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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 陳學禮 | |
dc.contributor.author | Kun-Che Hsieh | en |
dc.contributor.author | 謝坤哲 | zh_TW |
dc.date.accessioned | 2021-06-15T00:14:48Z | - |
dc.date.available | 2010-06-30 | |
dc.date.copyright | 2009-06-30 | |
dc.date.issued | 2009 | |
dc.date.submitted | 2009-06-24 | |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/41250 | - |
dc.description.abstract | 在本論文中,藉由奈米壓印、轉印、奈米球模板技術等先進微影技術在功能性材料,包括鐵電材料,奈米金屬粒子,奈米碳管中製作奈米結構或圖案,並探討其表面電漿共振與繞射之光學特性。
在鐵電材料中,利用簡單的化學合成方式,製備了含有奈米金粒子之鋯鈦酸鉛複合薄膜並使其誘發表面電漿共振現象。隨著燒結溫度的增加使奈米金粒子的大小增加,進而使表面電漿共振波長產生紅移。另一方面,利用奈米壓印的方式,可以直接壓印於金/鋯鈦酸鉛之雙層結構上,成功地製備週期性圖案並觀察到表面電漿共振的發生。此外,亦探討高吸收奈米結構材料,奈米碳管,其特殊結構所造成的光學行為。利用大角度入射的TE和TM的偏振光之反射光譜,來獲得垂直排列奈米碳管薄膜在該入射角時之等效非均向性光學常數。進一步,應用奈米球模板技術及奈米轉印技術等等技術,在可撓曲的基板上製備出不同圖案,例如光柵,六角形,花椰菜排列的奈米碳管薄膜。儘管奈米碳管會將入射光侷限於其中,而且與空氣的折射率對比很低,但經由圖案化後的奈米碳管,依舊可以觀察彩色影像。圖案化後的奈米碳管,其光學性質亦符合週期性結構之繞射現象。 之後更進一步,利用各種不同的方式,如外加電場或形變(彎曲)的方式,來調變各種不同的奈米結構材料所引發之特殊光波長。當施予外加電場於含金粒子之鋯鈦酸鉛複合薄膜時,鋯鈦酸鉛薄膜之折射率會隨之改變,進而造成表面電漿共振波長的偏移。另一方面,奈米圖案化之鋯鈦酸鉛/金/鋯鈦酸鉛多層結構,可以藉由外加電場來控制週期性圖案的週期與鋯鈦酸鉛薄膜的折射率,進而達到雙向調變表面電漿共振波長的元件。而利用彎曲的方式亦可以使得週期性圖案的週期改變,因而使得圖案化後的奈米碳管薄膜其繞射波長改變。因此,繞射之光學波長可以藉由彎曲的形式,如凸面或凹面,曲率半徑的大小,來進行動態的調變。 | zh_TW |
dc.description.abstract | In this thesis, the advanced lithography technology of nanoimprint, reversal nanoimprint and nanoshpere lithography are applied to fabricate patterns on functional materials, including ferroelectric materials, metal nanoparticles and carbon nanotubes (CNTs). The optical characteristics of surface plasmon resonance (SPR) and diffraction in these nanostructured materials are studied.
