Picosecond dynamic heterogeneity, hopping, and Johari-Goldstein relaxation in glass-forming liquids

We show that incoherent quasielastic neutron scattering from molecular liquids reveals a two-state dynamic heterogeneity on a 1 ps time scale, where molecules are either highly confined or are free to undergo relatively large excursions. Data ranging from deep in the glassy state to well above the m...

Ausführliche Beschreibung

Gespeichert in:
Bibliographische Detailangaben
Veröffentlicht in:Physical review letters 2014-09, Vol.113 (11), p.117801-117801, Article 117801
Hauptverfasser: Cicerone, Marcus T, Zhong, Qin, Tyagi, Madhusudan
Format: Artikel
Sprache:eng
Schlagworte:
Online-Zugang:Volltext
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
container_end_page 117801
container_issue 11
container_start_page 117801
container_title Physical review letters
container_volume 113
creator Cicerone, Marcus T
Zhong, Qin
Tyagi, Madhusudan
description We show that incoherent quasielastic neutron scattering from molecular liquids reveals a two-state dynamic heterogeneity on a 1 ps time scale, where molecules are either highly confined or are free to undergo relatively large excursions. Data ranging from deep in the glassy state to well above the melting point allows us to observe temperature-dependent population levels and exchange between these two states. A simple physical picture emerges from this data, combined with published work, that provides a mechanism for hopping and for the Johari-Goldstein (β_{JG}) relaxation, and allows us to accurately calculate the diffusion coefficient, D_{T}, and characteristic times for α, and β_{JG} relaxations from ps time scale neutron data.
doi_str_mv 10.1103/PhysRevLett.113.117801
format Article
fullrecord <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_miscellaneous_1786210439</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>1786210439</sourcerecordid><originalsourceid>FETCH-LOGICAL-c397t-d38b6110635e5b67c7f5a061e1ccba35b3391cdb24637e1613eabd58a3aafe8e3</originalsourceid><addsrcrecordid>eNqFUctOwzAQtBCIlsIvVDlyIGBnGzs5ogoKqBIVgnPkOJvGKIlTO0Hk7zFqQdw4rFY7mtnXEDJn9JoxCjebanQv-LHGvvcA-BAJZUdkyqhIQ8HY4phMKQUWppSKCTlz7p1SyiKenJJJFEfcV_GUqI1WxqEybREUYysbrYIKe7Rmiy3qfrwKKtN1ut1eBdJznkwlrQ5Xpi5cj7oNLNbyU_batIGvtrV0LiyNbbwiqPVu0IU7JyelrB1eHPKMvN3fvS4fwvXz6nF5uw4VpKIPC0hy7o_jEGOcc6FEGUvKGTKlcglxDpAyVeTRgoNAxhmgzIs4kSBliQnCjFzu-3bW7AZ0fdZop7CuZYtmcJl_EY8YXUD6PzXmfpUIkshT-Z6qrHHOYpl1VjfSjhmj2bcX2R8vPADZ3gsvnB9mDHmDxa_s5_nwBT-HiY0</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>1566112382</pqid></control><display><type>article</type><title>Picosecond dynamic heterogeneity, hopping, and Johari-Goldstein relaxation in glass-forming liquids</title><source>MEDLINE</source><source>APS: American Physical Society E-Journals (Physics)</source><creator>Cicerone, Marcus T ; Zhong, Qin ; Tyagi, Madhusudan</creator><creatorcontrib>Cicerone, Marcus T ; Zhong, Qin ; Tyagi, Madhusudan</creatorcontrib><description>We show that incoherent quasielastic neutron scattering from molecular liquids reveals a two-state dynamic heterogeneity on a 1 ps time scale, where molecules are either highly confined or are free to undergo relatively large excursions. Data ranging from deep in the glassy state to well above the melting point allows us to observe temperature-dependent population levels and exchange between these two states. A simple physical picture emerges from this data, combined with published work, that provides a mechanism for hopping and for the Johari-Goldstein (β_{JG}) relaxation, and allows us to accurately calculate the diffusion coefficient, D_{T}, and characteristic times for α, and β_{JG} relaxations from ps time scale neutron data.