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    Lab on a Chip c4lc00542b

    Controlled splitting and focusing of a stream of

    nanoparticles in a convergingdiverging

    microchannel

    Ravi Kumar Arun, Kaustav Chaudhury, Moumita Ghosh,

    Gautam Biswas, Nripen Chanda and Suman Chakraborty*WeQ3 demonstrate a convergingdiverging channel design fornanoparticle focusing that facilitates the interaction ofAgNPs with H2O2at an interface.

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    Lab on a Chip

    PAPER

    Cite this: DOI: 10.1039/c4lc00542b

    Received 8th May 2014,

    Accepted 14th July 2014

    DOI: 10.1039/c4lc00542b

    www.rsc.org/loc

    Q1 Controlled splitting and focusing of a stream ofnanoparticles in a convergingdivergingmicrochannel

    Q2 Ravi Kumar Arun,a Kaustav Chaudhury,b Moumita Ghosh,a Gautam Biswas,cd

    Nripen Chandaa and Suman Chakraborty*b

    We demonstrate the potential of a convergingdiverging microchannel to split a stream of nanoparticles

    towards the interfacial region of the dispersed and the carrier phases, introduced through the middle inlet

    and through the remaining two inlets respectively, while maintaining a low Reynolds number limit (

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    2 | Lab Chip, 2014,00, 19 This journal is The Royal Society of Chemistry 2014

    systems (TAS), medical diagnosis and in bottom-up fabrica-

    tion processes, where the primary requirement is to maintain

    controlled reactions and thereby separate specific products.1416

    It is important to mention in the present context that a lot

    of attempts have been made to split streams of micro or

    nano sized particles,13,1721 mainly by utilizing microchannels

    with different geometries.2224 However, the end results are

    mostly confined to the achievement of augmented mixing,

    separation and reaction. On the other hand, the intrinsicmicroscale dimension of the channels can be potentially uti-

    lized for focusing the nanoparticle stream over a particular

    region, by allowing the controlled deposition of particles over

    the channel surface in and around the targeted location.2527

    This may eventually provide a useful means for the fabrica-

    tion of microscale features with finer resolutions.28 Our study

    focuses on utilizing the potential of both the channel geome-

    try and the microscale dimensions, in tandem. Additionally,

    our approach can enable one to maintain control over the

    extent of splitting along the transverse direction.

    Materials and methodsQ5 Problem description with schematic

    Fig. 1 illustrates the schematic of the present converging

    diverging microchannel, with three inlet systems.

    We used the middl e inlet to introduce the dispersed

    phases (i.e. the nanoparticle laden solution), and the other

    two inlets were utilized to supply the carrier phase. We

    maintained the channel height, (H) = 0.15 mm, and length,

    (L) = 25 mm.29 The widths (W) of the converging and diverg-

    ing zones were maintained at 3.3 and 0.8 mm, respectively.

    Throughout the entire study, we maintained the flow rate of

    the nanoparticle laden solution at 25 L min1, and the flow

    rates of the carrier phase were varied as 25, 50, 100 and

    250 L min1. We defined the Reynolds number for a particu-

    lar entity as Re = Deqv/, whereDeqis the hydraulic diameter

    of the flow cross section,v = Q/A(Ais the cross-sectional area

    of the expansion region andQ is the flow rate), is dynamic

    viscosity and is the density of the solution. With the various

    possible combinations of the flow rates, as obtained from the

    mentioned data, we maintained a low Reynolds number limit

    (

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    Lab Chip, 2014, 00, 19 | 3This journal is The Royal Society of Chemistry 2014

    and used as the nanoparticle suspension for the present

    study. The movements of the nanoparticles were monitored

    under a LED fluorescence microscope (Leica DMI 4000B,

    Germany) at a fixed wavelength of 470 nm and 530 nm, for

    the 30 nm and 500 nm size particles, respectively. HereQ7 we

    also observed the controlled divergence of the nanoparticle

    stream, albeit to a further lateral extent than that of the for-

    mer case. Subsequent quantitative colorimetric intensity anal-

    ysis was used to demonstrate the controlled accumulation ofthe polystyrene beads over the interfacial regions of the two

    fluids. With the quantitative evidence in support of this, we

    then moved towards exploiting the potential of the present

    setup in maintaining a controlled reaction and allowing

    the separation of products towards a specific location, as

    endeavoured in the subsequent experimentation with the

    silver nanoparticles and hydrogenperoxide solution.

