Temperature-dependent Ellipsometry Research Articles

Temperature-dependent generalized ellipsometry of the metal–insulator phase transition in low-symmetry charge-transfer salts

Determining the optical and electronic properties of strongly anisotropic materials with symmetries below orthorhombic remains challenging; generalized ellipsometry is a powerful technique in this regard. Here, we employ Mueller matrix spectroscopic and temperature-dependent ellipsometry to determine the frequency dependence of six components of the dielectric-function tensor of the two-dimensional charge-transfer salt α-(BEDT-TTF)2I3 across its metal–insulator transition. Our results offer valuable insights into temperature-dependent changes of the components of the spectroscopic dielectric-function tensor across the metal–insulator transition. This advanced method allows extension to other electronic transitions.

Thermal and optical properties of P3HT:PC70BM:ZnO nanoparticles composite films

The results of studies on the influence of zinc oxide nanoparticles (ZnO-NPs) on the structural, thermal and optical properties of thin films of mixtures of phenyl-C71-butyric acid methyl ester (PCBM) with poly[3-hexylthiophene] (P3HT) of various molecular weights are described in this article. The structural properties of the layers of: polymers, mixtures of polymers with fullerenes and their composites with ZnO-NPs were investigated using X-ray diffraction. Whereas their glass transition temperature and optical parameters have been determined by temperature-dependent spectroscopic ellipsometry. The presence of ZnO-NPs was also visible in the images of the surface of the composite layers obtained using scanning electron microscopy. These blends and composite films have also been used as the active layer in bulk heterojunction photovoltaic structures. The molecular weight of P3HT (Mw = 65.2; 54.2 and 34.1 kDa) and the addition of nanoparticles affected the power conversion efficiency (PCE) of the obtained solar cells. The determined PCE was the highest for the device prepared from the blend of P3HT:PCBM with the polymer of the lowest molecular weight. However, solar cells with ZnO-NPs present in their active layer had lower efficiency, although the open-circuit voltage and fill factor of almost all devices had the same values whether they contained ZnO-NPs or not. It is worth noting that thermal studies carried out using temperature-dependent ellipsometry showed a significant effect of the presence of ZnO-NPs on the value of the glass transition temperature, which was higher for composite films than for films made of a polymer-fullerene blend alone.

Time-Resolved Temperature Mapping Leveraging the Strong Thermo-Optic Effect in Phase-Change Materials.

Optical phase-change materials are highly promising for emerging applications such as tunable metasurfaces, reconfigurable photonic circuits, and non-von Neumann computing. However, these materials typically require both high melting temperatures and fast quenching rates to reversibly switch between their crystalline and amorphous phases: a significant challenge for large-scale integration. In this work, we use temperature-dependent ellipsometry to study the thermo-optic effect in GST and use these results to demonstrate an experimental technique that leverages the thermo-optic effect in GST to enable both spatial and temporal thermal measurements of two common electro-thermal microheater designs currently used by the phase-change community. Our approach shows excellent agreement between experimental results and numerical simulations and provides a noninvasive method for rapid characterization of electrically programmable phase-change devices.

Spectroscopic ellipsometry from 10 to 700 K

Abstract The temperature dependence of the optical constants of materials (refractive index, absorption and extinction coefficients, and dielectric function) can be determined with spectroscopic ellipsometry over a broad range of temperatures and photon energies or wavelengths. Such results have practical value, for example for applications of optical materials at cryogenic or elevated temperatures. The temperature dependence of optical gaps and their broadenings also provides insight into the scattering of electrons and holes with other quasiparticles, such as phonons or magnons. This review presents a detailed discussion of the experimental considerations for temperature-dependent ellipsometry and selected results for insulators, semiconductors, and metals in the infrared to ultraviolet spectral regions.

Semiconductor-to-metal transition in atomic layer deposition (ALD) of VO2 films using VCl4 and water

The semiconductor-to-metal transition of vanadium dioxide (VO2) films is studied using temperature-dependent Raman, optical, and electrical measurements. The VO2 films are deposited via an atomic layer deposition (ALD) process using alternate pulses of vanadium tetrachloride and H2O at 350 °C. A growth rate of 0.021 nm/cycle and a thickness of 33 nm of VO2 are obtained for all films studied. The phase of the film is determined using x-ray diffraction. The as-deposited films are amorphous and are transformed to the monoclinic phase with a post-deposition, forming gas anneal at temperatures ≥ 500 °C for 60 min. The purity of the films is determined using x-ray photoelectron spectroscopy and no evidence of residual chlorine is detected. The temperature-dependent Raman Ag mode of the monoclinic VO2 phase is observed to monotonically decrease from 25 °C to 78 °C; where no evidence of the Ag peak is observed in the film beyond 68 °C. The refractive index and extinction coefficient extracted from temperature-dependent ellipsometry confirm that, beyond 68 °C, free carriers are generated in the film. Electrical measurements performed on a fabricated p++Si/VO2/Ti/Au device show a semiconductor-to-metal transition behavior with a high resistance of 14701 ± 2284 Ω at 62 °C and a low resistance of 1064.1 ± 143 Ω at 67 °C. This work demonstrates that a halide-based ALD process provides a clean and robust approach to synthesizing high-quality VO2 films.

