Low frequency 2D Raman-THz spectroscopy of ionic solution: A simulation study

Zhang, Pan; Wu, Theodore Y.; Jin, Tan; Liu, Yong; Nagata, Yuki; Zhang, Ruiting; Zhuang, Wei

doi:10.1063/1.4917260

Cited by 13 publications

(20 citation statements)

References 74 publications

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“…Poisson bracket of Equations 30-31 can also be evaluated using an equilibrium method via stability matrix: (Jeon & Cho, 2010;Mukamel, Khidekel, & Chernyak, 1996;Nagata & Mukamel, 2011;Pan et al, 2015;Saito & Ohmine, 1998…”

Section: Modeling the 2d Raman-thz Spectroscopy For The Ionic Aqueous Solutionsmentioning

confidence: 99%

“…Recently, the 2D Raman-THz spectra of a series of ionic solution had been simulated using stability matrix method (Pan et al, 2015;Pan, Zhang, & Zhuang, 2016). The 2D Raman-THz signals between the ionic solution and pure water are more distinguished and featured compared with the conventional Raman and THz spectra.…”

Section: Modeling the 2d Raman-thz Spectroscopy For The Ionic Aqueous Solutionsmentioning

confidence: 99%

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Ion effect on the dynamics of water hydrogen bonding network: A theoretical and computational spectroscopy point of view

Zhang

et al. 2018

WIREs Comput Mol Sci

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Understanding the elementary hydration dynamics of the ions and their couplings with the aqueous environments is important for researches in fields including energy, molecular biology, biomedical sciences, and chemical reactions. The concept of hydration shell is ubiquitously used to rationalize the differences of water behavior near the ions with respect to those in the bulk water. One intriguing issue, however, is to decide the spatial range of these hydration shells. Different experimental spectroscopic techniques such as the femtosecond infrared at high frequency and optical Kerr effect, dielectric relaxation, as well as terahertz measurements at low frequency often give controversial indications on this matter. As the optical transition observables provided by the spectroscopic measurements only indirectly reflect the realspace structure and dynamics information, the theoretical modeling of these signals is often desired in order to reveal the underlying physics in each of these measurements, and to understand the aforementioned apparent controversy. In this review, we outline recent progresses in the theoretical modeling of water dynamics around the ions and ionic moieties and the related vibrational spectroscopy, especially on the femtosecond infrared related single molecular water reorientation and the lowfrequency vibrational spectra related collective water dynamics. This article is categorized under: Theoretical and Physical Chemistry > Spectroscopy Theoretical and Physical Chemistry > Statistical Mechanics K E Y W O R D S hydrogen bond relaxation, ion effect, ionic solution, jump reorientation, molecular dynamic simulation, nonlinear spectroscopy

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Section: Modeling the 2d Raman-thz Spectroscopy For The Ionic Aqueous Solutionsmentioning

confidence: 99%

Section: Modeling the 2d Raman-thz Spectroscopy For The Ionic Aqueous Solutionsmentioning

confidence: 99%

Ion effect on the dynamics of water hydrogen bonding network: A theoretical and computational spectroscopy point of view

Zhang

et al. 2018

WIREs Comput Mol Sci

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“…2, we display the 2D spectra for the (i) AH, (ii) NL2, and (iii) NL3 contributions calculated using Eqs. (21)- (23). The 2D spectrum of the AH contribution exhibits positive and negative peaks labeled by "A" along the diagonal direction.…”

Section: Characteristic Features Of the 2d Spectrum In The Single-modmentioning

confidence: 99%

“…On the basis of the BO analysis, we find that the spectral peaks labeled by "H" and "I" correspond to the cross peaks of the HB-intermolecular libration and OH-stretching modes from the EAHC, which are expressed in terms of Eqs. (22) and (23) in the NL2 and NL3 cases.…”

