Sci. Rep. Kanazawa Univ.
Vol.48, No.1,2, p.107-133, 2004

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Finding abnormal events during the Iraq War monitored
at Japan 8000 km away from Iraq
Kazue TAZAKI1, Koushirou MIYATA2, Taichu Y. TANAKA3, Masaru CHIBA3,
Rie WAKIMOTO2, Ichiro SAJI2 and Kazuhiro SATO2
1. Department of Earth Sciences, Faculty of Science, Kanazawa University, Kakuma,
Kanazawa, Ishikawa, 920-1192, Japan
2. Graduate School of Natural Science and Technology, Kanazawa University, Kakuma,
Kanazawa, Ishikawa, 920-1192, Japan
3. Meteorological Research Institute/JST Cooperative System for Supporting Priority
Research, 1-1 Nagamine, Tsukuba, Ibaraki, 305-0052, Japan
Abstract : Unusual strong acidic rain recorded during the Iraq War in Japan Sea side
8000 km away from Iraq. In order to monitor the seasonal change of pH, the rainwater
was collected during the period from March 24th to September 24th, 2003 at Kanazawa,
Ishikawa Prefecture, Japan. For comparison, the rainwater at Wakayama (the Pacific
Ocean side) was collected, during the period from March 24th to April 30th, 2003. The
pH, Eh, EC, and DO of the rainwater were measured in laboratory periodically. Filteredrain dusts were investigated by scanning electron microscope equipped with energy dispersive X-ray spectrometer (SEM-EDX), electron probe micro analyzer (EPMA), transmission electron microscope (TEM), energy dispersive X-ray fluorescence spectrometer(ED-XRF), and X-ray powder diffraction (XRD) analyses. In this study, the fluctuationof pH values and electrical conductivity (EC) of rainwater during this half-year period
were measured to find abnormal events, such as the Iraq War effects.
Since March 21st, 2003, Iraq plunged into the war. The more than 30 oil field firesin Rumaylah, Basrah, Mosul, and other oil fields near the borderline of Kuwait and Iranwere reported in March and in April, 2003 in Japan. The first precipitation during the
Iraq War was caught on March 24th, 2003. In the period from March 24th to April 5th,
the notable low pH value of 3.4-4.4 and high EC value of 20-360 μS/cm were detectedin Kanazawa. The acidic rain associated with WNW wind (2.7-4.1 m/s) has continued to
the first 10 days of April in Kanazawa, during the 9 oil fields were burning in Rumaylah,
Iraq. In the same time, the upper current of air maps confirmed that the 5520-5700 m
lines cross over and spread on both Iraq and Japanese Honshu Island. It is consideredthat westerly wind crossed over both Iraq and Japan. The high EC values from March 24th to April 5th, 2003, suggest that high concentrations of water-soluble carbon particles
and soot contained in the rainwater. In addition, the black powdery dusts were detectedfrom the strong acidic rainwater on April 1st. The powdery dusts and carbon-bearing
particles contained in the rainwater have characteristics different from that of the Asian

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aerosol particles (Kosa). The results suggest that both powdery dusts and carbon-bearing
particles of rainwater have been produced by combustion of oil field in Iraq. Simulation
data support the directly cycling by westerly wind indicating the influence of the Iraq
War. Possible evidences provided in this paper, such as strong acidic rain and high EC
values with nm-sized carbon soot at Japan Sea side, was the influence of the Iraq War. It
was suggested that local events affect the global atmospheric environments. Smoke fromoil field fires around Baghdad and other wartime pollution could create long-term healthhazards.
Key words : acidic rain, pH, electrical conductivity, the Iraq War, the Japan Sea side,
the Pacific Ocean side, oil field fires, combustion, carbon-bearing particles, powdery
dusts, Westerly wind.

