1. Introduction
The phenomenon of Marangoni convection has been extensively studied in the past few decades, due to its importance in microgravity engineering and microfluidics (for reviews, see Simanovskii & Nepomnyashchy Reference Simanovskii and Nepomnyashchy1993; Nepomnyashchy, Simanovskii & Legros Reference Nepomnyashchy, Simanovskii and Legros2012). The early works on the development of Marangoni convection in a liquid layer heated from below have revealed two basic modes of Marangoni instabilities: (i) the Pearson mode (Pearson Reference Pearson1958) of cellular convection with a negligible deformation of the interface and (ii) the Scriven–Sternling mode (Scriven & Sternling Reference Scriven and Sternling1964) which manifests itself through a longwave interface deformation leading to layer rupture. The former instability mechanism prevails in relatively thick layers, while the latter one is observed only in very thin layers (Van Hook et al. Reference Van Hook, Schatz, McCormick, Swift and Swinney1995,Reference Van Hook, Schatz, Swift, McCormick and Swinney1997) or under microgravity conditions. The separation of ‘non-deformational’ and ‘deformational’ types of instabilities is essential also in the case of a thermocapillary flow generated by a temperature gradient applied along the layer. The non-deformational type of instabilities creates hydrothermal waves (Smith & Davis, Reference Smith and Davis1983a ; Madruga, Perez-Garcia & Lebon Reference Madruga, Perez-Garcia and Lebon2003), while the deformational type is responsible for the development of long surface waves (Smith & Davis, Reference Smith and Davis1983b ).
When the imposed gradient is inclined with respect to the interface, the Marangoni instability is developed on the background of a parallel thermocapillary flow generated by the horizontal component of the temperature gradient. The analysis of that problem in the case of a non-deformable interface has been carried out by Davis (Reference Davis1987) and Shklyaev & Nepomnyashchy (Reference Shklyaev and Nepomnyashchy2004) for a single layer, and by Nepomnyashchy, Simanovskii & Braverman (Reference Nepomnyashchy, Simanovskii and Braverman2001) for a two-layer system. A competition between three modes of instability, stationary longitudinal rolls, oblique hydrothermal waves and transverse travelling rolls, has been investigated. The problem has also been studied experimentally by Ueno, Kurosawa & Kawamura (Reference Ueno, Kurosawa and Kawamura2002).
The investigation of the longwave deformational Marangoni instability in ultrathin two-layer films under the action of an inclined temperature gradient has been started by Nepomnyashchy & Simanovskii (Reference Nepomnyashchy and Simanovskii2009a,Reference Nepomnyashchy and Simanovskiib, Reference Nepomnyashchy and Simanovskii2010). Though the basic instability in ultrathin films is due to vanderWaals forces, the influence of the thermocapillary flow created by the inclined temperature gradient is significant.
Similar kinds of instabilities are observed also in droplets on a liquid substrate (‘liquid lenses’). In some experiments, oscillatory convective flows generated by the thermocapillary effect and buoyancy have been observed (Rybalko et al. Reference Rybalko, Magome and Yoshikawa2004; Yakshi-Tafti et al. Reference Yakshi-Tafti, Cho and Kumar2010; Song et al. Reference Song, Moon, Lee, Kim and Pak2014; Buffone Reference Buffone2019). Note that the boundary-value problem that describes the dynamics of liquid lenses is quite similar to that governing the dynamics of two-layer films, except for accounting for the disjoining pressure solely in the region of the precursor film.Droplets on a liquid substrate play an important role in various branches of engineering, including microfluidics (Labanieh et al. Reference Labanieh, Nguyen, Zhao and Kang2015), chemical engineering (Yamini et al. Reference Yamini, Rezazadeh and Seidi2019), environment protection (Ju et al. Reference Ju, Yang, Li, Cheng and Shi2019), etc. Nevertheless, their dynamics has still attracted less attention. The dynamics and instabilities of non-isothermal floating droplets are of special interest. Recently, Nepomnyashchy & Simanovskii (Reference Nepomnyashchy and Simanovskii2021) studied the influence of homogeneous heating or cooling of the liquid substrate on the stability of a thin floating droplet under microgravity conditions. A number of instability modes leading to droplet oscillations, droplet decomposition or substrate layer rupture were revealed. The observed instabilities of droplets are reminiscent of longwave deformational instabilities in two-layer films (Nepomnyashchy & Simanovskii Reference Nepomnyashchy and Simanovskii2007).
The present paper is devoted to the investigation of the dynamics and instabilities of droplets on a liquid substrate under the action of an inclined temperature gradient. In the latter case, some qualitatively new phenomena are expected due to the action of the thermocapillary flow in the liquid substrate on the droplet dynamics, as well as the influence of the flows in the substrate and in the droplet on the development of the Marangoni instability. The droplet dynamics is studied in a wide range of transverse and longitudinal Marangoni numbers. To the best of our knowledge, the dynamics and instabilities of floating droplets under the action of an inclined temperature gradient have not been studied before.
The structure of the paper is as follows. The mathematical model is formulated in § 2. Section 3 contains the description of nonlinear regimes. A multistability of regimes has been found. The influence of an inclined temperature gradient on the shape of droplets in the presence of gravity is studied in § 4. Section 5 contains some concluding remarks.
2. Formulation of the problem
We consider a droplet of liquid 2 that floats on a layer of liquid 1, and it is in contact with gas phase 3 (see figure 1). Later on, we do not consider any processes in fluid 3: at the liquid–gas interface, the viscous stresses are neglected and the heat transfer is described using the heat exchange coefficient
$q$
. The
$m$
th fluid has density
$\rho _m$
, dynamic viscosity
$\eta _m$
and thermal conductivity
$\kappa _m$
,
$m=1,2$
.
Geometric configuration of the region and coordinate axes.

