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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Low-energy interband transition in the infrared response of the correlated metal SrVO 3 in the ultraclean limit

We studied the low-energy electronic response of the prototypical correlated metal SrVO 3 in the ultraclean and disordered limit using infrared spectroscopy and density functional theory plus dynamical mean field theory calculations (DFT+DMFT). A strong optical excitation at 70 meV is observed in the optical response of the ultraclean samples but is hidden by the low-energy Drude-like response from intraband excitations in the more disordered samples. DFT+DMFT calculations reveal that this optical excitation originates from interband transitions between the bands split by orbital off-diagonal hopping, which has often been ignored in cubic systems, such as SrVO 3 . A memory function analysis of the optical data shows that this interband transition can lead to deviations of optical self-energy from the expected Fermi-liquid behavior. Our findings demonstrate that analysis schemes employed to extract many-body effects from optical spectra may be oversimplified to study the true electronic ground state and that improvements in material quality can guide efforts to refine theoretical approaches.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Uncovering extreme nonlinear dynamics in solids through time-domain field analysis

Time-domain analysis of harmonic fields with sub-cycle resolution is now experimentally viable due to the emergence of sensitive, on-chip techniques for petahertz-scale optical-field sampling. We demonstrate how such a time-domain, field-resolved analysis uncovers the extreme nonlinear electron dynamics responsible for high-harmonic generation within solids. Time-dependent density functional theory was used to simulate harmonic generation from a solid-state band-gap system driven by near- to mid-infrared waveforms. Particular attention was paid to regimes where both intraband and interband emission mechanisms play a critical role in shaping the nonlinear response. We show that a time-domain analysis of the harmonic radiation fields identifies the interplay between intra- and interband dynamical processes underlying the nonlinear light generation. With further analysis, we show that changes to the dominant emission regime can occur after only slight changes to the peak driving intensity and central driving wavelength. Furthermore, time-domain analysis of harmonic fields also reveals, for the first time, the possibility of rapid changes in the dominant emission mechanism within the temporal window of the driving pulse envelope. Finally, we examine the experimental viability of performing time-domain analysis of harmonic fields with sub-cycle resolution using realistic parameters.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Phonon-Driven Femtosecond Dynamics of Excitons in Crystalline Pentacene from First Principles

Nonradiative exciton relaxation processes are critical for energy transduction and transport in optoelectronic materials, but how these processes are connected to the underlying crystal structure and the associated electron, exciton, and phonon band structures, as well as the interactions of all these particles, is challenging to understand. Here, in this work, we present a first-principles study of exciton-phonon relaxation pathways in pentacene, a paradigmatic molecular crystal and optoelectronic semiconductor. We compute the momentum- and band-resolved exciton-phonon interactions, and use them to analyze key scattering channels. We find that both exciton intraband scattering and interband scattering to parity-forbidden dark states occur on the same ~100 fs timescale as a direct consequence of the longitudinal-transverse splitting of the bright exciton band. Consequently, exciton-phonon scattering exists as a dominant nonradiative relaxation channel in pentacene. We further show how the propagation of an exciton wave packet is connected with crystal anisotropy, which gives rise to the longitudinal-transverse exciton splitting and concomitant anisotropic exciton and phonon dispersions. Our results provide a framework for understanding the role of exciton-phonon interactions in exciton nonradiative lifetimes in molecular crystals and beyond.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

Spin Berry points as crucial for ultrafast demagnetization

Laser-induced ultrafast demagnetization has puzzled researchers around the world for over two decades. Intrinsic complexity in electronic, magnetic and phononic subsystems is difficult to understand microscopically. So far, it is not possible to explain demagnetization using a single mechanism, which suggests a crucial piece of information still missing. In this paper, we return to a fundamental aspect of physics: spin and its change within each band in the entire Brillouin zone. We employ face-centered cubic (fcc) Ni as an example and use an extremely dense k mesh to map out spin changes for every band close to the Fermi level along all the high symmetry lines. To our surprise, spin angular momentum at some special k points abruptly changes from [Formula: see text] to [Formula: see text] simply by moving from one crystal momentum point to the next. This explains why intraband transitions, which the spin superdiffusion model is based upon, can induce a sharp spin moment reduction, and why electric current can change spin orientation in spintronics. These special k points, which are called spin Berry points [M. V. Berry, Proc. R. Soc. Lond. A 393 (1984) 45], are not random and appear when several bands are close to each other, so the Berry potential of spin majority states is different from that of spin minority states. Although within a single band, spin Berry points jump, when we group several neighboring bands together, they form distinctive smooth spin Berry lines. It is the band structure that disrupts those lines. Spin Berry points are crucial to laser-induced ultrafast demagnetization and spintronics.

