Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 130, Issue 11, Pages 3509-3515Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja0774414
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- Direct For Mathematical & Physical Scien
- Division Of Chemistry [0745892] Funding Source: National Science Foundation
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The-nonlinear optical signal generated in phenol by three femtosecond pulses with wavevectors k(1), k(2), and k(3) in the phase-matching direction k(1) + k(2) - k(3) is simulated. This two-dimensional coherent spectroscopy (2DCS) signal has a rich pattern containing information on double-excitation states. The signal vanishes for uncorrelated electrons due to interference among quantum pathways and, thus, provides direct signatures of correlated many-electron wavefunctions. This is illustrated by the very different 2DCS signals predicted by two levels of electronic structure calculations: state-averaged complete active space self-consistent field (SA-CASSCF) and multistate multiconfigurational second-order perturbation theory (MS-CASPT2).
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