
1.Beijing Key Laboratory for Precision Optoelectronic Measurement Instrument and Technology, School of Optics and Photonics, Beijing Institute of Technology, Beijing 100081, China
2.Beijing Advanced Innovation Center for Imaging Technology and Key Laboratory of Terahertz Optoelectronics (MoE), Department of Physics, Capital Normal University, Beijing 100048, China
3.Shenzhen Institutes of Advanced Technology, Chinese Academy of Sciences, Shenzhen 518055, China
4.The Institute of Optics, University of Rochester, Rochester, NY 14627, USA
Liangliang Zhang (zhlliang@126.com)
Yuejin Zhao (yjzhao@bit.edu.cn)
Published:2020,
Published Online:04 August 2020,
Received:23 September 2019,
Revised:04 July 2020,
Accepted:13 July 2020
Scan QR Code
Zhao, H. et al. Ultrafast hydrogen bond dynamics of liquid water revealed by terahertz-induced transient birefringence. Light: Science & Applications, 9, 1349-1358 (2020).
Zhao, H. et al. Ultrafast hydrogen bond dynamics of liquid water revealed by terahertz-induced transient birefringence. Light: Science & Applications, 9, 1349-1358 (2020). DOI: 10.1038/s41377-020-00370-z.
The fundamental properties of water molecules
such as their molecular polarizability
have not yet been clarified. The hydrogen bond network is generally considered to play an important role in the thermodynamic properties of water. The terahertz (THz) Kerr effect technique
as a novel tool
is expected to be useful in exploring the low-frequency molecular dynamics of liquid water. Here
we use an intense and ultrabroadband THz pulse (peak electric field strength of 14.9 MV/cm
centre frequency of 3.9 THz
and bandwidth of 1–10 THz) to resonantly excite intermolecular modes of liquid water. Bipolar THz field-induced transient birefringence signals are observed in a free-flowing water film. We propose a hydrogen bond harmonic oscillator model associated with the dielectric susceptibility and combine it with the Lorentz dynamic equation to investigate the intermolecular structure and dynamics of liquid water. We mainly decompose the bipolar signals into a positive signal caused by hydrogen bond stretching vibration and a negative signal caused by hydrogen bond bending vibration
indicating that the polarizability perturbation of water presents competing contributions under bending and stretching conditions. A Kerr coefficient equation related to the intermolecular modes of water is established. The ultrafast intermolecular hydrogen bond dynamics of water revealed by an ultrabroadband THz pump pulse can provide further insights into the transient structure of liquid water corresponding to the pertinent modes.
Cisneros, G. A. et al. Modeling molecular interactions in water: from pairwise to many-body potential energy functions.Chem. Rev.116, 7501–7528 (2016)..
Bellissent-Funel, M. C. et al. Water determines the structure and dynamics of proteins.Chem. Rev.116, 7673–7697 (2016)..
Omta, A. W. et al. Negligible effect of ions on the hydrogen-bond structure in liquid water.Science301, 347–349 (2003)..
Fecko, C. J. et al. Ultrafast hydrogen-bond dynamics in the infrared spectroscopy of water.Science301, 1698–1702 (2003)..
Smith, J. D. et al. Energetics of hydrogen bond network rearrangements in liquid water.Science306, 851–853 (2004)..
Stiopkin, I. V. et al. Hydrogen bonding at the water surface revealed by isotopic dilution spectroscopy.Nature474, 192–195 (2011)..
Richardson, J. O. et al. Concerted hydrogen-bond breaking by quantum tunneling in thewater hexamer prism.Science351, 1310–1313 (2016)..
Stokely, K. et al. Effect of hydrogen bond cooperativity on the behavior of water.Proc. Natl Acad. Sci. USA107, 1301–1306 (2010)..
Sharma, M., Resta, R.&Car, R. Intermolecular dynamical charge fluctuations in water: a signature of the H-bond network.Phys. Rev. Lett.95, 187401 (2005)..
