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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 451 records · Page 25
All sourcesNASA NTRSDOE OSTI
NASA NTRS1994

Fundamental mechanisms in premixed flame propagation via vortex-flame interactions: Numerical simulations

The goal of the present study is to assess numerically the ability of single-step and two-step chemical models to describe the main features encountered during the interaction between a two-dimensional vortex pair and a premixed laminar flame. In the two-step mechanism, the reaction kinetics are represented by a first chain branching reaction A + X yields 2X and a second chain termination reaction X + X yields P. This paper presents the fundamental mechanisms occurring during vortex-flame interactions and the relative impact of the major parameters encountered in turbulent premixed flames and suspected of playing a role in quenching mechanism: (1) Influence of stretch is investigated by analyzing the contribution of curvature and tangential strain on the local structure of the flame. The effect of Lewis number on the flame response to a strained field is analyzed. (2) Radiative heat losses which are suspected to be partially or totally responsible for quenching are also investigated. (3) The effect of the diffusion of the radicals is studied using a two-step mechanism in which an intermediate species is present. The parameters of the two-step mechanism are entirely determined from physical arguments. (4) Precise quantitative comparisons between the DNS and the experimental results of Samaniego et al are performed. These comparisons concern the evolution of the minimum heat release rate found along the flame front during the interaction and the distribution of the heat release rate along the flame front.

Mantel, Thierry↗
DOE OSTI2019

A Review of Magneto-Elastic Interaction and Its Theoretical Descriptions in Type-II Superconductors

It is well known that the interaction between defect-induced strain field and vortex lattice (VL) gives rise to vortex pinning behaviors. Likewise, magneto-elastic (ME) interaction is caused by the difference between specific volumes of normal phase and superconducting (SC) phase. Acting as inhomogeneous strain sources, the normal-state vortex cores produce local deformation in the surrounding SC matter and thus affect VL energy. ME interaction belongs to the fundamental physics of interdependences between vortex matter and crystal lattice. The review starts with the effects of ME interaction on magnetization, vortex morphology and intervortex interaction. In Sect. 2, theoretical descriptions of ME interaction are classified in terms of different simplifications. The core ideas and outstanding results of these theories are given. It is followed by Sect. 3, where the correlation and difference between ME and pinning interaction are outlined. Although pinning differs from ME interaction in their formation mechanisms, the pinning interaction is established upon the vortex-induced strain field from Ginzburg-Landau (GL) viewpoint. Section 4 goes further with the GL treatment for solving ME and pinning problem; the general thoughts and steps can be found in this section. The last section gives some outlooks which involve pressure dependence of T{sub c} and anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

The interaction between hexagonal boron nitride and water from first principles

The use of hexagonal boron nitride (h-BN) in microfluidic and nanofluidic applications requires a fundamental understanding of the interaction between water and the h-BN surface. A crucial component of the interaction is the binding energy, which is sensitive to the treatment of electron correlation. In this work, we use state of the art quantum Monte Carlo and quantum chemistry techniques to compute the binding energy. Compared to high-level many-body theory, we found that the second-order Møller-Plesset perturbation theory captures the interaction accurately and can thus be used to develop force field parameters between h-BN and water for use in atomic scale simulations. On the contrary, density functional theory with standard dispersion corrections tends to overestimate the binding energy by approximately 75%.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