First, with chemical reduction method, I prepared gold nanoparticle-embedded lead zirconate titanate (PZT) films to study its surface plasmon resonance phenomenon. As the sintering temperature increases, the size of gold nanoparticles is increased thus induce red shifts of SPR wavelength. Second, I successfully obtain a periodical pattern using nanoimprint the gold/PZT bilayer structure. Third, I also discuss the optical characteristics of high absorbed CNTs. Using the reflectance spectra of TE and TM polarized light measured at different incident angles, I can obtain the equivalent anisotropic optical constants of a vertical-aligned carbon nanotubes (VA-CNT) thin film. Furthermore, using nanosphere lithography and reversal nanoimprint techniques, I can fabricate various patterns on CNT thin films, such as gratings, hexagonal holes and broccoli like arrays. Despite the light could be trapped in the CNT forest and the low refractive index contrast between air and a CNT film is low, iridescence phenomenon can be observed in patterned CNTs samples. For the tuning wavelength study, I use two kinds of method, applying electric field or bending flexible substrates, to modulate the SPR or diffraction wavelength induced from the structured materials mentioned previously. When an electric field is applied on gold nanoparticle-embedded PZT films, the refractive index of PZT is changed that induce the shifting of SPR wavelength. On the other hand, in the patterned PZT/gold/ PZT multilayer structures, I can control both the period of the gold/ PZT patterns and the refractive index of the PZT layer. Thus I can obtain a bi-directionally tunable SPR device. By bending the flexible substrates, I demonstrated the period and diffraction wavelength changed in the flexible samples coated with patterned CNTs. The diffraction wavelength can be dynamically modulated depending on the radius of curvature, as well as the type of convex or concave bending. | en |
dc.description.provenance | Made available in DSpace on 2021-06-15T00:14:48Z (GMT). No. of bitstreams: 1 ntu-98-D91527010-1.pdf: 10349983 bytes, checksum: cd5a2247481f82277ee5b8f89cac93df (MD5) Previous issue date: 2009 | en |
dc.description.tableofcontents | Acknowledgements.......................................................................................i
Abstract……………………………………........……………………..…...v Contents……………………………………...........………………....….....ix Table list…………………………..……………........……………..……xiii Figure list………………………………………..........…………..……….xv Chapter I Introduction…………..............……………………………….1 1.1 Research background…………..…………….....………………………..1 1.2 Motivation………………………………………………………………3 1.3 Thesis organization……………………………………………………..6 Chapter II Literature review………............…………………………….9 2.1 Lithography technology…………………………………………………9 2.1.1 Traditional lithography…………………………………………9 2.1.2 Advanced lithography…………………………………......….10 2.1.2.1 Nanoimprint lithography (NIL)………………….……..11 2.1.2.2 Reversed imprint lithography (RIL)………………….13 2.1.2.3 Nanosphere lithography (NSL)………………………...15 2.2 Materials………………………………………………………………..17 2.2.1 Metal nanoparticles (NPs)……………………………………...17 2.2.2 Ferroelectric materials…............................…………………….22 2.2.3 Carbon nanotubes (CNTs)……………………………………...30 2.3 Optical phenomena……………………………………………………..40 2.3.1 Surface plasmon resonance (SPR)…………….………………..40 2.3.2 Diffraction light………………………………………………...45 2.3.3 Tunable wavelength……………………………………………48 Chapter III Experiments............................................................................73 3.1 Nanocomposite materials........................................................................73 3.2 Nanopatterning gold/ferroelectric structures...........................................76 3.3 Nanopatterning CNT structures...............................................................78 3.3.1 Vertical-aligned CNT (VA-CNT) films......................................78 3.3.2 Patterned VA-CNT films.............................................................79 3.3.3 Broccoli CNTs.............................................................................79 Chapter IV Optical properties and materials characterization of nanostructured materials.........................................................87 4.1 Nanocomposite materials........................................................................87 4.2 Nanopatterning gold/ferroelectric structures...........................................91 4.3 Nanopatterning CNT structures...............................................................97 4.3.1 Vertical-aligned CNT (VA-CNT) films......................................97 4.3.2 Patterned VA-CNT films...........................................................105 4.3.3 Broccoli CNTs...........................................................................110 Chapter V Tuning wavelength in nanostructured materials.................145 5.1 Nanocomposite materials......................................................................145 5.2 Nanopatterning gold/ferroelectric structures.........................................150 5.3 Nanopatterning CNT structures.............................................................155 Chapter VI Conclusions and future work................................................173 