JOURNALOF GEOPHYSICALRESEARCH 'VOL. 73, No.

20, OCTO•Eg 15, 1968

ChargeTransfer betweenUnchargedWater Drops in Free Fall

in an Electric Field

J. DOYNE SARTOR AND CHARLES E. ABBOTT

National Center/or Atmospheric Research, Boulder, Colorado 8030'2

The charging of uncharged, equal or very nearly equal radius drops falling freely in an
electric field has been observed to occur in two different modes. When the electric field exceeds
a thresholdvalue that is a function oœdrop size, the chargeis transferredvia a spark in the
air between the near surfacesof approachingdrops. Below this threshold,the rate of charge
transfer is slower and varies with the conductivity of the water. The onset of the spark trans-
fer mode occurswhen the voltage and the separationdistancebetween the surfacesof the
dropsreachesthe minimumsparkingpotentialrequiredfor breakdownbetweenparallelplate
electrodes.The ambient field strengthat the onsetof sparkingvaries with drop size according
to the theoretical enhancement of the local field between the surfaces for a fixed separation.
The informationobtainedin this way assistsstudiesof the electrificationof cloudsand cloud
particlesandthe growthof precipitation
in thunderstorms.
The previous
workon radioemis-
sion from collidingchargeddropscan presumablybe extendedto includeunchargedand
weakly chargeddropsin electricfields.

INTRODUCTION indirect measurementof the chargetransferred

betweenthe drops.By usingthe data obtained
Sparkdischarges betweenoppositely charged
in the spark dischargemode, the methodscan
water dropsin free fall havebeenobserved by
be extended to give a measurementof the
Miller et al. [1965].Sattour[1963] andAtkinson
charge transferredbetweendrops collidingin
and Paluch [1966] studiedthe electromagnetic
electric fields below the magnitude of those re-
radiation emitted in this way. The data were
quired for sparking.
usedby Sattot andAtkinson[1967] to provide
estimatesof the quasi-thermalradiation from APPARATUS AND TECI-INIQUES
thunderstormsand cloudy atmospheres.The
chargeson the dropsandtheir sizeswerewithin The data reported in this paper were ob-
the rangeof valuesreportedby Gunn [1957] tained with equal-radiuswater drops in a uni-
from observations within active thunderstorms. form field. The drops were producedusing the
The resultscan be applied to the remote sens- techniquesdescribedby Sattot [1963] and
ing of highly electrifiedclouds[Sartor, 1966] Atkinsonand Miller [1965]. They were allowed
and to theoretical studies of cloud electrifica- to fall betweentwo vertical parallel plates that
tion due to the electricalconsequencesof cloud- produce a uniform horizontal field and serve
particleinteraction[Sartor,1967]. as indirect sensorsof the electric charge trans-
The theoreticalexpressionfor the locally en- ferred between the drops. The plates were
hanced field between the near surfaces of two circular with a diameter of 3.6 cm and a spac-
spheresin a uniformfield is givenby Davis ing of 1.6 cm.
[1964]. When comparedwith the sparkingpo- The drops were formed from distilled water
tentials and electrode spacingsrequired for having a conductivityof 2 X 10-• ohm-• cm-•
breakdown between parallel plate electrodes, and had radii that varied between 370 and
the Davis solution suggeststhat discharges 816 •. The chargeon the dropswas reduced
should occur between two uncharged drops in to less than 15 X 10-8 esu (as measuredwith
a uniform field of sufficientstrength.The work a Carey electrometer) by applying a small
reportedin this paperconfirmsthis hypothesis biasing potential between the drop-producing
and givesthresholdfieldsfor the onsetof the hypodermicneedlesand the groundto neutral-
spark dischargebetweenfreely falling drops. ize the residual chargeson the drops.
In addition,the laboratorymethodspermit an The drop productionrate and angle of ap-
6415
6416 SARTOR AND ABBOTT