DOE-EPSCoR. Exchange interactions in epitaxial intermetallic layered systems

The goal of this research is to develop a fundamental understanding of the exchange interactions in epitaxial intermetallic alloy thin films and multilayers, including films and multilayers of Fe-Pt, Co-Pt and Fe-P-Rh alloys deposited on MgO and Al 2 O 3 substrates. Our prior results have revealed that these materials have a rich variety of ferromagnetic, paramagnetic and antiferromagnetic phases which are sensitive functions of composition, substrate symmetry and layer thickness. Epitaxial antiferromagnetic films of FePt alloys exhibit a different phase diagram than bulk alloys. The antiferromagnetism of these materials has both spin ordering transitions and spin orienting transitions. The objectives include the study of exchange-inversion materials and the interface of these materials with ferromagnets. Our aim is to formulate a complete understanding of the magnetic ordering in these materials, as well as developing an understanding of how the spin structure is modified through contact with a ferromagnetic material at the interface. The ultimate goal is to develop the ability to tune the phase diagram of the materials to produce layered structures with tunable magnetic properties. The alloy systems that we will study have a degree of complexity and richness of magnetic phases that requires the use of the advanced tools offered by the DOE-operated national laboratory facilities, such as neutron and x-ray scattering to measure spin ordering, spin orientations, and element-specific magnetic moments. We plan to contribute to DOE’s mission of producing “Materials by Design” with properties determined by alloy composition and crystal structure. We have developed the methods for fabricating and have performed neutron diffraction experiments on some of the most interesting phases, and our work will serve to answer questions raised about the element-specific magnetizations using the magnetic x-ray dichroism techniques and interface magnetism in layered structures using polarized neutron reflectometry. Through application of these techniques to understand the materials fabricated in our laboratory, we will employ a tight feedback loop to tailor the magnetic properties on demand. Developing the ability to control magnetic anisotropy is essential for creating the next generation of magnetic storage media (for hard disks, for example), where individual bit sizes have already become smaller than 100nm in the largest dimension. Still smaller bits and higher storage density will require the ability to exquisitely tailor magnetic media properties at the atomic level, the ultimate goal of our study.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Cooperative Agreement To Analyze variabiLity, change and predictabilitY in the earth SysTem (CATALYST)

CATALYST proposes to perform foundational coordinated research in a team-oriented collaborative effort aimed at advancing a robust understanding of modes of Earth system variability and change using models, observations and process studies. The proposed research will address the DOE/BER mission by exploring the limits to predictability, identifying fundamental underlying mechanisms, quantifying interactions among modes of variability, and discovering tipping points in the Earth system to understand the current and future impacts of these phenomena on regional and global climate. Four fundamental gaps are identified in our knowledge of the Earth system: 1) What are the limits to predictability on various timescales? 2) What are the interactions among modes of Earth system variability? 3) How may modes of Earth system variability change in response to changes in external forcing, and what are the tipping points involved with those changes? 4) How are high impact events connected to modes of Earth system variability and how may they change in the future? Related to those gaps in our knowledge, we formulate four research objectives to address those gaps using a combination of Earth system models (ESMs) and machine learning (ML) methods. Research Objective 1 (RO1) addresses the first gap above and proposes to understand modes of variability and their limits of predictability on subseasonal to decadal timescales using ESMs and ML. Research Objective 2 (RO2) addresses the second gap and proposes to use a hierarchy of models to understand relevant processes and feedbacks related to how modes of variability interact with each other. Research Objective 3 (RO3) is designed to study the third gap and proposes to examine the role of external forcings in changes of modes of Earth system variability and their interactions, and the likelihood and predictability of tipping points and irreversible changes. Research Objective 4 (RO4) will address the fourth gap and proposes to use high resolution ESMs, regionally refined models (RRMs), and ML methods to investigate the relationships between high impact events (e.g. flash droughts and precipitation extremes, atmospheric rivers (ARs), tropical cyclones (TCs), storm surge/sea level rise), the synoptic systems that produce them, and their changes related to modes of Earth system variability. The research will involve the use of the Community Earth System Model (CESM), Energy Exascale Earth System Model (E3SM), CMIP multi-model data sets, a hierarchy of simpler models, and numerous observational data sets. In the course of the proposed research, CATALYST will contribute to metrics and diagnostics that will be integrated in Coordinated Model Evaluation Capabilities (CMEC), particularly with regards to the Quasi-biennial Oscillation (QBO) and its interactions with the Madden-Julian Oscillation (MJO), high atmospheric pressure blocking, and new precipitation metrics.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Harnessing photoautotroph-methanotroph interactions for biogas conversion to fuels and chemicals using binary consortia (Project Final Technical Report)

