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Journal of Atmospheric and Solar-Terrestrial Physics 71 (2009) 477485

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Journal of Atmospheric and Solar-Terrestrial Physics


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Measurements of meteor smoke particles during the ECOMA-2006 campaign: 1. Particle detection by active photoionization
Markus Rapp , Irina Strelnikova
Department of Radar Soundings and Sounding Rockets, Leibniz-Institute of Atmospheric Physics, University of Rostock, Schlosstr. 6, 18225 Kuhlungsborn, Germany

a r t i c l e in fo
Article history: Accepted 2 June 2008 Available online 12 June 2008 Keywords: Meteor smoke particles In situ measurements

abstract
We present a new design of an in situ detector for the study of meteor smoke particles (MSPs) in the middle atmosphere. This detector combines a classical Faraday cup with a xenon-ashlamp for the active photoionization/photodetachment of MSPs and the subsequent detection of corresponding photoelectrons. This instrument was successfully launched in September 2006 from the Andya Rocket Range in Northern Norway. A comparison of photocurrents measured during this rocket ight and measurements performed in the laboratory proves that observed signatures are truly due to photoelectrons. In addition, the observed altitude cut-off at 60 km (i.e., no signals were observed below this altitude) is fully understood in terms of the mean free path of the photoelectrons in the ambient atmosphere. This interpretation is also proven by a corresponding laboratory experiment. Consideration of all conceivable species which can be ionized by the photons of the xenon-ashlamp demonstrates that only MSPs can quantitatively explain the measured currents below an altitude of 90 km. Above this altitude, measured photocurrents are most likely due to photoionization of nitric oxide. In conclusion, our results demonstrate that the active photoionization and subsequent detection of photoelectrons provides a promising new tool for the study of MSPs in the middle atmosphere. Importantly, this new technique does not rely on the a priori charge of the particles, neither is the accessible particle size range severely limited by aerodynamical effects. Based on the analysis described in this study, the geophysical interpretation of our measurements is presented in the companion paper by Strelnikova, I., et al. [2008. Measurements of meteor smoke particles during the ECOMA-2006 campaign: 2. results. Journal of Atmospheric and Solar-Terrestrial Physics, this issue, doi:10.1016/ j.jastp.2008.07.011]. & 2008 Elsevier Ltd. All rights reserved.

1. Introduction Meteor smoke particles (MSPs) are thought to be formed by the recondensation of metal- and silicon-containing molecules originating from the ablation of meteoroids in the 70120 km altitude range (Plane, 2003). Starting with the 1960s, model studies suggested that MSPs should exist in the mesosphere/lower thermosphere with number densities of up to 104 particles=cm3 and corresponding radii ranging from the sub-nanometer range to a few nanometers (Rosinski and Snow, 1961; Hunten et al., 1980). Despite these tiny dimensions, it has been suggested that MSPs are involved in a variety of atmospheric processes such as the nucleation of mesospheric ice clouds, heterogeneous chemistry, and the formation of nitric acid trihydrate (NAT)-particles in polar stratospheric clouds which are involved in ozone destruction in

Corresponding author. Tel.: +49 38293 68200; fax: +49 38293 6850.

E-mail address: rapp@iap-kborn.de (M. Rapp). 1364-6826/$ - see front matter & 2008 Elsevier Ltd. All rights reserved. doi:10.1016/j.jastp.2008.06.002

the polar spring (e.g., Rapp and Thomas, 2006; Summers and Siskind, 1999; Voigt et al., 2005). Despite obvious interest in MSPs, measurements of such particles have proven difcult so that today only a few measured altitude proles are available from charged particle measurements on sounding rockets (Schulte and Arnold, 1992; Gelinas et al., 1998; Horanyi et al., 2000; Croskey et al., 2001; Lynch et al., 2005; Rapp et al., 2005; Amyx et al., 2008) and from incoherent scatter radar experiments (Rapp et al., 2007; Strelnikova et al., 2007). Most of these earlier in situ measurements used Faraday cupbased instruments based on the original design of Havnes et al. (1996) who was the rst to detect charged (ice) particles in the polar summer mesopause region. For this type of detector, however, it has become clear in the meantime that it possesses a severely limited detection efciency for the smallest MSPs (i.e., below $12 nm) and for which the smallest detectable radius even varies with altitude as a consequence of aerodynamics (Horanyi et al., 1999; Rapp et al., 2005; Hedin et al., 2007). In addition, it has recently been speculated that such

