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  1. Article ; Online: Addressing the Dark State Problem in Strongly Coupled Organic Exciton-Polariton Systems.

    Michail, Evripidis / Rashidi, Kamyar / Liu, Bin / He, Guiying / Menon, Vinod M / Sfeir, Matthew Y

    Nano letters

    2024  Volume 24, Issue 2, Page(s) 557–565

    Abstract: The manipulation of molecular excited state processes through strong coupling has attracted significant interest for its potential to provide precise control of photochemical phenomena. However, the key limiting factor for achieving this control has been ...

    Abstract The manipulation of molecular excited state processes through strong coupling has attracted significant interest for its potential to provide precise control of photochemical phenomena. However, the key limiting factor for achieving this control has been the "dark-state problem", in which photoexcitation populates long-lived reservoir states with energies and dynamics similar to those of bare excitons. Here, we use a sensitive ultrafast transient reflection method with momentum and spectral resolution to achieve the selective excitation of organic exciton-polaritons in open photonic cavities. We show that the energy dispersions of these systems allow us to avoid the parasitic effect of the reservoir states. Under phase-matching conditions, we observe the direct population and decay of polaritons on time scales of less than 100 fs and find that momentum scattering processes occur on even faster time scales. We establish that it is possible to overcome the "dark state problem" through the careful design of strongly coupled systems.
    Language English
    Publishing date 2024-01-05
    Publishing country United States
    Document type Journal Article
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/acs.nanolett.3c02984
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: Propagating Hybrid Tamm Exciton Polaritons in Organic Microcavity

    Liu, Bin / Wu, Rong / Menon, Vinod M

    Journal of physical chemistry. 2019 Oct. 11, v. 123, no. 43

    2019  

    Abstract: Strong coupling between Tamm plasmons and organic cavity polaritons is observed at room temperature. Angle-resolved reflectometry experiments unambiguously indicate the anticrossing in the dispersion relations, which is characteristic of the strong ... ...

    Abstract Strong coupling between Tamm plasmons and organic cavity polaritons is observed at room temperature. Angle-resolved reflectometry experiments unambiguously indicate the anticrossing in the dispersion relations, which is characteristic of the strong coupling regime, and the Tamm plasmon–cavity polariton hybrid states can be energetically manipulated by tuning the Tamm plasmons. The experimental data are in good agreement with calculations based on the transfer matrix method. Emission from the lower energy Tamm plasmon–cavity polariton hybrid states is observed, and the propagation property of the hybrid Tamm plasmon polariton is also studied. The real-space imaging experiments reveal that the propagation distance is larger when the Tamm plasmon and cavity polariton are strongly coupled in comparison to both the exciton of the uncoupled organic neat film and the cavity polaritons. Moreover, the propagation length of the hybrid polaritons increases as the fraction of Tamm plasmon component in the hybrid states increases.
    Keywords ambient temperature ; energy ; image analysis ; physical chemistry ; reflectometry
    Language English
    Dates of publication 2019-1011
    Size p. 26509-26515.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1932-7455
    DOI 10.1021/acs.jpcc.9b06383
    Database NAL-Catalogue (AGRICOLA)

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  3. Article ; Online: Polariton chemistry: Thinking inside the (photon) box.

    Yuen-Zhou, Joel / Menon, Vinod M

    Proceedings of the National Academy of Sciences of the United States of America

    2019  Volume 116, Issue 12, Page(s) 5214–5216

    Language English
    Publishing date 2019-03-11
    Publishing country United States
    Document type Journal Article ; Research Support, U.S. Gov't, Non-P.H.S. ; Comment
    ZDB-ID 209104-5
    ISSN 1091-6490 ; 0027-8424
    ISSN (online) 1091-6490
    ISSN 0027-8424
    DOI 10.1073/pnas.1900795116
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    In stock of ZB MED Cologne/Königswinter

    Zs.A 1148: Show issues Location:
    Je nach Verfügbarkeit (siehe Angabe bei Bestand)
    bis Jg. 1994: Bestellungen von Artikeln über das Online-Bestellformular
    Jg. 1995 - 2021: Lesesall (1.OG)
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  4. Article ; Online: Direct Writing of Room Temperature Polariton Condensate Lattice.

    Yadav, Ravindra Kumar / Satapathy, Sitakanta / Deshmukh, Prathmesh / Datta, Biswajit / Sharma, Addhyaya / Olsson, Andrew H / Chen, Junsheng / Laursen, Bo W / Flood, Amar H / Sfeir, Matthew Y / Menon, Vinod M

    Nano letters

    2024  

    Abstract: Realizing lattices of exciton polariton condensates has been of much interest owing to the potential of such systems to realize analogue Hamiltonian simulators and physical computing architectures. Here, we report the realization of a room temperature ... ...

