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(Color online) Schematic of various nanofabrication processes using holographic nanopatterns. (a) The top photoresist (PR) is patterned by laser interference lithography. (b) The intermediate antireflective coating (ARC) layer is patterned by RIE. (c) A metal film (e.g., Cr) is deposited (e.g., by e-beam evaporation). (d) and (e) The metal/PR/ARC trilayer is released from the silicon substrate. (f) Silicon nanopillar structures are fabricated by DRIE, where the metal structures are used as etch mask. (g) The metal/PR/ARC trilayer is transferred on a new silicon substrate. (h) Silicon nanohole structures are fabricated by DRIE, where the trilayer is used as etch mask and then released again for repetitive processes. (i) The metal/PR/ARC trilayer is transferred on a new polydimethylsiloxane (PDMS) substrate and used as deposition mask for a metal (e.g., gold). (j) After the deposition of gold (Au), the trilayer is released again for repetitive processes.

(Color online) Schematic of various nanofabrication processes using holographic nanopatterns. (a) The top photoresist (PR) is patterned by laser interference lithography. (b) The intermediate antireflective coating (ARC) layer is patterned by RIE. (c) A metal film (e.g., Cr) is deposited (e.g., by e-beam evaporation). (d) and (e) The metal/PR/ARC trilayer is released from the silicon substrate. (f) Silicon nanopillar structures are fabricated by DRIE, where the metal structures are used as etch mask. (g) The metal/PR/ARC trilayer is transferred on a new silicon substrate. (h) Silicon nanohole structures are fabricated by DRIE, where the trilayer is used as etch mask and then released again for repetitive processes. (i) The metal/PR/ARC trilayer is transferred on a new polydimethylsiloxane (PDMS) substrate and used as deposition mask for a metal (e.g., gold). (j) After the deposition of gold (Au), the trilayer is released again for repetitive processes.

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In this article, the authors report a new lift-off process to obtain nanoporous free-standing trilayer film of metal/photoresist/antireflective coating (ARC) stack and to reuse the thin and flexible membrane as a versatile stencil lithography mask for the dual purposes. For the initial lift-off process of metal nanostructures, nanoperiodic pore pat...

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... advan- tages and potential applications of such an advanced nanofab- rication processes are also discussed in this paper. Figure 1 shows the overall fabrication schemes of the pro- posed lift-off process and the new applications of the free- standing PR membrane to the stencil lithography for both etching and deposition processes. First [ Fig. 1(a)], large-area (wafer-scale) periodic nanopore patterns are created on a PR film by using a laser interference lithography. ...
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... The advan- tages and potential applications of such an advanced nanofab- rication processes are also discussed in this paper. Figure 1 shows the overall fabrication schemes of the pro- posed lift-off process and the new applications of the free- standing PR membrane to the stencil lithography for both etching and deposition processes. First [ Fig. 1(a)], large-area (wafer-scale) periodic nanopore patterns are created on a PR film by using a laser interference lithography. Between the PR film and silicon substrate, an antireflective coating (ARC) is interlayered to minimize the vertical standing wave effects along the sidewall of the registered PR nanostructures. In order to make ...
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... laser interference lithography. Between the PR film and silicon substrate, an antireflective coating (ARC) is interlayered to minimize the vertical standing wave effects along the sidewall of the registered PR nanostructures. In order to make through-holes of the PR/ ARC bilayer, the opened ARC layer is also etched by reactive ion etching (RIE) [ Fig. 1(b)]. Similar to traditional lift-off process, a metal film (e.g., Cr) is deposited through the bilayer pore patterns [ Fig. 1(c)]. However, instead of remov- ing the metal/PR/ARC trilayer after the metal deposition, the trilayer composite film is just released as a free-standing membrane from the silicon substrate by using specially ...
