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Introduction
Rutherford Backscattering (RBS) is based on collisions between atomic nuclei and derives its name from Lord Ernest Rutherford, who in 1911 was the first to present the concept of atoms having nuclei. It involves measuring the number and energy of ions in a beam which backscatter after colliding with atoms in the near-surface region of a sample at which the beam has been targeted. With this information, it is possible to determine atomic mass and elemental concentrations versus depth below the surface. RBS is ideally suited for determining the concentration of trace elements heavier than the major constituents of the substrate. Its sensitivity for light masses, and for the makeup of samples well below the surface, is poor. When a sample is bombarded with a beam of high energy particles, the vast majority of particles are implanted into the material and do not escape. This is because the diameter of an atomic nucleus is on the order of 1e-15 m while the spacing between nuclei is on the order of 2e-10 m. A small fraction of the incident particles do undergo a direct collision with a nucleus of one of the atoms in the upper few micrometers of the sample. This "collision" does not actually involve direct contact between the projectile ion and target atom. Energy exchange occurs because of Coulombic forces between nuclei in close proximity to each other. However, the interaction can be modeled accurately as an elastic collision using classical physics. The energy measured for a particle backscattering at a given angle depends upon two processes. Particles lose energy while they pass through the sample, both before and after a collision. The amount of energy lost is dependent on that material's stopping power. A particle will also lose energy as the result of the collision itself. The collisional lost depends on the masses of the projectile the target atoms. The ratio of the energy of the projectile before and after collision is called the kinematic factor. The number of backscattering events that occur from a given element in a sample depend upon two factors: the concentration of the element and the effective size of its nucleus. The probability that a material will cause a collision is called its scattering cross section.
between two heavy elements. RBS has good mass resolution for light elements, but poor mass resolution for heavy elements. For example, when He++ strikes light elements such as C, N, or O, a significant fraction of the projectile's energy is transferred to the target atom and the energy recorded for that backscattering event is much lower than the energy of the beam. It is usually possible to resolve C from N or P from Si, even though these elements differ in mass by only about 1 amu. However, as the mass of the atom being struck increases, a smaller and smaller portion of the projectile energy is transferred to the target during collision, and the energy of the backscattered atom asymptotically approaches the energy of the beam. It is not possible to resolve W from Ta, or Fe from Ni when these elements are present at the same depths in the sample, even though these heavier elements also differ in mass by only about 1 amu. An important related issue is that He will not scatter backwards from H or He atoms in a sample. Elements as light as or lighter than the projectile element will instead scatter at forward trajectories with significant energy. Thus, these elements cannot be detected using classical RBS. However, by placing a detector so that these forward scattering events can be recorded, these elements can be quantitatively measured using the same principles as RBS.
The illustration shows relative yields for He backscattering from selected elements at an incident He energy of 2 MeV. The energies for He backscattering from these elements when present at the surface of a sample are also displayed. The graph indicates that RBS is over 100 times more sensitive for heavy elements than for light elements, due to the larger scattering cross sections of the heavier elements.
The figure illustrates the interaction between the kinematic factor and the scattering cross section. The two spectra come from two TaSi films of different Ta/Si compositions on Si substrates. In this example, one of the films is 230 nm thick, while the other film is 590 nm thick. The experiment uses an ion beam of He++ at 2.2 MeV. In both spectra, the high energy peak arises by scattering from tantalum in the TaSi film layer. The peak at lower energy is from silicon, which appears in both the TaSi film on the surface and in the Si substrate. Silicon is much less likely to cause scattering events than tantalum due to its smaller scattering cross section. To make the features of the silicon signal in these two spectra easily discernible, the silicon peaks have been multiplied by five. For scattering at the sample surface, the only energy loss is due to momentum transfer to the target atom. The high energy edge of the tantalum peaks near 2.1 MeV corresponds to backscattering from Ta at the surface. The high energy edge of the silicon peaks near 1.3 MeV corresponds to backscattering from Si at the surface.
The height of a backscattering peak for a given layer is inversely proportional to the stopping cross section for that layer. The stopping cross section of TaSi is known to be only 1.37 times that of Si. This explains why the height of the peak corresponding to Si in the TaSi layer is less than one-half the height of the peak corresponding to Si in the substrate, even for a film with a Si:Ta ratio of 2:3.
can be quite pronounced. If energy straggling is not taken into account, then sloping edges of peaks can be misinterpreted as intermixing between two layers. The accuracy of depth resolution depends on how accurately the contribution of straggling can be calculated.
raised about the accuracy of the technique. Whenever the actual density of a film is significantly different than the density assumed in an RBS calculation, the thickness obtained by RBS will diverge significantly from the thickness obtained by another technique. It is useful to note that
where TRBS is the thickness obtained by RBS, and D RBS is the density assumed when calculating the RBS thickness, TReal and DReal are the actual film thickness and density, and atoms/cm2 is the two-dimensional concentration of atoms in the film (the concentration which can be accurately calculated from the RBS results without making any assumptions). Another useful feature of RBS is that since RBS will provide an accurate concentration of the total atoms/cm which are present in a film, if the actual thickness of the film can be measured by another method, then the density of the film can be calculated.