Industrial, municipal, and agricultural waste streams containing stranded organic carbon represent a significant and underutilized feedstock to produce fuels and chemicals. With anaerobic digestion deployed at large scales to capture organic waste streams, over 6 million tons of biogas are available today. However, the utilization of biogas represents a significant challenge due to its low pressure and presence of contaminants such as H 2 S, ammonia, and volatile organic carbon compounds. To tap into this immense potential, effective biotechnologies that co-utilize both CO 2 and CH 4 are needed. Recent studies demonstrated that, in nature, microbial communities have developed a highly efficient way to recover energy and capture carbon from both CH 4 and CO 2 through metabolic coupling of methane oxidation to oxygenic photosynthesis. Using two synthetic methanotroph – photoautotroph (M-P) co-cultures that exhibit stable growth under a broad range of cultivation conditions, in this project we proposed to harness the interspecies interactions within these cocultures for biogas conversion to fuels and chemicals. To facilitate this overarching objective, we aim to develop experimental and computational tools to gain qualitative and quantitative understandings on the interactions and dynamics of the coculture at both systems and molecular levels, and to validate our findings through experiments and mutant development. The fundamental understanding on the interactions and dynamics of the photoautotroph-methanotroph will lay the foundation for the design and optimization of synthetic binary consortia for production of fuels and chemicals from biogas. We expect the knowledge gained from this project may be generally applicable to other cross-feeding binary consortium, and the tools developed can be adapted to study the interactions and dynamics of other multi-organism platforms.

09 BIOMASS FUELS↗
DOE OSTI2019

Molecular-Level Design of Heterogeneous Chiral Catalysts

A recent major focus of catalyst research has been on improving the selectivity or atom efficiency of catalytic processes. Perhaps the most subtle and difficult form of selectivity to control is enantioselectivity, a catalyst’s ability to preferentially yield one enantiomer of a chiral product. Since two enantiomers are identical in all respects except for their mirror reflection symmetry, both are formed in non-chiral environments at exactly equal rates; only by introducing some type of chiral modification to the system can the rate of formation of one enantiomer be favored over the other. This has been successfully achieved for homogeneous-phase, organometallic catalysts, but the empirical development of heterogeneous-phase analogs has proven elusive. The design of such heterogeneous-phase catalysts would obviate the need for inefficient purification steps to remove the heavy-metal catalysts. The goal of the proposed research by the Chiral Catalysis Group is to understand the interactions of prochiral reactants on chirally modified surfaces that lead to the preferential formation of one enantiomer over the other. There are two general concepts for designing heterogeneous-phase enantioselective catalysts. The first adopts the strategy used in homogeneous phase, by adding a chiral modifier to the surface. This approach, while conceptually simple has challenges associated with modifying an extended surface. The second concept, which is unique to extended surfaces, is the idea of creating surfaces that are themselves naturally chiral. A fundamental understanding of the interactions that control enantioselectivity will enable the Chiral Catalysis Group to develop the concepts necessary to design novel, heterogenous catalytic materials. Enantioselectivity is also central to catalytic processes that underpin the pharmaceutical and agrochemical industries. With funding from the Department of Energy, the Chiral Catalysis Group has played a leading role in developing a fundamental understanding of chiral catalysis and of the adsorbate structures, interactions and kinetic effects that control heterogenous-phase enantioselectivity. The proposed research program is organized conceptually around three types of enantiospecific interactions: interactions with naturally chiral surfaces; those with modified surfaces categorized as chirally templated surfaces; and one-to-one interactions of prochiral molecules with chiral surface modifiers. Our specific goals are to: (1) determine the structures of chiral surfaces, prochiral reactants, chiral products and chiral modifiers; (2) understand the enantiospecific interactions that occur between prochiral reactants and chiral products with chirally modified surfaces; (3) develop methods for detection of enantiospecific surface phenomena; and (4) elucidate enantioselective reaction pathways and the interactions that control them. The range of expertise within the Chiral Catalysis Group includes molecular-scale theory, surface science experiments, state-of-the-art spectroscopic, kinetic and atomic-scale imaging capabilities carried out in vacuum and under more-realistic liquid- and gas-phase environments complemented by catalytic measurements. By fully integrating such a breadth of approaches and extensive expertise, the Chiral Catalysis Group will, for the first time, be able to understand, rationally design and then control active sites for optimal enantioselectivity. In addition to having a significant impact on the field of chiral catalysis, the proposed research program will further our general understanding of the molecular-scale origins of catalytic selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Engineering microbial consortia with rationally designed cellular interactions

Synthetic microbial consortia represent a frontier of synthetic biology that promises versatile engineering of cellular functions. They are primarily developed through the design and construction of cellular interactions that coordinate individual dynamics and generate collective behaviors. Here we review recent advances in the engineering of synthetic communities through cellular-interaction programming. We first examine fundamental building blocks for intercellular communication and unidirectional positive and negative interactions. Here, we then recap the assembly of the building blocks for creating bidirectional interactions in two-species ecosystems, which is followed by the discussion of engineering toward complex communities with increasing species numbers, under spatial contexts, and via model-guided design. We conclude by summarizing major challenges and future opportunities of engineered microbial ecosystems.