    Experimentation with silver nanoparticles

    Firstly, we prepared the silver-nanoparticle (AgNP) laden solu-

    tion, following the reported chemical reduction method.

    Briefly, 10 mg of AgNO3 was added to 1 ml of DI water andused as the stock solution. Subsequently, 20 mg of NaBH 4

    was added to 1 ml of DI water and kept in a refrigerator to

    avoid decomposition. Then, 20 mg of sodium dodecyl sul-

    phate (SDS, Sigma Aldrich, Saint Louis, MO, USA) was mixed

    with 20 ml of DI water and stirred for 1015 min. During stir-

    ring, 100 l of AgNO3 from the stock solution was added to

    the SDS solution; the SDS solution was used to stabilize the

    silver nanoparticles. Immediately, 300 l of cooled NaBH4was added to the mixture and stirred for 10 min to achieve

    the yellow colored AgNP solution. Finally, the nanoparticles

    were characterized by UV-absorption spectroscopy and size

    analysis (Fig. S1). The size of the AgNPs was measured usinga NANOSIGHT particle size analyzer (NS500), and was found

    to be in the range of 45 nm. In this case, the movements of

    the nanoparticles were also monitored under a LED fluores-

    cence microscope (Lieca DMI 4000B, Germany). The AgNP

    solution was introduced through the middle inlet, whereas

    the H2O2 solution was introduced through the other two

    inlets. Under the mentioned flow conditions, we observed the

    accumulation of the reaction products in situover the interfa-

    cial region of the two fluids. We also found that the microscale

    dimension of the channel allowed controlled precipitation

    of the reaction products over the bottom glass surface of

    the channel. The microscale features were then observed

    using scanning electron microscopy (SEM) operated at 5 kV

    (Hitachi S-3000N).

    Results

    We began our observation with the coloured dye; the charac-

    teristic features are shown in Fig. 2. This behaviour was

    observed under the flow of the carrier phase at 25, 50, 100

    and 250 L min1 and the dispersed phase at 25 L min1.

    The first noteworthy fact is that we observed a divergence of

    the dye stream; the distribution is earmarked by the

    distribution of the coloured dye with the expansioncontraction

    zone, as shown inFig. 2. Under the mentioned flow rates, the

    Reynolds numbers for the carrier and the dispersed phases

    are found to be 0.585.8 and 1.123.64 respectively. When we

    progressively increased the flow rates of the carrier phase

    from 25 (ReDI = 0.58) to 250 L min1 (Re DI = 5.80), we

    observed a similar behaviour in the dye distribution, as

    shown in Fig. 3. From the figure it is evident that with an

    increase in the flow rate of the carrier phase, the width of the

    dye distribution decreases. From the mentioned observations,it is indicative that the present setup could be utilized to

    focus the stream of particles by controlling the expansion

    contraction of the dye distribution.

    However, it was imperative to investigate whether the

    mentioned behaviours are associated with the channel geometry

    or something else. To investigate this, we also conducted

    experiments with three inlet straight microchannels, with the

    same width as that of the expanded section of the present

    convergingdiverging channel. The results are shown in

    Fig. S2. With the various combinations of the flow rates of

    the carrier and the dispersed phases, we found that none of

    the combinations yield the expansioncontraction type dye

    distribution. Thus, by comparing Fig. 2 and S2, we can

    proclaim that the typical expansioncontraction type dye

    distribution in the convergingdiverging channel is inherent

    to the intrinsic geometry of the channel. However, with the

    change in the combinations of the flow rates, the width of

    the dye distribution changed within the straight channel as

    Fig. 2 Superimposed microscope image of a convergingdiverging

    PDMS microchannel showing the characteristic feature of dye

    distribution in DI water.

