Quantifying the hygroscopic properties of cyclodextrin containing aerosol for drug delivery to the lungs

Abstract. To investigate the hygroscopic properties of ultrafine particles during new particle formation events, the hygroscopic growth factors of size-segregated atmospheric particles were measured at an urban site in Sapporo, northern Japan, during the summer of 2011. The hygroscopic growth factor at 85 % relative humidity [g(85%)] of freshly formed nucleation mode particles was 1.11 to 1.28 (average: 1.16 ± 0.06) at a dry particle diameter (Dp) centered on 20 nm, which is equivalent to 1.17 to 1.35 (1.23 ± 0.06) at a dry Dp centered on 100 nm after considering the Kelvin effect. These values are comparable with those of secondary organic aerosols, suggesting that low-volatility organic vapors are important to the burst of nucleation mode particles. The equivalent g(85%) at a dry Dp of 100 nm for nucleated particles that have grown to Aitken mode sizes (1.24 to 1.34; average: 1.30 ± 0.04) were slightly higher than those of newly formed nucleation mode particles, suggesting that the growth of freshly formed nucleation mode particles to the Aitken mode size can be subjected to condensation of not only low-volatility organic vapors, but also water-soluble inorganic species. Based on this result, and previous measurement of radiocarbon in aerosols, we suggest that the burst of nucleation mode particles and their subsequent growth were highly affected by biogenic organic emissions at this measurement site, which is surrounded by deciduous forest. Gradual increases in mode diameter after the burst of nucleation mode particles were observed under southerly wind conditions, with a dominant contribution of intermediately hygroscopic particles. However, sharp increases in mode diameter were observed when the wind direction shifted to northwesterly or northeasterly, with a sharp increase in the highly hygroscopic particle fraction of the Aitken mode particles, indicating that the hygroscopic growth factor of newly formed particles is perturbed by the local winds that deliver different air masses to the measurement site.

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Design and Application of an Unattended Multifunctional H-TDMA System

Journal of Atmospheric and Oceanic Technology ◽

10.1175/jtech-d-12-00129.1 ◽

2013 ◽

Vol 30 (6) ◽

pp. 1136-1148 ◽

Cited By ~ 26

Author(s):

Haobo Tan ◽

Hanbing Xu ◽

Qilin Wan ◽

Fei Li ◽

Xuejiao Deng ◽

...

Keyword(s):

Particle Size ◽

Growth Factor ◽

Cloud Condensation Nuclei ◽

Polystyrene Latex ◽

Hygroscopic Growth ◽

Differential Mobility Analyzer ◽

Differential Mobility ◽

China Meteorological Administration ◽

Hygroscopic Properties ◽

Calibration Methods

Abstract The hygroscopic properties of aerosols have a significant impact on aerosol particle number size distributions (PNSD), formation of cloud condensation nuclei, climate forcing, and atmospheric visibility, as well as human health. To allow for the observation of the hygroscopic growth of aerosols with long-term accuracy, an unattended multifunctional hygroscopicity-tandem differential mobility analyzer (H-TDMA) system was designed and built by the Institute of Tropical and Marine Meteorology (ITMM), China Meteorological Administration (CMA), in Guangzhou, China. The system is capable of measuring dry and wet PNSD, hygroscopic growth factor by particle size, and mixing states. This article describes in detail the working principles, components, and calibration methods of the system. Standard polystyrene latex (PSL) spheres with five different diameters were chosen to test the system’s precision and accuracy of particle size measurement. Ammonium sulfate was used to test the hygroscopic response of the system for accurate growth factor measurement. The test results show that the deviation of the growth factor measured by the system is within a scope of −0.01 to −0.03 compared to Köhler theoretical curves. Results of temperature and humidity control performance tests indicate that the system is robust. An internal temperature gradient of less than 0.2 K for a second differential mobility analyzer (DMA2) makes it possible to reach a set-point relative humidity (RH) value of 90% and with a standard deviation of ±0.44%, sufficient for unattended field observation.

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Hygroscopic properties and mixing state of aerosol measured at the high altitude site Puy de Dôme (1465 m a.s.l.), France

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-14-6759-2014 ◽

2014 ◽

Vol 14 (5) ◽

pp. 6759-6802

Author(s):

H. Holmgren ◽

K. Sellegri ◽

M. Hervo ◽

C. Rose ◽

E. Freney ◽

...