42 ENGINEERING↗
DOE OSTI2025

From oversimplified to overlooked: The case for exploring rich dark sectors

The Standard Model (SM) of particle physics provides a very successful description of fundamental particles and their interactions but it is incomplete, as neutrino masses, dark matter and the baryon asymmetry of the Universe indicate. In addition, the origin of masses and of the approximate fundamental symmetries call out for deeper explanations. The quest for a New SM Theory, that extends the SM to a more general theory, is ongoing. For decades the main focus has been on the TeV scale, but despite an impressive theoretical and experimental effort, no hints of new physics at such scale has been found in experiments. Dark sectors provide an interesting alternative to TeV scale extensions of the SM to explain the open questions in particle and astroparticle physics. Going beyond minimal models, rich dark sectors extend the SM to a complex theory with multiple particles and interactions, in analogy to the SM itself. They have a wealth of theoretical and astrophysical/cosmological consequences and can lead to phenomenological signatures that can be markedly different to that of minimal ones. These include short-lived particles and semi-visible decay signatures, as opposed to minimal models where new states are typically long-lived and purely visible or invisible resonances. Given the experimental configurations and analysis strategies, current dark sector searches might miss such signatures. We advocate a dedicated programme of searches for rich dark sectors that overcomes the assumptions on minimality and on the long lifetime of particles and encompasses a broader range of possibilities. Here, we discuss a prototype model that includes a complex structure akin to the SM: multiple generations of fermions charged under a new spontaneously-broken gauge symmetry.

Dark matter↗
DOE OSTI2017

Measurement of the dynamic charge response of materials using low-energy, momentum-resolved electron energy-loss spectroscopy (M-EELS)

One of the most fundamental properties of an interacting electron system is its frequency- and wave-vector-dependent density response function, \chi({\bf q},\omega) . The imaginary part, \chi''({\bf q},\omega) , defines the fundamental bosonic charge excitations of the system, exhibiting peaks wherever collective modes are present. \chi χ quantifies the electronic compressibility of a material, its response to external fields, its ability to screen charge, and its tendency to form charge density waves. Unfortunately, there has never been a fully momentum-resolved means to measure \chi({\bf q},\omega) at the meV energy scale relevant to modern electronic materials. Here, we demonstrate a way to measure \chi χ with quantitative momentum resolution by applying alignment techniques from x-ray and neutron scattering to surface high-resolution electron energy-loss spectroscopy (HR-EELS). This approach, which we refer to here as “M-EELS”, allows direct measurement of \chi''({\bf q},\omega) with meV resolution while controlling the momentum with an accuracy better than a percent of a typical Brillouin zone. We apply this technique to finite-q excitations in the optimally-doped high temperature superconductor, Bi _2 2 Sr _2 2 CaCu _2 2 O _{8+x} 8 + x (Bi2212), which exhibits several phonons potentially relevant to dispersion anomalies observed in ARPES and STM experiments. Our study defines a path to studying the long-sought collective charge modes in quantum materials at the meV scale and with full momentum control.

36 MATERIALS SCIENCE↗
NASA NTRS1994

Development of the CSI phase-3 evolutionary model testbed

This report documents the development effort for the reconfiguration of the Controls-Structures Integration (CSI) Evolutionary Model (CEM) Phase-2 testbed into the CEM Phase-3 configuration. This step responds to the need to develop and test CSI technologies associated with typical planned earth science and remote sensing platforms. The primary objective of the CEM Phase-3 ground testbed is to simulate the overall on-orbit dynamic behavior of the EOS AM-1 spacecraft. Key elements of the objective include approximating the low-frequency appendage dynamic interaction of EOS AM-1, allowing for the changeout of components, and simulating the free-free on-orbit environment using an advanced suspension system. The fundamentals of appendage dynamic interaction are reviewed. A new version of the multiple scaling method is used to design the testbed to have the full-scale geometry and dynamics of the EOS AM-1 spacecraft, but at one-tenth the weight. The testbed design is discussed, along with the testing of the solar array, high gain antenna, and strut components. Analytical performance comparisons show that the CEM Phase-3 testbed simulates the EOS AM-1 spacecraft with good fidelity for the important parameters of interest.

