Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach

We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify cl...

Ausführliche Beschreibung

Gespeichert in:

Bibliographische Detailangaben
Veröffentlicht in:	Physical review letters 2023-03, Vol.130 (10), p.103001-103001, Article 103001
Hauptverfasser:	Zhang, Zhedong, Nie, Xiaoyu, Lei, Dangyuan, Mukamel, Shaul
Format:	Artikel
Sprache:	eng
Schlagworte:	ATOMIC AND MOLECULAR PHYSICS Atoms, ions, & molecules in cavities Chemical physics & physical chemistry light-matter interaction Molecules Organic microcavities Physics Polaritons
Online-Zugang:	Volltext
Tags:	Tag hinzufügen Keine Tags, Fügen Sie den ersten Tag hinzu!

container_end_page	103001
container_issue	10
container_start_page	103001
container_title	Physical review letters
container_volume	130
creator	Zhang, Zhedong Nie, Xiaoyu Lei, Dangyuan Mukamel, Shaul
description	We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.
doi_str_mv	10.1103/PhysRevLett.130.103001
format	Article
fullrecord	<record><control><sourceid>proquest_osti_</sourceid><recordid>TN_cdi_osti_scitechconnect_2422046</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2791374099</sourcerecordid><originalsourceid>FETCH-LOGICAL-c391t-a61d44021301e340b0cdc79ae55aeaeb6cb0d2cabade62b88ac808103e60f7a53</originalsourceid><addsrcrecordid>eNpNkMtOwzAQRS0EglL4hSpixSZlbKdOwq6qeElFlNfacpwpNUrtEDuV-vcYtSA2M9LozMy9l5ARhTGlwK8Wq61_wc0cQxhTHofAAegBGVDIyzSnNDskAwBO0xIgPyGn3n9CJJgojskJF6VgwGBAnh_7JpjarNF646xqkplbYYc2JK8t6tA5r127TdwyeXQN6r5RXbJwsZrgrL9O5sp-4MbYZNq2nVN6dUaOlqrxeL7vQ_J-e_M2u0_nT3cPs-k81bykIVWC1lkGLIqnyDOoQNc6LxVOJgoVVkJXUDOtKlWjYFVRKF1AEW2igGWuJnxILnZ3nQ9Gem0C6pV21kbVkmWMQSYidLmDoravHn2Qa-M1No2y6HovWV5SnmdQlhEVO1RHz77DpWw7s1bdVlKQP5nLf5nLKFvuMo-Lo_2Pvlpj_bf2GzL_BqIhgTA</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2791374099</pqid></control><display><type>article</type><title>Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach</title><source>American Physical Society Journals</source><source>Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals</source><creator>Zhang, Zhedong ; Nie, Xiaoyu ; Lei, Dangyuan ; Mukamel, Shaul</creator><creatorcontrib>Zhang, Zhedong ; Nie, Xiaoyu ; Lei, Dangyuan ; Mukamel, Shaul ; Wayne State Univ., Detroit, MI (United States)</creatorcontrib><description>We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.</description><identifier>ISSN: 0031-9007</identifier><identifier>EISSN: 1079-7114</identifier><identifier>DOI: 10.1103/PhysRevLett.130.103001</identifier><identifier>PMID: 36962020</identifier><language>eng</language><publisher>United States: American Physical Society (APS)</publisher><subject>ATOMIC AND MOLECULAR PHYSICS ; Atoms, ions, & molecules in cavities ; Chemical physics & physical chemistry ; light-matter interaction ; Molecules ; Organic microcavities ; Physics ; Polaritons</subject><ispartof>Physical review letters, 2023-03, Vol.130 (10), p.103001-103001, Article 103001</ispartof><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c391t-a61d44021301e340b0cdc79ae55aeaeb6cb0d2cabade62b88ac808103e60f7a53</citedby><cites>FETCH-LOGICAL-c391t-a61d44021301e340b0cdc79ae55aeaeb6cb0d2cabade62b88ac808103e60f7a53</cites><orcidid>0000-0002-0305-6064 ; 0000-0003-3408-1630 ; 0000000334081630 ; 0000000203056064</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>230,314,776,780,881,2862,2863,27903,27904</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/36962020$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/servlets/purl/2422046$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Zhang, Zhedong</creatorcontrib><creatorcontrib>Nie, Xiaoyu</creatorcontrib><creatorcontrib>Lei, Dangyuan</creatorcontrib><creatorcontrib>Mukamel, Shaul</creatorcontrib><creatorcontrib>Wayne State Univ., Detroit, MI (United States)</creatorcontrib><title>Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach</title><title>Physical review letters</title><addtitle>Phys Rev Lett</addtitle><description>We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.