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Science

Localization of Metastable Atom Beams with Optical Standing Waves: Nanolithography at the Heisenberg Limit

Kent S. Johnson, Joseph H. Thywissen, Nynke H. Dekker, Karl K. Berggren, A. P. Chu, Rebecca J. Younkin, Mara Goff Prentiss

Published Jun 5, 1998• 304 citations
Publisher

Abstract

The spatially dependent de-excitation of a beam of metastable argon atoms, traveling through an optical standing wave, produced a periodic array of localized metastable atoms with position and momentum spreads approaching the limit stated by the Heisenberg uncertainty principle. Silicon and silicon dioxide substrates placed in the path of the atom beam were patterned by the metastable atoms. The de-excitation of metastable atoms upon collision with the surface promoted the deposition of a carbonaceous film from a vapor-phase hydrocarbon precursor. The resulting patterns were imaged both directly and after chemical etching. Thus, quantum-mechanical steady-state atom distributions can be used for sub-0.1-micrometer lithography.

DOI
10.1126/science.280.5369.1583

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The spatially dependent de-excitation of a beam of metastable argon atoms, traveling through an optical standing wave, produced a periodic array of localized metastable atoms with position and momentum spreads approaching the limit stated by the Heisenberg uncertainty principle. Silicon and silicon dioxide substrates placed in the path of the atom beam were patterned by the metastable atoms. The de-excitation of metastable atoms upon collision with the surface promoted the deposition of a carbonaceous film from a vapor-phase hydrocarbon precursor. The resulting patterns were imaged both directly and after chemical etching. Thus, quantum-mechanical steady-state atom distributions can be used for sub-0.1-micrometer lithography.
Atom lithography uses standing wave light fields as arrays of lenses to focus neutral atom beams into line patterns on a substrate. Laser cooled atom beams are commonly used, but an atom beam source with a small opening placed at a large distance from a substrate creates atom beams which are locally geometrically collimated on the substrate. These beams have local offset angles with respect to the substrate. We show that this affects the height, width, shape, and position of the created structures. We find that simulated effects are partially obscured in experiments by substrate-dependent diffusion of atoms, while scattering and interference just above the substrate limit the quality of the standing wave lens. We find that in atom lithography without laser cooling the atom beam source geometry is imaged onto the substrate by the standing wave lens. We therefore propose using structured atom beam sources to image more complex patterns on subwavelength scales in a massively parallel way.
Atom lithography is a technique to structure layers of atoms during deposition, using interactions of near-resonant light fields with neutral atoms. The basic scheme uses a standing wave light field, aligned just above a substrate, while a beam of atoms impinges perpendicularly on the standing wave light field. The interaction of the light field and the atoms focuses the atoms towards the crests or troughs of the standing wave intensity, dependent on the tuning of the light field. The focused atoms are subsequently deposited on the substrate, resulting in an array of lines, whose periodicity is determined by the wavelength of the light field. The standing wave light field can therefore be seen as an array of lenses, focusing the atom beam into an array of lines. The first experiments on atom lithography were performed in the 1990s with sodium and chromium. In this thesis experiments with iron are described, which is a magnetic element and thus allows for the creation of magnetic nanostructures. To focus atom beams into structures using atom lithography, well-colimated atom beams are required. The most common technique to create collimated atom beams is transverse laser cooling, but iron has no closed optical transition suitable for laser cooling. Fortunately Smeets and Te Sligte found that even then atom lithography of iron is possible. If the standing wave light field is considered to be an array of lenses, the focusing of the atom beam on a single lens is determined by the local collimation of the atom beam at that position. This local collimation is determined by the geometry of the beam source and the distance of the beam source to the standing wave lens. Using a small beam source (e.g. 1 mm diameter) positioned far from the standing wave (e.g. 1 m), the geometrically collimated atom beam is suitable for atom lithography. Chapter 3 shows what the implications of geometric collimation are on the structure formation in atom lithography. The geometric effects that locally collimate the atom beam on the sample also introduce local offset angles of the atom beam with respect to the focusing light field. Structure formation has been observed with lines of up to 7 nm high on a background layer of 15 nm average height, over areas of up to 400 µm × 6 mm. This indicates that the offset angles can vary over an 8 mrad range, which is more than an order of magnitude larger than the local angle of collimation. The offset angle influence the local geometry of the deposited structures: an increasing offset angle decreases the local line height, increases the width and creates a skewness in the local line shape. The local geometry of the lines has been modelled with a Monte Carlo particle tracking model and the results were compared to experiments. It was found that the highest and narrowest lines suffer from significant broadening due to surface diffusion in experiments, limiting the achievable structure width of iron on SiOx samples to about 80 nm. We have also found that in atom lithography without laser cooling, each standing wave