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Determination of H-Atom Positions in Organic Crystal Structures by NEXAFS Combined with Density Functional Theory: a Study of Two-Component Systems Containing Isonicotinamide

Paul T. Edwards, Lucy K. Saunders, David C. Grinter, Pilar Ferrer, Georg Held, Elizabeth J. Shotton, Sven L. M. Schroeder

2022The Journal of Physical Chemistry A18 citationsDOIOpen Access PDF

Abstract

It is important to be able to identify the precise position of H-atoms in hydrogen bonding interactions to fully understand the effects on the structure and properties of organic crystals. Using a combination of near-edge X-ray absorption fine structure (NEXAFS) spectroscopy and density functional theory (DFT) quantum chemistry calculations, we demonstrate the sensitivity of core-level X-ray spectroscopy to the precise H-atom position within a donor-proton-acceptor system. Exploiting this sensitivity, we then combine the predictive power of DFT with the experimental NEXAFS, confirming the H-atom position identified using single-crystal X-ray diffraction (XRD) techniques more easily than using other H-atom sensitive techniques, such as neutron diffraction. This proof of principle experiment confirms the H-atom positions in structures obtained from XRD, providing evidence for the potential use of NEXAFS as a more accurate and easier method of locating H-atoms within organic crystals.

Topics & Concepts

XANESDensity functional theoryAtom (system on chip)Absorption (acoustics)CrystallographySpectroscopyMaterials scienceExtended X-ray absorption fine structureCrystal structureChemistryAbsorption spectroscopyComputational chemistryPhysicsOpticsComposite materialEmbedded systemQuantum mechanicsComputer scienceCrystallography and molecular interactionsX-ray Diffraction in CrystallographyAdvanced Chemical Physics Studies
Determination of H-Atom Positions in Organic Crystal Structures by NEXAFS Combined with Density Functional Theory: a Study of Two-Component Systems Containing Isonicotinamide | Litcius