The contact angles on the triple line surrounding the droplet are determined by the balance of interfacial tensions
$\sigma _{12}$
,
$\sigma _{23}$
and
$\sigma _{13}$
between the corresponding fluids according to the Neumann triangle construction (Neumann Reference Neumann1894). The droplet exists in two cases: (i) when the spreading coefficient
$S=\sigma _{13}-\sigma _{12}-\sigma _{23}\lt 0$
(partial wetting) and (ii) when
$S\gt 0$
, but only a small part of fluid 2 is spread between fluids 1 and 3 forming an ultrathin film (pseudo-partial wetting) due to the attractive interaction of those fluids through the film of fluid 2 (positive Hamaker constant A).
The temperature of the solid substrate is
$T_s+{\tilde A}x$
and the temperature of the gas near the interface is
$T_g+{\tilde A}x$
. Thus, it is assumed that the same constant temperature gradient is imposed in the direction of the axis
$x$
in the solid substrate and in the gas phase. Assuming that the temperature differences in the system are not too large, we disregard the dependence of liquid parameters on the temperature, with one exception: because we are interested in the investigation of the thermocapillary convection, we take into account the thermocapillary stresses proportional to derivatives of the interfacial tensions with respect to the temperature. The interfacial tension coefficients on the lower and upper surfaces of the droplet,
$\sigma _1\equiv \sigma _{12}$
and
$\sigma _2\equiv \sigma _{23}$
, are assumed to be linear functions of temperature
$T$
:
$\sigma _1=\sigma _1^0-\alpha _1 T$
,
$\sigma _2=\sigma _2^0-\alpha _2 T$
, where
$\alpha _1$
and
$\alpha _2$
are constants. It is assumed that
$|\alpha _1T|\ll \sigma _1$
and
$|\alpha _2T|\ll \sigma _2$
; therefore we disregard that dependence in the relations that contain the interfacial tensions as a whole, i.e. in the stress balances on the triple line and in the expressions for Laplace pressures.
The description of the temporal evolution of the triple line surrounding the droplet is technically difficult (see Kriegsmann & Miksis Reference Kriegsmann and Miksis2003). In Craster & Matar (Reference Craster and Matar2006), the precursor model was suggested for the description of a floating droplet: the interface between fluids 1 and 3 outside the droplet is replaced by an ultrathin precursor layer of fluid 2 (see figure 1). The latter model describes the droplet on the liquid substrate as a two-layer film. The same equations are used in the whole region, but outside the droplet, where the top layer is ultrathin, the corresponding disjoining pressure is taken into account. Let us emphasize that the latter approach can be applied in the case of both pseudo-partial wetting and partial wetting, because macroscopically both cases are identical. In the present paper, we apply that approach for the description of the dynamics of a non-isothermal floating droplet.
The deformable interfaces are described by equations
$z=H_1(x,y,t)$
and
$z=H_2(x,y,t)$
. Far from the droplet, the equilibrium thickness of layer 1 is
$H_1^0$
, and the thickness of the precursor film is
$H_{\infty }$
(see figure 1). The gravitational acceleration is
$g$
.
Later on, we consider a slender droplet, i.e. the slopes of both the droplet’s interfaces are small. Also, we assume that the characteristic horizontal scale of the interface deformations is large as compared with the characteristic vertical size of the droplet and the substrate. Those assumptions allow applying the mathematical model governing the longwave dynamics of non-isothermal liquid layers that has been derived using the lubrication approximation by Pototsky et al. (Reference Pototsky, Oron and Bestehorn2005) (see also Nepomnyashchy & Simanovskii Reference Nepomnyashchy and Simanovskii2007). In the framework of the longwave approach, the shapes of the interfaces
$z=H_1$
and
$z=H_2$
depend on the scaled horizontal coordinates
$X=\epsilon x$
and
$Y=\epsilon y$
,
$\epsilon \ll 1$
, rather than on
$x$
and
$y$
. Also, it is assumed that they depend on the scaled time variable
$\tau =\epsilon ^2 t$
. A comprehensive description of the longwave approach can be found in the review paper by Oron et al. (Reference Oron, Davis and Bankoff1997).
The problem is presented in non-dimensional form using the equilibrium thickness of the lower layer,
$H_1^0$
, as the vertical length scale. The choice of the horizontal scale
$L^*$
is arbitrary (Nepomnyashchy & Simanovskii Reference Nepomnyashchy and Simanovskii2012). We choose
as a time scale and
as a pressure scale.
The non-dimensional system of equations looks as follows (lower-case letters correspond to non-dimensional quantities):
The expressions for pressures,
include the contributions of the Laplacian pressures, hydrostatic pressures and disjoining pressures:
Note that the choice of scale is different from that used in Nepomnyashchy & Simanovskii (Reference Nepomnyashchy and Simanovskii2012), because here we consider the Marangoni instability rather than the vanderWaals instability. The derivation of the longwave evolution equations is given in Appendix A.
The non-dimensional parameters of the problem are as follows:
\begin{equation} M_{\bot }=\frac {\alpha _1(T_s-T_g)}{\sigma _1^0}\left (\frac {L^*}{H_1^0}\right )^2, \end{equation}
\begin{equation} M_{\|}=\frac {\alpha _1AL^*}{\sigma _1^0}\left (\frac {L^*}{H_1^0}\right )^2 \end{equation}
are the modified transverse and longitudinal Marangoni numbers, correspondingly,
is the Biot number,
$\eta =\eta _1/\eta _2$
,
$\kappa =\kappa _1/\kappa _2$
,
$\sigma =\sigma _2^0/\sigma _1^0$
,
$\alpha =\alpha _2/\alpha _1$
,
$\rho =\rho _2/\rho _1$
and
is the Bond number.
One can see that each flow rate,
$\textbf { q}_1^T$
and
$\textbf {q}_2^T$
, contains two contributions, one proportional to
$M_{\|}$
and another to
$M_{\bot }$
. The former contribution, which is caused by the imposed horizontal temperature gradient, is always directed opposite to vector
$\textbf { e}_x$
, i.e. towards the region with lower temperature and hence higher interfacial tensions. Note that the contribution of the horizontal temperature gradient to
$\nabla \cdot \textbf { q}_1$
can be written as
$u_1h_{1x}$
, where
(The subscript means the derivative, and the way of non-dimensionalization is described above.) Thus, each point of the droplet’s bottom surface moves to the left with velocity (2.17). The term with
$M_{\|}$
in the expression for
$\nabla \cdot \textbf { q}_2$
is
$u_2h_{2x}+w_2$
, where
Thus, in addition to the motion to the left with velocity (2.18), a point on the top surface of the droplet moves upward or downward with velocity (2.19).
A snapshot of the fields of (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-0.25$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
,
$\tau =1\times 10^6$
. The horizontal axis is
$X$
and the vertical axis is
$Y$
.