proach was controlled,so that the drops ap- 2.5 X 10-• secafter the appearanceof the rapid-
proached each other in pairs with their line rise pulse from the phototubeis illustrated in
of centersparallel to the imposedfield between Figure 1. This photographreveals a situation
the plates.The strengthof the imposedelectric very similar to that illustrated by Miller et al.
field was noted along with the mean radius of [1965] for oppositelychargeddrops.
the drops.Sparkingbetweendropswas identi- Connectinga sampling oscilloscopeacross
fied with an IP21 photomultiplierwith an S4 appropriately chosen resistorsto the parallel
spectral response and a luminous sensitivity plates used for producingthe field makes pos-
of 80 amp/lumen, operating into the 50-ohm siblethe observationof a rapid-risepulsecoin-
load of the sampling oscilloscope. When the cident with the current pulse from the photo-
ambient electricfield was sufficientlyhigh, the tube. These pulses have rise and fall times at
drops produced a short duration luminosity least as short as the limiting responsetime of
that was detected by the phototube and dis- the oscilloscope, 10-9 sec, and are probably
played on the oscilloscope.The rise and fall at least an order of magnitude shorter. The
time of the current pulsewas 2 X 10-9 seconds, apparatus is illustrated schematicallyin Fig-
the limit of the phototube response. ure 2.
In a previousinvestigation,Sattot and Atkin-
OBSERVATIONS OF ELECTRIC i•IELD AND
son [1967] presenteda time-exposurephoto-
ONSET OF SPARKING
graph of sparks' between oppositely charged
drops. In the presentcase,however,it was not The observedthresholdelectricfieldfor spark-
possibleto record photographicallythe sparksing betweenthe drops is plotted againstthe
between unchargeddrops in an electric field radius of the drops shown in Figure 3. The
becauseof the difficulty in ensuring that the
observationsweremadewith a streamof drop-
breakdownoccurredin the same small region let pairs and the threshold fields quoted are
of space over a sufficiently large number ofthose for the first appearanceof sparks be-
interactionsto producean image on film. How-tween the drops.For parallel plate electrodes,
ever, by restrictingthe viewing aperture of the
the minimum sparking potential of 327 volts
phototube to the immediate volume between occurswhen the product of the pressureand
the near surfacesof the droplet pairs, we were
sparkingdistanceis 0.567 mm Itg X cm, ac-
able to determinethat the luminosity occurred
cording to Cobine [1958]. By using these
only in this region. The drop configuration values and the atmosphericpressure in the

Fig. 1. Configuration
of two 'uncharged'
796-• dropsin an electricfield parallello lhe line of
centersand 2.5 X 10-• sec after initiation of spark discharge.
 ,=,

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Fig.2. Schematic
diagramof apparatus
for dropproduction
andindirectsensing
of charge
transfer.

I '
.

0 , I • ! , I , 8O0 I000
o zoo 400 600

DROP RADII (Microns)

Fig.3. Minimumelectricfieldrequiredto produce

a sparkdischargebetweentwo un-
charged,
equal-radii
dropsplottedagainst
dropradii.Thesolid-line
curvewascomputedfrom
equation2 by usingthe meanatmosphericpressure
of 621mm Hg in the labors.
tory •t•
Boulder, Colorado.
6418 SARTOR AND ABBOTT

laboratory, it is possibleto predict that the
onset of sparking will appear when the poten-
tial difference between the drops is 327 volts
and the spacingis of the order of 9 •. This
spacingcomparesfavorably with the length of
the bridgebetweenthe dropsshownin Figure 1.
Davis [1964] gives the ratio F of the field
between the near surfaces of two spheres to
the ambient field Eo as a function of the sepa-
ration S of the surfacesin units of sphereradius
R. Thus, if we assumethat the drops remain
approximately sphericalas they approacheach
other along the field Eo, sparking might be
expectedto appearwhen
relationbetweenthe fieldfor the onsetof spark-
ing and radius of the dropsshownas the solid
line curvein Figure 3. The observeddata points
are clustered closely about this curve. These
data are in Figure4 also,superimposed
on the
theoretical field enhancement curves. The cor-
respondence again appearsto be quite good,
and we now assumethat by usingthe appropri-
ate value of S/R in Figure 4 we obtain a theo-
reticalF that whenusedin (2) givesa predicted
thresholdvalue for Eo. In addition,the factor
F can be used to computethe chargetrans-
ferred betweenthe drops by the method de-
scribed below.

