PHYSICAL REVIEW E 77, 031807 2008

Phase-field modeling of the formation of lamellar nanostructures in diblock copolymer thin films under inplanar electric fields
Xiang-Fa Wu* and Yuris A. Dzenis
Department of Engineering Mechanics, Nebraska Center for Materials and Nanoscience, University of Nebraska-Lincoln, Lincoln, Nebraska 68588-0526, USA Received 27 June 2007; revised manuscript received 4 February 2008; published 26 March 2008 Recent experiments show that external inplanar electric field can be employed to guide the molecular self-assembly in diblock copolymer BCP thin films to form lamellar nanostructures with potential applications in nanotechnology. We study this self-assembly process through a detailed coarse-grained phaseseparation modeling. During the process, the free energy of the BCP films is modeled as the Ginzburg-Landau free energy with nonlocal interaction and electrostatic coupling. The resulting Cahn-Hilliard CH equation is solved using an efficient semi-implicit Fourier-spectral algorithm. Numerical results show that the morphology of order parameter formed in either symmetric or asymmetric BCP thin films is strongly influenced by the electric field. For symmetrical BCPs, highly ordered lamellar nanostructures evolved along the direction of the electric field. Phase nucleation and dislocation climbing in the BCP films predicted by the numerical simulation are in a good agreement with those observed in recent BCP electronanolithography. For asymmetrical BCPs, numerical simulation shows that nanodots are guided to align to the electric field. Furthermore, in the case of high electric field, nanodots formed in asymmetrical BCPs may further convert into highly ordered lamellar nanostructures sphere-to-cylinder transition parallel to the electric field. Effects of the magnitude of electric field, BCP asymmetry, and molecular interaction of BCPs on the self-assembly process are examined in detail using the numerical scheme developed in this study. The present study can be used for the prediction of the formation of nanostructures in BCP thin films and the quality control of BCP-based nanomanufacturing through optimizing the external electric fields. DOI: 10.1103/PhysRevE.77.031807 PACS number s : 83.80.Uv, 81.16.Rf, 82.35.Jk, 89.75.Kd

I. INTRODUCTION

Thin films of diblock copolymers BCPs bear the natural tendency to form periodical morphology in nanoscale that provides an efficient technique to produce nanostructured materials and nanodevices 1–7 . With the aid of proper external fields, molecular self-assembly in BCP thin films can be guided to form long-range ordered nanostructures. This has evoked increasing interests due to its promising applications in nanotechnology-based products such as high-density random-access memory devices, increased capacitance gate devices, acoustic transducer arrays, photonic imaging arrays, etc. 8–13 . To date, quite a few techniques have been developed for the fabrication of long-range ordered nanostructures in BCP thin films e.g., chemically patterned substrates 14–20 , topological templates 13,21–25 , electric fields 26–34 , elastic fields 35–37 , shear flows 38–45 , etc. . One may find that external electric field may be among the most efficient means, which has attracted substantial attention since the original work achieved in Russell’s and Jaeger’s groups 26–28 . Recent endeavor has also been dedicated to understanding the alignment mechanisms and the molecular self-assembly process in BCP thin films in electric fields. For instance, it was reported recently that when subjected to an inplanar electric field of sufficient magnitude, sphere-to-cylinder domain transition happened in polystyrene-b-poly methyl methacrylate PS-b-PMMA thin films 32 . In such process, in attempting to reduce the