Rutherford backscattering spectrometry (RBS) is the measurement of energies of these backscattered particles. These energies depend on the identity of the atom from which the alpha particle scatters, the angle of scatter, and the depth into the sample to which the particle travels before scattering. Thus, RBS can be used for elemental analysis, especially of surfaces. One early use of RBS (called the alpha-scattering experiment at the time) was elemental analysis of lunar soils as part of the Surveyor V scientific payload in 1967. Most early RBS experiments used radioactive sources of alpha particles. Today, the intense pencil like beam of alpha particles required to produce a modest backscattered signal is most commonly provided by a charged particle accelerator
The tandem accelerator is a clever innovation. The tandem accelerator uses a positive terminal located in the center of the device. Negatively charged particles are injected into the accelerator and attracted to the terminal where a stripper element removes two or more electrons from each particle. The positive terminal repels the resulting positive ion back toward ground. Thus the particle acquires energy both before and after the terminal.
The tandem configuration has two important advantages over a single-stage setup. First, lower terminal voltages are required, and second, both the source and the ion exit operate near ground potential. The main disadvantage is that inefficiencies of He- production and charge stripping lower He++ beam current to about 100 nA for a tandem versus 1 mA for a single-ended accelerator. Fortunately, most RBS experiments can only use about 100 nA because of detector limitations. A typical RBS installation uses a tandem accelerator, producing a 2.25 MeV He++ beam by removing three electrons from He- at the + 750 KV terminal.
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A charged particle beam line in a tank containing high voltage components and an insulating gas. An electrode called the terminal supplied by a high voltage source. An electron charge stripper located at the terminal. A vacuum system for the charge stripper and beam line.
Although large accelerators can often fill entire halls, smaller accelerators are suitable for RBS. Such accelerators require investments in the $300,000 range, and suitable end stations for analysis and control cost an additional $50,000 to $200,000. While these are certainly expensive devices, they are not out of line with other analytical instruments.
A well-known variation is the Pelletron which is identical to a Van de Graaff, except that a chain with alternate links (pellets) of metal and insulator replaces the belt. This chain provides more uniform charge transport than the belt, resulting in more stable voltage. A Tandetron accelerator uses a voltage doubler power supply fed by a radio frequency signal. There are no moving parts, reducing the need for expensive maintenance. The voltage from the Tandetron device is also very stable. Terminal voltage stability influences spectroscopic resolution.
arranged to minimize electric fields. Thus, one guiding principle of accelerator design is elimination of any sharp points or edges that produce high electric fields. The high voltage components are housed in a pressure vessel filled with sulfur hexafluoride gas (SF6) because this gas resists electrical breakdown better than air. The terminal and the beam line require mechanical support, a more demanding task because of the forces exerted by the pulley used as one end of a Van de Graaff or Pelletron voltage source. The beam line consists of alternating insulator and conductor sections connected to the terminal voltage along a resistor chain to linearize the electrical potentials and reduce electric fields between components. The beam line and the terminal are surrounded by a series of smooth conducting rings also connected along a resistor chain to the terminal voltage. These precautions serve to reduce voltage gradients between accelerator components and thus minimize electric fields. The precautions are necessary because the 750 kV terminal has the potential to produce very large sparks.
Because of the pressures required to maintain a gas cell, pressures in the flight tube (measured at the end of the accelerator) rise into the 1 to 10 microtorr range. Lower pressures are possible with a stripper foil. However, the modest collisional cross section of high energy ions with gas molecules diminishes the requirement for high vacuum in RBS experiments.
Tandem accelerators require negative helium ions. Helium is the most inert of the inert gases; it tends not to gain or lose electrons. The ion source must overcome this natural tendency of helium not to form negative ions. The source operates in two stages. First, positive ions are produced as described above. An alkali metal channel converts He+ into He- in a second stage. This charge exchange happens as He+ passes through hot alkali metal vapor. Rubidium is used in the illustration, but all of the alkali metals have sufficient reducing power to form He-. The charge exchange process is inefficient; 1 milliamp of He+ leads to 1 microamp of He-. The negative ions are extracted from the alkali metal channel and injected into the tandem accelerator at 20 to 30 keV.