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measurements which rely on the impact of particles on the detector electrode may be inuenced by secondary charging effects such as fragmentation and triboelectric charging (Barjatya and Swenson, 2006; Havnes and Naesheim, 2007; Amyx et al., 2008). Measurements with incoherent scatter radars, on the other hand, have so far only proven to be feasible with the most powerful incoherent scatter radar, i.e., the Arecibo radar, whereas measurements with even the EISCAT UHF radar were only indicative of the existence of MSPs (Rapp et al., 2007). In addition, even with the Arecibo radar, measurements could only be performed at altitudes with sufcient D-region ionization, i.e., in daytime and above $85 km (Strelnikova et al., 2007). Hence, it is obvious that new measurements which should cover a larger altitude range and which should be able to detect MSPs of all sizes are highly desirable. In the current manuscript, we present the concept and rst results of a new rocket borne particle detector which uses active photoionization to measure the concentration of MSPs and hence largely avoids limitations from aerodynamics and secondary charging effects and does not depend on the a priori charge of the particles. In Section 2 we introduce the basic design of this detector. Initial results from a rocket ight during the ECOMA2006 campaign (ECOMA existence and charge state of meteor smoke particles in the middle atmosphere) are presented in Section 3. These ight data are then discussed in the scope of laboratory measurements in Section 4.1 and with respect to contamination from other ionizable species (like nitric oxide) in Section 4.2. The geophysical results from the discussed rocket ight are presented in the companion paper by Strelnikova et al. (2008).
Fig. 1. Photo and schematic of the ECOMA-particle detector. See text for details.

2. Instrument description The particle detector applied for the current study is a combination of a Faraday cup and a xenon-ashlamp for the photoionization of particles. A photo of the instrument together with a schematic of the detector is shown in Fig. 1. The design of the Faraday cup itself is very close to the original design of Havnes et al. (1996) who were the rst to detect charged nanoparticles (in their case consisting of water ice) in the mesosphere. The Faraday cup comprises a collector electrode (held at payload potential by the negative feedback loop of the electrometer) for the measurement of particles of either positive or negative charge and two shielding grids (biased at 6:2 V relative to payload potential) to shield the collector electrode from ambient thermal electrons and ions. Note that unlike these thermal electrons and ions the particles have a much larger mass such that their kinetic energy (i.e., 1 mp v2 where mp is the particle r 2 mass and vr is the rocket velocity) is large enough to penetrate the potential barrier set by the shielding grids. The novelty of this instrument, however, is the combination of the Faraday cup design with a xenon-ashlamp. The ashlamp is a commercially available lamp (Perkin Elmer FX1162, see http:// optoelectronics.perkinelmer.com for technical details) which we operate at a repetition rate of 20 Hz with an energy per ash of 0.5 J. The broadband spectrum of each ash contains a sufciently large number of UV photons down to a minimum wavelength of $110 nm corresponding to a maximum photon energy of 11.3 eV (see Fig. 2). The UV photons may now create photoelectrons by photoionization and/or photodetachment of an electron from a neutral/negatively charged species with sufciently low work function (or electron afnity) which may in turn be detected at the detector electrode as a short charge pulse. We note that instruments employing lamps to actively ionize atmospheric

constituents were applied earlier (e.g., Croskey et al., 2003, and references therein). In order to be able to record both the continuous charge signal from the naturally charged MSPs which are large enough to penetrate to the detector electrode and the very short charge pulses excited by the UV ash, we have chosen to operate the electrometer in the so-called integrate and dump mode. This has the advantage that even the smallest charge signatures are not missed provided the noise level of the electrometer is sufciently low. This means that the electrometer is in fact operated as an integrator which has to be discharged shortly before a ash. The charge pulse created by the ash is then integrated by an inverting amplier (i.e., a positive charge leads to a negative slope registered by the integrator) and the resulting signal is digitized by a 16 bit analog-to-digital converter. In addition to the charge pulse, the amplier also samples any existent DC-current due to naturally charged particles of either polarity. In order to properly sample the shape of the UV-created charge pulses on the one hand and to measure the rather small DC-currents due to naturally charged particles on the other hand, we sample the output signal of the integrator at two sampling frequencies: the charge pulsewhich originates from an effective ionized volume between 2.5 cm (photoelectrons from closer distances are actually in the shadow of the ashlight itself and cannot reach the electrode) and 70 cm upstream of the detectorhas a typical duration of o0:5 ms and is sampled with 100 kS/s (=kilosamples/second), stored in a memory, and subsequently transmitted to ground by telemetry in non-real time (note, however, that the start time of each such data dump is exactly dened). DC-currents, however, are sampled with 1 kS/s and transmitted to ground in real time (note that the rst sample of this signal also contains the charge pulse, however, at a much poorer temporal resolution). If the integrator reaches its positive or negative maximum value it is automatically discharged such that

