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DOE OSTI2022

Developing a high-speed terahertz imaging system based on parametric upconversion imaging for penetrative sensing

Imaging using THz waves has been a promising option for penetrative measurements in environments that are opaque to visible wavelengths. However, available THz imaging systems have been limited to relatively low frame rates and cannot be applied to study fast dynamics. This work explores the use of upconversion imaging techniques based on nonlinear optics to enable wavelength-flexible high frame rate THz imaging. UpConversion Imaging (UCI) uses nonlinear conversion techniques to shift the THz wavelengths carrying a target image to shorter visible or near-IR wavelengths that can be detected by available high-speed cameras. This report describes the analysis methodology used to design a prototype high-rate THz UCI system and gives a detailed explanations of the design choices that were made. The design uses a high-rate pulse-burst laser system to pump both THz generation and THz upconversion detection, allowing for scaling to acquisition rates in excess of 10 kHz. The design of the prototype system described in this report has been completed and all necessary materials have been procured. Assembly and characterization testing is on-going at the submission of this report. This report proposes future directions for work on high-rate THz UCI and potential applications of future systems.

47 OTHER INSTRUMENTATION↗

DOE OSTI2021

Colossal switchable photocurrents in topological Janus transition metal dichalcogenides

Nonlinear optical properties, such as bulk photovoltaic effects, possess great potential in energy harvesting, photodetection, rectification, etc. To enable efficient light–current conversion, materials with strong photo-responsivity are highly desirable. In this work, we predict that monolayer Janus transition metal dichalcogenides (JTMDs) in the 1T' phase possess colossal nonlinear photoconductivity owing to their topological band mixing, strong inversion symmetry breaking, and small electronic bandgap. 1T'JTMDs have inverted bandgaps on the order of 10 meV and are exceptionally responsive to light in the terahertz (THz) range. By first-principles calculations, we reveal that 1T' JTMDs possess shift current (SC) conductivity as large as 2300 nm μA V -2 , equivalent to a photo-responsivity of 2800 mA/W. The circular current (CC) conductivity of 1T' JTMDs is as large as ~10 4 nm μA V -2 . These remarkable photo-responsivities indicate that the 1T' JTMDs can serve as efficient photodetectors in the THz range. We also find that external stimuli such as the in-plane strain and out-of-plane electric field can induce topological phase transitions in 1T' JTMDs and that the SC can abruptly flip their directions. The abrupt change of the nonlinear photocurrent can be used to characterize the topological transition and has potential applications in 2D optomechanics and nonlinear optoelectronics.

Chemistry↗

DOE OSTI2023

Discovery of enhanced lattice dynamics in a single-layered hybrid perovskite

Layered hybrid perovskites exhibit emergent physical properties and exceptional functional performances, but the coexistence of lattice order and structural disorder severely hinders our understanding of these materials. One unsolved problem regards how the lattice dynamics are affected by the dimensional engineering of the inorganic frameworks and their interaction with the molecular moieties. Here, we address this question by using a combination of spontaneous Raman scattering, terahertz spectroscopy, and molecular dynamics simulations. This approach reveals the structural dynamics in and out of equilibrium and provides unexpected observables that differentiate single- and double-layered perovskites. While no distinct vibrational coherence is observed in double-layered perovskites, an off-resonant terahertz pulse can drive a long-lived coherent phonon mode in the single-layered system. This difference highlights the dramatic change in the lattice environment as the dimension is reduced, and the findings pave the way for ultrafast structural engineering and high-speed optical modulators based on layered perovskites.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Realizing Steady-State Microbunching with Optical Stochastic Crystallization

Optical Stochastic Cooling (OSC) is a state-of-the-art beam cooling technology first demonstrated in 2021 at the IOTA storage ring at Fermilab's FAST facility. A second phase of the research program is planned to run in early 2025 and will incorporate an optical amplifier to enable significantly increased cooling rates and greater operational flexibility. In addition to beam cooling, an OSC system can be configured to enable advanced control over the phase space of the beam. An example operational mode could enable crystallization, where the particles in a bunch are locked into a self-reinforcing, regular microstructure at the OSC fundamental wavelength; we refer to this as Optical Stochastic Crystallization (OSX). OSX represents a new path toward Steady-State Microbunching (SSMB), which may enable light sources combining the high brightness of a free-electron laser with the high repetition rate of a storage ring. Such a source has applications from the terahertz to the extreme ultraviolet (EUV), including high-power EUV generation for semiconductor lithography. This contribution will discuss the status of the OSC experimental program and its potential to achieve the first demonstration of SSMB during the upcoming experimental run.

