Uniform Si nanostructures grown by oblique angle deposition with substrate swing rotation

Similar documents
PHYSICAL SELF-ASSEMBLY AND NANO-PATTERNING*

Quasi-periodic nanostructures grown by oblique angle deposition

Scaling during shadowing growth of isolated nanocolumns

Continuum model for nanocolumn growth during oblique angle deposition

Physical self-assembly and the nucleation of three-dimensional nanostructures by oblique angle deposition

Optical and Structural Properties of Bilayer Circular Filter Prepared by Glancing Angle Deposition

Magnetic properties of Co nanocolumns fabricated by oblique-angle deposition

"Enhanced Layer Coverage of Thin Films by Oblique Angle Deposition"

Near-perfect modulator for polarization state of light

Physical properties of nanostructures grown by oblique angle deposition

Controllable growth of metallic nano-helices at room temperature conditions

Effect of Spiral Microwave Antenna Configuration on the Production of Nano-crystalline Film by Chemical Sputtering in ECR Plasma

Microstructure Control of Fe Catalyst Films for the Growth of Multiwalled Carbon Nanotube Arrays

Structure-Thermal Property Correlation of Aligned Silicon. Dioxide Nanorod Arrays

Anisotropy properties of magnetic colloidal materials

Nanostructure Fabrication Using Selective Growth on Nanosize Patterns Drawn by a Scanning Probe Microscope

Dielectric Meta-Reflectarray for Broadband Linear Polarization Conversion and Optical Vortex Generation

Paper No. IMECE

Crystalline Surfaces for Laser Metrology

Title of file for HTML: Supplementary Information Description: Supplementary Figures and Supplementary References

Supplementary Information

Fabrication and Domain Imaging of Iron Magnetic Nanowire Arrays

Nanostrukturphysik (Nanostructure Physics)

Research on the Wide-angle and Broadband 2D Photonic Crystal Polarization Splitter

Growth-front roughening in amorphous silicon films by sputtering

Gaetano L Episcopo. Scanning Electron Microscopy Focus Ion Beam and. Pulsed Plasma Deposition

Thermal characterization of Au-Si multilayer using 3- omega method

Chapter 10. Nanometrology. Oxford University Press All rights reserved.

A Photonic Crystal Laser from Solution Based. Organo-Lead Iodide Perovskite Thin Films

Fabrication at the nanoscale for nanophotonics

NUCLEAR TRANSMUTATION IN DEUTERED PD FILMS IRRADIATED BY AN UV LASER

Self-assembled nanostructures for antireflection optical coatings

Hydrodynamics of Diamond-Shaped Gradient Nanopillar Arrays for Effective. DNA Translocation into Nanochannels. (Supplementary information)

Supplementary Figure 1 Detailed illustration on the fabrication process of templatestripped

Supporting Information

Nanosphere Lithography

Nanostrukturphysik (Nanostructure Physics)

SUPPLEMENTARY INFORMATION

High-density data storage: principle

Surface roughening in shadowing growth and etching in 2 1 dimensions

International Journal of Pure and Applied Sciences and Technology

ABSTRACT 1. INTRODUCTION 2. EXPERIMENT

Microstructured Porous Silica Obtained via Colloidal Crystal Templates

Name: School Name: PHYSICS CONTEST EXAMINATION

Ultra-narrow-band tunable laserline notch filter

Chapter 5. Effects of Photonic Crystal Band Gap on Rotation and Deformation of Hollow Te Rods in Triangular Lattice

Supporting Information

A Novel Self-aligned and Maskless Process for Formation of Highly Uniform Arrays of Nanoholes and Nanopillars

Multilayer coating facility for the HEFT hard X-ray telescope

Design of one-dimensional Lambertian diffusers of light

A novel sputtering technique: Inductively Coupled Impulse Sputtering (ICIS)

Focused-ion-beam milling based nanostencil mask fabrication for spin transfer torque studies. Güntherodt

Supplementary Figure 1. Large-area SEM images of rhombic rod foldectures (F1) deposited on Si substrate in (a) an in-plane magnetic field and (b) an

Off-axis unbalanced magnetron sputtering of YBa2Cu307 thin films

Electron Holography of Ferromagnetic Nanoparticles Encapsulated in Three-Dimensional Arrays of Aligned Carbon Nanotubes

A tunable corner-pumped Nd:YAG/YAG composite slab CW laser

Polarization of Light and Birefringence of Materials

Emission pattern control and polarized light emission through patterned graded-refractiveindex coatings on GaInN light-emitting diodes

The Controlled Evolution of a Polymer Single Crystal

ELECTROMAGNETISM. Challenging MCQ questions by The Physics Cafe. Compiled and selected by The Physics Cafe

Fabrication and Characterization of Sculptured Thin Silver Films

Supplementary Information for. Colloidal Ribbons and Rings from Janus Magnetic Rods

SUPPLEMENTARY INFORMATION

Structure analysis: Electron diffraction LEED TEM RHEED

Spontaneous Pattern Formation from Focused and Unfocused Ion Beam Irradiation

Anti-icing surfaces based on enhanced self-propelled jumping of condensed water microdroplets

Supporting Information

Supplementary Figure 1 Characterization of the synthesized BP crystal (a) Optical microscopic image of bulk BP (scale bar: 100 μm).