Keyword(s):

Boundary Layer ◽

Particle Size ◽

Growth Factor ◽

High Altitude ◽

Hygroscopic Growth ◽

Mixing State ◽

Air Mass ◽

Hygroscopic Properties ◽

Seasonal And Diurnal Variations ◽

Mass Type

Abstract. A Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France from September 2008 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal, and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of marine aerosol may be explained by large proportions of inorganic aerosol and sea salts, and it is speculated that continental particles are more hygroscopic than local and African ones due to ageing of fresh combustion aerosol. Aerosol measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less hygroscopic mode (GF < 1.3), a hygroscopic mode (GF 1.3–1.7) and a more hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less hygroscopic mode or the hygroscopic mode, and only few of them have more hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when the aerosol is found with two or more populations with different hygroscopic properties, is found to increase with particle size (average yearly values are 22, 33 and 49% for 25, 50, and 165 nm particles, respectively). The degree of external mixing is more sensitive to season than to air mass type, and it is higher in the cold seasons than in the warm seasons. This study gathers the results from one of the longest data sets of hygroscopic growth factor measurements to date, allowing a statistically relevant hygroscopic growth parameterization to be determined as a function of both air mass type and season.

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Development of an H-TDMA for long-term unattended measurement of the hygroscopic properties of atmospheric aerosol particles

Atmospheric Measurement Techniques Discussions ◽

10.5194/amtd-2-1057-2009 ◽

2009 ◽

Vol 2 (2) ◽

pp. 1057-1073

Author(s):

E. Nilsson ◽

E. Swietlicki ◽

S. Sjogren ◽

J. Löndahl ◽

M. Nyman ◽

...

Keyword(s):

Growth Factor ◽

Ammonium Sulphate ◽

Atmospheric Aerosol ◽

Aerosol Particles ◽

Temperature Stability ◽

Hygroscopic Growth ◽

Hygroscopic Properties ◽

Atmospheric Aerosol Particles ◽

New Generation

Abstract. A new hygroscopic tandem differential mobility analyzer (H-TDMA) has been constructed at Lund University within the frameworks of the EU FP6 Infrastructure Project EUSAAR (http://www.eusaar.org/). The aim of this coordinated H-TDMA development is to design and evaluate a new generation of H-TDMAs that are capable of conducting long term measurements of the hygroscopic growth and state of mixing of sub-micrometer atmospheric aerosol particles at the EUSAAR aerosol super-sites across Europe. The H-TDMA constructed for this project has been validated with respect to hygroscopic growth factor, stability of relative humidity (RH), temperature stability and its ability to operate unattended for longer periods of time. When measuring growth factors of ammonium sulphate, the new H-TDMA system was found to measure within a growth factor deviation of ±0.05 compared to previously recorded data by Tang et al. (1994). The long term RH of the system has been found stable at 90.0% with a standard deviation of ±0.23% and an average temperature variability of the second DMA less than ±0.1 K. Daily automated ammonium sulphate measurements have validated the ambient measurements. The instrument is operated at the EMEP/EUSAAR background station Vavihill in the southern part of Sweden.

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Particle hygroscopicity and its link to chemical composition in the urban atmosphere of Beijing, China, during summertime

Atmospheric Chemistry and Physics ◽

10.5194/acp-16-1123-2016 ◽

2016 ◽

Vol 16 (2) ◽

pp. 1123-1138 ◽

Cited By ~ 49

Author(s):

Z. J. Wu ◽

J. Zheng ◽

D. J. Shang ◽

Z. F. Du ◽

Y. S. Wu ◽

...

Keyword(s):