    Abstract Realizing lattices of exciton polariton condensates has been of much interest owing to the potential of such systems to realize analogue Hamiltonian simulators and physical computing architectures. Here, we report the realization of a room temperature polariton condensate lattice using a direct-write approach. Polariton condensation is achieved in a microcavity embedded with host-guest Frenkel excitons of an organic dye (rhodamine) in a small-molecule ionic isolation lattice (SMILES). The microcavity is patterned using focused ion beam etching to realize arbitrary lattice geometries, including defect sites on demand. The band structure of the lattice and the emergence of condensation are imaged using momentum-resolved spectroscopy. The introduction of defect sites is shown to lower the condensation threshold and result in the formation of a defect band in the condensation spectrum. The present approach allows us to study periodic, quasiperiodic, and disordered polariton condensate lattices at room temperature using a direct-write approach.
    Language English
    Publishing date 2024-04-10
    Publishing country United States
    Document type Journal Article
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/acs.nanolett.4c00586
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  5. Article ; Online: Author Correction: Magneto-optics in a van der Waals magnet tuned by self-hybridized polaritons.

    Dirnberger, Florian / Quan, Jiamin / Bushati, Rezlind / Diederich, Geoffrey M / Florian, Matthias / Klein, Julian / Mosina, Kseniia / Sofer, Zdenek / Xu, Xiaodong / Kamra, Akashdeep / García-Vidal, Francisco J / Alù, Andrea / Menon, Vinod M

    Nature

    2024  

    Language English
    Publishing date 2024-05-14
    Publishing country England
    Document type Published Erratum
    ZDB-ID 120714-3
    ISSN 1476-4687 ; 0028-0836
    ISSN (online) 1476-4687
    ISSN 0028-0836
    DOI 10.1038/s41586-024-07544-4
    Database MEDical Literature Analysis and Retrieval System OnLINE

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    In stock of ZB MED Cologne/Königswinter

    Zs.A 26: Show issues Location:
    Je nach Verfügbarkeit (siehe Angabe bei Bestand)
    bis Jg. 1994: Bestellungen von Artikeln über das Online-Bestellformular
    Jg. 1995 - 2021: Lesesall (1.OG)
    ab Jg. 2022: Lesesaal (EG)
    Zs.MG 9: Show issues
    Zs.MO 244: Show issues

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  6. Book ; Online: Ultrafast Thermal Modification of Strong Coupling in an Organic Microcavity

    Liu, Bin / Menon, Vinod M. / Sfeir, Matthew Y.

    2020  

    Abstract: There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as ... ...

    Abstract There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical response can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron-phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the promise of cavity polaritons as sensitive probes of non-equilibrium phenomena.
    Keywords Condensed Matter - Materials Science ; Condensed Matter - Mesoscale and Nanoscale Physics ; Physics - Chemical Physics ; Physics - Optics
    Subject code 535
    Publishing date 2020-08-23
    Publishing country us
    Document type Book ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

    Full text online

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  7. Book ; Online: The Role of Long-lived Excitons in the Dynamics of Strongly Coupled Molecular Polaritons

    Liu, Bin / Menon, Vinod M. / Sfeir, Matthew Y.

    2020  

    Abstract: The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics due to its potential to produce customized chemical systems with tailored photophysical properties. However, before such systems ... ...

    Abstract The concept of modifying molecular dynamics in strongly coupled exciton-polariton systems is an emerging topic in photonics due to its potential to produce customized chemical systems with tailored photophysical properties. However, before such systems can be realized, it is essential to address the open questions concerning the nature and strength of electronic interactions between exciton-polaritons and localized excited states in chemical system as well as the proper way to measure such interactions. Here, we use transient optical spectroscopy to investigate dynamical interactions between exciton-polaritons, singlet excitons, and triplet excitons in a molecular singlet fission system that is strongly coupled to an optical microcavity. We identify some of the major limitations to modify molecular dynamics in the strong coupling regime. Simultaneous excitation of cavity polaritons and 'reservoir' states, defined as dark polaritons and dark excitons (e.g. triplets) from coupled molecules and excitons from uncoupled molecules, always occurs. In addition, slow conversion from reservoir states to cavity polaritons results in minimal changes to the overall population dynamics. Furthermore, we demonstrate how in addition to the usual population dynamics, transient optical measurements on microcavities reveal information pertaining to modification of the exciton-polariton transition energies due to changes in the population of molecular excited states and the exciton-photon coupling conditions. As a consequence of weak interactions between reservoir states and cavity polaritons, judicious design considerations are required to achieve modified chemical dynamics, necessitating the use of molecular systems with long excited-state lifetimes or strong coupling approaches that require a small number of molecules.
    Keywords Condensed Matter - Materials Science ; Condensed Matter - Mesoscale and Nanoscale Physics ; Physics - Optics
    Subject code 541 ; 530
    Publishing date 2020-02-22
    Publishing country us
    Document type Book ; Online
    Database BASE - Bielefeld Academic Search Engine (life sciences selection)