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... minimize the vertical standing wave effects along the sidewall of the registered PR nanostructures. In order to make through-holes of the PR/ ARC bilayer, the opened ARC layer is also etched by reactive ion etching (RIE) [ Fig. 1(b)]. Similar to traditional lift-off process, a metal film (e.g., Cr) is deposited through the bilayer pore patterns [ Fig. 1(c)]. However, instead of remov- ing the metal/PR/ARC trilayer after the metal deposition, the trilayer composite film is just released as a free-standing membrane from the silicon substrate by using specially designed chemical solution (NH 3 /H 2 O 2 /H 2 O) [ Fig. 1(d)]. The chemical only helps the physical release process of the film by ...
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... a metal film (e.g., Cr) is deposited through the bilayer pore patterns [ Fig. 1(c)]. However, instead of remov- ing the metal/PR/ARC trilayer after the metal deposition, the trilayer composite film is just released as a free-standing membrane from the silicon substrate by using specially designed chemical solution (NH 3 /H 2 O 2 /H 2 O) [ Fig. 1(d)]. The chemical only helps the physical release process of the film by generating air bubbles between the ARC layer and silicon substrate with the aid of etching silicon in a slow rate. 13,14 After the complete separation of the trilayer film, we obtain only metal nanostructures on the silicon substrate [ Fig. 1(e)]. Such metal ...
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... (NH 3 /H 2 O 2 /H 2 O) [ Fig. 1(d)]. The chemical only helps the physical release process of the film by generating air bubbles between the ARC layer and silicon substrate with the aid of etching silicon in a slow rate. 13,14 After the complete separation of the trilayer film, we obtain only metal nanostructures on the silicon substrate [ Fig. 1(e)]. Such metal nanostructures (e.g., Cr) can further be used as robust etch mask in the deep reactive ion etching (DRIE) of the silicon, allowing to obtaining high-aspect-ratio silicon nanopillar structures [ Fig. 1(f)]. Meanwhile, the free-standing trilayer membrane can be transferred onto a new silicon substrate, where the flexible ...
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... slow rate. 13,14 After the complete separation of the trilayer film, we obtain only metal nanostructures on the silicon substrate [ Fig. 1(e)]. Such metal nanostructures (e.g., Cr) can further be used as robust etch mask in the deep reactive ion etching (DRIE) of the silicon, allowing to obtaining high-aspect-ratio silicon nanopillar structures [ Fig. 1(f)]. Meanwhile, the free-standing trilayer membrane can be transferred onto a new silicon substrate, where the flexible membrane is directly placed on the new substrate without using any spacers between them [ Fig. 1(g)]. Then, the conformable contact between the trans- ferred membrane and the new substrate can allow new etching ...
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... in the deep reactive ion etching (DRIE) of the silicon, allowing to obtaining high-aspect-ratio silicon nanopillar structures [ Fig. 1(f)]. Meanwhile, the free-standing trilayer membrane can be transferred onto a new silicon substrate, where the flexible membrane is directly placed on the new substrate without using any spacers between them [ Fig. 1(g)]. Then, the conformable contact between the trans- ferred membrane and the new substrate can allow new etching capability, which is not effective in typical stencil lithography using spacers, using the trilayer nanoporous membrane as a new etch mask. Then, it will result in nanohole structures [ Fig. 1(h)], instead of nanopillar ...
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... without using any spacers between them [ Fig. 1(g)]. Then, the conformable contact between the trans- ferred membrane and the new substrate can allow new etching capability, which is not effective in typical stencil lithography using spacers, using the trilayer nanoporous membrane as a new etch mask. Then, it will result in nanohole structures [ Fig. 1(h)], instead of nanopillar structures obtainable from the lift-off process [ Fig. 1(f)]. It suggests that just by perform- ing single holographic nanopatterning, we can obtain both nanopillar-and nanohole-type structures at the same time con- veniently. The trilayer membrane can also be released again from the new silicon substrate by ...
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... between the trans- ferred membrane and the new substrate can allow new etching capability, which is not effective in typical stencil lithography using spacers, using the trilayer nanoporous membrane as a new etch mask. Then, it will result in nanohole structures [ Fig. 1(h)], instead of nanopillar structures obtainable from the lift-off process [ Fig. 1(f)]. It suggests that just by perform- ing single holographic nanopatterning, we can obtain both nanopillar-and nanohole-type structures at the same time con- veniently. The trilayer membrane can also be released again from the new silicon substrate by using the same chemical solution (NH 3 /H 2 O 2 /H 2 O) and reused multiple times. In ...
