Chemical Engineering Science 245 (2021) 116808

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Chemical Engineering Science

journal homepage: www.elsevier.com/locate/ces

Dynamics of drop formation, growth and pinching phenomena from

a submerged nozzle
Abhik Majumder a, Dibyendu Ghosh b, Prasanta Kumar Das b,⇑
a
National Institute of Technology Agartala, Department of Mechanical Engineering, Agartala, Jirania 799046, India
b
Indian Institute of Technology Kharagpur, Department of Mechanical Engineering, Kharagpur 721302, India

h i g h l i g h t s

Drop formation from submerged nozzles in an immiscible liquid is reported.

Transition from dripping to jetting, shape oscillation, neck radius fluctuation investigated.

Dependents of pinching on velocity and fluid properties investigated.

Different regimes of drop formation identified.

a r t i c l e i n f o a b s t r a c t

Article history: Drop formation is studied through a comprehensive experimentation, injecting different lighter fluids in
Received 23 December 2020 an immiscible liquid, over a range of velocities, from submerged nozzles of four different diameters. The
Received in revised form 22 March 2021 process involves a number of unique interfacial developments, namely inception and growth, neck for-
Accepted 26 May 2021
mation and pinching, drop departure, etc. The study emphasizes on the dynamical aspects like shape
Available online 29 May 2021
oscillation on the nozzle tip, neck radius fluctuation, length variation of the leading edge (Lv ) etc. At a
low flow rate, the retractile motion of the remnant mass is found responsible for shape alteration. The
Keywords:
process of drop pinching exhibits radial fluctuation of the neck and depends on both flow rate and vis-
Drop generation
Immiscible liquid
cosity. Moreover, in an unconfined system, drops may be generated with increased frequency within
Necking and pinching the limit of the dripping regime while keeping Lv approximately unchanged. Different regimes of drop
Dripping formation have also been identified.
Jetting Ó 2021 Elsevier Ltd. All rights reserved.

1. Introduction
The formation of liquid drops by injecting one liquid into
another immiscible liquid through an orifice or a nozzle is widely
used in many industries. By regulating the operating parameters,
drops of the desired volume can be formed at a required frequency
by the breakup of the injected liquid mass. For convenience, let us
term the drop-forming liquid as the dispersed phase and the other
as the bulk liquid phase. If the dispersed phase is lighter than the
bulk phase, the opening of the nozzle or the orifice is made to face
upward, then the dispersed phase liquid drops move up. When the
dispersed phase is heavier, the nozzle is made to face down and
drops fall through the bulk liquid after formation. Further, irre-
spective of the upward or downward facing orientation of the noz-
zles, the drop may form immediately at the nozzle outlet or the
⇑ Corresponding author.
E-mail address: pkd@iitkgp.ac.in (P. Kumar Das).
injected liquid mass may take a shape of a liquid jet of finite length
at the nozzle outlet. Eventually, drops are produced from the tip of
the jet. The drop formation in the dripping and the jetting regimes
are illustrated in Fig. 1. The phenomenon of drop formation at the
nozzle end is termed as dripping irrespective of upward or down-
ward movement of the drops and the formation of a jet at the noz-
zle tip is commonly described as jetting (Homma et al., 2006). As
the dispersion of one liquid into the other, in the form of droplets,
provides a large interfacial area, these basic arrangements find
wide applications in a variety of processes and equipment like a
liquid–liquid contractor, chemical reactors, distillation, pathologi-
cal investigations, extraction and emulsification etc. (Chaurasia
et al., 2015; Hayworth and Treybal, 1950; Wang et al., 2009;
Zhang, 1999). In recent years, various unique applications of drop
formation in a host of an immiscible liquid have been proposed
for microfluidic devices and different flow focusing techniques
have also been postulated (Cramer et al., 2012; Nie et al., 2008;
Utada et al., 2007).

https://doi.org/10.1016/j.ces.2021.116808
0009-2509/Ó 2021 Elsevier Ltd. All rights reserved.
A. Majumder, D. Ghosh and P. Kumar Das Chemical Engineering Science 245 (2021) 116808

Nomenclature

As Drop Surface area, mm2 t Time, s

a Major axis of a drop, mm tp width of the elemental disk, mm
b Minor axis of a drop, mm Un Flow velocity through nozzle, m/s
a=b Aspect ratio Vd Final volume of drop, mm3
Di Inner diameter of nozzle, mm Vavg Average volume of drop, mm3
DF Diameter of the detached drop, mm Vp Primary volume of a drop, mm3
di the diameter of the ith elemental disk, mm
dw Wetting diameter, mm Greek symbol
g Gravitational acceleration, m/s2 q Density, kg/m3
ID Inner diameter, mm qd Density of dispersed phase, kg/m3
Lbf Break off length, mm ri Interfacial tension, N/m
Lv Leading edge length of a drop, mm l Viscosity, mPas
Oh Ohnesorge number lr Ratio of viscosity,
Ql Volume flow rate, ml/min h Instantaneous Contact angle, degree
Re Reynolds number Dq Density difference, kg/m3
Rn Neck radius, mm kc Capillary length, mm
R0 Nozzle outer radius, mm s Non dimensional time