The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-0.25$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
,
$\tau =1\times 10^6$
.

The second contribution proportional to
$M_{\bot }$
is generated by non-uniformities of the interfacial temperature field, which are caused by the deformations of interfaces.
Because the thickness of liquid layer 1 is always macroscopic, we can neglect the contribution of
$\pi _1$
. In layer 2, we apply the following expression for the disjoining pressure:
\begin{equation} \pi _2=\frac {a}{(h_2-h_1)^3} \left [1-\left (\frac {h_{\infty }}{h_2-h_1}\right )^3\right ], \end{equation}
where
$a$
is the non-dimensional Hamaker constant, which is related to the dimensional Hamaker constant
$A$
as
and
$h_{\infty }=H_{\infty }/H_1^0$
(for details, see Craster & Matar Reference Craster and Matar2006; Pototsky et al. Reference Pototsky, Oron and Bestehorn2019).
Note that in the absence of gravity, a liquid layer with a deformable interface is subject to a monotonic Marangoni instability for arbitrary
$M_{\bot }\gt 0$
, i.e. by any heating from below (Sternling & Scriven Reference Scriven and Sternling1964). That instability is not saturable, and it leads to the rupture of the substrate layer. The temperature disturbance caused by the droplet acts as a ‘seed’ of instability. Therefore, in the presence of the temperature gradient, one can expect the existence of a stable configuration containing a droplet on a layer flat on the infinity only if
$M_{\bot }\lt 0$
, i.e. by cooling from below.
The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-0.5$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
,
$\tau =4.12\times 10^5$
.