    Fig. 3 Dye solution distribution under the flow rates of the carrier

    phase at 25, 50, 100, 250 L min1, keeping the central dye flow rate at

    25 L min1.

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    4 | Lab Chip, 2014,00, 19 This journal is The Royal Society of Chemistry 2014

    well. Thus, the controllability of the system seems to stem,

    mainly, from the flow rate control.

    An important inference that can be drawn from the above

    observations is that the convergingdiverging microchannel

    can cause expansioncontraction of the dye stream. However,

    the size of the dye molecules is typically of the order of the

    size of the water molecules, acting as the carrier phase. Thus,

    it is difficult to analyse the ability of the present setup to split

    the stream of particles. Therefore, to investigate this abilitywe have conducted experiments with the dispersed phase,

    composed of an aqueous solution of polystyrene beads; the

    results are shown inFig. 4for the dispersed phase containing

    the nanoparticles with dimensions of the order of 30 nm. In

    this case we also maintained the flow rate of the dispersed

    phase at 25 L min1, while the flow rates of the carrier

    phase varied from 25 to 250 L min1 (alongFig. 4ad). For

    the sake of quantitative estimation, we also conducted a

    colorimetric intensity analysis by measuring the fluorescence

    intensity of the particles, as shown in the graphs along with

    the corresponding images. From these graphs we can identify

    that the intensities show a deepening tendency around thechannel centreline (specifically see Fig. 4f and g), while

    showing peaks near the interfacial region of the two fluids.

    This estimation suggests the localized distribution of the sub-

    merged nanoparticles, specifically near the interfacial region,

    in contrast to the homogenous distribution all over the dis-

    persed phase region. However, fromFig. 4h, the fluorescence

    intensity based estimation does not confirm the preferential

    splitting of the transported nanoparticles; this may be attrib-

    uted to issues with the resolution.

    For the sake of further verification, we also conductedexperiments with nanoparticles with dimensions of the order

    of 500 nm; the essential features are shown in Fig. 5. We

    obtained approximately similar interfacial distances for the

    500 nm particles with better focusing as compared to the

    30 nm fluorescent particles (compareFig. 4and5). Thus, the

    results confirm that the present setup can be potentially

    utilized for the splitting of streams of nanoparticles and to

    focus them towards the interfacial region of the two fluids.

    We performed similar experiments with the straight micro-

    channel (Fig. S3). We can clearly see that the focusing of the

    nanoparticles is almost absent at all of the flow rate ratios.

    Thus, with the experimental results in hand, it is suggestivethat the inherent geometry of the channel allows such typical

    splitting of the streams of particles and makes them settle

    over the interfacial region.

