Two-Libron Spectrum of Solid H2 and D2

It is shown that the "two-libron" lines in the Raman spectrum of solid hydrogen result from the large cubic anharmonicity of the quadrupole-quadrupole Hamiltonian. A localized picture is used to describe the interaction of two librational excitations on neighboring molecules, and dynamic interactions with other molecules are treated perturbatively. In this approximation the average single-libron energy agrees with the anharmonic calculation in the accompanying paper. Using a value of the quadrupole-coupling constant obtained from the single-libron spectrum, the resulting two-libron energies and Raman transition probabilities are in excellent agreement with the observed spectrum. Disciplines Physics | Quantum Physics This journal article is available at ScholarlyCommons: http://repository.upenn.edu/physics_papers/416 PHYSICAL REVIEW B VOLUME 4, NU MBKR 8 Two-Libron Spectrum of Solid H2 and D2~ 15 OCTOBER 1971 A. John Berlinsky and A. Brooks Harris Department of Physics, University of Pennsylvania, Philade/podia, Pennsylvania 19104 (Received 19 January 1971) It is shown that the "bvo-libron" lines in the Baman spectrum of solid hydrogen result from the large cubic anharmonicity of the quadrupole-quadrupole Hamiltonian. A localized picture is used to describe the interaction of two librational excitations on neighboring molecules, and dynamic interactions with other molecules are treated perturbatively. In this approximation the average single-libron energy agrees with the anharmonic calculation in the accompanying paper. Using a value of the quadrupole-coupling constant obtained from the single-libron spectrum, the resulting two-libron energies and Baman transition probabilities are in excellent agreement with the observed spectrum.