Electrodynamic balance for the optical elemental analysis of ice-nucleating particles

Diplomityössä esitellään uusi reaaliaikainen mittausmenetelmä pienhiukkasten alkuaineanalyysin suorittamiseksi. Menetelmä perustuu hiukkasen sähködynaamiseen tasapainoon sekä laser-indusoituun plasmaspektroskopiaan, jotka ovat omilla tieteenaloillaan tunnettuja ja suosittuja analyysimenetelmiä. Nykyisellään pienhiukkasten reaaliaikainen alkuaineanalyysi lepää aerosolimassaspektroskopian harteilla, mutta kompaktimpaan, kevyempään ja helppokäyttöisempään mittausvälineeseen on tarvetta esimerkiksi jäänukleaatiohiukkastutkimuksessa. Menetelmän toimivuutta tutkittiin numeerisesti ja kokeellisesti, ja tuloksia verrattiin aikaisempaan teoriaan ja tutkimukseen. Tutkimuksessa varmistettiin menetelmän toimivuus alkuaineanalyysiin ja saavutettiin lisätietämystä sähködynaamisen tasapainokammion toiminnasta mikrometrin hiukkaskokoluokassa. Tämän lisäksi valmistettiin ja karakterisoitiin uudentyyppinen aerosolivaraaja, jolla voidaan varata kyseisen kokoluokan hiukkasia suuren sähkökentän avulla aiempaa suurempiin varauslukuihin. Kehitetyn aerosolivaraajan avulla analyysimenetelmä saatiin toimimaan läpimitaltaan yli 800 nanometrin hiukkasille. Toistaiseksi analyysi voitiin toteuttaa manuaalisesti likimain nopeudella yksi hiukkanen minuutissa, eli tärkeä jatkokehityskohde on analyysin automatisointi ja nopeuden kasvattaminen. Emissiospektrien keräyksessä päädyttiin käytännössä sadan prosentin laserin osumatarkkuuteen. Kun menetelmällä analysoitiin kaoliinihiukkasia suoraan kaasufaasista, niiden emissiospektreistä kyettiin erottamaan alumiinin perustason hienorakenne ja vähentämään oleellisesti mittausartefaktina esiintyvän kalsiumin emissiota verrattuna vesiavusteisesti pirskotettuihin samanlaisiin hiukkasiin

Formation of segregation structures in Hafnarhraun pāhoehoe lobe, SW Iceland: a window into crystal–melt separation in basaltic magma

To gain insights into crystal–melt separation processes during basalt differentiation, we have studied an 8-m-thick pāhoehoe lava lobe from the Hafnarhraun lava flow field in SW Iceland. The lobe has abundant melt segregations, porous cylindrical and sheet-like structures, generally interpreted as separated residual melts of a lava lobe. We divide these melt segregations into three types based on morphology and composition: vesicle cylinders (VC), type 1 horizontal vesicle sheets (HVS1), and type 2 horizontal vesicle sheets (HVS2). Remarkably, the studied VC are not simple residual melts generated by fractional crystallization, but their composition points to removal of plagioclase from the parental lava. HVS1 resemble VC, but have fractionated more olivine (ol) + plagioclase (plg) ± augite and have lost most, if not all, of their olivine phenocrysts. HVS2 are Fe-rich and evolved, corresponding to residual melts after 50–60% fractional crystallization of the lobe. We suggest that the Hafnarhraun VC formed in a two-stage process. Firstly, VC forming residual melt and vapor detached as rising diapirs from ol+plg+melt+vapor mush near the lava base, and later, these VC diapirs accumulated ol phenocrysts and minor plg microphenocrysts in the lava core. HVS1 represent accumulations of VC to the viscous base of the solidifying upper crust of the lobe, and HVS2 formed as evolved vapor-saturated residual melts seeped into voids within the upper crust. Such vapor-aided differentiation, here documented for the Hafnarhraun lava, may also apply to shallow crustal magma storage zones, contributing to the formation of evolved basalts.Peer reviewe

Elemental analysis of single ambient aerosol particles using laser-induced breakdown spectroscopy

