Nonlinear Mie theory for second-harmonic and sum-frequency scattering

Beer, Alex G. F. de; Roke, Sylvie

doi:10.1103/physrevb.79.155420

Cited by 137 publications

(126 citation statements)

References 49 publications

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“…The droplet spectroscopy, pioneered by the Roke group (22)(23)(24)(25)(26), is conducted in a scattering geometry [vibrational sumfrequency scattering spectroscopy (VSFSS)], and the comparative planar surface studies (VSFS) are conducted in a total internal reflection geometry (TIR) as in previous work from this laboratory (16,18,27,28).…”

Section: Experimental Approachmentioning

confidence: 99%

“…The counterions were exchanged using previously published methods (47), with the surfactants and counterion identities verified using 1 H NMR and 23 Na NMR. Reverse nanoemulsions were made by dissolving enough M:AOT (M = Na + , K + , and Mg 2+ ) in CCl 4 to create a 1 mM AOT concentration and sonicated with a 1% aqueous phase.…”

Section: Orientation and Solvation Of The Aot Head Groupmentioning

confidence: 99%

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Molecular characterization of water and surfactant AOT at nanoemulsion surfaces

Hensel

Carpenter

Ciszewski

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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Nanoemulsions and microemulsions are environments where oil and water can be solubilized in one another to provide a unique platform for many different biological and industrial applications. Nanoemulsions, unlike microemulsions, have seen little work done to characterize molecular interactions at their surfaces. This study provides a detailed investigation of the near-surface molecular structure of regular (oil in water) and reverse (water in oil) nanoemulsions stabilized with the surfactant dioctyl sodium sulfosuccinate (AOT). Vibrational sum-frequency scattering spectroscopy (VSFSS) is used to measure the vibrational spectroscopy of these AOT stabilized regular and reverse nanoemulsions. Complementary studies of AOT adsorbed at the planar oil-water interface are conducted with vibrational sum-frequency spectroscopy (VSFS). Jointly, these give comparative insights into the orientation of interfacial water and the molecular characterization of the hydrophobic and hydrophilic regions of AOT at the different oil-water interfaces. Whereas the polar region of AOT and surrounding interfacial water molecules display nearly identical behavior at both the planar and droplet interface, there is a clear difference in hydrophobic chain ordering even when possible surface concentration differences are taken into account. This chain ordering is found to be invariant as the nanodroplets grow by Ostwald ripening and also with substitution of different counterions (Na:AOT, K:AOT, and Mg:AOT) that consequently also result in different sized nanoparticles. The results paint a compelling picture of surfactant assembly at these relatively large nanoemulsion surfaces and allow for an important comparison of AOT at smaller micellar (curved) and planar oil-water interfaces.nanoemulsions | oil-water interfaces | vibrational sum-frequency scattering spectroscopy | surface spectroscopy | surfactants W e are all familiar with the adage that "oil and water do not mix," but of course, it depends upon the definition of "mix." Emulsions are an important special case, where the oil is dispersed as tiny droplets in the aqueous phase, taxonomically called a regular emulsion, or where the water is dispersed as tiny droplets throughout the oil phase, called a reverse emulsion. Because both emulsions are thermodynamically unstable, overcoming this requires an emulsifying agent such as a surfactant. Recently, there has been interest in surfactant-stabilized emulsions with droplet diameters in the nanoscale range for unique applications in drug delivery (1, 2) and oil recovery (3, 4) and as nanoreactors to produce materials ranging from polymers to quantum dots (5). Regular or reverse emulsions with droplet diameters in the range of 10-1,000 nm are called nanoemulsions. Little is known about the processes or molecular structures that result in their stability via surfactants. Even less is known about the structure-function relationship, which is crucial to determine the best surfactant for a given nanoemulsion application. Their utility hinges on a ...

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Section: Experimental Approachmentioning

confidence: 99%

Section: Orientation and Solvation Of The Aot Head Groupmentioning

confidence: 99%

Molecular characterization of water and surfactant AOT at nanoemulsion surfaces

Hensel

Carpenter

Ciszewski

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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“…На настоящий момент имеется три наиболее используемых модели: модель Релея-Ганса-Дебая [8-10], модель на основе точного решения задачи о рассеянии [11,12] и модель Вентцеля-Крамерса-Бриллюэна [13]. Первая модель применима при малых размерах исследуемых систем и не учитывает рассеяние на границах раздела, однако для нее проще всего получить аналитическое решение.…”

