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1.
The recently developed cavity attenuated phase shift particulate matter single scattering albedo (CAPS PMSSA) monitor has been shown to be fairly accurate and robust for real-time aerosol optical properties measurements. The scattering component of the measurement undergoes a truncation error due to the loss of scattered light from the sample tube in both the forward and backward directions. Previous studies estimated the loss of scattered light typically using the Mie theory for spherical particles, assuming particles are present only on the sampling tube centerline, and without accounting for the effects of sampling tube surface reflection. This study overcomes these limitations by solving the radiative transfer equation in an axisymmetric absorbing and scattering medium using the discrete-ordinates method to estimate the scattering truncation error. The effects of absorption coefficient, scattering coefficient, asymmetry parameter of the scattering phase function, and the reflection coefficient at the sampling tube inner surface were investigated. Under typical conditions of CAPS PMSSA operation of low extinction coefficients below about 5000 Mm?1, the scattering loss remains independent of the absorption and scattering coefficients but is dependent on the scattering phase function and the reflection coefficient of the sampling glass tube inner surface. The proposed method was used to investigate the effects of asymmetry parameter and surface reflection coefficient on truncation for absorbing aerosol particles whose scattering phase function can be well represented by the Henyey-Greenstein approximation. The scattering loss increases with increasing the asymmetry parameter and the surface reflection coefficient.

Copyright © 2018 National Research Council Canada  相似文献   

2.
We present laboratory and field measurements of aerosol light extinction ( σep ) using an instrument that employs Cavity Attenuated Phase Shift (CAPS) spectroscopy. The CAPS extinction monitor comprises a light emitting diode (LED), an optical cavity that acts as the sample cell, and a vacuum photodiode for light detection. The particle σep is determined from changes in the phase shift of the distorted waveform of the square-wave modulated LED light that is transmitted through the optical cell. The 3-σ detection limit of the CAPS monitor under dry particle-free air is 3 Mm–1 for 1s integration time. Laboratory measurements of absolute particle extinction cross section ( σext ) using non-absorbing, monodisperse polystyrene latex (PSL) spheres are made with an average precision of ± 3% (2-σ) at both 445 and 632 nm. A comparison with Mie theory scattering calculations indicates that these results are accurate within the 10% uncertainty stated for the particle number density measurements. The CAPS extinction monitor was deployed twice in 2009 to test its robustness and performance outside of the laboratory environment. During these field campaigns, a co-located Multi Angle Absorption Photometer (MAAP) provided particle light absorption coefficient ( σap) at 635 nm: the single scattering albedo ( ω) of the ambient aerosol particles was estimated by combining the CAPS σep measured at 632 nm with the MAAP σap data. Our initial results show the high potential of the CAPS as lightweight, compact instrument to perform precise and accurate σep measurements of atmospheric aerosol particles in both laboratory and field conditions.  相似文献   

3.
High-quality in situ observations of aerosol particle optical properties, namely extinction, scattering, and absorption, provide important information needed to constrain the role of aerosols in the climate system. This paper outlines the design and performance of an aircraft instrument utilizing cavity ringdown spectroscopy for the measurement of aerosol extinction. The 8-channel cavity ringdown spectrometer measures extinction at multiple wavelengths (405, 532, and 662 nm) and at multiple relative humidities (e.g., 10%, 70%, and 95%). Key performance characteristics include a 1-s detection limit better than 0.1 Mm?1, accuracy of <2% for dry aerosol measurements, and a 1-s precision better than 40% for extinction levels of >10 Mm?1. Laboratory and field data demonstrate that the 1-s precision is limited by the statistics of aerosol particles in the laser beam rather than the precision of the extinction measurement per se. The measurement precision improves with averaging to 5% at 60 s for extinction levels of >10 Mm?1. Field data collected during a recent airborne campaign in California, which involved eighteen research flights during May and June 2010, are used to demonstrate the in-flight performance of new instrument.  相似文献   