lens is effectively imaging the source geometry onto the substrate. We therefore propose using structured atom beam sources to image more complex patterns on sub-wavelength scales in a parallel way. The reason to use iron in atom lithography, is the option to create magnetic nanostructures. However, in previous experiments no clear magnetic signature of the atom lithographic structuring of iron was found. Therefore in Chapter 4 firstly the magnetic properties of unstructured layers of iron (Fe), nickel (Ni) and FexNi1-x are investigated. These layers are all ferromagnetic, but with a reduced magnetic moment compared to bulk values due to contaminations and crystal growth effects. As a reference for periodic atom lithography structures, periodic line structures are created with interference lithography in a polymer layer and onto these structures thin layers of FexNi1-x are shadow deposited, thereby creating a layer periodically modulated in both height and elemental composition. This periodic modulation in composition has been observed with SEM-EDX on sub-micron scales. The structures showed a clear magnetic anisotropy with an easy axis along the direction of the lines, in accordance with expectations. In Chapter 5, the magnetic properties of atom lithographic iron line structures are presented. Using MOKE microscopy, direct comparison of structured and unstructured parts of a sample is possible, which allows for the observation of clear magnetic signatures due to the atom lithographic structuring. In layers of an average thickness of about 15 nm, no anisotropy is induced by the line structures, while a magnetic easy axis along the direction of the lines is expected. The line structures introduce an isotropic increase in the coercivity of the layers, indicating that the line structures can be considered as isotropic corrugations instead of directional line structures. For layers of 30 nm average thickness and thus higher line structures, a clear magnetic anisotropy is observed for the highest line structures. This anisotropy can be seen as a magnetic easy axis along the direction of the lines, as expected for line structures. However, we also observe a sharp increase in coercivity for applied fields perpendicular to the lines. This phenomenon is intriguing and may be explained by a pinning of head-to-head domain walls along the direction of the lines. In Chapter 5, we also report on the first results of co-deposition of FexNi1-x, where the Fe is structured into lines using atom lithography, while the Ni is deposited uniformly, thereby creating an alloy of modulating composition. Magnetic analysis of these structures indicates that these structures are anisotropic, both the coercivity and the shape of domain walls is dependent on the angle of the applied field relative to the line structures. Finally in Chapter 6, we investigate the possibilities to focus a thermal beam of atoms into a single 100 nm spot using light fields, thereby creating a nanopencil suitable for deposition of nanostructures. A Monte Carlo particle tracking program was developed to model the all optical focusing or funneling of 10 µm sized atom beams to a 100 nm spot. This model included effects of initial beam divergence, magnetic substructure, laser cooling, and spontaneous as well as stimulated diffusion and it was applied to a number of promising light field configurations. The best results obtained for experimentally realistic settings are a beam focused to a full width at half maximum of FWHM = 0.55 µm in a blue detuned hollow beam where atoms are focused towards the dark center, or a FWHM = 0.31 µm in a red detuned axicon light field, where atoms are focused towards the maximum intensity at the heart line. However, in the latter case the focused beam has a flux only 25 times larger than the background flux, which is unpractical for applications. The limiting factors of all schemes are heating due to stimulated diffusion and the limited interaction time available for a thermal beam of atoms. A nanopencil could be possible if it were based on the focussing of a slow and / or monochromatic atom beam, but this would seriously complicate the practical application of such a device.
A bright metastable helium (He∗) beam is collimated sequentially with the bichromatic force and three optical molasses velocity compression stages. Each He∗ atom in the beam has 20 eV of internal energy that can destroy a molecular resist assembled on a gold coated silicon wafer. Patterns in the resist are imprinted onto the gold layer with a standard selective etch. Patterning of the wafer with the He∗ was demonstrated with two methods. First, a mesh was used to protect parts of the wafer making an array of grid lines. Second, a standing wave of λ=1083 nm light was used to channel and focus the He∗ atoms into lines separated by λ/2. The patterns were measured with an atomic force microscope establishing an edge resolution of 80 nm. Our results are reliable and repeatable.
Diffraction of atomic wave packets from a standing laser wave with a Gaussian profile is studied theoretically and numerically in pursuing the aim of creating high-resolution spatial structures in optical nanolithography. To this end, we propose to use nonadiabatic transitions between two optical potentials which take place when square of the value of detuning off the resonance is approximately equal to the Doppler shift. In this case, atomic wave packets experience splitting at nodes of the standing wave, which allows creating atomic structures on a substrate with a period substantially smaller than the standard nanofabrication limit equal to half the wavelength of light. We propose a scheme of the experiment for the observation of nonadiabatic transitions and splitting of the wave of matter caused by them. A number of computer simulations with parameters corresponding to real atoms have been performed, which exhibit this effect in both momentum and coordinate spaces.