Ellipsometry is an optical technique for investigating the dielectric properties (complex refractive index or dielectric function) of thin films. Ellipsometry measures the change of polarization upon reflection or transmission and compares it to a model.
It can be used to characterize composition, roughness, thickness (depth), crystalline nature, doping concentration, electrical conductivity and other material properties. It is very sensitive to the change in the optical response of incident radiation that interacts with the material being investigated.
A spectroscopic ellipsometer can be found in most thin film analytical labs. Ellipsometry is also becoming more interesting to researchers in other disciplines such as biology and medicine. These areas pose new challenges to the technique, such as measurements on unstable liquid surfaces and microscopic imaging.
Etymology The name "ellipsometry" stems from the fact that elliptical polarization of light is used. The term "spectroscopic" relates to the fact that the information gained is a function of the light's wavelength or energy (spectra). The technique has been known at least since 1888 by the work of Paul DrudeP. Drude, Ueber die Gesetze der Reflexion und Brechung des Lichtes an der Grenze absorbirender Krystalle, Annalen der Physik, Volume 268, Issue 12, 1887, Pages: 584–625, DOI: 10.1002/andp.18872681205; Ueber Oberflächenschichten. I. Theil, Annalen der Physik, Volume 272, Issue 2, 1889, Pages: 532–560, DOI: 10.1002/andp.18892720214; Ueber Oberflächenschichten. II. Theil, Annalen der Physik, Volume 272, Issue 4, 1889, Pages: 865–897, DOI: 10.1002/andp.18892720409 (in German). and has many applications today.
The first documented use of the term "ellipsometry" was in 1945.
Basic principles The measured signal is the change in polarization as the incident radiation (in a known state) interacts with the material structure of interest (reflected, absorbed, scattered, or transmitted). The polarization change is quantified by the amplitude ratio, Ψ, and the phase difference, Δ (defined below). Because the signal depends on the thickness as well as the material properties, ellipsometry can be a universal tool for contact free determination of thickness and optical constants of films of all kinds.
Upon the analysis of the change of polarization of light, ellipsometry can yield information about layers that are thinner than the wavelength of the probing light itself, even down to a single atomic layer. Ellipsometry can probe the complex refractive index or dielectric function tensor, which gives access to fundamental physical parameters like those listed above. It is commonly used to characterize film thickness for single layers or complex multilayer stacks ranging from a few angstroms or tenths of a nanometer to several micrometers with an excellent accuracy.
Experimental details Typically, ellipsometry is done only in the reflection setup. The exact nature of the polarization change is determined by the sample's properties (thickness, complex refractive index or dielectric function tensor). Although optical techniques are inherently diffraction-limited, ellipsometry exploits phase information (polarization state), and can achieve sub-nanometer resolution. In its simplest form, the technique is applicable to thin films with thickness of less than a nanometer to several micrometers. Most models assume the sample is composed of a small number of discrete, well-defined layers that are optically homogeneous and isotropic. Violation of these assumptions requires more advanced variants of the technique (see below).
Methods of immersion or multiangular ellipsometry are applied to find the optical constants of the material with rough sample surface or presence of inhomogeneous media. New methodological approaches allow the use of reflection ellipsometry to measure physical and technical characteristics of gradient elements in case the surface layer of the optical detail is inhomogeneous.
Experimental setup
Electromagnetic radiation is emitted by a light source and linearly polarized by a polarizer. It can pass through an optional compensator (retarder, quarter wave plate) and falls onto the sample. After reflection the radiation passes a compensator (optional) and a second polarizer, which is called an analyzer, and falls into the detector. Instead of the compensators, some ellipsometers use a phase-modulator in the path of the incident light beam. Ellipsometry is a specular optical technique (the angle of incidence equals the angle of reflection). The incident and the reflected beam span the plane of incidence. Light which is polarized parallel to this plane is named p-polarized. A polarization direction perpendicular is called s-polarized (s-polarised), accordingly. The "s" is contributed from the German "" (perpendicular).
Data acquisition Ellipsometry measures the complex reflectance ratio of a system, which may be parametrized by the amplitude component and the phase difference . The polarization state of the light incident upon the sample may be decomposed into an s and a p component (the s component is oscillating perpendicular to the plane of incidence and parallel to the sample surface, and the p component is oscillating parallel to the plane of incidence). The amplitudes of the s and p components, after reflection and normalized to their initial value, are denoted by and respectively. The angle of incidence is chosen close to the Brewster angle of the sample to ensure a maximal difference in and .Butt, Hans-Jürgen, Kh Graf, and Michael Kappl. "Measurement of Adsorption Isotherms". Physics and Chemistry of Interfaces. Weinheim: Wiley-VCH, 2006. 206-09. Ellipsometry measures the complex reflectance ratio (a complex quantity), which is the ratio of over :
Thus, is the amplitude ratio upon reflection, and is the phase shift (difference). It is helpful to note that the right side of the equation is another way to represent a complex number. Since ellipsometry is measuring the ratio (or difference) of two values rather than the absolute value of either, it is less sensitive to variation than other optical techniques, making it robust and reproducible. For instance, it is relatively insensitive to scatter and fluctuations and requires no standard sample or reference beam.