4.
The optical properties of soot particles in plumes emanating from a high bypass turbofan aircraft engine (V2527) were measured at distances of 40–80 m behind the engine with a cavity-enhanced phase shift (CAPS)-based extinction monitor (known as the CAPS PMex) and a multi-angle absorption photometer, both operating at wavelength ~630 nm. Integrated plume measurements from the two instruments were highly correlated with each other (r 2 > 0.99, N = 12) and with measured carbon dioxide emission concentrations. Ancillary measurements indicated that the soot particle volume-weighted mobility diameter distribution peaked at 60 nm with a full width at half maximum of ~60 nm. The soot single scattering albedo determined using the absorption and extinction measurements under engine idle conditions was 0.05 ± 0.02 (where the uncertainty represents 2σ precision), in agreement with previous measurements of aircraft exhaust. The engine soot emission index (mass soot per mass fuel burned) for this particular engine, derived from these measurements and a wavelength-specific mass absorption coefficient and the measured in-plume carbon dioxide concentrations, was 225 ± 35 mg kg?1 at engine idle conditions. These results plus more limited data collected from in-use aircraft on the runway indicate that the CAPS extinction monitor can provide (with an appropriate albedo correction) a credible measurement of the engine soot emission index in situations where the time response and sensitivity of particle absorption monitors are not otherwise sufficient.  相似文献   

5.
Abstract

Atmospheric Aerosols affect Earth’s climate directly by scattering and absorbing solar radiation. In order to study the optical properties of aerosols, we developed a broadband cavity-enhanced spectrometer that uses a supercontinuum laser source and a compact spectrometer, to measure simultaneously the extinction coefficient of aerosols over a broad wavelength region from 420 to 540?nm. The system employs a dual cavity approach with a reference and a sample cavity, accounting for changes in gases background and for laser spectral and intensity fluctuations. We tested the system with aerosolized salt particles and polystyrene latex spheres. We performed calculations using Mie theory and found good agreement with the measured extinction. We also found that the extinction coefficient of non-absorbing aerosol favorably compares with the scattering coefficient measured by a nephelometer. Finally, we generated soot particles and found an extinction Ångström exponent in good agreement with values reported in the literature. Wavelength dependent detection limits (1σ) for the instrument at 5?nm wavelength resolution and for an integration time of ~10?min were found to be in the range ~5?Mm?1 to 13?Mm?1. The broadband dual-cavity extinction spectrometer is simple and robust and might be particularly useful for laboratory measurements of the extinction coefficient of brown carbon aerosol. The laboratory tests suggest that the prototype is promising for future developments of a field-deployable instrument.

Copyright © 2020 American Association for Aerosol Research  相似文献   

6.
An evaluation of the operation and performance of a Cavity Attenuated Phase-Shift Particle Extinction Monitor (CAPS PMex) was performed for use on board commercial aircraft as part of the research infrastructure IAGOS (In-service Aircraft for a Global Observing System, www.iagos.org). After extensive laboratory testing, a new flow system, using mass flow controllers, was installed to maintain constant purge and sample flows under low and varying pressure conditions. The instrument was then tested for pressures as low as 200 hPa and evaluated against particle-free compressed air and CO2. Extinction coefficients for the studied gases were in close agreement with literature values with differences between 2.2% and 8%, proving that the CAPS technology works at low pressures. The instrument's limit of detection, with respect to 3 times the variability of the background signal for the full pressure range, was 0.2 Mm?1 for 60s integration time. During its first research aircraft operations, the IAGOS instrument prototype, composed of one CAPS PMex and one OPC, showed excellent results regarding the stability of the instruments and the potential for characterizing different aerosol types and for estimating the contribution of sub- and super-μm sized particles to aerosol light extinction.

Copyright © 2017 American Association for Aerosol Research  相似文献   

7.
A novel optical instrument has been developed that estimates size segregated aerosol mass concentration (i.e., PM 10 , PM 4 , PM 2.5 , and PM 1 ) over a wide concentration range (0.001–150 mg/m 3 ) in real time. This instrument combines photometric measurement of the particle cloud and optical sizing of single particles in a single optical system. The photometric signal is calibrated to approximate the PM 2.5 fraction of the particulate mass, the size range over which the photometric signal is most sensitive. The electrical pulse heights generated by light scattering from particles larger than 1 micron are calibrated to approximate the aerodynamic diameter of an aerosol of given physical properties, from which the aerosol mass distribution can be inferred. By combining the photometric and optical pulse measurements, this instrument can estimate aerosol mass concentrations higher than typical single particle counting instruments while providing size information and more accurate mass concentration information than traditional photometers. Experiments have shown that this instrument can be calibrated to measure aerosols with very different properties and yet achieve reasonable accuracy.  相似文献   

