Pyroelectric Heat Detection for Calibrated Measurement of Atomic Layer Deposition Reaction Heat

Bielinski, Ashley R.; Sprague-Klein, Emily A.; Phelan, Brian T.; Martinson, Alex F.

doi:10.1021/acs.chemmater.1c01745

Title: Pyroelectric Heat Detection for Calibrated Measurement of Atomic Layer Deposition Reaction Heat

Journal Article · 30 July 2021 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.1c01745 · OSTI ID:1819648

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Argonne National Lab. (ANL), Argonne, IL (United States)

Atomic layer deposition (ALD) precursors and processes have been identified that enable the deposition of materials that span the periodic table. However, the detailed mechanisms, kinetics, thermodynamics, and complexities of even the most well-studied ALD half-reactions remain insufficiently resolved experimentally to test present computational hypotheses. In this work, a pyroelectric calorimeter is designed, implemented, calibrated, and electrically modeled to enable quantitative ALD reaction heat detection. The operation and response of three ALD calorimeter designs were evaluated for use as absolute ALD half-reaction heat detectors. The most effective design was calibrated in situ before being utilized to measure the heat generated by the reaction of trimethylaluminum with a hydroxylated alumina surface to produce 96 μJ/cm² over a reaction time of ~30 ms. With thermal and temporal resolutions down to 0.1 μJ/cm² and 50 ns, respectively, this sensitive and ultrafast probe is poised to improve our fundamental understanding of numerous ALD reaction mechanisms through quantitative comparison with first-principles computation predictions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1819648

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 15 Vol. 33; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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