1. Introduction
Asian aerosol particles (Kosa) were transported to Japan all the year around. Especially in spring, highly concentrated Kosa and acid precipitations were frequently observedon the Japan Sea side (Satake and Yamane, 1992 ; Kwon et al., 1997). Northeastern China
has the largest anthropogenic emission source of acid precipitations, which originate in fossil fuel combustion (Fujita et al., 2000). These Asian aerosols transported by westerly wind
are considered as cause substances of acid rain on the Japan Sea side (Iwasaka et al., 1998).
How Kosa aerosols and supplemental substances behaved in the same air mass based on
the size distributions of the chemical components in Kosa aerosols sampled along theirtransport routes have been discussed (e. g. Mori et al., 2003). There are few reports on theconcentration and chemical composition of Kosa aerosols at the source. Aerosol monitoring of Kosa sources is nearly impossible because of topographical and meteorological difficulties.
Local atmosphere reflects major or minor influences of world environment, as we remember the Gulf War in 1991. More than 700 oil field fires had produced a tremendous
amount of carbon soot to the world from Kuwait. On February 20-25, 1991, we had caught
black snow for a week at Matsue, Shimane Prefecture in Japan, faced to the Japanese Sea
Coast (Tazaki et al, 1992). It used to take 8 months to recover the fired environment in Kuwait. The public health changers of smoke from oil fires in the environments are not fully
known. Some argue that it causes asthma attack and allergy.
Again it happened before forgetting the Gulf War. Since March 21st, 2003 the Iraq
plunged into the war, more than 9 oil field fires were reported in March 25th, 2003 in Rumaylah oil field near the borderline of Kuwait. After that, more than 30 oil fields caused afire. Once the oil fields get fired it takes several months to extinguish fire. Produced black
carbon particles due to incomplete combustion are the principal light-absorbing atmospheric aerosol. The black smoke from burning oil trenches around Baghdad, meant to surround targets, contained many toxic substances that might affect the soils and drinking

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water.
Carbon-containing species constitute an important fraction of atmospheric aerosol in
the fine particle size range (<1 μm). According to different studies, the organic compounds
may account for 20-50 % of the total fine particle mass (Heintzenberg, 1989 ; Zappoli etal., 1999). Recent measurements show that significant part of the organic species is soluble
in water (Zappoli et al., 1999 ; Decesari et al., 2001 ; Varga et al., 2001). Organic particles can take place in the control of atmospheric processes like cloud formation and visibility degradation. Water-soluble organic compounds in the nucleation size range play a keyrole in cloud formation. They might be responsible for up to 80 % of the total cloud condensation nuclei concentration (Novakov and Penner, 1993). But that may have more to dowith the relatively precise methods and the lack of actual nm-sized observations.
In this paper we reported transport of carbon-bearing particles and nm-sized powdery dusts,
which results a short-term variation of atmospheric environment during the Iraq War. The
seasonal change of the characteristics of rainwater and powdery dusts after the Iraq War,reported also in order to know the influence of the Iraq War.
2. Materials and Methods
Rainwater was collected every day from March 24th to September 24th with the trayon the roof (1.5 m from green grass ground level) of the hut in Kanazawa University,
Kakuma, Kanazawa, Ishikawa Prefecture, located on the Japan Sea side. The sampling site
is about 10 km from the Japan Sea. Kanazawa city has a population of approximately
450,000. There is no large pollution source compared with most cities on the Japan Sea
side. Precipitation, temperatures, wind power and wind direction were measured by usingof AMeDAS (Automated Meteorological Data Acquisition System) in the Kakuma Campus of Kanazawa University.
In the meantime rainwater was also collected from March 24th to April 30th at Kawabe, Wakayama Prefecture, Japan located on the Pacific Ocean side in order to comparewith Japan Sea side in Kanazawa.
2.1. Measurements of rainwater
The pH, Eh, EC, DO and temperature of rainwater were immediately measured in thelaboratory by using pH, Eh, EC, and DO meters (pH : HORIBA pH Meter D-21, Eh :HORIBA Eh Meter D-13, EC : HORIBA Conductivity Meter ES-12, DO : TOA DO Meter DO-21P).
The rainwater (2 ml) were dried up on the Mylar film to analyze water chemistry byan energy dispersive X-ray fluorescence spectrometer (ED-XRF : JEOL JSX 3201 using
Rh Kα) which operated at an accelerating voltage of 30 kV under a vacuum condition. The
9 samples were collected at Kanazawa whereas the 3 samples were collected at Wakayama
for chemical analyses by using of ED-XRF. The 12 samples of rainwater were selected toclarify the relationship between pH and dissolved elements.

