Six-wave mixing in a ZnSe quantum well is investigated and compared with microscopic theory. We demonstrate that sixth-order Coulomb correlations have a significant qualitative impact on the nonlinear optical response. Six-wave mixing is shown to be a uniquely sensitive tool for investigation of correlations beyond the four-point level.
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http://dx.doi.org/10.1103/PhysRevLett.85.2002 | DOI Listing |
J Chem Phys
November 2011
Institut für Physikalische Chemie, Universität Mainz, 55099 Mainz, Germany.
A formulation of sixth-order direct perturbation theory (DPT) to treat relativistic effects in quantum-chemical calculations is presented in the framework of derivative theory. Detailed expressions for DPT6 are given at the Hartree-Fock level in terms of the third derivative of the energy with respect to the relativistic perturbation parameter defined as λ(rel)=c(-2). They were implemented for the computation of scalar-relativistic energy corrections.
View Article and Find Full Text PDFJ Chem Phys
April 2006
Department of Basic Science, Graduate School of Arts and Sciences, University of Tokyo, Komaba, 153-8902 Tokyo, Japan.
The validity range of the Born-Oppenheimer (BO) approximation is studied with respect to the variation of the mass (m) of negatively charged particle by substituting an electron (e) with muon (mu) and antiproton (p) in hydrogen molecule cation. With the use of semiclassical quantization applied to these (ppe), (ppmu), and (ppp) under a constrained geometry, we estimate the energy difference of the non-BO vibronic ground state from the BO counterpart. It is found that the error in the BO approximation scales to the power of 3/2 to the mass of negative particles, that is, m(1.
View Article and Find Full Text PDFPhys Rev Lett
August 2000
Department of Physics, University of California and Materials Sciences Division, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, MS 2-346, Berkeley, California 94720, USA.
Six-wave mixing in a ZnSe quantum well is investigated and compared with microscopic theory. We demonstrate that sixth-order Coulomb correlations have a significant qualitative impact on the nonlinear optical response. Six-wave mixing is shown to be a uniquely sensitive tool for investigation of correlations beyond the four-point level.
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