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Fig. 2. Spectrum of the xenon-ashlamp in the UV wavelength range measured with a plane grating vacuum spectrometer. Note that the cut-off at 110 nm is due to the transmission properties of the window of the ashlamp.

this amplier setup provides the capability to continuously measure a broad current range, i.e., from the sub-picoamp to the 0:5 mA range. Finally, after 50 ms (i.e., shortly before the next ash) the next discharge of the integrator is initiated and the whole sequence starts from the beginning. As applied to the measurement of MSPs, the conceptual idea behind our particle detector may be summarized as follows: In Fig. 3 we have sketched the particle size distribution of MSPs as predicted by microphysical models (Hunten et al., 1980; Megner et al., 2006). In this size distribution, particles with radii larger than a minimum radius (here indicated by the vertical blue line) may be directly detected by particle impact and subsequent charge deposition at the collector electrode of the Faraday cup. Particles with radii smaller than this minimum radius may not be detected because of aerodynamic effects on their trajectories (e.g., Rapp et al., 2005; Hedin et al., 2007). All of the particles, however, may be photoionized and corresponding photoelectrons may be detected as a charge pulse. Hence, the particle detector provides information on the number density of charged particles which are larger than a certain threshold size and on the total number density of all MSPs. Note that rst results of conventional Faraday cup measurements with this instrument from a rocket ight in October 2004 were already presented in Rapp et al. (2005). At that time, however, the photoelectron measurements with the detector were impaired by electromagnetic interference from the ashelectronics and could not be used. In the present manuscript, we will focus on new measurements obtained in September 2006 during which photoelectron measurements yielded high quality data. In the following section we will present actual data from this rocket ight with which we will demonstrate the feasibility of the detector concept described above.

3. Atmospheric measurements In September 2006, the ECOMA-2006 campaign was conducted from the North-Norwegian Andya Rocket Range 69 N. ECOMA

( existence and charge state of MSPs in the middle atmosphere) is an international research program led by the Leibniz Institute of Atmospheric Physics in Germany and the Norwegian Defence Research Establishment in Norway (with additional contributions from Austria, Sweden, and the USA) dedicated to the study of MSPs and their atmospheric environment. Besides the particle detector described in the preceding section, the payload carried instruments to characterize the D-region plasma, a particle sampler for the in-ight collection of MSPs, and instruments to measure neutral air density, temperature, and turbulence. The atmospheric background state was monitored by means of the EISCAT UHF and VHF radars, the ALOMAR RMR lidar, and the ALOMAR sodium lidar. An overview of all measurements obtained during the campaign along with a more detailed description of all involved instruments is presented in the companion paper by Strelnikova et al. (2008). In this manuscript, however, our focus is on the ight performance of the ECOMA particle detector. The ECOMA-01 payload was launched on September 8, 2006 at 22:17:00 UT and reached an apogee of 130.6 km. During the entire rocket ight the particle detector worked nominally and provided data in both data channels. In order to demonstrate the quality of these measurements we present an arbitrarily chosen raw data sample from about 83:95 0:05 km on the upleg part of the rocket ight. In Fig. 4, the black symbols and lines show the charge signal from the integrator circuit in digital units (du). The red symbols and lines are corresponding currents derived by taking the time derivative of the integrator output and taking into account that 1 du corresponds to a charge of 0.18 fC. Blue vertical lines indicate the times when the integrator was discharged after which a ash was triggered. The upper panel shows results from the 1 kHz data channel which primarily records charge signatures and currents due to the impact of particles on the collector electrode. In the lower panel, corresponding signals from the fast (100 kHz) data channel are shown which clearly show the pulse due to photoelectrons with an amplitude of $ 4:5 nA on top of a smooth DC-background, in this case of about 50 pA. Note that the photoelectron current due to the ash is certainly also recorded in the slow data channel, however, due to its poorer

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Fig. 3. Sketch of the particle size distribution of meteor smoke particles as predicted by microphysical models (Hunten et al., 1980; Megner et al., 2006). The blue vertical line indicates that only a part of the size distribution may be detected by direct particle impact in a particle detector due to aerodynamical effects on the trajectories of small particles (e.g., Rapp et al., 2005; Hedin et al., 2007). All of the particles, however, may be photoionized and corresponding photoelectrons may be detected as a charge pulse.