3. Nonlinear simulations
3.1. Methodology
The problem governed by equations (2.3)–(2.20) was solved numerically with some initial conditions. The evolution equations were discretized by central differences for spatial derivatives and solved using an explicit scheme. Periodic boundary conditions have been applied on the boundaries of the computational region
$L \times L$
.
Recall that we assume that the characteristic horizontal scale of the surface deformations is significantly larger than the thickness of the droplet and that of the substrate layer typically chosen as the length scale. The distance between the grid nodes can be chosen rather large. The computations have been performed in the region
$L \times L= 240\times 240$
using an
$80\times 80$
grid. Some trial simulations on
$100\times 100$
and
$120\times 120$
grids did not reveal any qualitative changes. The time step typically was changed between 0.00125 and 0.005, which is significantly below the linear scheme stability boundary. No quantitative changes have been observed for simulations made with different time steps.
We used two kinds of initial conditions. First, we applied the initial conditions
i.e. a droplet of liquid 2 with a Gaussian shape was imposed on a flat layer of liquid 1, where
$h_{-}$
,
$h_{+}$
, corresponding to the initial shape of the droplet, are constants and
$R$
is the radius of the droplet. In some other simulations, we used a solution formerly obtained for another set of parameters as the initial condition.
In the present paper, we perform computations for the system of fluorinert FC70 (liquid 1) and silicone oil 10 (liquid 2). This system of liquids was used in microgravity experiments (see e.g. Géoris et al. Reference Géoris, Hennenberg, Lebon and Legros1999). We applied the following set of liquid parameters that was formerly used in simulations of Marangoni instability in two-layer systems (Nepomnyashchy & Simanovskii Reference Nepomnyashchy and Simanovskii2012):
$\eta =3.04$
,
$\kappa =0.522$
,
$\alpha =2$
,
$\rho =0.482$
,
$\sigma =2.6$
,
$h_-=1.02$
,
$h_+=1$
,
$R=60$
,
$h_{\infty }=0.01$
and
$Bi=20$
. The value of
$a$
is chosen equal to
$0.31\times 10^{-6}$
(see Nepomnyashchy & Simanovskii Reference Nepomnyashchy and Simanovskii2021).
The primary analysis of the obtained nonlinear regimes has been performed using snapshots of the fields of
$h_j(X,Y,\tau ),$
$j=1,2.$
The analysis has been supplemented by the investigation of the time dependence for the maximum values of the variables
$h_j$
:
The oscillations of
$h_{max,2}(\tau )$
(solid line) and
$h_{max,1}(\tau )$
(dashed line) for
$M_{\bot }=-1.07$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
.

A snapshot of the fields of
$h_2(X,Y,\tau )$
for
$\bar {M}=-1.07$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
: (a)
$\tau =3\times 10^5$
; (b)
$\tau =3.6\times 10^5$
.

The oscillations of
$h_{max,2}(\tau )$
(solid line) and
$h_{max,1}(\tau )$
(dashed line) for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
.

The fields of
$h_2(X,Y,\tau )$
for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
: (a)
$\tau =912\,500$
;(b)
$\tau =925\,000$
;(c)
$\tau =937\,000$
; (d)
$\tau =942\,500$
; (e)
$\tau =948\,000$
;(f)
$\tau =962\,000$
.

The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
,
$\tau =912\,500$
.

3.2. Nonlinear regimes
3.2.1. Travelling droplets
Let us describe now the results of nonlinear simulations. The simplest structure observed for sufficiently small values of
$M_{\|}$
and
$|M_{\bot }|$
is the droplet, moving from the right-hand side to the left-hand side as a whole:
The snapshot of the fields of
$h_2(X,Y,\tau )$
and
$h_1(X,Y,\tau )$
is shown in figure 2. For all the figures showing the droplet, the horizontal axis is
$X$
and the vertical axis is
$Y$
. The shapes of interfaces are presented in figure 3. This type of motion has also been found for larger values of
$M_{\bot }$
(at
$M_{\bot }=-0.5$
). As in the previous case, the droplet moves from the right-hand side to the left-hand side. The shapes of interfaces are shown in figure 4. Let us emphasize that while in the case of an isothermal droplet the lower interface of the droplet is below the substrate level, in the case of the non-isothermal droplet and sufficiently large value of the Biot number, the lower interface of the droplet is mainly above the substrate. The change of the droplet’s shape is caused by the Marangoni effect.
3.2.2. Excitation of oscillations
Let us consider the evolution of the regimes at
$M_{\|}=0.0001$
for sufficiently large values of
$|M_{\bot }|$
. At
$M_{\bot }=-1.07$
, we observed periodic oscillations. The temporal evolution of
$h_{max,2}$
and
$h_{max,1}$
is shown in figure 5. The period of oscillations
$T=146\,700$
.The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are shown in figure 6. The droplet moves from right to left, changing its shape.
At
$M_{\bot }=-2$
(
$M_{\|}=0.0001$
), we get periodic oscillations of the droplet of a rather complex form. The temporal evolution of
$h_{max,2}$
and
$h_{max,1}$
is shown in figure 7. The period of oscillations
$T=75\,500$
. One can see that with an increase of
$M_{\bot }$
, the period of oscillations decreases (cf. Figures 5 and 7). The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are shown in figure 8 . The droplet moves from the right-hand side to the left-hand side, changing its shape during an oscillatory process. The shapes of interfaces at
$\tau =912\,500$
are shown in figure 9 (see also figure 8
a).
Let us emphasize that for the same values of
$M_{\|}$
and
$M_{\bot }$
, different spatial structures can be obtained, depending on the initial conditions.
With a further increase of
$|M_{\bot }|$
(
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
), the system makes a transition to another stable mode through quasi-periodic oscillations. The temporal evolution of
$h_{max,1}$
and
$h_{max,2}$
is shown in figure 10. The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are shown in figure 11. One can see that the system of droplets moves from right to left, changing shape during an oscillatory process. The shapes of interfaces at
$\tau =310\,000$
are shown in figure 12 (see also figure 11
e).
The oscillations of
$h_{max,2}(\tau )$
(solid line) and
$h_{max,1}(\tau )$
(dashed line) for
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
.

