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At least 91 records · Page 5

Terahertz inverse spin Hall effect in spintronic nanostructures with various ferromagnetic materials

Bilayers of ferromagnetic and heavy metal nanolayers excited with femtosecond laser pulses emit subpicosecond bursts of electromagnetic radiation with spectral frequencies up to several THz. We fabricated such spintronic THz emitters containing various ferromagnetic materials with vastly different magnetic remanence, saturation magnetization, and coercive fields. In all cases, the THz amplitude versus magnetic-field dependence follows the independently measured magnetization hysteresis loops and the THz polarization direction is perpendicular to the sample’s magnetization M, both consistent with the inverse spin Hall effect (ISHE) as the physical origin. The mV-level signals of observed THz transient also favor the ISHE over the anomalous Nernst effect (ANE). The M(T) variation governs the temperature dependence of the THz generation. Emitters with weakly remanent ferromagnets are magnetic-field tunable, while moderately and strongly remanent ferromagnets, once magnetized, allow intense THz generation even without an external field, nevertheless exhibiting low susceptibility to magnetic perturbations if the hysteresis loop is square. Hence, exploiting the magnetic properties of the ferromagnetic layer enables tailoring of weakly temperature-dependent spintronic THz emitters. Finally, we explored the applicability of perovskite oxide materials such as La-Sr-Mn-O (LSMO) for THz transient generation. We detected weak (<40-μV amplitude) THz emissions from both LSMO/Au and pure LSMO nanostructures with no sign flip upon the sample reversal. Furthermore, we excluded the ISHE and believe it was likely governed by the ANE in the thick-film regime, although we cannot exclude the transient demagnetization mechanism.

36 MATERIALS SCIENCE↗

Time-domain terahertz emission spectroscopy on van der Waals materials

Time-domain terahertz (THz) emission spectroscopy provides a direct method to probe transient photo-currents by recording the emitted terahertz electric field. Although the basic principles of THz surface emission have been understood for more than 30 years, the constant progress in ultrafast laser science to ever shorter pulses, the development of new materials and enhanced sensitivity promote THz emission spectroscopy as a reliable method to gain insights into charge carrier dynamics with unprecedented precision. It provides a versatile tool to study ultrafast processes, such as plasmon-driven hot carriers, dynamics of Dirac fermions, interfacial charge transfer, coherent phonon emission and quantum beating, to name only a few. However, despite the rapidly growing body of research on van der Waals materials, especially in their low-dimensional limit, THz emission spectroscopy has only been applied to a limited extent in these material systems. In this prospective, we review time-domain THz emission spectroscopy as a complementary approach to probe ultrafast charge carrier dynamics and the material’s nonlinear response. After a description of the experimental method, we report on THz emission spectroscopy of bulk and 2D van der Waals materials with special focus on graphene and transition metal dichalcogenide layers.

2D materials↗

Broadband sum-frequency generation of spectrally incoherent pulses

We study and demonstrate the nonlinear frequency conversion of broadband optical pulses from 1053 nm to 351 nm using sum-frequency generation with a narrowband pulse at 526.5 nm. The combination of angular dispersion and noncollinearity cancels out the wave-vector mismatch and its frequency derivative, yielding an order-of-magnitude increase in spectral acceptance compared to conventional tripling. This scheme can support the nonlinear frequency conversion of broadband spectrally incoherent nanosecond pulses generated by high-energy lasers and optical parametric amplifiers to mitigate laser−plasma instabilities occurring during interaction with a target. The experimental results obtained with KDP crystals are in excellent agreement with modeling, demonstrating the generation of spectrally incoherent pulses with a bandwidth larger than 10 THz at 351 nm.