8.
This article describes the design and performance of a cavity ring-down spectroscopic (CRDS) instrument for measuring extinction coefficients of laboratory and ambient atmospheric aerosols. Through averaging 1000 individual waveforms, a minimum detectable aerosol extinction coefficient of 6.1×10?7 m?1 is achieved. Tests with polystyrene spheres (PSS), we suggested this CRDS system could measure the extinction coefficient of aerosol with uncertainty <3% under laboratory controlled experimental conditions. The visual range measured with CRDS agrees well with visibility observations from Shanghai Meteorological Bureau. Combined with the TSI integrating nephelometer and NOx analyzer, CRDS was used to monitor the optical properties of ambient aerosols in the heavy pollution episode. The uncertainty for using the CRDS and TSI nephelometer to measure single scattering albedo (SSA) in an ambient measurement is estimated to be <12%.  相似文献   

9.
In this study, we describe a newly developed three-wavelength differential photoacoustic spectrometer, which we denote RGB-DPAS, for aerosol absorption measurement in the visible spectral range: 671?nm (red), 532?nm (green), and 473?nm (blue). This instrument utilizes the differential photoacoustic spectrometric (DPAS) technique, which simultaneously measures light absorption signals due to total particulate matter?+?gaseous samples and those of gaseous samples alone. The difference between the photoacoustic signals recorded from the two nearly identical acoustic cells (<0.2% variability in physical dimensions) yields the aerosol photoacoustic signals at the three wavelengths. This measurement approach eliminates the interferences from light-absorbing gaseous species as well as low-frequency ambient acoustic noise. In this study, we demonstrate the linearity of the RGB-DPAS signal response to the number concentration of the synthetic carbon black particles at electrical mobility diameter (Dm) = 350?nm, which is used as a calibration surrogate. Based on the Allan variance analysis, detection limits (2σ) of 0.20?Mm?1 at 671?nm, 0.22?Mm?1 at 532?nm, and 0.90?Mm?1 at 473?nm have been achieved in 100?s data acquisition for the RGB-DPAS instrument.

Copyright © 2018 American Association for Aerosol Research  相似文献   


10.
Refractive index and optical properties of biogenic and anthropogenic secondary organic aerosol (SOA) particles were investigated. Aerosol precursors, namely longifolene, α-pinene, 1-methylnaphthalene, phenol, and toluene were oxidized in a Teflon chamber to produce SOA particles under different initial hydrocarbon concentrations and hydroxyl radical sources, reflecting exposures to different levels of nitrogen oxides (NOx). The real and imaginary components (n and k, respectively) of the refractive index at 375?nm and 632?nm were determined by Mie theory calculations through an iterative process, using the χ2 function to evaluate the fitness of the predicted optical parameters with the measured scattering, absorption, and extinction coefficients from a Photoacoustic Extinctiometer and Cavity Attenuated Phase Shift Spectrometer. Single scattering albedo (SSA) and bulk mass absorption coefficient (MAC) at 375?nm were calculated. SSA values of SOA particles from biogenic precursors (longifolene and α-pinene) were ~0.98–0.99 (~6.3% uncertainty), reflecting purely scattering aerosols regardless of the NOx regime. However, SOA particles from aromatic precursors were more absorbing and displayed NOx-dependent SSA values. For 1-methylnaphthalene SOA particles, SSA values of 0.92–0.95 and ~0.75–0.90 (~6.1% uncertainty) were observed under intermediate- and high-NOx conditions, respectively, reflecting the absorbing effects of SOA particles and NOx chemistry for this aromatic system. In mixtures of longifolene and phenol or longifolene and toluene SOA under intermediate- and high-NOx conditions, k values of the aromatic-related component of the SOA mixture were higher than that of 1-methylnaphthalene SOA particles. With the increase in OH exposure, kphenol decreased from 0.10 to 0.02 and 0.22 to 0.05 for intermediate- and high-NOx conditions, respectively. A simple relative radiative forcing calculation for urban environments at λ?=?375?nm suggests the influence of absorbing SOA particles on relative radiative forcing at this wavelength is most significant for aerosol sizes greater than 0.4?µm.

