The Measurement of Liquid Water Mass Associated With Collected Hygroscopic Particles

Lee, Chung‐Te; Hsu, Wen Jing

doi:10.1016/s0021-8502(99)00048-8

Cited by 66 publications

(52 citation statements)

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“…Hereafter, the DRH of the "pure NaNO 3 limit" is defined as 74.0 %. On the other hand, most wet deposited aerosol particles (> 90 %) generated by nebulization from a NaNO 3 aqueous solution grew continuously and shrank without any phase transition during the humidifying and dehydration processes, which have also been reported (Gysel et al, 2002;McInnes et al, 1996;Lee et al, 2000;Hoffman et al, 2004). However, a few wet deposited particles showed ERH in the range, 25.8-18.9 %.…”

Section: Hygroscopic Behavior Of Pure Nacl and Nano 3 Particlesmentioning

confidence: 79%

Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates

et al. 2015

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Abstract. NaCl in fresh sea-salt aerosol (SSA) particles can partially or fully react with atmospheric NO x /HNO 3 , so internally mixed NaCl and NaNO 3 aerosol particles can co-exist over a wide range of mixing ratios. Laboratorygenerated, micrometer-sized NaCl and NaNO 3 mixture particles at 10 mixing ratios (mole fractions of NaCl (X NaCl ) = 0.1 to 0.9) were examined systematically to observe their hygroscopic behavior, derive experimental phase diagrams for deliquescence and efflorescence, and understand the efflorescence mechanism. During the humidifying process, aerosol particles with the eutonic composition (X NaCl = 0.38) showed only one phase transition at their mutual deliquescence relative humidity (MDRH) of 67.9 (±0.5) %. On the other hand, particles with other mixing ratios showed two distinct deliquescence transitions; i.e., the eutonic component dissolved at MDRH, and the remainder in the solid phase dissolved completely at their DRHs depending on the mixing ratios, resulting in a phase diagram composed of four different phases, as predicted thermodynamically. During the dehydration process, NaCl-rich particles (X NaCl > 0.38) showed a two stage efflorescence transition: the first stage was purely driven by the homogeneous nucleation of NaCl and the second stage at the mutual efflorescence RH (MERH) of the eutonic components, with values in the range of 30.0-35.5 %. Interestingly, aerosol particles with the eutonic composition (X NaCl = 0.38) also showed two-stage efflorescence, with NaCl crystallizing first followed by heterogeneous nucleation of the remaining NaNO 3 on the NaCl seeds. NaNO 3 -rich particles (X NaCl ≤ 0.3) underwent singlestage efflorescence transitions at ERHs progressively lower than the MERH because of the homogeneous nucleation of NaCl and the almost simultaneous heterogeneous nucleation of NaNO 3 on the NaCl seeds. SEM/EDX elemental mapping indicated that the effloresced NaCl-NaNO 3 particles at all mixing ratios were composed of a homogeneously crystallized NaCl moiety in the center, surrounded either by the eutonic component (for X NaCl > 0.38) or NaNO 3 (for X NaCl ≤ 0.38). During the humidifying or dehydration process, the amount of eutonic composed part drives particle/droplet growth or shrinkage at the MDRH or MERH (second ERH), respectively, and the amount of pure salts (NaCl or NaNO 3 in NaCl-or NaNO 3 -rich particles, respectively) drives the second DRHs or first ERHs, respectively. Therefore, their behavior can be a precursor to the optical properties and direct radiative forcing for these atmospherically relevant mixture particles representing the coarse, reacted inorganic SSAs. In addition, the NaCl-NaNO 3 mixture aerosol particles can maintain an aqueous phase over a wider RH range than pure NaCl particles as SSA surrogate, making their heterogeneous chemistry more probable.

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Section: Hygroscopic Behavior Of Pure Nacl and Nano 3 Particlesmentioning

confidence: 79%

Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates

et al. 2015

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“…The fraction of NaCl dihydrate forming via heterogeneous nucleation pathway is then estimated analogue to Equation (15),…”

Section: G Temperature-dependent Formation Of Nacl Dihydrate In Ssa mentioning

confidence: 99%

“…Some of these salts (e.g., gypsum) have lower solubility than NaCl and therefore would precipitate at humidity values higher than the ERH for micron size pure NaCl solution droplets. 2,[13][14][15][16][17][18] Such solid inclusions could facilitate the nucleation of crystalline NaCl.…”

Section: Introductionmentioning

confidence: 99%

Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea salt aerosol particles

Peckhaus¹,

Kiselev²,

Wagner³

et al. 2016

The Journal of Chemical Physics

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Recent laboratory studies indicate that the hydrated form of crystalline NaCl is potentially important for atmospheric processes involving depositional ice nucleation on NaCl dihydrate particles under cirrus cloud conditions. However, recent experimental studies reported a strong discrepancy between the temperature intervals where the efflorescence of NaCl dihydrate has been observed. Here we report the measurements of the volume specific nucleation rate of crystalline NaCl in the aqueous solution droplets of pure NaCl suspended in an electrodynamic balance at constant temperature and humidity in the range from 250 K to 241 K. Based on these measurements, we derive the interfacial energy of crystalline NaCl dihydrate in a supersaturated NaCl solution and determined its temperature dependence. Taking into account both temperature and concentration dependence of nucleation rate coefficients, we explain the difference in the observed fractions of NaCl dihydrate reported in the previous studies. Applying the heterogeneous classical nucleation theory model, we have been able to reproduce the 5 K shift of the NaCl dihydrate efflorescence curve observed for the sea salt aerosol particles, assuming the presence of super-micron solid inclusions (hypothetically gypsum or hemihydrate of CaSO 4 ). These results support the notion that the phase transitions in microscopic droplets of supersaturated solution should be interpreted by accounting for the stochastic nature of homogeneous and heterogeneous nucleation and cannot be understood on the ground of bulk phase diagrams alone.