*xfwu@unlserve.unl.edu
1539-3755/2008/77 3 /031807 10

global free energy of the PS-b-PMMA thin films, the spherical microdomains that nucleated in the thin films were gradually deformed into ellipsoids and consequently interlinked to form cylindrical lamellar microdomains along the direction of the applied electric field. Accordingly, efficient computational modeling of phaseseparation process provides a convenient method to understand and predict the nanostructure formation process in BCP thin films. Two basic numerical schemes have been employed extensively. The first is based on the dynamic selfconsistent field SCF simulation, and the second is the cell dynamics simulation CDS . In principle, CDS can be implemented to capture the entire evolution process of the molecular self-assembly, which is also more time-efficient compared to SCF. For SCF, the large demand of the computational time is mainly due to the heavy calculation of the path integrals for the chain conformation. In addition, several research groups have examined the sphere-to-cylinder transition process in BCP thin films by using either SCF 46–52 or CDS 32,53–55 . Predictions based on the computational models were very close to those observed in experiments. This indicates the power of computational modeling in nanodevice design and prediction of nanostructure formation. Due to the rapid increase of computational cost with increasing problem scale, explicit CDS can be only fulfilled on a computational cell with intermediate number of grids. Large scale CDS modeling, especially in the case of general three-dimensional modeling, has to resort to the computational capacity of supercomputers. Also, the time step used in CDS has to be very small in order to satisfy the stability requirement of the explicit algorithms. Thus, further research is still desired in
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031807-1

¯ k . x 5 where k = k2 + k2 with kx and ky as the variables in the x y Fourier domain. the molecular chain length. It shows great numerical stability and computational efficiency in time iteration. r is the local position vector. and magnitude of the applied electric field on the molecular selfassembly process in BCP thin films.20 . the free energy of the BCP thin films is modeled as the Ginzburg-Landau free energy with nonlocal interaction and electrostatic coupling 56–60 . 4 . Thus. 0 A and B are the dielectric constants of the pure A and B homopolymer phases of the BCP film. we are going to further examine the effects of BCP asymmetry. Hereafter. Here = 0 A − B 2E2 / kT . G r . Among these efforts. y .. CDS . the volumetric integrals above can be reduced to those with respect to the substrate surface. t is the Green’s function for the Laplace equation such that 2G = − r − r . As a result. t . and variables with upper bars denote the double Fourier transforms of the corresponding variables in the physical space. t = − r . 4 Molecular self-assembly in BCPs can be described by using the Landau-Ginzburg phenomenological model of phase separation. 2 and then rescaling it with M yields the dimensionless CH equation on the substrate surface t = 2 − + 3 − 2 + − 0 .t − 0 K 2 r. Substituting Eq.e. t is the local volume fraction of the A monomer in the A-B BCP. MODEL FORMULATION AND NUMERICAL PROCEDURE In this study. Similar derivation is also available in the literature 53–55. To do so.. 031807 2008 enhancing the computational efficiency and numerical reliability in modeling the molecular self-assembly in BCPs. and the mobility M. 2 where M is the mobility to be considered as constant for convenience. IV. therefore the time steps used in iterations can be selected much larger than those used in the conventional coarse-grained phaseseparation modeling e. t is the double Fourier transform of x . 