Fig. 5. Overview of current measurements from the ECOMA ight on September 8, 2006. Left panel: current measurements due to direct particle impacts on the electrode recorded as a DC-current in the slow data channel. Right panel: corresponding peak photoelectron currents recorded in the fast data channel. Black lines are for upleg measurements, red lines are for downleg.

Fig. 4. Raw data samples for the slow (i.e., 1 kHz, upper panel) and fast data channel (i.e., 100 kHz, lower panel) from an altitude of $83:95 km on the upleg part of the rocket trajectory. The blacksymbols and lines show the charge signal from the integrator circuit in digital units (du). The red symbols and lines are corresponding currents derived by taking the time derivative of the integrator output. Blue vertical lines indicate the times when the integrator is discharged after which the ash is triggered. Note that a positive slope in the integrator output indicates a negative current, in this case of about 50 pA. Note further that the photoelectron current due to the ash is also recorded in the slow data channel, however, due to its poorer time resolution, its peak value is not captured.

time resolution, its peak value is not captured (though the recorded charge signal is certainly the same). From the raw data of the type described above, we have now determined the background DC-currents from the slow data channel (where the rst sample after each ash which contains the additional charge due to photoelectrons has been omitted) and the maximum current from each photoelectron pulse due to the xenon-ash from the fast data channel. Corresponding altitude proles are presented in Fig. 5 for both the upleg and downleg part of the rocket ight. The background measurements of the particle charge (left panel in Fig. 5) reveal a prominent negative current layer in the altitude range between 80 and 90 km indicative of negatively charged particles. This layer is qualitatively very similar to the previous measurements by Faraday cup instruments reported, e.g., by Lynch et al. (2005) and Rapp et al. (2005). A striking difference to the Rapp et al. (2005) results is, however, the opposite polarity of the particle charge. As discussed

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in detail in Strelnikova et al. (2008), the major difference between these two ights is the much larger background ionization and a different electrode material in 2006 which might have caused potential differences in triboelectric charging. Above the negative layer, the current turns positive and even shows a very prominent positive peak at $93 km which is the altitude where the EISCAT radars observed a sporadic E-layer (see Strelnikova et al., 2008, for details). It is interesting to note that Horanyi et al. (2000) observed a similar morphology with a broad negative layer below a narrow positive layer which they interpreted as a sudden E-layer related to the deposition of meteoric metal ions. In our case, however, the positive peak is also seen on the downleg of the rocket ight when the instrument is not facing the ram (and no particles can enter the detector volume). Hence, we conclude that these currents must be due to contamination by positive ions. These measurements will be further discussedfor example with respect to the observed particle charge and triboelectric effectsin the companion paper by Strelnikova et al. (2008). Here, we now focus on the measurements due to the ash of the detector as shown in the right panel of Fig. 5. On upleg, large currents of up to 10 nA were recorded above an altitude of $80 km. This current decays to about 2 nA at apogee but never returns to zero. On downleg, the measured current shows a similar behavior with slightly enhanced values from apogee down to 80 km. The largest difference, however, is that on downleg the (negative) current further increases with decreasing altitude until it reaches a maximum value of 15 nA at $75 km and disappears at about 60 km, i.e., about 20 km lower than on upleg. In the next section we will critically discuss the following questions: (1) Is it possible to prove that the recorded currents in the fast data channel (called photo-currents hereafter) are indeed due to photoelectrons? (2) Is it possible to understand the differences of the recorded photo-currents on upleg and downleg? (3) And nally: Is it possible to show that the observed photocurrents originate from MSPs particles and not from other ionizable species such as nitric oxide, excited oxygen, or metal atoms?

Fig. 6. Setup of laboratory measurements to identify the origin (and other properties) of the recorded currents due to the xenon-ash. The ECOMA-particle detector is brought into a vacuum chamber and ashes at a conical target coated with aluminum. The electrode voltage with respect to the vacuum chamber was varied between 8 V in order to determine the kinetic energy of the recorded photoelectrons (retarding eld method).