Physics↗
DOE OSTI2022

Transparent conducting oxides: from all-dielectric plasmonics to a new paradigm in integrated photonics

During the past few years, the optics and photonics communities have renewed their attention toward transparent conducting oxides (TCOs), which for over two decades have been broadly employed for the fabrication of transparent electrodes in photovoltaic and communication technologies. This reinvigorated research curiosity is twofold: on the one hand, TCOs, with their metal-like properties, low optical absorption, and fabrication flexibility, represent an appealing alternative to noble metals for designing ultra-compact plasmonic devices. On the other hand, this class of hybrid compounds has been proved to possess exceptionally high optical nonlinearities when operating on a frequency window centered around their crossover point, the wavelength point at which the real part of the dielectric permittivity switches sign. Because TCOs are wide-bandgap materials with the Fermi level located in the conduction band, they are hybrid in nature, thus presenting both interband and intraband nonlinearities. This is the cause of a very rich nonlinear physics that is yet to be fully understood and explored. In addition to this, TCOs are epsilon-near-zero (ENZ) materials within a broad near-infrared spectral range, including the entire telecom bandwidth. In this operational window a myriad of novel electromagnetic phenomena have been demonstrated experimentally such as supercoupling, wavefront freezing, and photon doping. Furthermore, TCOs stand out among all other ENZ systems due to one fundamental characteristic, which is hardly attainable even by using structured materials. In fact, around their ENZ wavelength and for a quite generous operational range, these materials can be engineered to have an extremely small real index. This peculiarity leads to a slow-light effect that is ultimately responsible for a significant enhancement of the material nonlinear properties and is the cornerstone of the emerging field of near-zero-index photonics. In this regard, the recent history of nonlinear optics in conductive oxides is growing extremely fast due to a great number of experiments reporting unprecedentedly remarkable effects, including unitary index change, bandwidth-large frequency shift, efficient ultra-low-power frequency conversion, and many others. This review is meant to guide the reader through the exciting journey of TCOs, starting as an industrial material for transparent electrodes, then becoming a new alternative for low-loss plasmonics, and recently opening up new frontiers in integrated nonlinear optics. The present review is mainly focused on experimental observations.

42 ENGINEERING↗
DOE OSTI2022

Tunable plasmon-enhanced second-order optical nonlinearity in transition-metal dichalcogenide nanotriangles (Final Report for SC0008712)

The control of light-matter interaction at the nanoscale is a grand challenge that cuts across modern photonics, plasmonics, and optoelectronics. The development of simulation tools for predictive modeling of nanostructured light emitters and absorbers is critical to successfully tackling this grand challenge. Existing state-of-the-art tools are not suitable for the following reasons: a) Phenomenological models of materials, commonly employed in the full-wave solutions to Maxwell’s equations, are fit to experimental data for bulk materials and fall short when attempting to analyze nanostructures. b) Nonlinearities in optical response can arise solely from nanostructuring, and require time-dependent quantum electronic transport techniques to capture. c) Emergent materials with exotic and tunable physical properties are increasingly used, but their properties are very sensitive to the substrate, impurities, and edge termination, and require an accurate description of interband and intraband processes, as well as dissipation. d) Microscopic modeling of electronic transport usually employs simplified electrodynamics, and realistic models that couple full electronic transport with full-wave electrodynamics are needed for accurate photonics simulations. The objective of this project was to computational tools that will overcome the limitations faced by current modeling tools and provide an unprecedented level of accuracy for predictive modeling of light-matter interaction at the nanoscale.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Plasmon and Photon Excitations in Two-Dimensional and Layered Materials