Effects of annealing temperature, thickness and substrates on optical properties of m-plane ZnO films studied by photoluminescence and temperature dependent ellipsometry

A series of m-plane ZnO films grown on sapphire and Si substrates with different thicknesses (186–371 nm) and different annealing temperatures (150–200 °C) were studied in detail by comparing X-ray diffraction, photoluminescence and spectroscopic ellipsometry measurements. The impact of thickness, annealing temperature and substrates on optical properties was investigated by the systematical analysis of the highly correlated stain, grain size, exciton effect, absorption tailing and crystallinity. Our finding indicates that the improvement of crystal quality along with the increase of grain size and refractive index for m-plane ZnO can be observed with increasing annealing temperature, increasing thickness or by introducing sapphire instead of Si substrate. The refractive index and bandgap have stronger dependence on annealing temperature than on thickness, causing the blue-shift of bandgap with rising annealing temperature despite thicker film. This bandgap shift is more pronounced for ZnO in ZnO/Si system. Photoluminescence combined with ellipsometry analysis demonstrate that higher annealing temperature can strengthen the excitonic feature. Bose-Einstein equation, employed to fit the dependence of bandgap on experimental temperature (300–583 K) illustrates that, the reduction of bandgap at elevated temperatures is more significant for ZnO in ZnO/sapphire system due to the corresponding stronger electron/exciton-phonon interactions involved with larger longitudinal optical phonon energies.

Study on Melting and Deflagration of Nanometer-Sized Indium Particle Thin Films by Temperature-Dependent Ellipsometry

The melting and deflagration of nanometer indium particle thin films with an average diameter of 43.2 nm were characterized by temperature-dependent ellipsometry. During ellipsometric measurement, ...

Selective IR response of highly textured phase change VO2 nanostructures obtained via oxidation of electron beam deposited metallic V films

We demonstrate the growth of highly textured VO2 nanocrystals via annealing of e-beam deposited amorphous metallic V. Temperature dependent ellipsometry results reveal the pronounced reflection near the IR spectrum above the transition and an almost temperature independent weak reflection in the visible spectrum. The IR reflection displays a strong hysteresis during heating and cooling near the transition temperature at 68°C, indicating a first order transition and a strain-free structure. Our work demonstrates the feasibility to obtain high quality phase change nanostructures that transmit the visible spectrum but reflect IR and is suitable for large scale fabrication.

Temperature-Dependent Ellipsometry Measurements of Partial Coulomb Energy in Superconducting Cuprates

We performed an experimental study of the temperature and doping dependence of the energy-loss function of the bilayer and trilayer Bi-cuprate family. The primary aim is to obtain information on the energy stored in the Coulomb interaction between the conduction electrons, on the temperature dependence thereof, and on the change of Coulomb interaction when Cooper-pairs are formed. We performed temperature-dependent ellipsometry measurements on several Bi$_2$Sr$_2$CaCu$_2$O$_{8-x}$ single crystals: under-doped with $T_c=60, 70$ and 83K, optimally doped with $T_c=91$K, overdoped with $T_c=84, 81, 70$ and $58$K, as well as optimally doped Bi$_2$Sr$_2$Ca$_2$Cu$_3$O$_{10+x}$ with $T_c=110$K. Our first observation is that, as the temperature drops through $T_c$, the loss function in the range up to 2~eV displays a change of temperature dependence as compared to the temperature dependence in the normal state. This effect at - or close to - $T_c$ depends strongly on doping, with a sign-change for weak overdoping. The size of the observed change in Coulomb energy, using an extrapolation with reasonable assumptions about its $q$-dependence, is about the same size as the condensation energy that has been measured in these compounds. Our results therefore lend support to the notion that the Coulomb energy is an important factor for stabilizing the superconducting phase. Due to the restriction to small momentum, our observations do not exclude a possible significant contribution to the condensation energy of the Coulomb energy associated to the region of $q$ around $(\pi,\pi)$.

Confined water layers in graphene oxide probed with spectroscopic ellipsometry

The confinement of water in quasi two-dimensional layers is intriguing because its physical properties can be significantly different when compared to those of the bulk fluid. This work describes spectroscopic ellipsometry study of confined water layers trapped between sheets of graphene oxide at varied thermal annealing temperatures. The wavelength-dependent refractive index of graphene oxide changes abruptly with annealing temperatures for Tann ≈ 125–160 °C, and we demonstrate that these changes are primarily governed by the expulsion of trapped water. This expulsion is associated with the decrease of interlayer separation of graphene oxide sheets from 7.8 Å to 3.4 Å. Graphene oxide annealed at high temperatures lacks trapped water layers and robust estimates of refractive index can be obtained within a Lorentz oscillator model. The trends in oscillator parameters are extended to lower annealing temperatures, where trapped water is present, in order to estimate the refractive index of confined water, whose value is found to be enhanced as compared to that of bulk. Temperature-dependent ellipsometry data show anomalous changes in ellipsometric parameters over a wide temperature interval (−10 to 10 °C) about the ice-point and these may be attributed to possible phase transition(s) of confined water.