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Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens
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    Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens
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    • Dima Bolmatov*
      Dima Bolmatov
      Neutron Scattering Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      Department of Physics and Astronomy, University of Tennessee, Knoxville, Tennessee 37996, United States
      *E-mail: [email protected], [email protected]
    • Dmytro Soloviov
      Dmytro Soloviov
      Frank Laboratory of Neutron Physics, Joint Institute for Nuclear Research, Dubna 141980, Russia
      Taras Shevchenko National University of Kyiv, Kyiv 01033, Ukraine
      Moscow Institute of Physics and Technology, Dolgoprudny 141701, Russia
    • Dmitry Zav’yalov
      Dmitry Zav’yalov
      Volgograd State Technical University, Volgograd 400005, Russia
    • Lewis Sharpnack
      Lewis Sharpnack
      European Synchrotron Radiation Facility, Grenoble 38043, France
    • Deña M. Agra-Kooijman
      Deña M. Agra-Kooijman
      Liquid Crystal Institute, Kent State University, Kent, Ohio 44242, United States
    • Satyendra Kumar
      Satyendra Kumar
      Division of Research and Department of Physics, University at Albany, Albany, New York 12222, United States
    • Jiawei Zhang
      Jiawei Zhang
      Department of Physics and Astronomy, Stony Brook University, Stony Brook, New York 11794, United States
      More by Jiawei Zhang
    • Mengkun Liu
      Mengkun Liu
      Department of Physics and Astronomy, Stony Brook University, Stony Brook, New York 11794, United States
      More by Mengkun Liu
    • John Katsaras
      John Katsaras
      Neutron Scattering Directorate, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
      Department of Physics and Astronomy, University of Tennessee, Knoxville, Tennessee 37996, United States
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2018, 9, 10, 2546–2553
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.8b00926
    Published April 29, 2018
    Copyright © 2018 American Chemical Society

    Abstract

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    Recent inelastic X-ray scattering (IXS) experiments on mesogens have revealed entirely new capabilities with regards to their nanoscale phonon-assisted heat management. Mesogens such as nematic liquid crystals (LCs) are appealing systems for study because their structure and morphology can easily be tuned. We report on Q-resolved ultra-high-resolution IXS, X-ray diffraction, and THz time-domain spectroscopy experiments combined with large-scale all-atom molecular dynamics simulations on the dynamic properties of 5CB LCs. For the first time, we observe a strong mixing of phonon excitations originating from independent in-phase and out-of-phase van-der-Waals-mediated displacement patterns. The coexistence of transverse acoustic and optical modes of 5CB LCs at near room temperature is revealed through the emergent transverse phonon gap and THz light–phonon coupling taking place within the same energy range. Furthermore, our experimental observations are supported by analysis showing correlations of spontaneous fluctuations of LCs on picosecond time scales. These findings are significant for the design of a new generation of soft molecular vibration-sensitive nanoacoustic and optomechanical applications.

    Copyright © 2018 American Chemical Society

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    Cited By

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    This article is cited by 13 publications.