FEoS = 327 volts (1) INDIRECT MEASUaEME•TS or

SinceF is a function of S/R, we can find Eo from
Eo = 327/FS, voltscm-'
where S = 0.567/Po and Po is the atmospheric
pressure in millimeters of mercury. With S
fixed, F at the near surfacesof the spherevaries
with R, the radius of the spheres,giving the
C•:ARGE TRANSr•R
The quantity of chargetransferredbetween
(2) two unehargedequal-radiispheresin a uniform
electric field parallel to their line of centers
owingto touching,or by spark immediately
prior to touching can be derived from Davis
[1964] and is givenby Sattot [1967] as

I0•_ I I I I I I I •[ I ! I I I I I'1• _

_
_

• FIELD ON NEAR -
_x. SURFACEOF DROPS -

-% FIELD MIDWAY -

• BETWEEN
DROPS
-
u_ • •) OBSERVED -
rr
¸ •_ ENHANCEMENT
• FACTOR
(...) -

g,J
02
Z

iO [ I I I I I Illl I I I I i I i ,
I(53 IO'2 0-'

SEPARATION/RADIUS, S/R

Fig. 4. Ratio of theoretical

fieldbetweendropletsto ambientfieldis plottedagainstthe
separationof the dropsurfacesin unitsof dropradiusSIR. The samescalesare usedto plot
F versusSIR. F is takenfromDavis[1964]for a pointon the nearsurface of the dropsand
at the point midway between them.
 CHARGE TRANSFER BETWEEN
q, = 1.645ER2 esu (3)
Using the minimum sparkingseparationand
the field enhancement factor from Figure 4,
we can comparethe charge transfer obtained
from (3) with the changeof charge observed
inductively to occur betweenthe parallel plates.
A charge q at a position z on a perpendicular
line betweenthe two platesof a groundedparal-
lel plate capacitor with a separation distance enhancementfactor F varies inverselywith the
of L in vacuuminducesa charge--q(L -- z)/L
in one plate and --qz/L in the other. A rigor-
ous proof of theseexpressions is given by Fong
and Kittel [1967] for infinite plates. The finite
dimensionsand separationof our plates intro-
duce at most an error of 7.8% in the charge
measurements.Movement of the charge per-
pendicular to the plates will be reflectedby an
equal but opposite charge change in each of
the plates.The chargechangecan be measured
with an oscilloscopeconnectedby a capacitor
to the plates. If the senseof the current from
one plate is reversedand added to. the current
from the other, twice the measuredchargeAQ
is obtained from the oscilloscopetracing by
numericalintegrationof the current I over the to the electrical relaxation time of the water
period T of the chargetransfer.Usingthe above
expressions for chargesimaged in each of the
plates and assumingthat the movementof all
chargesbetweenthe platescanbe characterized
by somemean distanceAz, we find the charge
rearrangementobservedwith the oscilloscope
to be
fo
r
2AQ---- I dt= -•-Az2q (4)
allowingus to obtain the product of the charge