Light-matter interactions in layered and two-dimensional materials allows one to achieve extreme optical confinement approaching the atomic scale, enabling exploration of new materials phenomena. Layered narrow bandgap and zero bandgap materials, such as black phosphorus and graphene, support unusual and intriguing quantum-confined electronic states in thin layers and surface electronic states. The incomplete screening of applied electrostatic fields in ultrathin materials permits the exploration of light-matter interactions at high electric fields and over a wide range of carrier densities in a single sample, facilitating exploration of the optical and plasmonic properties of ultrathin and layered materials under electrochemical potential control. We have made advances in understanding the nature of optical interband and intraband plasmon excitations in layered materials such as graphene, black phosphorus, molybdenum diselenide, and molybdenum ditelluride.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Inter-Oligomer Interaction Influence on Photoluminescence in Cis-Polyacetylene Semiconductor Materials

Semiconducting conjugated polymers (CPs) are pivotal in advancing organic electronics, offering tunable properties for solar cells and field-effect transistors. Here, we carry out first-principle calculations to study individual cis-polyacetylene (cis-PA) oligomers and their ensembles. The ground electronic structures are obtained using density functional theory (DFT), and excited state dynamics are explored by computing nonadiabatic couplings (NACs) between electronic and nuclear degrees of freedom. We compute the nonradiative relaxation of charge carriers and photoluminescence (PL) using the Redfield theory. Our findings show that electrons relax faster than holes. The ensemble of oligomers shows faster relaxation compared to the single oligomer. The calculated PL spectra show features from both interband and intraband transitions. The ensemble shows broader line widths, redshift of transition energies, and lower intensities compared to the single oligomer. This comparative study suggests that the dispersion forces and orbital hybridizations between chains are the leading contributors to the variation in PL. It provides insights into the fundamental behaviors of CPs and the molecular-level understanding for the design of more efficient optoelectronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Polarization Flipping of Even-Order Harmonics in Monolayer Transition-Metal Dichalcogenides

We present a systematic study of the crystal-orientation dependence of high-harmonic generation in monolayer transition-metal dichalcogenides, WS 2 and MoSe 2 , subjected to intense linearly polarized midinfrared laser fields. The measured spectra consist of both odd- and even-order harmonics, with a high-energy cutoff extending beyond the 15th order for a laser-field strength around ~1 V/nm. In WS 2 , we find that the polarization direction of the odd-order harmonics smoothly follows that of the laser field irrespective of the crystal orientation, whereas the direction of the even-order harmonics is fixed by the crystal mirror planes. Furthermore, the polarization of the even-order harmonics shows a flip in the course of crystal rotation when the laser field lies between two of the crystal mirror planes. By numerically solving the semiconductor Bloch equations for a gapped-graphene model, we qualitatively reproduce these experimental features and find the polarization flipping to be associated with a significant contribution from interband polarization. In contrast, high-harmonic signals from MoSe 2 exhibit deviations from the laser-field following of odd-order harmonics and crystal-mirror-plane following of even-order harmonics. We attribute these differences to the competing roles of the intraband and interband contributions, including the deflection of the electron-hole trajectories by nonparabolic crystal bands.

36 MATERIALS SCIENCE↗
NASA NTRS1982

Optical conductivity of alpha-Mn

The optical constants were measured at room temperature in the photon-energy range 0.6 to 6.5 eV on evaporated thin films. Evaporation conditions were chosen that gave the alpha-Mn crystal structure with reasonably large grains. The optical conductivity was separated into intraband and interband contributions by fitting to the Drude formula at low energies. The results are anomalous in comparison to other 3d transition metals. The free-electron lifetime is exceptionally sort (in agreement with the large dc resistivity of Mn), and the interband transitions seem unusually weak at the lower energies. Possible explanations related to the complicated crystal structure of alpha-Mn are discussed.

Scoles, K. J.↗
NASA NTRS1981

Longitudinal mode behavior of PbSnTe buried heterostructure lasers

Experimental results are reported on the longitudinal mode characteristics of PbSnTe buried heterostructure laser diodes operating at 10 microns. It is found that both 'wide' (5 microns) and 'narrow' (2 microns) stripe lasers operate in a single longitudinal mode over a range up to two times the threshold, as expected on the basis of the homogeneous gain model. However, a systematic change to multimode operation is found above this pumping level, which this model cannot explain. The observed phenomenon is explained by spectral inhomogeneity with an intraband relaxation time of the order of 2 ps.