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... at the same time con- veniently. The trilayer membrane can also be released again from the new silicon substrate by using the same chemical solution (NH 3 /H 2 O 2 /H 2 O) and reused multiple times. In addi- tion to silicon substrates, the thin flexible trilayer membrane can also be transferred to many other substrate materials, such as PDMS [ Fig. 1(i)] where the direct lithography with photo- resist material is not effective as discussed earlier. Then, various nanostructures can also be effectively defined on the PDMS substrate through the nanoporous membrane, e.g., dep- osition of metals [ Fig. 1(j)]. The trilayer can also be released by using the detaching solution (NH 3 /H 2 O 2 ...
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... trilayer membrane can also be transferred to many other substrate materials, such as PDMS [ Fig. 1(i)] where the direct lithography with photo- resist material is not effective as discussed earlier. Then, various nanostructures can also be effectively defined on the PDMS substrate through the nanoporous membrane, e.g., dep- osition of metals [ Fig. 1(j)]. The trilayer can also be released by using the detaching solution (NH 3 /H 2 O 2 /H 2 O) and reused for many ...
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... the deposition of metal (Cr) layer on a silicon sub- strate [ Fig. 1(c)], a 50-70 nm thick Cr layer was deposited by using e-beam evaporation (PVD 75, Kurt Lesker, Inc.). The deposition rate was controlled to be less than 0.2 nm/s. During deposition, the pressure of the chamber was main- tained below 10 À5 mTorr to ensure uniform deposition. The same e-beam evaporation process was also applied for the ...
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... Inc.). The deposition rate was controlled to be less than 0.2 nm/s. During deposition, the pressure of the chamber was main- tained below 10 À5 mTorr to ensure uniform deposition. The same e-beam evaporation process was also applied for the deposition of a metal (Au) layer on the new PDMS substrate through the Cr/PR/ARC trilayer transferred [ Fig. 1(i)]. The aspect ratio of the gold nanopillar structures on the PDMS substrate [ Fig. 1(j)] was controlled by changing the deposi- tion time. In this experiment, two different thicknesses of the gold layers, 200 nm and 500 nm, were ...
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... the pressure of the chamber was main- tained below 10 À5 mTorr to ensure uniform deposition. The same e-beam evaporation process was also applied for the deposition of a metal (Au) layer on the new PDMS substrate through the Cr/PR/ARC trilayer transferred [ Fig. 1(i)]. The aspect ratio of the gold nanopillar structures on the PDMS substrate [ Fig. 1(j)] was controlled by changing the deposi- tion time. In this experiment, two different thicknesses of the gold layers, 200 nm and 500 nm, were ...
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... the release of the metal/PR/ARC trilayer film as a free-standing membrane from the substrate [ Fig. 1(d)], cus- tomized solution of NH 3 /H 2 O 2 /H 2 O mixture was prepared and the sample was directly immersed into the solution. The ratio of each chemical was characterized to make sure the bottom ARC layer could be separated from the silicon wafer effectively without fracturing. 13,14 The lift-off process was largely affected by the ...
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... the transfer of the free-standing membrane onto a new substrate [Figs. 1(g) and 1(i)], a new substrate (silicon or PDMS in this experiment) was also immersed into the solution to be placed underneath the trilayer film. Then, the solution was gradually drained out from the container until the trilayer membrane became contacted and spread out on the new substrate. In order to facilitate conformable and good bonding ...
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... and spread out on the new substrate. In order to facilitate conformable and good bonding between the transferred trilayer membrane and the new substrates, the sample was degassed in vacuum for several hours. The same release and transfer methods were applied to the trilayer membranes even after the DRIE etching on the new silicon substrate [ Fig. 1(h)] or the metal deposition on the new PDMS substrate [ Fig. ...
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... conformable and good bonding between the transferred trilayer membrane and the new substrates, the sample was degassed in vacuum for several hours. The same release and transfer methods were applied to the trilayer membranes even after the DRIE etching on the new silicon substrate [ Fig. 1(h)] or the metal deposition on the new PDMS substrate [ Fig. ...
