Validity of Förster Theory for Vibrational Energy Transfer in Low-Dimensional Water

Yang, Mino

doi:10.1021/acs.jpcb.5b10371

Cited by 3 publications

(2 citation statements)

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“…As shown recently, for Förster transfer at an interface, the original Förster model has to be modified from a spherical to a hemispherical geometry, as shown here where S 0 is the initial slope, N A is Avogadro’s constant, and r 0 is the Förster radius, that is, the distance at which the energy transfer occurs with 50% efficiency within a vibrational lifetime. Excluded volume effects are not considered here . Here, we use the Förster radius r 0 of 2.1 Å with a corresponding time period τ 1 of 1.7 ps previously determined for bulk D 2 O .…”

Section: Resultsmentioning

confidence: 99%

“…Excluded volume effects are not considered here. 48 Here, we use the Forster radius r 0 of 2.1 Å 47 with a corresponding time period τ 1 of 1.7 ps previously determined for bulk D 2 O. 8 The concentration of O−D oscillators, C O−D , is 110.6 mol −1 for pure D 2 O 47 and 55.3 and 33.18 mol −1 for the isotopic dilutions H 2 O/HOD/D 2 O = 1:2:1 and 5:4:1, respectively.…”

Section: ■ Experimental Methodsmentioning

confidence: 99%

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Water in Contact with a Cationic Lipid Exhibits Bulklike Vibrational Dynamics

et al. 2016

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Water in contact with lipids is an important aspect of most biological systems and has been termed "biological water". We used time-resolved infrared spectroscopy to investigate the vibrational dynamics of lipid-bound water molecules, to shed more light on the properties of these important molecules. We studied water in contact with a positively charged lipid monolayer using surface-specific two-dimensional sum frequency generation vibrational spectroscopy with subpicosecond time resolution. The dynamics of the O-D stretch vibration was measured for both pure DO and isotopically diluted DO under a monolayer of 1,2-dipalmitoyl-3-trimethylammonium-propane. It was found that the lifetime of the stretch vibration depends on the excitation frequency and that efficient energy transfer occurs between the interfacial water molecules. The spectral diffusion and vibrational relaxation of the stretch vibration were successfully explained with a simple model, taking into account the Förster transfer between stretch vibrations and vibrational relaxation via the bend overtone. These observations are very similar to those made for bulk water and as such lead us to conclude that water at a positively charged lipid interface behaves similarly to bulk water. This contrasts the behavior of water in contact with negative or zwitterionic lipids and can be understood by noting that for cationic lipids the charge-induced alignment of water molecules results in interfacial water molecules with O-D groups pointing toward the bulk.

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Section: Resultsmentioning

confidence: 99%

Section: ■ Experimental Methodsmentioning

confidence: 99%

Water in Contact with a Cationic Lipid Exhibits Bulklike Vibrational Dynamics

et al. 2016

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Theoretical study of vibrational energy transfer of free OH groups at the water-air interface

Zheng

Wei

Sun

et al. 2016

The Journal of Chemical Physics

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Recent experimental studies have shown that the vibrational dynamics of free OH groups at the water-air interface is significantly different from that in bulk water. In this work, by performing molecular dynamics simulations and mixed quantum/classical calculations, we investigate different vibrational energy transfer pathways of free OH groups at the water-air interface. The calculated intramolecular vibrational energy transfer rate constant and the free OH bond reorientation time scale agree well with the experiment. It is also found that, due to the small intermolecular vibrational couplings, the intermolecular vibrational energy transfer pathway that is very important in bulk water plays a much less significant role in the vibrational energy relaxation of the free OH groups at the water-air interface.

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Dimension of discrete variable representation for mixed quantum/classical computation of three lowest vibrational states of OH stretching in liquid water

Jeon

Yang

2017

The Journal of Chemical Physics

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Three low-lying vibrational states of molecular systems are responsible for the signals of linear and third-order nonlinear vibrational spectroscopies. Theoretical studies based on mixed quantum/classical calculations provide a powerful way to analyze those experiments. A statistically meaningful result can be obtained from the calculations by solving the vibrational Schrödinger equation over many numbers of molecular configurations. The discrete variable representation (DVR) method is a useful technique to calculate vibrational eigenstates subject to an arbitrary anharmonic potential surface. Considering the large number of molecular configurations over which the DVR calculations are repeated, the calculations are desired to be optimized in balance between the cost and accuracy. We determine a dimension of the DVR method which appears to be optimum for the calculations of the three states of molecular vibrations with anharmonic strengths often found in realistic molecular systems. We apply the numerical technique to calculate the local OH stretching frequencies of liquid water, which are well known to be widely distributed due to the inhomogeneity in molecular configuration, and found that the frequencies of the 0-1 and 1-2 transitions are highly correlated. An empirical relation between the two frequencies is suggested and compared with the experimental data of nonlinear IR spectroscopies.

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Validity of Förster Theory for Vibrational Energy Transfer in Low-Dimensional Water

Cited by 3 publications

References 56 publications

Water in Contact with a Cationic Lipid Exhibits Bulklike Vibrational Dynamics

Water in Contact with a Cationic Lipid Exhibits Bulklike Vibrational Dynamics

Theoretical study of vibrational energy transfer of free OH groups at the water-air interface

Dimension of discrete variable representation for mixed quantum/classical computation of three lowest vibrational states of OH stretching in liquid water

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