Amorphous silicon contains tunneling two-level systems, which are the dominant energy loss mechanisms for amorphous solids at low temperatures. These two-level systems affect both mechanical and electromagnetic oscillators and are believed to produce thermal and electromagnetic noise and energy loss. However, it is unclear whether the two-level systems that dominate mechanical and dielectric losses are the same; the former relies on phonon-TLS coupling, with an elastic field coupling constant, $γ$, while the latter depends on a TLS dipole moment, $p_0$, which couples to the electromagnetic field. Mechanical and dielectric loss measurements as well as structural characterization were performed on amorphous silicon thin films grown by electron beam deposition with a range of growth parameters. Samples grown at 425 $^{\circ}$C show a large reduction of mechanical loss (34 times) and a far smaller reduction of dielectric loss (2.3 times) compared to those grown at room temperature. Additionally, mechanical loss shows lower loss per unit volume for thicker films, while dielectric loss shows lower loss per unit volume for thinner films. Analysis of these results indicate that mechanical loss correlates with atomic density, while dielectric loss correlates with dangling bond density, suggesting a different origin for these two energy dissipation processes in amorphous silicon.
Topological insulators (TIs) are exotic materials which have topologically protected states on the surface due to the strong spin-orbit coupling. However, a lack of ordered growth of TI thin films on amorphous dielectrics and/or insulators presents a challenge for applications of TI-junctions. We report the growth of topological insulator Bi2Se3 thin films on amorphous SiO2 by molecular beam epitaxy (MBE). To achieve the ordered growth of Bi2Se3 on amorphous surface, the formation of other phases at the interface is suppressed by Se passivation. Structural characterizations reveal that Bi2Se3 …
High-kappa dielectrics for insulating layers are a current key ingredient of microelectronics. X2O3 sesquioxide compounds are among the candidates. Here we show for a typical material of this class, ScO3, that the relatively modest dielectric constant of its crystalline phase is enhanced in the amorphous phase by over 40% (from ~15 to ~22). This is due to the disorder-induced activation of low frequency cation-related modes which are inactive or inefficient in the crystal, and by the conservation of effective dynamical charges (a measure of atomic polarizability). The analysis employs density-…
Realistic models of amorphous ZrO2 are generated in a ``melt-and-quench'' fashion using ab-initio molecular dynamics in a plane-wave pseudopotential formulation of density-functional theory. The structural properties of the resulting amorphous models are analyzed, with special attention to coordination statistics. The vibrational and dielectric properties of one of these models are then investigated from first principles using linear-response methods. The electronic dielectric constant and Born effective charges are found to be very similar to those of the crystalline phases. Encouragingly, th…
Zirconia (ZrO2) and hafnia (HfO2) are leading candidates for replacing SiO2 as the gate insulator in CMOS technology. Amorphous versions of these materials (a-ZrO2 and a-HfO2)) can be grown as metastable phases on top of a silicon buffer; while they tend to recrystallize during subsequent annealing steps, they would otherwise be of considerable interest because of the promise they hold for improved uniformity and electrical passivity. In this work, we report our theoretical studies of a-ZrO2 and a-HfO2 by first-principles density-functional methods. We construct realistic amorphous models usin…
Magnesium nickel hydride films have earlier been suggested for several optoelectronic applications, but the optical properties and band gap have not been firmly established. In this work, the dielectric functions and the optical band gaps of thin films of Mg2NiH4 have been determined experimentally from optical modeling using spectroscopic ellipsometry and spectrophotometry in the photon energy range between 0.7 and 4.2 eV. Samples were prepared by reactive sputtering, resulting in a single-layer geometry that could easily be studied by ellipsometry. Crystalline samples were prepared by anneal…
High-$κ$ metal oxides are a class of materials playing an increasingly important role in modern device physics and technology. Here we report theoretical investigations of the properties of structural and lattice dielectric constants of bulk amorphous metal oxides by a combined approach of classical molecular dynamics (MD) - for structure evolution, and quantum mechanical first principles density function theory (DFT) - for electronic structure analysis. Using classical MD based on the Born-Mayer-Buckingham potential function within a melt and quench scheme, amorphous structures of high-$κ$ me…
We use density functional theory (DFT) to study the thermodynamic stability and migration of copper ions and small clusters embedded in amorphous silicon dioxide. We perform the calculations over an ensemble of statistically independent structures to quantify the role of the intrinsic atomic-level variability in the amorphous matrix affect the properties. The predicted formation energy of a Cu ion in the silica matrix is 2.7+/-2.4 eV, significantly lower the value for crystalline SiO2. Interestingly, we find that Cu clusters of any size are energetically favorable as compared to isolated ions;…
We report calculations indicating that amorphous RAO$_3$ oxides, with R and A trivalent cations, have approximately the same static dielectric constant as their perovskite crystal phase. The effect is due to the disorder-activated polar response of non-polar crystal modes at low frequency, which compensates a moderate but appreciable reduction of the ionic dynamical charges. The dielectric response was studied via density-functional perturbation theory. Amorphous samples were generated by molecular dynamics melt-and-quench simulations.