Kasemset, D.↗
NASA NTRS1982

Optical conductivity of alpha-Mn

The optical constants were measured at room temperature in the photon-energy range 0.6-6.5 eV on evaporated thin films. Evaporation conditions were chosen that gave the alpha-Mn crystal structure with relatively large grains. The optical conductivity was separated into intraband and interband contributions by fitting to the Drude formula at low energies. The results are anomalous in comparison to other 3d transition metals: the free-electron lifetime is exceptionally short (in agreement with the large dc resistivity of Mn), and the interband transitions seem unusually weak at the lower energies. Possible explanations related to the complicated crystal structure of alpha-Mn with its loss of point symmetry at the atom sites are discussed.

Scoles, K. J.↗
NASA NTRS1984

An Analysis LANDSAT-4 Thematic Mapper Geometric Properties

LANDSAT Thematic Mapper P-data of Washington, D. C., Harrisburg, PA, and Salton Sea, CA are analyzed to determine magnitudes and causes of error in the geometric conformity of the data to known Earth surface geometry. Several tests of data geometry are performed. Intraband and interband correlation and registration are investigated, exclusive of map based ground truth. The magnitudes and statistical trends of pixel offsets between a single band's mirror scans (due to processing procedures) are computed, and the inter-band integrity of registration is analyzed. A line to line correlation analysis is included.

Walker, R. E.↗
NASA NTRS1984

Investigation of LANDSAT D Thematic Mapper geometric performance: Line to line and band to band registration

The geometric accuray of LANDSAT TM raw data of Toulouse (France) raw data of Mississippi, and preprocessed data of Mississippi was examined using a CDC computer. Analog images were restituted on the VIZIR SEP device. The methods used for line to line and band to band registration are based on automatic correlation techniques and are widely used in automated image to image registration at CNES. Causes of intraband and interband misregistration are identified and statistics are given for both line to line and band to band misregistration.

Begni, G.↗
NASA NTRS1995

Thermal emission from particulate surfaces: A comparison of scattering models with measured spectra

Emissivity spectra of particulate mineral samples are highly dependent on particle size when that size is comparable to the wavelength of light emitted (5-50 micrometers for the midinfrared). Proper geologic interpretation of data from planetary infrared spectrometers will require that these particle size effects be well understood. To address this issue, samples of quartz powders were produced with narrow, well-characterized particle size distributions. Mean particle diameters in these samples ranged from 15 to 227 micrometers. Emission spectra of these powders allow the first detailed comparison of the complex spectral variations with particle size observed in laboratory data with the predictions of radiative transfer models. Four such models are considered here. Hapke's relectance theory (converted to emissivity via Kirchoff's law) is the first model tested. Hapke's more recently published emission theory is also employed. The third model, the 'Mie/Conel' model, uses Mie single scattering with a two-stream approximation for multiple scattering. This model, like the first, is a converted reflec- tance model. Mie scattering assumes particles are both spherical and well separated, which is not true for the quartz powders, but includes diffraction effects. The fourth model uses the Mie solution for single scattering by spheres and inputs those results into the multiple scattering formalism of Hapke's emission theory. The results of the four models are considered in relation to the values of the optical constants n and k. We have grouped these as class 1 (k large), class 2 (k moderate, n is approximately 2), class 3 (k small, n is approximately 2), and class 4 (k small, n is approximately 1). In general, the Mie/Hapke hybrid model does best at predicting variations with grain size. In particular, it predicts changes of the correct pattern, although incorrect magnitude, for class 1 bands, where large increases in emissivity with decreasing grain size are observed. This model also does an excellent job on moderate (class 2) and very weak and intraband (class 3) regions, and correctly predicts the emission maximum and its invariance with grain size near the Christiansen frequency (class 4). The Mie/Hapke hybrid model also has the fewest free parameters of the four models examined, while maintaining the most physical treatment of the radiative transfer. The Mie/Conel model performs as well as the Mie/Hapke hybrid model in strong bands (class 1) but does not accurately model the behavior of moderate (class 2) and very weak (class 3) bands.

