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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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90 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Limits to Electrical Mobility in Lead-Halide Perovskite Semiconductors

Semiconducting polycrystalline thin films are cheap to produce and can be deposited on flexible substrates, yet high-performance electronic devices usually utilize single crystal semiconductors, owing to their superior charge-carrier mobilities and longer diffusion lengths. Here we show that the electrical performance of polycrystalline films of metal-halide perovskites (MHPs) approaches that of single crystals at room temperature. Combining temperature-dependent terahertz conductivity measurements and ab initio calculations we uncover a complete picture of the origins of charge-carrier scattering in single crystals and polycrystalline films of CH 3 NH 3 PbI 3 . We show that Fröhlich scattering of charge carriers with multiple phonon modes is the dominant mechanism limiting mobility, with grain-boundary scattering further reducing mobility in polycrystalline films. We reconcile the large discrepancy in charge-carrier diffusion lengths between single crystals and films by considering photon reabsorption. Thus, polycrystalline films of MHPs offer great promise for devices beyond solar cells, including light-emitting diodes and modulators.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Near-octave lithium niobate soliton microcomb

Thin film lithium niobate (LN) is bringing renewed potential to the realm of integrated photonics. Its strong quadratic and cubic nonlinearities as well as wide transparency window are ideal for realizing on-chip self-referenced soliton microcombs. However, broadband Kerr cavity soliton generation in LN thin films remains challenging due to limited dispersion control and competition from strong stimulated Raman scattering (SRS). Here, we demonstrate the generation of soliton microcombs in LN thin films featuring broad spectral spans up to 4/5 octaves with the emission of dual dispersion waves (2/3 octaves apart) and sub-terahertz repetition rates (down to 335 GHz) by suppressing strong SRS. Numerical simulations based on coupled-mode equations that incorporate Raman effects further elucidate the soliton dynamics in this highly Raman-active material system.

Gong, Zheng (ORCID:0000000301704870)↗
DOE OSTI2021

Design and performance of a multi-terahertz Fourier transform spectrometer for axion dark matter experiments

Dedicated spectrometers for terahertz radiation with [0.3, 30] THz frequencies using traditional optomechanical interferometry are substantially less common than their infrared and microwave counterparts. This paper presents the design and initial performance measurements of a tabletop Fourier transform spectrometer (FTS) for multi-terahertz radiation using infrared optics in a Michelson arrangement. This is coupled to a broadband pyroelectric photodetector designed for [0.1, 30] THz frequencies. We measure spectra of narrowband and broadband input radiation to characterize the performance of this instrument above 10 THz, where signal-to-noise is high. This paves the groundwork for planned upgrades to extend below 10 THz. We also briefly discuss potential astroparticle physics applications of such FTS instruments to broadband axion dark matter searches, whose signature comprises low-rate monochromatic photons with unknown frequency.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2024

A Perspective on the Impact of Group Delay Dispersion in Future Terahertz Wireless Systems

This article discusses the challenges and opportunities of managing group delay dispersion (GDD), and its relation to the performance standards of future sixth-generation (6G) wireless communication systems utilizing terahertz frequency waves. The unique susceptibilities of 6G systems to GDD are described, along with a quantitative description of the sources of GDD, including multipath, rough surface scattering, intelligent reflecting surfaces, and propagation through the atmosphere. An experimental case-study is presented that confirms previous models quantifying the impact of atmospheric GDD. Several GDD manipulation strategies are presented, illustrating their hindered effectiveness in the 6G context. Conversely, some benefits of leveraging GDD to enhance 6G systems, such as improved security and simplified hardware, are also discussed. Finally, a perspective on using photonic GDD control devices is provided, revealing quantitative benefits that may unburden existing equalization schemes. Here, the article argues that GDD will uniquely and significantly impact some 6G systems, but that its careful consideration along with new mitigation strategies, including photonic devices, will help optimize system performance. The conclusion provides a perspective to guide future research in this area.