q and
qAz= -• I dt--=AQL (5)
If we assume that the data fit the curves in
Figure 4, FS can be set equalto Az for spark-
ing drops,and the chargetransfer observedin
this way can be comparedwith that predicted
by (3). When the drops collide in the space
between parallel plates that are L cm apart,
the charge transferred from one drop to the
other is
qo= AQ(L/FS) esu (6)
where F can be read from the solid line in Fig-
DROPS IN AN ELECTRIC •'IELD 6419
ure 4 for any SIR. $ is the minimum sparking
distanceas in (1), and AQ is the measured
charge change observedwith the oscilloscope
attached to the plates.
A slower transfer of charge is observedin
fieldsbelowthe sparkingthreshold.This charge
transfer can be indirectly measuredin the same
way as that of the sparking-thresholdmode.
For drop spacingsless than 10-•R the field
spacing,so that the product of the enhance-
ment factor and the spacing remains almost
constant as S decreasesfurther. Thus charge
transfer by conductionbetween the drop sur-
faces can be found for nonsparking drops in
the sameway as for sparkingdrops.
Some data are available to substantiate that
the chargeis transferredbetweenthe drop pairs
in electric fields below the sparking threshold
becauseof conduction when the drops touch.
The resolution time of the current pulse ob-
served with the oscilloscope employedas sche-
matically illustrated in Figure 2 is 4 X 10-8
sec. The bulk relaxation time of the charge
transferred was 3.6 X 10-6 sec, a value close
used, but contrastingmarkedly with the much
shorter relaxation time observedin the spark-
ing mode of the charge transfer; the limiting
responsetime of the oscilloscope, i.e., lessthan
I X 10-ø sec.Figure 5 is a photographof two
unchargeddrops of 780-• radius in a uniform
field of 3.85 kv cm-• parallel to their line of
centerstaken 3 •sec (photoflashduration of
I •sec) after the oscilloscope usedin the man-
ner illustratedin Figure 2 indicatedthat charge
transfer had started between the drops. The
near surfacesclearly have been bridged by a
small neck of water. The situation 12 •sec later
is illustrated in Figure 6. The neck of water
bridgingthe near surfacesis larger, but charge
has ceased to flow.
Other studies indicate that no charge flows
unless the surfacesare bridged. For example,
if drops bounce without direct evidenceof
bridging or the onsetof coalescence,no detect-
able charge transfer can be observedeither in-
directly with the oscilloscope
and the plates or
by direct intercept of the drops after they
have bounced. G•nerally speaking, when un-
charged or weakly charged drops of several
hundred microns collide in zero or weak am-
6420 SARTOR AND ABBOTT