Heyden, M.&Tobias, D. J. Spatial dependence of protein-water collective hydrogen-bond dynamics.Phys. Rev. Lett.111, 218101 (2013)..
Bakker, H. J.&Skinner, J. L. Vibrational spectroscopy as a probe of structure and dynamics in liquid water.Chem. Rev.110, 1498–1517 (2010)..
Perakis, F. et al. Vibrational spectroscopy and dynamics of water.Chem. Rev.116, 7590–7607 (2016)..
Vij, J. K., Simpson, D. R. J.&Panarina, O. E. Far infrared spectroscopy of water at different temperatures: GHz to THz dielectric spectroscopy of water.J. Mol. Liq.112, 125–135 (2004)..
Torii, H. Intermolecular electron density modulations in water and their effects on the far-infrared spectral profiles at 6 THz.J. Phys. Chem. B115, 6636–6643 (2011)..
Mizoguchi, K., Hori, Y.&Tominaga, Y. Study on dynamical structure in water and heavy water by low-frequency Raman spectroscopy.J. Chem. Phys.97, 1961–1968 (1992)..
Fukasawa, T. et al. Relation between dielectric and low-frequency Raman spectra of hydrogen-bond liquids.Phys. Rev. Lett.95, 197802 (2005)..
Rønne, C.&Keiding, S. R. Low frequency spectroscopy of liquid water using THz-time domain spectroscopy.J. Mol. Liq.101, 199–218 (2002)..
Penkov, N. et al. Terahertz spectroscopy applied for investigation of water structure.J. Phys. Chem. B119, 12664–12670 (2015)..
Savolainen, J., Ahmed, S.&Hamm, P. Two-dimensional Raman-terahertz spectroscopy of water.Proc. Natl Acad. Sci. USA110, 20402–20407 (2013)..
Torre, R., Bartolini, P.&Righini, R. Structural relaxation in supercooled water by time-resolved spectroscopy.Nature428, 296–299 (2004)..
Turton, D. A.&Wynne, K. Structural relaxation in the hydrogen-bonding liquids N-methylacetamide and water studied by optical Kerr effect spectroscopy.J. Chem. Phys.128, 154516 (2008)..
Taschin, A. et al. Evidence of two distinct local structures of water from ambient to supercooled conditions.Nat. Commun.4, 2401 (2013)..
Winkler, K., Lindner, J.&Vöhringer, P. Low-frequency depolarized Raman-spectral density of liquid water from femtosecond optical Kerr-effect measurements: lineshape analysis of restricted translational modes.Phys. Chem. Chem. Phys.4, 2144–2155 (2002)..
Sajadi, M., Wolf, M.&Kampfrath, T. Transient birefringence of liquids induced by terahertz electric-field torque on permanent molecular dipoles.Nat. Commun.8, 14963 (2017)..
Freysz, E.&Degert, J. Nonlinear optics: terahertz Kerr effect.Nat. Photon.4, 131–132 (2010)..
Finneran, I. A. et al. Coherent two-dimensional terahertz-terahertz-Raman spectroscopy.Proc. Natl Acad. Sci. USA113, 6857–6861 (2016)..
Kampfrath, T. et al. The nature of the dielectric response of methanol revealed by the terahertz Kerr effect.J. Phys. Chem. Lett.9, 1279–1283 (2018)..
Hoffmann, M. C. et al. Terahertz kerr effect.Appl. Phys. Lett.95, 231105 (2009)..
Bodrov, S. et al. Terahertz induced optical birefringence in polar and nonpolar liquids.J. Chem. Phys.147, 084507 (2017)..
Allodi, M. A., Finneran, I. A.&Blake, G. A. Nonlinear terahertz coherent excitation of vibrational modes of liquids.J. Chem. Phys.143, 234204 (2015)..