High Resolution Photoemission Study of the Spin-Dependent Band Structure of Permalloy and Ni

Collective effects in second-harmonic generation from plasmonic oligomers

Optical properties of nano-silicon

OSCILLATORY THICKNESS DEPENDENCE OF THE COERCIVE FIELD IN MAGNETIC 3D ANTI-DOT ARRAYS

Accepted Manuscript. Authors: Charbel S. Madi, Michael J. Aziz S (11) Reference: APSUSC 22249

SUPPLEMENTARY FIGURES

Everhart-Thornley detector

Magnetic Assisted Laser Micromachining for Highly Reflective Metals

Investigation on Mode Splitting and Degeneracy in the L3 Photonic Crystal Nanocavity via Unsymmetrical Displacement of Air-Holes

Helium effects on Tungsten surface morphology and Deuterium retention

Backscattered Electron Contrast Imaging of Scanning Electron Microscopy for Identifying Double Layered Nano-Scale Elements

Identifying the crystal orientation of the black phosphorus

Magnon-drag thermopile

A Broadband Flexible Metamaterial Absorber Based on Double Resonance

A new method of growing graphene on Cu by hydrogen etching

Light trapping in thin-film solar cells: the role of guided modes

Mal. Res. Soc. Symp. Proc. Vol Materials Research Society

Initial Results on the Feasibility of Hybrid X-Ray Microscopy

ARC-ASSISTED CO-CONVERSION OF COAL-BASED CARBON AND ACETYLENE

High-Precision Evaluation of Ultra-Shallow Impurity Profiles by Secondary Ion Mass Spectrometry

Negative Index of Refraction in Optical Metamaterials

Raman spectroscopy at the edges of multilayer graphene

Electronic Supplementary Information

Spectroscopic mapping polarimetry in Bragg Micro-cavities

Motion control of the wedge prisms in Risley-prism-based beam steering system for precise target tracking

Direct study of domain and domain wall structure in magnetic films and nanostructures

Paper No. IMECE

Supporting Information. Temperature dependence on charge transport behavior of threedimensional

A kinetic study of the ordering process in ternary III V semiconductor alloys

Nova 600 NanoLab Dual beam Focused Ion Beam IITKanpur

Supplementary Information

Double-distance propagation of Gaussian beams passing through a tilted cat-eye optical lens in a turbulent atmosphere

Transcription:

INSTITUTE OF PHYSICS PUBLISHING Nanotechnology 16 (2005) 1717 1723 NANOTECHNOLOGY doi:10.1088/0957-4484/16/9/052 Uniform Si nanostructures grown by oblique angle deposition with substrate swing rotation D-X Ye 1,3,TKarabacak 1, RCPicu 2,G-CWang 1 and T-M Lu 1 1 Center for Integrated Electronics, Department of Physics, Applied Physics, and Astronomy Rensselaer Polytechnic Institute, Troy, NY 12180-3590, USA 2 Department of Mechanical, Aerospace, and Nuclear Engineering, Rensselaer Polytechnic Institute, Troy, NY 12180-3590, USA E-mail: yed@rpi.edu Received 29 March 2005, in final form 7 June 2005 Published 6 July 2005 Online at stacks.iop.org/nano/16/1717 Abstract Slanted nano-columns and square nano-springs made of amorphous silicon (a-si) were fabricated on bare Si and patterned substrates by oblique angle deposition with a back forth substrate swing rotation mode. Scanning electron microscopy was used to characterize the grown nanostructures. The tilt angle of slanted nano-rods is determined by the incident angle of deposition flux and the azimuthal swing rotation angle of a substrate. The controlled substrate rotation affects the uniformity and the shape of the nanostructures. On the patterned substrate, the broadening of the size of individual nano-columns is greatly reduced and the nano-columns are not connected as they grow. A simple model based on decomposing the deposition flux is used to describe the effect of substrate rotation on tilt angle, uniformity, and the top-end shape of nanostructures. The feasibility of fabricating separated and well aligned nanostructures by our swing rotation method provides an effectiveand controllable way to fabricate nano-devices. 1. Introduction It is well known that oblique angle deposition produces columnar structures due to the shadowing effect and random fluctuations during film growth [1 16]. In a common oblique angle deposition system, a uniform deposition flux is obtained by evaporation techniques such as thermal evaporation, sputtering, electron-beam evaporation, and laser beam ablation. The deposition flux approaches a stationary substrate at an angle θ (with respect to the substrate normal) referred to as the incident angle or the deposition angle. Well separatedcolumnar structures (nano-columns) can be achieved only athigh deposition angles, particularly θ > 80 for amorphous silicon (a-si). The deposition angle θ determines the porosity of the deposited films and the tilt angle β of the grown columnar structures. Thus the porosity and the geometry of the nanostructures cannot be controlled separately in a traditional oblique angle deposition technique. One 3 Author to whom any correspondence should be addressed. approach to address this problem is through controlling the substrate rotation during growth. Oblique angle deposition with substrate rotation has the capability of fabricating a large variety of three-dimensional (3D) nanostructures [6, 14 16]. This process is not significantly sensitive to the nature of the substrates or the source materials. The shadowing effect is the dominant mechanism controlling the formation, distribution and shape of 3D nanostructures in oblique angle deposition without substrate motion. For a perfectly uniform deposition flux, which has no angular distribution, and ifthe deposition is on a smooth substrate, then the resulting nano-columns still can broaden along the direction perpendicular to the plane of deposition flux and substrate normal. The grown nano-columns have small bottoms but large top diameters due to the shadowing effect [17]. When the growth is on a pre-patterned surface, the broadening of nano-columns is prominent, which leads to a fan-out feature [11]. On the other hand, with a substrate rotation, the shadowing direction of deposited nuclei 0957-4484/05/091717+07$30.00 2005 IOP Publishing Ltd Printed in the UK 1717