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... compared to the Bosch process that normally results in scalloping sidewall profiles. 19 Due to the very high etch selectivity of the silicon material to metal (e.g., Cr), the degradation or the thinning of the trilayer membrane was not significant. Figures 2(a)-2(c) show the experimental results corre- sponding to the schematics illustrated in Figs. 1(a)-1(c), respectively. Figure 2(a) shows the square array (935 nm in periodicity) of nanopore patterns (pore size of $500 nm) of the negative PR layer (1.5 lm thick) created by using laser interference lithography. Although not shown here, the pore size can be regulated by adjusting the exposure conditions in the lithographic process. 15 ...
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... ARC interlayer. The size of the Cr nanostructures deposited on the bottom surface was $600 nm in diameter, which was slightly smaller than the pore size of the PR/ARC membrane ($650 nm in diameter). Figure 3 shows the Cr/PR/ARC trilayer released from the specially designed wet solution (NH 3 /H 2 O 2 /H 2 O), corre- sponding to the schematic of Fig. 1(d). NH 3 in the solution was designed to slowly etch the silicon and separate the ARC layer from the substrate. 14 In the meantime, H 2 O 2 generates gas bubbles not only in the bulk solution but also at the inter- face between the ARC layer and the silicon substrate. The gas bubbles help to separate and lift up the trilayer membrane from ...
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... process. It further shows that the thin trilayer membrane is mechanically flexible so that no cracks or fracture is shown on the surface even being bent or rolled. Figure 4(a) shows the Cr nanodot patterns ($600 nm in diameter) retained on the silicon substrate after the separation of the Cr/PR/ARC trilayer, corresponding to the schematic of Fig. 1(e). It shows that the release process using the wet chemical does not delaminate or deform the Cr layer depos- ited on the silicon substrate. Such a well-defined metal layer is useful as a robust etch mask layer, especially in plasma- based dry etching such as DRIE. Figure 4(b) shows the result of DRIE of the silicon substrate by using ...
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... not delaminate or deform the Cr layer depos- ited on the silicon substrate. Such a well-defined metal layer is useful as a robust etch mask layer, especially in plasma- based dry etching such as DRIE. Figure 4(b) shows the result of DRIE of the silicon substrate by using the thin Cr layer ($70 nm) as etch mask, corresponding to the schematic of Fig. 1(f). It shows the silicon nanopillar structures of $1 lm tall. On top of the silicon structures, a thin Cr cap layer is still observable, which indicates the high etch selectivity of the metal layer against the silicon material. Figure 5(a) shows the free-standing Cr/PR/ARC trilayer membrane after being released and then transferred onto a ...
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... $1 lm tall. On top of the silicon structures, a thin Cr cap layer is still observable, which indicates the high etch selectivity of the metal layer against the silicon material. Figure 5(a) shows the free-standing Cr/PR/ARC trilayer membrane after being released and then transferred onto a new silicon substrate, corresponding to the schematic of Fig. 1(g). It shows uniform contact of the transferred membrane onto the new silicon substrate with no fracture or wrinkles. In order to obtain the conformable contact, it was found that the degassing step was critical after physically transferring the free-standing membrane onto the new substrate. Such degassing process helps to remove the gas ...
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... of the PR nanostructures, which resulted in the larger pore dimension in the lower region of the film that directly con- tacted with the silicon substrate. Despite the slight deviation of the fabricated pore sizes compared to that of the stencil membrane, it shows that silicon nanohole structures are uni- formly fabricated, as illustrated in Fig. 1(h). It demonstrates that by using one same stencil, we can obtain both nanopillar patterns [ Fig. 4(b)] and nanohole patterns [ Fig. 5(b)]. It was enabled by the novel reuse of the holographic nanopatterns as a free-standing membrane for both the lift-off and the stencil lithography applications. Although stencil lithography has been ...
