作者: Audrey Dell Hammerich , Ronnie Kosloff , Mark A. Ratner
DOI: 10.1063/1.463948
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摘要: Time‐dependent quantum‐mechanical theories and simulations provide a clear intuitive description of molecular processes. Due to ensuing simplification the theory generally employed numerical algorithms, vast majority these treatments are based upon perturbation theory. Especially in light current level experimental sophistication, with experiments being realized which influenced by spectral, temporal, spatial shape laser pulse, it is important move beyond limited weak fields or idealized δ‐function wave forms. Various methods examine results high‐field presented. All techniques shown have familiar linear response form weak‐field limit. In time‐dependent framework difference between nonlinear expressions can be seen from expectation values over stationary versus nonstationary states. The photodissociation methyl iodide illustrates this approach. ...