We examine the ultrafast optical response of the crystalline and amorphous phases of the phase change material Ge$_2$Sb$_2$Te$_5$ below the phase transformation threshold. Simultaneous measurement of the transmissivity and reflectivity of thin film samples yields the time-dependent evolution of the dielectric function for both phases. We then identify how lattice motion and electronic excitation manifest in the dielectric response. The dielectric response of both phases is large but markedly different. At 800 nm, the changes in amorphous GST are well described by the Drude response of the gene…
The problem of both electron and phonon scattering by wedge disclination dipoles (WDD) is studied in the framework of the deformation potential approach. The exact analytical results for the mean free path are obtained within the Born approximation. The WDD-induced contribution to the residual resistivity in nanocrystalline metals is estimated. Using the WDD-based model of a grain boundary, the thermal conductivity, kappa, of polycrystals and amorphous dielectrics is studied. It is shown that the low-temperature crossover of kappa experimentally observed in LiF, NaCl, and sapphire can be expla…
Modeling the Dielectric Relaxation in Semicrystalline Polymers -- Understanding the Role of the Interphase between the Amorphous and Crystalline Domains
We have proposed a kind of nonvolatile resistive switching memory based on amorphous LaLuO3, which has already been established as a promising candidate of high-k gate dielectric employed in transistors. Well-developed unipolar switching behaviors in amorphous LaLuO3 make it suited for not only logic but memory applications using the conventional semiconductor or the emerging nano/CMOS architectures. The conduction transition between high- and low- resistance states is attributed to the change in the separation between oxygen vacancy sites in the light of the correlated barrier hopping theory.…
We report first principles modeling of quantum tunneling through amorphous HfO$_2$ dielectric layer of metal-oxide-semiconductor (MOS) nanostructures in the form of n-Si/HfO$_2$/Al. In particular we predict that chemically modifying the amorphous HfO$_2$ barrier by doping N and Al atoms in the middle region - far from the two interfaces of the MOS structure, can reduce the gate-to-channel tunnel leakage by more than one order of magnitude. Several other types of modification are found to enhance tunneling or induce substantial band bending in the Si, both are not desired from leakage point of …
Low-loss deposited dielectrics will benefit superconducting devices such as integrated superconducting spectrometers, superconducting qubits and kinetic inductance parametric amplifiers. Compared with planar structures, multi-layer structures such as microstrips are more compact and eliminate radiation loss at high frequencies. Multi-layer structures are most easily fabricated with deposited dielectrics, which typically exhibit higher dielectric loss than crystalline dielectrics. We measured the sub-kelvin and low-power microwave and mm-submm wave dielectric loss of hydrogenated amorphous sili…
We have measured the heat conduction between 0.05 K and 1.0 K of high purity silicon wafers carrying on their polished faces a variety of thin dielectric films and polycrystalline thin metallic films. Using a Monte Carlo simulation to analyze the conduction measurements, we have determined the phonon mean free path within the films, and found all of them to be much shorter even than in typical bulk amorphous solids, with no exceptions. We have also measured the internal friction of these films below 10 K and found, however, their internal friction at low temperatures strikingly close to that o…
Hydrogenated amorphous carbon (a-C:H), deposited by the rf-plasma enhanced chemical vapour deposition (rf-PECVD) technique, is a promising material for large area electronic and interlayer dielectric applications. The structural and electronic properties of rf-PECVD a-C:H, deposited at room temperature from CH4/He and CH4/Ar gas mixtures, are shown to be sensitive to the substrate on which the thin film is deposited. The choice of substrate (c-Si or C7059 glass), and the existence and geometrical dimensions of any metallic pattern on the substrate surface, can result in significant spatial var…
We find that O-vacancy (Vo) acts as a hole trap and play a role in negative bias illumination stress instability in amorphous In-Ga-Zn-O thin film transistors. Photo-excited holes drifted toward the channel/dielectric interface due to small potential barriers and can be captured by Vo in the dielectrics. While Vo(+2) defects are very stable at room temperature, their original deep states are recovered via electron capture upon annealing. We also find that Vo(+2) can diffuse in amorphous phase, including hole accumulation near the interface under negative gate bias.