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2.2. Analyses of filtered materials from the rainwater
The rainwater samples were filtered with a membrane filter (0.2 μm of pore diameter)using an aspirator. Solid materials left behind after filtering were analyzed by ScanningElectron Microscopy (SEM) equipped with Energy Dispersive X-ray spectrometer (EDX),
Transmission Electron Microscopy (TEM), Electron Micro Probe Analyzer (EPMA) and X-ray powder diffraction analyses (XRD) for the mineral composition, the micro morphology and the chemistry. The filtered samples were cut from each filter, attached to a glass
slide and analyzed by X-ray powder diffraction (XRD) with a Rigaku, Rint 1200 system X-ray diffract meter with CuKα radiation and accelerating voltage of 40 kV and an electric
current of 30 mA. The filtered samples attached to Mylar film were also analyzed by EDXRF.
Elemental concentration measurement was conducted using energy dispersive X-ray
spectrometer (EDS ; Philips-EDAX PV9800STD) attached to a JEOL-JSM-5200LV scanning electron microscope (SEM). Operation condition was as follows : an accelerating
voltage of 15 kV and an analytical time of 200 sec. Conversion of intensities into concentrations was accomplished using a standard less ZAF (Z = atomic number, A = absorption,
F = fluorescence) correction program set in a computer. Concentration of elements was
neutralized as wt.%.
Carbon content maps of the filter were conducted using EPMA (JEOL JXA 8800R
Super Probe) at an accelerating voltage of 15 kV. LDE (Layered Dispersion Element), LiF(Lithium Fluoride), PET (Pentaerythritol) and TAP (Thallium Acid Phthate) were used foranalyzing crystal for EPMA. In addition, EPMA analysis also shows the qualitative chemical composition of particles on the filter. The carbon spherical soot was observed by a
JEOL JEM 2000EX transmission electron microscope (TEM).
2.3. Meteorological data
The 500 hPa atmospheric pressure at 5520-5700 m height contour maps were provided by Kanazawa meteorological station in Kanazawa, Ishikawa Prefecture, Japan. Westerly wind blows along the line in this contour map.
2.4. Simulation of dust storm
The model used in this study is the Model of Aerosol Species In the Global Atmosphere (MASINGAR) (Tanaka et al., 2003 a), which is an on-line chemical transport modelfor tropospheric aerosol species with a four-dimensional data assimilation system.
3. Results
The distinguishing characteristics of rainwater and filtered dusts were physically,
chemically, and micro-morphologically summarized in Table 1 and Table 2. Almost all
samples show acidic rain at both sides of Japan Sea and the Pacific Ocean sides. However,the characteristics of rainwater at the Japan Sea side indicated abnormal physical, chemical,

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and micro-morphological factors in the beginning of April, 2003. However, the seasonalvariations and abnormal values of rainwater at both sides were described as follows :3.1. Characteristics of rainwater
Since the Iraq War started on March 21st, 2003, the Japan Sea side has first rain on
March 24th (pH 3.6), and continuously acidic rainfall for a week (pH 3.4-4.4), associatedwith a high electrical conductivity (360 μS/cm) (Fig. 1). The pH and EC of rainwater collected in Kanazawa indicated contrary interrelation, indicating a large amount of dissolved
ions exist in the acidic rain. After the middle of April, the pH and EC of the rainwater got
back to normal values to compare with that of the beginning of April. Especially the EC
values are back to constant as 20-＜50 μm/cm after on April 20th, which are contrary interrelated. Dissolved elements in rainwater collected after the Iraq War finished were analyzed by using ED-XRF, showing strong acidic rains contain considerable high S concentration of 29-53 wt.% (Table 3). In comparison, just only one sample of slightly acidic rain
(pH 4.4) contains high S concentration (50.4 wt.%) on September 7th. The high Si (28-48wt.%) and Ca (6-18 wt.%) concentrations were detected in slightly acidic rain. Additionally, the rainwater almost neutral pH shows high Si (16-39 wt.%) and K (12-47 wt.%) concentrations.
On the other hand, the pH and EC of rainwater at the Pacific Ocean side have notchanged since the Iraq War started on March 21st, 2003 (Fig. 2). The pH of rainwater collected at Wakayama shows constant (4.8-5.5), whereas the EC indicated changeable value
from 10-70 μS/cm. The pH is irrelevant to the EC in Wakayama, during the Iraq War. The
slightly acidic rainwater collected at Wakayama contains considerable high Na concentration (35-54 wt.%) because of seawater effect. Chemical compositions of rainwater anddusts at the Japan Sea side (Kanazawa) and the Pacific Ocean side (Wakayama) are summarized in Table 1, to know the chemical compositions between acidic rain and normalrain in March-April, 2003. The acidic rain can be characterized high sulfur contents in Kanazawa, whereas the normal rain indicated high concentration of Si, suggesting differencesof the origin of dusts where came from, and what is the source materials.
3.2 Characteristics of filtered materials from the rainwater
The filtered materials of acidic rainwater collected in Kanazawa since the Iraq War
started on March 21st, 2003, showed grayish blown and black in color suggesting the existence of a large amount of soot and rain dusts (Fig. 3). The filters during the period fromMarch 24th to April 1st show quite dark color compared with the filter after April 2. Especially, the filter of March 31st and April 1st indicated high concentration of soot because ofvery black in color. On March 31st the blackish brown colored filter indicating low pH andhigh EC might be mixtures of dusts and soot. On June 13th the brown colored filter withrelatively large sized grains suggest us much more mineralogical origin of dusts.
Filtered materials of rainwater collected on March 24th - June 16th, 2003 in Kanazawa,