The majority of the literature on drop formation can be catego-
rized into two groups, viz.: unconfined drop formation in quiescent
or flowing liquid and confined drop formation in microfluidic chan-
nel configurations (Utada et al. 2007; Shah et al. 2008; Meyer and
Crocker 2009; Cramer et al. 2012; Josephides and Sajjadi 2015;
Bertrandias et al. 2017). The unconfined arrangement of drop for-
mation is employed over the ages due to its simplicity,
buoyancy-driven upward or downward motion of drop based on
specific gravity (Hayworth and Treybal, 1950). Drops of macro,
micro, and nanometric dimensions from such systems may also
find application in process equipment, artificial cell, bio-
encapsulation, drug delivery, and membrane separation (Chang
2004; Bremond et al. 2010; Chaurasia et al. 2015). Though drop
formation in liquid–liquid systems enjoys diverse applications,
the phenomenon is still left with many unresolved issues such as
Fig. 1. Dripping and jetting of immiscible dispersed fluid in buoyancy assisted
unconfined system.
2
the effect of viscosity ratio on the mechanism of pinching, mecha-
nism of transition from dripping to jetting (Chaurasia et al. 2015),
apparent contact angle behavior (Wang et al. 2009), the effect of
dispersed liquid property and nozzle diameter on the transition
from dripping to jetting etc.
Over the years, a variety of research investigations have been
carried out on the formation of liquid drops in the host of an
immiscible liquid through a submerged nozzle (Harkin and
Brown, 1919; Smith and Moss, 1917; Hayworth and Treybal,
1950; Null and Johnson, 1958). The prediction of drop shape and
estimation of drop size has been the prime attention of such work
due to the importance of the interfacial area in the transport mech-
anism of different industrial processes. The review work of Bogy,
(1979), Lin and Reitz, (1998) and Eggers and Villermaux, (2008)
provides good detail of numerous investigations carried out on
drop formation in liquid, air, or gas phase. In the past, in addition
to experimental investigation for drop size estimation under varied
external fluid properties, several attempts have also been made to
develop correlation for drop volume (Rao et al.1966; Scheele and
Meister, 1968; Heertjes et al. 1970, Izard 1972) as a function of
fluid properties.
On the other hand, a good number of numerical simulation
works were also found to investigate the drop formation from a
submerged nozzle. For example, Homma et al. (2006)employing
the front tracking method computationally explored the immisci-
ble liquid jet formation for axisymmetric condition and predicted
a regime map of dripping to jetting transition while varying the
Weber number and the viscosity ratio of the phases. Lakdawala
et al. (2014, 2015) numerically investigated the formation of a drop
in the immiscible system and showed periodic and non-periodic
formation patterns both in dripping and jetting regime. More
recently, using a coupled level-set and VOF method, Borthakur
et al. (2017) showed a drop interface overturning at a critical
Ohnesorge number.
In a unique experimental study, Wang et al. (2009) studied the
change in current contact angle with time until the drop detached
from a nozzle of outer diameter 0.508 mm using the organic liquid
in stagnant water. They found that the slope of the current contact
angle coincides with the drop formation stages except for the
detachment stage. However, to date, no experimental data
reported on the effect of nozzle radius, dispersed phase viscosity,
and flow velocity on neck radius, pinching process, etc. More
recently, considering the effect of dynamic interfacial tension on
drop volume for a nozzle inner diameter of 0.23 mm, Chaurasia
A. Majumder, D. Ghosh and P. Kumar Das
et al. (2015) investigated the effect of injection velocity of dis-
persed phase on polydispersity and pinching time for three differ-
ent alkanes. However, the effect of nozzle diameter and dispersed
phase viscosity on transition remains mostly unexplored. The
necking and subsequent motion of a separated drop of aqueous
glycerol in silicon and mineral oil were investigated by Patrascu
et al. (2017). They found that neck filament rupture time increases
with the viscosity of the dispersed liquid and detached drop
rapidly attains constant velocity.
The majority of the semi-empirical or correlation-based
approaches for the prediction of drop characteristics use either
force balance type mechanistic and oversimplified models while
ignoring the effect of the contact line, wetting phenomena, an
approximate model for drag force, etc. On the other hand, the
numerical works are also handicapped from the limitations of suf-
ficient computational resources, absence of precise contact angle
model, wetting model, limitations of axisymmetric consideration,
etc. In view of the above, the role of experimental investigation
is beyond doubt for such a complex phenomenon.
Most of the earlier investigations attempted to predict the drop
volume, Sauter diameter, jet length, etc. under different flow con-
ditions. However, a very limited number of studies considered the
effect of dispersed liquid viscosity, interfacial tension and nozzle
diameter on resulting drop dynamics and mechanism of neck for-
mation and neck pinching. The neck pinching process is a very
important stage of drop separation and significantly influences
the drop dynamics. Moreover, the effect of properties of the dis-
persed phase and nozzle diameter on drop characteristics such as
drop size, drop leading edge length are not well understood. In
the present work a comprehensive study is undertaken to under-
stand the effect of (1) nozzle diameter, (2) dispersed phase viscos-
ity and (3) interfacial tension on (1) drop volume, (2) drop leading
edge length at detachment and (3) neck radius and pinching pro-
cess. In the present investigation dynamical aspects of drop forma-
tion such as shape oscillation on nozzle tip, neck radius fluctuation,
drop volume, and leading-edge length of a drop are revisited with
the parametric variation of nozzle diameter and viscosity ratio. The
process of drop pinching is found to depend on both the flow rate
Fig. 2. Schematic of the experimental facility.
3
Chemical Engineering Science 245 (2021) 116808
and viscosity of the injected fluid. Further, a radial fluctuation of
the neck was also noted for fluids of high Ohnumber. A wide range
of data for four different dispersed liquids injected through nozzles
of four different diameters is presented.
2. Experimental facility and procedure
The present investigation on drop formation is primarily
experimental. A schematic of the experimental facility is presented
in Fig. 2. The main constituent is an acrylic (poly-acrylic-
methacrylate) rectangular container of dimension 100 mm 
100 mm  300 mm with its top open to the atmosphere. An over-
flow hole of 4 mm diameter is placed in one of the container faces,
thus a constant height of 250 mm liquid is maintained. At the center
of the bottom surface of the container, a steel nozzle is fitted verti-
cally on top of an adjustable mount. A steel tube of 2 mm diameter
is connected to the other end of the mount. Through this steel tube
lighter liquid (dispersed fluid) is supplied at a constant flow rate
from a Harvard make infusion pump (accuracy 0.35%). A Phantom
make V1211 high-speed camera with Nikon 60 mm micro zoom
lens (maximum resolution of 1280  800 pixel) is used to record
the evolution of the drop at the nozzle tip at frame rates up to
8000 frames per second. The number of the representative pixel
corresponding to the nozzle outer diameter is counted to obtain
the scale of physical dimension from the captured images. The scale
of such physical dimension is shown in the respective images.
Before each of the experimental runs, the acrylic container is
thoroughly cleaned and is filled with de-ionized water up to a
height of 250 mm. The small air bubbles attached to the con-
tainer wall are carefully removed to establish a clear path for
recording the images. The overflow opening allows the drainage
of the accumulated lighter fluid on top of the heavier fluid during
the experiment and maintains a constant level of the heavier fluid
on top of the nozzle tip throughout the experimental run and for
all the experiments, ensuring uniform and constant hydrostatic
head at the open end of the nozzle. The lighter fluid is carefully
filled in a new syringe and the selected flow rate is maintained
A. Majumder, D. Ghosh and P. Kumar Das Chemical Engineering Science 245 (2021) 116808