    After gaining knowledge about the splitting and focusing

    ability of the present setup, we explored the possibility of

    achieving a controlled reaction and the subsequent separa-

    tion of products, as it is one of the primary requirements in

    micro-total-analysis systems. We explored the distribution of

    metallic silver nanoparticles, 45 4 nm in size, upon chemi-

    cal reaction with H2O2 in the present microchannel; shown

    in theFig. 6. We introduced dilute H2O2(0.9 M) as the carrier

    fluid which reacts with the AgNPs at the interfaces to form

    silver microstructures along the interfacial planes. Being an

    oxidizing agent, H2O2oxidizes the AgNPs to silver ions, at an

    alkaline pH (pH ~ 8.5) of the medium, that are spontaneously

    precipitated as micron-size structures at the interfaces. The

    interaction performance of the AgNPs and H2O2in the micro-

    channel, as shown inFig. 6, was recorded under an inverted

    microscope for 30 min. We determined this 30 min reaction

    time by monitoring the amount of reaction precipitate at dif-

    ferent time intervals (Fig. S4). At the beginning, there was

    no precipitate at the interfaces, indicating the absence of the

    reaction products from the interaction between the AgNPs

    and H2O2. However, as the flow of the fluids continued, the

    AgNPs started focusing at the interfaces and the formation of

    Fig. 4 Hydrodynamic focusing of fluorescent nanoparticles (30 nm) in

    the convergingdiverging microchannel. (ad) Microscopic

    fluorescence images at 470 nm wavelength at different flow ratios of

    the nanoparticle solution and DI water (25: 25, 25 : 50, 25: 100 and 25 : 250

    respectively). (eh) Plots of the fluorescence intensity versusdistance along

    the width of the channel showing particle distribution at the interfaces.

    Note, that the maximum concentrations of the nanoparticles are observed

    at two interfacial zones with a separation width of 100 m at the flow ratio

    of 25:50.

    Fig. 5 Hydrodynamic focusing of fluorescent nanoparticles (500 nm)

    in a convergingdiverging microchannel. (a) Fluorescent nanoparticles

    are systematically focused at both of the interfaces while flowing

    through the channel at a flow rate ratio of nanoparticles: DI of 25 : 50.

    (b) The particle distribution in terms of the fluorescence intensity

    versusdistance along the width of the channel.

    Fig. 6 Superimposed microscope image demonstrating the interaction

    of the AgNPs and H2O2 throughout the patterned micro-channel. A

    gray coloured precipitate can be seen at the interfaces indicating the

    in situformation of silver microstructures as a product of the reaction.

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    Lab Chip, 2014, 00, 19 | 5This journal is The Royal Society of Chemistry 2014

    the products in the presence of co-flowing H2O2was seen at

    10 min and gradually increased to a visible level at 30 min.

    From the outset, we stated that the microscale dimension

    of the channel can allow controlled deposition over the

    bottom surface of the channel. Fig. 7shows the precipitation

    of the silver ions over the channel surface, after reaction; this

    was confirmed by introducing aqueous NH3 to the channel

    after the reaction (Fig. S5). Aqueous NH3 dissolves the

    precipitate by forming a soluble diaminesilver complex([Ag(NH3)2]

    +) and confirms the existence of the Ag+ ions.30,31

    The gray coloured silver ion precipitate remains at the inter-

    facial planes; this can be attributed to the strong absorption

    of the silver ions onto the PDMS and glass substrate. Upon

    producing silver ions, the oxygen atoms of both of the

    substrates are bound with Ag+ ions in such way that the

    surface-bound Ag+ ions can subsequently function as seeds

    for the growth of silver microstructures on glass and PDMS

    substrates.

    In order to investigate the growth mechanism of the silver

    ion precipitate at the interfaces, we used SEM and EDS to

    observe the material at different flow rates.Fig. 7(ad)showsthe SEM images of the silver ion precipitate formed at the

    interface due to the interaction between the AgNP and H 2O2solutions at different flow rates after 30 min. The precipitate

    appears as three-dimensional (3-D) agglomerates or irregu-

    larly shaped micron-size structures. At a higher magnifica-

    tion, the topography of these structures was revealed to be

    formed by flower-like silver ion precipitates arranged at the

    micrometre scale (Fig. 8a). The EDS spectrum shows the pres-

    ence of elemental Ag in the precipitate (Fig. 8b). The peaks of

    the Si and O elements are due to the Si substrate.

    The reaction of AgNPs with H2O2 was performed by

    varying the flow rates of the carrier fluid (QH2O2 = 25, 50, 100

    and 250 L min1) while keeping the nanoparticle solution

    flow rate, QAgNPs, constant at 25 L min1. The applied

    flow rates and corresponding Reynolds numbers (Re) are

    shown inTable 1. At low ReAgNP(3.72), the precipitate started forming after

    5 min, but the amount was less at the interface compared to

    all lower ReAgNP (1.15, 1.88 and 2.35). This indicates thatReAgNP in between 1.152.35 is the optimum for the nano-

    particles to be distributed in a controlled manner at the

    interfaces and to increase the contact area for accelerating

    the interaction process with H2O2 in a controlled manner

    throughout the channel, as further confirmed by the SEM

    and EDS studies (Fig. 7(ac)and8).