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Fig. 1. The pH and EC changes in acid rainwater since the Iraq War started on March 21st, 2003, the Japan Sea side has first rain on March 24th (pH 3.6), and continuously acid rainfall for a week (pH
3.4-4.4), associated with a high Electrical Conductivity (360 μS/cm). The pH and EC of rainwater collected in Kanazawa are contrary interrelated, indicating a large amount of dissolved-ionspresent in the acid rain. After the middle of April, the pH and EC got normal values to comparewith that of the beginning of April.

Fig. 2. The pH and EC of the rainwater at the Pacific Ocean side (Kawabe, Wakayama) were notchanged since the Iraq War started on March 21st, 2003. The pH of rainwater collected at
Wakayama are constant values as 4.8-5.5 whereas the EC is changeable range from 10 to 70 μS/
cm.

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Fig. 3. The precipitation materials of filtered rainwater collected in Kanazawa since the Iraq War started
on March 21st, 2003, showed grayish blown and black in color suggesting the existence of alarge amount of soot and rain dusts.

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were identified by XRD showing mainly organic materials on March 24th and April 8th,
because of smooth patterns (Fig. 4). After the Iraq War the samples on June 13th - June 16th, 2003, indicated mainly amorphous materials showing low intensity and hilly background with quart and feldspars small peaks. The XRD results clearly revealed the differences of characters of dusts before and after the Iraq War.
3.2.1. Carbon-bearing powdery dusts and smooth spherules collected at Kanazawa in
April
The filtered samples were observed by using microscopical techniques showing detailed morphology, size and chemical data as follows :SEM-EDX analyses of the powdery dusts on April 1st, 2003 in Kanazawa show abundant few μm-sized spherules in general views (Fig. 5A, B). The EDX results indicatedpresence of organics because of high background. The organic components such as P and S
elements support this statement (Fig. 5C, D). The Al-Si-rich spherules 3-6 μm in diametershowing smooth surface coexisted with granular aggregates (Fig. 5E a, b and F an arrow).
TEM micrographs of S-bearing aggregates of sub-micron particles coated on the surface of
fly ashes and the spherules revealed more precise structures. The high dense large
spherules and nm-sized spherical chain structure can be seen in general views (Fig. 6A, B).
The carbon particles less than 100 nm in size showing fingerprint-like structures were detected on the black filter sample collected on April 1st, 2003. The high resolution TEM micrograph in Fig. 6D is a closed-up photograph of granular aggregates (Fig. 6C).
EPMA micro morphologies (Fig. 7A, B) and the carbon content maps (Fig. 7A’, B’)of filtered acid rainfall (pH 3.4) identified a high concentration of carbon with nm-orderedfine powdery dusts on April 1st, 2003 in Kanazawa at the Japan Sea side. The spherule 15

Fig. 4. X-ray powder diffraction patterns of filtered rainwater samples collected on March 24th - June 16th, 2003 in Kanazawa. The samples have not treated, showing smooth patterns between March 24th and April 8th. Whereas the sample composed of mainly amorphous materials after June 13th to
16th, 2003, showing hilly background.

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Fig. 5. Scanning electron microscopy equipped with energy dispersive analyses of the powdery dusts on
April 1st, 2003 in Kanazawa, showing abundant few μm sized spherules (A, B). Arrows indicate
the analytical points, showing high background of organics (C, D) and Al-Si inorganic sphericalmaterials (E, F).