Table 1
Properties and range of flow rate of the fluids used.

Type of Phase Fluid Viscosity (mPas) Density (kg/m3) Interfacial Tension (N/m) Refractive Index Flow rate (ml/min)
Dispersed kerosene 1.640 810.00 0.0324* 1.440 0.525–14.70
Dispersed cyclohexane 0.860 778.10 0.0480* 1.426 0.525–16.80
Dispersed n-heptane 0.336 679.50 0.0491* 1.385 0.525–12.39
Dispersed n-hexane 0.300 645.80 0.0494* 1.375 0.525–12.39
Bulk Deionized water 0.890 998.00 0.0729** 1.330 Stationary
*
Interfacial Tension of the dispersed liquid with water.
**
Surface tension of water with air.

by using the infusion pump. The length of the nozzle is kept 25
times the inner diameter of the nozzle. This acts as a flow
straightener and renders the flow axial at the nozzle exit. Four
nozzle of inner diameter (ID) 1.0, 0.6, 0.4 and 0.3 mm respec-
tively, are selected to study the effect of diameter. Also, four dif-
ferent lighter fluids are carefully selected for the present work (at
a temperature of 25 °C of all the fluids used in the investigation
are given in Table 1). These fluids were chosen for their water
immiscibility as well as a variation of properties such as viscosity,
density, and interfacial tension etc. The experiments are con-
ducted at room temperature, which was close to 25 °C and no
appreciable variation in properties was present. The immiscibility
with the bulk fluid and density lower than it (water in this case)
were two important criteria for the selection of the dispersed
fluid. It may further be noted that, only readily available natural
fluids have been considered. Among the available options a selec-
tion has been made so that some variation is there in the trans-
port properties of the dispersed fluids.
Before switching over from one dispersed fluid to the other, the
steel tube and nozzle are thoroughly cleaned and a fresh syringe is
used. The high-speed video camera is placed at the desired location
to obtain the best quality images through optimally choosing the
focal length of the lens. Sufficient backlight is provided by an
LED array placed behind a diffusion screen to capture the drop
images. Care is taken for proper illumination and camera position.
All the fluids used in the experiments are almost colorless and
transparent enabling the capture of images only due to the relative
difference of refractive index between the host and dispersed flu-
ids. No die/additive is added to any fluid to avoid contamination
and deviation in fluid properties.
Images are recorded two minutes after the appearance of the
first drop to allow the internal flow field of the heavier fluid to
develop and settle in response to the injected lighter fluid motion.
This is also done to confirm that the bulk liquid is pre-saturated
and the top surface of the heavier fluid in the container obtains a
thin layer of lighter fluid. This ensures the drainage of lighter fluid
becomes continuous, thereby endorse minimum disturbance in the
operating conditions. The repeatability of the experimental results
has been checked carefully. At a low flow rate (Re ¼ 27 for all the
fluids), the experiments were repeated at least four times. At other
conditions, random check of repeatability have been made from
time to time. Careful observations are made to understand drop
formation and evolution, pinching, post-pinch-off development of
remnant mass, detachment, etc. through the processing of the
recorded images. The images are recorded at a speed range of
2000 to 8000 frames per second. The captured images are analyzed
using P.C.C., MATLAB, and the software Image-Pro Plus. The details
of image processing are given in the subsequent section.

Fig. 3. Steps of image processing (a) to (e). (f) Unit disk representation of a typical fictitious drop. (g) Schematic of elemental frustum .

4
A. Majumder, D. Ghosh and P. Kumar Das
The original image is first converted to a greyscale image fol-
lowed by cropping operation to remove the nozzle from the image.
Initial wiener filter is applied on the greyscale image to reduce
noise. A threshold method with a user-defined fudge-factor value
of 0.8 is applied to identify the drop borderline. To eliminate the
unwanted spots from the image a secondary noise reduction filter
is also applied. The resultant image is then converted into a binary
image as shown in Fig. 3 (a) to (e). The final binary image is pro-
cessed to obtain the coordinates of elemental frustum as shown
in Fig. 3 (f) and (g) to calculated the drop surface area and volume
using following equations (Sabliov et al., 2002).
vffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
)ffi
u( 2
X
n
p u di diþ1
As ¼ ðdiþ1 þ di Þ t  þ tp 2
2 2 2 depending upon their length. Further, the separated drops may
i¼1
X
n
pt p  2 2