Samples in RBS can be insulating, in contrast to most charged particle analytical methods. Even if such samples charge to a few kilovolts, the rigid beam is barely deflected. Sample charging causes only slight perturbations in RBS spectra because the kilovolt charging effect is a small fraction of the megavolt particle energies.
The main sample chamber components are a stage, one or more detectors,a beam entrance, and the vacuum system. The chamber can be as simple asa flange with a sample and a single energy dispersive spectrometer attached.
More typically, the samples mount on a five-axis goniometer, which isconvenient for loading many samples into the vacuum system and analyzingthem sequentially. The goniometer can also tilt and rotate the samples.Comparing spectra obtained at different incident and exit beam angles providesbetter characterization of sample composition as a function of depth. Randomlytilting and rotating a sample relative to the incident beam avoids variationsin the spectrum that arise because the incident beam travels down a channelin the sample's crystal structure. Two surface barrier detectors (one normal angle, one grazing exit), are included in a typical RBS sample chamber.
The average energy expended by He++ to produce one electron-hole pair is approximately 3.7 eV. This is sometimes called the ionization energy of the detector. Each 1 MeV particle produces about 2700 electron-hole pairs. The fluctuation or variance in the number of charge carriers affects the spectroscopic resolution. The theoretical minimum variance (which follows Poisson statistics) is equal to the number of charge carriers. The standard deviation equals the square root of the variance. The Fano factor is the ratio of the observed to this theoretical minimum variance. The Fano factor implicates other sources of peak broadening, typically incomplete charge collection and variations in dead layer loss. Incomplete charge collection is minimized by high purity semiconductors which provide relatively few sites for electron-hole pair recombination. The energy lost before the charged particle reaches the active volume of the detector (dead layer loss) is minimal because this layer is thin (about 100 nanometer) in surface barrier detectors. Since this thickness corresponds to only about 0.4% energy loss for 1 MeV He++, small variations in the energy loss are insignificant for typical RBS experiments. High quality silicon surface barrier detectors are thus nearly ideal for alpha particle spectroscopy. Particle arrival times at the detector are randomly spaced in time, leading to the possibility of interference between measurements when particles arrive at nearly the same time. This phenomenon, called pulse pile-up, becomes a serious problem at high particle arrival rates. There are two types of pile-up. Tail pile-up involves the superposition of pulses on the long duration tail or undershoot from a preceding pulse, leading to reduced spectral resolution. High quality electronic circuits minimize tail pile-up. Two pulses sufficiently close together to be treated as a single pulse undergo peak pile-up, the second type. Detector dead time is the minimum time between successive ion arrivals if they are to be measured separately. Peak pile-up ultimately limits the rate at which RBS data collection can occur.
gives rise to X-ray fluorescence spectroscopy. Electron excitation in a scanning electron microscope or an electron microprobe provides energy dispersive or wavelength dispersive Xray spectroscopy (depending on the X-ray detector). Charged particle beams of He ++, or more commonly H+, afford PIXE spectroscopy. In all three cases, the excitation beam removes a core electron and X-rays are emitted with specific energies when outer shell electrons change state to inner shell. The X-ray energies are independent of the excitation process. The PIXE accessory is useful for heavy element identification on RBS instruments. These heavy elements have small differences in RBS energies, but distinct differences in PIXE spectra. Dedicated PIXE instruments usually use H+ rather than He++ because H+ provides higher sensitivity. If helium and hydrogen are mixed in the source, He ++-based RBS and H+-based PIXE can be performed with the same accelerator. PIXE has several advantages as an analytic technique. It offers signal levels similar to its electron beam counterparts, but better signal-to-background ratios. The background in electron spectroscopy arises from bremsstrahlung which is largely absent in PIXE because He+ + or H+ ions, even at PIXE energies, have much lower velocities than electrons. Another advantage of PIXE over electron induced spectroscopy is that, like RBS, PIXE works with insulating samples. Finally, a proton beam can pass through a thin window and penetrate several centimeters through air. Because of this, unusual samples, such as valuable art work, need not be subjected to the rigors of a vacuum. PIXE finds applications in geology, archaeology, and art conservation. [Top]
The accelerators and detectors are the same for HIBS and RBS, but different ion sources are required. A typical heavy ion source uses a sputtering Cs + beam impinging on a heavy element such as silicon from which negative ions (Si - in this example) are extracted. The charge stripper removes a variable number of electrons from Si -, leaving ions with mixed charge states and energies. The primary ion beam must be separated into components, usually in a magnetic field, before the beam strikes the sample. [Top]