Strecker, Karl↗
DOE OSTI2025

Terahertz-field activation of polar skyrons

Unraveling collective modes arising from coupled degrees of freedom is crucial for understanding complex interactions in solids and developing new functionalities. Unique collective behaviors emerge when two degrees of freedom, ordered on distinct length scales, interact. Polar skyrmions, three-dimensional electric polarization textures in ferroelectric superlattices, disrupt the lattice continuity at the nanometer scale with nontrivial topology, leading to previously unexplored collective modes. Here, using terahertz-field excitation and femtosecond x-ray diffraction, we discover subterahertz collective modes, dubbed “skyrons”, which appear as swirling patterns of atomic displacements functioning as atomic-scale gearsets. The key to activating skyrons is the use of the THz field that couples primarily to skyrmion domain walls. Momentum-resolved time-domain measurements of diffuse scattering reveal an avoided crossing in the dispersion relation of skyrons. Atomistic simulations and dynamical phase-field modeling provide microscopic insights into the three-dimensional crystallographic and polarization dynamics. The amplitude and dispersion of skyrons are demonstrated to be controlled by sample temperature and electric-field bias. The discovery of skyrons and their coupling with terahertz fields opens avenues for ultrafast control of topological polar structures.

ferroelectrics↗
DOE OSTI2025

Helical Photonic Metamaterials for Encrypted Chiral Holograms

Helical structures are among the most quintessential three-dimensional (3D) forms that exhibit mirror asymmetry, a hallmark of chirality. Various structural parameters of helices directly linked to chiroptical properties highlight their importance as essential optical metamaterials for polarization-resolved sensors, imaging, and spectroscopies. However, such function-defining properties remain incompletely understood due to fabrication challenges and the lack of a relationship between structure and optical properties. Here, helical structures are analyzed parametrically, and correlations are established that are applicable to the design of chiral helical optical metamaterials. By systematically varying independent parameters—such as from single-turn to five-turn helices and from small major radii to larger ones optimized to fit the unit cell—the underlying relationships with ellipticty are revealed. In addition to theoretical modeling, the findings are experimentally validated using 3D printing and terahertz spectroscopy. The results demonstrate that optimized helical structures are mechanically tunable and exhibit unprecedented optical properties, including broadband and high-magnitude ellipticity spectra. Being embedded in soft elastomers, helical arrays can serve as soft, stretchable optical-mechanical sensors and holograms containing encoded information, such as barcodes and quick response (QR) codes. Chiral QR codes are realized using pixelated single helices with different handedness, demonstrating their potential as advanced encryption/decryption systems for security applications and chiral metaholograms.

Encrypted QR codes↗
DOE OSTI2023

Chiral Spectroscopy of Nanostructures

Chirality is ubiquitous in the universe and in living creatures over detectable length scales from the subatomic to the galactic, as exemplified in the two extremes by subatomic particles (neutrinos) and spiral galaxies. Between them are living creatures that display multiple levels of chirality emerging from hierarchically assembled asymmetric building blocks. Not too far from the bottom of this pyramid are the foundational building blocks with chiral atomic centers on sp 3 carbon atoms exemplified by L-amino acids and D-sugars that are self-assembled into higher-order structures with increasing dimensions forming highly complex, amazingly functional, and energy-efficient living systems. The organization and materials employed in their construction inspired scientists to replicate complex living systems via the self-assembly of chiral components. Multiple studies pointed to unexpected and unique electromagnetic properties of chiral structures with nanoscale and microscale dimensions, including giant circular dichroism and collective circularly polarized scattering that their constituent units did not possess. To address the wide variety of chiral geometries observed in continuous materials, singular particles, and their complex systems, multiple analytic techniques are needed. Simultaneously, their spectroscopic properties create a pathway to multiple applications. For example, mirror-asymmetric vibrations at chiral centers formed by sp 3 carbon atoms lead to optical activity for the infrared (IR) wavelength regions. At the same time, understanding the optical activity in, for example, the IR region enables biomedical applications because multiple modalities of biomedical imaging and vibrational optical activity (VOA) of biomolecules are known for IR range. In turn, VOA can be realized in both absorption and emission modalities due to large magnetic transition moments, as vibrational circular dichroism (VCD) or Raman optical activity (ROA) spectroscopy. In addition to the VOA, in the range of longer wavelengths, lattice vibrational mode or phononic behavior occurs in chiral crystals and nanoassemblies, which can be readily detected by terahertz circular dichroism (TCD) spectroscopy. Meanwhile, chiral self-assembly can induce circularly polarized light emission (CPLE) regardless of the existence of chirality in coassembled fluorophores. The CPLE from self-assembled chiral materials is particularly interesting because the CPLE can originate from both circularly polarized luminescence and circularly polarized scattering (CPS). Furthermore, because self-assembled nanostructures often exhibit stronger optical activity than their building blocks owing to dimension and resonance effects, the optical activity of single assembled nanostructures can be investigated by using microscopic technology combined with chiral optics. Here, we describe the state of the art for spectroscopic methods for the comprehensive analysis of chiral nanomaterials at various photon wavelengths, addressed with special attention given to new tools emerging both for materials with self-organized hierarchical chirality and single-particle spectroscopy.