47 OTHER INSTRUMENTATION↗

Surface-Emitting Distributed Feedback Terahertz Quantum-Cascade Lasers in Metal-Metal Waveguides

Single-mode surface-emitting distributed feedback terahertz quantumcascade lasers operating around 2.9 THz are developed in metal-metal waveguides. A combination of techniques including precise control of phase of reflection at the facets, and u e of metal on the sidewalls to eliminate higher-order lateral modes allow robust single-mode operation over a range of approximately 0.35 THz. Single-lobed far-field radiation pattern is obtained using a pi phase-shift in center of the second-order Bragg grating. A grating device operating at 2.93 THz lased up to 149 K in pulsed mode and a temperature tuning of 19 .7 GHz was observed from 5 K to 147 K. The same device lased up to 78 K in continuous-wave (cw) mode emitting more than 6 m W of cw power at 5 K. ln general, maximum temperature of pulsed operation for grating devices was within a few Kelvin of that of multi-mode Fabry-Perot ridge lasers

Kumar, Sushil↗

Effect of THz-bandwidth incoherent laser radiation on bulk damage in potassium dihydrogen phosphate crystals

Abstract The laser-damage performance characteristics of potassium dihydrogen phosphate (KDP) samples under exposure to a distinctive broadband incoherent laser pulse are investigated. A laser system providing such pulses is intended to explore improved energy-coupling efficiency on the target in direct-drive inertial confinement fusion experiments and provides incoherent bandwidths as large as 10 THz in a nanosecond pulse. A consequence of this bandwidth is very rapid fluctuations in intensity capable of reaching maxima much larger than the average intensity within the pulse. A custom damage-test station has been built to perform measurements with broadband incoherent pulses in order to determine what effect these fast and high-intensity oscillations have on laser damage. A set of experiments under different bandwidth and beam configurations shows the effect to be minimal when probing bulk damage in KDP. Modeling indicates this behavior is supported by long electron-relaxation times compared to the source-field fluctuations, following excitation of individual electrons in the conduction band. The results help better understand the laser-induced–damage mechanisms in KDP, and its ability to operate in broadband temporally incoherent high-energy lasers that may be particularly suitable for future laser-fusion energy systems.

36 MATERIALS SCIENCE↗

Improved temporal resolution in ultrafast electron diffraction measurements through THz compression and time-stamping

We present an experimental demonstration of ultrafast electron diffraction (UED) with THz-driven electron bunch compression and time-stamping that enables UED probes with improved temporal resolution. Through THz-driven longitudinal bunch compression, a compression factor of approximately four is achieved. Moreover, the time-of-arrival jitter between the compressed electron bunch and a pump laser pulse is suppressed by a factor of three. Simultaneously, the THz interaction imparts a transverse spatiotemporal correlation on the electron distribution, which we utilize to further enhance the precision of time-resolved UED measurements. We use this technique to probe single-crystal gold nanofilms and reveal transient oscillations in the THz near fields with a temporal resolution down to 50 fs. These oscillations were previously beyond reach in the absence of THz compression and time-stamping.

43 PARTICLE ACCELERATORS↗

Femtosecond photocurrents at the FeRh/Pt interface

Femtosecond laser excitations of FeRh/Pt bilayers launch an ultrafast pulse of electric photocurrents in the Pt-layer and subsequently result in the emission of electromagnetic radiation in the THz spectral range. Analysis of the THz emission as a function of the polarization of the femtosecond laser pulse, external magnetic field, sample temperature, and sample orientation shows that the photocurrent can emerge due to vertical spin pumping and photo-induced inverse spin–orbit torque at the FeRh/Pt interface. Additionally, the vertical spin pumping from FeRh into Pt does not depend on the polarization of light and originates from ultrafast laser-induced demagnetization of the ferromagnetic phase of FeRh. The photo-induced inverse spin–orbit torque at the FeRh/Pt interface can be described in terms of a helicity-dependent effect of circularly polarized light on the magnetization of the ferromagnetic FeRh and the subsequent generation of a photocurrent.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Coherent control of asymmetric spintronic terahertz emission from two-dimensional hybrid metal halides

Abstract Next-generation terahertz (THz) sources demand lightweight, low-cost, defect-tolerant, and robust components with synergistic, tunable capabilities. However, a paucity of materials systems simultaneously possessing these desirable attributes and functionalities has made device realization difficult. Here we report the observation of asymmetric spintronic-THz radiation in Two-Dimensional Hybrid Metal Halides (2D-HMH) interfaced with a ferromagnetic metal, produced by ultrafast spin current under femtosecond laser excitation. The generated THz radiation exhibits an asymmetric intensity toward forward and backward emission direction whose directionality can be mutually controlled by the direction of applied magnetic field and linear polarization of the laser pulse. Our work demonstrates the capability for the coherent control of THz emission from 2D-HMHs, enabling their promising applications on the ultrafast timescale as solution-processed material candidates for future THz emitters.