6.1 Conclusions......................................................................173 6.2 Future work...........................................................................................177 List of Publications....................................................................................179 Journal paper.....................................................................................................179 Conference paper...............................................................................................180 On-line News.....................................................................................................181 Reference...................................................................................................183 Table list Table 5-1 Measured and simulated SPR absorption signals at various external electric fields, incorporating the measured refractive indices of the surrounding PZT.............................................................................................................160 Table 5-2 Measured and simulated refractive indices of PZT media at various external electric fields, incorporating the SPR absorption signals...........................160 Figure list Figure 2-1 Lithography exposure tool potential solutions...........................................53 Figure 2-2 Schematic diagrams of imprint technologies (a) conventional nanoimprint lithography (b) direct imprint on a metal film............................................53 Figure 2-3 Thermal NIL pattern transfer process to metal: (1) NIL mold was separated from imprint polymer. (2) An oxygen plasma anisotropically etched the polymer to remove the residue polymer and expose the substrate surface. (3) Metal was evaporated over the sample surface. (4) Patterned polymer was dissolved in solvent, leaving the sample surface with a patterned metal film mirroring the pattern on the mold..................54 Figure 2-4 Schematic illustrations of the pattern transfer processes in (a)conventional nanoimprinting, (b) reversal imprinting at temperatures well above Tg, (c) “inking” at temperatures around Tg with nonplanarized mold, and (d) ”whole-layer transfer” around Tg with planarized mold.......................54 Figure 2-5 Schematic two routes to achieve arrays of different nanostructures. (a) Substrate with patterned cylindrical pillars. (b) Substrate with patterned prismatic pillars. EBE: Electron beam evaporation; RIE: reactive ion etching........................................................................................................55 Figure 2-6 Schematic of plasmon oscillation for a sphere, showing the displacement of the conduction electron charge cloud relative to the nuclei...................55 Figure 2-7 Exact electrodynamic calculation of the extinction spectra of oblate spheroids, all with the same equivalent volume, corresponding to a sphere radius of 80 nm. The major to minor axis ratio, r, is from left to right: 10, 5, 3.33, 2.5, 2, 1.67, 1.43, 1.25, 1.11, and 1...................................................56 Figure 2-8 Schematics of the piezoelectric effect: (a) bulk after polarization (poling); the direct piezoelectric effect: (b) bulk compressed: generated voltage has same polarity as poling voltage; (c) bulk stretched: generated voltage has polarity opposite that of poling voltage. The converse piezoelectric effect: (d) applied voltage has same polarity as poling voltage: bulk lengthens; (e) applied voltage has polarity opposite that of poling voltage: bulk shortens.......................................................................................................57 Figure 2-9 Phase stabilities in the system Pb(Zrx,Ti1-x)O3...........................................58 Figure 2-10 Coupling coefficient kp and permittivity εr values across the PZT compositional range...................................................................................58 Figure 2-11 A principal section of the wavefront surfaces for a uniaxial crystal; the dots on SO represent the E vectors which are normal to the plane of the paper...........................................................................................................59 Figure 2-12 Non-linearity in the D versus E relationship..............................................59 Figure 2-13 (a) Arrangement for optical shutter; (b) detail of the electroding configuration..............................................................................................59 Figure 2-14 Principle of the PZT reflective display......................................................60 Figure 2-15 Total internal reflection thin-film optical switches....................................60 Figure 2-16 Typical carbon nanotube structures. (a) Schematic representations of a single-walled carbon nanotube (SWNT), a multiwalled carbon nanotube (MWNT) and a bundle of SWNTs. (b) Conceptually, a SWNT is formed by rolling up graphene along a chiral vector to form a cylinder. (c) Schematic representation of two SWNTs with nearly identical diameters but different chiral indices. (d) Schematic representation of two SWNTs with identical chiral vectors but different chiral handedness.....................61 Figure 2-17 A schematic of arc-discharge