Gronet, M. J.↗
DOE OSTI2018

Mellin bootstrap for scalars in generic dimension

We use the recently developed framework of the Mellin bootstrap to study perturbatively free scalar CFTs in arbitrary dimensions. This approach uses the crossing-symmetric Mellin space formulation of correlation functions to generate algebraic bootstrap equations by demanding that only physical operators contribute to the OPE. We find that there are no perturbatively interacting CFTs with only fundamental scalars in d > 6 dimensions (to at least second order in the perturbation). Our results can be seen as a modest step towards understanding the space of interacting CFTs in d > 6 and are consistent with the intuition that no such CFTs exist.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Electron and neutrino scattering from nuclei [Slides]

The knowledge of how electrons and neutrinos interact in nuclei is fundamental for many reasons, and the proper inclusion of many-body correlations between nucleons is crucial. The calculation of the nuclei from two- and three-nucleon interactions obtained from first principle is, however, one of the most challenging problems for many-body nuclear physics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Fundamental Neutron Physics: Theory and Analysis

The research topic of the project focus on the theoretical study of the possibility to search for manifestations of new physics beyond the Standard model in fundamental neutron physics, with emphasis on fundamental symmetries and "exotic'' interactions. The mail goals concentrate on the search for Time Reversal Invariance Violation (TRIV) in neutron nuclei scattering, and on possible manifestations of new physics in neutron-antineutron oscillations and their interactions with nuclei. Theoretical methods for analysis and interpretations of TRIV parameters in neutron scattering with the possible background interactions, and for unambiguous separation of the effects related to manifestations of new physics have been developed. The obtained results will be applied for the development of experimental programs in fundamental neutron physics at the Spallation Neutron Sources (SNS) in USA, Japan, and Europe.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2016

Improving our fundamental understanding of the role of aerosol-cloud interactions in the climate system

The effect of an increase in atmospheric aerosol concentrations on the distribution and radiative properties of Earth’s clouds is the most uncertain component of the overall global radiative forcing from pre-industrial time. General Circulation Models (GCMs) are the tool for predicting future climate, but the treatment of aerosols, clouds, and aerosol-cloud radiative effects carries large uncertainties that directly affect GCM predictions, such as climate sensitivity. Predictions are hampered by the large range of scales of interaction between various components that need to be captured. Observation systems (remote sensing, in situ) are increasingly being used to constrain predictions but significant challenges exist, to some extent because of the large range of scales and the fact that the various measuring systems tend to address different scales. Fine-scale models represent clouds, aerosols, and aerosol-cloud interactions with high fidelity but do not include interactions with the larger scale and are therefore limited from a climatic point of view. Lastly, we suggest strategies for improving estimates of aerosol-cloud relationships in climate models, for new remote sensing and in situ measurements, and for quantifying and reducing model uncertainty.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2014

Collaborative Research. Fundamental Science of Low Temperature Plasma-Biological Material Interactions

Low temperature plasma (LTP) treatment of biological tissue is a promising path toward sterilization of bacteria due to its versatility and ability to operate under well-controlled and relatively mild conditions. The present collaborative research of an interdisciplinary team of investigators at University of Maryland, College Park (UMD), and University of California, Berkeley (UCB) focused on establishing our knowledge based with regard to low temperature plasma-induced chemical modifications in biomolecules that result in inactivation due to various plasma species, including ions, reactive radicals, and UV/VUV photons. The overall goals of the project were to identify and quantify the mechanisms by which low and atmospheric pressure plasma deactivates endotoxic biomolecules. Additionally, we wanted to understand the mechanism by which atmospheric pressure plasmas (APP) modify surfaces and how these modifications depend on the interaction of APP with the environment. Various low pressure plasma sources, a vacuum beam system and several atmospheric pressure plasma sources were used to accomplish this. In our work we elucidated for the first time the role of ions, VUV photons and radicals in biological deactivation of representative biomolecules, both in a UHV beam system and an inductively coupled, low pressure plasma system, and established the associated atomistic biomolecule changes. While we showed that both ions and VUV photons can be very efficient in deactivation of biomolecules, significant etching and/or deep modification (~200 nm) accompanied these biological effects. One of the most important findings in this work is the significant radical-induced deactivation and surface modification can occur with minimal etching. However, if radical fluxes and corresponding etch rates are relatively high, for example at atmospheric pressure, endotoxic biomolecule film inactivation may require near-complete removal of the film. These findings motivated further work at atmospheric pressure using several types of low temperature plasma sources, for which radical induced interactions generally dominate due to short mean free paths of ions and VUV photons. For these conditions we demonstrated the importance of environmental interactions when atmospheric pressure plasma sources are used to modify biomolecules. This is evident from both gas phase characterization data and in-situ surface characterization of treated biomolecules. Environmental interactions can produce unexpected outcomes due to the complexity of reactions of reactive species with the atmosphere which determines the composition of reactive fluxes and atomistic changes of biomolecules. Overall, this work clarified a richer spectrum of scientific opportunities and challenges for the field of low temperature plasma-biomolecule surface interactions than initially anticipated, in particular for plasma sources operating at atmospheric pressure. The insights produced in this work, e.g. demonstration of the importance of environmental interactions, are generally important for applications of APP to materials modifications. Thus one major contributions of this research has been the establishment of methodologies to more systematically study the interaction of plasma with bio-molecules. In particular, our studies of atmospheric pressure plasma sources using very well-defined experimental conditions enabled to combine atomistic surface modifications of biomolecules with changes in their biological function. The clarification of the role of ions, VUV photons and radicals in deactivation of biomolecules during low pressure and atmospheric pressure plasma-biomolecule interaction has broad implications, e.g. for the emerging field of plasma medicine. The development of methods to detect the effects of plasma treatment on immune-active biomolecules will be helpful in many future studies.