36 MATERIALS SCIENCE↗

Multilayer Dielectric Transmissive Optical Phase Modulator

A multilayer dielectric device has been fabricated as a prototype of a low-loss, low-distortion, transmissive optical phase modulator that would provide as much as a full cycle of phase change for all frequency components of a transmitted optical pulse over a frequency band as wide as 6.3 THz. Arrays of devices like this one could be an alternative to the arrays of mechanically actuated phase-control optics (adaptive optics) that have heretofore been used to correct for wave-front distortions in highly precise optical systems. Potential applications for these high-speed wave-front-control arrays of devices include agile beam steering, optical communications, optical metrology, optical tracking and targeting, directional optical ranging, and interferometric astronomy. The device concept is based on the same principle as that of band-pass interference filters made of multiple dielectric layers with fractional-wavelength thicknesses, except that here there is an additional focus on obtaining the desired spectral phase profile in addition to the device s spectral transmission profile. The device includes a GaAs substrate, on which there is deposited a stack of GaAs layers alternating with AlAs layers, amounting to a total of 91 layers. The design thicknesses of the layers range from 10 nm to greater than 1 micrometer. The number of layers and the thickness of each layer were chosen in a computational optimization process in which the wavelength dependences of the indices of refraction of GaAs and AlAs were taken into account as the design was iterated to maximize the transmission and minimize the group-velocity dispersion for a wavelength band wide enough to include all significant spectral components of the pulsed optical signal to be phase modulated.

Keys, Andrew Scott↗

Ultrafast bipolar conductivity driven by intense single-cycle terahertz pulses in a topological insulator Bi 2 Se 3

We present the measurement of ultrafast terahertz (THz) conductivity of a 50 nm thick topological insulator Bi 2 Se 3 at low temperature 5 K by using a THz pump and THz probe spectroscopy scheme. Here, the THz conductivity driven by a single-cycle intense THz pump exhibits a bipolar lineshape and frequency-dependent relaxation dynamics due to the separated surface and bulk charge carriers with distinctly different scattering rates and relaxation times. We also demonstrate THz pump field-dependent excitation of the surface and bulk spectral weights, which suggests one of the optimal THz excitation conditions for generating the most charge carriers from the topology-protected surface state relative to the bulk. This also allows THz control of surface and bulk transport channels in a selective way.

36 MATERIALS SCIENCE↗

Investigation of Fiber Waviness in a Thick Glass Composite Beam Using THz NDE

Fiber waviness in laminated composite material is introduced during manufacture because of uneven curing, resin shrinkage, or ply buckling caused by bending the composite lay-up into its final shape prior to curing. The resulting waviness has a detrimental effect on mechanical properties, therefore this condition is important to detect and characterize. Ultrasonic characterization methods are difficult to interpret because elastic wave propagation is highly dependent on ply orientation and material stresses. By comparison, the pulsed terahertz response of the composite is shown to provide clear indications of the fiber waviness. Pulsed Terahertz NDE is an electromagnetic inspection method that operates in the frequency range between 300 GHz and 3 THz. Its propagation is influenced by refractive index variations and interfaces. This work applies pulsed Terahertz NDE to the inspection of a thick composite beam with fiber waviness. The sample is a laminated glass composite material approximately 15mm thick with a 90-degree bend. Terahertz response from the planar section, away from the bend, is indicative of a homogeneous material with no major reflections from internal plies, while the multiple reflections at the bend area correspond to the fiber waviness. Results of these measurements are presented for the planar and bend areas.

