{"id":{"repo_id":"uiuc","oai_identifier":"oai:www.ideals.illinois.edu:2142/99456"},"canonical_url":"https://search.dev.ndltd.org/etd/uiuc/oai:www.ideals.illinois.edu:2142/99456","repository":{"repo_id":"uiuc","name":"University of Illinois - Urbana-Champaign","base_url":"https://www.ideals.illinois.edu/oai-pmh"},"display":{"title":"Ab initio modeling of hydrogen pipe diffusion in palladium","abstract":"A hydrogen economy will require metals for separation, transport and/or storage. Therefore, we need to better understand the behavior of hydrogen in metals. Hydrogen in palladium is a model system, for which there exists an abundance of experimental data. Specifically, quasielastic neutron scattering (QENS) experiments, for the first time, directly measured hydrogen pipe diffusion. The diffusivities and energy barriers from ab initio simulations support these findings, but open questions remain, the most concerning of which pertains to the unusual jump distances reported from fitting the experimental data. Instead of comparing diffusivities and energy barriers from simulation with the parameters extracted from fits to the experimental data, we calculate the spherically-averaged incoherent scattering function to directly compare with experimental data. We find that the experimental fitting procedure introduces errors in the extracted diffusivities and jump distances. We also calculate the intermediate scattering function to compare our simulation results with a wider range of experimental data. From direct comparison of the intermediate scattering function, we find disagreement at small times, which is likely due to the contributions from the vibrational motion of the diffusing hydrogen atom, the host palladium atoms and resonate vibrations. This computational approach allows for validation against experiment, along with a more detailed understanding of the QENS results.","abstract_html":"A hydrogen economy will require metals for separation, transport and/or storage. Therefore, we need to better understand the behavior of hydrogen in metals. Hydrogen in palladium is a model system, for which there exists an abundance of experimental data. Specifically, quasielastic neutron scattering (QENS) experiments, for the first time, directly measured hydrogen pipe diffusion. The diffusivities and energy barriers from ab initio simulations support these findings, but open questions remain, the most concerning of which pertains to the unusual jump distances reported from fitting the experimental data. Instead of comparing diffusivities and energy barriers from simulation with the parameters extracted from fits to the experimental data, we calculate the spherically-averaged incoherent scattering function to directly compare with experimental data. We find that the experimental fitting procedure introduces errors in the extracted diffusivities and jump distances. We also calculate the intermediate scattering function to compare our simulation results with a wider range of experimental data. From direct comparison of the intermediate scattering function, we find disagreement at small times, which is likely due to the contributions from the vibrational motion of the diffusing hydrogen atom, the host palladium atoms and resonate vibrations. This computational approach allows for validation against experiment, along with a more detailed understanding of the QENS results.","abstract_has_math":false,"creators":["Schiavone, Emily"],"institution":"University of Illinois at Urbana-Champaign","degree_name":"Ph.D.","degree_level":"Dissertation","degree_discipline":"Materials Science & Engr","degree_department":null,"school":null,"contributors":["Trinkle, Dallas R.","Bellon, Pascal","Heuser, Brent J.","Schleife, André"],"advisors":[],"committee_chairs":[],"committee_members":[],"year":2018,"date_issued":"2018-03-13T17:28:59Z","date_published":"2018-03-13T17:28:59Z","updated_at":"2026-07-22T22:24:37Z","subjects":["Hydrogen","Diffusion","Simulation"],"languages":["en"],"rights":["Copyright 2017 Emily Schiavone"],"rights_urls":[],"identifier_entries":[]},"links":{"outbound_url":"http://hdl.handle.net/2142/99456","outbound_label":"Handle","outbound_source":"dc:identifier"},"metadata_groups":[{"id":"people","label":"People","entries":[{"key":"dc:contributor","label":"Contributor","values":["Trinkle, Dallas R.","Bellon, Pascal","Heuser, Brent J.","Schleife, André"]},{"key":"dc:creator","label":"Author","values":["Schiavone, Emily"]}]},{"id":"academic_context","label":"Academic Context","entries":[{"key":"dc:date","label":"Dc Date","values":["2018-03-13T17:28:59Z","2020-03-14T09:15:25Z","2017-08-21","2017-12"]},{"key":"dc:type","label":"Dc Type","values":["text"]},{"key":"thesis:degree_discipline","label":"Discipline","values":["Materials Science & Engr"]},{"key":"thesis:degree_level","label":"Degree Level","values":["Dissertation"]},{"key":"thesis:degree_name","label":"Degree Name","values":["Ph.D."]