Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens

Abstract

Recent inelastic X-ray scattering (IXS) experiments on mesogens have shown 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. Moreover, 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.

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [5];  [6];  [7];  [7]; ORCiD logo [1]
+ Show Author Affiliations
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)
  2. Joint Inst. for Nuclear Research (JINR), Dubna (Russian Federation); Taras Shevchenko National Univ. of Kyiv (Ukraine); Moscow Inst. of Physics and Technology (MIPT), Moscow (Russian Federation)
  3. Volgograd State Technical Univ. (Russian Federation)
  4. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  5. Kent State Univ., Kent, OH (United States)
  6. Univ. at Albany, NY (United States)
  7. Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1566960
Grant/Contract Number:  
AC05-00OR22725; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry Letters
Additional Journal Information:
Journal Volume: 9; Journal Issue: 10; Journal ID: ISSN 1948-7185
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Bolmatov, Dima, Soloviov, Dmytro, Zav’yalov, Dmitry, Sharpnack, Lewis, Agra-Kooijman, Deña M., Kumar, Satyendra, Zhang, Jiawei, Liu, Mengkun, and Katsaras, John. Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens. United States: N. p., 2018. Web. doi:10.1021/acs.jpclett.8b00926.
Copy to clipboard
Bolmatov, Dima, Soloviov, Dmytro, Zav’yalov, Dmitry, Sharpnack, Lewis, Agra-Kooijman, Deña M., Kumar, Satyendra, Zhang, Jiawei, Liu, Mengkun, & Katsaras, John. Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens. United States. https://doi.org/10.1021/acs.jpclett.8b00926
Copy to clipboard
Bolmatov, Dima, Soloviov, Dmytro, Zav’yalov, Dmitry, Sharpnack, Lewis, Agra-Kooijman, Deña M., Kumar, Satyendra, Zhang, Jiawei, Liu, Mengkun, and Katsaras, John. Sun . "Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens". United States. https://doi.org/10.1021/acs.jpclett.8b00926. https://www.osti.gov/servlets/purl/1566960.
Copy to clipboard
@article{osti_1566960,
title = {Anomalous Nanoscale Optoacoustic Phonon Mixing in Nematic Mesogens},
author = {Bolmatov, Dima and Soloviov, Dmytro and Zav’yalov, Dmitry and Sharpnack, Lewis and Agra-Kooijman, Deña M. and Kumar, Satyendra and Zhang, Jiawei and Liu, Mengkun and Katsaras, John},
abstractNote = {Recent inelastic X-ray scattering (IXS) experiments on mesogens have shown 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. Moreover, 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.},
doi = {10.1021/acs.jpclett.8b00926},
journal = {Journal of Physical Chemistry Letters},
number = 10,
volume = 9,
place = {United States},
year = {Sun Apr 29 00:00:00 EDT 2018},
month = {Sun Apr 29 00:00:00 EDT 2018}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.jpclett.8b00926
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 8 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

New family of nematic liquid crystals for displays
journal, January 1973

  • Gray, G. W.; Harrison, K. J.; Nash, J. A.
  • Electronics Letters, Vol. 9, Issue 6
  • DOI: 10.1049/el:19730096

Characterization of a new helical smectic liquid crystal
journal, February 1989

  • Goodby, J. W.; Waugh, M. A.; Stein, S. M.
  • Nature, Vol. 337, Issue 6206
  • DOI: 10.1038/337449a0

A new molecular ordering in helical liquid crystals
journal, October 1989

  • Goodby, J. W.; Waugh, M. A.; Stein, S. M.
  • Journal of the American Chemical Society, Vol. 111, Issue 21
  • DOI: 10.1021/ja00203a009

Observations of the Liquid-Crystal Analog of the Abrikosov Phase
journal, October 1992

Biaxial Nematic Phase in Bent-Core Thermotropic Mesogens
journal, April 2004

Position-Dependent Three-Dimensional Diffusion in Nematic Liquid Crystal Monitored by Single-Particle Fluorescence Localization and Tracking
journal, April 2015

Photoinduced Micropattern Alignment of Semiconductor Nanorods with Polarized Emission in a Liquid Crystal Polymer Matrix
journal, April 2017

Sound and heat revolutions in phononics
journal, November 2013

Ballistic Phonon Penetration Depth in Amorphous Silicon Dioxide
journal, November 2017

Structural Instabilities Related to Highly Anharmonic Phonons in Halide Perovskites
journal, June 2017

  • Marronnier, Arthur; Lee, Heejae; Geffroy, Bernard
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 12
  • DOI: 10.1021/acs.jpclett.7b00807

Phonon Hydrodynamic Heat Conduction and Knudsen Minimum in Graphite
journal, December 2017