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Fig. 6. Transmission electron micrographs of the S-bearing aggregates of sub-micron particles coated on
the surface of fly ashes and the spherules (A, B). The nm-sized carbon particles showing
fingerprint-like structure were observed on the black filter paper on April 1st, 2003 (C, D).
Table 1. Chemical compositions of rainwater at the Japan Sea side (Kanazawa) and the Pacific
Ocean side (Wakayama) in March and April, 2003.

Table 2. The characteristcs of rainwater and filtered dusts at the Japan Sea side (Kanazawa).

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Fig. 7. EPMA micro morphologies (A and B) and carbon content maps (A’ and B’) of filtered acid rainwater (pH 3.4) indicated a high concentration of carbon distributions with nm-sized fine powdery
dusts on April 1st, 2003 in Kanazawa at the Japan Sea side. The sphere indicated by an arrow in
B composed of Si-Al elements without carbon signal suggesting melted secondary products byoil field fires in the Iraq War.
Table 3. Energy dispersive X-ray fluorescence spectrometer analyses of rain water without filteration at
the Japan Sea side (Kanazawa) and the Pacific Ocean side (Wakayama). The data are listed on
pH order from acidic to neutral rainwater.

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Fig. 8. EPMA analytical patterns of the powdery dusts (in Fig. 7) on April 1st, 2003 in Kanazawa, showing high contents of Carbon and Oxygen at the soot area whereas high concentration of Si and Al
at the spherule (an arrow in Fig. 7B). The peaks of Au are due to coating material.

μm in diameter indicated by an arrow in Fig. 7B composed of Si-Al elements without any
carbon signals suggesting the materials were melted and secondary products by oil field
fires in the Iraq War. The EPMA analytical patterns of the spherule (an arrow in Fig. 7B)
on April 1st, 2003 in Kanazawa reconfirmed high concentration of Si and Al (Fig. 8). The
concentration of C and O elements were also determined by EPMA quantitative analysis(Fig. 8). Small amount of K and Fe were detected in the spherule.

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3.2.2. Dusts collected at Kanazawa from May to September
ED-XRF analytical results of rainwater and the filtered samples are listed in Table 3
and in Table 4, respectively. Both Tables are listed on pH order from acidic to neutral rainwater. The chemical data indicated both water-soluble and insoluble materials showing
quite differences between in Kanazawa and in Wakayama.
Chemical compositions of filtrated materials are mainly composed of Si associatedwith traces of P, Ca, Al, K, Mg, Fe, Ti and Mn (Table 4). Dusts in acidic rain contain large
amount of P in Kanazawa compared with that of normal rain in Wakayama. On the other
hand, the dusts in normal rain contain high concentration of Fe and Si, suggesting presenceof mineralogical materials.
SEM-EDX data show various typed grains few μm in size were observed in the rain
dusts in the period from June 13th to June 16th, 2003 in Kanazawa (Fig. 9). Some particles
morphologically identified as microorganisms, coccolith (Fig. 9A) and diatoms (Fig. 9C).
EDX analyses indicated Si-rich (Fig. 9A) or Si-Al-rich (Fig. 9B, D, E and F) chemicalcompositions with traces of P, S, K and Ca suggesting presence of mineral aggregates. It
should be noted that no carbon spherules with them are recognized on the filter samples
collected from May to September.
TEM observation of sub-micron particles on the light-colored filter on June13th June 16th were clearly confirmed presence of microorganisms of coccus 1000 nm in size
(Fig. 10A, B), filamentous (Fig. 10C, E and F) and nm-sized bacteria (Fig. 10D). Thesemicroorganisms are covered by thin organic films showing dimness images. The elementsof Mg, K, Ti and Mn are water-soluble, whereas Si, P and Ca are insoluble elements according to the result in Table 4. Note that the S content is quite high in acidic rainwater,which are water-soluble elements (Table 3).
3.2.3. Dusts collected at Wakayama
Rainwater collected from Wakayama contains a large amount of Na and Mg watersoluble elements because of seawater effects (Table 3). The filtered sample is composed ofmainly Si as same as the dusts collected at Kanazawa (Table 4). However, the rain dusts ofWakayama contain various kinds of elements such as Fe, Al, K, Ti, Ca, Mn and Mg. Especially the Al, Si and Fe are prominent high in Wakayama to compare with dusts in Kanazawa, suggesting mineralogical materials are rich in Wakayama.
3.3. Meteorological Data
The 500 hPa atmospheric pressure at 5520-5700 m contour maps of the westerly windindicated the transport systems of dusts of the Northern hemisphere from March 24th toApril 8th, 2003 (Fig. 11 and 12). The upper current of air maps confirmed that the 55205700 m height lines cross over and covered on both places of Iraq and Japan Honshu Island. The hundred lines of 5520-5700 m heights on March 28th have covered on southernpart of Japan Island, whereas the lines on March 30th - April 1st exactly covered on Ka-