Copyright © 2019 American Association for Aerosol Research  相似文献   


11.
Aerosols directly affect Earth's climate by scattering and absorbing solar radiation. Although they are ubiquitous in Earth's atmosphere, direct, in situ, wavelength-resolved measurements of aerosol optical properties remain challenging. As a result, the so-called aerosol direct effects are one of the largest uncertainties in predictions of Earth's future climate, and new instrumentation is needed to provide measurements of the absorption of sunlight by atmospheric particles. We have developed a portable, four-wavelength, single-cell photoacoustic spectrometer for simultaneous measurement of aerosol absorption at 406, 532, 662, and 785 nm, with an additional extinction measurement at 662 nm via a built-in cavity ringdown spectrometer. The instrument, dubbed MultiPAS-IV, is compact, robust, has low power requirements, and utilizes a multipass optical arrangement to achieve typical detection limits of 0.6–0.7 Mm?1 for absorption (2σ, 2-min average). Tests with nigrosin aerosols show agreement with Mie theory calculations to within 2%, and comparison with a 7-wavelength aethalometer shows good correlation for ambient (Athens, GA, USA) aerosols. We demonstrate the utility of the broad spectral coverage and sensitivity of the MultiPAS-IV for calculating the absorption Ångström exponent of black carbon (AAEBC, median value of 0.70) in ambient aerosols and use this value to derive the brown carbon contributions to absorption at 406 nm (43%) and 532 nm (13%) and its wavelength dependence (AAEBrC = 6.3).

Copyright © 2018 American Association for Aerosol Research  相似文献   

12.
Aerosol light absorption still remains a difficult quantity to measure at the precision, accuracy and temporal resolution necessary to quantitatively bound the contribution of this direct effect on aerosol radiative forcing. These continuing difficulties are due, in part, because aerosol extinction is dominated by light scattering. In response to these and other issues, the aerosol community has been developing a new generation of instrumentation that can measure aerosol absorption without the need to deposit aerosols on a filter. Here we introduce work on the application of photothermal interferometry (PTI) towards this measurement problem. The advantages of this approach are: its complete insensitivity to aerosol scattering (true for any photothermal technique) and high sensitivity resulting from use of an interferometric technique. Using NO2 as a calibration standard, the accuracy of the PTI technique was measured to be 5% (95% confidence interval). Measurement at a 10-second time constant yields a precision of 0.2 Mm?1 (95% confidence interval) and a lower limit of detection of 0.4 Mm?1 for a sample pathlength of 5 cm. Using laboratory-generated nigrosin aerosols an intercomparison between the PTI and a 3-λ Particle Soot Absorption Photometer (PSAP) gives a slope of 0.96 ± 0.02. Acquisition of absorption coefficients for ambient aerosols reveals very good agreement between the two instruments except for periods of high relative humidity (>70%) whereupon the PSAP reports a larger absorption coefficient.  相似文献   

13.
We describe a new open-path aerosol extinction cavity ringdown spectrometer (CRDS), which measures extinction coefficients as aerosol is drawn transversely through the optical cavity. With no inlet tubing, particle losses in the open-path CRDS due to impaction of coarse particles or evaporation of highly humidified particles in transfer lines are minimized, improving aerosol extinction measurements in dusty and humid environments. This report presents the key elements of the new open-path CRDS design as well as comparisons with a conventional closed-path CRDS and data obtained during a field study at NOAA's instrumented 300 m tower in Erie, Colorado. The open-path CRDS's 1σ detection limit for one second averaged data was 0.05 Mm?1, comparable to the limit of our closed-path CRDS.

Copyright 2015 American Association for Aerosol Research  相似文献   

14.
Particle aerodynamic diameter measurement using an aerosizer (a time-of-flight (TOF) particle size measurement instrument) requires assuming the density of particle being measured. In this paper, a relationship between TOF of spherical particles with different densities through three laser beams, and the lumped parameter, Log[daeCD−1/2], is found. This allows the effect of density in particle aerodynamic diameter measurement to be minimized.  相似文献   