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  8. Article ; Online: Molecular Emission near Metal Interfaces: The Polaritonic Regime.

    Yuen-Zhou, Joel / Saikin, Semion K / Menon, Vinod M

    The journal of physical chemistry letters

    2018  Volume 9, Issue 22, Page(s) 6511–6516

    Abstract: The strong coupling of a dense layer of molecular excitons with surface-plasmon modes in a metal gives rise to polaritons (hybrid light-matter states) called plexcitons. Surface plasmons cannot directly emit into (or be excited by) free-space photons due ...

    Abstract The strong coupling of a dense layer of molecular excitons with surface-plasmon modes in a metal gives rise to polaritons (hybrid light-matter states) called plexcitons. Surface plasmons cannot directly emit into (or be excited by) free-space photons due to the fact that energy and momentum conservation cannot be simultaneously satisfied in photoluminescence. Most plexcitons are also formally nonemissive, even though they can radiate via molecules upon localization due to disorder and decoherence. However, a fraction of them are bright even in the presence of such deleterious processes. In this Letter, we theoretically discuss the superradiant emission properties of these bright plexcitons, which belong to the upper energy branch and reveal huge photoluminescence enhancements compared to bare excitons, due to near-divergences in the density of photonic modes available to them. Our study generalizes the well-known problem of molecular emission next to a metal interface to the polaritonic regime.
    Language English
    Publishing date 2018-11-02
    Publishing country United States
    Document type Journal Article
    ISSN 1948-7185
    ISSN (online) 1948-7185
    DOI 10.1021/acs.jpclett.8b02980
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  9. Article ; Online: Spin-correlated exciton-polaritons in a van der Waals magnet.

    Dirnberger, Florian / Bushati, Rezlind / Datta, Biswajit / Kumar, Ajesh / MacDonald, Allan H / Baldini, Edoardo / Menon, Vinod M

    Nature nanotechnology

    2022  Volume 17, Issue 10, Page(s) 1060–1064

    Abstract: Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum ... ...

    Abstract Strong coupling between light and elementary excitations is emerging as a powerful tool to engineer the properties of solid-state systems. Spin-correlated excitations that couple strongly to optical cavities promise control over collective quantum phenomena such as magnetic phase transitions, but their suitable electronic resonances are yet to be found. Here, we report strong light-matter coupling in NiPS
    Language English
    Publishing date 2022-09-12
    Publishing country England
    Document type Journal Article
    ZDB-ID 2254964-X
    ISSN 1748-3395 ; 1748-3387
    ISSN (online) 1748-3395
    ISSN 1748-3387
    DOI 10.1038/s41565-022-01204-2
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  10. Article ; Online: Highly nonlinear dipolar exciton-polaritons in bilayer MoS

    Datta, Biswajit / Khatoniar, Mandeep / Deshmukh, Prathmesh / Thouin, Félix / Bushati, Rezlind / De Liberato, Simone / Cohen, Stephane Kena / Menon, Vinod M

    Nature communications

    2022  Volume 13, Issue 1, Page(s) 6341

    Abstract: Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in ... ...

    Abstract Realizing nonlinear optical response in the low photon density limit in solid-state systems has been a long-standing challenge. Semiconductor microcavities in the strong coupling regime hosting exciton-polaritons have emerged as attractive candidates in this context. However, the weak interaction between these quasiparticles has been a hurdle in this quest. Dipolar excitons provide an attractive strategy to overcome this limitation but are often hindered by their weak oscillator strength. The interlayer dipolar excitons in naturally occurring homobilayer MoS
    Language English
    Publishing date 2022-10-25
    Publishing country England
    Document type Journal Article
    ZDB-ID 2553671-0
    ISSN 2041-1723 ; 2041-1723
    ISSN (online) 2041-1723
    ISSN 2041-1723
    DOI 10.1038/s41467-022-33940-3
    Database MEDical Literature Analysis and Retrieval System OnLINE

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