setup............................................................62 Figure 2-18 The schematic experiment of laser ablation method..................................62 Figure 2-19 A schematic experimental setup for chemical vapor deposition (CVD) growth.........................................................................................................63 Figure 2-20 Schematics of (a) base-growth and (b) tip-growth mechanisms for carbon filament growth..........................................................................................63 Figure 2-21 Dielectric functions of the nanotube films as determined by ellipsometry................................................................................................64 Figure 2-22 The optical anisotropy of vertically aligned SWNTs grown on quartz substrate. The 488 nm s-polarized (left) and p-polarized (right) light was used. The solid curves represent theoretical transmittances for s- and p-polarizations calculated from the classical electromagnetic formula using the refractive index of glass to be 1.5.........................................................64 Figure 2-23 Reflectance measurements of the s- and p-polarized components of two CNT samples with different degrees of alignment.....................................65 Figure 2-24 (a) Scanning electron micrograph (SEM) of a VA-CNT sample. (b) A side-view SEM image of the same sample at a higher magnification. (c) A top-view SEM image of the sample. (d) A transmission electron micrograph of the sample. (e) A photograph of a 1.4% reflectance standard, a CNT sample, and a piece of glassy carbon, taken under a flash light illumination................................................................................................66 Figure 2-25 Demonstration field emission light source using carbon nanotubes as the cathodes......................................................................................................67 Figure 2-26 (a) Pixels are formed as the intersection of cathode and anode stripes. (b) A prototype field emission display fabricated by Samsung using carbon nanotubes....................................................................................................67 Figure 2-27 The mechanical properties of MWNT-polymer (epoxy) composites........68 Figure 2-28 Flexible transparent coating of CNTs on a Polyester foil (left: slightly bent, right: same sample heavily crumpled).......................................................68 Figure 2-29 The interaction between the surface charges and the electromagnetic field.............................................................................................................69 Figure 2-30 (a) ATR coupler or prism coupler and (b) Its optical behavior..................69 Figure 2-31 Configuration of the ATR method. (a) The air lies between the prism and the metal surface, Otto configuration. (b) The metal contact the prism and couples the SPs with the evanescent fields of the totally reflected light wave, Kretschmann-Raether configurations..............................................70 Figure 2-32 Geometry of hexagonal two-dimensional scanering array. Here α = 60o............................................................................................................70 Figure 2-33 Schematic illustrating the approach to electric-field-induced tuning of the rejection wavelength of PBG composites: (a) Upper and lower compliant electrodes are attached to a 80 μm thick composite. b) The electrodes are energized with a direct-current (DC) voltage (typical range: 0.5-3 kV) resulting in a biaxial stretching of the composite in the x-y plane of the electrodes and a contraction perpendicular to the plane (z-direction)........71 Figure 2-34 Reflectance characteristics at normal incidence of (a) an unbiased PBG composite under increasing electric-field strength up to an electric field with magnitude of 25 V μm-1; (b) variation in the rejection wavelength and corresponding thickness strain with electric-field strength........................71 Figure 2-35 Schematic illustration of tunable SPR coupler...........................................72 Figure 3-1 Schematic of organic chemical addition method of nanocomposite films............................................................................................................81 Figure 3-2 A schematic representations of the nanoimprint for patterning (a) ferroelectric and (b) metal/ferroelectric structures.....................................82 Figure 3-3 The schematic diagram of VA-CNT thin films on flexible substrate........83 Figure 3-4 The schematic diagram of nano-patterned CNT films on flexible substrate......................................................................................................84 Figure 3-5 The schematic diagram of broccoli CNTs on flexible substrate................85 Figure 4-1 XRD spectra of the Au/PZT nanocomposite films prepared using various annealing temperatures.............................................................................115 Figure 4-2 TEM images and EDS analyses of the Au/PZT nanocomposite films prepared using (a) 120, (b) 450, and (c) 650 °C (inset: diffraction pattern and high-resolution TEM) annealing temperatures..................................115 Figure 4-3 HR-TEM