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Fig. 9. Scanning electron microscopy equipped with energy dispersive analysis of the rain dusts in the
period from June 13th to June 16th, 2003 in Kanazawa, showing various typed particles few μm
in size. Arrows indicate the analytical points of indicated Si-rich (A) or Si-Al-rich (B, D, E and F)
chemical compositions with traces of P, S, K and Ca. Some particles morphologically look likemicroorganisms, such as coccolith (A) and diatoms (C).

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Fig. 10. Transmission electron micrographs of sub-micron particles on the light-colored filter on June 13
th - June 16th. Coccus (A, and B), filamentous (C, E, and F) and nm-sized bacteria (D) were observed in this sample.

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Contour lines of altitude for atmosphere 500 hPa

Fig. 11. Weather maps showing the 500 hPa atmospheric pressure at 5520-5700 m high indicated thestream of westerly wind from March 24th to March 31st, 2003, showing the currents cross overon both Iraq and Japan under sandstorm conditions in the Iraq War.

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Fig. 12. Weather maps showing the 500 hPa atmospheric pressure at 5520-5700 m high indicated thestream of westerly wind from April 1st to April 8th, 2003. The map of April 1st shows the currents cross over on both Iraq and Japan under sandstorm conditions in the Iraq War. However,after April 1st the streams of westerly wind have no traversed over the Iraq.

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Table 4. Energy dispersive X-ray fluorescence spectrometer analyses of filtered samples from the rainwater at the Japan Sea side (Kanazawa) and the Pacific Ocean side (Wakayama). The data arelisted on pH order from acidic to neutral rainwater.

nazawa. At that time, the westerly wind carried abnormal materials from Iraq precipitated
at Kanazawa. The lines on April 3rd had no crossed over on Iraq anymore, suggesting thatan air current influenced the powdery dusts to Japan for ≧ 4 days.
3.4. Simulation data of dust storm
Simulation with a global aerosol transport model called MASINGAR, which treats
nss-sulphate, carbonaceous, mineral dusts, and sea-salt aerosols, was performed (Tanaka etal., 2003 a, b). Fig. 13 a-c show the simulated column integrated dusts for March 19th, 22nd,and 26th, 2003. The model shows that a strong mid-latitudinal cyclone in the eastern Mediterranean caused severe dust storms over the Sahara and Arabia on March 19th (Fig. 13a).
The dusts traveled northeastward over the north of the Tien Shan Mountains (Fig. 13b).
Then the dusts went southeastward, passing Mongolia, and reached Japan, where many observatories reported the Kosa (Fig. 13c).
To identify the relative contributions of the dusts from different regions, we divide theland area into 9 dust source regions (East and West China, Central Asia, Arabian Peninsula,
North and South Africa, North and South America, and Australia). MASINGAR, a global
tropospheric aerosol chemical transport model indicated following results. On March 26th,
about 53 % of the simulated dust is from North Africa, 25-30 % from the Middle East, 10 %from Central Asia, and about 10 % from China. The simulation data of dust storm agreed
with the data in Fig. 11, and supported the abnormal events during the Iraq War effected
the global atmospheric environments. Moreover, it indicates that a large part of dust on
other days originated in North Africa and the Middle East.

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Fig. 13. Simulated column integrated dust concentration on March 19th (a), 22nd (b), and 26th (c), 2003.
Units are g m−2. The arrows represent the horizontal wind velocity at 700 hPa. The horizontal
resolution of the model is about 1.1°
×1.1°
in Gaussian grid and vertical coordinate is the sigma-pressure hybrid coordinate with 30 sigma-pressure layers from the surface to a height of 0.8
hPa.

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Fig. 14. Iraqi map showing locations of oil fields, oil factory districts, and the places where explosions
and the fires occurred on March 29th, 2003. Note that SE hot wind (20-25℃）blows hard toward
the Zagros Mountains of NE to carry up clouds of black smoke.