D-X Ye et al is changed during a rotation. One would expect that the resulting nano-columns would be much more uniform in their cross-section diameters. The instability of growth can also be limited by the substrate rotation. Some schemes of substrate rotation were designed to fabricate uniform nanostructures based on oblique angle deposition. Previously, we reported our experiments of creating uniform slanted nano-columns by a two-phase rotation method on smooth surfaces [10] and pre-patterned surfaces [11]. This two-phase rotation method decouples the incident flux direction and the column growth direction through an asymmetric azimuthal substrate rotation so that some of the column receives more flux than the rest [10, 11]. Recently, Jensen and Brett designed an algorithm of substrate rotation or PhiSweep in which the substrate rotates rapidly between two azimuthal positions about the intended column growth direction without changing the deposition angle θ [13]. The geometric structure of the thin films deposited by the PhiSweep method is determined by the thickness of the growing film at each pause time (sweep pitch) and the angle spanned by the two directions of an incident flux. In this method, they decoupled the incident flux direction and the column growth direction and the growing slanted nanocolumns effectively receive a flux from both sides of a column because the sample has a pause time at the two end-positions of a sweep. Therefore, the shadowing direction is changed, associated with the substrate rotation. In this paper, we introduce a substrate rotation method referred as swing rotation to grow uniform 3D nanostructures. During a swing rotation, the substrate is rotated azimuthally back-and-forth within an angular range called the swing angle with a fixed rotation speed. It differs from the two-phase rotation method where a second rotation speed was used outside the swing angle. It also differs from the PhiSweep method where a pause time is used at the two ends of a sweep. We present our results of slanted Si nanocolumns and square Si nano-spirals to demonstrate how the swing rotation affects the microstructure of thin films deposited by oblique angle deposition. We show that the tilt angle of aslantedsinano-column can be tuned from 0 to 60. In contrast, the tilt angle of slanted nano-columns can only be changed in the range of 0 40 by the two-phase rotation method [10, 11]. A difference between our swing rotation method and the PhiSweep substrate rotation method is that the latter results in a zigzag shape of nano-fibre where several nano-fibres are bundled together to form a fibrous slanted nanocolumn [13]. No results have been reported on the growth of nano-columns on patterned substrates using the PhiSweep technique. The largest angle of the substrate sweeps is 180 in the PhiSweep method but the largest swing angle can be any angle within 360 in our swing rotation method. In this report, we present the fabrication of slanted nano-columns and square nano-springs grown on smooth substrates and patterned surfaces by swing rotation. Our emphasis is to find the growth parameters that allow uniform nano-columns to be grown on patterned surfaces. Therefore, we are able to assemble more complicated 3D nanostructures such as square nano-spirals. 2. Experimental details Our oblique angle deposition system set-up has been described in detail elsewhere [9]. The depositions were performed Effective deposition angle α( ) 90 80 70 60 50 40 30 20 10 θ =60 θ =45 θ =80 θ =75 θ =70 θ=85 0 0 30 60 90 120 150 180 210 240 270 300 330 360 Swing angle φ ( ) Figure 1. Schematic diagrams of the swing rotation method in oblique angle deposition. (a) Definitions of deposition angle θ and tilt angle β of grown nano-columns. These angles are measured from the surface normal n. The deposition flux F is decomposed into two partsin theplaneof n and F. (b)the swing rotationand the decomposition of F on the substrate surface. (c) The plot of effective deposition angle α as a function of swing angle φ for various θ values. The decrease of α is small for small φ values. in ahigh vacuum chamber with a background pressure of 2 10 4 Pa. The Si (99.9995%, Alfa Aesar) was evaporated by an electron beam bombardment method. The pressure during deposition was less than 5 10 4 Pa. The whole chamber was cooled by circulating chilling water. A quartz crystal microbalance (Maxtek TM-350/400) was used to monitor the evaporation rate. The quartz crystal microbalance was faced to the incident flux without any tilting. The normal growth rate was controlled at 0.50 ± 0.03 nm s 1.Astepper motor was used to rotate the substrate azimuthally without changing the deposition angle θ. See figure 1(a). The substrate was rotated back and forth continuously within an azimuthal angle φ(<360 ). The rotation speed ω was chosen to be 0.15 rev min 1. A set of φ values, φ = {30, 45, 60, 75, 90, 120 }, was chosen for fabrication of slanted Si nano-columns. We refer to this method as swing rotation, shown schematically in figure 1(b). In each experiment, one bare Si(100) substrate and one patterned substrate were loaded into the chamber for deposition. The size of the substrates is about 1 cm 1cmforboth the bare Si substrate and patterned substrate. The patterned substrate has been described elsewhere [11]. The patterned substrates have tungsten nano-pillars of 450 nm height and 150 nm diameter arranged in a two-dimensional (2D) square lattice with lattice constant and a 2D triangular lattice with 700 nm lattice constant on the same piece of substrate. We (c) 1718