},{"key":"thesis:institution_name","label":"Thesis Institution Name","values":["University of Illinois at Urbana-Champaign"]}]},{"id":"subjects_keywords","label":"Subjects and Keywords","entries":[{"key":"dc:subject","label":"Dc Subject","values":["Hydrogen","Diffusion","Simulation"]}]},{"id":"language_rights","label":"Language and Rights","entries":[{"key":"dc:language","label":"Dc Language","values":["en"]},{"key":"dc:rights","label":"Dc Rights","values":["Copyright 2017 Emily Schiavone"]}]},{"id":"identifiers","label":"Identifiers","entries":[{"key":"dc:identifier","label":"Identifier","values":["http://hdl.handle.net/2142/99456"]}]},{"id":"additional","label":"Additional Metadata","entries":[{"key":"dc:description","label":"Description","values":["A hydrogen economy will require metals for separation, transport and/or storage. Therefore, we need to better understand the behavior of hydrogen in metals. Hydrogen in palladium is a model system, for which there exists an abundance of experimental data. Specifically, quasielastic neutron scattering (QENS) experiments, for the first time, directly measured hydrogen pipe diffusion. The diffusivities and energy barriers from ab initio simulations support these findings, but open questions remain, the most concerning of which pertains to the unusual jump distances reported from fitting the experimental data. Instead of comparing diffusivities and energy barriers from simulation with the parameters extracted from fits to the experimental data, we calculate the spherically-averaged incoherent scattering function to directly compare with experimental data. We find that the experimental fitting procedure introduces errors in the extracted diffusivities and jump distances. We also calculate the intermediate scattering function to compare our simulation results with a wider range of experimental data. From direct comparison of the intermediate scattering function, we find disagreement at small times, which is likely due to the contributions from the vibrational motion of the diffusing hydrogen atom, the host palladium atoms and resonate vibrations. This computational approach allows for validation against experiment, along with a more detailed understanding of the QENS results.","Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2019-12-01","The student, Emily Schiavone, accepted the attached license on 2017-08-21 at 12:31.","The student, Emily Schiavone, submitted this Dissertation for approval on 2017-08-21 at 12:46.","This Dissertation was approved for publication on 2017-08-21 at 14:50.","DSpace SAF Submission Ingestion Package generated from Vireo submission #11608 on 2018-03-13 at 10:32:18","Made available in DSpace on 2018-03-13T17:28:59Z (GMT). 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Therefore, we need to better understand the behavior of hydrogen in metals. Hydrogen in palladium is a model system, for which there exists an abundance of experimental data. Specifically, quasielastic neutron scattering (QENS) experiments, for the first time, directly measured hydrogen pipe diffusion. The diffusivities and energy barriers from ab initio simulations support these findings, but open questions remain, the most concerning of which pertains to the unusual jump distances reported from fitting the experimental data. Instead of comparing diffusivities and energy barriers from simulation with the parameters extracted from fits to the experimental data, we calculate the spherically-averaged incoherent scattering function to directly compare with experimental data. We find that the experimental fitting procedure introduces errors in the extracted diffusivities and jump distances. We also calculate the intermediate scattering function to compare our simulation results with a wider range of experimental data. From direct comparison of the intermediate scattering function, we find disagreement at small times, which is likely due to the contributions from the vibrational motion of the diffusing hydrogen atom, the host palladium atoms and resonate vibrations. This computational approach allows for validation against experiment, along with a more detailed understanding of the QENS results.","Submission published under a 24 month embargo labeled 'Closed Access', the embargo will last until 2019-12-01","The student, Emily Schiavone, accepted the attached license on 2017-08-21 at 12:31.","The student, Emily Schiavone, submitted this Dissertation for approval on 2017-08-21 at 12:46.","This Dissertation was approved for publication on 2017-08-21 at 14:50.","DSpace SAF Submission Ingestion Package generated from Vireo submission #11608 on 2018-03-13 at 10:32:18","Made available in DSpace on 2018-03-13T17:28:59Z (GMT). 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