36 MATERIALS SCIENCE↗
NASA NTRS2009

Fundamental Study of a Jet-in-Cross-Flow Interacting with a Vortex Generator for Film Cooling Applications

Results of an experimental study are presented on the effectiveness of a vortex generator (VG) in preventing lift-off of a jet-in-cross-flow (JICF). The study is pertinent to film-cooling applications and its relevance to NASA programs is first briefly discussed. In the experiment, the jet issues into the boundary layer at an angle of 20deg to the free-stream. The effect of a triangular, ramp-shaped VG is studied while varying its geometry and location. Detailed flow-field properties are obtained for a case in which the height of the VG and the diameter of the orifice are comparable to the approach boundary layer thickness. The VG produces a streamwise vortex pair with vorticity magnitude three times larger (and of opposite sense) than that found in the JICF alone. Such a VG appears to be most effective in keeping the jet attached to the wall. The effect of parametric variation is studied mostly from surveys ten diameters downstream from the orifice. Results over a range of jet-to-freestream momentum flux ratio (1<J<11) show that the VG has a significant effect even at the highest J covered in the experiment. When the VG height is halved there is a lift-off of the jet. On the other hand, when the height is doubled, the jet core is dissipated due to larger turbulence intensity. Varying the location of the VG, over a distance of three diameters from the orifice, is found to have little impact.

Zaman, Khairul↗
NASA NTRS1998

In Situ Infrared Spectroscopy of the Gaseous Species Present in a Diamond Chemical Vapor Deposition System

We interfaced a Hot-Filament Chemical Vapor Deposition (HFCVD) system to the emission port of an FT-IR spectrometer, in order to study the gas phase species present during the deposition of diamond thin films. The implementation of the infrared (IR) emission technique in situ allowed the study of various carbon-containing species believed to be crucial in diamond film growth. The two IR-active vibrational fundamentals of methane, v(3)(f2) and v(4)(f2), were observed at three different filament temperatures: 1000, 1500 and 2000 C. However, the net signal of v(3) was emission, while that of v(4) was absorption. These results indicate that the v(4) fundamental is excited beyond equilibrium, while the v(3) fundamental remains mostly in the ground state. This is due to the small concentration of methane, the low energy of v(4) compared to v(3) or to the Hz vibrational mode, and symmetry considerations that forbid interaction among the four fundamentals of methane. Thus, the excitation of v(3) is more likely than its decay under HFCVD conditions, producing a non-equilibrium population. At a filament temperature of 2000 C, the v(3) (sigma(+)(3)) fundamental of acetylene and a band at 1328 cm-l also ascribed to acetylene (v5 (pi(U)) + v4) appear in net absorption. This correlates well with the onset of molecular hydrogen breaking by the filament, which occurs at temperatures around 2000 C and above. The hydrogen atoms produced in this heterogeneous reaction give rise to a chain of reactions that lead to acetylene, among other carbonaceous species.

Morell, G.↗