Data collapse enables comparison of measurement data measured in different laboratories on different samples. In the case of energy losses in Soft Magnetic Materials (SMM) the data collapse is possible to achieved only if the measurement data can be described by the two components formula. For more complicated cases we propose to perform data collapse's sequence in the two-dimensional subspaces $L_{i,i+1}$ spanned by the appropriate powers of frequency $\{f^{i},f^{i+1}\}$. Such approach enables the data comparison in the different two-dimensional subspaces. This idea has been tested with measu…
We have investigated the nonlinear surface impedance and two-tone intermodulation distortion of nine epitaxial YBa2Cu3O7-d films on MgO substrates, using stripline resonators, at frequencies f=2.3-11.2GHz and temperatures T=1.7K-Tc. The power dissipation decreased by up to one order of magnitude as the microwave electric field was increased to about 100V/m for T<20 K, while the reactance Xs showed only a weak increase. The minimum of the losses correlated with a plateau in the intermodulation signal. The same features were observed for a Nb film on MgO. The anomalous response is due to nonline…
We have measured the excited state lifetimes in Josephson junction phase and transmon qubits, all of which were fabricated with the same scalable multi-layer process. We have compared the lifetimes of phase qubits before and after removal of the isolating dielectric, SiNx, and find a four-fold improvement of the relaxation time after the removal. Together with the results from the transmon qubit and measurements on coplanar waveguide resonators, these measurements indicate that the lifetimes are limited by losses from the dielectric constituents of the qubits. We have extracted the individual …
In this study, we demonstrated experimentally and theoretically that the charge transport mechanism in amorphous Hf$_{0.5}$Zr$_{0.5}$O$_2$ is phonon-assisted tunneling between traps like in HfO$_2$ and ZrO$_2$. The thermal trap energy of 1.25 eV and optical trap energy of 2.5 eV in Hf$_{0.5}$Zr$_{0.5}$O$_2$ were determined based on comparison of experimental data on transport with different theories of charge transfer in dielectrics. A hypothesis that oxygen vacancies are responsible for the charge transport in Hf$_{0.5}$Zr$_{0.5}$O$_2$ was discussed.
Phase-change materials (PCMs), which are well-established in optical and random-access memories, are increasingly studied for emerging topics such as brain-inspired computing and active photonics. These applications take advantage of the pronounced reflectivity and resistivity changes that accompany the structural transition in PCMs from their amorphous to crystalline state. However, PCMs are typically fabricated as thin films via sputtering, which is costly, requires advanced equipment, and limits the sample and device design. Here, we investigate a simpler and more flexi-ble approach for app…
Artificial tuning of dielectric parameters can result from interface conductivity in polycrystalline materials. In ferroelectric single crystals, it was already shown that ferroelectric domain walls can be the source of such artificial coupling. We show here that low temperature dielectric losses can be tuned by a dc magnetic field. Since such losses were previously ascribed to polaron relaxation we suggest this results from the interaction of hopping polarons with the magnetic field. The fact that this losses alteration has no counterpart on the real part of the dielectric permittivity confir…
Atomically Thin Amorphous Carbon with an Ultralow Dielectric Constant
National University of Singapore（新加坡国立大学）；Centre for Advanced 2D materials, National University of Singapore（新加坡国立大学二维材料中心）；Donostia International Physics Center (DIPC)（圣塞巴斯蒂安国际物理中心）；IKERBASQUE Basque Foundation for Science（伊克尔巴斯克巴斯克科学基金会）；Freie Universität Berlin（柏林自由大学）；Leibniz Institute for Solid State and Materials Research（莱布尼茨固体与材料研究所）；Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Joint Laboratory “Functional Quantum Materials” at BESSY II（BESSY II功能量子材料联合实验室）；Institute of Materials Research and Engineering, Agency for Science, Technology and Research (A*STAR)（新加坡科技研究局材料研究与工程研究所）；Sanken, Osaka University（大阪大学三冈研究所）；Nanomaterials Research Institute, National Institute of Advanced Industrial Science and Technology (AIST)（日本产业技术综合研究所纳米材料研究所）；Institute for Functional Intelligent Materials, National University of Singapore（新加坡国立大学功能智能材料研究所）
The mechanisms governing mechanical dissipation in amorphous tantala are studied at microscopic scale via Molecular Dynamics simulations, namely by mechanical spectroscopy in a wide range of temperature and frequency. We find that dissipation is associated with irreversible atomic rearrangements with a sharp cooperative character, involving tens to hundreds of atoms arranged in spatially extended clusters of polyhedra. Remarkably, at low temperature we observe an excess of plastically rearranging oxygen atoms which correlates with the experimental peak in the macroscopic mechanical losses. A d…
