Two-Dimensional Infrared Spectroscopy of Supercooled Water
Fivos Perakis,Peter Hamm +1 more
TLDR
It is tentatively concluded that the power law provides the better physical picture to describe the dynamics of liquid water around the freezing point.Abstract:
We present two-dimensional infrared (2D IR) spectra of the OD stretch vibration of isotope diluted water (HOD/H2O) from ambient conditions (293 K) down to the metastable supercooled regime (260 K). We observe that spectral diffusion slows down from 700 fs to 2.6 ps as we lower the temperature. A comparison between measurements performed at the magic angle with those at parallel polarization shows that the 2D IR line shape is affected by the frequency-dependent anisotropy decay in the case of parallel polarization, altering the extracted correlation decay. A fit within the framework of an Arrhenius law reveals an activation energy of Ea = 6.2 ± 0.2 kcal/mol and a pre-exponential factor of 1/A = 0.02 ± 0.01 fs. Alternatively, a power law fit results in an exponent γ = 2.2 and a singularity temperature Ts = 221 K. We tentatively conclude that the power law provides the better physical picture to describe the dynamics of liquid water around the freezing point.read more
Citations
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Journal ArticleDOI
Water: A Tale of Two Liquids
Paola Gallo,Katrin Amann-Winkel,Charles Angell,Mikhail A. Anisimov,Frédéric Caupin,Charusita Chakravarty,Erik Lascaris,Thomas Loerting,Athanassios Z. Panagiotopoulos,John Russo,Jonas A. Sellberg,Harry Eugene Stanley,Hajime Tanaka,Carlos Vega,Limei Xu,Lars G. M. Pettersson +15 more
TL;DR: The behavior of water in the regime from ambient conditions to the deeply supercooled region is described and some of the possible experimental lines of research that are essential to complete a global picture that still needs to be completed.
Journal ArticleDOI
Vibrational Spectroscopy and Dynamics of Water
Fivos Perakis,Luigi De Marco,Luigi De Marco,Andrey Shalit,Fujie Tang,Zachary R. Kann,Thomas D. Kühne,Renato Torre,Mischa Bonn,Yuki Nagata +9 more
TL;DR: An overview of recent static and time-resolved vibrational spectroscopic studies of liquid water from ambient conditions to the supercooled state, as well as of crystalline and amorphous ice forms, reveals a coherent picture of water dynamics and energetics.
Journal ArticleDOI
Two-dimensional Raman-terahertz spectroscopy of water
TL;DR: The work extends multidimensional vibrational spectroscopy into the far-IR regime where thermally excited soft modes are found that are directly responsible for molecular dynamics, and can elucidate couplings and inhomogeneities of the various degrees of freedoms.
Journal ArticleDOI
Surface-Sensitive and Surface-Specific Ultrafast Two-Dimensional Vibrational Spectroscopy
Jan Philip Kraack,Peter Hamm +1 more
TL;DR: This review introduces the basic principles of the different methods of 2D vibrational spectroscopy at surfaces along with a balanced overview on the technological aspects as well as benefits and shortcomings, and discusses the current scope of applications.
Journal ArticleDOI
Collective Hydrogen Bond Reorganization in Water Studied with Temperature-Dependent Ultrafast Infrared Spectroscopy∥
TL;DR: In this paper, temperature-dependent ultrafast infrared spectroscopy of dilute HOD in H2O was used to study the picosecond reorganization of the hydrogen bond network of liquid water.
References
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Book
Concepts and Methods of 2D Infrared Spectroscopy
Peter Hamm,Martin T. Zanni +1 more
TL;DR: In this paper, the essential concepts of 2D IR spectroscopy step-by-step to build an intuitive and in-depth understanding of the method are presented. But they do not cover the design considerations for implementing the methods in the laboratory.