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“…For example, aerosol particles composed of certain watersoluble inorganic salts can reversibly take up water vapor without the prompt deliquescence and efflorescence phase transitions and hysteresis effects typically observed for the corresponding crystalline bulk material: CaCl 2 and MnSO 4 (Cohen at al., 1987); NH 4 NO 3 (Tang, 1980;Dougle et al, 1998;Cziczo and Abbatt, 2000;Lee and Hsu, 2000;Mikhailov et al, 2004;Schlenker et al, 2004;Schlenker and Martin, 2005;Svenningson et al, 2006), NH 4 HSO 4 (Tang and Munkelwitz, 1994;Cziczo et al, 1997;Cziczo and Abbatt, 2000;Lee and Hsu, 2000;Martin et al, 2003;Colberg et al, 2003Colberg et al, , 2004Schlenker et al, 2004;Schlenker and Martin, 2005), NaNO 3 (McInnes et al, 1996;Hsu, 2000, Gysel et al, 2002;Hoffmann et al, 2004), Ca(NO 3 ) 2 (Liu et al, 2008), and sea salt .…”

Section: Introductionmentioning

confidence: 99%

Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations

et al. 2009

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Abstract. Interactions with water are crucial for the properties, transformation and climate effects of atmospheric aerosols. Here we present a conceptual framework for the interaction of amorphous aerosol particles with water vapor, outlining characteristic features and differences in comparison to crystalline particles. We used a hygroscopicity tandem differential mobility analyzer (H-TDMA) to characterize the hydration and dehydration of crystalline ammonium sulfate, amorphous oxalic acid and amorphous levoglucosan particles (diameter ∼100 nm, relative humidity 5-95% at 298 K). The experimental data and accompanying Köhler model calculations provide new insights into particle microstructure, surface adsorption, bulk absorption, phase transitions and hygroscopic growth. The results of these and related investigations lead to the following conclusions:(1) Many organic substances, including carboxylic acids, carbohydrates and proteins, tend to form amorphous rather than crystalline phases upon drying of aqueous solution droplets. Depending on viscosity and microstructure, the amorphous phases can be classified as glasses, rubbers, gels or viscous liquids.(2) Amorphous organic substances tend to absorb water vapor and undergo gradual deliquescence and hygroscopic growth at lower relative humidity than their crystalline counterparts.(3) In the course of hydration and dehydration, certain organic substances can form rubber-or gel-like structures Correspondence to: U. Pöschl (u.poschl@mpic.de) (supramolecular networks) and undergo transitions between swollen and collapsed network structures.(4) Organic gels or (semi-)solid amorphous shells (glassy, rubbery, ultra-viscous) with low molecular diffusivity can kinetically limit the uptake and release of water and may influence the hygroscopic growth and activation of aerosol particles as cloud condensation nuclei (CCN) and ice nuclei (IN). Moreover, (semi-)solid amorphous phases may influence the uptake of gaseous photo-oxidants and the chemical transformation and aging of atmospheric aerosols.(5) The shape and porosity of amorphous and crystalline particles formed upon dehydration of aqueous solution droplets depend on chemical composition and drying conditions. The apparent volume void fractions of particles with highly porous structures can range up to ∼50% or more (xerogels, aerogels).(6) For efficient description of water uptake and phase transitions of aerosol particles, we propose not to limit the terms deliquescence and efflorescence to equilibrium phase transitions of crystalline substances. Instead we propose generalized definitions according to which amorphous and crystalline components can undergo gradual or prompt, partial or full deliquescence or efflorescence.We suggest that (semi-)solid amorphous phases may be important not only in the upper atmosphere as suggested in recent studies of glass formation at low temperatures. Depending on relative humidity, (semi-)solid phases and moisture-induced glass transitions may also play a role in gas-particle intera...

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The Measurement of Liquid Water Mass Associated With Collected Hygroscopic Particles

Cited by 66 publications

References 0 publications

Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates

Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates

Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea salt aerosol particles

Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations

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The Measurement of Liquid Water Mass Associated With Collected Hygroscopic Particles

Cited by 66 publications

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Hygroscopic properties of NaCl and NaNO&lt;sub&gt;3&lt;/sub&gt; mixture particles as reacted inorganic sea-salt aerosol surrogates

Hygroscopic properties of NaCl and NaNO&lt;sub&gt;3&lt;/sub&gt; mixture particles as reacted inorganic sea-salt aerosol surrogates

Temperature-dependent formation of NaCl dihydrate in levitated NaCl and sea salt aerosol particles

Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations

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Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates

Hygroscopic properties of NaCl and NaNO<sub>3</sub> mixture particles as reacted inorganic sea-salt aerosol surrogates