Moersch, J. E.↗
NASA NTRS1998

Computational Modeling of Semiconductor Dynamics at Femtosecond Time Scales

The main objective of the Joint-Research Interchange NCC2-5149 was to develop computer codes for accurate simulation of femtosecond pulse propagation in semiconductor lasers and semiconductor amplifiers [I]. The code should take into account all relevant processes such as the interband and intraband carrier relaxation mechanisms and the many-body effects arising from the Coulomb interaction among charge carriers [2]. This objective was fully accomplished. We made use of a previously developed algorithm developed at NASA Ames [3]-[5]. The new algorithm was tested on several problems of practical importance. One such problem was related to the amplification of femtosecond optical pulses in semiconductors. These results were presented in several international conferences over a period of three years. With the help of a postdoctoral fellow, we also investigated the origin of instabilities that can lead to the formation of femtosecond pulses in different kinds of lasers. We analyzed the occurrence of absolute instabilities in lasers that contain a dispersive host material with third-order nonlinearities. Starting from the Maxwell-Bloch equations, we derived general multimode equations to distinguish between convective and absolute instabilities. We find that both self-phase modulation and intensity-dependent absorption can dramatically affect the absolute stability of such lasers. In particular, the self-pulsing threshold (the so-called second laser threshold) can occur at few times the first laser threshold even in good-cavity lasers for which no self-pulsing occurs in the absence of intensity-dependent absorption. These results were presented in an international conference and published in the form of two papers.

Agrawal, Govind P.↗
NASA NTRS1996

Computational Modeling of Ultrafast Pulse Propagation in Nonlinear Optical Materials

There is an emerging technology of photonic (or optoelectronic) integrated circuits (PICs or OEICs). In PICs, optical and electronic components are grown together on the same chip. rib build such devices and subsystems, one needs to model the entire chip. Accurate computer modeling of electromagnetic wave propagation in semiconductors is necessary for the successful development of PICs. More specifically, these computer codes would enable the modeling of such devices, including their subsystems, such as semiconductor lasers and semiconductor amplifiers in which there is femtosecond pulse propagation. Here, the computer simulations are made by solving the full vector, nonlinear, Maxwell's equations, coupled with the semiconductor Bloch equations, without any approximations. The carrier is retained in the description of the optical pulse, (i.e. the envelope approximation is not made in the Maxwell's equations), and the rotating wave approximation is not made in the Bloch equations. These coupled equations are solved to simulate the propagation of femtosecond optical pulses in semiconductor materials. The simulations describe the dynamics of the optical pulses, as well as the interband and intraband.

Goorjian, Peter M.↗
NASA NTRS1998

Ultrafast Modulation and Switching of Quantum-Well Lasers using Terahertz Fields

Modulation and switching of semiconductor lasers are important for laser-based information technology. Typically the speed of modulation and switching is limited by interband processes such as stimulated and spontaneous recombinations which occur on a nanosecond time scale. This is why the diode laser modulation has been restricted to tens of GHz. Modulation at higher speed is highly desirable as the information technology enters into the so-called tera-era. In this paper, we study the possibility of utilizing THz-field-induced plasma heating to modulate quantum-well lasers. This is a timely study since, with the advancement of THz solid-state sources and free-electron lasers, THz physics and related technology is currently coming out of its infancy. The investigation of interplaying THz and optical fields is also of intruiging fundamental interest. First, we introduce theoretical plasma heating results for the quantum-well optical amplifier in the presense of an intense half-cycle THz pulse. The heated carrier distributions are then utilized to calculate the THz-pulse-induced change in refractive index and gain profile. Since the electron-hole-plasma is heated using intraband transitions, we circumvent the usual complications due to an overall change in density, and the nonlinear recovery is governed solely by the carrier-LO-phonon interactions, typically 5 ps for a complete recovery. This procedure implies THz and sub-THz switching and recovery rates, respectively; using either gain modulation or index modulation. Plasma heating via steady-state THz fields is also studied. Finally, numerical simulation of a coupled set of equations to investigate the THz modulation based on a simplified model for quantum-well lasers is presented. Our results show that a semiconductor laser can be modulated at up to 1 THz with little distortion with a THz field amplitude at the order of a few kV/cm. Laser responses to a change in THz frequency will be shown. Constraints, practicalities, and applications will be discussed.

Ning, Cun-Zheng↗