Sum-frequency vibrational spectroscopy of centrosymmetric molecule at interfaces
Ren‐Hui Zheng, Wen‐Mei Wei, Shuocang Zhang
Abstract
The centrosymmetric benzene molecule has zero first-order electric dipole hyperpolarizability, which results in no sum-frequency vibrational spectroscopy (SFVS) signal at interfaces, but it shows very strong SFVS experimentally. We perform a theoretical study on its SFVS, which is in good agreement with the experimental results. Its strong SFVS mainly comes from the interfacial electric quadrupole hyperpolarizability rather than the symmetry-breaking electric dipole, bulk electric quadrupole, and interfacial and bulk magnetic dipole hyperpolarizabilities, which provides a novel and completely unconventional point of view.
Topics & Concepts
HyperpolarizabilityQuadrupoleDipoleSpectroscopyChemistryElectric dipole momentMolecular physicsAtomic physicsMoleculeComputational chemistryPhysicsPolarizabilityQuantum mechanicsOrganic chemistrySpectroscopy and Quantum Chemical StudiesSolid-state spectroscopy and crystallographyNonlinear Optical Materials Research