Advanced scanning probe lithography

Journal name:
Nature Nanotechnology
Year published:
Published online


The nanoscale control afforded by scanning probe microscopes has prompted the development of a wide variety of scanning-probe-based patterning methods. Some of these methods have demonstrated a high degree of robustness and patterning capabilities that are unmatched by other lithographic techniques. However, the limited throughput of scanning probe lithography has prevented its exploitation in technological applications. Here, we review the fundamentals of scanning probe lithography and its use in materials science and nanotechnology. We focus on robust methods, such as those based on thermal effects, chemical reactions and voltage-induced processes, that demonstrate a potential for applications.

At a glance


  1. Scanning probe lithography.
    Figure 1: Scanning probe lithography.

    a, Schematic of scanning probe lithography (SPL) where imaging and patterning applications are orthogonal. b, Classification of SPL methods according to the dominant tip–surface interaction used for patterning, namely electrical, thermal, mechanical and diffusive processes.

  2. Nanofabrication landscape.
    Figure 2: Nanofabrication landscape.

    a, Resolution and throughput in nanolithography. High-volume techniques (red shapes) require throughput values >1012 μm2 h−1. At lower throughput, maskless electron beam (blue shapes) and scanning probe techniques (green shapes) converge roughly on a single line, called Tennant's law. GEB, Gaussian beam lithography; EBID, electron-beam-induced deposition; CAR, chemically amplified resists; VSB, variable shaped beam; DUV, deep ultraviolet; EUV, extreme ultraviolet; NIL, nanoimprint lithography; UHV, ultrahigh vacuum. b, Within the advanced scanning probe techniques (ambient SPL in a) a similar correlation exists. High-resolution results are shown for bias-induced scanning probe lithography (b-SPL), oxidation SPL (o-SPL), current-controlled SPL (c-SPL) and thermal SPL (t-SPL). tc-SPL, thermochemical SPL. Figure reprinted with permission from: a, ref. 8, © Springer; b, images for b-SPL, ref. 61, © American Chemical Society; c-SPL, ref. 51, © SPIE; t-SPL, ref. 27, © American Chemical Society.

  3. Thermal and thermochemical scanning probe lithography.
    Figure 3: Thermal and thermochemical scanning probe lithography.

    a, Silicon thermal cantilever comprising integrated joule heaters for tip heating and for thermal sensing. Inset: Scanning electron micrograph of the tip region of the cantilever. b, High-speed thermal scanning probe lithography (t-SPL). Topographical image of a fractal pattern comprising 880 × 880 pixels written in 12.8 seconds29. c, Silicon structures created from a reactive ion etching transfer of t-SPL-written nested L-lines at 27-nm half-pitch27. d, Direct patterning of field-effect transistors by conversion of a precursor material into pentacene31. Drain current, ISD, plotted against gate voltage, Vg, for different drain voltage levels, VD. Inset: Device configuration schematic. W and L are the width and length of the channel, respectively; S and D are the source and drain electrodes, respectively. e, Direct thermal conversion of graphene oxide to conductive graphene using thermochemical SPL (tc-SPL)32. f, Top: Local crystallization by tc-SPL of a precursor film on plastic or Si to form nanostructures of PbTiO3 (PTO) ceramics. Scale bar, 1 μm. Bottom: Piezo-force-microscopy measurement of the typical ferroelectric hysteresis loop acquired on a PTO nanodot fabricated by tc-SPL, and shown in the inset17. Scale bar, 1 μm. Figure reprinted with permission from: a, ref. 126, © SPIE; b, ref. 29, © Institute of Physics; c, ref. 27, © American Chemical Society; d, ref. 31, © Wiley; e, ref. 32, © American Association for the Advancement of Science; f, ref. 17, © Wiley.