4. Discussions
Since 1984 Ishikawa Research Laboratory for Public Health and Environment has
been observed the acid precipitation in Kanazawa. The pH value of each precipitation used
to be constantly 4.5-4.6 for 20 years (Kitamura, 1989). In this study, it was the first casethat low pH value (3.4-bellow 4.4) and high EC (360 μS/cm) of the rainwater were detected in Kanazawa for almost half month from March 24th to April 8th, 2003.
4.1. Characteristics of rainwater
In Kanazawa, the pH and EC of rainwater were relatively constant for 20 years. However, it happened that the pH and EC of rainwater dramatically changed after March 24thas shown in Fig. 1. The lowest pH value of 3.4 recorded in the beginning of April. The EC
also indicated the highest value of 360 μS/cm. The unusual values of such low pH andhigh EC suggest that large amounts of dissolved-ions are included to cause substances ofstrong acidic rain. The ED-XRF analytical results agreed with the low pH coexisting with

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Table 5. Meteorological data (temperatures, wind power and wind direction, precipitation) analyzed byusing AMeDAS (Automated Meteorological Data Acquisition System) in the Kakuma Campusof Kanazawa University.

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the high S concentration. In other words, the fluctuation of pH has resulted in the concen．Tazaki et al. (2003) reported the concentration of SO4 2- in the
tration of sulfate ion (SO4 2-）
acidic rainwater at that period was 38.9-149 μeq/l. The significant value of pH in the beginning of April suggested certain unusual events have happened such as the influence ofthe combustion of oil field fires in Iraq.
On the other hand, the characteristics of rainwater at the Pacific Ocean side of Japandiffer from those of the Japan Sea side. The pH 4.8-5.5 at Wakayama was not notably low
compared with that of Kanazawa. The EC (8-70 μS/cm) of rainwater at Wakayama waslower than that of Kanazawa. In addition, after several months since the Iraq War finished,
the pH of rainwater at Kanazawa got back to normal pH. The influence of the oil field fires
had not appeared visibly at the Pacific Ocean side compared with the Japan Sea side.
4.2. Characteristics of filtered materials from the rainwater
There are obvious differences between the dusts collected in April and in June at Kanazawa. During oil field fires, almost filters were covered with thick carbon films black incolor. The sizes of particles are < 10 μm in diameter, which are defined suspended particulate matters. TEM observations districted the finer carbon particles less than 100 nm. The
carbon soot was occurred in the atmosphere, which contained high amount of organic vapors (Blando and Turpin, 2000). Carbon-bearing dusts were notably detected from theblack filter in the beginning of April at Kanazawa. The XRD analysis of the black filter
identified organic materials without any crystalline materials such as quart and feldspars,suggesting these particles are caused by fly ashes from combustion. These particles wereformed as cloud condensation nuclei and can be transported long distance by wind (Novakov and Penner, 1993 ; Blando and Turpin, 2000).

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Rie WAKIMOTO, Ichiro SAJI and Kazuhiro SATO

