Abstract

Abstract. Atmospheric aerosol is a key component of the chemistry and climate of the Earth's atmosphere. Accurate measurement of the concentration of atmospheric particles as a function of their size is fundamental to investigations of particle microphysics, optical characteristics, and chemical processes. We describe the modification, calibration, and performance of two commercially available, Ultra-High Sensitivity Aerosol Spectrometers (UHSASs) as used on the NASA DC-8 aircraft during the Atmospheric Tomography Mission (ATom). To avoid sample flow issues related to pressure variations during aircraft altitude changes, we installed a laminar flow meter on each instrument to measure sample flow directly at the inlet as well as flow controllers to maintain constant volumetric sheath flows. In addition, we added a compact thermodenuder operating at 300 ∘C to the inlet line of one of the instruments. With these modifications, the instruments are capable of making accurate (ranging from 7 % for Dp < 0.07 µm to 1 % for Dp > 0.13 µm), precise (< ±1.2 %), and continuous (1 Hz) measurements of size-resolved particle number concentration over the diameter range of 0.063–1.0 µm at ambient pressures of > 1000 to 225 hPa, while simultaneously providing information on particle volatility. We assessed the effect of uncertainty in the refractive index (n) of ambient particles that are sized by the UHSAS assuming the refractive index of ammonium sulfate (n= 1.52). For calibration particles with n between 1.44 and 1.58, the UHSAS diameter varies by +4/−10 % relative to ammonium sulfate. This diameter uncertainty associated with the range of refractive indices (i.e., particle composition) translates to aerosol surface area and volume uncertainties of +8.4/−17.8 and +12.4/−27.5 %, respectively. In addition to sizing uncertainty, low counting statistics can lead to uncertainties of < 20 % for aerosol surface area and < 30 % for volume with 10 s time resolution. The UHSAS reduction in counting efficiency was corrected for concentrations > 1000 cm−3. Examples of thermodenuded and non-thermodenuded aerosol number and volume size distributions as well as propagated uncertainties are shown for several cases encountered during the ATom project. Uncertainties in particle number concentration were limited by counting statistics, especially in the tropical upper troposphere where accumulation-mode concentrations were sometimes < 20 cm−3 (counting rates ∼ 5 Hz) at standard temperature and pressure.

Highlights

  • The concentration of particles as a function of size is fundamentally related to both direct and indirect effects of aerosol on climate

  • Measurements of particle volatility help identify the contribution of secondary particles formed in the free troposphere (FT) to the budget of cloud condensation nuclei (CCN)-sized particles in the marine boundary layer (MBL), and how this contribution varies with altitude and location in the remote atmosphere

  • The modified flow system of the Ultra-High Sensitivity Aerosol Spectrometers (UHSASs) allowed direct monitoring of the sample flow rate and eliminated flow measurement issues associated with the pressure variations during aircraft altitude changes

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Summary

Introduction

The concentration of particles as a function of size is fundamentally related to both direct (aerosol–radiation) and indirect (aerosol–cloud) effects of aerosol on climate. The ground-type UHSAS instruments were chosen for this study over the wing-mounted version because we wished to dry the air sample and to install a thermodenuder used to distinguish non-volatile particles. We describe modifications to the ground-based UHSAS for airborne operation, detail the installation of a compact thermodenuder in a second UHSAS for aerosol volatility studies, and evaluate the accuracy, precision, and in-flight performance of both UHSAS instruments during the first two of four ATom airborne campaigns. By operating two well-calibrated UHSAS instruments, one with a thermodenuder (UHSAS-1) and one without (UHSAS-2), the size-dependent particle volatility can be determined continuously, which is useful for airborne sampling where fast time response is needed. Measurements of particle volatility help identify the contribution of secondary particles formed in the free troposphere (FT) to the budget of CCN-sized particles in the marine boundary layer (MBL), and how this contribution varies with altitude and location in the remote atmosphere

Operating principles
Modified flow system
Aerosol generation method
Atomized aerosol and DMA
Flow tube reactor and DMA
The effect of composition on particle sizing
Particle detection efficiency
The effect of concentration on particle counting
The effect of pressure on sample flow and particle sizing
Thermodenuder
Design
Thermodenuder performance
Uncertainties due to refractive index
Uncertainties due to flow and pressure
Uncertainties due to counting statistics
Uncertainties due to instrument stability and calibration repeatability
Total uncertainties
In-flight performance
Measurements of non-volatile aerosol fraction
Findings
Summary and context
Full Text
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