  4. Greyscale thermal and thermochemical scanning probe lithography.
    Figure 4: Greyscale thermal and thermochemical scanning probe lithography.

    a, Greyscale patterning of a photograph of Richard Feynman (courtesy of the Archives, California Institute of Technology; used with the permission of Melanie Jackson Agency, LLC) with single-nanometre absolute depth precision written by closed-loop thermal scanning probe lithography (t-SPL). Inset: Programmed bitmap. Bottom: Cross-sectional profile of experimental data (black) and target pattern (red) taken along the dotted line. b, Precise positioning of Au nanorods on a silicon wafer after template removal36. The red lines mark the position of the guiding structures. A placement accuracy of 10 nm was achieved (standard deviation of the distance d from the centre of the guiding structures). The angle α indicates the largest error in rod alignment. c, Thermochemical SPL (tc-SPL) is used to control the density of amine groups on a polymer film. The thermally deprotected amines are then labelled with a fluorescent dye for visualization, showing in pink the optical fluorescence image of a Mona Lisa picture20. d, AFM topography image (full z-range 20 nm) of a three-dimensional Mona Lisa image nanopatterned by tc-SPL conversion of a precursor film into poly-p-phenylene vinylene (PPV)22. e, Image of an array of five thermal cantilevers and corresponding five fluorescence images of PPV Mona Lisa patterns obtained with the array22. Figure reprinted with permission from: b, ref. 36, © American Chemical Society; c, ref. 20, American Chemical Society; d,e, ref. 22, © Royal Society of Chemistry.

  5. Oxidation scanning probe lithography.
    Figure 5: Oxidation scanning probe lithography.

    a, The oxidation process used in oxidation SPL (o-SPL) is mediated by the formation of a water bridge that provides the oxyanions. The effective width of the liquid bridge together with the kinetics controls the feature size. b, General electrochemical reactions in local anodic oxidation. c, Molecular dynamics snapshot of the field-induced formation of a 2.5-nm-long water bridge (1,014 water molecules). Oxygen atoms are in red and hydrogen in white. d, Main steps to pattern ferritin proteins on a silicon surface by combining bottom-up electrostatic interactions and local oxidation. The silicon oxide pattern made on the silicon surface is shown in orange. OTS, octadecyltrichlorosilane; APTES, aminopropyltriethoxysilane. e, AFM image of an array of ferritin molecules. The bottom-right inset shows an AFM phase image of a section containing individual ferritin molecules. The space within the arrows is 10 nm. The top-right inset illustrates the structure of the ferritin. The polypeptide shell of the protein is shown in blue. Figure reprinted with permission from: b, ref. 42, © Royal Society of Chemistry; c, ref. 97, © American Chemical Society; d,e, ref. 6, © Wiley.

  6. Silicon and graphene nanolectronic devices fabricated by oxidation scanning probe lithography.
    Figure 6: Silicon and graphene nanolectronic devices fabricated by oxidation scanning probe lithography.

    a, Scheme of the fabrication of a very thin and narrow oxide mask. That mask defines the width of a silicon nanowire. b, Atomic force microscopy images of silicon nanowires of different geometries fabricated by oxidation SPL (o-SPL). The image of the gold pads and connections has been obtained by optical microscopy. Scale bars in the AFM images, 100 nm. c, Transfer characteristics of a silicon nanowire field-effect transitor made by o-SPL. SS, subthreshold swing; Vth, threshold voltage; Vg, gate voltage; Ids, drain current. d, Scheme of the fabrication of a graphene quantum dot. A graphene layer deposited on a silicon dioxide film is locally oxidized by an atomic force microscope tip. e, Atomic force microscopy image of a single quantum dot (QD). f, Coulomb blockade diamond of the quantum dot measured at T = 50 mK. Figure reprinted with permission from: b, ref. 15, © Institute of Physics; c, ref. 102, © Institute of Physics; e,f, ref. 90, © American Institute of Physics.


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  1. Instituto de Ciencia de Materiales de Madrid, CSIC, Sor Juana Inés de la Cruz 3. 28049 Madrid, Spain

    • Ricardo Garcia
  2. IBM Research - Zurich, Saeumerstr. 4, 8803 Rueschlikon, Switzerland

    • Armin W. Knoll
  3. School of Physics, Georgia Institute of Technology, Atlanta, Georgia 30332-0400, USA

    • Elisa Riedo

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