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At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Extreme terahertz magnon multiplication induced by resonant magnetic pulse pairs

Nonlinear interactions of spin-waves and their quanta, magnons, have emerged as prominent candidates for interference-based technology, ranging from quantum transduction to antiferromagnetic spintronics. Yet magnon multiplication in the terahertz (THz) spectral region represents a major challenge. Intense, resonant magnetic fields from THz pulse-pairs with controllable phases and amplitudes enable high order THz magnon multiplication, distinct from non-resonant nonlinearities such as the high harmonic generation by below-band gap electric fields. Here, we demonstrate exceptionally high-order THz nonlinear magnonics. It manifests as 7th-order spin-wave-mixing and 6th harmonic magnon generation in an antiferromagnetic orthoferrite. We use THz two-dimensional coherent spectroscopy to achieve high-sensitivity detection of nonlinear magnon interactions up to six-magnon quanta in strongly-driven many-magnon correlated states. The high-order magnon multiplication, supported by classical and quantum spin simulations, elucidates the significance of four-fold magnetic anisotropy and Dzyaloshinskii-Moriya symmetry breaking. Moreover, our results shed light on the potential quantum fluctuation properties inherent in nonlinear magnons.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Ultrafast Terahertz Field Control of the Emergent Magnetic and Electronic Interactions at Oxide Interfaces

Ultrafast electric-field control of emergent electronic and magnetic states at oxide interfaces offers exciting prospects for the development of the next generation of energy-efficient devices. Here, it is demonstrated that the electronic structure and emergent ferromagnetic interfacial state in epitaxial LaNiO3/CaMnO3 superlattices can be effectively controlled using intense, single-cycle THz electric-field pulses. A suite of advanced X-ray spectroscopic techniques is employed to measure a detailed magneto-optical profile and the thickness of the ferromagnetic interfacial layer. Then, a combination of time-resolved and temperature-dependent optical measurements is used to disentangle several correlated electronic and magnetic processes driven by ultrafast, high-field THz pulses. Sub-picosecond non-equilibrium Joule heating of the electronic system is observed, ultrafast demagnetization of the ferromagnetic interfacial layer, and slower dynamics indicative of a change in the magnetic state of the superlattice due to the transfer of spin-angular momentum to the lattice. These findings suggest a promising avenue for the efficient control of 2D ferromagnetic states at oxide interfaces using ultrafast electric-field pulses.

X-ray spectroscopy and scattering↗
DOE OSTI2023

Designing polar textures with ultrafast neuromorphic features from atomistic simulations

This review summarizes recent works, all using a specific atomistic approach, that predict and explain the occurrence of key features for neuromorphic computing in three archetypical dipolar materials, when they are subject to THz excitations. The main ideas behind such atomistic approach are provided, and illustration of model relaxor ferroelectrics, antiferroelectrics, and normal ferroelectrics are given, highlighting the important potential of polar materials as candidates for neuromorphic computing. Some peculiar emphases are made in this Review, such as the connection between neuromorphic features and percolation theory, local minima in energy path, topological transitions and/or anharmonic oscillator model, depending on the material under investigation. By considering three different and main polar material families, this work provides a complete and innovative toolbox for designing polar-based neuromorphic systems.

THz pulses↗
DOE OSTI2022

Electro-optic sampling based characterization of broad-band high efficiency THz-FEL

Extremely high beam-to-radiation energy conversion efficiencies can be obtained in a THz FEL using a strongly tapered helical undulator at the zero-slippage resonant condition, where a circular waveguide is used to match the radiation group velocity to the electron beam longitudinal velocity. In this paper we report on the first electro-optic sampling (EOS) based measurements of the broadband THz FEL radiation pulses emitted in this regime. The THz field waveforms are reconstructed in the spatial and temporal domains using multi-shot and single-shot EOS schemes respectively. The measurements are performed varying the input electron beam energy in the undulator providing insights on the complex dynamics in a waveguide FEL.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2023