    From the experimental results we can see that the con-

    vergingdiverging microchannel is capable of splitting and

    subsequently focusing a stream of nanoparticles. Further

    cross examination reveals that it is the very geometry of the

    channel that makes this splitting possible. Therefore, it is

    now imperative to analyze the inherent physics leading

    towards these characteristic features. We discuss this issue in

    the perspective of our numerical simulation studies.

    Discussions

    In order to unveil the underlying physics leading to particle

    focusing, we conducted 3D numerical simulations for a

    convergingdiverging channel with the same dimensions as

    those used in the experiments (see the ESI for details).

    Essentially, the velocity field, assuming incompressible flow,

    is divergence free and is obtained by solving the Navier

    Stokes equation. Subsequently, the particle distributions were

    obtained from Lagrangian tracking. Owing to the periodicrepetition of the channel geometry, we conducted a simula-

    tion over a domain which was periodic along the direction of

    the mean flow. Then the imposed flow rate was maintained

    Fig. 7 Scanning electron microscopy images of the Ag ion precipitate

    formed at the interfaces due to the interaction between the AgNP and

    H2O2solutions at different flow rates of the carrier phase at (a) 25 L min1,

    (b) 50L min1, (c) 100 L min1 and (d) 250 L min1 for 30 min. The AgNP

    solution flow rate was kept constant at 25 L min1. The insets show

    the magnified images of the silver ion precipitate.

    Fig. 8 (a) Magnified SEM image of the silver ion precipitates which

    appear as flower-like structures. (b) The EDS spectrum of Ag ion

    precipitates showing the presence of Ag. The peaks of the Si and Oelements are due to the Si substrate.

    Table 1 Flow ratio and corresponding Reynolds number of the AgNP

    and H2O2solutions

    Flow ratio Q= 25:25 Q= 25:50 Q= 25: 100 Q= 25: 250

    ReH2O2 0.58 1.16 2.32 5.79ReAgNP 1.15 1.88 2.35 3.72

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    6 | Lab Chip, 2014,00, 19 This journal is The Royal Society of Chemistry 2014

    as the sum of the flow rates of the carrier and the dispersed

    phases. InFig. 9, we show the 3D simulation results of the

    distributions of the 45 nm particles, with 10 500 kg m3

    density (resembling the density of silver), at a flow rate of

    25 L min1 for both the carrier and the dispersed phases.

    The figure shows that the observation from the present simu-

    lation is in close agreement with the experimental results

    (compared withFig. 7a).

    Initially, the particles were distributed in and around thecentral axis of the channel. In response to the flow field, the

    distribution of the particles was then obtained by solving the

    kinetics equation for each particle

    d

    dand

    d

    d

    p

    D g M S

    p

    p

    uf f f f

    xu

    t t (1)

    where xp and up represent, respectively, the position and

    velocity of the particle (in vector form), measured with

    respect to a fixed-to-the-lab Cartesian reference frame, as

    indicated inFig. 9. The forces (per unit mass of the particle),

    as shown in eqn (1), are the hydrodynamic drag force ( fD),

    force due to gravity (fg), virtual mass force (fM) and the

    Saffman lift force (fS). They are estimated as3235

    f u u

    f g

    f u u

    D

    p p

    D p

    p

    g

    p

    M

    p

    p

    Re

    d

    d

    18

    24

    1

    1

    2

    2

    d

    C

    t

    ,

    ,

    ,

    .

    :

    .

    and

    S

    p p

    pf D

    D D

    u u5 1881 2

    1 4

    d

    (2)

    Here g denotes the acceleration due to gravity (acting

    along the z direction),CDbeing the drag coefficient, and ,

    and are the density, dynamic viscosity and kinematic

    viscosity of the carrier phase (aqueous medium). Accordingly,

    pand dpdenote the density and the diameter of the particle.