images and diffraction pattern of the Au/PZT nanocomposite films prepared using 650 °C annealing temperatures...............................116 Figure 4-4 Transmittance spectra of the nanocomposite films prepared using various HAuCl4 contents and annealing temperatures of (a) 120, (b) 450, and (c) 650 °C. (d) Transmittance spectra of the nanocomposite films prepared using 1 mL of the HAuCl4 precursor solution.........................................116 Figure 4-5 Ferroelectric hysteresis curves of the PZT and Au/PZT nanocomposite films after annealing at 650 °C.................................................................117 Figure 4-6 XRD spectra of PZT films at different temperature.................................117 Figure 4-7 SEM images of hexagonal pyramid mold (a) top-view (b) cross-section.......................................................................................................118 Figure 4-8 the hardness of different materials structures at different temperature. -■- : PZT /Si; -●- : Au/ Si; -▲- : Si..................................................................118 Figure 4-9 SEM images of PZT gel films imprinted by hexagonal pyramid mold under (a)14 MPa and (b) 20 MPa pressure..............................................119 Figure 4-10 SEM image of the mold after the imprint PZT gel film process..............120 Figure 4-11 A schematic representations of the nanoimprint for patterning metal/ferroelectric structures....................................................................120 Figure 4-12 SEM images of Au/PZT structures imprinted by hexagonal pyramid mold under (a)14 MPa and (b) 20 MPa pressure..............................................121 Figure 4-13 AFM topography of imprinted Au/PZT structure with hexagonal pyramid mold under (a)14 MPa and (b) 20 MPa pressure.....................................122 Figure 4-14 (a) SEM and AFM images of mold and patterned gold/PZT structure,(b) SEM image of the PZT/gold/PZT structure after sintering process.........123 Figure 4-15 Transmission spectra of gold/PZT films before and after patterning with periodical structure...................................................................................124 Figure 4-16 The SEM images of various CNT length with (a) 0.5, (b) 2, (c) 8, and (d) 80μm, respectively.(Inset: migrification).................................................125 Figure 4-17 The optical spectra vs. different thickness of VA-CNT films are measured by (a) 5° incident angle and (b) integrating sphere on Si substrates........126 Figure 4-18 The experimental and simulated reflectance spectra of VA-CNT films having different length on Si substrates...................................................126 Figure 4-19 The refractive index and extinction coefficient of VA-CNT film having a length of 2 μm..........................................................................................127 Figure 4-20 Plane waves propagated from 1 μm above the air–structure interface to the silicon substrates (a) without structure and possessing (b) VA-CNTs and (c) pyramidal structures with a period of 15 nm and a height of 2 μm.........127 Figure 4-21 A scheme shows the relative orientation of the aligned CNTs with respect to RTE and RTM......................................................................................128 Figure 4-22 A scheme of the multi-layer optical model..............................................128 Figure 4-23 Reflectance spectra of 2.1 μm VA-CNT with different incident angles of (a) TE and (b) TM polarized light on the Si substrate...................................129 Figure 4-24 The effective optical constants of the VA-CNT film measured with TE polarized light at the incident angle of (a) 20° and (b) 60°. The effective optical constants of the VA-CNT film measured with TM polarized light at the incident angle of (c) 20° and (d) 60°..................................................130 Figure 4-25 SEM images of (a) grating-patterned substrates which the period, line width and depth are about 800, 400 and 400 nm, respectively. And (b) hexagonal-patterned substrates which the period, hole and depth are about 800, 400 and 500 nm, respectively...........................................................131 Figure 4-26 SEM images of CNTs growth on (a) grating- and (b) hexagonal- patterned Si substrates..............................................................................................130 Figure 4-27 SEM images of grating-patterned CNT films (a) on PC substrates, and after adhesion on (b) PC substrate side and ............................................132 Figure 4-28 The phtography of CNT films on grating-patterned substrates. (a) As incident light is perpendicular to grating direction. (b) The other direction which incident light is parallel to grating direction..................................133 Figure 4-29 A scheme represent that the detector is rotated around the grating direction and normal the grating direction with normal incident light....................134 Figure 4-30 The diffraction spectra of CNTs with grating-pattern are red-shifted as increasing the detection angles from transmit light.....................................135 Figure 4-31 The diffraction spectra of CNTs with grating-pattern are