Space-Time Quantum Information from the Entangled States of Magnetic Molecule (STI Product)

This collaborative project combines synthesis, measurement, and theory by three faculty members at the Eddleman Quantum Institute of UC Irvine to effectively investigate the quantum properties of molecules in the space, time, and frequency domains. Through synthetic chemistry, molecules are tailored for their magnetic and coherent properties. By combining femtosecond (fs) terahertz (THz) light and a continuous wave (cw) THz laser with a low temperature scanning tunneling microscope (STM), quantum phenomena are probed with simultaneous femtosecond temporal and atomic-scale spatial resolution. In particular, the invention of the quantum superposition microscope (QSM) advances quantum sensing for enhanced spectroscopy and imaging capabilities. Coupling theory to the experimental efforts offers a deeper understanding and predictive power for the molecular systems. The phenomena of superposition, entanglement, and coherence is central to quantum information science and can be realized in qubit states. Many systems can be modeled by a double-well potential in which two levels are formed in the two lowest energy states interacting with the environment and external radiation. In focusing on molecules as two-level systems, the underlying expectation is that their tunable composition and structure allows an effective parameter space to optimize their use as qubits for quantum sensing and computing. The THz radiation induces the superposition between the two states, appearing as temporal oscillations that damp in amplitude. Enhanced spectroscopy and imaging in the time and frequency domains is achieved through the extreme sensitivity of the frequency and damping of coherence of two-level systems to its environment. A single hydrogen molecule trapped in the STM tunneling gap experiences a double-well potential and absorption of THz femtosecond pulses of light creates the superposition of its two levels, appearing as damped oscillations in the light induced direct current (DC). The oscillation frequency depends sensitively on the electric field distribution of the copper nitride (Cu 2 N) surface, through the Stark effect, and associated with the different charge distributions at the copper and nitrogen sites and in between. This QSM can resolve variation in the surface electric field with 0.02 nanometer resolution. In addition, the single hydrogen molecule entaes with nearby hydrogen molecules as seen in the avoided level crossings of energy (oscillation frequency) versus the voltage across the tunneling gap. Thus, the first application of the QSM senses and images the surface electric field at the atomic scale. Results from this project advance fundamental understanding of quantum phenomena, develop novel synthesis, measurement, and theory, provide the knowledge foundation for molecule-based qubits and sensing that enable the development of the QSM and emergent technologies. This project trained researchers in quantum information science, extended knowledge in classrooms, and outreached to the community.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Ultra-short pulse generation from mid-IR to THz range using plasma wakes and relativistic ionization fronts

In this work, we discuss numerical and experimental results on frequency downshifting and upshifting of a 10 μ m infrared (IR) laser to cover the entire wavelength (frequency) range from λ = 1 to 150 μ m ( ν = 300–2 THz) using two different plasma techniques. The first plasma technique utilizes frequency downshifting of the drive laser pulse in a nonlinear plasma wake. Based on this technique, we have proposed and demonstrated that in a tailored plasma structure, multi-millijoule energy, single-cycle, long-wavelength IR (3–20 μ m) pulses can be generated by using an 810 nm Ti:sapphire drive laser. Here, we extend this idea to the THz frequency regime. We show that sub-joule, terawatts, single-cycle terahertz (2–12 THz or 150–25 μ m) pulses can be generated by replacing the drive laser with a picosecond 10 μ m CO 2 laser and a different shaped plasma structure. The second plasma technique employs frequency upshifting by colliding a CO 2 laser with a rather sharp relativistic ionization front created by ionization of a gas in less than half cycle (17 fs) of the CO 2 laser. Even though the electrons in the ionization front carry no energy, the frequency of the CO 2 laser can be upshifted due to the relativistic Doppler effect as the CO 2 laser pulse enters the front. The wavelength can be tuned from 1 to 10 μ m by simply changing the electron density of the front. While the upshifted light with 5 < λ ( μ m ) < 10 propagates in the forward direction, that with 1 < λ ( μ m ) < 5 is back-reflected. These two plasma techniques seem extremely promising for covering the entire molecular fingerprint region.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Optical Spectrometer With a Pulse-to-Pulse Resolution for Terahertz and mm-Wave Signals