    In eqn (2), the velocity vectors for the carrier phase and the

    particle are denoted byu and up. Accordingly, the strain rate

    tensor is defined as D = u+ (u)T. Note that here the parti-

    cle based Reynolds number is defined as Re p = dp|u u p|/.It is worth mentioning that for the simulation purpose, we

    considered the contributions from all of the mentioned

    forces.

    During the tracking of particles, we considered the particle

    particle and particlewall interactions to be elastic type. To the

    present level of approximation, we did not take into account

    the implication of any electrostatic interaction between the par-

    ticles. In fact, any implication due to its accounting can be con-

    sidered to be significant where the length scale over which the

    characteristic changes in the particle distribution can be

    observed, approaches the nanoscale regime.36 Pertaining to the

    present situation, the characteristic dimension of the zone ofthe particles'divergence is well above this limit. However, in

    our model we consider the two way coupling between the parti-

    cles and the continuous phase. Specifically, that the gain (loss)

    in momentum of a particle is accommodated as the loss (gain)

    in momentum of the continuous phase.

    It is now prudent to estimate the contribution of each of

    the contributing forces in deciding the particle distribution

    observed in mutually agreeing simulations and experiments.

    First we note that studies have shown the influence of the

    Saffman lift force on nanoparticle distribution.25,26,36,37

    However, their magnitudes are generally very small (~1014 N

    to 1016 N, as estimated for the present experiments) and

    there seems to be only a marginal change in the distribution

    of the particles due to the accounting of this force. However,

    for the sake of verification, we also conducted simulations

    with and without the Saffman lift consideration in the model;

    the comparison is shown inFig. 10. From the figure, it is evi-

    dent that the Saffman lift force does not induce any consider-

    able change in particle distribution, at least for the present

    setup. Subsequently, by comparing the order of magnitude

    Fig. 9 3D simulation results of the distributions of 45 nm particles in a

    converging diverging channel at a flow rate of 25 L min1, for both

    the carrier and the dispersed phases. The flow was imposed along the

    xdirection and the particles were initially distributed axially around the

    central axis of the channel.

    Fig. 10 Splitting of the nanoparticle stream withdp = 45 nm and p=

    10500 kg m3, with and without considering the Saffman lift force in

    the convergingdiverging channel at a flow rate of 25 L min1, for

    both the carrier and the dispersed phases.

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    Lab Chip, 2014, 00, 19 | 7This journal is The Royal Society of Chemistry 2014

    contributions of the other forces, we found that fg and fScould be neglected as compared to fD. Thus, it seems that the

    particles are basically dragged along the flow field. Addition-

    ally from our simulation we found thatu ~ u p. Thus, we can

    consider that the particles move in the flow field as passive

    tracer particles. Therefore, it is the inherent feature of the

    intrinsic flow field that determines the distribution of the

    particles. The dimension and the subsequent mass of each of

    the nanoparticles are indicative of the fact that the particlescan be considered as passive tracer particles that are likely to

    follow the streamlines closely at the steady state.13,38

    In search of the intrinsic flow features for the present

    setup, inFig. 11awe present the distribution of the stream-

    lines, on an xyplane passing through the central axis. From

    the figure it is evident that the streamlines are compressed

    and expanded in the converging and diverging sections,

    respectively. The distribution of particles, therefore, follows a

    similar pattern. For further verification, we performed simu-

    lations in a straight channel with similar dimensions as

    those used in the experiment; the particle distribution and

    the streamlines are shown inFig. 11b. The simulations werealso conducted with p = 10 500 kg m

    3 and dp = 45 nm and

    all the above mentioned forces were retained for Lagrangian

    tracking of the particles. FromFig. 11bit is evident that the

    particles with the given size closely follow the streamlines at

    the given flow rate. Therefore, by comparingFig. 11a and b

    we can proclaim that the typical splitting of the nanoparticle

    stream is a characteristic of the convergingdiverging

    channel geometry as considered in our work.

