Title: Integrated atomic force microscopy and x-ray irradiation for in situ characterization of radiation-induced processes

Abstract

Understanding radiation-induced chemical and physical transformations at material interfaces is important across diverse fields, but experimental approaches are often limited to either ex situ observations or in situ electron microscopy or synchrotron-based methods, in which cases the radiation type and dose are inextricably tied to the imaging basis itself. In this work, we overcome this limitation by demonstrating integration of an x-ray source with an atomic force microscope to directly monitor radiolytically driven interfacial chemistry at the nanoscale. We illustrate the value of in situ observations by examining effects of radiolysis on material adhesion forces in aqueous solution as well as examining the production of alkali nitrates at the interface between an alkali halide crystal surface and air. For the examined salt–air interface, direct visualization under flexible experimental conditions greatly extends prior observations by enabling the transformation process to be followed comprehensively from source-to-sink with mass balance quantitation. Our novel rad-atomic force microscope opens doors into understanding the dynamics of radiolytically driven mass transfer and surface alteration at the nanoscale in real-time.

Authors:

Riechers, Shawn L.  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-5713-5534"
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Petrik, Nikolai G.  ^[1];

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• Search DOE PAGES for ORCID "0000-0001-7129-0752"
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Loring, John S. ^[1]; Murphy, Mark K. ^[1]; Pearce, Carolyn I. ^[1]; Kimmel, Gregory A.  ^[1];

• Search DOE PAGES for author "Kimmel, Gregory A."
• Search DOE PAGES for ORCID "0000-0003-4447-2440"
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Rosso, Kevin M.  ^[1]

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• Search DOE PAGES for ORCID "0000-0002-8474-7720"
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+ Show Author Affiliations

1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Publication Date:

2021-11-02

Research Org.:

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Org.:

USDOE

OSTI Identifier:

1832988

Alternate Identifier(s):

OSTI ID: 1828640

Report Number(s):

PNNL-SA-161333
Journal ID: ISSN 0034-6748; TRN: US2216875

Grant/Contract Number:  

AC05-76RL01830; AC05-76RL0-1830

Resource Type:

Accepted Manuscript

Journal Name:

Review of Scientific Instruments

Additional Journal Information:

Journal Volume: 92; Journal Issue: 11; Journal ID: ISSN 0034-6748

Publisher:

American Institute of Physics (AIP)

Country of Publication:

United States

Language:

English

Subject:

47 OTHER INSTRUMENTATION; AFM; Atomic force microscopy; In situ; Irradiation; X-ray; Alkali-halides; Surface and interface chemistry; Mass transfer; Mass balance; Adhesion; Electron microscopy; Inorganic compounds; Synchrotrons; Phase transitions