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Register a new userSurface Diffusion Control Enables Tailored Aspect Ratio Nanostructures in Area-Selective Atomic Layer Deposition
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Area-selective atomic layer deposition is a key technology for modern microelectronics as it eliminates alignment errors inherent to conventional approaches by enabling material deposition only in specific areas. Typically, the selectivity originates from surface modifications of the substrate that allow or block precursor adsorption. The control of the deposition process currently remains a major challenge as the selectivity of the no-growth areas is lost quickly. Here, we show that surface modifications of the substrate strongly manipulate the surface diffusion. The selective deposition of TiO$_2$ on poly (methyl methacrylate) and SiO$_2$ yields localized nanostructures with tailored aspect ratios. Controlling the surface diffusion allows to tune such nanostructures as it boosts the growth rate at the interface of the growth and no-growth areas. Kinetic Monte-Carlo calculations reveal that species move from high to low diffusion areas. Further, we identify the catalytic activity of TiCl$_4$ during the formation of carboxylic acid on poly (methyl methacrylate) as the reaction mechanism responsible for the loss of selectivity, and show that process optimization leads to higher selectivity. Our work enables the precise control of area-selective atomic layer deposition on the nanoscale, and offers new strategies in area-selective deposition processes by exploiting surface diffusion effects.
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Homogeneous highly epitaxial LaSrMnO3 (LSMO) thin films have been grown on Yttria-stabilized-Zirconia (YsZ) / CeO2 buffer layers on technological relevant 4 silicon wafers using a Twente Solid State Technology B.V. (TSST) developed large area Pulsed Laser Deposition (PLD) setup. We study and show the results of the effect of an additional SrRuO3 buffer layer on the growth temperature dependent structural and magnetic properties of LSMO films. With the introduction of a thin SrRuO3 layer on top of the buffer stack, LSMO films show ferromagnetic behaviour for growth temperatures as low as 250C. We suggest that occurrence of epitaxial crystal growth of LSMO at these low growth temperatures can be understood by an improved surface diffusion, which ensures sufficient intermixing of surface species for formation of the correct phase. This intermixing is necessary because the full plume is collected on the 4 wafer resulting in a compositional varying flux of species on the wafer, in contrast to small scale experiments.
Atomic layer deposition was used to synthesize niobium silicide (NbSi) films with a 1:1 stoichiometry, using NbF5 and Si2H6 as precursors. The growth mechanism at 200oC was examined by in-situ quartz crystal microbalance (QCM) and quadrupole mass spectrometer (QMS). This study revealed a self-limiting reaction with a growth rate of 4.5 {AA}/cycle. NbSi was found to grow only on oxide-free films prepared using halogenated precursors. The electronic properties, growth rate, chemical composition, and structure of the films were studied over the deposition temperature range 150-400oC. For all temperatures, the films are found to be stoichiometric NbSi (1:1) with no detectable fluorine impurities, amorphous with a density of 6.65g/cm3, and metallic with a resistivity {rho}=150 {mu}{Omega}.cm at 300K for films thicker than 35 nm. The growth rate was nearly constant for deposition temperatures between 150-275oC, but increases above 300oC suggesting the onset of non-self limiting growth. The electronic properties of the films were measured down to 1.2K and revealed a superconducting transition at Tc=3.1K. To our knowledge, a superconducting niobium silicide film with a 1:1 stoichiometry has never been grown before by any technique.
Despite its interest for CMOS applications, Atomic Layer Deposition (ALD) of GeO$_{2}$ thin films, by itself or in combination with SiO$_{2}$, has not been widely investigated yet. Here we report the ALD growth of SiO$_{2}$/GeO$_{2}$ multilayers on Silicon substrates using a so far unreported Ge precursor. The characterization of multilayers with various periodicities reveals successful layer-by-layer growth with electron density contrast and absence of chemical intermixing, down to a periodicity of 2 atomic layers.
Two-level system (TLS) defects in dielectrics are known to limit the performance of electronic devices. We study TLS using millikelvin microwave loss measurements of three atomic layer deposited (ALD) oxide films--crystalline BeO ($rm{c-BeO}$), amorphous $rm{Al_2O_3}$ ($rm{a-Al_2O_3}$), and amorphous $rm{LaAlO_3}$ ($rm{a-LaAlO_3}$)--and interpret them with room temperature characterization measurements. We find that the bulk loss tangent in the crystalline film is 6 times higher than in the amorphous films. In addition, its power saturation agrees with an amorphous distribution of TLS. Through a comparison of loss tangent data to secondary ion mass spectrometry (SIMS) impurity analysis we find that the dominant loss in all film types is consistent with hydrogen-based TLS. In the amorphous films excess hydrogen is found at the ambient-exposed surface, and we extract the associated hydrogen-based surface loss tangent. Data from films with a factor of 40 difference in carbon impurities revealed that carbon is currently a negligible contributor to TLS loss.
B-doped $delta$-layers were fabricated in Si(100) using BCl$_{3}$ as a dopant precursor in ultrahigh vacuum. BCl$_{3}$ adsorbed readily at room temperature, as revealed by scanning tunneling microscopy (STM) imaging. Annealing at elevated temperatures facilitated B incorporation into the Si substrate. Secondary ion mass spectrometry (SIMS) depth profiling demonstrated a peak B concentration $>$ 1.2(1) $times$ 10$^{21}$ cm$^{-3}$ with a total areal dose of 1.85(1) $times$ 10$^{14}$ cm$^{-2}$ resulting from a 30 L BCl$_{3}$ dose at 150 $^{circ}$C. Hall bar measurements of a similar sample were performed at 3.0 K revealing a sheet resistance of $R_{mathrm{s}}$ = 1.91 k$Omegasquare^{-1}$, a hole concentration of $n$ = 1.90 $times$ 10$^{14}$ cm$^{-2}$ and a hole mobility of $mu$ = 38.0 cm$^{2}$V$^{-1}$s$^{-1}$ without performing an incorporation anneal. Further, the conductivity of several B-doped $delta$-layers showed a log dependence on temperature suggestive of a two-dimensional system. Selective-area deposition of BCl$_{3}$ was also demonstrated using both H- and Cl-based monatomic resists. In comparison to a dosed area on bare Si, adsorption selectivity ratios for H and Cl resists were determined by SIMS to be 310(10):1 and 1529(5):1, respectively, further validating the use of BCl$_{3}$ as a dopant precursor for atomic precision fabrication of acceptor-doped devices in Si.
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