Vd ¼ diþ1 þ di þ diþ1 di
i¼1
12
3. Result and discussion
3.1. Overview of submerged drop formation
To provide an overall idea of the evolution of the dripping pro-
cess through submerged nozzles, we have selected some typical
experimental runs involving the flow of cyclohexane as the dis-
persed fluid through a nozzle ID of 1.0 mm. Initially, at a very
low flow rate, nearly monodispersed drops are produced as can
be observed in snapshots 1–3 of Fig. 4. Furthermore, the drops
are also formed at very regular intervals. The flow rate is gradually
increased, and eventually, the lighter liquid issues in the form of a
jet and a liquid column of constant height appear at the nozzle exit
with a shift of the drop formation process from the nozzle tip to the
tip of the jet. The uniformity in drop diameter is ultimately lost at
higher flow rates.
In general, as the flow rate increases, drop generation frequency
increases along with a decrease in drop size. The break-off length
of the liquid jet, as marked with an arrow in snapshot 6, increases
gradually (snapshot 1–5) with the increase in flow rate. Interest-
ingly, a steep increase in break-off length, as noticed in snapshot
5, reveals a probable onset of transition from dripping to the jetting
regime. The onset of the transition state is identified by quantifying
this break-off length, which is found approximately three times the
nozzle’s outer diameter (Chaurasia et al. 2015). Till snapshot 3,
Fig. 4. Cyclohexene drop formation in stagnant water at various flow rates from a nozzle of the inner diameter of 0.99 mm. Starting from snap 1–11, corresponding flow rates
are (1) 3.07 ml/min; (2) 8.200 ml/min; (3) 10.250 ml/min; (4) 12.300 ml/min; (5) 14.350 ml/min; (6) 16.400 ml/min; (7) 18.450 ml/min; (8) 22.550 ml/min; (9) 26.65 ml/min;
(10) 30.750 ml/min; and (11) 34.850 ml/min respectively. The bar represents the outer diameter of the nozzle.
Chemical Engineering Science 245 (2021) 116808
separated droplets are more or less spherical and waves are not
seen in the stem or the column of the lighter liquid emanating from
the nozzle end. In snapshot 6 the formation of the wave in the liq-
uid jet is discernable and the pinching point corresponds to a node
of the wave. Further, the separated droplet is rather elongated indi-
cating an early pinch-off at a particular node before the liquid mass
above the node has enough time to assume a spherical shape. The
presence of the wave becomes more prominent in the succeeding
snapshots, and interestingly, the separated mass of the lighter liq-
uid depicts a tadpole-like shape with an oval head and a narrow
thread-like tail (snapshot 8 and 9). Nodes and anti-nodes are also
visible in the elongated structure severed from the liquid jet. The
severed liquid structures are seen to generate a number of drops
ð1Þ
be seen colliding with one another downstream of the jet tip where
the succeeding drops are forming. Thus the process of collision
may affect the formation of succeeding drops (snapshot 9). With
ð2Þ
the increase of flow rate, the jet becomes sinuous, particularly at
the upper end, as can be seen in snapshot 11.
3.2. Evolution of remnant mass into a new drop
The detachment of a drop from the nozzle is an important stage
of drop formation. The evolution of the prevailing interface drasti-
cally varies with the change in flow rates. The remnant of the
pinched drop attached to the nozzle tip serves as the nucleus for
the succeeding drop. The separation of a drop at the near nozzle
and far nozzle is discussed in the preceding sections. After a suc-
cessful drop separation, interfacial force driven recoiling of a liquid
interface attached to the nozzle tip is observed at a low flow rate.
Immediately after a successful pinching, the remnant liquid mass
attached to the nozzle tip undergoes retracting motion due to
the interfacial force acting to minimize the elongated conical inter-
facial area against the inertial and viscous force of the dispersed
liquid. In due course, these motions establish a greater degree of
interface sphericity through a transition of interfacial shape
(Zhang, 1999). The pre-pinching flow momentum can significantly
affect the recoiling shape (Sierou and Lister, 2004). At low and
intermediate flow rates, it is noticed that this retracting recoil
velocity is sufficient enough to overcome the combined instanta-
neous buoyancy and internal flow inertia resistance. The present
investigation also reveals that such retracting motion can intro-
duce oscillations and readjustment of shape (such as prolate to
oblate) as shown in Fig. 5.
5
A. Majumder, D. Ghosh and P. Kumar Das
Fig. 5. Shape oscillation of a the remnant mass after a successful pinch-off;
dispersed fluid cyclohexane, flow rate of 1.06 ml/min, nozzle ID of 0.3 mm. The first
shape reversal may be noted at 1.5 ms (approx.).
Fig. 5 illustrates the shape oscillation of remnant mass for a typ-
ical cyclohexane drop formed through nozzle ID of 0.3 mm; the
aspect ratio a=b decreases initially due to the retracting motion.
At 1.5 ms, the initial shape alteration of interface configuration is
due to retraction, as shown in Fig. 5. Thereafter, the aspect ratio
reaches 1.29 at 3.62 ms, again only to assume a value approxi-
mately unity at 6.0 ms. Here, aand b are the longitudinal and lateral
dimensions of the remnant liquid mass respectively. During the
period of shape oscillation, the three-phase contact line may also
undergo advancing and retracting motion and may modify the
wetting perimeter. Subsequently, the oscillation of the drop is seen
to dampen with elapsed time. However, as the nozzle diameter
Fig. 6. The formation of a cyclohexane drop from jet column and retracting motion of the interface induced by interfacial force. The formation of neck at a flow rate of
8.25 ml/min through a nozzle of ID 0.3 mm. The bar represents 0.56 mm.
6
Chemical Engineering Science 245 (2021) 116808
increases, we observe a relatively lesser variation in aspect ratio.
This may be primarily due to the effect of gravitational force (large
liquid mass attached to bigger nozzle tip) in addition to the viscous
and inertial resistance responsible for the rapid dwindling of the
retracting momentum. At higher flow rates, the drop forms by sep-
aration from a liquid jet far away from the nozzle tip. The forma-
tion of node and anti-nodes are clearly visible on the liquid
column. Post-separation of a drop, the retracting motion induced
by interfacial force at this stage causes backward motion of the
interface which may assist in the formation of neck as illustrated
in Fig. 6 with a series of snapshots taken for cyclohexane at a flow
rate of 8.25 ml/min. The phenomena are also observed for other
dispersed fluids.
3.3. Process of pinching of a drop
The process of pinching is the last stage of drop formation. At
this stage, the drop finally separates from the nozzle tip. At the
dripping regime, the quantitative estimation of the duration of
drop formation not only helps to understand the pinching process
but also brings out the effect of viscosity ratio (lr ) on the pinching.
Fig. 7 shows a comparison of cyclohexane, kerosene and n-hexane
drop formation at an identical flow rate of 3.07 ml/min through a
nozzle ID of 1.0 mm. The transport properties of the dispersed liq-
uids are not identical. Since the flow rate is the same for all the flu-
ids presented in series a, b and c in Fig. 7; the comparison depicts
the fluid properties on drop generation. Wang et al. (2009) showed
the dynamics of wetting radius for a first drop formation through a
nozzle and reported that the dispersed fluid interface may be
pinned at the nozzle outer radius for subsequent drop formation.
For the present analysis, the neck thinning and pinching of a drop
are reported where the drop interface is pinned at the outer radius
of the nozzle. The photographic evidence from Fig. 7 shows that
the nozzle is completely wetted by all the fluids suggesting an
equality of wetting radius. Therefore, considering the same wetting
radius, the variation in pinching time can be explained by compar-
ing thelr (viscosity ratio). In view of that, the drop evolution time is
divided into two intervals; namely, pre necking time or drop-
growth time (primary growth time) and post necking time or
pinching time.
Snapshot series d1 to d6 shows the evolution of neck radius of a
kerosene drop for a flow rate of 11.13 ml/min. An Oscillatory
A. Majumder, D. Ghosh and P. Kumar Das
Fig. 7. Drop formation of cyclohexane (a1-a5), kerosene (b1-b5) and n-hexane (c1-c5) at a flow rate of 3.07 ml/min. Snapshots a3, b3, and c3 depict a typical drop