Fig. 7. Comparison of recorded current pulses due to photoelectrons produced by the Xe-ash from the actual rocket ight (red curve) and laboratory measurements (black curve).

4. Discussion 4.1. Laboratory experiments In order to answer questions 1 and 2 raised in Section 3 we devised a laboratory experiment as sketched in Fig. 6. The ECOMA particle detector was mounted inside a large vacuum chamber which was evacuated to a pressure below 104 mbar. Opposite the detector we mounted a conical target coated with an aluminum surface shaped such that ash photons emitted by the xenonashlamp of the detector were not reected back towards the collector electrode. In consequence, currents due to unwanted photoemission from the collector electrode could be avoided. UV photons from the xenon-ash, however, were sufciently energetic (maximum energy 11.3 eV, see Section 2) to create photoelectrons at the surface of the aluminum target (workfunction 4.2 eV), part of which were then ying towards the collector electrode. A typical current pulse recorded during such measurements along with a current pulse recorded during the rocket ight in September 2006 is presented in Fig. 7. Obviously, both pulses, i.e., from the laboratory experiment and from the rocket ight, have exactly the same shape (note that the coincidence in amplitude is certainly by chance and is not meant to imply that

the two pulses have exactly the same origin) which indicates that the pulses recorded during the rocket ight are indeed photoelectrons emitted by an ionizable species (see Section 4.2 below for arguments that these species must have been MSPs in most of the altitude range where photo-currents were observed). Note further that we were able to verify that the signals recorded in the laboratory were due to photoelectrons by varying a retarding potential between the target and the collector electrode. As expected for photoelectrons, the signal dropped to zero when the retarding potential reached a value of $ 6 V, i.e., at the expected kinetic energy of the photoelectrons ( flash energy minus work function). Note further that we also studied the effect of the potentials of the shielding grids on the collection of the photoelectrons. This showed that the potentials of the two grids only had a negligible effect on the collection of the photoelectrons indicating that the rejection of electrons in the eV energy range by this grid type is poor. Note, however, that another experiment in which we tested the rejection of thermal electrons (energy o0:1 eV) in a plasma chamber revealed that the rejection efciency of these was close to 100%. Finally, we used the laboratory setup described above to study the pressure dependence of the recorded photocurrents. I.e., we varied the stationary pressure in the vacuum chamber between 104 and 1 mbar and measured the maximum current due to photoelectrons emitted from the target. The results from this experiment are shown in the upper panel of Fig. 8. This indicates

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we nd that laboratory and ight results are in excellent agreement. Note that we may ignore the effect of the rather weak compression in the rst few centimeters upstream of the detector on the creation of photoelectrons because the rst 2.5 cm of the ionization volume are actually in the shadow of the ashlight such that photoelectrons from this volume can never reach the detector electrode (see Hedin et al., 2007 and our discussion of the effective ionization volume above). As for the downleg measure ments, the Lubken (1999)-climatology predicts a pressure of 0.24 mbar at 60 km altitude. During this part of the rocket ight, however, the particle detector is in the wake, for which Monte Carlo simulations by Gumbel (2001) predict that the pressure should be reduced by about a factor of 2. Hence, on downleg, the current due to photoelectrons vanishes at a pressure of about 0:5 0:24 mbar 0:12 mbar, which is again almost exactly the pressure predicted by our laboratory experiments. Hence, the difference in the photoelectron measurements between upleg and downleg can be completely understood on the basis of the pressure dependence of the mean free path of the photoelectrons in the environment of the particle detector and its modication by the aerodynamics of the rocket ight. Interestingly, this analysis shows that the altitude range over which our method is capable of detecting signatures from ionizable species like meteor smoke particles is enhanced by$20 km on the downleg part of the rocket ight when the detector is in the wake.
Fig. 8. Upper panel: pressure dependence of the photoelectron current recorded in the laboratory (black symbols with blue error bars). The red lines are drawn to guide the eye. Lower panel: results of the calculation of the mean free path of a photoelectron in air as a function of air pressure.