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

Spin-induced linear polarization of photoluminescence in antiferromagnetic van der Waals crystals

Antiferromagnets are promising components for spintronics due to their terahertz resonance, multilevel states and absence of stray fields. However, the zero net magnetic moment of antiferromagnets makes the detection of the antiferromagnetic order and the investigation of fundamental spin properties notoriously difficult. Here, we report an optical detection of Néel vector orientation through an ultra-sharp photoluminescence in the van der Waals antiferromagnet NiPS 3 from bulk to atomically thin flakes. The strong correlation between spin flipping and electric dipole oscillator results in a linear polarization of the sharp emission, which aligns perpendicular to the spin orientation in the crystal. By applying an in-plane magnetic field, we achieve manipulation of the photoluminescence polarization. Furthermore, this correlation between emitted photons and spins in layered magnets provides routes for investigating magneto-optics in two-dimensional materials, and hence opens a path for developing opto-spintronic devices and antiferromagnet-based quantum information technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Theory of terahertz pulse transmission through ferroelectric nanomembranes

An analytical model is developed to predict the temporal evolution of the lattice polarization in ferroelectric nanomembranes upon the excitation by a terahertz (THz) electromagnetic pulse of an arbitrary waveform and the concurrent transmission of the THz pulse in both linear and nonlinear regimes. It involves the use of the perturbation method to solve the equation of motion for the lattice polarization in both unclamped and strained ferroelectric nanomembranes within the framework of Landau-Ginzburg-Devonshire theory. The model is applicable to perovskite oxides such as BaTiO 3 and SrTiO 3 , wurtzite Al 1−𝑥 ⁢Sc 𝑥 ⁢N, and trigonal LiNbO 3 . Our analytical model provides a theoretical basis for determining the thermodynamic and kinetic parameters of ferroelectric materials through a THz transmission experiment. The calculation results also suggest an approach to reversing the chirality of a circularly polarized THz pulse by harnessing the resonant polarization-photon coupling in ferroelectrics. This capability of chirality reversal, along with the high tunability from a strain applied along any arbitrarily oriented in-plane axis, provides new opportunities for THz wave modulation without relying on complex metasurface designs.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Optical information transfer through random unknown diffusers using electronic encoding and diffractive decoding

Free-space optical information transfer through diffusive media is critical in many applications, such as biomedical devices and optical communication, but remains challenging due to random, unknown perturbations in the optical path. We demonstrate an optical diffractive decoder with electronic encoding to accurately transfer the optical information of interest, corresponding to, e.g., any arbitrary input object or message, through unknown random phase diffusers along the optical path. This hybrid electronic-optical model, trained using supervised learning, comprises a convolutional neural network-based electronic encoder and successive passive diffractive layers that are jointly optimized. After their joint training using deep learning, our hybrid model can transfer optical information through unknown phase diffusers, demonstrating generalization to new random diffusers never seen before. The resulting electronic-encoder and optical-decoder model was experimentally validated using a 3D-printed diffractive network that axially spans <70λ, where λ = 0.75 mm is the illumination wavelength in the terahertz spectrum, carrying the desired optical information through random unknown diffusers. The presented framework can be physically scaled to operate at different parts of the electromagnetic spectrum, without retraining its components, and would offer low-power and compact solutions for optical information transfer in free space through unknown random diffusive media.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Terahertz parametric amplification as a reporter of exciton condensate dynamics

Condensates are a hallmark of emergence in quantum materials with superconductors and charge density wave as prominent examples. An excitonic insulator (EI) is an intriguing addition to this library, exhibiting spontaneous condensation of electron-hole pairs. However, condensate observables can be obscured through parasitic coupling to the lattice. Time-resolved terahertz (THz) spectroscopy can disentangle such obscurants through measurement of the quantum dynamics. We target Ta 2 NiSe 5 , a putative room-temperature EI where electron-lattice coupling dominates the structural transition (T c = 326 K), hindering identification of excitonic correlations. A pronounced increase in the THz reflectivity manifests following photoexcitation and exhibits a BEC-like temperature dependence. This occurs well below the T c , suggesting a novel approach to monitor exciton condensate dynamics. Nonetheless, dynamic condensate-phonon coupling remains as evidenced by peaks in the enhanced reflectivity spectrum at select infrared-active phonon frequencies. This indicates that parametric reflectivity enhancement arises from phonon squeezing, validated using Fresnel-Floquet theory and density functional calculations. In conclusion, our results highlight that coherent dynamics can drive parametric stimulated emission with concomitant possibilities, including entangled THz photon generation.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Performance analysis of photodetectors based on 2D materials and heterostructures