Particle Size ◽

Chemical Composition ◽

Growth Factor ◽

Mass Concentration ◽

Particle Formation ◽

High Time Resolution ◽

New Particle Formation ◽

Hygroscopic Growth ◽

Hygroscopic Properties ◽

Beijing China

Abstract. Simultaneous measurements of particle number size distribution, particle hygroscopic properties, and size-resolved chemical composition were made during the summer of 2014 in Beijing, China. During the measurement period, the mean hygroscopicity parameters (κs) of 50, 100, 150, 200, and 250 nm particles were respectively 0.16  &pm;  0.07, 0.19  &pm;  0.06, 0.22  &pm;  0.06, 0.26  &pm;  0.07, and 0.28  &pm;  0.10, showing an increasing trend with increasing particle size. Such size dependency of particle hygroscopicity was similar to that of the inorganic mass fraction in PM1. The hydrophilic mode (hygroscopic growth factor, HGF  >  1.2) was more prominent in growth factor probability density distributions and its dominance of hydrophilic mode became more pronounced with increasing particle size. When PM2.5 mass concentration was greater than 50 μg m−3, the fractions of the hydrophilic mode for 150, 250, and 350 nm particles increased towards 1 as PM2.5 mass concentration increased. This indicates that aged particles dominated during severe pollution periods in the atmosphere of Beijing. Particle hygroscopic growth can be well predicted using high-time-resolution size-resolved chemical composition derived from aerosol mass spectrometer (AMS) measurements using the Zdanovskii–Stokes–Robinson (ZSR) mixing rule. The organic hygroscopicity parameter (κorg) showed a positive correlation with the oxygen to carbon ratio. During the new particle formation event associated with strongly active photochemistry, the hygroscopic growth factor or κ of newly formed particles is greater than for particles with the same sizes not during new particle formation (NPF) periods. A quick transformation from external mixture to internal mixture for pre-existing particles (for example, 250 nm particles) was observed. Such transformations may modify the state of the mixture of pre-existing particles and thus modify properties such as the light absorption coefficient and cloud condensation nuclei activation.

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Development of an H-TDMA for long-term unattended measurement of the hygroscopic properties of atmospheric aerosol particles

Atmospheric Measurement Techniques ◽

10.5194/amt-2-313-2009 ◽

2009 ◽

Vol 2 (1) ◽

pp. 313-318 ◽

Cited By ~ 26

Author(s):

E. Nilsson ◽

E. Swietlicki ◽

S. Sjogren ◽

J. Löndahl ◽

M. Nyman ◽

...

Keyword(s):

Growth Factor ◽

Ammonium Sulphate ◽

Atmospheric Aerosol ◽

Aerosol Particles ◽

Temperature Stability ◽

Hygroscopic Growth ◽

Hygroscopic Properties ◽

Atmospheric Aerosol Particles ◽

New Generation

Abstract. A new hygroscopic tandem differential mobility analyzer (H-TDMA) has been constructed at Lund University within the frameworks of the EU FP6 Infrastructure Project EUSAAR (http://www.eusaar.org/). The aim of this coordinated H-TDMA development is to design and evaluate a new generation of H-TDMAs that are capable of conducting long term measurements of the hygroscopic growth and state of mixing of sub-micrometer atmospheric aerosol particles at the EUSAAR aerosol super-sites across Europe. The H-TDMA constructed for this project has been validated with respect to hygroscopic growth factor, stability of relative humidity (RH), temperature stability and its ability to operate unattended for longer periods of time. When measuring growth factors of ammonium sulphate, the new H-TDMA system was found to measure within a growth factor deviation of ±0.05 compared to previously recorded data by Tang et al. (1994). The long term RH of the system has been found stable at 90.0% with a standard deviation of ±0.23% and an average temperature variability of the second DMA less than ±0.1 K. Daily automated ammonium sulphate measurements have validated the ambient measurements. The instrument is operated at the EMEP/EUSAAR background station Vavihill in the southern part of Sweden.

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Hygroscopic growth of urban aerosol particles in Beijing (China) during wintertime: a comparison of three experimental methods

Atmospheric Chemistry and Physics ◽

10.5194/acp-9-6865-2009 ◽

2009 ◽

Vol 9 (18) ◽

pp. 6865-6880 ◽

Cited By ~ 62

Author(s):

J. Meier ◽

B. Wehner ◽

A. Massling ◽

W. Birmili ◽

A. Nowak ◽

...

Keyword(s):