    It is worth mentioning at this point that studies have

    shown that even for flows with low Reynolds number,

    secondary flows may exists specifically near the zones of

    spatially varying curvatures of the channel geometry, and can

    lead to some interesting features.3942 It is to be noted that

    the cross section of the present device is also spatially vary-

    ing. It is, therefore, imperative to unveil the possibility of the

    influence of any such flow features. For this purpose, we

    conducted simulations with different flow rates (Q). The flow

    rate as maintained for presenting the results in Fig. 9, is con-

    sidered as the base flow rate (Qbase). Starting from Q/Qbase =

    1, we carried out simulations up to Q/Qbase = 10; note that

    this consideration is in tune with the present experimental

    setup. As per our choice of reference frame, the central axis

    was defined by the locus y = 0 and z = h/2, as shown in

    Fig. 12a. In all the simulations, we then monitored the veloci-

    ties at offsets y = (keepingz= h/2) as indicated inFig. 12a.In the left column ofFig. 12bwe demonstrate the flow veloci-

    tiesux, uyand uz, along the x,y and zdirections respectively,

    as obtained from the data monitored at = 5 102 mm at

    different x/Lref; here Lref was chosen as the width of the

    expansion section. It needs to be emphasized that we

    Fig. 11 (a) Distribution of the streamlines on an xyplane passing

    through the central axis, for (a) the convergingdiverging channel and

    (b) a straight channel. In both cases, the flow rates of both the carrier

    and the dispersed phases were maintained at 25 L min1.

    Fig. 12 (a) The description of the central axis and the offset. (b) The

    variation of ux, uyand uz, (left column), measured along the x, yand z

    directions respectively, and the corresponding ux/Uref, uy/Uref and

    uz/Uref (right column), with x/Lrefas obtained from the data monitored

    at = 5 102 mm.

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    8 | Lab Chip, 2014,00, 19 This journal is The Royal Society of Chemistry 2014

    specifically focused our attention over the region around the

    central axis where the particles are distributed. Specifically,

    we endeavoured to scrutinize the hydrodynamic features

    (namely the flow velocities) over this region so as to unveil

    the essential physics of interest. Thus, we considered the

    location at the mentioned offset around the central axis. The

    gross flow feature at different zones within the channel is

    already shown in Fig. 11a, through the distribution of the

    streamlines. For distributions ofuxand uy, here we only showvariations over a characteristic extent ofx/Lref. The distribu-

    tion over the entire extent ofx/Lrefis just the periodic repeti-

    tion of those characteristic features. From the distributions

    ofux in Fig. 12b, it is noteworthy thatux attains maxima at

    the contraction zone. This is in tune with the continuity of

    the flow rates across different cross sections. From the distri-

    butions ofuzin Fig. 12b, one can appreciate that at the con-

    traction zone, it assumes magnitudes that are close to zero.

    However,Q8 near the contraction zone, peaks of uy can be

    observed at just upstream and downstream sides. Signifi-

    cance of those optima were delineatedQ9 post priory. Neverthe-

    less, if we observe the variation ofux/Uref, uy/Urefand uz/Uref,whereUref= Q/A(A is the cross-section area of the expansion

    section), the corresponding curves collapse on each other, as

    shown in the right column ofFig. 12b. The collapse indicates

    that ux, uy and uzchange proportionally with the imposed

    flow rate. From this collapsing, we can also infer an impor-

    tant fact: with the choice of a normalization scheme (using

    the chosenLrefandUref) it is possible to provide a generalized

    depiction of the inherent hydrodynamics, so long as the

    Reynolds number is kept low.