4.2. Ionization of other species than MSPs After we have demonstrated that the photocurrents recorded in our fast data channel are indeed due to photoelectrons excited by the photons of the xenon-ash, we now turn to the question if these photoelectrons truly originate from MSPs or from some other species. In order to answer this question, a survey of middle atmospheric species and corresponding threshold energies for either photoionization of a neutral molecule or an atom (i.e., the ionization potential), or for the photodetachment of an electron from a negative ion (i.e., the electron afnity) reveals a list of candidates which we have summarized in Table 1. These candidates are nitric oxide (NO), excited molecular oxygen O2 1 Dg , the metal atoms Fe and Na, and the negative ions NO , 3 CO , and O . Note that also other metal atoms like K, Ca, Mg, and 3 2 Si have sufciently low ionization potentials, however, for the calculations below we restrict ourselves to the case of Fe and Na which are by far the most abundant metal atoms in altitude range of interest (e.g., Plane, 2003). In order to judge whether the recorded photocurrents could be due to these species, we have tried to estimate the expected currents based on altitude proles of their concentrations (see Fig. 9) and their properties with respect to photoionization/photodetachment (see Table 1). NO number densities have been taken from the HALOE-climatology of Siskind et al. (1998), O2 1 Dg number densities from the rocket measurements by Gumbel et al. (1998), metal atom proles are from Plane (2003), and number densities of negative ions are taken from the model study of Thomas and Bowman (1985). As for the meteor smoke particles, hypothetical proles of number densities of MSPs of different sizes have been taken from the model study by Megner et al. (2006). References for corresponding photoionization cross sections and threshold energies are provided in Table 1. The photoionization/photodetachment cross sections of MSPs with radius r p at photon wavelength l are estimated using Mietheory, i.e.,

that for pressures below $102 mbar, all photoelectrons can reach the collector electrode and are not affected by collisions with gas molecules. At higher pressures, however, the current due to photoelectrons drops until at $0:1 mbar no more photoelectrons can be detected. The reason for this behavior can be understood by considering the lower panel in Fig. 8. This gure shows calculations of the mean free path of an electron in air as a function of pressure. A pressure of 102 mbar corresponds to a mean free path of $5 cm, which is about the dimension of our particle detector. For lower pressures, the mean free path of a photoelectron is hence sufciently large such that it can be detected in our instrument without undergoing collisions with gas molecules. For higher pressures, however, collisions with gas molecules lead to the loss of a part of the photoelectrons until at a pressure of 0.1 mbar the mean free path has dropped by about a factor of 10 and no more photoelectrons can reach the collector electrode. We now come back to the results from our rocket ight, showing that on upleg the minimum altitude for photoelectron detection was 80 km, whereas it decreased to 60 km on downleg. Taking into account the laboratory measurements shown in Fig. 8, this can be explained as follows: On upleg, the instrument is facing the ram such that the pressure inside the instrument is enhanced because of the aerodynamical compression of the ambient air. Monte Carlo simulations for a cup-like detector geometry as well as calculations using the RayleighPitot formula imply that for a rocket ight with an apogee of 130 km the pressure should increase by about a factor of 13 at an altitude of 80 km (see Fig. 7 in Rapp et al., 2001). Using the densities and temperatures for the beginning of September from the climatol ogy of Lubken (1999) this implies that at 80 km, the pressure should have been 13 102 mbar 0:13 mbar. Comparing this pressure to the pressure for which our laboratory measurements show that the photoelectron-current should have dropped to zero,

sMSP rp ; l pr2 Q abs rp ; l; nl; kl Y p photo

(1)

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Table 1 Electron production by photoionization/photodetachment Species NO O2 1 D g Na Fe NO 3 CO 3 O 2 Threshold energy (eV) 9.25 11.1 5.14 7.87 3.90 2.90 0.43 Threshold wavelength (nm) 134.0 111.8 241.0 157.5 317.9 427.6 2883.6 Cross section cm2 1 1018 2 1018 1 1019 2 1018 1 1019 1 1018 1 1018 Reference Watanabe et al. (1953) Clark and Wayne (1970) Bautista et al. (1998) Kelly and Ron (1971) Smith et al. (1979) Cosby et al. (1976) Cosby et al. (1976)

Fig. 9. Altitude proles of the concentration of constituents in the mesosphere/ lower thermosphere which could potentially be photoionized, or from which an electron could be photodetached. Concentrations of sodium and iron atoms (black lines) are taken from Plane (2003), of nitric oxide (blue line) from Siskind et al. (1998) for 70 N and equinox conditions, O2 (1 Dg ) number densities (yellow line) are from Gumbel et al. (1998), number densities of negative ions (red lines) from Thomas and Bowman (1985), and of meteor smoke particles (green lines) from Megner et al. (2006).