Wallbank, M.↗

DOE OSTI2025

Realizing Steady-State Microbunching with Optical Stochastic Crystallization

Optical Stochastic Cooling (OSC) is a state-of-the-art beam cooling technology first demonstrated in 2021 at the IOTA storage ring at Fermilab's FAST facility. A second phase of the research program is planned to run in 2026 and will incorporate an optical amplifier to enable significantly increased cooling rates and greater operational flexibility. In addition to beam cooling, an OSC system can be configured to enable advanced control over the phase space of the beam. An example operational mode could enable crystallization, where the particles in a bunch are locked into a self-reinforcing, regular microstructure at the OSC fundamental wavelength; we refer to this as Optical Stochastic Crystallization (OSX). OSX represents a new path toward Steady-State Microbunching (SSMB), which may enable light sources combining the high brightness of a free-electron laser with the high repetition rate of a storage ring. Such a source has applications from the terahertz to the extreme ultraviolet (EUV), including high-power EUV generation for semiconductor lithography. This contribution will discuss the integration of OSX development as part of the OSC program at IOTA. The design of an accelerator lattice to enable the mechanism and associated high fidelity simulations will be shown, and a path to realizing an experimental demonstration will be discussed.

Wallbank, Michael James [Fermilab]↗

DOE OSTI2025

Steady-State Microbunching using Optical Stochastic Cooling

Optical Stochastic Cooling (OSC) is a state-of-the-art beam cooling technology first demonstrated in 2021 at the IOTA storage ring at Fermilab's FAST facility. A second phase of the research program is planned to run in 2026 and will incorporate an optical amplifier to enable significantly increased cooling rates and greater operational flexibility. In addition to beam cooling, an OSC system can be configured to enable advanced control over the phase space of the beam. An example operational mode could enable crystallization, where the particles in a bunch are locked into a self-reinforcing, regular microstructure at the OSC fundamental wavelength; we refer to this as Optical Stochastic Crystallization (OSX). OSX represents a new path toward Steady-State Microbunching (SSMB), which may enable light sources combining the high brightness of a free-electron laser with the high repetition rate of a storage ring. Such a source has applications from the terahertz to the extreme ultraviolet (EUV), including high-power EUV generation for semiconductor lithography. This contribution will discuss the integration of OSX development as part of the OSC program at IOTA. The design of an accelerator lattice to enable the mechanism and associated high fidelity simulations demonstrating the beam dynamics will be shown, and a path to realizing an experimental demonstration will be discussed.

Wallbank, Michael James [Fermilab]↗

DOE OSTI2024

Realizing Steady-State Microbunching with Optical Stochastic Crystallization

43 PARTICLE ACCELERATORS↗

DOE OSTI2025

Terahertz conductivity of two-dimensional materials: a review

Two-dimensional (2D) van der Waals materials are shaping the landscape of next-generation devices, offering significant technological value thanks to their unique, tunable, and layer-dependent electronic and optoelectronic properties. Time-domain spectroscopic techniques at terahertz (THz) frequencies offer noninvasive, contact-free methods for characterizing the dynamics of carriers in 2D materials. They also pave the path toward the applications of 2D materials in detection, imaging, manufacturing, and communication within the increasingly important THz frequency range. In this paper, we overview the synthesis of 2D materials and the prominent THz spectroscopy techniques: THz time-domain spectroscopy, optical-pump THz-probe technique, and optical pump–probe THz spectroscopy. Through a confluence of experimental findings, numerical simulation, and theoretical analysis, we present the current understanding of the rich ultrafast physics of technologically significant 2D materials: graphene, transition metal dichalcogenides, MXenes, perovskites, topological 2D materials, and 2D heterostructures. Finally, we offer a perspective on the role of THz characterization in guiding future research and in the quest for ideal 2D materials for new applications.

2D materials↗

DOE OSTI2025

Harnessing Nonlinear Light: Exploring Plasmonic Nanoparticles for Amplification, Frequency Conversion, and Terahertz Emission

Explore the source record for details and available documents.

Plasmonnics, Nonlinear Optics, Photonics, Nano-par↗

NASA NTRS2009

Where is the Best Site on Earth? Domes A, B, C, and F, and Ridges A and B

The Antarctic plateau contains the best sites on earth for many forms of astronomy, but none of the existing bases were selected with astronomy as the primary motivation. In this paper, we try to systematically compare the merits of potential observatory sites. We include South Pole, Domes A, C and F, and also Ridge B (running NE from Dome A), and what we call Ridge A (running SW from Dome A). Our analysis combines satellite data, published results and atmospheric models, to compare the boundary layer, weather, free atmosphere, sky brightness, pecipitable water vapour, and surface temperature at each site. We find that all Antarctic sites are likely compromised for optical work by airglow and aurorae. Of the sites with existing bases, Dome A is the best overall; but we find that Ridge A offers an even better site. We also find that Dome F is a remarkably good site. Dome C is less good as a thermal infrared or terahertz site, but would be able to take advantage of a predicted OH hole over Antarctica during Spring.