Data analysis Ellipsometry is an indirect method, i.e. in general the measured and cannot be converted directly into the optical constants of the sample. Normally, a model analysis must be performed, for example the Forouhi Bloomer model. This is one weakness of ellipsometry. Models can be physically based on energy transitions or simply free parameters used to fit the data.
Direct inversion of and is only possible in very simple cases of isotropic, homogeneous and infinitely thick films. In all other cases a layer model must be established, which considers the optical constants (refractive index or dielectric function tensor) and thickness parameters of all individual layers of the sample including the correct layer sequence. Using an iterative procedure (least-squares minimization) unknown optical constants and/or thickness parameters are varied, and and values are calculated using the Fresnel equations. The calculated and values which match the experimental data best provide the optical constants and thickness parameters of the sample.
Definitions Modern ellipsometers are complex instruments that incorporate a wide variety of radiation sources, detectors, digital electronics and software. The range of wavelength employed may be far in excess of what is visible to human eyes.
Single-wavelength vs. spectroscopic ellipsometry Single-wavelength ellipsometry (SWE) employs a monochromatic light source, which is usually a laser in the visible spectral region, for instance, a HeNe laser with a wavelength of 632.8 nm. Therefore, single-wavelength ellipsometry is also called laser ellipsometry. The advantage of laser ellipsometry is that laser beams can be focused on a small spot size, and is more precise than Spectroscopic ellipsometry. Furthermore, lasers have a higher power than broad band light sources. Therefore, laser ellipsometry can be used for imaging (see below). However, the experimental output is restricted to only two parameters (one set of and values per measurement). Due to these limitations, SWE is limited to a single layer system.
By contrast Spectroscopic ellipsometry (SE) employs broad band light sources, which cover the infrared, visible and/or ultraviolet spectral region. By that the complex refractive index or the dielectric function tensor in the corresponding spectral region can be obtained. Infrared spectroscopic ellipsometry (IRSE) can probe lattice vibrational (phonon) and free charge carrier (plasmon) properties. Spectroscopic ellipsometry in the near infrared, visible up to ultraviolet spectral region studies the refractive index in the transparency or below-band-gap region and electronic properties, for instance, band-to-band transitions or excitons. When measuring thickness, lower wavelength ranges are utilized for thinner films, while longer wavelength ranges (for example Infrared) are utilized for thicker films.
Standard vs. generalized ellipsometry (anisotropy) Standard ellipsometry (often shortened to 'ellipsometry') is applied when no s polarized light is converted into p polarized light or vice versa. This is the case for optically isotropic samples, for instance, amorphous materials or crystalline materials with a cubic crystal structure. Standard ellipsometry is also sufficient for optically uniaxial samples in the special case, when the optical axis is aligned parallel to the surface normal. In all other cases, when s polarized light is converted into p polarized light and/or vice versa, the generalized ellipsometry approach must be applied. Examples are arbitrarily aligned, optically uniaxial samples, or optically biaxial samples.
Jones matrix vs. Mueller matrix formalism (depolarization) There are typically two different ways of mathematically describing how an electromagnetic wave interacts with the elements within an ellipsometer (including the sample): the Jones matrix and the Mueller matrix formalisms. In the Jones matrix formalism, the electromagnetic wave is described by a Jones vector with two orthogonal complex-valued entries for the electric field (typically and ), and the effect that an optical element (or sample) has on it is described by the complex-valued 2×2 Jones matrix. In the Mueller matrix formalism, the electromagnetic wave is described by Stokes vectors with four real-valued entries, and their transformation is described by the real-valued 4x4 Mueller matrix. When no depolarization occurs both formalisms are fully consistent. Therefore, for non-depolarizing samples, the simpler Jones matrix formalism is sufficient. If the sample is depolarizing the Mueller matrix formalism should be used, because it also gives the amount of depolarization. Reasons for depolarization are, for instance, thickness non-uniformity or backside-reflections from a transparent substrate.
Advanced experimental approaches
Imaging ellipsometry
Imaging ellipsometry (IE) extends classical ellipsometry by integrating an objective lens and an image sensor (e.g. CCD or CMOS image sensor). The objective lens projects the illuminated sample area onto the detector, which enables real-time high-contrast visualization and spatially resolved ellipsometry measurements. IE is particularly suited for structured or inhomogeneous thin-film samples. It provides detailed information about film thickness distributions, surface uniformity, and dynamic processes such as molecular adsorption or film growth. IE combines the quantitative precision of ellipsometry with the lateral resolution of microscopy.