Growth Factors ◽

Growth Factor ◽

The Other ◽

Hygroscopic Growth ◽

Differential Mobility ◽

Accumulation Mode ◽

Hygroscopic Properties ◽

Solubility Model ◽

Particle Sizer ◽

Beijing China

Abstract. The hygroscopic properties of atmospheric aerosols are highly relevant for the quantification of radiative effects in the atmosphere, but also of interest for the assessment of particle health effects upon inhalation. This article reports measurements of aerosol particle hygroscopicity in the highly polluted urban atmosphere of Beijing, China in January 2005. The meteorological conditions corresponded to a relatively cold and dry atmosphere. Three different methods were used: 1) A combination of Humidifying Differential Mobility Particle Sizer (H-DMPS) and Twin Differential Mobility Particle Sizer (TDMPS) measurements, 2) A Hygroscopic Tandem Differential Mobility Analyzer (H-TDMA), and 3) A simplistic solubility model fed by chemical particle composition determined from Micro Orifice Uniform Deposit Impactor (MOUDI) samples. From the H-DMPS and TDMPS particle number size distributions, a size-resolved descriptive hygroscopic growth factor (DHGF) was determined for the relative humidities (RH) 55%, 77% and 90%, and particle diameters between 30 and 400 nm. In Beijing, the highest DHGFs were observed for accumulation mode particles, 1.40 (±0.03) at 90% RH. DHGF decreased significantly with particle size, reaching 1.04 (±0.15) at 30 nm. H-TDMA data also suggest a decrease in growth factor towards the biggest particles investigated (350 nm), associated with an increasing fraction of nearly hydrophobic particles. The agreement between the H-DMPS/TDMPS and H-TDMA methods was satisfactory in the accumulation mode size range (100–400 nm). In the Aitken mode range (<100 nm), the H-DMPS/TDMPS method yielded growth factors lower by up to 0.1 at 90% RH. The application of the solubility model based on measured chemical composition clearly reproduced the size-dependent trend in hygroscopic particle growth observed by the other methods. In the case of aerosol dominated by inorganic ions, the composition-derived growth factors tended to agree (± 0.05) or underestimate (up to 0.1) the values measured by the other two methods. In the case of aerosol dominated by organics, the reverse was true, with an overestimation of up to 0.2. The results shed light on the experimental and methodological uncertainties that are still connected with the determination of hygroscopic growth factors.

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Hygroscopic properties and mixing state of aerosol measured at the high-altitude site Puy de Dôme (1465 m a.s.l.), France

Atmospheric Chemistry and Physics ◽

10.5194/acp-14-9537-2014 ◽

2014 ◽

Vol 14 (18) ◽

pp. 9537-9554 ◽

Cited By ~ 17

Author(s):

H. Holmgren ◽

K. Sellegri ◽

M. Hervo ◽

C. Rose ◽

E. Freney ◽

...

Keyword(s):

Boundary Layer ◽

Particle Size ◽

Growth Factor ◽

High Altitude ◽

Hygroscopic Growth ◽

Mixing State ◽

Air Mass ◽

Hygroscopic Properties ◽

Seasonal And Diurnal Variations ◽

Mass Type

Abstract. A Hygroscopicity Tandem Differential Mobility Analyser (HTDMA) was used to evaluate the hygroscopic properties of aerosol particles measured at the Puy de Dôme research station in central France, periodically from September 2008 to January 2010, and almost continuously from October 2010 to December 2012. This high-altitude site is ideally situated to allow for both the upper part of the planetary boundary layer and the lower free troposphere to be sampled. The aim of the study is to investigate both the influence of year-to-year, seasonal and diurnal cycles, as well as the influence of air mass type on particle hygroscopicity and mixing state. Results show that particle hygroscopicity increases with particle size and depends both on air mass type and on season. Average growth factor values, GFs, are lowest in winter (1.21 ± 0.13, 1.23 ± 0.18 and 1.38 ± 0.25 for 25, 50 and 165 nm particles, respectively) and highest in autumn (1.27 ± 0.11, 1.32 ± 0.12 and 1.49 ± 0.15 for 25, 50 and 165 nm particles, respectively). Particles are generally more hygroscopic at night than during the day. The seasonal and diurnal variations are likely to be strongly influenced by boundary layer dynamics. Furthermore, particles originating from oceanic and continental regions tend to be more hygroscopic than those measured in African and local air masses. The high hygroscopicity of oceanic aerosol can be explained by large proportions of inorganic aerosol and sea salts. Aerosols measured at the Puy de Dôme display a high degree of external mixing, and hygroscopic growth spectra can be divided into three different hygroscopic modes: a less-hygroscopic mode (GF < 1.3), a hygroscopic mode (GF~1.3–1.7) and a more-hygroscopic mode (GF > 1.7). The majority of particles measured can be classified as being in either the less-hygroscopic mode or the hygroscopic mode, and only few of them have more-hygroscopic properties. The degree of external mixing, evaluated as the fraction of time when the aerosol is found with two or more aerosol populations with different hygroscopic properties, increases with particle size (average yearly values are 20, 28 and 45 {%} for 25, 50, and 165 nm particles, respectively). The degree of external mixing is more sensitive to season than to air mass type, and it is higher in the cold seasons than in the warm seasons. With more than two years of nearly continuous measurements, this study gathers the results from one of the longest data sets of hygroscopic growth factor measurements to date, allowing a statistically relevant hygroscopic growth parameterization to be determined as a function of both air mass type and season.