Optomechanical crystals
journal, October 2009

  • Eichenfield, Matt; Chan, Jasper; Camacho, Ryan M.
  • Nature, Vol. 462, Issue 7269, p. 78-82
  • DOI: 10.1038/nature08524

Controlling sound with acoustic metamaterials
journal, February 2016

  • Cummer, Steven A.; Christensen, Johan; Alù, Andrea
  • Nature Reviews Materials, Vol. 1, Issue 3
  • DOI: 10.1038/natrevmats.2016.1

Exploring Periodic Bicontinuous Cubic Network Structures with Complete Phononic Bandgaps
journal, September 2017

  • Hur, Kahyun; Hennig, Richard G.; Wiesner, Ulrich
  • The Journal of Physical Chemistry C, Vol. 121, Issue 40
  • DOI: 10.1021/acs.jpcc.7b07267

Engineering the Hypersonic Phononic Band Gap of Hybrid Bragg Stacks
journal, April 2012

  • Schneider, Dirk; Liaqat, Faroha; El Boudouti, El Houssaine
  • Nano Letters, Vol. 12, Issue 6
  • DOI: 10.1021/nl300982d

A new class of tunable hypersonic phononic crystals based on polymer-tethered colloids
journal, September 2015

  • Alonso-Redondo, E.; Schmitt, M.; Urbach, Z.
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms9309

Piezoelectric Nanoparticle-Assisted Wireless Neuronal Stimulation
journal, June 2015

Modulation of Low-Frequency Acoustic Vibrations in Semiconductor Nanocrystals through Choice of Surface Ligand
journal, October 2016

  • Mork, A. Jolene; Lee, Elizabeth M. Y.; Dahod, Nabeel S.
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 20
  • DOI: 10.1021/acs.jpclett.6b01659

Deep-tissue focal fluorescence imaging with digitally time-reversed ultrasound-encoded light
journal, January 2012

  • Wang, Ying Min; Judkewitz, Benjamin; DiMarzio, Charles A.
  • Nature Communications, Vol. 3, Issue 1
  • DOI: 10.1038/ncomms1925

Tuning and Switching the Hypersonic Phononic Properties of Elastic Impedance Contrast Nanocomposites
journal, May 2010

  • Sato, Akihiro; Pennec, Yan; Shingne, Nitin
  • ACS Nano, Vol. 4, Issue 6
  • DOI: 10.1021/nn100519h

Phase-Defined van der Waals Schottky Junctions with Significantly Enhanced Thermoelectric Properties
journal, June 2017

  • Wang, Qiaoming; Yang, Liangliang; Zhou, Shengwen
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 13
  • DOI: 10.1021/acs.jpclett.7b01089

Liquid-Phase Vibrational Strong Coupling
journal, March 2015

  • George, Jino; Shalabney, Atef; Hutchison, James A.
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 6
  • DOI: 10.1021/acs.jpclett.5b00204

Electrochemical THz-SERS Observation of Thiol Monolayers on Au(111) and (100) Using Nanoparticle-assisted Gap-Mode Plasmon Excitation
journal, August 2017

  • Inagaki, Motoharu; Motobayashi, Kenta; Ikeda, Katsuyoshi
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 17
  • DOI: 10.1021/acs.jpclett.7b01901

Graphene-to-Substrate Energy Transfer through Out-of-Plane Longitudinal Acoustic Phonons
journal, February 2014

  • Chen, I-Ju; Mante, Pierre-Adrien; Chang, Cheng-Kai
  • Nano Letters, Vol. 14, Issue 3
  • DOI: 10.1021/nl404297r

Strongly Coupled Quantum Heat Machines
journal, August 2015

  • Gelbwaser-Klimovsky, David; Aspuru-Guzik, Alán
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 17
  • DOI: 10.1021/acs.jpclett.5b01404

Enhancement of Friction by Water Intercalated between Graphene and Mica
journal, July 2017

  • Lee, Hyunsoo; Ko, Jae-Hyeon; Choi, Jin Sik
  • The Journal of Physical Chemistry Letters, Vol. 8, Issue 15
  • DOI: 10.1021/acs.jpclett.7b01377

Phonon Driven Floquet Matter
journal, January 2018

Dynamical Ordering of Hydrogen Molecules Induced by Heat Flux
journal, July 2017

Strong Coupling between Nanoscale Metamaterials and Phonons
journal, May 2011

  • Shelton, D. J.; Brener, I.; Ginn, J. C.
  • Nano Letters, Vol. 11, Issue 5
  • DOI: 10.1021/nl200689z