value of r min is not critical for the value of Imax because these smallest particles contribute only weakly to the overall current since sMSP / r 3 . Furthermore, ve is the velocity of a photoelecp photo tron, Dt 10 ms is the sampling interval in the fast data channel (and hence also the charge integration time of our integrator circuit), h is Plancks constant, c is the speed of light, and W p is the threshold energy for photoionization/photodetachment of a particle, i.e., the workfunction or electron afnity of the corresponding material. dF=dl is the number of photons per wavelength interval emitted in one ash and l is the distance from 2 the particle detector. P S=4pl is the probability that the photoelectron is emitted towards the detector electrode with area S. dNp =dr p is the number density of MSPs per size interval dr p , and dl and dl are the length and wavelength elements over which the integrations above are carried out. Finally, e is the charge of an electron. Note that the integration over the wavelength l starts at 110 nm because of the transmission properties of the MgF2 -window of the Xe-ashlamp. Likewise, photocurrents due to photoionization/photodetachment of the species in Table 1 can be calculated as ! dF e si l P ni dl dl Dt 2:5 cm 110 nm dl ! Z ve Dt e F i si ni P dl tot Dt 2:5 cm Z
ve Dt

where Q abs is the Mie absorption efciency which we calculated using the publicly available Mie-code from the text book by Bohren and Huffman (1983), n and k are the real and imaginary parts of the refractive index of the MSP material, and Y is the quantum yield for photoemission/photodetachment. Guided by the experimental nding that the yields of nanoparticles may reach very large values which are up to three orders of magnitude larger than the yields for the corresponding bulk material (e.g., Schmidt-Ott et al., 1980; Muller et al., 1991) and in order to derive upper estimates of the currents that we may expect, we have chosen a value of Y 1:0 for our calculations. Finally, following Plane (2003) who argues that MSPs should be some sort of iron or silicon oxides, we consider refractive indices for Fe2 O3 and SiO, respectively (see http://www.astro.uni-jena.de/Laboratory/OCDB/oxsul.htm and http://luxpop.com/RefractiveIndexList. htm, for corresponding internet data bases). Assuming that only single photoelectrons are emitted, that the photoemission/photodetachment processes are independent, and nally that the maximum charge is collected by the electrode during the duration of the rst sampling interval after the ash, we estimate the corresponding maximum currents as IMSP max Z
1

Imax %

hc=W i

(3) (4)

ve Dt

hc=W p

 dF MSP e sphoto r p ; l P dr p dl dl dl Dt

r min

2:5 cm

110 nm

dN p dr p

(2)

where r min 0:2 nm is the minimum assumed size of MSPs following the original proposal of Hunten et al. (1980) and taking into account the argument that immediate re-condensation in a meteor trail is highly unlikely (Plane, 2000). Note that the exact

where ni is the number density of species i, si l is the cross section for photoionization/photodetachment of species i at wavelength l, and W i is the corresponding threshold energy (i.e., workfunction or electron afnity). Note that for approximation (4) we have assumed that R dF=dlsi l dl may be approximated as F i si where F i is tot tot the total number of photons emitted in one ash with an energy larger than W i and si is the average cross section over the corresponding wavelength interval. Altitude proles of expected maximum currents based on Eqs. (2) and 4 and the altitude proles shown in Fig. 9 assuming either Fe2 O3 or SiO particles are presented in Fig. 10. This gure clearly shows that photoionization/photodetachment of MSPs quantitatively explains the observed photocurrents. In contrast, however, potential contributions to the detected photocurrents from the photoionization of metal atoms or from the photodetachment of negative ions reach maximum currents of o1 pA and can hence be safely ignored. Even in the case of O2 1 Dg , which is by far the most abundant of the considered species, we see that expected currents reach a maximum of $100 pA. This is still a factor of 10100 less than the currents observed during our rocket ight (gray shaded area). Likewise, currents due to NO can only dominate the measurements above an altitude of $90 km. In the companion paper by Strelnikova et al. (2008) we will come back to this point and try to estimate the actual NO density above

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Fig. 10. Expected maximum currents to be detected due to photoelectrons from photoionization/photodetachment from the species shown in Fig. 9 by the ECOMAparticle detector and assuming Fe2 O3 or SiO particles. The violet (green) solid lines show results assuming photodetachment from Fe2 O SiO particles for an 3 electron afnity of 2 eV (Wang et al., 1996). The corresponding dashed lines show corresponding results assuming photoionization of neutral particles with a workfunction of 5.5 eV. The gray shaded area in each panel indicates the range of currents observed by the ECOMA-particle detector.