2 t = 2 − + 3 − 2 + − 0 + x2 . II. we present the results from a detailed numerical study of the molecular selfassembly in BCP thin films subjected to an inplanar electric field. the order parameter . i. in this study. 3 . 1 into Eq. Thus. This process can be modeled by the CH equation or model B in the Hoherberg-Halperin notation 64 such that t = M F .t + r. by performing double Fourier transform with respect to the spatial variables x and y at two sides of Eq. we adopt the efficient semi-implicit Fourier-spectral method 61–63 to solve Eq. i. stable phases will form through phase separation in order to reduce the global free energy of the BCP system. 4 . For instance. an additional term contributed by the electric field is added into Eq. the above free energy functional recovers that of a symmetric BCP. the time-dependent free energy functional for a general BCP confined on a flat substrate free of external field can be expressed 56–60 as F = k BT f r. 5 in the time domain for the use of the semiimplicit numerical scheme. The modified CH equation 4 can be solved conveniently by means of explicit finite difference methods within a representative computational cell under periodic boundary conditions well discussed in the literature. respectively. The remainder of this paper is organized as follows. K is a constant to delineate the phase boundary energy.XIANG-FA WU AND YURIS A. monolayer as used in BCP nanolithography recently 6–11. t exp −i kxx + ky y dxdy. III. by using this numerical scheme.r . During the process. and is a compound dimensionless parameter. Conclusions and potential applications of the present study are addressed in Sec. 0 is the mean value of the order parameter averaging spatially. t + + = − − x .g. r .t − 2 dr + A0 2 G r.. 3 where is a compound dimensionless phenomenological parameter that characterizes the nonlocal A-B potential A0.18.t 1 0 drdr .t r . r . after a quench from the high-temperature disordered melting state to a temperature below the microphase segregation temperature. The derivation of the governing CH equation of the BCP thin films and relevant numerical algorithm are presented in Sec. f r . In reality.e. 0 is the vacuum permittivity. t is the local coarse-grained free energy density of mixing that takes the Landau form such that f r . i. molecular interaction. The key idea is that treating the linear terms im- 031807-2 .. the BCP films are assumed very thin. kB is the Boltzmann constant.t . 5 separately.e. In order to discretize Eq. Numerical results for the evolution of lamellar nanostructures in symmetric BCP films and the sphere-to-cylinder domain transition in asymmetric BCP films are detailed in Sec. DZENIS PHYSICAL REVIEW E 77. where the interface energy between the BCP and the substrate is assumed constant and therefore ignored since it does not affect the phase separation process in the present study.62 . The derivation of the electric contribution is based on linear perturbation theory. T is the absolute temperature. t − 1. The resulting Cahn-Hilliard CH equation is solved using an efficient semi-implicit Fourier-spectral algorithm 61. we deal with the terms in Eq. This numerical scheme has been examined successfully in capturing the evolution of phase domains in BCP thin films on chemically patterned substrates 63 . we obtain the CH equation 4 in the time-Fourier domain ¯ t = k2 ¯ − 3 − k 2¯ − ¯ − ¯ 0 − k 2¯ .65. t is the local concentration difference between two different BCP monomers that are assumed as A and B such that r . t = 2 r . in this study. where r . y . This numerical scheme is unconditionally stable. When an external electric field is adopted along the x axis in the given BCP system. For 0 = 0. t 4 / 4. ¯ k .66 . II.16. t 2 / 2 + r .

. 2 b that for stronger monomer interaction = 0. tn . As a matter of fact. One can observe that the phase separation consists of phase nucleation and phase coarsening. the formation of lamellar nanostructures in BCP thin films can be accelerated through applying lateral electric field of high magnitude. However. respectively. tn at all spatial grids xi . independent of the spatial grid size.e. By using the efficient semi-implicit Fourier-spectral scheme in this study. 1 shows those of the BCP film in the electric field of sufficient magnitude = 0. the double Fourier transform and its inverse of the order parameter at each time step can be implemented by means of the efficient twodimensional fast Fourier transform 2D FFT and its inverse 2D IFFT . 2 c and 2 d give these in a lateral electric field of = 0. 1.e. the parameter is selected as 0. tn at time step n. evaluate 3 xi . Compared to those in Fig. . molecules in BCP films free of electric field have more degrees of freedom DOFs to move than those of electrified BCP films. numerous phase dislocations are detected in the simulation. 7 In the above numerical iteration. numerical results in Fig. . The left column in Fig.002 around the average values designated in the following.. One can observe that phase dislocations exist in the lamellar nanostructures during the process of phase coarsening. 1. lamellar nanostructures are formed along the direction of the electric field as shown in the right column in Fig. while treating the nonlinear term explicitly can avoid directly solving the nonlinear equation at each time step during the numerical iteration. It has been validated that the present semi-implicit Fourier-spectral method is unconditionally stable in the sense that given a fixed set of physical parameters. x which leads to the iteration format as ¯ n+1 = ¯n + 1+ + ¯ 0 − k2 k2 x 2 3n 4 3n − k4¯ n+1 − ¯ n+1 + ¯ 0 6 t t −k +k . . A. in the very beginning of phase separation. 1 also shows that besides the formation of lamellar nanostructures. This is because the molecular motion in a lateral electric field belongs to constrained motion. Hereafter.PHASE-FIELD MODELING OF THE FORMATION OF… PHYSICAL REVIEW E 77. 031807 2008 plicitly can reduce the stability constraints. simulation of the phase separation free of electric field has also been performed. tn+1 . When subjected to lateral inplanar electric field. and 0 in Eq. In the following simulations. In addition. The size of the computational cell in each simulation is fixed as 256 256. such that for all t tc. Figure 2 b shows the results free of electric field. y j .2.1. III. the present numerical scheme is capable of remarkably enhancing the computational efficiency and simultaneously improving the numerical stability.5 is fixed for the time integration of all cases in this study.2 . Figs.1 and 0. higher rate of phase separation. NUMERICAL RESULTS Within the framework of above computational scheme. tn and ¯ pq k . y j and time step n + 1.. the morphology of order parameter for either neutral or electrified BCP films has tended to be stable though it continues evolving and coarsening afterwards. y j . 2 a shows the morphology of order parameter of the above BCP thin films = 0. tn+1 and then obtain xi . 1 and 2. Fig. 2 b –2 d show the morphologies of order parameter of the BCP films with = 0. Due to use of the semi-implicit algorithm in the time domain and the Fourier-spectral scheme in spatial domain. 1. and 5000 during the phase separation process free of electric field = 0 . 4 Perform 2D IFFT to invert ¯ pq k . when subjected to weak lateral electric field. After 5000 iterations in each case. and 0 on the self-assembly process in the BCP thin films within a 2D computational cell under periodic boundary conditions. For the purpose of examining the effect of molecular interaction on the phase separation process. 2 Perform 2D FFT to determine 3 k .5 .2 after 5000 iterations. BCP film 1000. we obtain the final form of the discretized equation ¯ n+1 − ¯ n / t = k2¯ n+1 − k2 − k2¯ n+1 .1 at five sequential instants t = 10. As a result. Among these. Sufficient large time step of 0. As a result. respectively. y j . After 1000 iterations. 100. while the right column in Fig. pq 3 Evaluate relation 7 to determine ¯ pq k . we examine the effects of .8 . Phase separation of symmetric BCP films in electric field Let us first consider the phase separation process in symi. the rate of electrified phase separation in the very beginning is lower than that free of the electric field t = 100 for instance . compared to that of the left column in Fig. one can find that three parameters i. there always exists a time threshold tc. and therefore is much more efficient than the classic CDS. The typical operations from time step n to n + 1 are the following: 1 With xi . 1 indicates in the symmetric the morphologies of order parameter = 0.e. after the beginning stage of phase nucleation. tn+1 at all spatial grids xi . The initial concentration of the order parameter is assumed to have a Gaussian fluctuation of magnitude 0. 0 = 0 in a metric BCP thin films of varying and lateral electric field along the x axis. Consequently. i. Furthermore. to show the effects of the BCP incompatibility and external electric field on the phase separation. For comparison. The dislocations gradually disappear through climbing and molecular diffusion under the action of the electric driving force. well-developed serpentine and lamellar nanostructures have formed in both neutral and electrified BCP thin films as shown in Figs.62 .1 after 5000 iterations. Fig. 5 dominate the entire phase separation in the BCP thin films. the time step has been selected very large in the iterations t = 0. One can observe in Fig. the time steps can be selected as orders of those utilized in the conventional explicit Euler forward method.05 and 0. the extent of the corresponding phase separation is 031807-3 . the above scheme is stable for all spatial grid sizes 61. y j . and 0 are related to the BCP molecular structures and is linked to the combined effect of the external electric field and the BCP dielectric properties. electric field has no significant effect on the extent of phase separation due to the characteristic of the global action exerted by the electric force on the molecular chains of the BCP films. 1 indicate that electric field has no noticeable effect on the rate of phase separation. while Figs. Furthermore.

8 . and 5000 in the case of lateral inplanar electric field . respectively. The right column are those obtained at the same five sequential instants t = 10. and 5000 in the phase separation process free of electric = 0. 1000. f . 1000. respectively. as indicated as e . 031807-4 field.1 and 0=0 .XIANG-FA WU AND YURIS A. DZENIS PHYSICAL REVIEW E 77. g . 100. 100. 1. as indicated as a . Color online The morphology of order parameter numerical results of order parameter in symmetric BCP thin films = 0. and h . c . and d . b . The left column are the at five sequential instants t = 10. 031807 2008 FIG.

1 . III A. we also examine the phase separation process in the same BCP thin film in weak electric field = 0. 3 shows the morphologies of order parameter in neutral and electrified asymmetric BCP thin films = 0. Phase separation of asymmetric BCP films in electric field Now let us consider the molecular self-assembly in asymmetric BCP thin films. b = 0. In this case. 2 c and 2 d fields indicate that a variety of phase dislocations exist due to the slow formation of lamellar nanostructures under weak electric driving forces.1 in electric field .PHASE-FIELD MODELING OF THE FORMATION OF… PHYSICAL REVIEW E 77.35 at five sequential instants t = 10. the morphology of order parameter in Fig. Color online The morphology of order parameter in symmetric BCP thin films 0 = 0 after 5000 iterations. 3. lower than that with weak monomer interaction such as = 0.1 in electric field . The left column are these free of electric field. When subjected to relatively high lateral electric field. 4 a shows a variety of intermediate phase struc- 031807-5 . 3 shows that lamellar nanostructures begin to form in the very beginning of the process. Based on the above numerical scheme. After 5000 iterations. and d = 0. coarsening of the random nanodots accompanies with the annihilation of unstable nanodots usually in relatively smaller size through molecular diffusion.05 in electric field . one can observe that well-defined morphologies of random nanodots and lamellar nanostructures have formed after 5000 iterations. for instance . due to the introduction of electric field of high magnitude. respectively. 1000.1 see Fig.2 . sphere-to-cylinder domain transition happened in the very beginning of the process. Figs. c = 0. the phase separation process in this case also consists of phase nucleation and phase coarsening to reduce the global free energy of the BCP system.05 and 0 = 0. Similar to that of symmetric BCPs as discussed in Sec. In the cases of relatively weak electric = 0. 100. a = 0. phase dislocations nucleate and then climb to reduce the global free energy. 031807 2008 FIG. and 5000. Fig. From Fig. 2. Furthermore. while the right column are those in lateral electric field = 1.8 .2 and = 0 free of electric field .2 and = 0. For asymmetric BCP films free of electric field. the right column of Fig.1 and = 0. it can be found that with the aid of the electric driving force. In order to examine this transition.05 and 0.1.2 and = 0. B.

100. f . respectively. 1000. b . 1000. as indicated as e . as indicated as a . The left column are at five sequential instants t = 10. The right column are those results obtained at the same five sequential instants t = 10. c .8 .05 and 0 = 0. respectively. 031807 2008 FIG. DZENIS PHYSICAL REVIEW E 77. g . Color online The morphology of order parameter the numerical results of order parameter in asymmetric BCP thin films = 0. and 5000 in the case of lateral inplanar electric field 031807-6 . and h . electric field. and 5000 in the phase separation process free of = 1. 3. 100.XIANG-FA WU AND YURIS A.35 . and d .

15. similar to those observed in recent experiments 32. the morphology of order parameter in BCP thin films has been determined through detailed phaseseparation modeling. t and I kx . 4 b . and = 0. 0 = 0. and Figs.4 in electric field . the morphology of order parameter includes random nanodots and nanoislands as shown in Fig. we further consider the evolution of domain size by introducing the transient average domain size Ry t along the y direction. a = 0.05. In this section. and = 0.PHASE-FIELD MODELING OF THE FORMATION OF… PHYSICAL REVIEW E 77. In the latter cases.02. 4 c and 4 d show the intermediate lamellar nanostructures of the BCP films in relatively weak electric fields with = 0. and = 0 free of electric field . the inverse of the transient average wave numbers ky t 63. 10 In the above.t = 1 ¯ kx. and d = 0.ky .4 asymmetric BCP thin films = 0. which is defined by where N = L is the total number of grids within the computational cell.02. after 5000 iterations.t 9 kx ky In relations 8 and 9 ky is the variable in Fourier domain. This formation process can be accelerated by increasing the magnitude of electric field. b = 0. and cylinders.t ky t = kx ky 8 . S kx. 0 = 0. the lamellar nanostructures are still evolving.2 and 0.t ¯ − kx. Color online The morphology of order parameter in asymmetric BCP thin films after 5000 iteration. ky .2 in electric field . and S kx .4. Domain size evolution I kx.35.15.ky. ky are the coefficients of 2D FFT of 2 031807-7 . ky .02. 4. and ¯ kx . 0 = 0. In the case free of electric field. where kyS kx. t is the element of the structure factor matrix defined by 67–69 S kx. ellipsoids. 031807 2008 FIG. we also investigate the phase separation process in neutral = 0 and electrified = 0.02 and 0 = 0. tures including spheres. 0 = 0.ky.15.2 in electric field .53 .2 and 0. c = 0. In addition.− ky.t − N 2 C.15 . is the average order parameter.67–69 as Ry t = 2 / ky t . and = 0.ky.ky. respectively.

031807-8 . In the case of symmetric BCP thin films = 0. one can draw the conclusion that the adoption of lateral electric field can decrease the transverse domain size Ry t for both symmetric and asymmetric BCP thin films. and it can also be used for the analysis and prediction of the process of nanostructure formation in BCP thin films. the stable Ry t is reduced to 13. while in lateral electric field = 0. Figs. x . CONCLUDING REMARKS In this study. Variation of the domain size Ry t vs the time of the asymmetric BCP thin films = 0. 031807 2008 Dimensionless domain size (Ry) 50 40 30 20 10 0 0 500 b=0 (Free of electric field) b=0. The present study also indicates that external electric field has no noticeable effect on the extent of phase separation. y . usually formed free of electric field. 6. the stable Ry t is close to 20. It can be observed that the domain size along y direction Ry t in each case decreases abruptly in the very beginning of phase separation i.8 . the corresponding stable Ry t is reduced to around 17.1 and 0 = 0 during the molecular self-assembly process. respectively. The entire process of forming lamellar nanostructures consists of phase nucleation and phase coarsening through climbing of phase dislocations and molecular diffusion. the stable Ry t is close to 17. the domain size decreases accordingly with the formation of ordered lamellar nanostructures due to the “electric stretching” effect.35 case of asymmetric BCP thin film free of electric field. Numerical results indicate that lateral electric field can be employed to form ordered lamellar nanostructures in both symmetric and asymmetric BCPs.5. For asymmetric BCP thin films in electric field of sufficient magnitude. sphere-to-cylinder transition happened during the formation of lamellar nanostructures. IV. 1–4.5. 5 and 6 show the evolution of domain size of the BCP thin films in above simulations. It shows that the semi-implicit Fourier-spectral algorithm adopted in this study can obviously enhance the computational efficiency and numerical stability. Moreover. In practice..8 . Such “electric stretching” decreases the domain size of the random nanostructures in BCP thin films perpendicular to the direction of the inplanar electric field. we have examined the molecular selfassembly in both symmetric and asymmetric BCP thin films by solving the resulting CH equation numerically. into highly ordered lamellar nanostructures along the direction of the inplanar electric field as shown in Figs.8 (In electric field) 1000 1500 2000 2500 Dimensionless time (t) FIG. Detailed morphology of order parameter of the BCP thin films and the evolution of domain size have been examined. 5. With definition 8 . FIG.e.35 during the molecular self-assembly process. In addition. In the = 0.05 and 0 = 0. the phase nucleation stage . and then tends to constant through phase coarsening in both the symmetric and asymmetric BCP films. This is because the lateral electric field is able to “organize” the random nanostructures. ACKNOWLEDGMENT Partial support of this work by the NSF/AFOSR/ARO/ ARL is greatly appreciated.1 and 0 = 0 free of electric field. Thus. thus electrically guided molecular self-assembly in BCP thin films can be utilized efficiently in manufacturing highly ordered nanostructures and nanodevices.XIANG-FA WU AND YURIS A. t and the unit in the computational cell. the numerical method presented in this study can be used for intelligent BCP-based nanomanufacturing for targeted nanostructures through optimizing the applied electric field.05 and 0 = 0. DZENIS 60 PHYSICAL REVIEW E 77. The rate of phase separation in the BCP thin films depends upon both the type of molecular chain structures and the magnitude of electric field. lateral electric field can be introduced conveniently. when introducing a lateral electric field = 1. Variation of the domain size Ry t vs the time of the symmetric BCP thin films = 0.

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