Vibrational Spectroscopy of Water with High Spatial Resolution

Jacob R. Jokisaari, Jordan A. Hachtel, Xuan Hu, Arijita Mukherjee, Canhui Wang, Andrea Konecna, Tracy C. Lovejoy, Niklas Dellby, Javier Aizpurua, Ondrej L. Krivanek, Juan Carlos Idrobo, Robert F. Klie

Research output: Contribution to journalArticlepeer-review

40 Scopus citations

Abstract

The ability to examine the vibrational spectra of liquids with nanometer spatial resolution will greatly expand the potential to study liquids and liquid interfaces. In fact, the fundamental properties of water, including complexities in its phase diagram, electrochemistry, and bonding due to nanoscale confinement are current research topics. For any liquid, direct investigation of ordered liquid structures, interfacial double layers, and adsorbed species at liquid–solid interfaces are of interest. Here, a novel way of characterizing the vibrational properties of liquid water with high spatial resolution using transmission electron microscopy is reported. By encapsulating water between two sheets of boron nitride, the ability to capture vibrational spectra to quantify the structure of the liquid, its interaction with the liquid-cell surfaces, and the ability to identify isotopes including H2O and D2O using electron energy-loss spectroscopy is demonstrated. The electron microscope used here, equipped with a high-energy-resolution monochromator, is able to record vibrational spectra of liquids and molecules and is sensitive to surface and bulk morphological properties both at the nano- and micrometer scales. These results represent an important milestone for liquid and isotope-labeled materials characterization with high spatial resolution, combining nanoscale imaging with vibrational spectroscopy.

Original languageEnglish
Article number1802702
JournalAdvanced Materials
Volume30
Issue number36
DOIs
StatePublished - Sep 6 2018

Funding

J.R.J. and J.A.H. contributed equally to this work. Microscopy research performed as part of a user proposal at Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility (J.A.H, J.C.I.). This research was conducted, in part, using instrumentation within ORNL’s Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. This manuscript was authorized by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/ downloads/doe-public-access-plan). Acquisition of UIC JEOL ARM200CF was supported by an MRI-R2 grant from the National Science Foundation (DMR-0959470). The Gatan Quantum GIF acquisition at UIC was supported by an MRI grant from the National Science Foundation (DMR-1626065). Theoretical simulations were supported by Spanish Ministry project FIS2016-80174-P. J.R.J. and J.A.H. contributed equally to this work. Microscopy research performed as part of a user proposal at Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), which is a U.S. Department of Energy, Office of Science User Facility (J.A.H, J.C.I.). This research was conducted, in part, using instrumentation within ORNL's Materials Characterization Core provided by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. This manuscript was authorized by UT-Battelle, LLC under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The U.S. Government retains and the publisher, by accepting the article for publication, acknowledges that the U.S. Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for U.S. Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). ?Acquisition of UIC JEOL ARM200CF was supported by an MRI-R2 grant from the National Science Foundation (DMR-0959470). The Gatan Quantum GIF acquisition at UIC was supported by an MRI grant from the National Science Foundation (DMR-1626065). Theoretical simulations were supported by Spanish Ministry project FIS2016-80174-P.

FundersFunder number
CNMS
DOE Public Access Plan
Oak Ridge National Laboratory
U.S. Government
UT-Battelle, LLCDE-AC05-00OR22725
National Science FoundationDMR-1626065, 1626065, DMR-0959470, FIS2016-80174-P
U.S. Department of Energy
Office of Science

    Keywords

    • EELS
    • STEM
    • liquid cells
    • nanoscale
    • spectroscopy

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