The relaxation dynamics and thermodynamic properties of supercooled and glassy gambogic acid are investigated using both theory and experiment. We measure the temperature dependence of the relaxation times in three polymorphs (alpha-, beta-, and gamma-form). To gain insight into the relaxation processes, we propose a theoretical approach to quantitatively understand nature of these three relaxations. The alpha-relaxation captures cooperative motions of molecules while the beta-process is mainly governed by local dynamics of a single molecule within the cage formed by its nearest neighbors. Bas…
Historically, the design of hybrid solar photovoltaic thermal (PVT) systems has focused on cooling crystalline silicon (c-Si)-based photovoltaic (PV) devices to avoid temperature-related losses. This approach neglects the associated performance losses in the thermal system and leads to a decrease in the overall exergy of the system. Consequently, this paper explores the use of hydrogenated amorphous silicon (a-Si:H) as an absorber material for PVT in an effort to maintain higher and more favourable operating temperatures for the thermal system. Amorphous silicon not only has a smaller temperat…
Superconducting resonators used in millimeter-submillimeter astronomy would greatly benefit from deposited dielectrics with a small dielectric loss. We deposited hydrogenated amorphous silicon films using plasma-enhanced chemical vapor deposition, at substrate temperatures of 100°C, 250°C and 350°C. The measured void volume fraction, hydrogen content, microstructure parameter, and bond-angle disorder are negatively correlated with the substrate temperature. All three films have a loss tangent below $10^{-5}$ for a resonator energy of $10^5$ photons, at 120 mK and 4-7 GHz. This makes these film…
Quantum two-level systems (TLSs) intrinsic to glasses induce decoherence in many modern quantum devices, such as superconducting qubits. Although the low-temperature physics of these TLSs is usually well-explained by a phenomenological standard tunneling model of independent TLSs, the nature of these TLSs, as well as their behavior out of equilibrium and at high energies above 1 K, remain inconclusive. Here we measure the non-equilibrium dielectric loss of TLSs in amorphous silicon using a superconducting resonator, where energies of TLSs are varied in time using a swept electric field. Our re…
The complex dielectric constant $\hatε = ε_1 + i ε_2$ of SrTiO$_3$ reaches high values $ε_1 \approx 2*10^{4}$ at cryogenic temperatures, while the dielectric losses ($ε_2$) are much stronger than for other crystalline dielectrics. SrTiO$_3$ is a common substrate for oxide thin films, like the superconducting LaAlO$_3$/SrTiO$_3$ system, but the large $ε_1$ and $ε_2$ restrict high-frequency quantum devices on SrTiO$_3$. Here we present superconducting coplanar Nb resonators on SrTiO$_3$, which we successfully operate in a distant-flip-chip geometry at frequencies that exceed 1 GHz. We find a pro…
We Study in this paper the scaling and statistical properties of the $ac$ conductivity of thin metal-dielectric films in different regions of the loss in the metallic components and particularly in the limit of vanishing loss. We model the system by a 2D $RL-C$ network and calculate the effective conductivity by using a real space renormalization group method. It is found that the real conductivity strongly fluctuates for very small losses. The correlation length, which seems to be equivalent to the localization length, diverges for vanishing losses confirming our previous results for the deca…
The glasses in the system (100-x)TeO2-xCaCu3Ti4O12, (x=0.25 to 3 mol %) were fabricated. The color varied from olive green to brown as the CaCu3Ti4O12 (CCTO) content increased in TeO2 matrix. The X-ray powder diffraction and differential scanning calorimetric analyses that were carried out on the as-quenched samples confirmed their amorphous and glassy nature respectively. The dielectric constant and loss in the 100 Hz-1MHz frequency range were monitored as a function of temperature (50-400oC). The dielectric constant and the loss (D) increased as the CCTO content increased in TeO2 at all the …
We study the TE polarized electromagnetic surface wave propagating along the interface between materials with positive and negative magnetic permeability. Contrary to the TM polarized surface wave, the TE surface wave exhibits almost no radiation losses when scattered at semi-infinite dielectric interfaces.