The fields of
$h_2(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
: (a)
$\tau =300\,000$
; (b)
$\tau =302\,500$
; (c)
$\tau =305\,000$
; (d)
$\tau =307\,500$
; (e)
$\tau =310\,000$
; (f)
$\tau =312\,700$
.

The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
,
$\tau =310\,000$
.

The thermocapillary flow influences the interaction between droplets. Let us take as the initial conditions the structure consisting of several fragments (see figure 13). This structure was created at
$M_{\bot }=-4$
,
$M_{\|}=0$
as the result of droplet destruction by an intensive Marangoni flow. The motion of droplets under the action of an inclined temperature gradient (
$M_{\bot }=-4$
,
$M_{\|}=0.0001)$
can simplify their coalescence leading to the creation of a film covering the whole computational region. The film instability creates a more or less ordered system of in-phase deformations of interfaces (see figure 14). One can compare figures 14(a) and 11(e) obtained for the same values of parameters from different initial conditions.
A snapshot of the fields of (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0$
,
$Bo=0$
,
$Bi=20$
,
$\tau =1\times 10^6$
.

A snapshot of the fields of (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0$
,
$Bi=20$
,
$\tau =1\times 10^6$
; figure 13 has been taken as initial conditions.

For sufficiently large values of
$|M_{\bot }|$
and
$M_{\|}$
(we take
$M_{\bot } =-4$
and
$M_{\|}=0.0005$
), the nonlinear growth of disturbances with non-commensurable frequencies leads to the appearance of quasi-periodic motion. The temporal evolution of
$h_{max,2}$
and
$h_{max,1}$
is shown in figure 15. The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are shown in figure 16. The pattern moves from the right-hand side to the left-hand side, changing shape during an oscillatory process. The shapes of interfaces at
$\tau =402\,500$
are shown in figure 17 (see also figure 16
b).
The oscillations of
$h_{max,2}(\tau )$
(solid line) and
$h_{max,1}(\tau )$
(dashed line) for
$M_{\bot }=-4$
,
$M_{\|}=0.0005$
,
$Bo=0$
,
$Bi=20$
.

The fields of
$h_2(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0005$
,
$Bo=0$
,
$Bi=20$
: (a)
$\tau =400\,000$
; (b)
$\tau =402\,500$
; (c)
$\tau =405\,000$
; (d)
$\tau =407\,500$
.

The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0005$
,
$Bo=0$
,
$Bi=20$
,
$\tau =402\,500$
.

A snapshot of the fields of
$h_2(X,Y,\tau )$
for
$M_{\bot }=-0.25$
,
$M_{\|}=0.004$
,
$Bo=0$
,
$Bi=20$
: (a)
$\tau =430\,000$
; (b)
$\tau =442\,000$
. The structure has been obtained from asymmetricinitial conditions with respect to axis
$Y=L/2$
. The horizontal axis is
$X$
and the vertical axis is
$Y$
.