Uniform Si nanostructures grown by oblique angle deposition with substrate swing rotation fabricated slanted nano-columns andfour-turn square nanospirals that consist of straight nano-columns with equal lengths for the arms. The arm was created by the same swing rotation method with φ = 60 and θ = 85.Atthe end of the deposition of each arm, the substrate was turned through 90 to start the deposition of the next arm. Thus, four adjacent arms make one complete turn of a nano-spiral. After the deposition, the samples were imaged by a field emission scanning electron microscope (FE-SEM, JEOL Ltd, Tokyo, Japan). For the cross-sectional views, the samples were cleaved along the direction of the deposition flux and the direction perpendicular to the deposition flux. The samples were mounted on a specimen holder and then coated with about 10 nm Au. Top-view and cross-sectional images were taken and digitalized for handling and further analysis. We used Adobe Photoshop 6.0 (Adobe Systems Inc., USA) software to measure the tilt angles of nano-columns from the crosssectional views. The size of nano-columns deposited on the pre-patterned substrates was measured from the crosssectional views along the two directions in which each sample was cut. Weassigned h as the size of the slanted nano-columns measured from the cross-sectional images along the direction of the deposition flux and w as the size of the slanted nanocolumns measured along the perpendicular direction of the deposition flux. 3. Results and discussions 3.1. Model of effective angle of nano-columns grown by the swing method The swing rotation method can be schematically represented in figures 1(a) and (b). The definitions of the angles are illustrated in a 3D view in figure 1(a) and the azimuth rotation of the substrate is shown in figure 1(b). In figure 1(a), the incident angle of deposition flux θ and the tilt angle of nano-columns β are measured from the surface normal n. Following our previous discussion on the deposition flux, we decompose the deposition flux F into a parallel part F and a vertical part F [10]. F is projected into the substrate surface and changes its direction during substrate rotation. In figure 1(b) we decompose F into two parts, one part along the y-axis F y and the other part along the x-axis F x. The part along the y-axis changes sign twice during one period of swing (T ). Subsequently, the deposition associated with this part has no effect on the tilt angle β of the grown nano-columns. The tilt angle β is determined by F, F x and θ. In one period of swing T = 2φ/ω, thefluxdeposited along the x-axis G can be calculated as T φ 2 G = F x dt = 2 F ω 1 cos η dη = 4 F 0 φ ω sin φ 2. 2 (1) At the same time, the deposit along the surface normal n is G = F T = 2 F φ ω. (2) Thus, the effective deposition angle α can be obtained from tan α = G G = 2 F sin φ 2 F φ = 2tanθ sin φ 2 φ. (3) We have derived an expression similar to equation (3) in our previous analysis of the two-phase rotation method, shown as the following equation [10]: tan α = 2( ω 2 ω 1 1 ) tan θ 2π + ( ω 2 ω 1 1 ) φ sin φ 2 (ω 1 <ω 2 ). (4) Equation (4) can be reduced to equation (3) bytakingthe limit of ω 2 in equation (4). However, in terms of substrate rotation, our swing rotation method is not a special case ofthe two-phase rotation method. In the two-phase rotation method the substrate always rotates in one direction (either clockwise or anticlockwise). In the swing method the substrate rotates clockwise and anticlockwise in a swing angle. We plotted α as a function of φ at given values of θ values in figure 1(c). As shown in figure 1(c), α decreases monotonically with the increases of φ. Butthedecrease of α is slow in the region of small φ(φ<90 ). The tilt angle β is determined by α following the same relation in the case of oblique angle deposition without substrate rotation, i.e. the tangent rule [18, 19], tan β = 1 2 tan α (for α<50 ), or the cosine rule [20], β = α arcsin ( 1 cos α 2 ) (for α>50 ). 3.2. Slanted nano-columns grown on smooth Si substrate and nano-pillars in 2D square and triangular patterned substrates under various swing angles 3.2.1. On smooth substrate. In figure 2, representative top-view and cross-sectional view of SEM images of slanted Si nano-columns are presented in the left column and the right column, respectively. These slanted Si nano-columns were grown by the swing rotation method at θ = 85 with φ = 30, 60, 90 and 120,arranged from the top row to the bottom row as in figures 2(a) (d). A sample deposited at θ = 85 without substrate rotation as a reference is shown in figure 2(e). The SEM images were aligned in such a way that the deposition flux came from the left side of each image as indicated by the white arrows shown in figure 2(e). The x- axis and y-axis were assigned in the left image of figure 2(e). The small white scale bars marked in all images correspond to. Compared to the reference sample, the slanted nanocolumns grown by swing rotation are larger in diameter as well as the separation ofneighbouring nano-columns. The size of nano-columns fabricated by swing rotation ranges from 35 to 70 nm, while the columns in the reference sample are about 20 40 nm in diameter, as measured from the cross-sectional SEM images along the x-axis. In the cross-sectional SEM image of the reference sample, thesmall fibrous nano-columns are bundled apparently because of their small separations. In contrast, the nano-columns are separated in the samples fabricated by swing rotation. The size of the nano-columns is smaller at their earlier growing stage in swing rotation growth. Some of the growing nano-columns are hindered by their neighbours at certain film thickness. In the reference sample, nano-columns are connected from the side along the y-axis. In contrast, well defined individual nano-columns can be found in the swing rotation samples. The nano-columns are much more uniform when the swing angle φ changes from 90 to 120.However,bunching of nano-columns can be seen from the SEM top-view images while φ is as small as 30. 1719