Anastasi, Robert F.↗

Quenched lattice fluctuations in optically driven SrTiO3

Abstract Crystal lattice fluctuations, which are known to influence phase transitions of quantum materials in equilibrium, are also expected to determine the dynamics of light-induced phase changes. However, they have only rarely been explored in these dynamical settings. Here we study the time evolution of lattice fluctuations in the quantum paraelectric SrTiO 3 , in which mid-infrared drives have been shown to induce a metastable ferroelectric state. Crucial in these physics is the competition between polar instabilities and antiferrodistortive rotations, which in equilibrium frustrate the formation of long-range ferroelectricity. We make use of high-intensity mid-infrared optical pulses to resonantly drive the Ti–O-stretching mode at 17 THz, and we measure the resulting change in lattice fluctuations using time-resolved X-ray diffuse scattering at a free-electron laser. After a prompt increase, we observe a long-lived quench in R-point antiferrodistortive lattice fluctuations. Their enhancement and reduction are theoretically explained by considering the fourth-order nonlinear phononic interactions to the driven optical phonon and third-order coupling to lattice strain, respectively. These observations provide a number of testable hypotheses for the physics of light-induced ferroelectricity.

36 MATERIALS SCIENCE↗

Detection and imaging of chemicals and hidden explosives using terahertz time-domain spectroscopy and deep learning

Detecting concealed chemicals and explosives remains a critical challenge in global security. Terahertz time-domain spectroscopy (THz-TDS) offers a promising non-invasive and stand-off detection technique owing to its ability to penetrate optically opaque materials without causing ionization damage. While many chemicals exhibit distinct spectral features in the terahertz range, conventional terahertz-based detection methods often struggle in real-world environments, where variations in sample geometry, thickness, and packaging can lead to inconsistent spectral responses. In this study, we present a chemical imaging system that integrates THz-TDS with deep learning to enable accurate pixel-level identification and classification of different explosives. Operating in reflection mode and enhanced with plasmonic nanoantenna arrays, our THz-TDS system achieves a peak dynamic range of 96 dB and a detection bandwidth of 4.5 THz, supporting practical, stand-off operation. By analyzing individual time-domain pulses with deep neural networks, the system exhibits strong resilience to environmental variations and sample inconsistencies. Blind testing across eight chemicals—including pharmaceutical excipients and explosive compounds—resulted in an average classification accuracy of 99.42% at the pixel level. Notably, the system maintained an average accuracy of 88.83% when detecting explosives concealed under opaque paper coverings, demonstrating its robust generalization capability. These results highlight the potential of combining advanced terahertz spectroscopy with neural networks for highly sensitive and specific chemical and explosive detection in diverse and operationally relevant scenarios.

Imaging and sensing↗

Tapering-enhanced high-efficiency THz waveguide oscillator

Using a waveguide in a THz FEL has been shown to maximize the coupling and enable efficient extraction of relativistic electron beam energy from a single passage through a tapered helical undulator. An oscillator configuration can further boost energy extraction above the single-pass limits and open the door toward very high average power THz sources. Embedding the undulator in an oscillator cavity is particularly useful in combination with high repetition rate electron sources, even if at reduced peak brightness, since recycling a fraction of the radiation as an intense seed can compensate for lower single-pass gain. In this paper, we investigate the efficiency scaling of a tapering-enhanced waveguide oscillator, showcasing its capability for frequency-tuning operation and high-efficiency operation at different wavelengths. Using a thermionic-driven beamline equipped with compression elements, numerical start-to-end simulation results indicate a 16% efficiency at 200 GHz and a 2.1% efficiency at 1.5 THz, resulting in kW-level average power out-coupled in radiation pulses with few hundred μ J energy and tens of MW peak power. Published by the American Physical Society 2024

Yang, Y. N. (ORCID:0009000849540151)↗

Operation of Terahertz Quantum-cascade Lasers at 164 K in Pulsed Mode and at 117 K in Continuous-wave Mode

We report the demonstration of a terahertz quantum-cascade laser that operates up to 164 K in pulsed mode and 117 K in continuous-wave mod e at approximately 3.0 THz. The active region was based on a resonant -phonon depopulation scheme and a metal-metal waveguide was used for modal confinement. Copper to copper thermocompression wafer bonding w as used to fabricate the waveguide, which displayed improved thermal properties compared to a previous indium-gold bonding method.

