Polariton response in the presence of Brownian dissipation from molecular vibrations
We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in...
Uloženo v:
| Vydáno v: | The Journal of chemical physics Ročník 154; číslo 4; s. 044108 |
|---|---|
| Hlavní autoři: | , , |
| Médium: | Journal Article |
| Jazyk: | angličtina |
| Vydáno: |
United States
28.01.2021
|
| ISSN: | 1089-7690, 1089-7690 |
| On-line přístup: | Zjistit podrobnosti o přístupu |
| Tagy: |
Přidat tag
Žádné tagy, Buďte první, kdo vytvoří štítek k tomuto záznamu!
|
| Abstract | We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, the uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed "zero-detuning" point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to "prove" results originating from strong coupling, such as vacuum-enhanced chemical reaction rate. |
|---|---|
| AbstractList | We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, the uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed "zero-detuning" point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to "prove" results originating from strong coupling, such as vacuum-enhanced chemical reaction rate.We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, the uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed "zero-detuning" point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to "prove" results originating from strong coupling, such as vacuum-enhanced chemical reaction rate. We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main dissipation channels due to the finite cavity linewidth and molecular vibrations. We show that the frequently used coupled oscillator model fails in describing this response especially due to the non-Lorentzian dissipation of the molecules to their vibrations. Signatures of this failure are the temperature dependent minimum point of the polariton peak splitting, the uneven polariton peak height at the minimum splitting, and the asymmetric shape of the polariton peaks even at the experimentally accessed "zero-detuning" point. Using a rather generic yet representative model of molecular vibrations, we predict the polariton response in various conditions, depending on the temperature, molecular Stokes shift and vibration frequencies, and the size of the Rabi splitting. Our results can be used as a sanity check of the experiments trying to "prove" results originating from strong coupling, such as vacuum-enhanced chemical reaction rate. |
| Author | Kansanen, Kalle S U Heikkilä, Tero T Toppari, J Jussi |
| Author_xml | – sequence: 1 givenname: Kalle S U orcidid: 0000000234337926 surname: Kansanen fullname: Kansanen, Kalle S U organization: Department of Physics and Nanoscience Center, University of Jyväskylä, P.O. Box 35, FI-40014 University of Jyväskylä, Finland – sequence: 2 givenname: J Jussi orcidid: 0000000216985591 surname: Toppari fullname: Toppari, J Jussi organization: Department of Physics and Nanoscience Center, University of Jyväskylä, P.O. Box 35, FI-40014 University of Jyväskylä, Finland – sequence: 3 givenname: Tero T orcidid: 000000027732691X surname: Heikkilä fullname: Heikkilä, Tero T organization: Department of Physics and Nanoscience Center, University of Jyväskylä, P.O. Box 35, FI-40014 University of Jyväskylä, Finland |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/33514103$$D View this record in MEDLINE/PubMed |
| BookMark | eNpNkDtPxDAQhC10iHtAwR9ALmlyrOM4jks48ZJOguKoI8dZC6PEDnYOxL8ngkOi2p3Zma_YJZn54JGQcwZrBiW_EmsAXioQR2TBoFKZnMTs3z4ny5TeAIDJvDghc84FKxjwBdk9h05HNwZPI6Yh-ITUeTq-Ih0mA71BGiy9ieHTO-1p61Jygx7dVLAx9LQPHZr9xKAfrok_h3RKjq3uEp4d5oq83N3uNg_Z9un-cXO9zQwv-JgVSoAqmBFQVK3lIm_Blih13oBRTY7GKtlq01gprC5FaayQwBvRSoVCNCpfkctf7hDD-x7TWPcuGew67THsU50XFa8Y55JP0YtDdN_02NZDdL2OX_XfJ_JvvthhjQ |
| ContentType | Journal Article |
| DBID | NPM 7X8 |
| DOI | 10.1063/5.0036905 |
| DatabaseName | PubMed MEDLINE - Academic |
| DatabaseTitle | PubMed MEDLINE - Academic |
| DatabaseTitleList | MEDLINE - Academic PubMed |
| Database_xml | – sequence: 1 dbid: NPM name: PubMed url: http://www.ncbi.nlm.nih.gov/entrez/query.fcgi?db=PubMed sourceTypes: Index Database – sequence: 2 dbid: 7X8 name: MEDLINE - Academic url: https://search.proquest.com/medline sourceTypes: Aggregation Database |
| DeliveryMethod | no_fulltext_linktorsrc |
| Discipline | Chemistry Physics |