D-X Ye et al 90 80 Experimental result ( θ=85, φ varies) 70 (a)θ =85, φ =30 Tilting angle β ( ) 60 50 40 30 20 Tilting angle β ( ) 65 60 55 50 45 40 35 30 Experimental result ( φ=90, θ varies) x (b) θ =85, φ =60 (c) θ =85, φ =90 (d) θ =85, φ =120 y (e) θ =85, φ=0 (fix deposition) Figure 2. SEM images of slanted Si nano-columns grown at θ = 85 on bare Si(100) substrates. Top-view (left) and cross-sectional (right) SEM images of Si nano-columns grown by swing rotation with (a) φ = 30,(b)φ = 60,(c)φ = 90, (d) φ = 120,(e)Sinano-columns grown by traditional oblique angle deposition without substrate rotation. The white arrow in figure 3(e) indicates the direction of the deposition flux. A two-dimensional frame parallel to the plane of substrate with the x-axis and the y-axis labelled is shown in figure 3(e). The white scale bar in each image represents a length of. This observation can be explained by the shadowing effect during oblique angle deposition. Since the substrate is rotated back-and-forth within the swing angle φ,the shadowing effect increases the separation of nano-columns in the y-axis, thus preventing them from merging in this direction. If the swing angle φ is too small, the nano-columns can still touch each other starting at a certain point due to the enhanced diffusiondriven growth in the y-axis. The tilt angles were measured from the substrate normal in the SEM cross-sectional images of grown nano-columns. As shown in figure 3, the change of tilt angle β of nano-columns as a function of the swing angle investigated at a fixed θ is very small, as indicated by the dotted straight line. The inset 10 25 20 50 55 60 65 70 75 80 85 90 Incident angle θ ( ) 0 0 10 20 30 40 50 60 70 80 90 100 110 120 130 Swing angle φ ( ) Figure 3. Experimental results of tilt angle β at different swing angles with θ = 85.Thechange of β is small up to φ = 120.The inset plot is the change of β at different deposition angle θ with φ fixed at 90. in figure 3 shows the trend of β as a function of θ with a fixed φ = 90.Theincrease of β can be very quick as θ is close to 90.Thus, the tilt angle β is determined by the incident angle of the flux θ while the swing angle φ is not larger than 90. The tilt angle β is controlled by the effective deposition α when the swing angle is larger than 90 through a so-called cosine rule as discussed in the two-phase rotation method [10]. As shown infigure 1,thefilmscan be designed to possess a small value of β by rotating the substrate to a large swing angle φ. In aparticular case, when φ = 360, one could fabricate vertical nano-columns (i.e., β = 0 ). As a comparison, using the twophase rotation method, one only can select the tilt angle from asmallrange of 0 36 for Si nano-columns at θ = 85 [11]. Forthe tilt angle of metallic Co nano-columns fabricated using the same deposition parameters in two-phase rotation method the range is from 0 to 40 [11]. The flux deposited along the y-axis has no effect on the tilt angle of the resulting nano-columns because of the cancellation of flux from both sides of the x-axis. However, it has an effect on the morphology of the deposited films. In our swing rotation scheme, the larger the swing angle φ, thegreater the deposited flux along the y-axis. Meanwhile, the shadowing effect in this direction is increased with the larger φ values. One could imagine that the deposited films become porous with the increasing shadowing effect in the y-axis. In other words, one could control the porosity of the films without changing the tilt angle of the films too much. This is desirable for the magnetic and optical applications where the anisotropy of the films is preferred [17, 21 23]. 3.2.2. On nano-pillars arranged on a 2D square symmetry substrate. To obtain a periodic array of nanostructures, patterned surfaces are required in order to control the locations where the nanostructures are grown. We used 450 nm height tungsten nano-pillars as the seeds tofabricate regular arrays of nano-columns and nano-spirals (in section 3.3). Figure 4 shows the slanted nano-columns grown on the pre-fabricated nano-pillar seeds arranged in a 2D square lattice. The flux 1720