15.
Chemically resolved submicron (PM1) particle mass fluxes were measured by eddy covariance with a high resolution time-of-flight aerosol mass spectrometer over temperate and tropical forests during the BEARPEX-07 and AMAZE-08 campaigns. Fluxes during AMAZE-08 were small and close to the detection limit (<1 ng m?2 s?1) due to low particle mass concentrations (<1 μg m?3). During BEARPEX-07, concentrations were five times larger, with mean mid-day deposition fluxes of ?4.8 ng m?2 s?1 for total nonrefractory PM1 (Vex,PM1 = ?1 mm s?1) and emission fluxes of +2.6 ng m?2 s?1 for organic PM1 (Vex,org = +1 mm s?1). Biosphere–atmosphere fluxes of different chemical components are affected by in-canopy chemistry, vertical gradients in gas-particle partitioning due to canopy temperature gradients, emission of primary biological aerosol particles, and wet and dry deposition. As a result of these competing processes, individual chemical components had fluxes of varying magnitude and direction during both campaigns. Oxygenated organic components representing regionally aged aerosol deposited, while components of fresh secondary organic aerosol (SOA) emitted. During BEARPEX-07, rapid in-canopy oxidation caused rapid SOA growth on the timescale of biosphere-atmosphere exchange. In-canopy SOA mass yields were 0.5–4%. During AMAZE-08, the net organic aerosol flux was influenced by deposition, in-canopy SOA formation, and thermal shifts in gas-particle partitioning. Wet deposition was estimated to be an order of magnitude larger than dry deposition during AMAZE-08. Small shifts in organic aerosol concentrations from anthropogenic sources such as urban pollution or biomass burning alters the balance between flux terms. The semivolatile nature of the Amazonian organic aerosol suggests a feedback in which warmer temperatures will partition SOA to the gas-phase, reducing their light scattering and thus potential to cool the region.

Copyright 2013 American Association for Aerosol Research  相似文献   

16.
This work designed and tested a shelter to protect a passive sampler for measuring coarse particulate matter, PM 10 ? 2.5 . The shelter protects the sampler from precipitation and reduces the effects of wind on the deposition of particles to its collection surface. Six shelters were tested in a wind tunnel at three wind speeds: 2, 8, and 24 km hr ?1 . Shelter performance was expressed as the ratio of PM 10 ? 2.5 measured with the passive samplers to that measured with a filter-based dichotomous sampler. For most shelters, the PM 10 ? 2.5 ratio averaged across wind speeds was well above one (2.4 to 8.5) and was generally dependent on wind speed. However, the PM 10 ? 2.5 ratio for one shelter, the Flat Plates shelter, was 1.04 with substantially less effect on particle deposition from wind speed. Eight week-long field tests were conducted to compare PM 10 ? 2.5 measured with a passive sampler installed in a Flat Plates shelter to that measured with a collocated filter-based dichotomous sampler. In these tests, the mean PM 10 ? 2.5 ratio was 1.29. The linear relationship between PM 10 ? 2.5 measured passively to that measured with the filter-based sampler had a Pearson correlation coefficient of 0.97 and was not significantly affected by the addition of weekly mean wind speed (p = 0.35). Although temperature was significant in this regression model (p = 0.02), it only improved the relationship marginally. The passive sampler in a Flat Plates shelter offers an inexpensive means to assess ambient PM 10 ? 2.5 without on-site measurement of wind speed.  相似文献   

17.
Wearable ionization air cleaners are compact in size and marketed for personal respiratory protection by removing air pollutants from users' breathing zone. In this study, ozone emission and particle removal rates of four wearable ionization air cleaners (namely, AC1 through AC4) were evaluated inside a 0.46 m3 stainless steel chamber. Continuous measurements were conducted for ozone concentration, PM2.5 concentration, and particle size distribution in the size range of 18.1–289 nm. Two of the four wearable air cleaners (i.e., AC1 and AC2) had detectable ozone emissions. The 10-h average ozone emission rates were quite different (i.e., 0.67 mg·h?1 for AC1 and 3.40 × 10?2 mg·h?1 for AC2); however, the ozone emissions were negligible for AC3 and AC4. The number removal rates for particles within the measured size range were highly variable (i.e., 2.20 h?1, 0.52 h?1, 8.10 h?1, and 27.9 h?1 for AC1 through AC4, respectively). The corresponding mass removal rates of PM2.5 were 1.85 h?1, 0.48 h?1,1.52 h?1, and 5.37 h?1, respectively. Regulatory guidelines are needed to assure these devices can effectively remove particles without ozone emissions to protect public health.

