Long-wavelength fluctuations and anomalous dynamics in 2-dimensional liquids
In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature which is the divergence of the vibrational amplitude with the system size also affects disordered solids and it washes out the...
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| Published in | Proceedings of the National Academy of Sciences - PNAS Vol. 116; no. 46; pp. 22977 - 22982 |
|---|---|
| Main Authors | , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
National Academy of Sciences
12.11.2019
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0027-8424 1091-6490 1091-6490 |
| DOI | 10.1073/pnas.1909319116 |
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| Abstract | In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature which is the divergence of the vibrational amplitude with the system size also affects disordered solids and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where D ∝ τ–κ, with κ > 1. Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems. |
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| AbstractList | Long-wavelength elastic modes, which have an infinitesimal energy cost, destroy the long-range translational order of 2D solids at finite temperatures. Here we demonstrate that these long-wavelength fluctuations also influence the dynamical properties of 2D systems in their normal liquid regimes. Hence, long-wavelength fluctuations make 2- and 3D molecular particulate systems behave differently from high- to very low-temperature regimes.
In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature, which is the divergence of the vibrational amplitude with the system size, also affects disordered solids, and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime, these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient
D
and structural relaxation time
τ
, where
D
∝
τ
−
κ
, with
κ
>
1
. Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems. In 2-dimensional systems at finite temperature, long-wavelength Mermin-Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature, which is the divergence of the vibrational amplitude with the system size, also affects disordered solids, and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime, these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where [Formula: see text], with [Formula: see text] Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems.In 2-dimensional systems at finite temperature, long-wavelength Mermin-Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature, which is the divergence of the vibrational amplitude with the system size, also affects disordered solids, and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime, these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where [Formula: see text], with [Formula: see text] Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems. In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature, which is the divergence of the vibrational amplitude with the system size, also affects disordered solids, and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime, these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where D∝τ−κ, with κ>1. Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems. In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature which is the divergence of the vibrational amplitude with the system size also affects disordered solids and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where D ∝ τ–κ, with κ > 1. Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems. In 2-dimensional systems at finite temperature, long-wavelength Mermin-Wagner fluctuations prevent the existence of translational long-range order. Their dynamical signature, which is the divergence of the vibrational amplitude with the system size, also affects disordered solids, and it washes out the transient solid-like response generally exhibited by liquids cooled below their melting temperatures. Through a combined numerical and experimental investigation, here we show that long-wavelength fluctuations are also relevant at high temperature, where the liquid dynamics do not reveal a transient solid-like response. In this regime, these fluctuations induce an unusual but ubiquitous decoupling between long-time diffusion coefficient D and structural relaxation time τ, where [Formula: see text], with [Formula: see text] Long-wavelength fluctuations have a negligible influence on the relaxation dynamics only at extremely high temperatures in molecular liquids or at extremely low densities in colloidal systems. |
| Author | Li, Yan-Wei Sun, Zhao-Yan Ciamarra, Massimo Pica Mason, Thomas G. Mishra, Chandan K. Zhao, Kun Ganapathy, Rajesh |
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| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/31659051$$D View this record in MEDLINE/PubMed |
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| Cites_doi | 10.1103/PhysRevLett.68.2559 10.1017/CBO9780511813467 10.1088/0953-8984/21/3/035117 10.1103/PhysRevLett.74.1250 10.1002/jcc.23365 10.1073/pnas.1815097116 10.1002/andp.201200232 10.1002/9783527622979.ch11 10.1103/PhysRevLett.17.1133 10.1126/science.287.5453.627 10.1103/PhysRevLett.114.198302 10.1103/PhysRevLett.73.1376 10.1103/PhysRevE.68.011306 10.1038/nphys1025 10.1063/1.4792356 10.1126/sciadv.1700399 10.1038/35065704 10.1103/PhysRevLett.81.120 10.1103/PhysRevLett.63.1747 10.1038/31189 10.1088/1361-648X/aaa8b8 10.1103/PhysRevLett.110.188301 10.1103/RevModPhys.60.161 10.1103/RevModPhys.17.323 10.1103/PhysRevLett.117.245701 10.1103/PhysRevLett.121.228003 10.1038/ncomms8392 10.1103/PhysRevLett.123.265501 10.1103/PhysRevA.1.18 10.1103/PhysRevLett.115.158302 10.1142/7300 10.1073/pnas.1507897112 10.1039/C9SM00302A 10.1073/pnas.1612964114 10.1137/1010093 10.1073/pnas.1607226113 |
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| Keywords | long-wavelength fluctuations normal liquid diffusion relaxation |
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| Notes | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 14 content type line 23 Edited by Eric R. Weeks, Emory University, Atlanta, GA, and accepted by Editorial Board Member Pablo G. Debenedetti October 1, 2019 (received for review May 30, 2019) Author contributions: K.Z., T.G.M., and M.P.C. designed research; Y.-W.L., C.K.M., Z.-Y.S., and R.G. performed research; and Y.-W.L., K.Z., T.G.M., and M.P.C. wrote the paper. |
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| Snippet | In 2-dimensional systems at finite temperature, long-wavelength Mermin–Wagner fluctuations prevent the existence of translational long-range order. Their... Long-wavelength elastic modes, which have an infinitesimal energy cost, destroy the long-range translational order of 2D solids at finite temperatures. Here we... In 2-dimensional systems at finite temperature, long-wavelength Mermin-Wagner fluctuations prevent the existence of translational long-range order. Their... |
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| SubjectTerms | Decoupling Diffusion coefficient Divergence Fluctuations High temperature Liquids Long range order Physical Sciences Relaxation time Wavelength |
| Title | Long-wavelength fluctuations and anomalous dynamics in 2-dimensional liquids |
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