Dewetting during Terahertz Vibrations of Nanoparticles
journal, January 2018

Ballistic Phonon Transport in Holey Silicon
journal, April 2015

Revealing the Mechanism of the Viscous-to-Elastic Crossover in Liquids
journal, July 2015

  • Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry
  • The Journal of Physical Chemistry Letters, Vol. 6, Issue 15
  • DOI: 10.1021/acs.jpclett.5b01338

Hidden solidlike properties in the isotropic phase of the 8CB liquid crystal
journal, November 2013

Terasonic Excitations in 2D Gold Nanoparticle Arrays in a Water Matrix as Revealed by Atomistic Simulations
journal, August 2016

  • Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry
  • The Journal of Physical Chemistry C, Vol. 120, Issue 35
  • DOI: 10.1021/acs.jpcc.6b08250

Revealing the mechanism of passive transport in lipid bilayers via phonon-mediated nanometre-scale density fluctuations
journal, May 2016

  • Zhernenkov, Mikhail; Bolmatov, Dima; Soloviov, Dmitry
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms11575

Emergent Optical Phononic Modes upon Nanoscale Mesogenic Phase Transitions
journal, May 2017

The Structure of a Number of Nematogens
journal, March 1975

  • Leadbetter, A. J.; Richardson, R. M.; Colling, C. N.
  • Le Journal de Physique Colloques, Vol. 36, Issue C1
  • DOI: 10.1051/jphyscol:1975105

The Ultrahigh Resolution IXS Beamline of NSLS-II: Recent Advances and Scientific Opportunities
journal, March 2013

Thermally triggered phononic gaps in liquids at THz scale
journal, January 2016

  • Bolmatov, Dima; Zhernenkov, Mikhail; Zav’yalov, Dmitry
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep19469

Symmetry breaking gives rise to energy spectra of three states of matter
journal, September 2013

  • Bolmatov, Dima; Musaev, Edvard T.; Trachenko, K.
  • Scientific Reports, Vol. 3, Issue 1
  • DOI: 10.1038/srep02794

Unified phonon-based approach to the thermodynamics of solid, liquid and gas states
journal, December 2015

Low-frequency dynamics of liquid crystals
journal, April 1997

An Improved Empirical Potential Energy Function for Molecular Simulations of Phospholipids
journal, August 2000

  • Feller, Scott E.; MacKerell, Alexander D.
  • The Journal of Physical Chemistry B, Vol. 104, Issue 31
  • DOI: 10.1021/jp0007843

Towards in Silico Liquid Crystals. Realistic Transition Temperatures and Physical Properties for n -Cyanobiphenyls via Molecular Dynamics Simulations
journal, January 2009

  • Tiberio, Giustiniano; Muccioli, Luca; Berardi, Roberto
  • ChemPhysChem, Vol. 10, Issue 1
  • DOI: 10.1002/cphc.200800231

Markoff Random Processes and the Statistical Mechanics of Time‐Dependent Phenomena. II. Irreversible Processes in Fluids
journal, March 1954

  • Green, Melville S.
  • The Journal of Chemical Physics, Vol. 22, Issue 3
  • DOI: 10.1063/1.1740082

Reciprocal Relations in Irreversible Processes. I.
journal, February 1931

Part-crystalline part-liquid state and rattling-like thermal damping in materials with chemical-bond hierarchy
journal, October 2014

  • Qiu, Wujie; Xi, Lili; Wei, Ping
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 42
  • DOI: 10.1073/pnas.1410349111

Materials for terahertz science and technology
journal, September 2002

  • Ferguson, Bradley; Zhang, Xi-Cheng
  • Nature Materials, Vol. 1, Issue 1
  • DOI: 10.1038/nmat708

Terahertz-field-induced insulator-to-metal transition in vanadium dioxide metamaterial
journal, July 2012

  • Liu, Mengkun; Hwang, Harold Y.; Tao, Hu
  • Nature, Vol. 487, Issue 7407
  • DOI: 10.1038/nature11231

Ultrabroadband terahertz spectroscopy of a liquid crystal
journal, January 2012

  • Vieweg, N.; Fischer, B. M.; Reuter, M.
  • Optics Express, Vol. 20, Issue 27
  • DOI: 10.1364/OE.20.028249

The phonon theory of liquid thermodynamics
journal, May 2012

  • Bolmatov, D.; Brazhkin, V. V.; Trachenko, K.
  • Scientific Reports, Vol. 2, Issue 1
  • DOI: 10.1038/srep00421

A phonon thermodynamics approach of gold nanofluids synthesized in solution plasma
journal, March 2014

  • Heo, YongKang; Antoaneta Bratescu, Maria; Aburaya, Daiki
  • Applied Physics Letters, Vol. 104, Issue 11
  • DOI: 10.1063/1.4868872