Copyright © 2016 American Association for Aerosol Research  相似文献   

18.
A multi-wavelength photoacoustic instrument is described, which measures the wavelength dependent optical absorption coefficient (OAC) of soot or soot-containing aerosols in-situ in a range from the ultra-violet to the near-infrared region. The instrument combines a Nd:YAG disc laser (fundamental wavelength 1064 nm, harmonics at 532, 355 and 266 nm) and four photoacoustic detection cells, each purged with the same aerosol sample flow, while being irradiated with one of the four light beams. With the help of a supplementary optical arrangement to illuminate each detection cell with 532 nm light, the system is calibrated against OAC by purging the cells with known concentrations (and hereby known OAC values) of NO2. This calibration eliminates differences in sensitivity of the detection PA cells and makes the measurement of OAC absolute.The minimum detectable OAC was determined to be 0.2 Mm?1 at 1064 nm and 35.5 Mm?1 at 266 nm, corresponding to a minimum detectable black carbon mass concentration of about 0.1–1 μg/m3, depending on the wavelength. Comparison measurements with artificially generated soot aerosols showed good agreement of the device with a reference instrument, based on a long path extinction cell (LOPES).  相似文献   

19.
The objective of this study was to compare two real-time condensation particle counters for measurement of number concentrations of ultrafine particles (UFPs). The comparison is based on the data from side-by-side measurements conducted in several locations, both indoors and outdoors. CPC 3007 and P-Trak? 8525 manufactured by TSI (instruments A and B, respectively) were used simultaneously. They measure particles in sizes from 0.01 to greater than 1 μ m and 0.02 to greater than 1 μ m, respectively. The results reveal a good correlation between the two instruments. The ratios of measured aerosol concentrations varied from 0.81 to 1.17, which implies that in all data sets the difference between the two instruments was less than ± 20%. About 63% of the results were in the range of ± 10%, and about 44% showed differences less than ± 5%. The maximum particle concentration detected by instrument A was approximately 105,000 particles cm ? 3 and the minimum was about 230 particles cm ? 3 . Because of the lower particle size threshold for instrument A, it was expected that this instrument should never show concentrations lower than those detected by instrument B. This was the case in most of the measurement series. The results revealed that the concentration of UFPs changes rapidly, especially in the presence of a local UFP source. A sampling interval of 1 min is sufficient to provide substantial information about the change in concentration level.  相似文献   

20.

The size and composition of ambient airborne particulate matter is reported for winter conditions at five locations in (or near) the San Joaquin Valley in central California. Two distinct types of airborne particles were identified based on diurnal patterns and size distribution similarity: hygroscopic sulfate/ammonium/nitrate particles and less hygroscopic particles composed of mostly organic carbon with smaller amounts of elemental carbon. Daytime PM10 concentrations for sulfate/ammonium/nitrate particles were measured to be 10.1 μ g m?3, 28.3 μ g m?3, and 52.8 μ g m?3 at Sacramento, Modesto and Bakersfield, California, respectively. Nighttime concentrations were 10–30% lower, suggesting that these particles are dominated by secondary production. Simulation of the data with a box model suggests that these particles were formed by the condensation of ammonia and nitric acid onto background or primary sulfate particles. These hygroscopic particles had a mass distribution peak in the accumulation mode (0.56–1.0 μ m) at all times. Daytime PM10 carbon particle concentrations were measured to be 9.5 μ g m?3, 15.1 μ g m?3, and 16.2 μ g m?3 at Sacramento, Modesto, and Bakersfield, respectively. Corresponding nighttime concentrations were 200–300% higher, suggesting that these particles are dominated by primary emissions. The peak in the carbon particle mass distribution varied between 0.2–1.0 μ m. Carbon particles emitted directly from combustion sources typically have a mass distribution peak diameter between 0.1–0.32 μ m. Box model calculations suggest that the formation of secondary organic aerosol is negligible under cool winter conditions, and that the observed shift in the carbon particle mass distribution results from coagulation in the heavily polluted concentrations experienced during the current study. The analysis suggests that carbon particles and sulfate/ammonium/nitrate particles exist separately in the atmosphere of the San Joaquin Valley until coagulation mixes them in the accumulation mode.  相似文献   

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