Analysing the composition of aerosol particles is essential when studying their health effects, sources and atmospheric impacts. In many environments the relevant particles occur in very low concentrations, meaning that their analysis requires efficient single particle techniques. Here we introduce a novel method to analyse the elemental composition of single aerosol particles sampled directly from the aerosol phase using size amplification aided aerosol charging (SAAC), linear electrodynamic quadrupole (LEQ) and laser-induced breakdown spectroscopy. We present results of the charging and focusing efficiencies of the SAAC and of the LEQ, and a proof-of-concept of the analysis method. The proof-of-concept test series was conducted with particle diameters down to 300 nm, sampled directly from the aerosol phase. The method shows unprecedented performance for spectroscopic submicron particle analysis from arbitrarily low concentrations and has exceptional potential for a portable analysis platform for various applications in the field of aerosol research.publishedVersionPeer reviewe

Formation of segregation structures in Hafnarhraun pāhoehoe lobe, SW Iceland: a window into crystal–melt separation in basaltic magma

Publisher's version (útgefin grein).To gain insights into crystal–melt separation processes during basalt differentiation, we have studied an 8-m-thick pāhoehoe lava lobe from the Hafnarhraun lava flow field in SW Iceland. The lobe has abundant melt segregations, porous cylindrical and sheet-like structures, generally interpreted as separated residual melts of a lava lobe. We divide these melt segregations into three types based on morphology and composition: vesicle cylinders (VC), type 1 horizontal vesicle sheets (HVS1), and type 2 horizontal vesicle sheets (HVS2). Remarkably, the studied VC are not simple residual melts generated by fractional crystallization, but their composition points to removal of plagioclase from the parental lava. HVS1 resemble VC, but have fractionated more olivine (ol) + plagioclase (plg) ± augite and have lost most, if not all, of their olivine phenocrysts. HVS2 are Fe-rich and evolved, corresponding to residual melts after 50–60% fractional crystallization of the lobe. We suggest that the Hafnarhraun VC formed in a two-stage process. Firstly, VC forming residual melt and vapor detached as rising diapirs from ol+plg+melt+vapor mush near the lava base, and later, these VC diapirs accumulated ol phenocrysts and minor plg microphenocrysts in the lava core. HVS1 represent accumulations of VC to the viscous base of the solidifying upper crust of the lobe, and HVS2 formed as evolved vapor-saturated residual melts seeped into voids within the upper crust. Such vapor-aided differentiation, here documented for the Hafnarhraun lava, may also apply to shallow crustal magma storage zones, contributing to the formation of evolved basalts.The Nordic Volcanological Center funded this work 2015–2017. We thank Robert A. Askew and Leó Kristjánsson for the aid in sampling, Atli Hjartarson and Guðmundur H. Guðfinnsson for the help in sample preparation and microprobe analyses, and Richard J. Brown for the editorial handling. Comments from Kaisa Nikkilä, Scott Rowland, and anonymous reviewer significantly improved the manuscript. Funding information: Open access funding provided by University of Helsinki including Helsinki University Central Hospital.Peer Reviewe

The effect of audiovisual speech training on the phonological skills of children with specific language impairment (SLI)

We developed a computerized audiovisual training programme for school-aged children with specific language impairment (SLI) to improve their phonological skills. The programme included various tasks requiring phonological decisions. Spoken words, pictures, letters and written syllables were used as training material. Spoken words were presented either as audiovisual speech (together with the talking face), or as auditory speech (voice alone). Two groups (10 children/group) trained for six weeks, five days per week: the audiovisual group trained with audiovisual speech, and the other group received analogically the same training but with auditory speech. Before and after training, language skills and other cognitive skills were assessed. The audiovisual group improved in a non-word-repetition test. Such improvement was not observed with auditory training. This result suggests that audiovisual speech may be helpful in the rehabilitation of children with SLI.Peer reviewe