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Aerosol hygroscopicity at Ispra EMEP-GAW station

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-12-5293-2012 ◽

2012 ◽

Vol 12 (2) ◽

pp. 5293-5340 ◽

Cited By ~ 3

Author(s):

M. Adam ◽

J. P. Putaud ◽

S. Martins dos Santos ◽

A. Dell'Acqua ◽

C. Gruening

Keyword(s):

Growth Factor ◽

Relative Humidity ◽

Mie Theory ◽

Data Consistency ◽

Absorption Enhancement ◽

Hygroscopic Growth ◽

Extinction Coefficients ◽

Aerosol Absorption ◽

Hygroscopic Properties ◽

Enhancement Factors

Abstract. This study focuses on the aerosol hygroscopic properties as determined from ground-based measurements and Mie theory. Usually, aerosol ground-based measurements are taken in dry conditions to ensure data consistency within networks. The dependence of the various aerosol optical characteristics (e.g. aerosol absorption, scattering, backscattering or extinction coefficients) on relative humidity has therefore to be established in order to determine their values in the atmosphere, where relative humidity can reach high values. We calculated mean monthly diurnal values of the aerosol hygroscopic growth factor at 90% relative humidity GF(90) based on measurements performed at EMEP-GAW station of Ispra with a Hygroscopicity Tandem Differential Mobility Analyzer over eight months in 2008 and 2009. Particle hygroscopicity increases with particle dry diameter ranging from 35 to 165 nm for all seasons. We observed a clear seasonal variation in GF(90) for particles larger than 75 nm, and a diurnal cycle in spring and winter for all sizes. For 165 nm particles, GF(90) averages 1.32 ± 0.06. The effect of the particle hygroscopic growth on the aerosol optical properties (scattering, extinction, absorption and backscatter coefficients, asymmetry parameter and backscatter faction) was computed using the Mie theory, based on data obtained from a series of instruments running at our station. We found median enhancement factors (defined as ratios between the values of optical variables at 90% and 0% relative humidity) equal to 1.1, 2.1, 1.7, and 1.8, for the aerosol absorption, scattering, backscattering, and extinction coefficients, respectively. All except the absorption enhancement factor show a strong correlation with the hygroscopic growth factor. The enhancement factors observed at our site are among the lowest observed across the world for the aerosol scattering coefficient, and among the highest for the aerosol backscatter fraction.

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Aerosol hygroscopicity at a regional background site (Ispra) in Northern Italy

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-5703-2012 ◽

2012 ◽

Vol 12 (13) ◽

pp. 5703-5717 ◽

Cited By ~ 32

Author(s):

M. Adam ◽

J. P. Putaud ◽

S. Martins dos Santos ◽

A. Dell'Acqua ◽

C. Gruening

Keyword(s):

Growth Factor ◽

Relative Humidity ◽

Mie Theory ◽

Absorption Enhancement ◽

Research Station ◽

Hygroscopic Growth ◽

Extinction Coefficients ◽

Aerosol Absorption ◽

Hygroscopic Properties ◽

Enhancement Factors

Abstract. This study focuses on the aerosol hygroscopic properties as determined from ground-based measurements and Mie theory. Usually, aerosol ground-based measurements are taken in dry conditions in order to have a consistency within networks. The dependence of the various aerosol optical characteristics (e.g. aerosol absorption, scattering, backscattering or extinction coefficients) on relative humidity has therefore to be established in order to determine their values in the atmosphere, where relative humidity can reach high values. We calculated mean monthly diurnal values of the aerosol hygroscopic growth factor at 90% relative humidity GF(90) based on measurements performed at the atmospheric research station in Ispra (Italy) with a Hygroscopicity Tandem Differential Mobility Analyzer over eight months in 2008 and 2009. Particle hygroscopicity increases with particle dry diameter ranging from 35 to 165 nm for all seasons. We observed a clear seasonal variation in GF(90) for particles larger than 75 nm, and a diurnal cycle in spring and winter for all sizes. For 165 nm particles, GF(90) averages 1.32 &pm; 0.06. The effect of the particle hygroscopic growth on the aerosol optical properties (scattering, extinction, absorption and backscatter coefficients, asymmetry parameter and backscatter faction) was computed using the Mie theory, based on data obtained from a series of instruments running at our station. We found median enhancement factors (defined as ratios between the values of optical variables at 90% and 0% relative humidity) equal to 1.1, 2.1, 1.7, and 1.8, for the aerosol absorption, scattering, backscattering, and extinction coefficients, respectively. All except the absorption enhancement factors show a strong correlation with the hygroscopic growth factor. The enhancement factors observed at our site are among the lowest observed across the world for the aerosol scattering coefficient, and among the highest for the aerosol backscatter fraction.

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