Uniform Si nanostructures grown by oblique angle deposition with substrate swing rotation (a) φ=30 (a) φ=30 (b) φ=60 (b) φ=60 (c) φ=90 (c) φ=90 y y x x (d) φ=120 Figure 4. SEM images of slanted Si nano-columns grown on nano-pillars arranged in a square lattice. Top-view (left) and cross-sectional (right) SEM images of the nano-columns grown by swing rotation at θ = 85 with (a) φ = 30,(b)φ = 60, (c) φ = 90,and(d)φ = 120.The white scale bar corresponds to a length of. (d) φ=120 Figure 5. SEM images of slanted Si nano-columns grown on nano-pillars arranged in a triangular lattice. Top-view (left) and cross-sectional (right) SEM images of the nano-columns grown by swing rotation at θ = 85 with (a) φ = 30,(b)φ = 60, (c) φ = 90,and(d)φ = 120.The white scale bar corresponds to a length of. came in from the left shown as the white arrow in the bottom figure. The top-view and cross-sectional SEM images are arranged in the left column and the right column, respectively. The samples were cleaved along the direction of incident flux to show the cross-sectional views of the grown nano-columns. From the top row to the bottom row in figure 4,theSEMimages correspond to the samples prepared at φ = 30, 60, 90 and 120 with θ = 85 and ω = 0.15 rev min 1 fixed for all samples. We have imaged the other two samples prepared at φ = 45 and 75 which are not shown in this paper. As shown in figure 4, the nano-columns continuously broaden along the y-axis to form a shell feature for samples prepared at swing rotation angle φ<90 on square patterned substrates. This means the growth of nano-columns does not reach the constant growth region if the swing angle φ is smaller than 90. Consequently, the nano-columns are still able to touch their neighbours along the y-axis, the direction perpendicular to the deposition flux. The size of nano-columns in the y-axis direction increases as the growth time increases for the samples with swing rotation angle φ<90.forthesamples grown at φ = 90 and 120,thesizeof the nano-columns in the y-axis direction increases initially but saturates very quickly after a short period of growth time. After this, nano-columns with a uniform size were obtained by the swing rotation method. As a result, well aligned nano-columns can be fabricated to a length of several micrometres by choosing a swing angle φ 90 for asquare patterned substrate. 3.2.3. On nano-pillars arranged on a 2D triangular symmetry substrate. The nano-columns grown on triangular patterned substrates are shown in figure 5. The lattice constant of the 2D triangular lattice is about 700 nm, which is shorter than the lattice constant of the square lattice (). The number density of the nano-pillar seeds in the triangular lattice is about 2.356 10 10 cm 2 and is larger than the number density of the square lattice which is 1 10 10 cm 2.Consequently, the size of the nano-columns on these seeds is smaller than the size of nano-columns on square patterned seeds which are listed in table 1. Itcompares the measured values of h and w for the triangular lattice and square lattice under the same swing angle φ. 1721

