Importance of van der Waals interaction on structural, vibrational, and thermodynamic properties of NaCl

Marcondes, Michel L.; Wentzcovitch, Renata M.; Assali, L. V. C.

doi:10.1016/j.ssc.2018.01.008

Cited by 18 publications

(15 citation statements)

References 90 publications

(119 reference statements)

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“… 48 − 50 Both LC-ωHPBE and ωB97XD are long-range-corrected (ωB97XD additionally has added corrections for atom–atom dispersion interactions), which are required for more accurate description of van der Waals (vdw) interactions during modeling of NaCl crystals. 51 , 52 Along with these functionals, we applied the def2-TZV, def2-TZVP, and def2-TZVPD basis sets 53 , 54 to evaluate the necessity of including polarization or diffuse functions in the basis set. As the def2-TZVPD basis set is not included in the Gaussian library, the basis set parameters were extracted from the Basis Set Exchange database.…”

Section: Computational Methodologymentioning

confidence: 99%

Heterogeneous Nucleation of Butanol on NaCl: A Computational Study of Temperature, Humidity, Seed Charge, and Seed Size Effects

et al. 2021

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Using a combination of quantum chemistry and cluster size distribution dynamics, we study the heterogeneous nucleation of n -butanol and water onto sodium chloride (NaCl) 10 seeds at different butanol saturation ratios and relative humidities. We also investigate how the heterogeneous nucleation of butanol is affected by the seed size through comparing (NaCl) 5 , (NaCl) 10 , and (NaCl) 25 seeds and by seed electrical charge through comparing (Na 10 Cl 9 ) + , (NaCl) 10 , and (Na 9 Cl 10 ) − seeds. Butanol is a common working fluid for condensation particle counters used in atmospheric aerosol studies, and NaCl seeds are frequently used for calibration purposes and as model systems, for example, sea spray aerosol. In general, our simulations reproduce the experimentally observed trends for the NaCl–BuOH–H 2 O system, such as the increase of nucleation rate with relative humidity and with temperature (at constant supersaturation of butanol). Our results also provide molecular-level insights into the vapor–seed interactions driving the first steps of the heterogeneous nucleation process. The main purpose of this work is to show that theoretical studies can provide molecular understanding of initial steps of heterogeneous nucleation and that it is possible to find cost-effective yet accurate-enough combinations of methods for configurational sampling and energy evaluation to successfully model heterogeneous nucleation of multicomponent systems. In the future, we anticipate that such simulations can also be extended to chemically more complex seeds.

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Section: Computational Methodologymentioning

confidence: 99%

Heterogeneous Nucleation of Butanol on NaCl: A Computational Study of Temperature, Humidity, Seed Charge, and Seed Size Effects

et al. 2021

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“…On the other side, it should be noted that the intrinsic anharmonicity (which will be described in more details in the following discussion, Section 3.4) plays an important role in simulating the thermodynamic properties of minerals at the high-temperature conditions of the deep mantle, such as heat capacities [50,51], P-V-T Equations of State [52,53], equilibrium isotope fractionation at high-P,T condition [54,55], etc. Gillet et al [50] revealed that the anharmonic contribution to the heat capacity of anhydrous forsterite could be as large as 5.5% at 2000 K, while Qin et al [33] and Marcondes et al [56] also pointed out the anharmonic effects might be even more important when weak bonds (such as H bond) are involved.…”

Section: Introductionmentioning

confidence: 99%

In Situ Infrared Spectra for Hydrous Forsterite up to 1243 K: Hydration Effect on Thermodynamic Properties

et al. 2019

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Hydrogen substitution has significant effect on the physical properties of olivine, the most abundant mineral in the upper mantle. We collected high-temperature polarized Fourier Transform infrared (FTIR) spectra on hydrous forsterite (Mg-pure olivine) crystals, which were synthesized at 12 GPa, 1473–1673 K. The modes at 3612, 3578, 3566, 3551 cm−1 show comparable negative temperature dependence, and the magnitude of (∂vi/∂T)P decreases dramatically with frequency increasing. Whereas, the peak at 3477 cm−1, which is attributed to protonation along the O1...O2 edge on the Si tetrahedron, has a positive temperature dependence. The absorbance intensities of all these OH bands remained almost the same when quenched to room temperature. On the other hand, we also evaluate the hydration effect on the thermodynamic properties (heat capacities). For the anhydrous forsterite sample, the intrinsic anharmonicity could significantly increase the heat capacity by 5~6% when extrapolated to 2000 K. Hydration further increase such difference to ~9%, in both the cases of M-substitution or Si-substitution. Hence, hydration in olivine has significant impact on the anharmonic contribution to the thermodynamic properties, as well as Equations of State and equilibrium isotope fractionation β-factor at high-P,T conditions in the deep mantle.