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... damage. When used more times, it was observed that the flexibility of the trilayer mem- brane was degraded, often resulting in the fracture of the membrane into pieces in the release/transfer process. Figure 6 shows the free-standing Cr/PR/ARC trilayer membrane (3 cm  3 cm) transferred onto a PDMS substrate, corresponding to the schematic of Fig. 1(i). Figure 6(a) reveals that the transferred trilayer membrane of a large area does not show significant delamination and cracks even when the PDMS substrate is bent or twisted. It demonstrates another advantage of the use of flexible stencil, compared to hard and rigid stencils that were typically used in conven- tional stencil ...
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... trilayer mem- brane and the PDMS substrate. It was also made possible by applying the degassing process of the sample in vacuum, which helps to remove any entrapped gas at the interface. Figure 7 shows the deposition result of a gold layer through the transferred trilayer membrane on the PDMS substrate, corresponding to the schematics of Fig. 1(j). The trilayer membrane was released again from the PDMS sub- strate after the deposition of the gold film by using the same chemical method (NH 3 /H 2 O 2 /H 2 O) used for the silicon sub- strate. In comparison to the release from the silicon substrate, the time required for the release of the trilayer membrane from the PDMS substrate ...

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Hierarchical nanostructures are typically fabricated with multiple lithography steps on prepatterned micro- or nanostructures. However, such conventional multiple lithography steps result in poor coverage and uniformity, especially when patterning on high-aspect-ratio micro- or nanostructures. In this work, the authors present a new fabrication method which can make hierarchical nanostructures even on high-aspect-ratio prepatterns, using a free-standing trilayer membrane. The nanoporous trilayer composite films, consisting of metal/photoresist/antireflective coating, is created on a planar silicon substrate by using laser interference lithography, reactive ion etching, and e-beam deposition. Then, a customized solution of ammonia (NH3), hydrogen peroxide (H2O2), and water (H2O) is used to release the composite film from the supporting substrate. The free-standing composite membrane is then transferred on a prepatterned silicon substrate. Showing no major defects on the membrane surface, the flexible and soft trilayer membrane allows a good, uniform contact with the top surface of the prepatterns and is utilized as a robust etch mask in the deep reactive ion etching (DRIE) process of silicon to fabricate hierarchical nanopore structures. Since the membrane covers the top surfaces of the prepatterns seamlessly, the nanopore patterns of the membrane are transferred onto the top surfaces with great fidelity during the etching process. The membrane can also be used as a stencil for deposition processes. For example, metal is deposited through the nanoporous membrane by a lift-off process. Then, the transferred metal nanodot patterns are used as an etch mask in the DRIE process to achieve high-aspect-ratio hierarchical nanopillar structures. Compared to conventional methods to fabricate hierarchical nanostructure, the introduced new approach is more reliable and versatile to realize large-area hierarchical nanostructures with a- good uniformity, in both nanopore and nanopillar array by using the same single membrane.
... A variant of this technique uses epoxy to bond the metal layer directly to a glass carrier [13]. Alternatively, the metal plus photoresist pattern can be further transferred into the underlying antireflection layer using RIE and then peeled off the wafer, producing a thin, flexible perforated stencil which may then be placed on another surface or substrate as a mask for etching or deposition [20]. ...
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The non-uniform intensity profile of Gaussian-like laser beams used in interference lithography (IL) leads to a non-uniform dose and feature size distribution across the sample. Previously described methods to improve dose uniformity are reviewed. However, here we examine the behavior of the non-uniformity from the viewpoint of photoresist response rather than the IL system configuration. Samples with a fixed intra-sample dose profile were exposed with an increasing average dose. A line/space pattern with a period of 240 nm across an area of 2 × 2 cm(2) was produced using IL on identical samples using a HeCd laser operated at 325 nm and a Lloyd's mirror IL system. A binary model of photoresist response predicts that the absolute range of line widths in nanometers should be significantly reduced as the overall sample dose is increased. We have experimentally verified a reduction in the range of line widths within a given sample from 50 to 16 nm as the overall dose is increased by only 60%. This resulted in a drop in the narrowest line width from 120 to 65 nm. An etch process is demonstrated to increase the line width by generating a wider secondary chrome hard mask from the narrowly patterned primary chrome hard mask. The subsequent fabrication of a silicon nanoimprint mold is used as a demonstration of the technique.