Kampfrath, T., Wolf, M.&Sajadi, M. Anharmonic coupling between intermolecular motions of water revealed by terahertz Kerr effect. Preprint athttps://arxiv.org/abs/1707.07622https://arxiv.org/abs/1707.07622(2017).
Zalden, P. et al. Molecular polarizability anisotropy of liquid water revealed by terahertz-induced transient orientation.Nat. Commun.9, 2142 (2018)..
Novelli, F. et al. Strong anisotropy in liquid water upon librational excitation using terahertz laser fields. Preprint athttps://arxiv.org/abs/1809.04261https://arxiv.org/abs/1809.04261(2018).
Zasetsky, A. Y. Dielectric relaxation in liquid water: two fractions or two dynamics?Phys. Rev. Lett.107, 117601 (2011)..
Hale, G. M.&Querry, M. R. Optical constants of water in the 200-nm to 200-µm wavelength region.Appl. Opt.12, 555–563 (1973)..
Afsar, M. N.&Hasted, J. B. Measurements of the optical constants of liquid H2O and D2O between 6 and 450 cm−1.J. Opt. Soc. Am.67, 902–904 (1977)..
Maroulis, G. Hyperpolarizability of H2O revisited: accurate estimate of the basis set limit and the size of electron correlation effects.Chem. Phys. Lett.289, 403–411 (1998)..
Kalmykov, Y. P. Matrix method calculation of the Kerr effect transient and ac stationary responses of arbitrary shaped macromolecules.J. Chem. Phys.131, 074107 (2009)..
Coffey, W. T.&Kalmykov, Y. P.The Langevin Equation. 3rd edn. (World Scientific Publishing Company, Singapore City, 2012).
Boyd, R. W.Nonlinear Optics. 2nd edn (Elsevier, Amsterdam, 2003).
Demtröder, W.Laser Spectroscopy: Vol. 2 Experimental Techniques.(Springer, Berlin, Heidelberg, 2008).
Levenson, M.Introduction to Nonlinear Laser Spectroscopy.(Elsevier, Amsterdam, 2012).
Sekino, H.&Bartlett, R. J. Molecular hyperpolarizabilities.J. Chem. Phys.98, 3022–3037 (1993)..
Palese, S. et al. Femtosecond optical Kerr effect studies of water.J. Phys. Chem.98, 6308–6316 (1994)..
Shalaby, M., Vicario, C.&Hauri, C. P. Extreme nonlinear terahertz electro-optics in diamond for ultrafast pulse switching.APL Photon.2, 036106 (2017)..
Sajadi, M., Wolf, M.&Kampfrath, T. Terahertz-field-induced optical birefringence in common window and substrate materials.Opt. Express23, 28985–28992 (2015)..
Ahmed, S., Savolainen, J.&Hamm, P. The effect of the Gouy phase in optical-pump-THz-probe spectroscopy.Opt. Express22, 4256–4266 (2014)..
Amo, Y.&Tominaga, Y. Low-frequency Raman study of ethanol–water mixture.Chem. Phys. Lett.320, 703–706 (2000)..
Fecko, C. J., Eaves, J. D.&Tokmakoff, A. Isotropic and anisotropic Raman scattering from molecular liquids measured by spatially masked optical Kerr effect spectroscopy.J. Chem. Phys.117, 1139–1154 (2002)..
Jin, Q. et al. Observation of broadband terahertz wave generation from liquid water.Appl. Phys. Lett.111, 071103 (2017)..
Gallot, G.&Grischkowsky, D. Electro-optic detection of terahertz radiation.J. Opt. Soc. Am. B16, 1204–1212 (1999)..
Leitenstorfer, A. et al. Detectors and sources for ultrabroadband electro-optic sampling: experiment and theory.Appl. Phys. Lett.74, 1516–1518 (1999)..
0
Views
0
Downloads
0
CSCD
Publicity Resources
Related Articles
Related Author
Related Institution
京公网安备11010802024621