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“…First, the charge redistribution could lead to a lattice reorganization that reduces strain inhomogeneity, [65,66] which would result in less inhomogeneous broadening. [67] Second, it could result from a reduction of lattice anharmonicity, which is sensitive to dispersion forces [68] that can in turn be modified by screening. [64] We can also study the time dependence of the conductivity after photoexcitation using a 2D scan, which allows us to probe the picosecond evolution of the charge redistribution.…”

Section: Peak-shift and Picosecond Charge Redistribution Dynamicsmentioning

confidence: 99%

Ultrafast Photoconductivity and Terahertz Vibrational Dynamics in Double‐Helix SnIP Nanowires

et al. 2021

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SnIP could be the first of a new class of inorganic double-helix materials. [7][8][9] With strong intra-helix covalent bonds and weak inter-helix dispersion forces, SnIP belongs to the group of newly emerging 1D van der Waals (vdW) materials with potential applications in nanoelectronics and photonics. [10][11][12][13] In contrast to the DNA structure, which consists of two equal radius helices, SnIP forms with an outer [SnI] + helix wrapping around an inner [P] − helix, as pictured in Figure 1a. SnIP crystallizes monoclinically with a unit cell containing two opposite-handed double helices so that there is no net chirality. It is composed of abundant and non-toxic elements and can grow uninhibited to cm-length needles with a low-temperature synthesis [6,14] (Sections S1 and S2, Supporting Information) or in nanotubes using vapor deposition. [15,16] Its 1.86 eV band gap, as determined by band structure calculations (Figure 1b,c) and verified experimentally (see ref.[ 6 ] and Section S3, Supporting Information), is well situated for solar absorption and photocatalytic water splitting. [8,10,15] SnIP is also an extremely soft and flexible semiconductor and is therefore a promising material for applications in flexible electronics, [6,10] where these properties are highly desirable. [17] It is predicted to have a high carrier mobility; [8] however, as-grown SnIP is highly resistive so that the current lack of doped samples has made it difficult to explore its electronic properties. [6] Moreover, despite the exciting properties and unique structure of SnIP, there have been no investigations probing its ultrafast photophysical properties.Here, we use time-resolved terahertz (THz) spectroscopy (TRTS) to study picosecond charge carrier dynamics in SnIP nanowire films, as shown in Figure 1d. TRTS, a powerful non-contact ultrafast probe, has been used extensively to probe carrier dynamics in low-dimensional materials, accelerating scientific understanding of transport mechanisms and enabling materials optimization for potential applications. [18,19] From analysis of the photoconductivity spectra, along with insight into the highly anisotropic energy landscape from density functional theory (DFT), we make the first measurement of the carrier mobility in SnIP. We find a maximum electron mobility of 280 cm 2 V −1 s −1 along the double-helix axis, an extraordinarily high mobility for a material as soft and flexible as SnIP. On Tin iodide phosphide (SnIP), an inorganic double-helix material, is a quasi-1D van der Waals semiconductor that shows promise in photocatalysis and flexible electronics. However, the understanding of the fundamental photophysics and charge transport dynamics of this new material is limited. Here, time-resolved terahertz (THz) spectroscopy is used to probe the transient photoconductivity of SnIP nanowire films and measure the carrier mobility. With insight into the highly anisotropic electronic structure from quantum chemical calculations, an electron mobility as high as 280 cm 2 V −1 s −1 along the doub...

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Importance of van der Waals interaction on structural, vibrational, and thermodynamic properties of NaCl

Cited by 18 publications

References 90 publications

Heterogeneous Nucleation of Butanol on NaCl: A Computational Study of Temperature, Humidity, Seed Charge, and Seed Size Effects

Heterogeneous Nucleation of Butanol on NaCl: A Computational Study of Temperature, Humidity, Seed Charge, and Seed Size Effects

In Situ Infrared Spectra for Hydrous Forsterite up to 1243 K: Hydration Effect on Thermodynamic Properties

Ultrafast Photoconductivity and Terahertz Vibrational Dynamics in Double‐Helix SnIP Nanowires

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