Suanders, Will↗

DOE OSTI2024

Paratellurite Nanowires as a Versatile Material for THz Phonon Polaritons

Polaritons, i.e., hybrid quasi-particles of light and matter resonances, have been extensively investigated due to their potential to enhance light-matter interactions. Although polaritonic applications thrive in the mid-infrared range, their extension to the terahertz (THz) range remains limited. Here, we present paratellurite (α-TeO 2 ) nanowires, a versatile material acting as a platform for different types of phonon polaritons. Utilizing synchrotron infrared nanospectroscopy from 10 to 24 THz, we uncover the polaritonic properties of α-TeO 2 nanowires, showcasing their dual functionality as both a Fabry-Pérot cavity and a waveguide for surface phonon polaritons. Furthermore, near-field measurements with a free-electron laser as a THz source reveal a localized optical contrast down to 5.5 THz, an indication of hyperbolic bands. In conclusion, our findings complement the repertoire of polaritonic materials, with significant implications for advancing THz technologies.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Harnessing complexity: Nonlinear optical phenomena in L-shapes, nanocrescents, and split-ring resonators

Here, we conduct systematic studies of the optical characteristics of plasmonic nanoparticles that exhibit C 2v symmetry. In particular, we analyze three distinct geometric configurations: an L-type shape, a crescent, and a split-ring resonator shaped like the Greek letter π. Optical properties are examined using the finite-difference time-domain method. It is demonstrated that all three shapes exhibit two prominent plasmon modes associated with the two axes of symmetry. This is in addition to a wide range of resonances observed at high frequencies corresponding to quadrupole modes and peaks due to sharp corners. Next, to facilitate nonlinear analysis, we employ a semiclassical hydrodynamic model, where the electron pressure term is explicitly accounted for. This model goes beyond the standard Drude description and enables capturing nonlocal and nonlinear effects. Employing this model enables us to rigorously examine the second-order angular resolved nonlinear optical response of these nanoparticles in each of the three configurations. Two pumping regimes are considered, namely, continuous wave (CW) and pulsed excitations. For CW pumping, we explore the properties of the second harmonic generation (SHG). Polarization and angle-resolved SHG spectra are obtained, revealing strong dependence on the nanoparticle geometry and incident wave polarization. The C 2v symmetry is shown to play a key role in determining the polarization states and selection rules of the SHG signal. For pulsed excitations, we discuss the phenomenon of broadband terahertz (THz) generation induced by the difference-frequency generation . It is shown that the THz emission spectra exhibit unique features attributed to the plasmonic resonances and symmetry of the nanoparticles. The polarization of the generated THz waves is also examined, revealing interesting patterns tied to the nanoparticle geometry. To gain deeper insight, we propose an analytical theory that agrees very well with the numerical experiments. The theory shows that the physical origin of the THz radiation is the mixing of various frequency components of the fundamental pulse by the second-order nonlinear susceptibility. An expression for the far-field THz intensity is derived in terms of the incident pulse parameters and the nonlinear response tensor of the nanoparticle. The results presented in this work offer new insights into the linear and nonlinear optical properties of nanoparticles with C 2v symmetry. The demonstrated strong SHG response and efficient broadband THz generation hold great promise for applications in nonlinear spectroscopy, nanophotonics, and optoelectronics. The proposed theoretical framework also provides a valuable tool for understanding and predicting the nonlinear behavior of other related nanostructures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Ultra-low-power second-order nonlinear optics on a chip

Second-order nonlinear optical processes convert light from one wavelength to another and generate quantum entanglement. Creating chip-scale devices to efficiently control these interactions greatly increases the reach of photonics. Existing silicon-based photonic circuits utilize the third-order optical nonlinearity, but an analogous integrated platform for second-order nonlinear optics remains an outstanding challenge. Here we demonstrate efficient frequency doubling and parametric oscillation with a threshold of tens of micro-watts in an integrated thin-film lithium niobate photonic circuit. We achieve degenerate and non-degenerate operation of the parametric oscillator at room temperature and tune its emission over one terahertz by varying the pump frequency by hundreds of megahertz. Finally, we observe cascaded second-order processes that result in parametric oscillation. These resonant second-order nonlinear circuits will form a crucial part of the emerging nonlinear and quantum photonics platforms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Selection rules and dynamic magnetoelectric effect of the spin waves in multiferroic Bi Fe O 3