Fig. 5. Unchargeddrops of 780-tzradius in a uniform field of 3.85 kv cm-• parallel to their

line of centers,3 gsecafter the start of chargetransfer.

bient fields, their near hemispheresare greatly dropsis the appearanceof a number of small air
flattenedas in Figures7 and 8. In Figure 7 the bubblesin the newly formeddropsin a coalescing
apparent 'collision'is followed by an elastic situation like that illustrated in Figure 8. It is
bounce,but, in Figure 8, 'collision'is followedby probable,then, that the lack of chargetransfer
coalescence. Further evidence that an air film betweenbouncingdropsin weak fields,the situ-
is trappedbetweenthe near surfacesof the two ation depicted in Figure 7, is due to an inter-

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•s•.•g•;•;•;;•.•.•.•.•.•........;;•;•;•;•;:•*;•;;•;;•;;•s•;•.•;•;J;•;;•;•;•;•;s•)•;•;•;.....:•:•.•;•s•*•;```..•.•..•..•;•;*;•;•5•;.•:•;;•:•:•.•`.•;•:•;•.•;•..•..••••;••;•.•.•*•
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""'•
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- ..••":'"':*•'
"':':':'"'"::•:'
'•--.
-'"'•-.;":':':"'"""":•:•:•
"•ß •-•-..-•ii'""':::"
'"':'•'•½;!;""'"'"•:':':'•'••?"'"---"-'-"d;i
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"'"'"'""••":•':•'••
••,•,•i!'"'"'"'"'""•:':':•:•'•:::
a
Fig. 6. Unchargeddrops of 780½ radius in a uniform field of 3.85 kv cm-• parallel to their
line of centers taken 12 gsecafter Figure 5. The charge has ceasedto flow
 CIIARGE TRANSFER BETWEEN
Fig. 7. Oppositely charged 390-•zradius bounc-
ing drops in zero ambient field. Charge on each
drop is 6 X 10-ø esu. Relative velocity is 30 cm
sec-•.
veningair film that is never bridgedwhen they
'collide.' The reader is referred back to Figures
1, 5, and 6 for contrastingsituationswhen the
drops are highly charged or in strong fields.
Here the near surfaces reach out towards each
DROPS IN AN ELECTRIC FIELD 6421
other forming pre-collisionelectricaland phys-
ical contact. Figures 7 and 8 also serve as a
general illustration of the successive1.6-msec
positionsof the drop pairs as they passthrough
the test section between the plates shown in
Figure 2.
Although the responsetime of the electronic
system is sufficientto resolvethe rise time of
the pulse owing to electrical conductionin the
water, the pulseshapeis determinedby the RC
time constantof the parallel resistanceR• and
capacitanceC• of the system. Thus the current
AQ in (6) is obtained from the oscilloscope
tracing of the voltage versus time t by nu-
merical integration of the area under the curve
by usingthe equation
The charge transferred according to (3),
which is exact for spheres,is comparedin Table
1 with calculationsmade from (6) using the
indirect measurementsof the charge transfer
imaged in the plates. The reader is reminded
that the drops are initially unchargedand be-
come chargedwhen they spark or touch in the
ambient electric field supplied by the potential
difference between the plates and that the
measurementswere carried out with pairs of
drops of equal or very nearly equal radius. The
results of this study can be extendedto drops
of arbitrary radius in the hundreds-of-microns
range through the Davis [1964] electrostatic
theory for fields and forcesbetween spheresof
any size and charge. However, the great dif-
ferences in the physical interaction processes
for drops outside this range or of greatly dif-
ferent radii makes the extrapolation of the re-
sults obtained here to such drops extremely
hazardous. Application of the results to the
natural atmosphere can only be made safely
by observingtheselimitations.
We immediatelynote from Table I that the
observed charge transfer generally increases
over that predicted theoretically as the fields
becomestronger. This is most likely accounted
for by distensionof the near surfaces of the
drops toward each other in the stronger elec-
tric fields.
The failure of the observations
to give charge
transfers in the weaker fields as large as those
predicted theoreticallymay be due in part to
6422 SARTOR AND ABBOTT

.....................
......

.............................
:- :::::::::::::::::::::::::::::::::::::::::,,..,.,.
..........................

..........................

,•,.....:•?..? -...----:-:::::::-:
.......
.......
:::::::::::::::::::::::
.................
.......
...::.:
.............
......... .. --..:::..:....:.:::.
................
:........ ...............
,.......::::.::.:::...:::::::::: ..

Fig. 8. Oppositelycharged390-• radiusdropscoalescing

in a zero ambientfield. The charge
or: each drop is 6 X 10-6 esu. The relative velocity is 120 cm sec-L
TABLE 1. TheoreticalChargeTransfer(Equation3) Comparedwith Observed
ChargeTransferusing
Equation 6

qt = 1.645 ER 2 (es•) q0 = AQL/FS (esu)

R, • E, kv/cm (Equation3) (Equation6) qo/q•
402 2.82 2.51 X 10-•- 2.42 X 10-•- 0.96
4.94 4.39 4.53 1.03
7.85* 6.98 8.97 1.28
7.85* 6.98 9.57 1.37
673 0.847 2.10 1.88 0.89
1.73 4.30 4.38 1.02
3.1 7.66 7.92 1.03
4.57* 11.3 14.7 1.30
8!6 0.606 2.21 1.92 0.87
1.15 4.20 4.50 1.07
1.86 6.79 7.41 1.09
3.62* 13.3 17.90 1.35

