RADIATIVE EXCITATION OF THE HARMONIC-OSCILLATOR WITH APPLICATIONS TO STEREOMUTATION IN CHIRAL MOLECULES

We present theoretical considerations and quantitative numerical simul ations of the coherent radiative excitation of chiral molecules exhibi ting a double well potential in the electronic ground state (with stab le enantiomers) and a harmonic oscillator potential with achiral minim um geometry in the excited electronic state following a scheme propose d in [33]. The one-dimensional short time dynamics is presented on the femtosecond time scale. We demonstrate the phenomena of quasiexponent ial, radiationless decay of the survival probability in the excited el ectronic state by simple harmonic oscillator wave packet motion, as we ll as coherent periodic chiral stereomutation. The differences and sim ilarities of the excited state harmonic oscillator dynamics with two q uite different ground state potentials are discussed. A designed pulse sequence allows for chemically efficient laser controlled stereomutat ion with high enantiomeric specificity. The results are discussed in r elation to Friedrich Hund's early work on stereomutation by tunneling and in relation to our current understanding of chiral molecules inclu ding dynamical chirality and anharmonic vibrational dynamics on the fe mtosecond time scale and the violation of parity and other fundamental symmetries.