C.W. Hagen

A critical literature review of focused electron beam induced deposition

An extensive review is given of the results from literature on electron beam induced deposition. Electron beam induced deposition is a complex process, where many and often mutually dependent factors are involved. The process has been studied by many over many years in many different experimental setups, so it is not surprising that there is a great variety of experimental results. To come to a better understanding of the process, it is important to see to which extent the experimental results are consistent with each other and with the existing model. All results from literature were categorized by sorting the data according to the specific parameter that was varied (current density, acceleration voltage, scan patterns, etc.). Each of these parameters can have an effect on the final deposit properties, such as the physical dimensions, the composition, the morphology, or the conductivity. For each parameter-property combination, the available data are discussed and (as far as possible) interpreted. By combining models for electron scattering in a solid, two different growth regimes, and electron beam induced heating, the majority of the experimental results were explained qualitatively. This indicates that the physical processes are well understood, although quantitatively speaking the models can still be improved. The review makes clear that several major issues remain. One issue encountered when interpreting results from literature is the lack of data. Often, important parameters (such as the local precursor pressure) are not reported, which can complicate interpretation of the results. Another issue is the fact that the cross section for electron induced dissociation is unknown. In a number of cases, a correlation between the vertical growth rate and the secondary electron yield was found, which suggests that the secondary electrons dominate the dissociation rather than the primary electrons. Conclusive evidence for this hypothesis has not been found. Finally, there is a limited understanding of the mechanism of electron induced precursor dissociation. In many cases, the deposit composition is not directly dependent on the stoichiometric composition of the precursor and the electron induced decomposition paths can be very different from those expected from calculations or thermal decomposition. The dissociation mechanism is one of the key factors determining the purity of the deposits and a better understanding of this process will help develop electron beam induced deposition into a viable nanofabrication technique.

Resists for sub-20-nm electron beam lithography with a focus on HSQ: state of the art

In the past decade, the feature size in ultra large-scale integration (ULSI) has been continuously decreasing, leading to nanostructure fabrication. Nowadays, various lithographic techniques ranging from conventional methods (e.g. photolithography, x-rays) to unconventional ones (e.g. nanoimprint lithography, self-assembled monolayers) are used to create small features. Among all these, resist-based electron beam lithography (EBL) seems to be the most suitable technique when nanostructures are desired. The achievement of sub-20-nm structures using EBL is a very sensitive process determined by various factors, starting with the choice of resist material and ending with the development process. After a short introduction to nanolithography, a framework for the nanofabrication process is presented. To obtain finer patterns, improvements of the material properties of the resist are very important. The present review gives an overview of the best resolution obtained with several types of both organic and inorganic resists. For each resist, the advantages and disadvantages are presented. Although very small features (2-5 nm) have been obtained with PMMA and inorganic metal halides, for the former resist the low etch resistance and instability of the pattern, and for the latter the delicate handling of the samples and the difficulties encountered in the spinning session, prevent the wider use of these e-beam resists in nanostructure fabrication. A relatively new e-beam resist, hydrogen silsesquioxane (HSQ), is very suitable when aiming for sub-20-nm resolution. The changes that this resist undergoes before, during and after electron beam exposure are discussed and the influence of various parameters (e.g. pre-baking, exposure dose, writing strategy, development process) on the resolution is presented. In general, high resolution can be obtained using ultrathin resist layers and when the exposure is performed at high acceleration voltages. Usually, one of the properties of the resist material is improved to the detriment of another. It has been demonstrated that aging, baking at low temperature, immediate exposure after spin coating, the use of a weak developer and development at a low temperature increase the sensitivity but decrease the contrast. The surface roughness is more pronounced at low exposure doses (high sensitivity) and high baking temperatures. A delay between exposure and development seems to increase both contrast and the sensitivity of samples which are stored in a vacuum after exposure, compared to those stored in air. Due to its relative novelty, the capabilities of HSQ have not been completely explored, hence there is still room for improvement. Applications of this electron beam resist in lithographic techniques other than EBL are also discussed. Finally, conclusions and an outlook are presented.