The development of ultra-compact particle accelerators and accelerator-based high-power THz generators are some of the top priorities for research and development programs around the world. These tools require the development of accelerating structures, operating in the mm-Wave and THz range, where diagnostics are not available or are insufficient. This article presents the design of a pulse-to-pulse THz spectrometer, primarily developed for diagnostics of accelerating structures and THz radiation sources. In particular, this spectrometer can be used to detect RF pulse shortening caused by vacuum breakdown and beam misalignment in THz accelerators, as well as for bunch length monitoring and radiation source diagnostics. The spectrometer is based on a diffraction grating and is capable of covering a frequency range where RF-based breakdown measurements are not possible. We have built and tested the first prototype with different sources in a frequency range of 0.1-1.0 THz. In this article, we present the physical design, supported numerical simulations, electronics development, and test results.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Pulse Length Monitor for Breakdown Diagnostics in THz and Mm-Wave Accelerators

The development of novel high-gradient accelerating structures operating at THz frequencies is critical for future free-electron lasers and TeV scale linear colliders. To reach high energies with reasonable length requires high accelerating gradients of ~100 MV/m. The main limitation to reaching these high-energy gradients is the vacuum RF breakdown phenomenon, which disrupts normal accelerator operations. For stable operations and to understand the breakdown microscopic dynamics, a new device capable of detecting the breakdown occurrences is required. In this paper, we provide the design of a pulse length monitor based on an analog to digital converter for fast signal digitization without the need to use high-speed digitizers to be used in a commercial mm-wave heterodyne spectrometer.

43 PARTICLE ACCELERATORS↗
DOE OSTI2024

Thin-film lithium niobate electro-optic terahertz wave detector

Here, the design, fabrication, and validation of a thin-film lithium niobate on insulator (LNOI) electro-optic (EO) time-domain terahertz (THz) wave detector is reported. LNOI offers unprecedented properties for the EO detection of freely propagating THz wave radiation pulses and transient electric fields because of the large EO coefficient of the material, engineering of the velocity matching of the THz wave and optical wave, and much reduced detector size. The proof-of-concept device is realized using thin-film lithium niobate optical waveguides forming a Mach–Zehnder interferometer with interferometer arms electrically poled in opposite directions. THz waves are coupled effectively to the fully dielectric device from free space without using antennas or plasmonics. The detection of THz waves with frequencies up to 800 GHz is successfully demonstrated. The detector allows for the detection of THz frequency electric fields up to 4.6 MV/m. The observed frequency response of the device agrees well with theoretical predictions.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Light quantum control of persisting Higgs modes in iron-based superconductors

The Higgs mechanism, i.e., spontaneous symmetry breaking of the quantum vacuum, is a cross-disciplinary principle, universal for understanding dark energy, antimatter and quantum materials, from superconductivity to magnetism. Unlike one-band superconductors (SCs), a conceptually distinct Higgs amplitude mode can arise in multi-band, unconventional superconductors via strong interband Coulomb interaction, but is yet to be accessed. Here we discover such hybrid Higgs mode and demonstrate its quantum control by light in iron-based high-temperature SCs. Using terahertz (THz) two-pulse coherent spectroscopy, we observe a tunable amplitude mode coherent oscillation of the complex order parameter from coupled lower and upper bands. The nonlinear dependence of the hybrid Higgs mode on the THz driving fields is distinct from any known SC results: we observe a large reversible modulation of resonance strength, yet with a persisting mode frequency. Together with quantum kinetic modeling of a hybrid Higgs mechanism, distinct from charge-density fluctuations and without invoking phonons or disorder, our result provides compelling evidence for a light-controlled coupling between the electron and hole amplitude modes assisted by strong interband quantum entanglement. Such light-control of Higgs hybridization can be extended to probe many-body entanglement and hidden symmetries in other complex systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Ultrafast Activation and Tuning of Topological Textures in Ferroelectric Nanostructures