</description><identifier>ISSN: 0031-9007</identifier><identifier>EISSN: 1079-7114</identifier><identifier>DOI: 10.1103/PhysRevLett.113.117801</identifier><identifier>PMID: 25260005</identifier><language>eng</language><publisher>United States</publisher><subject>Dynamics ; Exchange ; Glass - chemistry ; Glass formation ; Heterogeneity ; Liquids ; Mathematical analysis ; Models, Chemical ; Neutron Diffraction ; Neutron scattering ; Phase Transition ; Thermodynamics ; Time</subject><ispartof>Physical review letters, 2014-09, Vol.113 (11), p.117801-117801, Article 117801</ispartof><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c397t-d38b6110635e5b67c7f5a061e1ccba35b3391cdb24637e1613eabd58a3aafe8e3</citedby><cites>FETCH-LOGICAL-c397t-d38b6110635e5b67c7f5a061e1ccba35b3391cdb24637e1613eabd58a3aafe8e3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,2876,2877,27924,27925</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/25260005$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Cicerone, Marcus T</creatorcontrib><creatorcontrib>Zhong, Qin</creatorcontrib><creatorcontrib>Tyagi, Madhusudan</creatorcontrib><title>Picosecond dynamic heterogeneity, hopping, and Johari-Goldstein relaxation in glass-forming liquids</title><title>Physical review letters</title><addtitle>Phys Rev Lett</addtitle><description>We show that incoherent quasielastic neutron scattering from molecular liquids reveals a two-state dynamic heterogeneity on a 1 ps time scale, where molecules are either highly confined or are free to undergo relatively large excursions. Data ranging from deep in the glassy state to well above the melting point allows us to observe temperature-dependent population levels and exchange between these two states. A simple physical picture emerges from this data, combined with published work, that provides a mechanism for hopping and for the Johari-Goldstein (β_{JG}) relaxation, and allows us to accurately calculate the diffusion coefficient, D_{T}, and characteristic times for α, and β_{JG} relaxations from ps time scale neutron data.</description><subject>Dynamics</subject><subject>Exchange</subject><subject>Glass - chemistry</subject><subject>Glass formation</subject><subject>Heterogeneity</subject><subject>Liquids</subject><subject>Mathematical analysis</subject><subject>Models, Chemical</subject><subject>Neutron Diffraction</subject><subject>Neutron scattering</subject><subject>Phase Transition</subject><subject>Thermodynamics</subject><subject>Time</subject><issn>0031-9007</issn><issn>1079-7114</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><sourceid>EIF</sourceid><recordid>eNqFUctOwzAQtBCIlsIvVDlyIGBnGzs5ogoKqBIVgnPkOJvGKIlTO0Hk7zFqQdw4rFY7mtnXEDJn9JoxCjebanQv-LHGvvcA-BAJZUdkyqhIQ8HY4phMKQUWppSKCTlz7p1SyiKenJJJFEfcV_GUqI1WxqEybREUYysbrYIKe7Rmiy3qfrwKKtN1ut1eBdJznkwlrQ5Xpi5cj7oNLNbyU_batIGvtrV0LiyNbbwiqPVu0IU7JyelrB1eHPKMvN3fvS4fwvXz6nF5uw4VpKIPC0hy7o_jEGOcc6FEGUvKGTKlcglxDpAyVeTRgoNAxhmgzIs4kSBliQnCjFzu-3bW7AZ0fdZop7CuZYtmcJl_EY8YXUD6PzXmfpUIkshT-Z6qrHHOYpl1VjfSjhmj2bcX2R8vPADZ3gsvnB9mDHmDxa_s5_nwBT-HiY0</recordid><startdate>20140912</startdate><enddate>20140912</enddate><creator>Cicerone, Marcus T</creator><creator>Zhong, Qin</creator><creator>Tyagi, Madhusudan</creator><scope>CGR</scope><scope>CUY</scope><scope>CVF</scope><scope>ECM</scope><scope>EIF</scope><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>7U5</scope><scope>8FD</scope><scope>H8D</scope><scope>L7M</scope></search><sort><creationdate>20140912</creationdate><title>Picosecond dynamic heterogeneity, hopping, and Johari-Goldstein relaxation in glass-forming liquids</title><author>Cicerone, Marcus T ; Zhong, Qin ; Tyagi, Madhusudan</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c397t-d38b6110635e5b67c7f5a061e1ccba35b3391cdb24637e1613eabd58a3aafe8e3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Dynamics</topic><topic>Exchange</topic><topic>Glass - chemistry</topic><topic>Glass formation</topic><topic>Heterogeneity</topic><topic>Liquids</topic><topic>Mathematical analysis</topic><topic>Models, Chemical</topic><topic>Neutron Diffraction</topic><topic>Neutron scattering</topic><topic>Phase Transition</topic><topic>Thermodynamics</topic><topic>Time</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Cicerone, Marcus T</creatorcontrib><creatorcontrib>Zhong, Qin</creatorcontrib><creatorcontrib>Tyagi, Madhusudan</creatorcontrib><collection>Medline</collection><collection>MEDLINE</collection><collection>MEDLINE (Ovid)</collection><collection>MEDLINE</collection><collection>MEDLINE</collection><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>Technology Research Database</collection><collection>Aerospace Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Physical review letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Cicerone, Marcus T</au><au>Zhong, Qin</au><au>Tyagi, Madhusudan</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Picosecond dynamic heterogeneity, hopping, and Johari-Goldstein relaxation in glass-forming liquids</atitle><jtitle>Physical review letters</jtitle><addtitle>Phys Rev Lett</addtitle><date>2014-09-12</date><risdate>2014</risdate><volume>113</volume><issue>11</issue><spage>117801</spage><epage>117801</epage><pages>117801-117801</pages><artnum>117801</artnum><issn>0031-9007</issn><eissn>1079-7114</eissn><abstract>We show that incoherent quasielastic neutron scattering from molecular liquids reveals a two-state dynamic heterogeneity on a 1 ps time scale, where molecules are either highly confined or are free to undergo relatively large excursions. Data ranging from deep in the glassy state to well above the melting point allows us to observe temperature-dependent population levels and exchange between these two states. A simple physical picture emerges from this data, combined with published work, that provides a mechanism for hopping and for the Johari-Goldstein (β_{JG}) relaxation, and allows us to accurately calculate the diffusion coefficient, D_{T}, and characteristic times for α, and β_{JG} relaxations from ps time scale neutron data.</abstract><cop>United States</cop><pmid>25260005</pmid><doi>10.1103/PhysRevLett.113.117801</doi><tpages>1</tpages></addata></record>
fulltext fulltext
identifier ISSN: 0031-9007
ispartof Physical review letters, 2014-09, Vol.113 (11), p.117801-117801, Article 117801
issn 0031-9007
1079-7114
language eng
recordid cdi_proquest_miscellaneous_1786210439
source MEDLINE; APS: American Physical Society E-Journals (Physics)
subjects Dynamics
Exchange
Glass - chemistry
Glass formation
Heterogeneity
Liquids
Mathematical analysis
Models, Chemical
Neutron Diffraction
Neutron scattering
Phase Transition
Thermodynamics
Time
title Picosecond dynamic heterogeneity, hopping, and Johari-Goldstein relaxation in glass-forming liquids
url https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-20T15%3A32%3A32IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_cross&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Picosecond%20dynamic%20heterogeneity,%20hopping,%20and%20Johari-Goldstein%20relaxation%20in%20glass-forming%20liquids&rft.jtitle=Physical%20review%20letters&rft.au=Cicerone,%20Marcus%20T&rft.date=2014-09-12&rft.volume=113&rft.issue=11&rft.spage=117801&rft.epage=117801&rft.pages=117801-117801&rft.artnum=117801&rft.issn=0031-9007&rft.eissn=1079-7114&rft_id=info:doi/10.1103/PhysRevLett.113.117801&rft_dat=%3Cproquest_cross%3E1786210439%3C/proquest_cross%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=1566112382&rft_id=info:pmid/25260005&rfr_iscdi=true