultrashort pulses to control the reaction The physics of coherent control Trying to do the theory for coherent control Coherent control of a simple gas phase reaction Coherent control is here! Successful closed-loop coherent control experiments in physics and chemistry * Wave-function Potential C = catalyst Conventional methods of chemical control Much can be done, but not everything we’d like. Coherent control slides mostly thanks to Gustav Gerber, University of Wurzberg, Germany Margaret Murnane and Henry Kapteyn, JILA Robert Levis, Temple University IVR occurs on a few-fs time scale, so long pulses excite entire molecule, and the weakest bond breaks, no matter which bond was excited. Excite one bond A few fs later, however, the entire molecule is vibrating. The bond vibrates Single-parameter control Surprisingly, these simple methods often work, but they are not general. Can an ultrashort pulse cause a molecule to vibrate in such a way as to break the bond of our choice? Molecule E-field of Laser Perturbed System Wave-function Potential The pulse electric field perturbs the molecule and potentially dissociates it. The trick is to compute the required pulse electric field. Wave-function Potential H system = H molecule + H radiation + H interaction H radiation known H molecule small molecules: approximate large molecul