The loss of amorphous hydrogenated silicon nitride (a-SiN$_{x}$:H) is measured at 30 mK and 5 GHz using a superconducting LC resonator down to energies where a single-photon is stored, and analyzed with an independent two-level system (TLS) defect model. Each a-SiN$_{x}$:H film was deposited with different concentrations of hydrogen impurities. We find that quantum-regime dielectric loss tangent $\tanδ_{0}$ in a-SiN$_{x}$:H is strongly correlated with N-H impurities, including NH$_{2}$. By slightly reducing $x$ we are able to reduce $\tanδ_0$ by approximately a factor of 50, where the best fil…
It was experimentally found that the evolution of dielectric loss with processing temperature displays a common trend in ferroelectric and dielectric thin oxide films: firstly an increase and then a decrease in dielectric loss when the processing temperature is gradually raised. Such a dielectric response of ferroelectric/dielectric thin films has been theoretically addressed in this work. We propose that at the initial stage of the crystallization process in thin films, the transformation from amorphous to crystalline phase should increase substantially the dielectric loss; then, with further…
Strong suppression of the photonic density of states in three-dimensional disordered silicon networks
University of Fribourg（弗里堡大学）；Université Côte d’Azur（蔚蓝海岸大学）；CNRS, Institut de Physique de Nice – INPHYNI（法国国家科学研究中心，尼斯物理研究所-INPHYNI）；Optoelectronics Research Centre, University of Southampton（南安普顿大学光电研究中心）
Great achievements in last five years, such as record-efficient amorphous/crystalline silicon heterojunction (SHJ) solar cells and cutting-edge perovskite/SHJ tandem solar cells, place hydrogenated amorphous silicon (a-Si:H) at the forefront of emerging photovoltaics. Due to the extremely low doping efficiency of trivalent boron (B) in amorphous tetravalent silicon, light harvesting of aforementioned devices are limited by their fill factors (FF), which is a direct metric of the charge carrier transport. It is challenging but crucial to develop highly conductive doped a-Si:H for minimizing the…
Brownian thermal noise is a limiting factor for the sensitivity of many high precision metrology applications, among other gravitational-wave detectors. The origin of Brownian noise can be traced down to internal friction in the amorphous materials that are used for the high reflection coatings. To properly characterize the internal friction in an amorphous material, one needs to consider separately the bulk and shear losses. In most of previous works the two loss angles were considered equal, although without any first principle motivation. In this work we present a method that can be used to…
Disentangling superconductor and dielectric microwave losses in sub-micron $\rm Nb$/$\rm TEOS-SiO_2$ interconnects using a multi-mode microstrip resonator
Our study shows that deposited Ge and Si dielectric thin-films can exhibit low microwave losses at near single-photon powers and sub-Kelvin temperatures ($\approx$40 mK). This low loss enables their use in a wide range of devices, including low-loss coplanar, microstrip, and stripline resonators, as well as layers for device isolation, inter-wiring dielectrics, and passivation in microwave and Josephson junction circuit fabrication. We use coplanar microwave resonator structures with narrow trace widths of 2-16 $μ\textrm{m}$ to maximize the sensitivity of loss tangent measurements to the inter…