D-X Ye et al Table 1. The measured tilt angle β,thesizeh of nano-columns in the direction of deposition flux, and the size w of nano-columns in the perpendicular direction to the flux. The slanted nano-columns weredeposited on nano-pillar seeds in a square lattice (left column) or a triangular lattice (right column) by swing rotation with different angle φ values. The incident angle of the deposition flux was kept at 85 for all the samples. Square lattice Triangular lattice Swing Size of Size of Size of Size of angles φ Tilt angle β column h column w Tilt angle β column h column w (deg) (deg) (nm) (nm) (deg) (nm) (nm) 30 58.0 ± 0.7 289 ± 17 681 ± 12 61.3 ± 0.2 175 ± 11 408 ± 8 45 56.9 ± 0.6 252 ± 8 615 ± 7 57.7 ± 0.5 187 ± 12 402 ± 17 60 59.9 ± 1.0 273 ± 9 639 ± 6 61.6 ± 0.3 266 ± 5 384 ± 10 75 56.9 ± 0.4 305 ± 14 500 ± 13 58.4 ± 0.3 173 ± 5 349 ± 9 90 56.6 ± 0.4 300 ± 10 638 ± 16 59.2 ± 0.4 175 ± 6 409 ± 18 120 54.5 ± 0.4 265 ± 11 474 ± 14 56.9 ± 0.4 178 ± 8 356 ± 8 From table 1, itcan also be found that the measured tilt angle β of slanted nano-columns deposited on patterned substrates slightly fluctuates around 60,whichisthe same as the result of tilt angle of the nano-columns deposited on a smooth surface in figure 3. Thefluctuation is induced mainly by the mis-cut of the patterned 2D lattice along the x-axis when prepared the samples for SEM imaging. The mis-cut can be seen from the cross-sectional views in the right columns of figures 4 and 5 that show some nano-pillars missing or closer to the cutting edge of the samples than other nano-pillars in the same row. The above result shows a great improvement compared with our previous results. For example, as we showed previously, isolated individual nanostructures would not be easily fabricated on the nano-pillars if the substrate is kept stationary at one position for a long deposition time [11]. The fan-out growth of nano-columns would result in a connected structure along the y-axis. We applied our two-phase rotation method to solve this problem and demonstrated that well aligned nano-columns can be fabricated using this method [11]. Likewise, our new method of swing rotation has the capability of preventing the fan-out growth. The mechanism of reducing thefan-out feature is the same for these two rotation methods. Since the substrate is rotated, the direction of the shadowing effect is changing and the growth along the side of nanocolumns is interrupted during a rotation. During a swing rotation, the centre of a growing nano-column can receive the flux without interruption. But the side perpendicular to the flux only receives the flux when the nano-column is rotated to face theflux on this side. If the rotational speed is fast enough, only several short small rods grow on the sides. Rectangular cross sections of nano-columns can be expected to grow on a square lattice of pre-fabricated nano-pillars according to the symmetry of the square lattice. Likewise, we expected that a triangular shape of the cross section of nano-columns can be formed on the nano-pillars arranged in a triangular lattice. 3.3. Square nano-spirals grown on smooth Si substrate and nano-pillars in 2D square and 2D triangular patterned substrates To demonstrate the capabilities of our swing rotation method in fabricating different 3D nanostructures, we deposited a square nano-spiral sample with the swing angle φ = 60 and incident angle θ = 85 on both bare Si(100) surfaces and pre-patterned substrates. The SEM images of the four-turn nano-spirals are A (a) (c) (e) B (b) (d) (f) Figure 6. (a) Top-view and (b) cross-sectional SEM images of square Si nano-spirals on a bare Si(100) substrate. The nano-spiral circled by a dotted circle A has a large diameter and the one circled by B has a small diameter. (c) Top-view and (d) cross-sectionalsem images of square nano-spirals grown on nano-pillars arranged in a square lattice. (e) Top-view and (f) cross-sectional SEM images of square nano-springs grown on nano-pillars arranged in a triangular lattice. Each arm of the nano-spirals is grown by swing rotation at θ = 85 and φ = 60.The white scale bar represents. shown in figure 6. The top-view images and cross-sectional images are arranged in the left column and the right column, respectively. When taking the images of the cross-sectional views, we tilted the samples by 10 to show the top surface of the samples. The nano-spirals fabricated on bare Si(100) substrates are uniformly distributed across the whole sample as shown in the top-view and cross-sectional SEM images shown in figures 6(a) and (b), respectively. The cross-section of the arms constructing the nano-spirals is not a circle but a shape close to a rectangle with its longer side perpendicular to the 1722