Section: Appendix C: 2d Spectral Analysis Of Mode-mode Interactions Umentioning

confidence: 99%

“…To realize irreversible chemical reaction processes, in which energy is not conserved, interplay between the interactions among intramolecular modes and intermolecular modes is essential. [1][2][3] In numerical calculations employing classical molecular dynamics (MD) simulations, two-dimensional (2D) infrared (IR), and 2D heterodyne-detected vibrational sum frequency generation (HD-VSFG), and 2D IR surface spectra have been applied to study high-frequency intramolecular motion in bulk water, [4][5][6][7][8][9] the vapor/water interface, 9 and CO molecule on the Cu(100) surface, 10 while 2D Raman [11][12][13][14][15][16][17][18] and 2D THz-Raman [17][18][19][20][21][22][23] signals have been applied to detect low-frequency intermolecular vibrational modes. Theoretical studies of 2D spectroscopic approaches for intermolecular modes have demonstrated a capability to elucidate the difference a) Electronic mail: h.ito@kuchem.kyoto-u.ac.jp b) Electronic mail: tanimura@kuchem.kyoto-u.ac.jp between homogeneous and inhomogeneous broadening, [24][25][26][27] the anharmonicity of the potential, [28][29][30] and the modemode coupling mechanism.…”

Section: Introductionmentioning

confidence: 99%

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Simulating two-dimensional infrared-Raman and Raman spectroscopies for intermolecular and intramolecular modes of liquid water

Ito

Tanimura

2016

The Journal of Chemical Physics

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Full classical molecular dynamics (MD) simulations of two-dimensional (2D) infrared-Raman and 2D Raman spectroscopies of liquid water were carried out to elucidate a mode-mode coupling mechanism using a polarizable water model for intermolecular and intramolecular vibrational spectroscopy (POLI2VS). This model is capable of describing both infrared and Raman spectra. Second-order response functions, which consist of one molecular polarizability and two molecular dipole moments for 2D IR-Raman and three molecular polarizabilities for 2D Raman spectroscopies, were calculated using an equilibrium-non-equilibrium hybrid MD approach. The obtained signals were analyzed using a multi-mode Brownian oscillator (BO) model with nonlinear system-bath interactions representing the intramolecular OH stretching, intramolecular HOH bending, hydrogen bonded (HB)-intermolecular librational motion and HB-intermolecular vibrational (translational) motion of liquid water. This model was applied through use of hierarchal Fokker-Planck equations. The qualitative features of the peak profiles in the 2D spectra obtained from the MD simulations are accurately reproduced with the BO model. This indicates that this model captures the essential features of the intermolecular and intramolecular motion. We elucidate the mechanisms governing the 2D signal profiles involving anharmonic mode-mode coupling, the nonlinearities of the polarizability and dipole moment, and the vibrational dephasing processes of liquid water even in the case that the 2D spectral peaks obtained from the MD simulation overlap or are unclear. The mode coupling peaks caused by electrical anharmonic coupling (EAHC) and mechanical anharmonic coupling (MAHC) are observed in all of the 2D spectra. We find that the strength of the MAHC between the OH-stretching and HB-intermolecular vibrational modes is comparable to that between the OH-stretching and HOH bending modes. Moreover, we find that this OH-stretching and HB-intermolecular vibrational coupling should be observed as off-diagonal cross peaks in the 2D spectra.

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Full molecular dynamics simulations of liquid water and carbon tetrachloride for two-dimensional Raman spectroscopy in the frequency domain

Ito

Tanimura

2016

Chemical Physics

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Frequency-domain two-dimensional Raman signals, which are equivalent to coherent two-dimensional Raman scattering (COTRAS) signals, for liquid water and carbon tetrachloride were calculated using an equilibrium-nonequilibrium hybrid MD simulation algorithm. We elucidate mechanisms governing the 2D signal profiles involving anharmonic mode-mode coupling and the nonlinearities of the polarizability for the intermolecular and intramolecular vibrational modes. The predicted signal profiles and intensities can be utilized to analyze recently developed single-beam 2D spectra, whose signals are generated from a coherently controlled pulse, allowing the single-beam measurement to be carried out more efficiently.

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Low frequency 2D Raman-THz spectroscopy of ionic solution: A simulation study

Cited by 13 publications

References 74 publications

Ion effect on the dynamics of water hydrogen bonding network: A theoretical and computational spectroscopy point of view

Ion effect on the dynamics of water hydrogen bonding network: A theoretical and computational spectroscopy point of view

Simulating two-dimensional infrared-Raman and Raman spectroscopies for intermolecular and intramolecular modes of liquid water

Full molecular dynamics simulations of liquid water and carbon tetrachloride for two-dimensional Raman spectroscopy in the frequency domain

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