Condensation/immersion mode ice-nucleating particles in a boreal environment

Ice-nucleating particle (INP) measurements were performed in the boreal environment of southern Finland at the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR II) in the winter-spring of 2018. Measurements with the Portable Ice Nucleation Chamber (PINC) were conducted at 242 K and 105 % relative humidity with respect to water. The median INP number concentration [INP] during a 6-week measurement period was 13 L-1. The [INP] spanned 3 orders of magnitude and showed a general increase from mid-February until early April. No single dominant local or regional sources of INPs in the boreal environment of southern Finland could be identified. Rather, it is hypothesised that the INPs detected at SMEAR II are a result of long-range transport and dilution of INPs sourced far from the measurement site. Despite high variability, the measured [INP] values fall within the range expected for the [INP] measured elsewhere under similar thermodynamic conditions. The [INP] did not correlate with any of the examined parameters during the entire field campaign, indicating that no one single parameter can be used to predict the [INP] at the measurement location during the examined time period. The absence of a correlation across the entire field campaign also suggests that a variety of particles act as INPs at different times, although it was indirectly determined that ambient INPs are most likely within the size range of 0.1-0.5 mu m in diameter on average. On shorter timescales, several particle species correlated well with the [INP]. Depending on the meteorological conditions, black carbon (BC), supermicron biological particles and sub-0.1 mu m particles, most likely nanoscale biological fragments such as ice-nucleating macromolecules (INMs), correlated with the INP signal. However, an increase in the concentration of any of these particle species may not necessarily lead to the increase in the [INP]; the reasons for this remain unknown. Limitations of the instrumental set-up and the necessity for future field INP studies are addressed.Peer reviewe

The seasonal cycle of ice-nucleating particles linked to the abundance of biogenic aerosol in boreal forests

Ice-nucleating particles (INPs) trigger the formation of cloud ice crystals in the atmosphere. Therefore, they strongly influence cloud microphysical and optical properties and precipitation and the life cycle of clouds. Improving weather forecasting and climate projection requires an appropriate formulation of atmospheric INP concentrations. This remains challenging as the global INP distribution and variability depend on a variety of aerosol types and sources, and neither their short-term variability nor their long-term seasonal cycles are well covered by continuous measurements. Here, we provide the first year-long set of observations with a pronounced INP seasonal cycle in a boreal forest environment. Besides the observed seasonal cycle in INP concentrations with a minimum in wintertime and maxima in early and late summer, we also provide indications for a seasonal variation in the prevalent INP type. We show that the seasonal dependency of INP concentrations and prevalent INP types is most likely driven by the abundance of biogenic aerosol. As current parameterizations do not reproduce this variability, we suggest a new mechanistic description for boreal forest environments which considers the seasonal variation in INP concentrations. For this, we use the ambient air temperature measured close to the ground at 4.2 m height as a proxy for the season, which appears to affect the source strength of biogenic emissions and, thus, the INP abundance over the boreal forest. Furthermore, we provide new INP parameterizations based on the Ice Nucleation Active Surface Site (INAS) approach, which specifically describes the ice nucleation activity of boreal aerosols particles prevalent in different seasons. Our results characterize the boreal forest as an important but variable INP source and provide new perspectives to describe these new findings in atmospheric models.Peer reviewe

Measurement report : Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.Peer reviewe

Measurement report : Introduction to the HyICE-2018 campaign for measurements of ice-nucleating particles and instrument inter-comparison in the Hyytiala boreal forest

The formation of ice particles in Earth's atmosphere strongly influences the dynamics and optical properties of clouds and their impacts on the climate system. Ice formation in clouds is often triggered heterogeneously by ice-nucleating particles (INPs) that represent a very low number of particles in the atmosphere. To date, many sources of INPs, such as mineral and soil dust, have been investigated and identified in the low and mid latitudes. Although less is known about the sources of ice nucleation at high latitudes, efforts have been made to identify the sources of INPs in the Arctic and boreal environments. In this study, we investigate the INP emission potential from high-latitude boreal forests in the mixed-phase cloud regime. We introduce the HyICE-2018 measurement campaign conducted in the boreal forest of Hyytiala, Finland, between February and June 2018. The campaign utilized the infrastructure of the Station for Measuring Ecosystem-Atmosphere Relations (SMEAR) II, with additional INP instruments, including the Portable Ice Nucleation Chamber I and II (PINC and PINCii), the SPectrometer for Ice Nuclei (SPIN), the Portable Ice Nucleation Experiment (PINE), the Ice Nucleation SpEctrometer of the Karlsruhe Institute of Technology (INSEKT) and the Microlitre Nucleation by Immersed Particle Instrument (mu L-NIPI), used to quantify the INP concentrations and sources in the boreal environment. In this contribution, we describe the measurement infrastructure and operating procedures during HyICE-2018, and we report results from specific time periods where INP instruments were run in parallel for inter-comparison purposes. Our results show that the suite of instruments deployed during HyICE-2018 reports consistent results and therefore lays the foundation for forthcoming results to be considered holistically. In addition, we compare measured INP concentrations to INP parameterizations, and we observe good agreement with the Tobo et al. (2013) parameterization developed from measurements conducted in a ponderosa pine forest ecosystem in Colorado, USA.Peer reviewe