Marc Papenheim

Flexible composite stamp for thermal nanoimprint lithography based on OrmoStamp

Flexible stamps are common for roll-to-roll processing but less common with planar processing, although they offer a number of benefits as, e.g., an improved conformal contact at reduced pressure. A simple way to realize such a flexible stamp is to use a two layer system with a structured top layer and a flexible backplane. The structured top layer is most easily obtained by molding, the backplane provides the flexibility envisaged. For use in a thermal nanoimprint process, a high thermal stability is required for both. This investigation addresses the preparation of flexible composite stamps with OrmoStamp as the structured top layer and polyimide as the flexible backplane. The process recommended for stamp preparation with OrmoStamp has to be modified to avoid bending after the hard bake that is required after ultraviolet-curing of the material to obtain a high stability of the top layer. Reduction of bending is advised, in particular, for large area stamps, where the hard bake step is in conflict with ...

Guided wrinkling with nanoimprinted SU-8 surfaces

The wrinkling of SU-8 may be useful for microelectromechanical systems and optical applications, but highly regular and periodic wrinkles are the most convenient for such applications. This paper reports wrinkles generated on SU-8 by exposure to 172 nm-wavelength ultraviolet under ozone. To identify the relevant processing parameters, the impact of the SU-8 layer thickness and the effects of the postexposure bake temperature and UV-ozone treatment time are investigated. With 5 μm-thick SU-8 layers, distinct wrinkles are obtained with an ultraviolet-ozone treatment of 3 min and at a postexposure bake temperature of at least 140 °C. To guide the wrinkling, topography is induced on the SU-8 surface via capillary force lithography. By using a stamp with equidistant cavities possessing different widths, the structure size dependence is investigated. Owing to local stress relaxation, single or double wrinkles form along the elevated lines depending upon the line width. Within the gaps between the lines, wrinkle...

Effect of residual stress on replication fidelity with nanoimprint

Relief of residual stress in an imprinted polymer may affect the replication fidelity by leading to recovery. The level of stress induced in the polymer depends on the method of imprint. For example, a “soft” imprint with an elastomeric stamp uses capillary forces to fill the cavities whereas a “hard” imprint with a rigid stamp relies on external pressure. To study the effect of residual stress after imprint, both methods are applied with different imprint times to vary the level of residual stress, as the stress remaining relaxes with imprint time. To visualize the residual stress a temperature treatment is performed after imprint. This temperature treatment allows recovery within a convenient experimental time. A comparison of the shape of the imprinted structures before and after temperature treatment clearly shows that with a hard imprint at short imprint times a considerable amount of stress remains in the polymer, in particular when the residual layer is thin and the imprinted stamp structures are w...

Thermal wrinkling of nanoimprinted SU-8 with masked UV-exposure

When wrinkling can be provided in a controlled way, this has potential for a lot of applications, e.g., in optics or microelectromechanical systems. This paper reports on localized wrinkles generated with an SU-8 layer on silicon; the surface is hardened by a deep-ultraviolet (UV) treatment (172 nm); the size of the wrinkling area is defined by masked UV-exposure. In addition, the SU-8 surface is provided with topography via capillary force lithography beforehand. To identify the interaction between masked UV-exposure and deep-UV treatment several issues are addressed; the size of the wrinkling area, the deep-UV treatment time, and the dose for the masked exposure. Different types of wrinkling are observed, an undulated type, a parallel type, and a zig-zag type. To define a clear wrinkling area an exposure dose of at least 160 mJ/cm2 is advised with a 5 μm-thick SU-8 layer. Then, the wrinkles orient in parallel to the edges of the wrinkling area. The impact of topography on wrinkling within a defined wrin...

Thermal nanoimprint to improve the morphology of MAPbX3 (MA = methylammonium, X = I or Br)

Perovskites have high potential for future electronic devices, in particular, in the field of opto-electronics. However, the electronic and optic properties of these materials highly depend on the morphology and thus on the preparation; in particular, highly crystalline layers with large crystals and without pinholes are required. Here, nanoimprint is used to improve the morphology of such layers in a thermal imprint step. Two types of material are investigated, MAPbI3 and MAPbBr3, with MA being methylammonium, CH3NH3+. The perovskite layers are prepared from solution, and the crystal size of the domains is substantially increased by imprinting them at temperatures of 100–150 °C. Although imprint is performed under atmospheric conditions which, in general, enhances the degradation, the stamp that covers the layer under elevated temperature is able to protect the perovskite largely from decomposition. Comparing imprinting experiments with pure annealing at a similar temperature and time proves this. Furthe...