Here, we report the magnetic-field dependence of the THz absorption and nonreciprocal directional dichroism spectra of BiFeO 3 measured on the three principal crystal cuts for fields applied along the three principal directions of each cut. From the systematic study of the light polarization dependence, we deduced the optical selection rules of the spin-wave excitations. Our THz data, combined with small-angle neutron scattering results showed that (i) an in-plane magnetic field rotates the q vectors of the cycloids perpendicular to the magnetic field and (ii) the selection rules are mostly determined by the orientation of the q vector with respect to the electromagnetic fields. We observed a magnetic field history-dependent change in the strength and the frequency of the spin-wave modes, which we attributed to the change of the orientation and the length of the cycloidal q vector, respectively. Finally, we compared our experimental data with the results of linear spin-wave theory that reproduces the magnetic-field dependence of the spin-wave frequencies and most of the selection rules, from which we identified the spin-polarization coupling terms relevant for the optical magnetoelectric effect.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2023

Unconventional room-temperature carriers in the triangular-lattice Mott insulator TbInO3

Abstract The strong correlations between electrons in Mott insulator materials may produce highly entangled many-body states with unconventional emergent excitations. The signatures of such excitations, if any, are commonly believed to be observable only at low temperatures. Here, we challenge this common belief and show using terahertz time-domain spectroscopy that exotic carriers exist even at room temperature in TbInO 3 , a candidate material for realizing a low-temperature quantum spin-liquid phase. In particular, over the entire temperature range of 1.5–300 K, we observe a quadratic frequency dependence in the real part of the in-plane optical conductivity as well as Fano asymmetry of an optical phonon mode strongly interacting with the excitation continuum. These features are robust even under external magnetic fields of up to 7 T. Our data confirm the presence of emergent charge carriers within the Mott charge gap of TbInO 3 , suggesting that it is possible to probe and manipulate highly entangled quantum many-body states at room temperature.

Physics↗

DOE OSTI2024

Photonic time-crystalline behaviour mediated by phonon squeezing in T a 2 NiSe 5

Photonic time crystals refer to materials whose dielectric properties are periodic in time, analogous to a photonic crystal whose dielectric properties is periodic in space. Here, we theoretically investigate photonic time-crystalline behaviour initiated by optical excitation above the electronic gap of the excitonic insulator candidate Ta 2 NiSe 5 . We show that after electron photoexcitation, electron-phonon coupling leads to an unconventional squeezed phonon state, characterised by periodic oscillations of phonon fluctuations. Squeezing oscillations lead to photonic time crystalline behaviour. The key signature of the photonic time crystalline behaviour is terahertz (THz) amplification of reflectivity in a narrow frequency band. The theory is supported by experimental results on Ta 2 NiSe 5 where photoexcitation with short pulses leads to enhanced THz reflectivity with the predicted features. We explain the key mechanism leading to THz amplification in terms of a simplified electron-phonon Hamiltonian motivated by ab-initio DFT calculations. Our theory suggests that the pumped Ta 2 NiSe 5 is a gain medium, demonstrating that squeezed phonon noise may be used to create THz amplifiers in THz communication applications.

36 MATERIALS SCIENCE↗

NASA NTRS2010

Real-time, continuous-wave terahertz imaging using a microbolometer focal-plane array

The present invention generally provides a terahertz (THz) imaging system that includes a source for generating radiation (e.g., a quantum cascade laser) having one or more frequencies in a range of about 0.1 THz to about 10 THz, and a two-dimensional detector array comprising a plurality of radiation detecting elements that are capable of detecting radiation in that frequency range. An optical system directs radiation from the source to an object to be imaged. The detector array detects at least a portion of the radiation transmitted through the object (or reflected by the object) so as to form a THz image of that object.

Hu, Qing↗

NASA NTRS2014

Characterization of MgB2 Superconducting Hot Electron Bolometers

Hot-Electron Bolometer (HEB) mixers have proven to be the best tool for high-resolution spectroscopy at the Terahertz frequencies. However, the current state of the art NbN mixers suffer from a small intermediate frequency (IF) bandwidth as well as a low operating temperature. MgB2 is a promising material for HEB mixer technology in view of its high critical temperature and fast thermal relaxation allowing for a large IF bandwidth. In this work, we have fabricated and characterized thin-film (approximately 15 nanometers) MgB2-based spiral antenna-coupled HEB mixers on SiC substrate. We achieved the IF bandwidth greater than 8 gigahertz at 25 degrees Kelvin and the device noise temperature less than 4000 degrees Kelvin at 9 degrees Kelvin using a 600 gigahertz source. Using temperature dependencies of the radiation power dissipated in the device we have identified the optical loss in the integrated microantenna responsible as a cause of the limited sensitivity of the current mixer devices. From the analysis of the current-voltage (IV) characteristics, we have derived the effective thermal conductance of the mixer device and estimated the required local oscillator power in an optimized device to be approximately 1 microwatts.

Superconducting Devices↗