The role of secondary electrons in electron-beam-induced-deposition spatial resolution

Abstract Electron-beam-induced-deposition (EBID) is a versatile direct writing technique occasionally used in micro- and nanofabrication. We focus in our study on the EBID spatial resolution, defined as the lateral size of the smallest deposited structure. The lateral size of dot structures always exceeds the diameter of the electron probe. Many authors have argued that this is due to the secondary electrons emitted as a result of primary electron bombardment, but it has never been modeled quantitatively. We developed a model based on Monte Carlo methods that simulates the role of secondary electrons in the spatial evolution of EBID dots. The results show that the secondary electrons are indeed responsible for the shapes and sizes observed during EBID. The secondary electrons generated inside the substrate by a pin-point primary beam produce initially a very small structure broadening, of about one nanometer. Then using a dynamic Monte Carlo profile simulator which includes the electron scattering in the already grown tip structure, we show for the first time that the laterally emerging secondary electrons are continuously enlarging the tip diameter, up to saturation values of 20–30 nm, in agreement with experiments.

Direct fabrication of nanowires in an electron microscope

Electron-beam-induced deposition (EBID) is a potentially fast and resistless deposition technique which might overcome the fundamental resolution limits of conventional electron-beam lithography. We advance the understanding of the EBID process by simulating the structure growth. The merit of our model is that it explains the shapes of structures grown by EBID quantitatively. It also predicts the possibility to directly fabricate structures with lateral sizes smaller than 10 nm and points out the ideal conditions to achieve this goal. We verify these predictions by fabricating sub-10-nm lines and dots in a state-of-the-art scanning transmission electron microscope.

Spatial resolution limits in electron-beam-induced deposition

Electron-beam-induced deposition (EBID) is a versatile micro- and nanofabrication technique based on electron-induced dissociation of metal-carrying gas molecules adsorbed on a target. EBID has the advantage of direct deposition of three-dimensional structures on almost any target geometry. This technique has occasionally been used in focused electron-beam instruments, such as scanning electron microscopes, scanning transmission electron microscopes (STEM), or lithography machines. Experiments showed that the EBID spatial resolution, defined as the lateral size of a singular deposited dot or line, always exceeds the diameter of the electron beam. Until recently, no one has been able to fabricate EBID features smaller than 15–20?nm diameter, even if a 2-nm-diam electron-beam writer was used. Because of this, the prediction of EBID resolution is an intriguing problem. In this article, a procedure to theoretically estimate the EBID resolution for a given energetic electron beam, target, and gaseous precursor is described. This procedure offers the most complete approach to the EBID spatial resolution problem. An EBID model was developed based on electron interactions with the solid target and with the gaseous precursor. The spatial resolution of EBID can be influenced by many factors, of which two are quantified: the secondary electrons, suspected by almost all authors working in this field, and the delocalization of inelastic electron scattering, a poorly known effect. The results confirm the major influence played by the secondary electrons on the EBID resolution and show that the role of the delocalization of inelastic electron scattering is negligible. The model predicts that a 0.2-nm electron beam can deposit structures with minimum sizes between 0.2 and 2?nm, instead of the formerly assumed limit of 15–20?nm. The modeling results are compared with recent experimental results in which 1-nm?W dots from a W(CO)6 precursor were written in a 200-kV STEM on a 30-nm SiN membrane.

Focused Electron-Beam-Induced Deposition of 3 nm Dots in a Scanning Electron Microscope

Electron-beam-induced deposition allows the creation of three-dimensional nanodevices within a scanning electron microscope. Typically the dimensions of the fabricated structure are from 20 nm to several micrometers. Until now the record for the smallest deposited feature in an SEM was 3.5 nm, measured by an indirect method. We have achieved a nanodot having a full width half-maximum of 2.8 +/- 0.3 nm, measured directly in the same microscope after deposition.