configuration (h  p=2). Snapshots 5 for all the three fluids depict pinch off, nozzle inner diameter 1.0 mm.
evolution of neck radius is shown in d4 and d5. The bar represents
1.264 mm.
Here, necking time signifies the time elapsed starting from the
inception of a drop to reach the state of neck formation, identified
by h  p=2(see a3, b3, and c3 in Fig. 7). Whereas, the pinching time
indicates the separation time of a drop from the state of h  p=2.
The evaluation of photographic data shows that even though the
dispersed fluid flow rate and nozzle diameter are the same for all
the liquids, the estimated drop generation frequencies differ
(0.729, 1.081 and 1.159 for cyclohexane, kerosene and n-hexane
respectively). For instance, for a flow rate of 3.07 ml/min, for a typ-
ical cyclohexane drop, as shown in Fig. 7 (series a1-a3), the time of
neck formation is 1.371 sec. For the same flow rate, this value is
much larger than those recorded for kerosene and n-hexane. On
the other hand, for the same flow rate of 3.07 ml/min, the pinching
time (0.091 sec) for kerosene is found higher than that of cyclohex-
ane (0.073 sec) and n-hexane (0.064 sec). The high viscosity of the
dispersed liquid resists the gravitational acceleration (Longmire
et al., 2001) causing the thinning of the drop stem during a final
pinch; the pinching time is found large in case of higherlr fluids.
Initially, for the same flow rate, the pinch-off of a drop from the
nozzle tip through the process of thin liquid thread formation is
found similar for all the fluids. The length of the liquid thread is
small and the neck radius is seen to decrease monotonically as
shown in Fig. 7 for a flow rate of 3.07 ml/min. Here, the computa-
tion of pinch-off time begins from the position (h  p=2) as shown
in a3, b3, c3 and d3 of Fig. 7. The pinch-off time is found dependent
on dispersed phase viscosity and increases with an increase in vis-
cosity. One can easily note the largest pinching time (0.113 sec) of
kerosene (highestlr ) at a flow rate of 1.06 ml/min compared to
that of the other fluids as shown in Fig. 8. In this range, as the iner-
tia force is less, the buoyancy force pulls the liquid interface
against the interfacial tension. However, close to the end of the
dripping regime (flow rates 10.6–12.72 ml/min), such pinch-off
process is found to occur from longer liquid threads and is sub-
jected to an oscillatory radial reduction of the neck as shown in
Fig. 8 (a) and (b). Also, the pinching time in these cases is found
to increase due to the high viscous resistance during neck filament
thinning. Such phenomena are not observed for dispersed fluids of
low lr as noted in Fig. 8 (c) and (d). Fig. 7 (series d1-d5) provides a
photographic sequence of the oscillatory reduction of the neck of a
7
Chemical Engineering Science 245 (2021) 116808
kerosene drop for a flowrate of 11.13 ml/min. After an initial thin-
ning attempt at time 0.278 sec, the neck radius reaches to
0.486 mm. However, with the additional support of viscous resis-
tance of the dispersed liquid, the relatively high momentum flux
intends to resist the breakup by acting against the strong capillary
force driving the breakup process (Patrascu et al., 2017). Such
resistance may even lead to expansion of the neck as shown in
Fig. 7 (d5) at 0.291 sec. Finally, the drop pinch-off takes place at
0.306 sec.
3.4. Effect of nozzle diameter and dispersed fluid property on the drop
volume
For efficient transport of species and heat transfer enhance-
ment, surface area and volume of a drop are considered the most
important influencing parameters. Therefore, the study of these
significant drop characteristics is necessary. Fig. 9 (a) depicts the
variation of average volume of cyclohexane drop and standard
deviation of drop sizes against the injection velocity in nozzle ID
of 1.0 mm. In general, the average drop volumes are noted to
increase at the beginning up to injection velocity of 0.092 m/s;
beyond this velocity, a decrease in average drop volume is
observed. As the injection velocity of the dispersed liquid
increases, fluctuations are noted in the process of drop formation.
As a result, at a particular injection velocity, a range of drop sizes
(around a mean drop) are noted. It is thought that the standard
deviation of the drop volume could be a good indicator of the
hydrodynamics o the drop formation. The standard deviation of
drop volumes is found insignificant for low injection velocities;
however, it increases considerably as the velocity increases. Based
on the values of standard deviation (SD), the process of drop gen-
eration can be divided into three regimes viz. regime 1 (0 < SD < 0.
2), regime 2 (0.2 < SD < 1.5) and regime 3 (1.5 < SD < 6.0).
In regime 1, the drop formation is essentially dripping in nature.
The drop formation process is periodic, symmetric, and mono-
dispersed. In regime 2, with intermediate standard deviation,
uneven drop formation is noted. The process of drop formation is
still dripping in nature; however, variation in drop volume and
asymmetry in drop shape at the instant of detachment is often
observed. In this regime, we also noted the formation of the long
stem at the nozzle tip (See d1 and d6 in Fig. 7). This is the regime
A. Majumder, D. Ghosh and P. Kumar Das
Fig. 8. Change of non-dimensional Neck radius with pinching time. The inner diameter of the nozzle is 1.0 mm.
where the transition from dripping to jetting takes place. In regime
3, the drop formation is essentially jetting in nature. The drops are
now formed from a steady liquid column far away from the nozzle
tip. In this regard, it is essential to know the drop volume distribu-
tion to ascertain the effect of injection velocity. In regime 1, the
standard deviation of the volume is very low implying uniform
drop generation.
Fig. 9 (b) shows the probability distribution of drop volume at
an injection velocity of 0.275 and 0.321 m/s in regime 2; and
0.367, 0.413 and 0.504 m/s in regime 3. In regime 2, the probability
distribution exhibits a narrow range compared to regime 3, essen-
tially signifying a lesser variation of drop volume in regime 2. Also,
as the injection velocity increases, the left arm of the bell curve
shifts towards the lower end of the range. This indicates the forma-
tion of smaller drops at a higher velocity.
Though experiments have been conducted with four different
nozzles, systematic variations of flow rates over a considerable
range could be made only in nozzle IDs of 1.0 mm, 0.6 mm and
0.4 mm. Nozzle ID of 0.3 mm, which has the lowest inner diameter,
could not be operated over a wide range of flow rates. Within the
operational limits, efforts have been made to collect the maximum
number of experimental data to facilitate a good comparison and
cover a wide range of flow rates. Fig. 9 (c), (d), and (e) show the
8
Chemical Engineering Science 245 (2021) 116808
drop volume variation for all the fluids generated in nozzle ID of
1.0 mm, 0.6 mm, and 0.4 mm respectively. In this plot, only the
drop volume of the primary drops (largest) are considered. This
does not affect the results as the primary drop volume is of the
order of mean drop volume. From these plots, it is clearly discern-
able that for a particular nozzle, the drop volume differs as the
injected fluid is varied in all three regimes identified earlier. More-
over, as the nozzle size decreases, the drop volume also decreases
irrespective of injected dispersed fluid. Further, it is noticed that at
any particular flow rate within the regime 1 and 2, the cyclohexane
drop volume is the highest compared to other fluids (see Fig. 9 (c),
(d) and (e)). This difference in drop volume reduces after the tran-
sition. It has been observed that with the change in dispersed liq-
uid properties such as interfacial tension, density, and viscosity;
significant variations in the final drop diameter and volume are
noted particularly in the dripping regime.
At a particular nozzle, the generated drop sizes are measured
for variation in dispersed fluid properties and injection velocity.
Such an assessment may help understand and compare the influ-
ence of interfacial tension and the viscosity ratio on overall drop
size. In Fig. 10 the drop volume of cyclohexane, kerosene, n-
heptane, and n-hexane are plotted against the injection velocity
of the dispersed phase for nozzle ID 1.0 mm. Within the range of
A. Majumder, D. Ghosh and P. Kumar Das Chemical Engineering Science 245 (2021) 116808