90 km on the basis of our measured photocurrents. Below 90 km, however, measured photocurrents can only be explained by photoionization/photodetachment of MSPs. Looking at Fig. 10 we also nd it noteworthy to point out that differences between currents owing to photoionization of neutral particles and photodetachment of electrons from negatively charged particles are minor. The reason for this lies in the fact that the absorption cross sections vary as $r 3 =l, i.e., the cross sections at the shortest p relevant wavelengths are considerably larger than the ones at longer wavelengths. Hence, it does not matter too much if the integration over wavelength starts at corresponding energies of 2 or 5.5 eV. In conclusion of this section, we may state that all available arguments do support our initial assumption, i.e., that the recorded photocurrents are due to photoelectrons from MSPs, at least at altitudes below $90 km.

rocket ight is a direct consequence of the mean free path of the photoelectrons in the ambient atmosphere. Interestingly, this effect makes our measurement more sensitive if the instrument is in the wake of the rocket than when it is in the ram. Finally, we investigated the question whether the observed photocurrents originated from MSPs or whether they could be due to other ionizable species like NO, excited molecular oxygen, metal atoms, or negative ions. This analysis shows that all these alternative species fall short to explain the observed photocurrents by several orders of magnitude below an altitude of 90 km. Below an altitude of 90 km, we succeeded to explain the measured currents quantitatively by assuming that they originated from the photoionization/photodetachment of MSPs where we assumed that the particles consisted of iron or silicon oxides and had a photoionization/photodetachment yield Y 1. Above 90 km, measured photocurrents are most likely due to NO and can hence be used to derive NO concentrations. This is discussed in detail in the companion paper by Strelnikova et al. (2008). In summary, our results demonstrate that the active photoionization and subsequent detection of photoelectrons provides a promising new tool for the study of meteor smoke particles in the middle atmosphere. Importantly, this new technique does not rely on the a priori charge of the particles, neither is the accessible particle size range severely limited by aerodynamical effects. In the companion paper by Strelnikova et al. (2008) we apply the expressions for the photocurrents presented in this study to derive quantitative information on MSP properties which were so far unaccessible by any other technique.

Acknowledgments We are indebted to F.-J. Lubken for his support of the ECOMA project, to J. Gumbel and M. Friedrich for valuable comments to the manuscript, to von Hoerner System GmbH in Schwetzingen, Germany, for their excellent contribution to the development of the ECOMA ight electronics, to H.-J. Heckl for building the hardware of the ECOMA-detector, and to Misha Khaplanov, Department of Meteorology of Stockholm University, for his help with measuring the spectrum of the xenon-ashlamp. We also appreciate the excellent support by the mobile rocket base of the German Space Center. This work was supported by the German Space Agency (DLR) under Grant 50 OE 0301 (Project ECOMA). References
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5. Conclusions In the current study we have introduced a new detector design for the measurement of MSPs in the middle atmosphere. The new detector combines the classical Faraday cup-design of Havnes et al. (1996) with a xenon-ashlamp for the active photoionization/ photodetachment of MSPs. Accordingly, our new detector has two measurement channels, one for the detection of a priori charged MSPs which can penetrate into the Faraday cup and deposit their charge signature on the electrode, and one for the detection of very short photoelectron pulses which are actively created by xenon-ash photons. The rst successful launch of this detector took place in September 2006 from the Andya Rocket Range and yielded high quality data in both data channels. The direct Faraday cup measurements showed signatures of negatively charged MSPs in the limited altitude range between 80 and 90 km in qualitative agreement with earlier measurements with this technique. In our companion paper by Strelnikova et al. (2008) we show quantitatively that this limited altitude range is most probably a mere consequence of aerodynamical effects and does not reect a layering process in the atmosphere. In agreement with this conclusion, measured photocurrents were detected in a much broader altitude range between 60 and 110 km. We have then devised a laboratory experiment which veries that measured charge pulses truly originate from photoelectrons. With the same laboratory setup we could further demonstrate that the observed disappearance of photocurrents at 60 km on the descent of the

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