Let us take as initial conditions the steady droplet moving from the right-hand side to the left-handside at
$M_{\bot }=-0.25$
and
$M_{\|}=0.0001$
. With an increase of
$M_{\|}$
(at
$M_{\|}=0.004$
), the droplet is split, and we get a pair of pulsating droplets. The height and the shape of the droplets change with a small amplitude and large period (
$\tau =110\,000$
) during an oscillatory process. The snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are shown in figure 18.
3.2.3. Suppression of oscillations
Now, let us fix
$M_{\bot }$
(
$M_{\bot }=-2$
), changing
$M_{\|}$
. For sufficiently large values of
$M_{\|}$
, spreading of the droplet leads to the creation of a film covering the substrate. Periodic oscillations are suppressed. In a certain region of parameters, film instability leads to the formation of ordered structures that consist of equally sized deformations of interfaces moving from the right to the left with equal velocities and located at equal distances from each other. An example of the formation of the ordered structure is shown in figure 19 (
$M_{\bot }=-2$
,
$M_{\|}=0.0002$
,
$\tau =1\times 10^6$
). Note that the locations of the deformations on both interfaces are correlated. Let us emphasize that the system of ordered patterns is not a result of a casual monodispersity of droplets due to a specific choice of initial conditions but a result of a natural evolution of the system to its stable configuration. The diagram of flow regimes in the plane (
$M_{\|}$
,
$M_{\bot }$
) is constructed in figure 20. Let us note that we observed two stable regimes that have been obtained from different initial conditions: (i) oscillations of a droplet, obtained from the oscillatory state, corresponding to
$M_{\|}=0.0001$
and
$M_{\bot }=-2$
, and (ii) stationary droplet, obtained from the state corresponding to
$M_{\|}=0.0003$
and
$M_{\bot }=-2$
. Thus, bistability at several points takes place.
A snapshot of the fields of (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-2$
,
$M_{\|}=0.0002$
,
$Bo=0$
,
$Bi=20$
,
$\tau =1\times 10^6$
. The horizontal axis is
$X$
and the vertical axis is
$Y$
.

The diagram of flow regimes in the plane (
$M_{\|}$
,
$M_{\bot }$
). Squares, two-dimensional waves; asterisks, time-periodic three-dimensional waves; circles, non-periodic three-dimensional waves.

4. Droplets with an inclined temperature gradient in the presence of gravity
Let us consider the influence of the gravity force on droplet dynamics. It is known that gravity stabilizes the monotonic deformational instability (Smith Reference Smith1966) and the oscillatory Marangoni instability in two-layer systems (Simanovskii & Nepomnyashchy Reference Simanovskii and Nepomnyashchy2006), because the gravity force tends to suppress the surface deformation and flatten the surface. Similarly, gravity flattens the droplet and suppresses the oscillatory instability of the droplet. Let us take as initial conditions periodic oscillations presented in figures 7 and 8(a) at
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0$
. Under the action of a sufficiently small value of the gravity force (we take
$Bo=0.02$
), periodic oscillations become of a rather simple form. The temporal evolution of
$h_{max,2}$
and
$h_{max,1}$
is shown in figure 21. One can see that the amplitude of oscillations decreases in comparison with the case
$Bo=0$
(cf. figures 7 and 21). The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are presented in figure 22 and three-dimensional shapes of interfaces corresponding to figure 22(f) are shown in figure 23. Let us note that for droplets of the same volume, in the presence of gravity, both the top and the bottom interfaces are significantly lower and flatter than in the absence of gravity (cf., for example, figures 9 and 23).
The oscillations of
$h_{max,2}(\tau )$
(solid line) and
$h_{max,1}(\tau )$
(dashed line) for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0.02$
,
$Bi=20$
.

The fields of
$h_2(X,Y,\tau )$
for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0.02$
,
$Bi=20$
: (a)
$\tau =872\,700$
; (b)
$\tau =893\,000$
;(c)
$\tau =898\,500$
;(d)
$\tau =908\,500$
;(e)
$\tau =928\,750$
;(f)
$\tau =942\,500$
.

The shapes of (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$\bar {M}=-2$
,
$M_{\|}=0.0001$
,
$Bo=0.02$
,
$Bi=20$
,
$\tau =942\,500$
.

With an increase of the gravity force (we take
$Bo=0.05$
), the oscillations are suppressed. The temporal evolution of
$h_{max,2}$
,
$h_{max,1}$
and
$h_{min,1}$
is shown in figure 24. The droplets presented in figure 8 at
$Bo=0$
are destroyed and finally transform to a new stable configuration–one large wave, moving from the right-hand side to the left-hand side. The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
and
$h_1(X,Y,\tau )$
corresponding to a ‘vertical stripe’ are shown in figure 25. The shapes of interfaces are presented in figure 26.
The oscillations of
$h_{max,2}(\tau )$
(solid line),
$h_{max,1}(\tau )$
(dashed line) and
$h_{min,1}(\tau )$
(dotted line)for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0.05$
,
$Bi=20$
.

The fields of (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0.05$
,
$Bi=20$
,
$\tau =1\times 10^6$
. The horizontal axis is
$X$
and the vertical axis is
$Y$
.