The unprecedented demand for sophisticated, self-powered, compact, ultrafast, cost-effective, and broadband light sensors for a myriad of applications has spurred a lot of research, precipitating in a slew of studies over the last decade. Apart from the photosensing ability of an active element in the light sensor, the device architecture is crucial in terms of photoinduced charge carrier generation and separation. Since the inception of graphene and the subsequent research growth in the atomically thin 2D materials, researchers have developed and adapted different families of 2D materials and device architectures, including single element 2D, 0D/2D, 2D/2D, 1D/2D stacked structures, and so on. Here this review discusses the recent reports on the light-sensing properties of various 2D materials, their heterostructures, and characteristics applicable to the ultraviolet-near infrared (UV-NIR), short-wave IR (SWIR), mid-wave IR (MWIR), long-wave IR (LWIR), and terahertz (THz) spectral ranges. It highlights the novelty of the burgeoning field, the heightened activity at the boundaries of engineering and materials science, particularly in the generation of charge carriers, their separation, and extraction, and the increased understanding of the underpinning science through modern experimental approaches. Devices based on the simultaneous effects of the pyro-phototronic effect (PPE) and the localized surface plasmon resonance (LSPR) effect, the photothermoelectric effect (PTE)-assisted photodetectors (PDs), waveguide-integrated silicon-2D PDs, metal-2D-metal PDs, and organic material PDs are examined rigorously. Theoretical treatment utilizing various computational approaches to investigate 2D materials and heterostructures for photodetection applications is also briefly discussed. At the end, current challenges and solutions to enhance the figures of merit of photodetectors are proposed.

2D transition metal chalcogenides↗
DOE OSTI2026

Nanoscale strain wave generation by a piezoelectric grating from polar vortices

Nanostructures formed by spontaneously broken symmetry have provided new ways to manipulate quantum states. Specifically, topological structures with periodic spatial ordering, such as polar vortices and skyrmions, can be ideal hosts for creating engineered responses in both spatial and frequency domains. So far, however, only a few examples of such hierarchical engineering have been reported in the literature. Here we demonstrate that the spatially modulated piezoelectric response of a polar vortex structure can create strain waves with a characteristic nanoscale wavefront. Using time-resolved pump–probe resonant X-ray scattering and diffraction measurements, coupled with dynamical phase-field simulations, we show that the piezoelectric modulation of the spontaneously formed polar vortex crystal functions as an acoustic diffraction grating. This system converts incoming laterally uniform strain waves into outgoing waves with a characteristic sub-terahertz frequency, driven by an intrinsic excitation of the polar vortex crystal. Moreover, our phase-field simulations suggest that the dynamic mechanical displacements exhibiting vortex textures are generated from both space- and time-varying piezoelectric responses. Our findings illustrate a new method for generating nanoscale strain waves with unique spatial textures by tuning the hierarchical order of polar topologies to engineer new collective modes, allowing for a wide range of control through the topological lattice.

ferroelectrics↗
DOE OSTI2024

Surface plasmon-cavity hybrid state and its graphene modulation at THz frequencies

Fabry–Pérot (F–P) cavity and metal hole array are classic photonic devices. Integrating F–P cavity with holey metal typically enhances interfacial reflection and dampens wave transmission. In this work, a hybrid bound surface state is found within rectangular metal holes on a silicon substrate by merging an extraordinary optical transmission (EOT) mode and a high-order F–P cavity mode both spatially and spectrally. Transmission, Q-factor, and bandwidth can be enhanced significantly with respect to the classical EOT and F–P interference by simply sweeping the cavity length. This state can provide EOT properties and ten times broader EOT bandwidth well below the effective plasma frequency of the periodic metal holes, where the metal holes typically show evanescent properties and do not support EOT in theory. Furthermore, a large modulation range of 25 % and 39 % is demonstrated with various graphene patterns for the transmittance of this hybrid state at 500 and 582 GHz, respectively.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Direct Evidence of Photoinduced Charge Transport Mechanism in 2D Conductive Metal Organic Frameworks