Fig. 9. (a) Average drop size vitiation with an increase in the flow rate of cyclohexane in nozzle 1; (b) Probability density of cyclohexane drop volume formed at nozzle ID of
1.0 mm with an increase in injection velocity; (c), (d) and (e) drop volume variation with an increase in injection velocity in nozzle ID of 1.0 mm, nozzle ID of 0.6 mm and
nozzle ID of 0.4 mm respectively.

reported injection velocity, the variations in drop formation regime
like dripping (a, d, g, and j), intermediate (b, e, h, and k), and jetting
(c, f, i, and l) are also noted (see the snapshots of individual dis-
persed fluid in Fig. 10). In the present case, the drop volume is
obtained by averaging ten consecutive drops since an uneven drop
formation is present in the intermediate and jetting regime. To
compare the present experimental result, the proposed correlation
of Scheele and Meister,(1968) is also plotted in the same figure for
each fluid separately.
2 !1=3 3
pri Di 20lQ l Di 4qd Q l U n Q 2l D2i qd ri
V d ¼ F4 þ 2  þ 4:5 5 ð3Þ
g Dq D F g Dq 3g Dq ðg DqÞ2
At a very low injection velocity, we find a very well match
between the present experimental results except for kerosene.
The reason for the deviation in the case of kerosene is not apparent.
Although, the correlation is found to predict the trend correctly.
9
For high flow rates, we find a large deviation between experimen-
tal data and the correlation. It is factual to mention here that the
proposed correlation is limited to low injection velocities only.
Nonetheless, cyclohexane is found to generate the largest drop
among the groups, especially in the dripping regime. It is reported
in the literature (Byakova et al., 2003; Gnyloskurenko et al., 2003)
that the final drop volume is dependent on factors such as three-
point contact line position, the wetting characteristics of the liq-
uids, the contact angle hysteresis, the thickness of the nozzle wall
(Clanet and Lasheras, 1999), etc. We propose to probe the issue fur-
ther. While recognizing the difficulty to practically separate out the
effect of all the above factors, at a very low flow rate, we assume
and define capillary length as, kc  ðri =Dqd g Þ1=2 by comparing
the interfacial tension with gravitational force and used it as the
characteristic length. The value of kc is 4.69 mm, 4.14 mm,
3.95 mm and 3.84 mm for cyclohexane, kerosene, n-heptane, and
n-hexane respectively. Moreover, to understand the effect of
A. Majumder, D. Ghosh and P. Kumar Das
Fig. 10. Comparison of drop volume of cyclohexane, kerosene, n-heptane, and n-hexane are plotted against the injection velocity; the nozzle ID is 1.0 mm. The bar represents
1.264 mm.
dispersed phase viscosity on drop formation, the combined role of
viscous, inertia, and interfacial tension forces needs to be ascer-
tained. With kc a characteristic length, we define Ohnesorge (Oh)
number as (Mckinley et al., 2011)
!1=2
 