| EISSN | 1089-7690 |
| ExternalDocumentID | 33514103 |
| Genre | Journal Article |
| GroupedDBID | --- -DZ -ET -~X 123 1UP 2-P 29K 4.4 53G 5VS 85S AAAAW AABDS AAEUA AAPUP AAYIH ABJGX ABPPZ ABZEH ACBRY ACLYJ ACNCT ACZLF ADCTM ADMLS AEJMO AENEX AFATG AFHCQ AGKCL AGLKD AGMXG AGTJO AHSDT AJJCW AJQPL ALEPV ALMA_UNASSIGNED_HOLDINGS AQWKA ATXIE AWQPM BDMKI BPZLN CS3 D-I DU5 EBS ESX F5P FDOHQ FFFMQ HAM M6X M71 M73 N9A NPM NPSNA O-B P2P RIP RNS RQS TN5 TWZ UPT WH7 YQT YZZ ~02 7X8 AAGWI |
| ID | FETCH-LOGICAL-c343t-4950941c5048df352d0f6e7a2b0c9b2ecf97dacbf75fa656cf5703b5d79e55b92 |
| IEDL.DBID | 7X8 |
| ISICitedReferencesCount | 8 |
| ISICitedReferencesURI | http://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=Summon&SrcAuth=ProQuest&DestLinkType=CitingArticles&DestApp=WOS_CPL&KeyUT=000630494800003&url=https%3A%2F%2Fcvtisr.summon.serialssolutions.com%2F%23%21%2Fsearch%3Fho%3Df%26include.ft.matches%3Dt%26l%3Dnull%26q%3D |
| ISSN | 1089-7690 |
| IngestDate | Fri Jul 11 16:58:02 EDT 2025 Wed Feb 19 02:30:02 EST 2025 |
| IsDoiOpenAccess | false |
| IsOpenAccess | true |
| IsPeerReviewed | true |
| IsScholarly | true |
| Issue | 4 |
| Language | English |
| LinkModel | DirectLink |
| MergedId | FETCHMERGED-LOGICAL-c343t-4950941c5048df352d0f6e7a2b0c9b2ecf97dacbf75fa656cf5703b5d79e55b92 |
| Notes | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ORCID | 000000027732691X 0000000234337926 0000000216985591 |
| PMID | 33514103 |
| PQID | 2483813373 |
| PQPubID | 23479 |
| ParticipantIDs | proquest_miscellaneous_2483813373 pubmed_primary_33514103 |
| PublicationCentury | 2000 |
| PublicationDate | 2021-Jan-28 20210128 |
| PublicationDateYYYYMMDD | 2021-01-28 |
| PublicationDate_xml | – month: 01 year: 2021 text: 2021-Jan-28 day: 28 |
| PublicationDecade | 2020 |
| PublicationPlace | United States |
| PublicationPlace_xml | – name: United States |
| PublicationTitle | The Journal of chemical physics |
| PublicationTitleAlternate | J Chem Phys |
| PublicationYear | 2021 |
| SSID | ssj0001724 |
| Score | 2.3972254 |
| Snippet | We study the elastic response of a stationarily driven system of a cavity field strongly coupled with molecular excitons, taking into account the main... |
| SourceID | proquest pubmed |
| SourceType | Aggregation Database Index Database |
| StartPage | 044108 |
| Title | Polariton response in the presence of Brownian dissipation from molecular vibrations |
| URI | https://www.ncbi.nlm.nih.gov/pubmed/33514103 https://www.proquest.com/docview/2483813373 |
| Volume | 154 |
| WOSCitedRecordID | wos000630494800003&url=https%3A%2F%2Fcvtisr.summon.serialssolutions.com%2F%23%21%2Fsearch%3Fho%3Df%26include.ft.matches%3Dt%26l%3Dnull%26q%3D |
| hasFullText | |
| inHoldings | 1 |
| isFullTextHit | |
| isPrint | |
| link | http://cvtisr.summon.serialssolutions.com/2.0.0/link/0/eLvHCXMwpV07T8MwELaAgmDhUV7lJSOxWnXsOI4nhCoqBqg6FNStih1b6kBSmtLfz9lJ1AkJiSVDlEiJdef7vvN3dwg9JCpRLPfqBkEtiY20JOVUk1gYZRPphAzjfD5e5WiUTqdq3CTcqkZW2e6JYaPOS-Nz5H0WpxBcOJf8cfFF_NQof7rajNDYRh0OUMZLuuR00y0cgnNcC-wVkUAD285CCe_7TAqHW-J3ZBkizPDov992jA4bbImfamM4QVu26KL9QTvSrYv2gt7TVKdoMvaUFry5wMtaJWvxvMCABvEiFCQZi0uHA0kHA8L-2L4RX2NfkYI_27G6eO0Jd7DeM_Q-fJ4MXkgzYIEYHvMVAXIE7C4yAtw4dwDFcuoSKzOmqVGaWeOUzDOjnRQuA-BnnO_XpUUulRVCK3aOdoqysJcIJyqjScYjZpWJIe5qnUce7DB4EDgj7aH7dulm8NP-VCIrbPldzTaL10MX9frPFnWnjRn3dQYR5Vd_ePsaHTCvN6ERYekN6jhwX3uLds16Na-Wd8Ey4Doav_0AmU7DXg |
| linkProvider | ProQuest |
| openUrl | ctx_ver=Z39.88-2004&ctx_enc=info%3Aofi%2Fenc%3AUTF-8&rfr_id=info%3Asid%2Fsummon.serialssolutions.com&rft_val_fmt=info%3Aofi%2Ffmt%3Akev%3Amtx%3Ajournal&rft.genre=article&rft.atitle=Polariton+response+in+the+presence+of+Brownian+dissipation+from+molecular+vibrations&rft.jtitle=The+Journal+of+chemical+physics&rft.au=Kansanen%2C+Kalle+S+U&rft.au=Toppari%2C+J+Jussi&rft.au=Heikkil%C3%A4%2C+Tero+T&rft.date=2021-01-28&rft.issn=1089-7690&rft.eissn=1089-7690&rft.volume=154&rft.issue=4&rft.spage=044108&rft_id=info:doi/10.1063%2F5.0036905&rft.externalDBID=NO_FULL_TEXT |
| thumbnail_l | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/lc.gif&issn=1089-7690&client=summon |
| thumbnail_m | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/mc.gif&issn=1089-7690&client=summon |
| thumbnail_s | http://covers-cdn.summon.serialssolutions.com/index.aspx?isbn=/sc.gif&issn=1089-7690&client=summon |