Let us take as the initial conditions the oscillatory flow presented in figures 15 and 16(a) for the larger value of
$M_{\bot }$
(
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0$
). Under the action of the gravity force (we take
$Bo=0.04$
), the amplitude of oscillations decreases. The two-dimensional snapshots of the fields
$h_2(X,Y,\tau )$
at different instants of time are presented in figure 27 and three-dimensional shapes of interfaces corresponding to figure 27(a) are shown in figure 28. With an increase of
$Bo$
(at
$Bo\gt 0.045$
), oscillations are suppressed and we get the ‘vertical stripe’ similar to that presented in figures 25 and 26.
5. Conclusions
The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-2$
,
$M_{\|}=0.0001$
,
$Bo=0.05$
,
$Bi=20$
,
$\tau =1\times 10^6$
.

We have analysed the development of the longwave deformational instability of a floating droplet under the action of an inclined temperature gradient. The problem was studied numerically in the framework of the longwave approximation and the precursor model. The evolution equations were discretized by central differences for spatial derivatives and solved using an explicit scheme. Periodic boundary conditions have been applied on the boundaries of the computational region. Because of the anisotropy of the problem, in a contradistinction to the case of a vertical temperature gradient, the regimes of travelling droplets prevail. An inclined temperature gradient enhances the oscillatory instability threshold and it can suppress oscillations, leading to the formation of steady droplets. In a definite region of parameters, the action of an inclined temperature gradient can lead to the excitation of periodic oscillations. The diagram of regimes in the plane of two Marangoni numbers has been constructed. Bbistability at several points has been obtained. The influence of the gravity force on the floating droplets with an inclined temperature gradient has been considered. Gravity flattens the droplets and suppresses oscillations. Under the action of the gravity force, the droplets are destroyed and transform into one large wave.
The flow regimes described in the paper can be observed under microgravity conditions. Specifically, the values of parameters
$M_{\bot }$
and
$Bo$
can be reached in an experiment under normal gravity,
$g=g_0=9.8\,{\rm m \,s}^{-2}$
, in the case of
$H_1^0\sim 5$
μm, or under reduced gravity,
$g=10^{-5}g_0$
, for
$H_1^0\sim 1.5\,\rm mm$
(the temperature difference
$T_s-T_g$
is assumed to be less than 10 K).
Appendix A. Derivation of the evolution equations for deformations of interfaces
In this appendix, we describe briefly the derivation of the evolution equations for interfaces from the original system of equations and boundary conditions.
A.1. Original boundary-value problem
For sake of simplicity, for the first stage we disregard gravity and the disjoining pressures.
The complete system of nonlinear equations governing Marangoni convection is written in the following form (Simanovskii & Nepomnyashchy Reference Simanovskii and Nepomnyashchy1993):
Here,
$\textbf { v}_j$
and
$p_j$
are the velocity and the difference between the overall pressure and atmospheric pressure in the
$m$
th liquid, respectively. The boundary conditions on the rigid boundary are
On the deformable interface
$z=H_1$
, the following boundary conditions hold. The balance of normal stresses:
the balance of tangential stresses:
\begin{equation} \begin{aligned}&\left [-\eta _1\left (\frac {\partial v_{1i}}{\partial x_k}+\frac {\partial v_{1k}}{\partial x_i}\right )+\eta _2\left (\frac {\partial v_{2i}}{\partial x_k}+\frac {\partial v_{2k}}{\partial x_i}\right )\right ]\tau _{1i}^{(l)}n_{1k}\\ & \qquad -\alpha _1\tau _{1i}^{(l)}\frac {\partial T_1}{\partial x_i}=0,\quad l=1,2;\quad i,k=1,2,3; \end{aligned}\end{equation}
the continuity of the velocity field:
the kinematic equation for the interface motion:
the continuity of the temperature field:
and the balance of normal heat fluxes:
We disregard the viscosity of the gas, which is small compared to the liquid viscosities, and impose the following boundary conditions on the deformable interface
$z=H_2$
:
In the formulae presented above,
$K_1$
and
$K_2$
are the mean curvatures,
$\boldsymbol { n}_1$
and
$\boldsymbol { n}_2$
are the normal vectors and
$\boldsymbol {\tau }_1^{(l)}$
and
$\boldsymbol {\tau }_2^{(l)}$
are the tangential vectors of the lower and upper interfaces. In the quantities with two subscripts, the first subscript corresponds to the number of the liquid (
$m=1,2$
) and the second subscript determines the number of the Cartesian coordinate (
$i,k=1,2,3$
;
$x_1=x$
,
$x_2=y$
,
$x_3=z$
). The usual summation convention is applied. For a heat flux on the liquid–gas interface we use an empirical condition:
where
$q$
is the heat exchange coefficient which is assumed to be constant.
The fields of
$h_2(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0.04$
,
$Bi=20$
: (a)
$\tau =330\,000$
; (b)
$\tau =342\,500$
; (c)
$\tau =355\,000$
; (d)
$\tau =370\,000$
.