    Among the ux/Uref, uy/Uref and uz/Uref distributions, as

    shown in Fig. 12b, we found that ux/Uref and uy/Uref play

    dominant roles in determining the inherent dynamics of the

    present device, as can be appreciated from the negligible

    order of magnitude ofuz/Uref, in comparison to that ofux/Urefand uy/Uref.Q10 It is worth mentioning that the distribution of

    both uz (Fig. 12b left column) and uz/Uref (Fig. 12b right

    column) appear as noises. However, the ranges of the abso-

    lute values within which their variations occur implicate that

    the apparent fluctuations in uzand uz/Urefare not likely to

    make any significant contribution in comparison to the veloc-

    ity components along the other directions. Here the varia-

    tions of uz and uz/Urefare presented to highlight the issue

    that uz ux and uz uy. Thus, the essential physics is

    primarily decided byux and uy (subsequently byux/Urefand

    uy/Urefrespectively).InFig. 13we have compared the distributions ofux/Uref

    anduy/Ureffor = 5 102 mm. From the figure it is evident

    that in both cases, ux/Uref remains same. However, from

    the distribution ofuy/Urefone can appreciate that at a given

    x/Lref, the uy/Urefdistributions are the same in magnitude but

    with a different sign. When the particles are approaching

    the contraction zone, they experience symmetrically opposite

    uy/Uref that endorses the squeezing of the distribution zone

    of the particles. Subsequently, after coming out of the con-

    traction zone, the uy/Urefdistribution aides the expansion of

    the distribution zone. The symmetrically opposite features

    explain the symmetric distribution of the particles around

    the central axis. With the above mentioned considerations

    and the contrasting observations concerning the particle dis-tributions in straight channels and convergingdiverging

    channels, we infer that the present splitting behaviour of

    particles, in the present setup, is primarily due to the inher-

    ent flow field, as realized from the geometrical features of

    the confining domain. The very geometry of the channel

    endorses periodic divergence and expansion of the stream-

    lines, thereby causing the nanoparticles to trail along.

    This type of distribution of nano-sized particles can be

    beneficial to fabricate various microstructures inside the con-

    fined channels for numerous applications. In the present

    study, for example, the focused silver nanoparticles formed a

    precipitate after reacting with H2O2 at the interfaces thus

    containing highly active Ag+ ions and can directly be involved

    in specific chemical or biological reactions for catalytic

    purposes.43 In the reported literature, silver is deposited at

    the interfaces of microfluidic channels to encounter many

    practical settings.28,44 However, their fabrication processes

    follow expensive and multi-step methods including multi-

    stage photolithography, etching, accurate alignment and so

    on. Moreover, there is little information known about the

    morphological features of the precipitate formed inside

    microchannels. In the present study, we have utilized a pro-

    cess for the controlled synthesis of silver microstructures

    throughout its interfacial length in a wavy fashion which will

    provide a large surface area as compared to the straightmicrochannel. The micro-structured silver ion precipitate

    may have potential use in microelectronics and catalysis and

    we may utiliz e this precipitate as microcatalysts for various

    catalytic reactions in microchannels.29

    Conclusions

    Our observations reveal that in a convergingdiverging micro-

    channel, with a smoothly varying cross-section, a stream of

    nanoparticles can be split into two halves, and can be made

    Fig. 13 The distributions of ux/Uref and uy/Uref at = 5 102 mm to

    show the particle distribution at the near contraction and near

    expansion zones.

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    Lab Chip 2014 00 19 | 9This journal is The Royal Society of Chemistry 2014

    to remain focused over a particular region, specifically over

    the interfacial region of the dispersed and carrier phases.

    Moving a step ahead, one can conduct a controlled reaction,

    and thereby separate the reaction-product over the targeted

    location, using the present setup. Moreover the reaction

    product is found to be deposited over the bottom surface of

    the channel along a track parallel to the interfacial region of

    the two fluids. The splitting and subsequent focusing ability

    of the present setup primarily stems from the geometryassisted convergence and divergence of the streamlines, and

    thereby induces the dispersed particles to trail along. The

    controlled deposition, on the other hand, endorses a simple

    strategy for bottom-up fabrication of microscale features.

    Acknowledgements

    The authors are thankful to the CSIR-CMERI, India, for the

    financial support through the projects OLP-190312 and OLP-

    101512. The authors also acknowledge the help of the insti-

    tute CRF facility for conducting SEM studies.

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