t Viscocapillary ld k c q k3 l a decrease in drop volume. Recently Chaurasia et al. (2015) also
Oh ¼ ¼ = d c ¼ pffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi
d
ð4Þ
tRayleigh ri ri ðqd kc ri Þ
The calculated values of Oh are 4.469  103, 10.170  103,
2.125  103, and 1.676  103 for cyclohexane, kerosene, n-
heptane, and n-hexane, respectively. Clearly, there are two groups,
viz. higher (cyclohexane and kerosene) and lower Oh (n-heptane
and n-hexane). The Oh number essentially signifies the ratio
between visco-capillary time tViscocapillary (which describes the thin-
ning mechanics of liquid thread under visco-capillary effect) and
Rayleigh time tRayleigh (which characterizes the breakup of inviscid
liquid thread or jet) (Eggers, 1993). Since, for a fluid with a large
Ohnumber, visco-capillary time is large, hence the time required
for liquid necking is more, which would eventually feed more liq-
uid into the drop during the drop growth stage as constant flow
rate condition is maintained at nozzle end.
The above comparison shows that cyclohexane has the highest
value of kc and an intermediate value of Ohnumber. This combina-
tion of Ohand kc completes the picture of all forces excluding iner-
tia force, which can be neglected in the dripping regime. For the
present study, cyclohexane with the highest kc (largest capillary
length) and the intermediateOh number may yield the largest
drop, compared to other dispersed liquids irrespective of nozzle
diameter as experimentally evident from Fig. 9 (c), (d), and (e).
Even though kerosene shows the largestOh value, its capillary
length is smaller than cyclohexane. Therefore, kerosene forms
smaller drops compared to those formed by cyclohexane, espe-
cially in the dripping regime. However, the exact role of nozzle
top surface wettability by different dispersed fluids could not be
10
Chemical Engineering Science 245 (2021) 116808
ascertained since the observation from images gives a perception
of complete wetting of the top surface.
It is also found that, for kerosene, and cyclohexane, initially, the
drop volume slightly increases with flow rate and reaches the max-
imum value, beyond which a further increase in flow rate results in
observed such phenomena for Octane, Dodecane, and Hexadecane;
but they attributed this change to dynamic interfacial tension (due
to the added surfactant). Since no surfactant is added to the dis-
persed fluid in the present work, the reason for a local maximum
in drop volume in low injection velocity may not be a surfactant.
The higher Ohvalue fluids (cyclohexane and kerosene) have high
visco-capillary time, signifying a longer time for neck and final
pinching of the drop (as already discussed in Section 3.3). There-
fore, a small window may be present in which an increase in flow
rate essentially adds more liquid in the forming drop while pinch-
ing takes place, yielding a larger drop. Accordingly, no sign of local
maximum in drop volume in the case of n-heptane and n-hexane
(which are part of the low Ohgroup) is found as shown in Fig. 9
(c), (d) and (e).
3.5. Effect of dispersed fluid property on drop leading edge length
From the preceding section, we observed that drop formation in
an immiscible environment might exhibit phenomenological dif-
ference in drop separation process, such as drop formation on tip
of the nozzle and drop formation from tip of liquid jet. To study
the influence of nozzle geometry, injection velocity and fluid vis-
cosities etc. on drop geometry, one unifying factor is drop leading
edge length. Drop leading edge length (Lv ) is the distance between
the farthest point of the drop interface in the direction of flow
injection and the nozzle top surface. This dimension is also an
important characteristic length (Zhang, 1999) to investigate the
effect of dispersed fluid properties and flow rate on drop growth.
A. Majumder, D. Ghosh and P. Kumar Das Chemical Engineering Science 245 (2021) 116808

Fig. 11. Variation of Lv against time at different lighter phase Reis illustrated. At the inception of a drop, the seeding height is small for low Re; however, it increases with the
flow rate. The subplot (a) and (b) for nozzle ID of 0.3 mm (smallest); (c) and (d) for nozzle ID of 1.0 mm (largest). The capillary length is shown in solid lines.