    1. Dima Bolmatov. The Phonon Theory of Liquids and Biological Fluids: Developments and Applications. The Journal of Physical Chemistry Letters 2022, 13 (31) , 7121-7129. https://doi.org/10.1021/acs.jpclett.2c01779
    2. Dima Bolmatov, Dmytro Soloviov, Mikhail Zhernenkov, Dmitry Zav’yalov, Eugene Mamontov, Alexey Suvorov, Yong Q. Cai, John Katsaras. Molecular Picture of the Transient Nature of Lipid Rafts. Langmuir 2020, 36 (18) , 4887-4896. https://doi.org/10.1021/acs.langmuir.0c00125
    3. Dima Bolmatov, Qi Zhang, Dmytro Soloviov, Yuk Mun Li, Jörg G. Werner, Alexey Suvorov, Yong Q. Cai, Ulrich Wiesner, Mikhail Zhernenkov, John Katsaras. Nanoscale Q-Resolved Phonon Dynamics in Block Copolymers. ACS Applied Nano Materials 2018, 1 (9) , 4918-4926. https://doi.org/10.1021/acsanm.8b01087
    4. James E. Fitzgerald, Dmytro Soloviov, Yong Q. Cai, Frederick A. Heberle, Daisuke Ishikawa, Alfred Q.R. Baron, Dima Bolmatov, Mikhail Zhernenkov, Edward R. Lyman. Phonons reveal coupled cholesterol-lipid dynamics in ternary membranes. Biophysical Journal 2024, 175 https://doi.org/10.1016/j.bpj.2024.10.017
    5. S. T. Lynch, A. De Francesco, L. Scaccia, A. Suvorov, Y. Q. Cai, D. M. Agra-Kooijman, L. L. Sharpnack, Satyendra Kumar, A. Cunsolo. Shear wave propagation in a liquid crystal: An inelastic X-ray scattering study. The Journal of Chemical Physics 2024, 160 (23) https://doi.org/10.1063/5.0212229
    6. Yanyun Lin, Xingjuan Wu, Kaicheng Wang, Sen Shang, Yubin Gong, Hongwei Zhao, Dai Wu, Peng Zhang, Xiaoyun Lu. Spectral Characteristics and Functional Responses of Phospholipid Bilayers in the Terahertz Band. International Journal of Molecular Sciences 2023, 24 (8) , 7111. https://doi.org/10.3390/ijms24087111
    7. Dima Bolmatov, C. Patrick Collier, Dmitry Zav’yalov, Takeshi Egami, John Katsaras. Real Space and Time Imaging of Collective Headgroup Dipole Motions in Zwitterionic Lipid Bilayers. Membranes 2023, 13 (4) , 442. https://doi.org/10.3390/membranes13040442
    8. Jacob J. Kinnun, Haden L. Scott, Dima Bolmatov, C. Patrick Collier, Timothy R. Charlton, John Katsaras. Biophysical studies of lipid nanodomains using different physical characterization techniques. Biophysical Journal 2023, 122 (6) , 931-949. https://doi.org/10.1016/j.bpj.2023.01.024
    9. Ahlam Nemati, Lara Querciagrossa, Corinne Callison, Sasan Shadpour, Diana P. Nunes Gonçalves, Taizo Mori, Ximin Cui, Ruoqi Ai, Jianfang Wang, Claudio Zannoni, Torsten Hegmann. Effects of shape and solute-solvent compatibility on the efficacy of chirality transfer: Nanoshapes in nematics. Science Advances 2022, 8 (4) https://doi.org/10.1126/sciadv.abl4385
    10. M. G. Izzo, B. Wehinger, S. Cazzato, A. Matic, C. Masciovecchio, A. Gessini, G. Ruocco. Rayleigh scattering and disorder-induced mixing of polarizations in amorphous solids at the nanoscale: 1-octyl-3-methylimidazolium chloride glass. Physical Review B 2020, 102 (21) https://doi.org/10.1103/PhysRevB.102.214309
    11. Dima Bolmatov, Jacob J. Kinnun, John Katsaras, Maxim O. Lavrentovich. Phonon-mediated lipid raft formation in biological membranes. Chemistry and Physics of Lipids 2020, 232 , 104979. https://doi.org/10.1016/j.chemphyslip.2020.104979
    12. Dima Bolmatov, Yong Q. Cai, Dmitry Zav’yalov, Mikhail Zhernenkov. Crossover from picosecond collective to single particle dynamics defines the mechanism of lateral lipid diffusion. Biochimica et Biophysica Acta (BBA) - Biomembranes 2018, 1860 (11) , 2446-2455. https://doi.org/10.1016/j.bbamem.2018.07.004
    13. Maria G. Izzo, Giancarlo Ruocco, Stefano Cazzato. The Mixing of Polarizations in the Acoustic Excitations of Disordered Media With Local Isotropy. Frontiers in Physics 2018, 6 https://doi.org/10.3389/fphy.2018.00108

    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2018, 9, 10, 2546–2553
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.8b00926
    Published April 29, 2018
    Copyright © 2018 American Chemical Society

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