* Minimum sparkingfield.
 CHARGE TRANSFER BETWEEN DROPS IN AN ELECTRIC FIELD 6423

the substitutionin the laboatory of finite plates Acknowledgments. We acknowledge the help
where the theory assumesinfinite plates; a of Dr. M. H. Davis in providing us with the, field
enhancement factors used in this report. Mrs.
maximum error of 7.8%. This discrepancyis Ilga Paluch assisted us with the evaluation of
not so large as some of those shown in Table 1 the error in using finite plates for indirectly
for the weaker fields. These fields are large sensing charge transfer.
enough,however,to causethe dropsto extend
l•EFEREN CES
their near surfaces toward each other, thus
ruling out the flattening of the near surfaces A tkinson, W. R., and A. H. Miller, Versatile tech-
as a possiblecauseof the discrepancy.The most nique for the production of uniform drops at
a constant rate and ejection velocity, Rev. Sci.
reasonableexplanationliesin the fact that water Instr., 36, 846-847, 1965.
has a finite dielectricconstant(81), whereasthe A tkinson, W. R., and Ilga Paluch, Electromag-
theory giving rise to equation 3 assumesthe netic emission from pairs of water drops ex-
spheresto be conductors.Davis [1968] shows changing charge, J. Geophys. Res., 71, 3811-
3816, 1966.
that water drops behave electrostaticallyas
Cobine,J. D., GaseousConductors,606 pp., Dover
conductorsexcept when their surfacesare less Publishers, New York, 1958.
than 10-•' radii apart, and the chargeis trans- Davis, M. H., Two charged spherical conductors
ferred in a time that is comparableto the re- in a uniform electric field: forces and field
laxation time for water. This is the situation strength, Quart. J. Mech. Appl. Math., 17, 499-
511, 1964.
for the drops in our experimentjust as their Davis, M. H., Electrostatic field and force on a
surfacesmake contact and the charge starts dielectric sphere near a conducting plane--a
to flow. note on the application of electrostatic theory
to water droplets, submitted to Am. J. Phys.,
CONCLUSIONS 1968.
Fong, C. Y., and C. Kittel, Induced charge on
The electromagnetic emissionproperties capacitor plates, Am. J. Phys., 35, 1091-1092,
oppositelychargeddrops reported by Atkinson 19,67.
and Paluch [1966] and Sattot and Atkinson Gunn, R., The electrification of precipitation and
[1967] shouldbe valid for discharges between •hunderstorrns, Proc. IRE, j5, 1331-1358. 1957.
unchargeddropsin strong electricfields.Thus Miller, A. I-I., C. E. Sheldon, and W. R. A tkinson,
Spectral study of the luminosity produced dur-
the resultsof this study are applicableto the ing coalescence of oppositely charged falling
remote sensingof highly electrified clouds.Al- water drops, Phys. Fluids, 8, 1921-1928, 1965.
thoughthe electrostaticprinciplesdiscussed in Sartor, J. D., Radio emissionfrom clouds,J. Geo-
thisstudyare universal,
considerable
extrapo- phys. Res., 68, 5169-5172, 1963.
Sar!or, J. D., The remote sensing of radio emis-
lation is necessaryto apply the resultsto the sion from convective clouds,Proc. Fourth Symp.
electrificationof drops or particles of different. Remote Sensing Environment, Ann Arbor,
sizein cloudsor thunderstorms. The fact, how- Mich.. 285-292, 1966.
ever, that dropsin free fall can be chargedin Sartor, J. D., The role of particle interactions in
this way may be of considerablesignificance the distribution of electricity in thunderstorms,
J. Atmospheric Sci., œ4, 601-615, 1967.
in the distribution of electricity in thunder- Sartor, J. D., and W. R. Atkinson, Charge trans-
storms. More information is needed on the fer between raindrops, Science',157, 1267-1269,
mechanicaland hydrodynamicconsequences of 1967.

collisionsbetweenchargedand unchargedpar-
ticles of differentsizesin the presenceand ab- (Received May 9, 1968;
sence of electric fields.
revised July 5, 1968.)