Polar topological textures are recently discovered in ultra–thin ferroelectrics, including stripe, labyrinth, or bubble states. Enabling to shape on–demand, these topologies herein can provide an original platform for potential applications. Here, using first–principle–based calculations, it is shown that THz electric field pulses are an efficient means for generating a plethora of topological states in ultrathin films made by a prototypical ferroelectric system, depending on the characteristics of these pulses and films. Consequently, these ultrafast electrical pulses in ultra–thin ferroelectrics offer key ingredients for mimicking neuronal and synaptic behaviors, including all–optical devices, and open a new avenue for topological objects to neuromorphic systems.

36 MATERIALS SCIENCE↗
DOE OSTI2025

First high peak and average power single-pass THz free-electron laser in operation

We report on the operation of the first high peak and average power single-pass terahertz free-electron laser (THz FEL) based on a high-brightness photoinjector for developing a THz source for pump-probe experiments at advanced x-ray FELs (XFELs). Electron beams with 17 MeV/c momentum and charge up to 2.4 nC were used to generate narrow-band 3 THz radiation with pulse energies of more than 0.1 mJ. The novelty of the realized method is that the undulator radiation by electron beams is much longer than the radiation wavelength, with FEL starting from coherent beam contribution rather than shot noise. This proved to be not a simple scaling of the XFEL mechanism due to the significant role of the bunching factor in the considered case.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Spatiotemporal control of two-color terahertz generation

A laser pulse composed of a fundamental and properly phased second harmonic exhibits an asymmetric electric field that can drive a time-dependent current of photoionized electrons. The current produces an ultrashort burst of terahertz (THz) radiation. When driven by a conventional laser pulse, the THz radiation is emitted into a cone with an angle determined by the dispersion of the medium. Here we demonstrate that the programmable-velocity intensity peak of a spatiotemporally structured, two-color laser pulse can be used to control the emission angle, focal spot, and spectrum of the THz radiation. Of particular interest for applications, a structured pulse with a subluminal intensity peak can drive highly focusable, on-axis THz radiation. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Multidimensional coherent spectroscopy of light-driven states and their collective modes in multiband superconductors

We present a comprehensive theory of light-controlled multiband superconductivity, and apply it to predict distinctive signatures of light-driven superconducting (SC) states in terahertz multidimensional coherent spectroscopy (THz-MDCS) experiments. We first derive gauge-invariant Maxwell-Bloch equations for multiband BCS superconductors with spatial fluctuations. We consider driving electromagnetic fields determined self-consistently by Maxwell's equations. By calculating the THz-MDCS spectra measured experimentally in the clean SC limit, we identify unique signatures of finite-momentum Cooper-pairing states that live longer than the laser pulse. They are controlled by a pair of THz laser pulses with well-defined relative phase (pulse pair). The pseudospin oscillators that describe the properties of these SC states are parametrically driven by both finite-momentum Cooper pairing and by time oscillations of the order-parameter relative phase. We show that such strong parametric driving leads to drastic changes in the THz-MDCS spectral shape from the predictions of third-order nonlinear susceptibility calculations. These spectral changes strongly depend on the interband-to-intraband interaction ratio and on the collective modes of the light-driven state. For negligible interband interaction, the spectra show a transition with increasing field, from traditional pump-probe, four-wave-mixing, and third-harmonic generation peaks determined by the laser frequency to sidebands determined by the excitations of the driven system. These sidebands emerge from difference-frequency Raman processes in the nonequilibrium SC state. For interband couplings weaker than the intraband pairing, we show that the Leggett phase collective mode leads to harmonic sidebands around the traditional pump-probe peaks. Additional Higgs collective mode peaks result from light-induced inversion-symmetry breaking in a thin-film geometry. For strong interband coupling, we find a transition from a nonequilibrium finite Cooper-pair momentum state characterized by hybrid-Higgs amplitude mode peaks in THz-MDCS spectra to a driven state identified experimentally by the emergence of Floquet-type sidebands at bi-Higgs frequencies. Those dominant bi-Higgs-frequency satellites are manifestations of a new order parameter relative phase collective mode that characterizes the nonequilibrium SC state. The predicted interaction- and field-dependent transitions in the spectral profile allow us to propose THz-MDCS experiments for quantum tomography of light-driven superconductivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
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↗
DOE OSTI2020