Uniform Si nanostructures grown by oblique angle deposition with substrate swing rotation incident flux as observed in top-view SEM images. There were small slanted rods starting to growatthe beginning growth time of nano-spirals. Some bigrods dominate the growth due to the shadowing effect, which continuously grow and form complete spirals. Some small rods diminish after a short period of growth time. After the first turn, the size of individual nanospirals is uniform for the remaining three turns of the same nano-spirals. Due to the competition between adjacent nanospirals, however, the cross-sectional diameter fluctuated from one nano-spiral to another. There is a group of large nanospirals (such as spring A marked in figure 6)with a diameter of 357±33 nm and a group of small nano-spirals (spring B marked in figure 6(a), for example) with a diameter of 180±30 nm. The diameter was measured from the SEM top-view image along the direction perpendicular to the incident flux for a particular arm, which is the long axis of the cross-sectional shape of the nano-spirals. Both groups of nano-spirals interweave into the deposited films in that a large nano-spring is surrounded by some small nano-spirals. We believe that the difference in the diameters of the two groups of nano-spirals (A and B in figure 6(a)) can be reduced by rotating the substrate to a swing angle φ>120. Another way to deposit uniform spirals is to introduce the patterned nano-seeds. The nano-spirals grown on our nanopillar seeds in a square lattice and triangular lattice are shown in figures 6(c) (f). The scale bars in the figure correspond to. The nano-spirals form a regular array which has the same periodicity as the seeds in the lateral plane. The pitches of each turn of the nano-spirals measured from the cross-sectional images are 1042 ± 5and 1024 ± 8nmforthenano-spirals grown on a square lattice and a triangular lattice, respectively. The sizes of the nano-spirals measured from side to side, as indicated by white arrows in figures 6(d) and (e), are 1052±59 and 915 ± 37 nm for the square lattice and triangular lattice. We also estimated the diameter of the arms of the spiral from the cross-sectional SEM images. The diameters are measured to be 379±15 nm and 259±20 nm for the nano-spirals grown on a square lattice and a triangular lattice, respectively. From the measurements, the nano-spirals grown on a square lattice are fat compared to the nano-spirals grown on a triangular lattice. Other complex 3D nanostructures such as slanted zigzags, S-shape nano-wires, and round nano-spirals can be grown using swing rotation in the future. We believe that the swing rotation might have a profound effect on the texture of the grown nanostructures if one chooses metals to construct the nanostructures. Recently, Jensen et al reported the growth of square nanospirals on a smooth surface using the PhiSweep substrate rotation scheme [13]. They found close packed nano-spirals can be grown with uniform size as the sweep pitch was chosen to be 45 nm at a total swept angle of 90 [13]. In their experiment, the fine structure of the nano-spirals has a zigzag shape due to the sweep of substrate. The growth of nanocolumns has not been demonstrated by the PhiSweep method yet. In this paper, we mainly focused on our fabrication of slanted nano-columns grown on patterned substrates. By choosing a large swing angle such as φ = 90,weshowthe capability of creating uniform nano-columns on nano-pillars. However, the nano-columns grown on a smooth surface are not very uniform in size at φ = 90.Compared to the result of the PhiSweep method, we believe that the reason is a shorter growth time on both sides of the nano-columns in our approach. This deficit could be overcome if we chose a non-uniform rotational speed ω with slower rotation speed when close to both ends of the swing angle. 4. Conclusions In conclusion, we have developed an improved method to fabricate slanted Si nano-columns and square nano-spirals by using a substrate swing rotation in the plane of the substrate surface. Well separated and uniform nano-columns were fabricated in our experiment. We constructed a simple model to predict the tilt angle of the columns by decomposing the incident flux into parallel and vertical parts. An expression of the effective deposition angle was obtained for the swing rotation method. By varying the swing angles and fixing the incident angle, one can change the porosity of the deposited films without changing the tilt angle of the grown nanocolumns. This technique can be used to design new optical and other devices. Acknowledgment This work is supported by NSF under grant No. 032449. References [1] Krug J and Meakin P 1991 Phys. Rev. A 43 900 [2] Abelmann L and Lodder C 1997 Thin Solid Films 305 1 [3] Leamy H J, Gilmer G H and Dirks A G 1980 Current Topics in MaterialsScience vol 6, ed E Kaldis (Amsterdam: North-Holland) [4] Karabacak T, Wang G-C and Lu T-M 2004 J. Vac. Sci. Technol. A 22 1778 [5] Meakin P 1998 Fractals, Scaling and Growth Far From Equilibrium (Cambridge: Cambridge University Press) [6] Lakhtakia A and Messier R 2004 Sculptured Thin Films: Nanoengineered Morphology and Optics (Bellingham, WA: SPIE Optical Engineering Press) [7] Robbie K, Friedrich L J, Dew S K, Smy T and Brett M J 1995 J. Vac. Sci. Technol. A 13 1032 [8] Robbie K, Sit J C and Bret M J 1998 J. Vac. Sci. Technol. B 16 1114 [9] Zhao Y-P, Ye D-X, Wang G-C and Lu T-M 2002 Nano Lett. 2 351 [10] Ye D-X, Zhao Y-P, Yang G-R, Wang G-C and Lu T-M 2002 Nanotechnology 13 615 [11] Ye D-X, Karaback T, Lim B K, Wang G-C and Lu T-M 2004 Nanotechnology 15 817 [12] Messier R and Lakhtakia A 1999 Mater. Res. Innovat. 2 217 [13] Jensen M O and Brett M J 2004 Appl. Phys. A 80 763 [14] Robbie K, Beydaghyan G, Brown T, Dean C, Adams J and Buzea C 2004 Rev. Sci. Instrum. 75 1089 [15] Dick B and Brett M J 2004 Encyclopedia of Nanoscience and Nanotechnology ed H S Nalwa (Stevenson Ranch: American Scientific Publishers) [16] Suzuki M, Ito T and Taga Y 2001 Appl. Phys. Lett. 78 3968 [17] Leamy H J and Dirks A G 1977 J. Phys. D: Appl. Phys. 10 L95 [18] Niuewenhuizen J M and Haanstra H B 1966 Philips Tech. Rev. 27 87 [19] Dirks A G and Leamy H J 1977 Thin Solid Films 47 219 [20] Trait R N, Smy T and Brett M J 1993 Thin Solid Films 226 196 [21] Motohiro T and Taga Y 1989 Appl. Opt. 28 2466 [22] Shiraishi K and Aoyagi T 1998 Opt. Lett. 23 1232 [23] Liu F, Umlor T, Shen L, Weston J, Eads W, Barnard J A and Mankey G J 1999 J. Appl. Phys. 85 5486 1723