With the decrease in nozzle diameter, in the present experiments,
the drop volume decreases all through dripping to jetting. How-
ever, a wide distribution of drop size exists. To understand the
effect of nozzle geometry on drop formation, kc is compared with
Lv , and both are plotted against drop formation time over a range
of dispersed phase Reynolds number (Re)as shown in Fig. 11 for
nozzle ID 0.3 mm (smallest) and 1.0 mm (largest). For both the
nozzles, Lv remains constant over the entire range of Re, as illus-
trated in Fig. 11. However, at the higher end of Re, a sudden
increase in Lv may be witnessed. For nozzle ID of 0.3 mm (smallest),

Fig. 12. Non-dimensional plot of Lv and time for cyclohexane drop (a) nozzle ID of 0.3 mm; (b) nozzle ID of 1.0 mm.

11
A. Majumder, D. Ghosh and P. Kumar Das
Lv is found very close to kc , for all the fluids, only cyclohexane and
n-hexane are shown in (a) and (b) of Fig. 11, respectively.
It is observed that, in the dripping regime, irrespective of dis-
persed fluid, Lv is found very close to kc , particularly in nozzle ID
of 0.3 mm. As the nozzle diameter is increased, a wide difference
in kc and Lv is noticed. One such comparison is presented for nozzle
ID of 1.0 mm in (c) and (d) of Fig. 11. As the nozzle diameter
increases, Lv also increase. However, for a wide range of Re, Lv
remains the same. This is shown with a dotted line in Fig. 11 for
cyclohexane and n-hexane. This implies that in the dripping
regime, even though the inertial force of the dispersed fluid
increases with increases in Re, the drop formation transpires fol-
lowing a consistent geometric pattern (see in Fig. 11). Whereas,
the drop volume found to decrease with the increased generation
frequency. The corresponding snapshot of a typical drop at the
instant of pinch-off is also shown in the plots.
The initial point in the plot of Lv in Fig. 10 shows the inception of
a typical drop. The last point of any individual curve represents the
pinching of a drop from the nozzle tip. Barring the initial shape
reversal (as discussed in Fig. 5), Lv increases monotonically as the
drop grows to exhibit three distinct stages: initial rapid growth
phase during which the drop acquires the stable spherical shape,
steady growth phase up to a state of equilibrium between resistive
and disruptive force while the drop retains its spherical symmetry;
and finally rapid necking phase followed by a detachment of the
drop. These three stages are not very clearly discernable for high
Reflow shown in Fig. 11; however, the non-dimensional plot
shown in Fig. 12 clearly illustrates these stages I, II, and III. This sig-
nifies that in an unconfined system with an increase in flow rate
through the nozzle, drops may be generated with increased fre-
quency keeping the Lv approximately the same.
4. Summary and conclusions
Drop generation in a host quiescent immiscible liquid through a
submerged nozzle is one of the simplest mechanism, yet involves
complex and intriguing interfacial evolution owing to the interplay
among counteractive forces. Although the fundamental theories
underlining the mechanism are reasonably well-advanced; even
so, this requires improvement to apprehend some crucial aspects
of the process. Experiments are conducted to study the dynamics
of drop formation in an unconfined system where the dispersed
liquid is injected through a submerged nozzle into bulk immiscible
liquid. The main focus of the study is to understand the effect of
injection velocity and dispersed fluid property on the behavior of
remnant mass, pinching, drop characteristics, and leading-edge
length variations. Four different nozzles and dispersed fluid are
used to study the effect of some important parametric variation.
High-speed imaging is used to capture the dynamics of different
drop formation stages. In the dripping regime, the measured drop
volume compared well with the existing correlation. Immediately
after a successful drop detachment, the remnant liquid mass
attached to the nozzle tip undergoes retracting motion. The pre-
sent investigation reveals that such retracting motion can intro-
duce oscillations and shape readjustment of the remnant mass.
The process of pinching is the last stage of drop formation. In order
to study the effect of lr on the pinching process, the pinching time
for all the fluids is compared at the same flow rate. The quantita-
tive measurement of the time scale of the drop formation process
at the dripping regime shows the pinching time is large in higherlr
fluids. Whereas close to the end of the dripping regime, such a
pinch-off process occurs from longer liquid threads and is sub-
jected to radial oscillation and subsequent reduction of the neck
radius. The pinching time in these cases is found to increase partic-
ularly for high lr fluids.
12
Chemical Engineering Science 245 (2021) 116808
Based on the values of standard deviation (SD), the process of
drop generation is divided into three regimes viz. regime 1
(0 < SD < 0.2), regime 2 (0.2 < SD < 1.5) and regime 3 (1.5 < SD < 6.
0). The probability distribution exhibits a narrow range in regime 2
compared with regime 3, essentially signifying a lesser variation of
drop volume in regime 2. Also, in the dripping regime, the effect of
dispersed liquid properties such as interfacial tension, density, and
viscosity is found significant and large variations in the final drop
volume are noted. Whereas in regime 3 the effect of dispersed fluid
properties is insignificant. It is also found that barring the initial
shape reversal, Lv increases monotonically as the drop grows to
exhibit three distinct stages in the dripping regime. Also in the
dripping regime, with an increase in Re, even though with
increased frequency and decreased drop volume the drop forma-
tion ensures a consistent geometric pattern.
CRediT authorship contribution statement
Abhik Majumder: Methodology, Conceptualization, Investiga-
tion, Formal analysis, Writing - original draft, Writing - review &
editing. Dibyendu Ghosh: Software, Validation, Writing - review
& editing. Prasanta Kumar Das: Resources, Conceptualization,
Supervision, Project administration, Writing - review & editing.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
Acknowledgement
The authors of this manuscript acknowledge the help and sup-
port received from IIT Kharagpur and NIT Agartala.
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