Section: Introductionunclassified

Генерация Суммарной Частоты От Тонкого Цилиндрического Слоя

Шамына¹,

Капшай²

2018

Журнал Технической Физики

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Поступила в редакцию 03.08.2017 г.В приближении Релея-Ганса-Дебая решена задача о генерации гармоники суммарной частоты двумя плоскими эллиптически поляризованными электромагнитными волнами от поверхности диэлектрической частицы цилиндрической формы, покрытой тонким слоем, обладающим нелинейными оптическими свой-ствами. Формулы, описывающие поле суммарной частоты, представлены в тензорной и векторной формах для тензора нелинейной диэлектрической восприимчивости второго порядка, выбранного в общем виде, содержащем киральные компоненты. Получены выражения, описывающие поле суммарной частоты от торцов цилиндрической частицы, для случая нелинейного слоя, обладающего киральными свойствами. Трехмерные диаграммы направленности излучения суммарной частоты проанализированы для различных комбинаций параметров (углы падения, степени эллиптичности, ориентация эллипсов поляризации, размеры цилиндрической частицы). Обнаружены математические свойства функций пространственного распределения поля суммарной частоты, характеризующие симметрию диаграмм направленности. ВведениеРост интереса к нелинейным оптическим эффектам второго порядка от поверхностей не прекращается на протяжении последних 20 лет. Это объясняется тем, что в дипольной модели, широко используемой в элек-тродинамике, такие эффекты в объеме центросиммет-ричных сред запрещены. Однако их можно наблюдать на границах раздела сред и в тонких пленках, что де-лает нелинейные оптические эффекты второго порядка уникальным инструментом для исследования свойств поверхностей.Генерация суммарной частоты, благодаря большому количеству варьируемых параметров эксперимента (на-правления, частоты и поляризации падающих волн), является одним из самых перспективных нелинейных явлений для исследования поверхностей. На практике генерация суммарной частоты (и ее частный случай генерация второй гармоники) применяется для исследо-Эффективное использование этого инструмента тре-бует построения адекватной математической модели. На настоящий момент имеется три наиболее используемых модели: модель Релея-Ганса-Дебая [8-10], модель на основе точного решения задачи о рассеянии [11,12] и модель Вентцеля-Крамерса-Бриллюэна [13]. Первая модель применима при малых размерах исследуемых систем и не учитывает рассеяние на границах раздела, однако для нее проще всего получить аналитическое решение. Вторая модель учитывает рассеяние, но ее ис-пользование затруднено для частиц произвольной фор-мы, а также требует применения достаточно сложного математического аппарата. Третья модель лучше опи-сывает нелинейные эффекты, чем первая, и применима для частиц произвольных размеров, но для нее можно получить только численное решение. В модели Релея-Ганса-Дебая имеется ряд особенностей, не замеченных ранее, которым и посвящена настоящая статья. Дипольное приближениеПусть плоские электромагнитные волны в задаче за-даются выражениями вида (у всех волн подразумевается временная часть exp(−iωt))где E 0 -это комплексная амплитуда волны, e -единичный комплексный вектор (|e| 2 = ee * = 1, где сим-вол * означает комплекс...

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“…Note that several theoretical methods such as the perturbation theory [20], nonlinear Mie theory [21] and reciprocity theory combined with linear Mie scattering [22], have been adopted to describe SHG cases in nanoparticles. However, most of these methods are limited to handle spherical nanoparticles, and a universal model is still rare for nanoparticles in arbitrary shapes.…”

mentioning

confidence: 99%

“…where 22 kc   , 2 P is the linear polarization of the SHG signal, and (2) P denotes the second-order nonlinear polarization. Similar to the linear case in Eq.…”

mentioning

confidence: 99%

Giant enhancement of second harmonic generation by engineering double plasmonic resonances at nanoscale

Ren¹,

Liu²,

Wang³

et al. 2014

Opt. Express

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We have investigated second harmonic generation (SHG) from Ag-coated LiNbO 3 (LN) core-shell nanocuboids and found that giant SHG can occur via deliberately designed double plasmonic resonances. By controlling the aspect ratio, we can tune fundamental wave (FW) and SHG signal to match the longitudinal and transverse plasmonic modes simultaneously, and achieve giant enhancement of SHG by 3×10 5 in comparison to a bare LN nanocuboid and by about one order of magnitude to the case adopting only single plasmonic resonance. The underlying key physics is that the double-resonance nanoparticle enables greatly enhanced trapping and harvesting of incident FW energy, efficient internal transfer of optical energy from FW to SHW, and much improved power to transport the SHG energy from the nanoparticle to the far-field region. In this work we will address this problem by insightful design. The most important thing is to look for a nanoparticle with double SPR modes. For this purpose, we turn to nanoparticles of anisotropic geometry, among which nanorods have attracted great attention due to their dimension induced wavelength tunability and polarization sensitivity [11][12][13]. One can control the aspect ratio of nanorods easily and obtain double SPR modes simultaneously, which are associated with the longitudinal and transverse SPR modes [14,15]. Moreover, the optical cross-sections of nanorods are much higher than those of nanospheres, and this has attributed nanorods promising features in wide applications like low-threshold surface plasmon amplification [16,17] and ultrafast optical devices [18]. The two SPR modes can be designed to enable their wavelengths matched to the absorption bands and emission bands of fluorescent molecules absorbed in gold nanorods [19] for enhancing their fluorescence intensity. It would be expected that this double-resonance mechanism should also play a very good role in enhancing SHG intensity of nanostructured materials.To illustrate and confirm this hypothesis, we propose and design an anisotropic nanoparticle, an Ag-coated LiNbO 3 (LN) core-shell nanocuboid [Ag-LN in Fig. 1(a) [23,24]. This approach is efficient equally for nonlinear optical problem solutions.Assume a plane wave FW at the frequency of ω 1 is incident upon a nonlinear particle. The FW electric field 1

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Nonlinear Mie theory for second-harmonic and sum-frequency scattering

Cited by 137 publications

References 49 publications

Molecular characterization of water and surfactant AOT at nanoemulsion surfaces

Molecular characterization of water and surfactant AOT at nanoemulsion surfaces

Генерация Суммарной Частоты От Тонкого Цилиндрического Слоя

Giant enhancement of second harmonic generation by engineering double plasmonic resonances at nanoscale

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