Williams, Benjamin S.↗

High-speed fiber-coupled terahertz time-domain spectroscopy system using a bias-free plasmonic source

We demonstrate a high-speed fiber-coupled terahertz time-domain spectroscopy (THz-TDS) system using a bias-free plasmonic terahertz source. The system is powered by a compact, low-power femtosecond fiber laser oscillator that drives a dual-branch fiber amplifier to pump and probe a plasmonic terahertz source and detector, respectively. A polarization-maintaining, fiber-coupled optical delay line is employed to precisely control the temporal offset between the pump and probe beams through a compact, robust platform. Operating in the self-similar amplification regime, the fiber amplifiers are engineered to mitigate nonlinear pulse distortion and dispersion while delivering robust, high-energy pulses at a 1560-nm wavelength, with an output power exceeding 326 mW. In reflection mode, the THz-TDS system achieves a peak dynamic range of 81 dB and a bandwidth greater than 3.5 THz at a scan rate of 3.75 Hz. The utility of the system for rapid sensing is further demonstrated by quantifying the porosity and density of pharmaceutical tablets through measurements of their physical thickness and effective refractive index.

Jiang, Xinghe [University of California, Los Angel↗

Rotational spectroscopy at the Jet Propulsion Laboratory

Environmental monitoring, atmospheric remote sensing and astrophysical studies promoted by NASA require a strong basis of spectroscopic information. The rotational spectroscopy capabilities at NASAs Jet Propulsion Laboratory (JPL) are currently maintained for the measurement of key mission priorities that enable modeling and retrieval of geophysical data from the atmosphere as well as validation of the space-borne instruments in the Earth Observing System, particularly the Microwave Limb Sounder. Rotational spectra are measured using a variety of spectroscopic techniques including pulsed-beam Fourier transform microwave spectroscopy (at CalTech); millimeter wavelength Stark spectroscopy; millimeter, submillimeter and THz FM spectroscopy; laser sideband spectroscopy and Fourier Transform far-infrared spectroscopy. Remote measurements of atmospheric rotational spectra are made using two limb-sounder instruments in the submillimeter and THz. Recent advances in the direct synthesis of THz radiation that enable more efficient laboratory science will be presented. Software for comprehensive and systematic study of different molecular systems is maintained at JPL, the software is freely available via http://spec.jpl.nasa.gov and is used by our group to create and sustain the JPL spectral line catalog also available online.

molecular spectroscopy↗

The birth and evolution of solvated electrons in the water

The photo-induced radiolysis of water is an elementary reaction in biology and chemistry, forming solvated electrons, OH radicals, and hydronium cations on fast time scales. Here, we use an optical-pump terahertz-probe spectroscopy setup to trigger the photoionization of water molecules with optical laser pulses at ~400 nm and then time-resolve the transient solvent response with broadband terahertz (THz) fields with a ~90 fs time resolution. We observe three distinct spectral responses. The first is a positive broadband mode that can be attributed to an initial diffuse, delocalized electron with a radius of (22 ± 1) Å, which is short lived (<200 fs) because the absorption is blue-shifting outside of the THz range. The second emerging spectroscopic signature with a lifetime of about 150 ps is attributed to an intermolecular mode associated with a mass rearrangement of solvent molecules due to charge separation of radicals and hydronium cations. After 0.2 ps, we observe a long-lasting THz signature with depleted intensity at 110 cm -1 that is well reproduced by ab initio molecular dynamics. We interpret this negative band at 110 cm -1 as the solvent cage characterized by a weakening of the hydrogen bond network in the first and second hydration shells of the cavity occupied by the localized electron.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