An explanation of the Al2O3 nanofluid thermal conductivity based on the phonon theory of liquid
journal, December 2016

Size and Shape Dependence of the Vibrational Spectrum and Low-Temperature Specific Heat of Au Nanoparticles
journal, November 2013

  • Sauceda, Huziel E.; Salazar, Fernando; Pérez, Luis A.
  • The Journal of Physical Chemistry C, Vol. 117, Issue 47
  • DOI: 10.1021/jp408976f

Vibration spectroscopy of weakly interacting mesoscopic colloids
journal, January 2012

  • Mattarelli, Maurizio; Montagna, Maurizio; Still, Tim
  • Soft Matter, Vol. 8, Issue 15
  • DOI: 10.1039/c2sm07034k

Spectroscopic Imaging of Deep Tissue through Photoacoustic Detection of Molecular Vibration
journal, June 2013

  • Wang, Pu; Rajian, Justin R.; Cheng, Ji-Xin
  • The Journal of Physical Chemistry Letters, Vol. 4, Issue 13
  • DOI: 10.1021/jz400559a

An Effective Procedure for Analyzing Molecular Vibrations in Terms of Local Fragment Modes
journal, September 2016

  • Huix-Rotllant, Miquel; Ferré, Nicolas
  • Journal of Chemical Theory and Computation, Vol. 12, Issue 10
  • DOI: 10.1021/acs.jctc.6b00514

Molecular Plasmon–Phonon Coupling
journal, September 2016

Targeting a Rate-Promoting Vibration with an Allosteric Mediator in Lactate Dehydrogenase
journal, June 2016

  • Dzierlenga, Michael W.; Schwartz, Steven D.
  • The Journal of Physical Chemistry Letters, Vol. 7, Issue 13
  • DOI: 10.1021/acs.jpclett.6b01209

Cell–Extracellular Matrix Mechanobiology: Forceful Tools and Emerging Needs for Basic and Translational Research
journal, December 2017

Origin of the “Waterfall” Effect in Phonon Dispersion of Relaxor Perovskites
journal, September 2003

Mixing of Longitudinal and Transverse Dynamics in Liquid Water
journal, September 1997

Molecular dynamics simulation of short-wavelength collective dynamics of phospholipid membranes
journal, May 2014

Optical Amplification of Ligand-Receptor Binding Using Liquid Crystals
journal, March 1998

Real-Time Liquid Crystal pH Sensor for Monitoring Enzymatic Activities of Penicillinase
journal, December 2009

  • Bi, Xinyan; Hartono, Deny; Yang, Kun-Lin
  • Advanced Functional Materials, Vol. 19, Issue 23
  • DOI: 10.1002/adfm.200900823

Liquid crystal self-assembly of random-sequence DNA oligomers
journal, January 2012

  • Bellini, T.; Zanchetta, G.; Fraccia, T. P.
  • Proceedings of the National Academy of Sciences, Vol. 109, Issue 4
  • DOI: 10.1073/pnas.1117463109

Adsorbate-Induced Anchoring Transitions of Liquid Crystals on Surfaces Presenting Metal Salts with Mixed Anions
journal, February 2014

  • Hunter, Jacob T.; Abbott, Nicholas L.
  • ACS Applied Materials & Interfaces, Vol. 6, Issue 4
  • DOI: 10.1021/am404632r

Liquid-Crystal Biosensor Based on Nickel-Nanosphere-Induced Homeotropic Alignment for the Amplified Detection of Thrombin
journal, October 2015

  • Zhao, Dongyu; Peng, Yi; Xu, Lihong
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 42
  • DOI: 10.1021/acsami.5b08924

Molecular Modeling of Liquid Crystal/Phospholipid Interface as a Label-Free Biosensor
journal, February 2017

Molecular dynamics investigations of an indicator displacement assay mechanism in a liquid crystal sensor
journal, January 2017

  • Liu, Qingyu; Zuo, Fang; Zhao, Zhigang
  • Physical Chemistry Chemical Physics, Vol. 19, Issue 35
  • DOI: 10.1039/C7CP02292A

Cholesteric Liquid Crystal Droplets for Biosensors
journal, September 2016

  • Lee, Hyun-Gyu; Munir, Sundas; Park, Soo-Young
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 39
  • DOI: 10.1021/acsami.6b09624

Liquid-Crystal-Based Biosensor without Alignment Substrate
journal, January 2014

    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    The Mixing of Polarizations in the Acoustic Excitations of Disordered Media With Local Isotropy
    journal, October 2018

    The mixing of polarizations in the acoustic excitations of disordered media with local isotropy
    text, January 2017

      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: