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WO2000021689A1 - Formation de motifs microscopiques et articles formes - Google Patents

Formation de motifs microscopiques et articles formes Download PDF

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Publication number
WO2000021689A1
WO2000021689A1 PCT/US1999/023717 US9923717W WO0021689A1 WO 2000021689 A1 WO2000021689 A1 WO 2000021689A1 US 9923717 W US9923717 W US 9923717W WO 0021689 A1 WO0021689 A1 WO 0021689A1
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WO
WIPO (PCT)
Prior art keywords
mask
pattern
pillars
polymer
substrate
Prior art date
Application number
PCT/US1999/023717
Other languages
English (en)
Inventor
Stephen Y. Chou
Lei Zhuang
Original Assignee
The Trustees Of Princeton University
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by The Trustees Of Princeton University filed Critical The Trustees Of Princeton University
Priority to US09/807,266 priority Critical patent/US6713238B1/en
Priority to AU14448/00A priority patent/AU1444800A/en
Publication of WO2000021689A1 publication Critical patent/WO2000021689A1/fr
Priority to US10/731,818 priority patent/US7482057B2/en
Priority to US11/933,170 priority patent/US8852494B2/en
Priority to US12/136,964 priority patent/US20090084492A1/en

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y40/00—Manufacture or treatment of nanostructures
    • G—PHYSICS
    • G03—PHOTOGRAPHY; CINEMATOGRAPHY; ANALOGOUS TECHNIQUES USING WAVES OTHER THAN OPTICAL WAVES; ELECTROGRAPHY; HOLOGRAPHY
    • G03F—PHOTOMECHANICAL PRODUCTION OF TEXTURED OR PATTERNED SURFACES, e.g. FOR PRINTING, FOR PROCESSING OF SEMICONDUCTOR DEVICES; MATERIALS THEREFOR; ORIGINALS THEREFOR; APPARATUS SPECIALLY ADAPTED THEREFOR
    • G03F7/00—Photomechanical, e.g. photolithographic, production of textured or patterned surfaces, e.g. printing surfaces; Materials therefor, e.g. comprising photoresists; Apparatus specially adapted therefor
    • G03F7/0002—Lithographic processes using patterning methods other than those involving the exposure to radiation, e.g. by stamping

Definitions

  • the present invention relates generally to forming patterns on or in a surface material, assemblies used therefor, and articles formed thereby. More specifically, the present invention relates to microscale patterning and/or lithography. Microscale patterning and microscale lithography have a broad spectrum of applications, e.g. in the production of integrated circuits, microdevices, and the like. The patterns formed can be utilized to perform an array of functions, including electrical, magnetic, optical, chemical and/or biological functions.
  • Lithography is often used to create a pattern in a thin film carried on a substrate so that, in subsequent process steps, the pattern will be replicated in the substrate or in another material which is added onto the substrate.
  • One purpose the thin film satisfies is protecting a part of the substrate so that in subsequent replication steps, the unprotected portion can be selectively etched or patterned.
  • the thin film is often referred to as a resist.
  • a typical lithography process for the integrated circuits fabrication involves exposing a resist with a beam of energetic particles which are electrons, or photons, or ions, by either passing a flood beam through a mask or scanning a focused beam.
  • the particle beam changes the chemical structure of the exposed area of the film, so that when immersed in a developer, either the exposed area or the unexposed area of the resist will be removed to recreate the pattern or obverse of the pattern, of the mask.
  • a limitation on this type of lithography is that the resolution of the image being formed is limited by the wavelength of the particles, the particle scattering in the resist, the substrate, and the properties of the resist.
  • U.S. Patent No. 5,772,905 describes a method and apparatus for performing ultra-fine line lithography wherein a layer of thin film is deposited upon a surface of a substrate and a mold having at least one protruding feature and a recess is pressed into the thin film.
  • Block copolymer films have been suggested for use as lithography masks wherein micelles of the copolymer which form on the surface of a water bath are subsequently picked up on a substrate.
  • self-assembly has been primarily on either phase separation of a polymer blend, of di-block copolymers, or of local modification of surface chemistry (i.e., chemical lithography).
  • phase separation the periodic structures are multidomain, and their orientation and locations are uncontrollable and random.
  • a long-sought after goal in self-assembly is precise control of the orientation and location of a self-assembled polymer structure.
  • the present invention is generally directed to the formation of patterns in a material through deformation induced by a mask placed above a material, as well as assemblies used therefor, and products formed thereby.
  • An important aspect of the present invention is novel method, referred to herein as "lithographically-induced self-assembly" (LISA).
  • a mask is used to induce and control self-assembly of a deformable surface, preferably a thin film into a pre-determined pattern.
  • One advantage of the present invention is relatively accurate control of the lateral location and orientation of a self-assembled structure.
  • a substantially uniform, film is cast on a substrate.
  • a mask preferably with protruding patterns representing the pattern to be formed in or on the film, is placed above the film, but physically separated from the film by a gap.
  • the mask, the film, and the substrate are manipulated, if necessary, to render the film deformable.
  • the polymer film may be heated to a temperature above the polymer's glass transition temperature and then cooled down to room temperature.
  • the initially flat film assembles into discrete periodic pillar arrays.
  • the pillars formed by rising against the gravitational force and surface tension, bridge the two plates to form periodic pillar arrays.
  • the pillars generally have a height equal to the plate-mask separation.
  • the pillar array is generally formed only under the protruding pattern with the edge of the array generally aligned to the boundary of the mask pattern. After the pillar formation, due to a constant polymer volume, there is little polymer left in the area between pillars.
  • the shape and size of the mask pattern can be used to determine the pillar array's lattice structure. The location of each pillar can be controlled by the patterns on the mask. This process can be used repeatedly to demagnify the self-assembled pattern size. This demagnification permits a self-assembled structure to have a size smaller than that of the mask pattern(s).
  • the basic LISA process can also be modified to form a non-pillared pattern that is substantially identical to the features of the mask.
  • One embodiment of the present invention is a patterning method or method of patterning which comprises depositing a material on a substrate.
  • the material and substrate may be already formed, and the material and substrate may be the same or different.
  • the step of depositing a material would not be necessary, but rather a surface layer(s) would be selectively manipulated so that a pre-determined thickness of surface material is deformable. This thickness must be small enough that the mask can interact with the material through the separation distance to form a contact therebetween.
  • the thin film or surface layer(s) preferably has a thickness in the range of about 1 nm to about 2,000 nm, more preferably about 10 nm to about 1,000 nm, more preferably about 100 nm to about 500 nm and even more preferably about 50 nm to about 250 nm.
  • the deposited material is deformable at room temperature (e.g., a liquid polymer or polymer dispersion, the material may not need to be deformed).
  • a liquid polymer is used, it may be cured (e.g., photo curing) after either pillar formation, usually before removal of the mask.
  • it may be necessary to render the material deformable e.g.
  • Heating may occur by any conventional means (e.g., laser, light sources, heat radiating or microwave induction), and the heat may be pulsed or continuous.
  • the substrate can be any number of compositions which are capable of supporting the film, but the present invention has particular applicability to substrates which are, themselves intended to be processed to have patterns formed thereon or therein.
  • the substrate can have pre-existing relief patterns or be flat.
  • the mask can be of any suitable material as described herein, in many cases, the mask, will often be very similar in composition to the underlying substrate. Indeed, it is envisioned to use a suitably patterned substrate from a previous LISA process in a second or more LISA process or LISC process.
  • the mask can have any suitable surface coating and the protrusion may be formed from a surfactant or other suitable protruding material (e.g., monolayers or self-assembled monolayers) with a different surface energy.
  • the protruding pattern may be of varying heights on the same pattern resulting in like pillars. Of course, any combination of protrusion pattern protrusion coating or monolayer material pattern may be used to form the relief structure.
  • Another embodiment of the present invention is the relief structure formed by either or both the LISA and LISC process.
  • Fig. 1 schematically illustrates lithographically-induced self-assembly (LISA): (a) a flat substrate, (b) a thin layer of deformable material deposited thereon, (c) a mask with a protruding pattern a distance above the deformable material; and (d) self-assembly into a periodic supramolecular pillar array after a heat-and-cool cycle;
  • Fig. 2 is an (a) optical and (b) AFM images of periodic pillars formed using a mask of a plain flat surface. The pillars have a closely-packed hexagonal lattice and are multi-domain, covering the entire wafer with a single-domain size of about 50 ⁇ m;
  • Fig. 3 is an optical micrograph of (a) a protruding triangle pattern on the mask and (b) pillar array formed under the triangle pattern using LISA, and (c) AFM of the pillar array;
  • Fig. 4 is an optical and AFM images of the LISA pillar arrays formed under protruding square patterns of a side of (a) 10 ⁇ m, (b) 14 ⁇ m, and (c) 14 ⁇ m. The separation between the mask and the substrate
  • Fig. 5 is (a) optical micrograph of a protruding line pattern spelling "PRINCETON' on the mask and (b) AFM image of pillars formed under the mask pattern;
  • Fig. 6 is an AFM image of a pillar array formed under a grid-line mask pattern with each pillar aligned under an intersection of the grid;
  • Fig. 7(a) illustrates schematically lithographically-induced self-assembly using a surfactant as the pattern: (i) A thin layer of homopolymer cast on a flat silicon wafer, (ii) A mask of surfactant patterns placed a distance above the PMMA film, but separated by a spacer, (iii) During a heat-and-cool cycle, the polymer film self-assembled into a periodic supramolecular pillar array, (b) Schematic of the experimental setup;
  • Fig. 8 shows the observed dynamic behavior of the growth of the first pillar under a square mask pattern at 120°C.
  • the polymer was featureless before heating the system. The beginning of 120°C was set as time zero,
  • the polymer under the corners of the mask pattern is being pulled up;
  • the first pillar just touched the mask;
  • the pillar expanded to its final size:
  • Fig. 9 shows the observed dynamic behavior of the growth of an array formed under the square mask pattern at 120°C from the first pillar to the last pillar.
  • the pillars were formed in an orderly manner, one by one, first under the corners of the mask pattern, then along the edges, later new corners and new edges, until the area under the mask pattern was filled with pillars.
  • the completion of the first pillar was set as time zero;
  • Fig. 10 is the atomic force image of the same LISA pillar array (5x5 pillars) as in Fig. 8 and 9.
  • the pillars with a flat top have a height, diameter, and period of 310 nm, 5 ⁇ m, and 9 ⁇ m, respectively.
  • the array has a simple cubic lattice;
  • Fig. 11 schematically illustrates a proposed model for LISA: (a) surface roughening, (b) roughening enhancement due to a long range attractive force, (c) pillar formation, and (d) self-organization;
  • Fig. 12 schematically illustrates lithographically induced self- construction ("LISC") schematic of LISC: (a) a thin polymer film cast on a flat substrate (e.g. silicon), (b) a mask with protruding patterns placed a distance above the polymer film, (c) during a heat-and-cool cycle, the polymer film self- constructs into a mesa under a mask protrusion.
  • the mesa has a lateral dimension identical to that of the mask protrusion, a height equal to the distance between the mask and the substrate, and a steep side wall;
  • Fig. 13 shows (a) optical image of protruded pattern of "PRINCETON” on the mask, and (b) AFM image of the LISC patterns formed underneath the mask pattern.
  • the LISC pattern duplicates the lateral dimension of the mask pattern.
  • Fig. 14 illustrates Self- Assembly (SALSA) of a Random-Access Electronic Device. DETAILED DESCRIPTION OF THE PRESENT INVENTION
  • placing a mask a distance above a surface results in the formation of a self-assembled periodic supramolecular array of pillars during a heat-and- cool cycle.
  • the pillars are formed in the area under the protruding mask pattern and are normal to the substrate.
  • the pillars generally extend all the way to the mask (or to protrusion patterns on the mask).
  • the location of each pillar as well as the size, shape, and lattice structure of the array can be controlled by the patterns on the mask with a great deal of precision.
  • the period and diameter of the pillars also can be controlled, depending, for example, on the molecular weight of the polymer.
  • LISA Low-density polystyrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene, acrylonitrile-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-styrene-
  • Fig. 1 schematically illustrates the lithographically induced self-assembly of the present invention.
  • a material 33 which, in the preferred embodiment, is a thin layer of a homopolymer, preferably polymethyl-methacrylate (PMMA).
  • PMMA polymethyl-methacrylate
  • the PMMA was first spun on substrate 31, in this case, a silicon wafer having a substantially plain flat surface, followed by baking at 80°C to drive out the solvent.
  • a mask 35 typically made of silicon dioxide, with a protruding pattern 37 on its surface that faces a deformable material 33 is placed above the PMMA film 33.
  • Fig. 1 schematically illustrates the lithographically induced self-assembly of the present invention.
  • the mask 35 is separated, using a spacer 39, from the PMMA by several hundred nanometers.
  • the distance between the protrusion 37 and film 33 is preferably in the range of about lOnm to about 1000 nm, more preferable 50 nm to 800 nm, and never more preferably that about 100 nm to about 700 nm.
  • the spacer 39 may be either integrally formed with the mask or a separate element (see e.g. Fig. 12).
  • Pattern forming assembly 41 was heated from room temperature to a temperature above the glass transition temperature of the
  • a press or chuck 51 shown in Fig. 8b was used to hold the substrate 31, the spacer 39, and the mask 35 (i.e. the pattern forming assembly) in their respective positions, thereby preventing substantial relative movement and maintaining the mask-substrate separation constant.
  • the substrate 31 is wet to the deformable material 33.
  • the silicon substrate surface preferably has a thin layer of native oxide, making it a high energy surface and wet to a PMMA melt.
  • the mask surface 47 has a monolayer surfactant, making it a low energy surface and non-wet to a PMMA melt. The heat-cool cycling was performed either in atmosphere or a vacuum of 0.3 torr, which has little effects on the final results.
  • the height of the protruding patterns 37 on the mask 35 is typically micro scale and generally in the range of about 50 nm to about 500 nm (in this example 150 nm). It was observed that without a mask placed on the top, after a heat-cool cycle, the PMMA film 33 remains flat and featureless. But, with a mask 35 placed a certain distance above the surface of the PMMA film 33, after the same heat-cool cycle, the initially flat PMMA film 33 became self- assembled into periodic supramolecular pillars 49 shown in Fig. 1. The pillars 49 were formed only under the protruding patterns 37 of the mask 35, but not under the recessed areas of the mask 35.
  • the pillars 49 are normal to the substrate 31 and extend all the way from the substrate 31 to the mask 35, making their height generally equal to the initial separation 43 between the substrate 31 and the surface of the mask 35.
  • the location of each pillar 49 as well as the size, shape and lattice structure of the array is determined by the pattern 37 on the mask 35.
  • the atomic force microscopy (AFM) showed that the top of each pillar 49 is flat (due to contact with the mask) and the sidewall is quite vertical (due to the tip size effect, the AFM tip is not good for profiling the sidewall).
  • Two-dimensional Fourier transform of the AFM images showed six sharp points arranged in a hexagonal shape in the k-space, further confirming the hexagonal lattice structure of the pillars.
  • the initial PMMA thickness was about 95 nm.
  • the substrate and the mask were heated to 130 °C and were held together for 20 min by a pressure of 300 psi. Then they were cooled down for 10 min to room temperature before being separated.
  • a smgle-domain PMMA pillar 79 array of a close-packed hexagonal lattice is formed under the mask pattern 67.
  • Both optical and AFM images show that the shape and size of the pillar 79 array are identical to that of the mask pattern, with the pillars 79 on the edges of the array aligned along the edges of the triangle mask pattern 67.
  • the polymer initially under the recessed area of the mask 35 is depleted after the LISA process and no pillars 79 are formed under the area.
  • initial thickness of the PMMA film 33 was 95 nm.
  • the initial separation between the substrate and the mask pattern 67 was 530 nm.
  • the LISA pillar array is a close-packed hexagonal structure that has a periodicity of 3 ⁇ m, an average pillar diameter of 1.6 um.
  • the triangle mask pattern 67 has a side of 53 ⁇ m; a larger size will make the pillar array multi-domain.
  • the pillar arrays 99a formed in LISA also have a shape and size identical to the mask patterns with the pillars 99a at the edges aligned to the edges of the mask patterns, just as in the case of the triangle mask pattern.
  • the lattice structures of the pillar arrays are not hexagonal. It appears that the pillars 99a on the edges are formed and aligned to the mask pattern edges first. Then the other pillars will be formed later according to the position of the edge pillars.
  • the shape of the mask and the pillar height determine the final lattice structure of a pillar array.
  • Table 1 The size and shape of a number mask used in our experiment as well as the diameter, period and height of the pillars formed in LISA are summarized in Table 1 below. Table 1 below provides a summary of the geometry of the mask patterns and the LISA Pillars.
  • the pillar diameter seems to decrease, with increasing the pillar height (i.e., the separation between the substrate and the mask), that can be understood from the fact that the total polymer volume is constant.
  • the pillar period was found to vary slightly with different mask pattern geometry. Further experiments showed that the pillar period and size depend on the polymer molecular weight. When PMMA of 15K molecular weight (made by a vendor different from 2K PMMA) was used, the pillar period and diameter became about 8 ⁇ m and about 5 ⁇ m, respectively. It was also found that as the heating time could impact pillar formation.
  • An example of high ratio of pillar height to the pillar diameter we achieved is 0.5 (800 nm height and 1.6 ⁇ m diameter). As can be seen in Fig. 5, if the mask pattern is a protruding line of a width less than 5 ⁇ m, a single pillar line will be formed and aligned under the line pattern.
  • the mask pattern is a grid
  • a pillar 109 is formed and aligned under each intersection of the grid mask pattern.
  • the pillar 109 period is fixed by the period of the grid on the mask.
  • the plate or mask when placed a distance above a thin melt film, preferably a single-homopolymer melt film, causes the polymer film, initially flat on another plate, to self-assemble into periodic pillar arrays.
  • the pillars form by raising against the gravitational force and the surface tension, bridge the two plates, having a height equal to the plate- mask separation.
  • the mask surface has either a protruding pattern, a surfactant pattern (e.g. with a shape of a triangle or rectangle, etc.), or a combination of the two, a pillar array is formed under the pattern with its boundary aligned to the boundary of the mask pattern and with its lattice structure determined by the mask pattern geometry.
  • a monitoring assembly 110 was used to monitor the development of the pattern forming process of LISA in a polymer film.
  • the monitoring assembly 110 is shown in Fig. 7b.
  • the mask was made of glass, thus allowing for observation through the mask using an optical microscope 112.
  • a CCD camera 114 and video recorder 116 with a time resolution of 30 millisecond recorded the pattern forming behavior.
  • the sample consists of 2,000 molecular weight (2K) PMMA polymer 103 cast on a silicon substrate 101 that has a surface that wets the PMMA polymer 103.
  • the glass transition temperature of the PMMA was found to be 96°C.
  • the mask 105 has various patterns of a monolayer of self-assembled surfactant 117.
  • the surfactant 117 was applied to the mask 105 via photolithography and a lift-off.
  • the substrate 101 and mask 105 were separated by a 220 nm spacer 109 and were held together by a metal holder comprised of a chuck 51 and a screw 53 with the pattern forming assembly interposed therebetween.
  • the entire pattern forming assembly 111 was heated by a hot plate 55. The temperature was monitored by a thermocouple mounted on the holder.
  • Fig. 8 shows the growth of the first pillar in the array.
  • the sample holder was heated from room temperature to 120°C and maintained that temperature for the remainder of the experiment.
  • the PMMA was featureless.
  • the temperature was increased at a rate of about 10°C/min up to 100°C and then at l°C/min after that. Once the temperature exceeded 110°C, a very faint image showing the outline of a pattern could be observed. As can be seen in Fig. 6 this latent image was clearly visible once the system reached 120°C.
  • the beginning of 120°C was chosen as the zero time reference in Fig. 8.
  • the latent pattern indicates the onset of pattern formation and is visible because the polymer in that region is several tens of nanometers higher than the surrounding film.
  • a latent image formed first under the corners of the mask pattern and then the edges.
  • the latent image at the corners becomes much more pronounced, indicating the growth of polymer pillars at the corners
  • Fig. 8c-e It was observed that one pillar always grew faster than the rest. In this particular example, it took 58 minutes for the first pillar to reach the mask. When a pillar just touched the mask, its image became a black point in the center of a bright circle (see Fig. 8g), and then expanded into a bright dot of 5 ⁇ m diameter in 6 seconds (see Fig. 8i). This suggests that pillars first grow as a cone-shaped spike in the polymer film and then, after touching the mask, reshape into a pillar with a flat top.
  • the mask surface should be a low energy surface to limit the distance that a pillar can spread.
  • Fig. 9 shows the growth behavior from the first pillar to the last pillar of a LISA array formed under the square mask pattern.
  • the time zero in this figure is set at the completion of the first pillar.
  • the formation of the second pillar was completed 9 seconds after the first pillar, in a corner of the mask pattern adjacent to the first pillar (See Fig. 9b).
  • the third pillar was completed 58 seconds later and was in a corner adjacent to the second pillar (See Fig. 9c).
  • the fourth pillar was formed at 2 min 59 seconds (See Fig. 9d).
  • new pillars started to form at the edges of the mask pattern (See Fig. 9e-g). A new edge pillar was observed to always form adjacent to an existing pillar.
  • the first ring of pillars was completed, which took about 50 minutes beyond the first pillar formation, the second latent pattern images formed just inside the ring.
  • a new pillar was formed at a new corner, then the adjacent corners, later the new edges.
  • pillar formation propagated from the corners to the edges and from outside to inside (See Fig. 9h-l). Similar dynamic behavior has been observed in square patterns with different sizes as well as with mask patterns with different shapes (e.g., triangles and rectangles).
  • the atomic force microscope image of the LISA pillar array shown in Fig. 10 shows that the diameter of each pillar is uniform and that the top of each pillar is substantially flat.
  • the pillar height, diameter, and period is 310 nm, 5 ⁇ m, and 9 ⁇ m, respectively. The measured height suggests that the actual mask- substrate spacing was 310 nm and that the spacer was pressed 45 nm into the PMMA.
  • Fig. 11 illustrates a proposed model for the formation of periodic supramolecular pillar arrays in a film utilizing the LISA process.
  • LISA appears to occur in four stages. The first stage is the surface roughening shown in Fig. 11a.
  • a polymer 133 When a polymer 133 is heated above its glass transition temperature, it becomes a deformable and/or viscous liquid than can flow. Since there is an open space between the polymer 133 and the mask 135, the polymer 133 will flow and deform three-dimensionally to relieve the polymer film's internal stress and surface tension, roughening the surface of the polymer film surface.
  • the second stage is the enhancement of the polymer surface roughening shown in Fig. lib.
  • Placing a mask 135, preferably a dielectric mask polymer 133, on top of the PMMA can create a Nan der Waals attractive force, which is long-range and inversely proportional to a power of the distance between the film 133 and the mask 135. The closer to the mask 135, the larger the attractive force on the polymer 133, making the film roughness grow until some polymer touches the surface 147 of the mask.
  • the third stage is the pillar 149 formation shown in Fig. lie.
  • the low energy surface of the mask forces the polymer melt 133 to ball up on the mask surface 147, forming round pillars 149.
  • the high energy surface of the substrate 131 always keeps its surface 148 covered with a thin layer of polymer 133.
  • the thin film layer connects all polymer pillars 149, allowing a polymer mass flow between the pillars 149.
  • the thin film layer also acts as a polymer reservoir, supplying polymer to the pillars 149.
  • the connectivity and the polymer mass-transfer equalize the pressure inside all pillars, and hence the pillar diameter.
  • the final diameter of a pillar 149 also depends on the other forces applied to the pillar 149, as discussed in the next paragraph.
  • the fourth and final stage is the self-organization shown in Fig. lid.
  • the polymer pillars 149 have random locations and various diameters, and can move around inside the area defined by a mask pattern 137. But, once a pillar 149 moves to an edge of the mask pattern 137, part of its triple-phase line (i.e. the line that intersects the liquid, solid and vapor phase) is trapped to the edge, limiting the pillar's movement to only along the edge. When a pillar 149 reaches a corner of the mask pattern 137, another part of its triple-line is trapped by another edge.
  • the LISA process is related to (i) a long-range attractive force between the polymer melt film and the mask, (ii) the hydrodynamic forces in the polymer melt, (iii) the surface tension, and (iv) the interplay of all the forces.
  • the long range force could be electrostatic, dipole, or Nan der Waals forces, or a combination of all. It appears that electrostatic force is the driving force.
  • the patterns are formed as a result of interplay and instability of charges in a polymer melt, image charges in a mask, and hydrodynamic force in the polymer melt. We observed that because the polymer melt thickness is ultra-thin, LISA is not due to the instabilities from the thermal convection
  • the charges in the PMMA film should be uniformly distributed due to a flat surface and symmetry.
  • an image charge will be induced in the mask.
  • the interplay of the charges and the image charges can cause instability and pattern formations.
  • the growth will reduce the distance between the charges and the image charges, hence increasing the strength of the electrostatic force and speeding up the growth.
  • the PMMA pillars reach the mask, forming a full pillar. Once the full PMMA pillars are formed at the corners, the charges and image charges must redistribute.
  • the pillars formed become a boundary for the capillary waves in the PMMA melt surface.
  • the capillary wave a linear wave of amplitude of about one-hundredth of the film thickness (less than 1 nm in our case) will form standing waves set by the boundary.
  • the standing wave peak next to a boundary pillar has an amplitude slightly larger than the rest of the peaks, more charges will be accumulated in that peak and more image charges in the mask area above the peak, making the peak grow into a full pillar.
  • the process will repeat, until all small amplitude capillary peaks under the mask protruding patterns develop into full pillars.
  • the formation of the PMMA pillars starts at the corners, then the edges, and later propagates into the center of the mask protruding pattern.
  • the polymer under the recess areas of the mask is too far away to have an electrostatic force to overcome surface tension to develop into full pillars.
  • the protruding patterns on the mask guide the boundary of the pillar array.
  • the pillar array has a size, shape and period, that are not only different, but smaller than the features on the mask. Such demagnification is technologically significant and could be used repeatedly to achieve even smaller patterns.
  • a suitable set of polymers of desired properties e.g., viscosity, surface tension, etc
  • LISA showed for the first time the role of trapping the three-phase lines by a mask pattern in self-organization of a polymer melt.
  • the LISA process would appear to be applicable to other polymers and materials, especially single phase materials, such as semiconductors, metals, and biological materials.
  • the periodic arrays formed by LISA have many applications, such as memory devices, photonic materials, new biological materials, just to name a few. With a proper design, a single crystal lattice of pillar array with predetermined diameter, period, location, and orientation could be achieved over an entire wafer.
  • LISC lithographically- induced self-construction
  • a mask 235 with a protruded pattern 237 is placed a certain distance above an initially flat polymer 233 that is cast on a substrate 231.
  • the polymer was attracted, against gravitational force and surface tension, to mask protrusions 237, but not to the recess areas of the mask, forming the polymer mesas 249 on their own.
  • the mesas have a lateral dimension substantially identical to the protruded patterns on the mask 235, a height equal to the distance between the mask 235 and the substrate, and a relatively steep sidewall.
  • both the mask and the substrate are made of silicon.
  • the protrusions with a variety of shapes have a height of -300 nm.
  • the polymer is polymethal methalcrylate (PMMA) which was spin- cast on the substrate and was baked at 80°C to drive out the solvent.
  • PMMA polymethal methalcrylate
  • the molecular weight and thickness is typically 2000 and 100 nm, respectively.
  • the gap between the initially flat polymer film and the mask protrusions ranged from 100 to 400 nm, and was controlled by a spacer.
  • the temperature was cycled from room temperature to 170°C.
  • the heat was from the top and bottom of the sample, making the thermal gradient on the sample very small.
  • a press was used to supply the heat and to hold the gap constant.
  • a surfactant with a low surface energy was coated on the mask to facilitate the mask-sample separation after LISC.
  • the materials (for the mask and substrate) and the parameters are not very critical to LISC.
  • LISC can be formed over a wide range of these parameters.
  • the typical diameter of the masks and substrate is larger than 2 cm.
  • the masks are made by photolighography and etching.
  • the temperature was cycled to 175°C.
  • the minimum size of the polymer microstructures formed by LISC is limited by the patterns on the mask.
  • the demagnification effect observed in LISA could be used to form a resist wherein the substrate is etched in the recessed areas of the pattern to thereby form smaller and smaller patterns on masks.
  • Another embodiment of the present invention is self-aligned self-assembly (SALSA) of random access electronic device arrays.
  • SALSA self-aligned self-assembly
  • the conventional approach in fabricating such an array is to fabricate each individual device first, then connect them with word lines and bit lines. As the devices become smaller, the precision alignment between the wires and devices becomes more difficult to fabricate, substantially increasing the fabrication cost.
  • LISA LISA principle, we can first fabricate a word-line array and a bit-line array in two different substrates, and then let the device self-assemble between the word-line and bit-line.
  • Fig. 14 illustrates the applicability of SALSA to Random Access Electronic Devices.
  • a word line assembly is fabricated utilizing a silicon wafer as is known in the art (e.g., by acid etching).
  • bit line is fabricated with a silicon wafer as is known in the art.
  • a thin film or polymer 73 e.g., PMMA
  • the bit line 75 is placed a pre-determined distance above the word line 77 or vice versa, e.g. a distance of less than 1 micron and preferably in the range of about 100 to 400 nm.
  • the temperature is cycled from room temperature to the glass transition temperature of the polymer 73 and then cooled back down, to thereby form a pillar structure at the juncture of each word/bit line.

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  • Manufacturing & Machinery (AREA)
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Abstract

L'invention concerne un procédé et un appareil de lithographie, permettant de créer un micromètre, et plus particulièrement des motifs de sous-micromètre dans une couche mince appliquée sur un substrat. L'invention utilise l'auto-formation de réseaux de colonnettes (49) supramoléculaires périodiques dans un mélange fondu, afin de former des motifs. L'auto-formation est induite par placement d'une plaque ou d'un masque (35) à distance du film polymère. Les colonnettes qui relient la plaque et le masque, présentent une hauteur égale à la distance plaque-masque, et de préférence 2-7 fois celle de l'épaisseur initiale du film. Si la surface du masque possède un motif en saillie, les colonnettes formées sur les bords du réseau de colonnettes sont alignées par rapport à la limite du motif de masque.
PCT/US1999/023717 1998-10-09 1999-10-08 Formation de motifs microscopiques et articles formes WO2000021689A1 (fr)

Priority Applications (5)

Application Number Priority Date Filing Date Title
US09/807,266 US6713238B1 (en) 1998-10-09 1999-10-08 Microscale patterning and articles formed thereby
AU14448/00A AU1444800A (en) 1998-10-09 1999-10-08 Microscale patterning and articles formed thereby
US10/731,818 US7482057B2 (en) 1998-10-09 2003-12-09 Microscale patterning and articles formed thereby
US11/933,170 US8852494B2 (en) 1999-10-08 2007-10-31 Method and apparatus of electrical field assisted imprinting
US12/136,964 US20090084492A1 (en) 1998-10-09 2008-06-11 Microscale patterning and articles formed thereby

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US10379098P 1998-10-09 1998-10-09
US60/103,790 1998-10-09

Related Child Applications (4)

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US09807266 A-371-Of-International 1999-10-08
US09/807,266 A-371-Of-International US6713238B1 (en) 1998-10-09 1999-10-08 Microscale patterning and articles formed thereby
US09/860,037 Continuation US20020042027A1 (en) 1998-10-09 2001-09-24 Microscale patterning and articles formed thereby
US10/731,818 Continuation US7482057B2 (en) 1998-10-09 2003-12-09 Microscale patterning and articles formed thereby

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WO2000021689A1 true WO2000021689A1 (fr) 2000-04-20

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WO2007046110A1 (fr) * 2005-10-19 2007-04-26 Indian Institute Of Technology, Kanpur Procédé et dispositif de traçage de motifs sur des surfaces et assemblage et alignement de leur structure
US7241395B2 (en) 2004-09-21 2007-07-10 Molecular Imprints, Inc. Reverse tone patterning on surfaces having planarity perturbations
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US7252777B2 (en) 2004-09-21 2007-08-07 Molecular Imprints, Inc. Method of forming an in-situ recessed structure
EP1509379A4 (fr) * 2002-05-24 2007-08-08 Stephen Y Chou Procedes et appareil d'empreinte lithographique par pression induite par des champs
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US7309225B2 (en) 2004-08-13 2007-12-18 Molecular Imprints, Inc. Moat system for an imprint lithography template
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US7357876B2 (en) 2004-12-01 2008-04-15 Molecular Imprints, Inc. Eliminating printability of sub-resolution defects in imprint lithography
US7365103B2 (en) 2002-12-12 2008-04-29 Board Of Regents, The University Of Texas System Compositions for dark-field polymerization and method of using the same for imprint lithography processes
US7396475B2 (en) 2003-04-25 2008-07-08 Molecular Imprints, Inc. Method of forming stepped structures employing imprint lithography
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US7547398B2 (en) 2006-04-18 2009-06-16 Molecular Imprints, Inc. Self-aligned process for fabricating imprint templates containing variously etched features
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US7636999B2 (en) 2005-01-31 2009-12-29 Molecular Imprints, Inc. Method of retaining a substrate to a wafer chuck
US7641840B2 (en) 2002-11-13 2010-01-05 Molecular Imprints, Inc. Method for expelling gas positioned between a substrate and a mold
WO2011114018A2 (fr) 2010-03-18 2011-09-22 Centre National De La Recherche Scientifique Procede de formation d'un motif sur une surface d'un support
CN103159164A (zh) * 2013-03-01 2013-06-19 西安交通大学 一种高深宽比微柱阵列的电场诱导压印方法
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US7241395B2 (en) 2004-09-21 2007-07-10 Molecular Imprints, Inc. Reverse tone patterning on surfaces having planarity perturbations
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US7244386B2 (en) 2004-09-27 2007-07-17 Molecular Imprints, Inc. Method of compensating for a volumetric shrinkage of a material disposed upon a substrate to form a substantially planar structure therefrom
US7307118B2 (en) 2004-11-24 2007-12-11 Molecular Imprints, Inc. Composition to reduce adhesion between a conformable region and a mold
US7292326B2 (en) 2004-11-30 2007-11-06 Molecular Imprints, Inc. Interferometric analysis for the manufacture of nano-scale devices
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US7357876B2 (en) 2004-12-01 2008-04-15 Molecular Imprints, Inc. Eliminating printability of sub-resolution defects in imprint lithography
US7635263B2 (en) 2005-01-31 2009-12-22 Molecular Imprints, Inc. Chucking system comprising an array of fluid chambers
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US7256131B2 (en) 2005-07-19 2007-08-14 Molecular Imprints, Inc. Method of controlling the critical dimension of structures formed on a substrate
WO2007046110A1 (fr) * 2005-10-19 2007-04-26 Indian Institute Of Technology, Kanpur Procédé et dispositif de traçage de motifs sur des surfaces et assemblage et alignement de leur structure
US8850980B2 (en) 2006-04-03 2014-10-07 Canon Nanotechnologies, Inc. Tessellated patterns in imprint lithography
US7547398B2 (en) 2006-04-18 2009-06-16 Molecular Imprints, Inc. Self-aligned process for fabricating imprint templates containing variously etched features
WO2011114018A2 (fr) 2010-03-18 2011-09-22 Centre National De La Recherche Scientifique Procede de formation d'un motif sur une surface d'un support
CN103159164A (zh) * 2013-03-01 2013-06-19 西安交通大学 一种高深宽比微柱阵列的电场诱导压印方法
CN105776126A (zh) * 2015-01-14 2016-07-20 韩国科学技术院 用于制造排列成大面积单域的有机分子的柱状或层状结构的方法
WO2016114501A3 (fr) * 2015-01-14 2016-10-20 한국과학기술원 Procédé de préparation d'une structure verticale cylindrique ou lamellaire constituée de molécules organiques agencées en un seul domaine de grande taille
US10457012B2 (en) 2015-01-14 2019-10-29 Korea Advanced Institute Of Science And Technology Method for fabricating columnar or lamellar structures of organic molecules aligned into large-area single domain

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