</description><subject>ATOMIC AND MOLECULAR PHYSICS</subject><subject>Atoms, ions, & molecules in cavities</subject><subject>Chemical physics & physical chemistry</subject><subject>light-matter interaction</subject><subject>Molecules</subject><subject>Organic microcavities</subject><subject>Physics</subject><subject>Polaritons</subject><issn>0031-9007</issn><issn>1079-7114</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNpNkMtOwzAQRS0EglL4hSpixSZlbKdOwq6qeElFlNfacpwpNUrtEDuV-vcYtSA2M9LozMy9l5ARhTGlwK8Wq61_wc0cQxhTHofAAegBGVDIyzSnNDskAwBO0xIgPyGn3n9CJJgojskJF6VgwGBAnh_7JpjarNF646xqkplbYYc2JK8t6tA5r127TdwyeXQN6r5RXbJwsZrgrL9O5sp-4MbYZNq2nVN6dUaOlqrxeL7vQ_J-e_M2u0_nT3cPs-k81bykIVWC1lkGLIqnyDOoQNc6LxVOJgoVVkJXUDOtKlWjYFVRKF1AEW2igGWuJnxILnZ3nQ9Gem0C6pV21kbVkmWMQSYidLmDoravHn2Qa-M1No2y6HovWV5SnmdQlhEVO1RHz77DpWw7s1bdVlKQP5nLf5nLKFvuMo-Lo_2Pvlpj_bf2GzL_BqIhgTA</recordid><startdate>20230310</startdate><enddate>20230310</enddate><creator>Zhang, Zhedong</creator><creator>Nie, Xiaoyu</creator><creator>Lei, Dangyuan</creator><creator>Mukamel, Shaul</creator><general>American Physical Society (APS)</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0002-0305-6064</orcidid><orcidid>https://orcid.org/0000-0003-3408-1630</orcidid><orcidid>https://orcid.org/0000000334081630</orcidid><orcidid>https://orcid.org/0000000203056064</orcidid></search><sort><creationdate>20230310</creationdate><title>Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach</title><author>Zhang, Zhedong ; Nie, Xiaoyu ; Lei, Dangyuan ; Mukamel, Shaul</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c391t-a61d44021301e340b0cdc79ae55aeaeb6cb0d2cabade62b88ac808103e60f7a53</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>ATOMIC AND MOLECULAR PHYSICS</topic><topic>Atoms, ions, & molecules in cavities</topic><topic>Chemical physics & physical chemistry</topic><topic>light-matter interaction</topic><topic>Molecules</topic><topic>Organic microcavities</topic><topic>Physics</topic><topic>Polaritons</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Zhang, Zhedong</creatorcontrib><creatorcontrib>Nie, Xiaoyu</creatorcontrib><creatorcontrib>Lei, Dangyuan</creatorcontrib><creatorcontrib>Mukamel, Shaul</creatorcontrib><creatorcontrib>Wayne State Univ., Detroit, MI (United States)</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>Physical review letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Zhang, Zhedong</au><au>Nie, Xiaoyu</au><au>Lei, Dangyuan</au><au>Mukamel, Shaul</au><aucorp>Wayne State Univ., Detroit, MI (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach</atitle><jtitle>Physical review letters</jtitle><addtitle>Phys Rev Lett</addtitle><date>2023-03-10</date><risdate>2023</risdate><volume>130</volume><issue>10</issue><spage>103001</spage><epage>103001</epage><pages>103001-103001</pages><artnum>103001</artnum><issn>0031-9007</issn><eissn>1079-7114</eissn><abstract>We present a microscopic theory for nonlinear optical spectroscopy of N molecules in an optical cavity. Using the Heisenberg-Langevin equation, an analytical expression is derived for the time- and frequency-resolved signals accounting for arbitrary numbers of vibrational excitations. We identify clear signatures of the polariton-polaron interaction from multidimensional projections of the signal, e.g., pathways and timescales. Cooperative dynamics of cavity polaritons against intramolecular vibrations is revealed, along with a crosstalk between long-range coherence and vibronic coupling that may lead to localization effects. Our results further characterize the polaritonic coherence and the population transfer that is slower.</abstract><cop>United States</cop><pub>American Physical Society (APS)</pub><pmid>36962020</pmid><doi>10.1103/PhysRevLett.130.103001</doi><tpages>1</tpages><orcidid>https://orcid.org/0000-0002-0305-6064</orcidid><orcidid>https://orcid.org/0000-0003-3408-1630</orcidid><orcidid>https://orcid.org/0000000334081630</orcidid><orcidid>https://orcid.org/0000000203056064</orcidid><oa>free_for_read</oa></addata></record>
fulltext	fulltext
identifier	ISSN: 0031-9007
ispartof	Physical review letters, 2023-03, Vol.130 (10), p.103001-103001, Article 103001
issn	0031-9007 1079-7114
language	eng
recordid	cdi_osti_scitechconnect_2422046
source	American Physical Society Journals; Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals
subjects	ATOMIC AND MOLECULAR PHYSICS Atoms, ions, & molecules in cavities Chemical physics & physical chemistry light-matter interaction Molecules Organic microcavities Physics Polaritons
title	Multidimensional Coherent Spectroscopy of Molecular Polaritons: Langevin Approach
url	https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2025-01-25T12%3A59%3A04IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_osti_&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Multidimensional%20Coherent%20Spectroscopy%20of%20Molecular%20Polaritons:%20Langevin%20Approach&rft.jtitle=Physical%20review%20letters&rft.au=Zhang,%20Zhedong&rft.aucorp=Wayne%20State%20Univ.,%20Detroit,%20MI%20(United%20States)&rft.date=2023-03-10&rft.volume=130&rft.issue=10&rft.spage=103001&rft.epage=103001&rft.pages=103001-103001&rft.artnum=103001&rft.issn=0031-9007&rft.eissn=1079-7114&rft_id=info:doi/10.1103/PhysRevLett.130.103001&rft_dat=%3Cproquest_osti_%3E2791374099%3C/proquest_osti_%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2791374099&rft_id=info:pmid/36962020&rfr_iscdi=true