Conductive metal organic frameworks (MOFs) represent a promising class of porous crystalline materials that have demon-strated potential in photo-electronics and photocatalytic applications. However, the lack of fundamental understanding on charge transport (CT) mechanism as well as the correlation of CT mechanism with their structure hampered their further development. Herein, we report the direct evidence of CT mechanism in 2D Cu-THQ MOFs and the correlation of temporal and spatial behaviors of charge carriers with their photoconductivity by combining three advanced spectroscopic methods including time resolved optical and X-ray absorption spectroscopy and terahertz spectroscopy. In addition to Cu-THQ, the CT in Cu/Zn-THQ after incorporating Zn2+ guest metal was also examined to uncover the contribution of through space pathway as the presence of the redox inactive 3d10 Zn2+ is expected to perturb the long range in-plane CT. We show that the hot carriers in Cu-THQ generated after photoexcitation are highly mobile and undergo fast localization to a lower energy state (cool carriers) with electrons occupying Cu center and holes in ligands. The cool carriers, which have super long lifetime (> 17 ns) are responsible for the long-term photoconductivity in Cu-THQ and transport through O-Cu-O motif with negligible contribution from interlayer ligand π-π stacking as incorporation of Zn2+ in Cu-THQ significantly reduced photoconductivi-ty. These unprecedent results not only demonstrate the capability to experimentally probe CT mechanism but also provide important insight in the rational design of 2D MOFs for photoelectronic and photocatalytic applications.

14 SOLAR ENERGY↗
DOE OSTI2025

Ultrafast simultaneous manipulation of multiple ferroic orders through nonlinear phonon excitation

Recent experimental studies have demonstrated the possibility of utilizing strong terahertz pulses to manipulate individual ferroic orders on pico- and femtosecond timescales. Here, we extend these findings and showcase the simultaneous manipulation of multiple ferroic orders in BiFeO 3 , a material that is both ferroelectric and antiferromagnetic at room temperature. We find a concurrent enhancement of ferroelectric and antiferromagnetic second-harmonic generation (SHG) following the resonant excitation of a high-frequency fully-symmetric phonon mode. Based on first-principles calculations and phenomenological modeling, we ascribe this observation to the inherent coupling of the two ferroic orders to the nonequilibrium distortions induced in the crystal lattice by nonlinearly driven phonons. Our finding highlights the potential of nonlinear phononics as a technique for manipulating multiple ferroic order parameters at once. In addition, this approach provides a promising avenue to studying the dynamical magnetic and polarization behavior, as well as their intrinsic coupling, on ultrashort timescales.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Substrate birefringence as a source of artifacts in spintronic THz emission spectra

Terahertz (THz) emission from spintronic THz emitters (STEs) has been extensively studied, both for its potential application in THz technologies and as a tool for probing spin dynamics, conductivity, and crystal anisotropy via time-domain THz spectroscopy. However, substrate birefringence can modify the emitted THz polarization, distorting the measured spectra and leading to potential misinterpretation of the results. While some aspects of substrate birefringence on THz emission have been studied in the time domain, its effects on THz spectra have not been discussed in detail. In the THz emission spectrum from STEs, we observe distinct spectral signatures that depend on sample orientation. To understand these signatures, we use STEs grown on c-cut sapphire and systematically vary the orientation of a (100) rutile TiO 2 window in both pump-through and THz-through geometries to identify the birefringence-induced effects. These findings demonstrate that substrate birefringence plays a critical role in the emitted THz spectrum and must be carefully considered in the analysis of time-domain THz spectroscopy data. We also show that artifacts from smaller birefringence can have a more misleading effect on the THz spectra.

Shrestha, Shreya [Univ. of Delaware, Newark, DE (U↗
DOE OSTI2025

Observation of polarization density waves in SrTiO 3

The nature of the incipient ferroelectric transition in SrTiO 3 has been a long-standing puzzle in condensed matter physics. One explanation involves the competition between ferroelectricity and an instability characterized by the mesoscopic modulation of the polarization. These polarization density waves, which should intensify near the quantum critical point, break local inversion symmetry and are difficult to characterize with conventional X-ray scattering methods. Here, in this study, we probe inversion symmetry breaking at finite momenta and visualize the instability of the polarization at the nanometre scale in SrTiO3 by combining a femtosecond X-ray free-electron laser with terahertz coherent control methods. We found polar-acoustic collective modes that are soft, particularly at the tens of nanometre scale. These precursor collective excitations provide evidence for the conjectured mesoscopic-modulated phase in SrTiO 3 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