Terahertz Second-Harmonic Generation from Lightwave Acceleration of Symmetry-Breaking Nonlinear Supercurrents

We report terahertz (THz) light-induced second harmonic generation, in superconductors with inversion symmetry that forbid even-order nonlinearities. The THz second harmonic emission vanishes above the superconductor critical temperature and arises from precession of twisted Anderson pseudospins at a multicycle, THz driving frequency that is not allowed by equilibrium symmetry. We explain the microscopic physics by a dynamical symmetry breaking principle at sub-THz-cycle by using quantum kinetic modeling of the interplay between strong THz-lightwave nonlinearity and pulse propagation. In this work, the resulting nonzero integrated pulse area inside the superconductor leads to light-induced nonlinear supercurrents due to subcycle Cooper pair acceleration, in contrast to dc-biased superconductors, which can be controlled by the band structure and THz driving field below the superconducting gap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

6 MeV novel hybrid (standing wave - traveling wave) photo-cathode electron gun for a THz superradiant FEL

A novel 6 MeV hybrid photo-injector has been designed and constructed, based on a smaller-scale prototype previously built in UCLA’s Particle Beam Physics Laboratory. It has been commissioned at Ariel University in Israel as an on-going collaboration between the two universities. This unique, new generation design provides a radically simpler approach to RF feeding of a gun/buncher system, leading to a much shorter beam via velocity bunching owed to an attached traveling wave section of the photo-injector. This design offers better performance in beam parameters, providing a high quality electron beam, with energy of 6 MeV. The hybrid photo-injector was designed to provide emittance of approximately 3 μm, and pulse duration of 150 fs at up to 1 nC per pulse. The hybrid gun is driven by a SLAC XK5 klystron as the high power RF source, and third harmonic of a ~35 fs IR Laser amplifier (266 nm) to extract electrons from the photo-cathode. The unique electron gun will produce a bunched electron pulse to drive a THz FEL, which will operate at the super-radiant regime, and therefore requires ambitious beam properties. This paper describes the gun and presents experimental results from the gun and its sub-systems, including energy and charge measurements, compared with the design simulations.

150fs↗
DOE OSTI2023

Searching for optimal THz generation through calculations of the asymmetry of photoelectron momentum distributions by an improved strong-field-approximation method

From the solution of the time-dependent Schrödinger equation (TDSE), it has been shown that in a two-color laser pulse the relative phase that optimizes terahertz (THz) radiation also optimizes the asymmetry of the angular distribution of photoelectrons. Here, in this work, we show that a second-order strong-field approximation can accurately calculate the asymmetry of photoelectrons and thus can locate the phase delay that optimizes THz generation, doing so four orders of magnitude faster than TDSE calculations. We further trace that this is possible because THz emission originates from a free-free radiative transition between the rescattered electron and the target ion, similar to other electron-ion collisions in the laser field, e.g., high-harmonic generation and nonsequential double ionization. Our results pave the way to locate the optimal phase delay for any typical laser pulses for maximal THz generation in the laboratory.

74 ATOMIC AND MOLECULAR PHYSICS↗