Flat and highly flexible composite stamps for nanoimprint, their preparation and their limits

To reduce the overall costs, replica stamps have become more and more relevant in the past years. These replicas often are composite stamps with at least two layers, a structured top layer and a backplane. In most cases, the composite stamps are rigid, which limits their use for rolling processes or low-pressure imprints. Flexible composite stamps avoid these limitations. However, due to the flexibility, preparation-induced bending may occur. A concept to avoid such a bending will be introduced and verified by the preparation of a flat and flexible composite stamp consisting of a structured OrmoStamp top layer and a polydimethylsiloxan (PDMS) backplane. To increase the adhesion between both layers, two measures will be adopted: one relies on an increase in the surface energy of the PDMS and the other one on an increase in the interface area. Finally, these flat and highly flexible composite stamps are tested in a critical imprint situation, where particles are dusted to the substrate before imprint. Impri...

Method for high temperature nanoimprint of an organic semicrystalline polymer

Performance and functionality of devices prepared from organic semicrystalline polymers strongly depend on the size and the orientation of the ordered crystalline domains, as the conductivity is distinctly different in the different lattice directions. This investigation addresses the potential of thermal nanoimprint to control the size of the ordered domains as well as their orientation with respect to the substrate. Poly-3-hexylthiophene (P3HT) is chosen as one of the prominent semicrystalline polymers available at high quality. In order to control the ordering of the domains freely, the imprint is performed at a temperature beyond the melting point to eliminate the domains already existing after spin-coating and soft-bake. To avoid a degradation of P3HT at such a high temperature under oxygen contact—the imprint system used operates in air—a novel imprint procedure is employed, where a distinct prepressure is applied already during the heating of the imprint stack (stamp/substrate with P3HT layer). To ...

Resist reflow minimization via viscosity control by exposure

Hybrid lithography is applied to the negative tone resist ma-N 405, successfully combining thermal nanoimprint lithography (to define submicron patterns) with conventional photolithography (for micrometer-pattern definition). When employing such a hybrid technology scheme, one often finds it difficult to achieve a good pattern fidelity in the overlapping areas due to uneven exposure relating to the formation of standing waves during exposure. To avoid such standing waves, one has to infer an antireflective layer. Alternatively, one can make a short heat treatment. Such a heat treatment levels the uneven exposure but may lead to a reflow of the preimprinted pattern. In order to minimize reflow during this postexposure bake, flood exposure is integrated into the processing sequence whereby the dose required must be optimized. The results show that with an adequate choice of dose for flood exposure and masked exposure, the reflow can be avoided, and the standing waves are reduced to an acceptable state. Part...

Sputtering with an etch-free lift-off in thermal nanoimprint lithography

Two low-cost techniques suitable for large area processing are combined to define submicrometer metal structures, thermal nanoimprint lithography, and sputtering. With very low residual layers after thermal nanoimprint, as obtained under partial cavity filling conditions, it is possible to skip the etching step for residual layer removal before sputtering. As imprinted structures typically feature a positive sidewall angle, the authors investigate the morphology of sputtered layers on sloped sidewalls. Independent from inclination, the sputtered layers exhibit a columnar structure with only a slight taper, where the crystallites extend perpendicular to the substrate through the whole layer thickness. This structure allows penetration of the solvent, swelling of the polymer, and lifting of the top layer as long as the adhesion to the substrate within the contact area is sufficiently high, thus enabling successful lift-off.

Low reflection Fresnel lenses via double imprint combined with vacuum-UV surface hardening

To improve the optical performance of Fresnel lenses, a technique for preparing them with antireflective structures of the moth-eye type is developed. Masters featuring such hierarchical structures are prepared in SU-8, a negative tone photoresist, by two consecutive thermal imprint steps. The moth-eye structures imprinted first are vacuum ultraviolet-treated at 172 nm to provide a surface-near the cross-linked layer that remains stable during the second imprint of the 100 μm sized Fresnel structures. A successful combination of both structure types is possible at an imprint temperature as low as 45 °C. This can be understood on the basis of the typical exposure and the crosslinking behavior of a chemically amplified negative tone resist like SU-8. The masters prepared in this way will be subjected to extrusion coating, the process of choice for future large area preparation of such structures in a single step.To improve the optical performance of Fresnel lenses, a technique for preparing them with antireflective structures of the moth-eye type is developed. Masters featuring such hierarchical structures are prepared in SU-8, a negative tone photoresist, by two consecutive thermal imprint steps. The moth-eye structures imprinted first are vacuum ultraviolet-treated at 172 nm to provide a surface-near the cross-linked layer that remains stable during the second imprint of the 100 μm sized Fresnel structures. A successful combination of both structure types is possible at an imprint temperature as low as 45 °C. This can be understood on the basis of the typical exposure and the crosslinking behavior of a chemically amplified negative tone resist like SU-8. The masters prepared in this way will be subjected to extrusion coating, the process of choice for future large area preparation of such structures in a single step.