Electron induced dissociation of trimethyl (methylcyclopentadienyl) platinum (IV): Total cross section as a function of incident electron energy

The total cross section has been measured for the electron induced dissociation of trimethyl (methylcyclopentadienyl) platinum (IV) [MeCpPt(IV)Me3], a Pt precursor often used in focused electron beam induced processing (FEBIP), for incident electron energies ranging between 3–3 keV. Measurements were performed for the precursor in the adsorbed state under ultrahigh vacuum conditions. The techniques used in this study were temperature programmed desorption, x-ray photoelectron spectroscopy and mass spectrometry. Two surfaces were used in these experiments, amorphous carbon overlayers containing embedded Pt atoms (a:C-Pt), formed by the electron decomposition of the Pt precursor, and atomically clean Au. The results from these three experiments revealed a comparatively low total cross section at 8 eV (4.2+/-0.3xE?17 cm2 on the a:C-Pt and 1.4+/-0.1xE?17 cm2 on the Au) that increases with increasing incident electron energy, reaching a maximum at around 150 eV (4.1+/-0.5xE?16 cm2 on the a:C-Pt and 2.3+/-0.2xE?16 cm2 on the clean Au), before decreasing at higher incident electron energies, up to 3000 eV. Differences in the measured cross sections between Au and a:C-Pt surfaces demonstrate that the substrate can influence the reaction cross section of adsorbed species. Temperature programmed desorption was also used to measure the adsorption energy of MeCpPt(IV)Me3, which was found to depend on both the substrate and the adsorbate coverage. The work in this paper demonstrates that surface science techniques can be used to quantitatively determine the total cross section of adsorbed FEBIP precursors for electron induced dissociation as a function of incident electron energy. These total cross section values are necessary to obtain quantitatively accurate information from FEBIP models and to compare the reaction efficiencies of different precursors on a quantitative basis. (doi:10.1063/1.3225091)

Determination of line edge roughness in low-dose top-down scanning electron microscopy images

We investigated the off-line metrology for line edge roughness (LER) determination by using the discrete power spectral density (PSD). The study specifically addresses low-dose scanning electron microscopy (SEM) images in order to reduce the acquisition time and the risk of resist shrinkage. The first attempts are based on optimized elliptic filtering of noisy experimental SEM images, where we use threshold-based peak detection to determine the edge displacements. The effect of transversal and longitudinal filterings cannot be ignored, even when considering an optimized filter strength. We subsequently developed a method to detect the edge displacements without the use of a filter and thus avoiding biasing. This makes it possible to study how much image noise is acceptable and still determine the LER. The idea is to generate random images of line edges using the model of Palasantzas and the algorithm of Thorsos. We study the simulated PSDs as a function of the number of line edges and report on the convergence of the parameters (LER, correlation length, and roughness exponent) by fitting the Palasantzas model extended with a white noise term. This study demonstrates that a very noisy image with 12 line edges and about 2 electrons per pixel on average (charge density ≈10  μC) already produces an estimation for LER with a relative error (one-sigma) of about 10%. Furthermore, increasing the dose beyond 20 electrons per pixel does not significantly improve the LER determination.

Ultrahigh resolution focused electron beam induced processing: the effect of substrate thickness

It is often suggested that the growth in focused electron beam induced processing (FEBIP) is caused not only by primary electrons, but also (and even predominantly) by secondary electrons (SEs). If that is true, the growth rate for FEBIP can be changed by modifying the SE yield. Results from our Monte Carlo simulations show that the SE yield changes strongly with substrate thickness for thicknesses below the SE escape depth. However, our experimental results show that the growth rate is independent of the substrate thickness. Deposits with an average size of about 3 nm were written on 1 and 9 nm thick carbon substrates. The apparent contradiction between simulation and experiment is explained by simulating the SE emission from a carbon substrate with platinum deposits on the surface. It appears that the SE emission is dominated by the deposits rather than the carbon substrate, even for deposits as small as 0.32 nm(3).

Solutions to a proximity effect in high resolution electron beam induced deposition

A new type of proximity effect in electron beam induced deposition (EBID) is presented. Proximity effects are well known in resist based electron beam lithography (EBL), where they present themselves as an extra and unintentional exposure of the resist layer surrounding the irradiated areas. Several types of proximity effects have already been reported for EBID, which are of a different nature. The authors report a proximity effect where the amount of deposited mass increases with each new line that is deposited. This effect occurs when parallel lines are deposited at a spacing close to the width of the lines. The increase in deposition rate was found to be dependent on the angle between the irradiated target and the incident electron beam. Results from a simulation based on this model qualititatively show the same trend. A successful strategy for reducing the effect is presented.