The shapes of interfaces (a)
$h_2(X,Y,\tau )$
and (b)
$h_1(X,Y,\tau )$
for
$M_{\bot }=-4$
,
$M_{\|}=0.0001$
,
$Bo=0.04$
,
$Bi=20$
,
$\tau =330\,000$
.

Below we assume that the dependence of interfacial tensions on the temperature is relatively weak and can be neglected in the boundary conditions for normal stresses (but not in those for tangential stresses where it is the source of a thermocapillary motion).
A.2. Longwave approach: scaling
We assume that the characteristic spatial scale of the temperature modulation of the substrate is much larger than the thickness of the layer, i.e. the temperature modulation depends on the scaled coordinates
$\tilde {X}=\epsilon x$
and
$\tilde {Y}=\epsilon y$
,
$\epsilon \ll 1$
, rather than on
$x$
and
$y$
. Later on, we denote the vectors
$(\tilde {X},\tilde {Y})$
as
$ {\tilde {\mathbf X}}$
and
$(\partial /\partial \tilde {X},\partial /\partial \tilde {Y})$
as
$\tilde {\nabla }$
.
We intend to apply the longwave approach for studying the instability phenomena. That is possible if the physical system is subject to a longwave instability rather than a shortwave Marangoni instability leading to creation to short-scale hexagonal cells. There exist several types of longwave Marangoni instabilities. For instance, the characteristic horizontal scale of patterns is large near the instability threshold in the case of small Biot number (Sivashinsky 1983). Another kind of Marangoni instability, which is characterized by large wavelength near the threshold, develops in thin films or under microgravity conditions (Scriven & Sternling Reference Scriven and Sternling1964).
Below we apply the formal asymptotic expansions of variables in powers of
$\epsilon$
. The appropriate scaling of variables for a long-scale flow governed by system (A1)–(A14) is as follows:
The appropriate rescaling of time is
$\tilde {\tau }=\epsilon ^2t$
.
A.3. Thermocapillary flow generated by deformations of interfaces
Solving the system of equations and boundary conditions at the leading order in
$\epsilon$
, we obtain expressions for the temperature fields:
where
Therefore, the temperature on the interface between liquids is
hence
and the temperature on the upper surface is
\begin{equation}\begin{aligned} B({\tilde {\mathbf X}},\tilde {\tau })&=T_2(\tilde {X},H_2(\tilde {X},\tilde {\tau }))\\&= T_s({\tilde {\mathbf X}})- (T_s({\tilde {\mathbf X}})-T_g)D({\tilde {\mathbf X}})q [(\kappa _2-\kappa _1)H_1({\tilde {\mathbf X}})+ \kappa _1H_2({\tilde {\mathbf X}})], \end{aligned}\end{equation}
hence
The horizontal components of the flow velocities
$\textbf { V}_m^T$
(
$m=1,2$
) generated by the thermocapillary stresses are
and the flow rates produced by the thermocapillary effect are as follows:
where
The evolution of a heated two-layer film under the action of the thermocapillary effect is governed by the closed system of equations:
A.4. Flows created by interfacial tensions, gravity and disjoining pressures
We do not intend to impose any restrictions on the values of the Marangoni and Biot numbers. Even far from the instability threshold, the longwave approach is justified if the interfacial tensions are strong. In the case of infinite horizontal layers, the linear stability theory predicts that the disturbances are unstable for wavenumbers
$k^2\lt k_m^2$
, where
$k_m^2$
is inversely proportional to the interfacial tensions. Therefore, following Fisher & Golovin (Reference Fisher and Golovin2005), we retain the Laplacian pressures at the leading order of the asymptotic expansions.
The Laplacian, hydrostatic and disjoining pressures form together the following fields of pressures in a two-layer film:
Note that although
$\tilde {\nabla }^2H_j=O(\epsilon ^2)$
for longwave deformations, the Laplacian pressures are included (see the explanation above). Formally, that corresponds to
$k^2\sim k_m^2\sim \Sigma _1^{-1}\sim \Sigma _2^{-1}=O(\epsilon ^2)$
.
The pressure gradients create flows with flow rates
where pressures
$P_1$
and
$P_2$
are determined by expressions (A30) and (A31), and the mobility functions are
Finally, we obtain the following evolution equations:
The asymptotic expansions and rescaling of the variables have allowed us to calculate the total flow rates and derive the closed equations governing the temporal evolution of the interface shapes. Now we can return to the original variables and rewrite equations (A36) as follows:
where the coefficients
$G_{ij}$
and
$F_{ij}$
are determined by formulas (A27), (A28), (A33)–(A35).
In the main text of the paper, we use equations (A37)–(A39) as the basic equations governing the problem.
Declaration of interests.
The authors declare that they have no conict of interest.




















































































































































































