Additionally, it is noted that Cl and Ca elements in the dust of the beginning of April
were not detected in this year. These two components are common in the Asian aerosols
particles (Kosa ; yellow sand) (Kim et al., 2000 ; Chang et al., 2001 ; Fang et al., 2001 ;Seto et al., 2002 ; Terada et al., 2002 ; Mori et al., 2002, 2003). Comparing with Asian
aerosols particles, the dusts of the beginning of April in Kanazawa had different characteristics, not only Ca and Cl detection but also, other soil elements such as Fe and Al could
not detected. In the other words, the carbon-rich dusts of the beginning of April also included the fly ashes came from Iraq oil field fires.
In contrast to April, filtrated materials in the period from June to September in Kanazawa have not detected carbon dusts confirmed it under TEM observations. In these periods, the filters are covered with tinged with gray-colored dusts, containing Si-Al-rich materials. These particles are mainly composed of mineralogical materials associated withsilicate minerals. The influences of the Iraq War, especially air pollution decreased after 12 month. Nevertheless smoke from oil field fires around Baghdad and other wartime pollution could create long-term health hazards (Airhart, 2003). Unusual strong acid rain included nm-sized dusts could be dangerous to breath, and leach into the soils and groundwater.
4.3. Meteorological data and Simulation data
Sandstorms periodically attacked to Iraq every week-cycle from SW bare dried landin April (Fig. 14). The hot wind carried on fine particles (< 0.04 mm in diameter), andblew hard to 1000-2000 m high with clouds of smoke. The sight was enveloped by smoke,and the visibility was sometimes only below 1m (Revkin, 2003). It is considered that the
hot wind in the Iraq blow up to 2000 m high by an up current of air and join the westerly
wind to transport powdery dusts to Japan taking ≧ 4 days (Figs. 11 and 12).
On the other hand, it has known that mass concentration in Asian dust-storm eventswas roughly 3-5 times higher than that of the highest concentration measured in non-Asian
dust storm seasons (Mori et al., 2002, 2003). Comparing with the Asian aerosols particles,
the powdery dusts from Iraq have different characteristics of chemistry and grain sizes.
SEM and TEM observations show that most of powdery dusts have diameters extremely
finer than a sand grain, suggesting that they can be more rapid transported by air currents
and long-distance transported with the winds.
However, it is suggested that yellow sand (Kosa) nearly had not arrived in Kanazawa
from China at that periods, based on the weather maps and visibility in the beginning ofApril. If abundant yellow sand arrived in Kanazawa, the pH of rainwater would increase to
7-8, because calcium contents derived from desert soils got higher (Terada et al., 2002).
In the meantime, the simulation data (Fig. 13) indicated that 25-30 % of dust camefrom Middle East on March 26th, and from China are only 10 % of total dust reach to Japan. The simulation data totally supported the SEM-EDX, EPMA, TEM, and XRF resultsthat powdery dusts and strong acidic rain are related to oil combustion in Iraq.

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Our AMeDAS weather data in the Kakuma Campus of Kanazawa University associated with the meteorological maps in Kanazawa local weather observatory also agreed withthese results. These evidences confirmed that the acidic rain with carbon-bearing particles
in the beginning of April in Kanazawa derived from the burning of oil field fires in the Iraq
War.
5. Conclusions
We analyzed rainwater included with nm-sized dusts during the period from March 24th to September 24th, 2003 in Kanazawa (Japan Sea side), and in Wakayama (Pacific
Ocean side) to compare with influences of the Iraq War, in succession along its transportroute from Iraq to Japan.
Our results led to the following conclusions :(1) The extreme low pH and high EC values in the rainwater of the beginning of April in
Kanazawa showed a rare case, suggesting the unusual events are caused by the combustionof oil field fires in the Iraq War.
(2) High concentration of carbon-bearing particles and nm-sized powdery dusts show thecharacteristic differences from that of Asian aerosols particles. It could be related to the uncompleted combustion of oil burning in Iraq. The carbon-bearing particles may be transported as nuclei of cloud from Iraq to Japan.
(3) Based on the weather maps and rough calculations suggest that westerly wind should
transfer the powdery dusts from Iraq to Japan for ≧ 4 days. We could catch powdery dusts
included with carbon soot and Si-Al spherules in strong acidic rain in Kanazawa, Japan Sea
side. The pH in Wakayama, Pacific Ocean side, shows normal pH values (4.8-5.5) inMarch and in April. The results remind us of the scientific data of short-term atmosphericenvironment records during the Iraq War. This has consequences for primary production of
powdery dusts coming from Iraq. We found abnormal events during the Iraq War monitored at Japan 8000 km away from Iraq.
Acknowledgements
We are thankful to Kanazawa local weather observatory for the provision of meteorological maps. We would like to thank Dr. Yukiya Minami (Ishikawa Agricultural college),
Dr. Masayoshi Yamamoto (LLRL, K-INET, Kanazawa University), Prof. Tomoaki Morishita (Department of Earth Science, Kanazawa University) and undergraduate students ofKanazawa University (Hiroki Imanishi, Rie Kato, Yusuke Otani and Tomoko Watanabe)
for their technical supports. The rainwater was provided from Pacific Ocean side (Kawabe,
Wakayama) by Ms. Fumie Tazaki. Thanks are also due to the students of the Tazaki’s
laboratory at Kanazawa University for their cooperation. This study was supported by the
grants from the Japanese Ministry of Education, Science and Culture to K. Tazaki.

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Kazue TAZAKI, Koushirou MIYATA, Taichu Y. TANAKA, Masaru CHIBA,
Rie WAKIMOTO, Ichiro SAJI and Kazuhiro SATO

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