red-shifted as increasing the detection angles from reflected light....................................135 Figure 4-32 The relationship between experimental measured and diffraction theory calculation for grating-patterned CNT films............................................136 Figure 4-33 SEM images of hexagonal-patterned CNT films (a) on PC substrate, and after adhesion on (b) PC substrate side and (c) tape side.........................137 Figure 4-34 The phtography of colorful CNT films with hexagonal-pattern after tape adhesion....................................................................................................137 Figure 4-35 Transmittance spectrum of hexagonal-patterned CNT films before tape adhesion....................................................................................................138 Figure 4-36 Transmittance spectrum of hexagonal-patterned CNT films after tape adhesion....................................................................................................138 Figure 4-37 Cross-section SEM images of hexagonal-patterned CNT films after tape adhesion on PC substrate..........................................................................139 Figure 4-38 The relationship between experimental measured and diffraction theory calculation for hexagonal-patterned CNT films.......................................139 Figure 4-39 SEM images of broccoli CNTs by the (a) 1 μm and (b) 0.5 μm diameters PS spheres as the templates on Si substrate.............................................140 Figure 4-40 SEM images of broccoli CNTs by the (a) 1 μm and (b) 0.5 μm diameters PS spheres as the templates on PC substrate............................................140 Figure 4-41 A monolayer of PS spheres having a diameter of 1 μm was arranged in hexagonal close-packed arrays.................................................................141 Figure 4-42 The honeycomb pattern of Mo film was formed on the Si substrate.......141 Figure 4-43 The obviously colorful image of broccoli CNTs on a PC substrate.........141 Figure 4-44 Transmittance spectra of broccoli CNTs which used the (a) 1 μm and (b) 0.5 μm diameters PS spheres as the templates on PC substrates.............142 Figure 4-45 The relationship between experimental measured and diffraction theory calculation of broccoli CNTs which used the 1 and 0.5 μm diameters PS spheres as the templates on PC substrates................................................143 Figure 5-1 Transmission spectra of the nanocomposite films subjected to various external electric fields..............................................................................161 Figure 5-2 Simulated spectra of the Au/PZT nanocomposite films under various applied external electric fields, using the measured refractive indices of the PZT films..................................................................................................161 Figure 5-3 The SPR positions under the cyclic electric fields immediately in the Au NP-embedded ferroelectric films.............................................................162 Figure 5-4 The schematic diagrams of patterned PZT/gold/PZT structure (a) before applying voltage, (b) applying positive voltage and (c) applying negative voltage......................................................................................................163 Figure 5-5 Transmittance spectra and SPR wavelength shifts of patterned PZT/gold/PZT structure under different (a) positive voltages (b) negative voltages.....................................................................................................164 Figure 5-6 Piezoelectric coefficient (d33) of PZT films plotted as a function of the applied electric field.................................................................................165 Figure 5-7 The SPR positions of PZT/metal/PZT structure under the cyclic electric fields immediately....................................................................................165 Figure 5-8 The types of bending compare to incident light.......................................166 Figure 5-9 The diffraction peaks of bending and unbending sample in the different detector angles. (a) unbending; (b) concave; (d) convex types................166 Figure 5-10 The diffraction peaks of bending and unbending sample in the different detector angles. (a) 30°; (b) 35°; (d) 40°..................................................167 Figure 5-11 Three independent unbending substrates with incident angle of +5 | |
dc.language.iso | en | |
dc.title | 應用先進微影技術製備具可調變光波長之奈米結構材料 | zh_TW |
dc.title | Using Advanced Lithography to Prepare Nanostructured Materials with the Capability of Tuning Optical Wavelength | en |
dc.type | Thesis | |
dc.date.schoolyear | 97-2 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 楊哲人,段維新,戴念華,任貽均,謝健 | |
dc.subject.keyword | 鐵電材料,奈米粒子,奈米碳管,表面電漿共振,奈米壓印,可撓曲元件, | zh_TW |
dc.subject.keyword | ferroelectric materials,nanoparticles,carbon nanotubes (CNTs),surface plasmon resonance (SPR),nanoimprint,flexible devices, | en |
dc.relation.page | 190 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2009-06-24 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 材料科學與工程學研究所 | zh_TW |
顯示於系所單位: | 材料科學與工程學系 |
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