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At least 37 records · Page 2

Near-field terahertz nonlinear optics with blue light

Abstract The coupling of terahertz optical techniques to scattering-type scanning near-field microscopy (s-SNOM) has recently emerged as a valuable new paradigm for probing the properties of semiconductors and other materials on the nanoscale. Researchers have demonstrated a family of related techniques, including terahertz nanoscopy (elastic scattering, based on linear optics), time-resolved methods, and nanoscale terahertz emission spectroscopy. However, as with nearly all examples of s-SNOM since the technique’s inception in the mid-1990s, the wavelength of the optical source coupled to the near-field tip is long, usually at energies of 2.5 eV or less. Challenges in coupling of shorter wavelengths (i.e., blue light) to the nanotip has greatly inhibited the study of nanoscale phenomena in wide bandgap materials such as Si and GaN. Here, we describe the first experimental demonstration of s-SNOM using blue light. With femtosecond pulses at 410 nm, we generate terahertz pulses directly from bulk silicon, spatially resolved with nanoscale resolution, and show that these signals provide spectroscopic information that cannot be obtained using near-infrared excitation. We develop a new theoretical framework to account for this nonlinear interaction, which enables accurate extraction of material parameters. This work establishes a new realm of possibilities for the study of technologically relevant wide-bandgap materials using s-SNOM methods.

47 OTHER INSTRUMENTATION↗

Giant topological longitudinal circular photo-galvanic effect in the chiral multifold semimetal CoSi

The absence of mirror symmetry, or chirality, is behind striking natural phenomena found in systems as diverse as DNA and crystalline solids. A remarkable example occurs when chiral semimetals with topologically protected band degeneracies are illuminated with circularly polarized light. Under the right conditions, the part of the generated photocurrent that switches sign upon reversal of the light’s polarization, known as the circular photo-galvanic effect, is predicted to depend only on fundamental constants. The conditions to observe quantization are non-universal, and depend on material parameters and the incident frequency. In this work, we perform terahertz emission spectroscopy with tunable photon energy from 0.2 –1.1 eV in the chiral topological semimetal CoSi. We identify a large longitudinal photocurrent peaked at 0.4 eV reaching ~550 μ A/V 2 , which is much larger than the photocurrent in any chiral crystal reported in the literature. Using first-principles calculations we establish that the peak originates only from topological band crossings, reaching 3.3 ± 0.3 in units of the quantization constant. Our calculations indicate that the quantized circular photo-galvanic effect is within reach in CoSi upon doping and increase of the hot-carrier lifetime. The large photo-conductivity suggests that topological semimetals could potentially be used as novel mid-infrared detectors.

79 ASTRONOMY AND ASTROPHYSICS↗

Linear and nonlinear optical responses in the chiral multifold semimetal RhSi

Chiral topological semimetals are materials that break both inversion and mirror symmetries. They host interesting phenomena such as the quantized circular photogalvanic effect (CPGE) and the chiral magnetic effect. In this work, we report a comprehensive theoretical and experimental analysis of the linear and nonlinear optical responses of the chiral topological semimetal RhSi, which is known to host multifold fermions. We show that the characteristic features of the optical conductivity, which display two distinct quasi-linear regimes above and below 0.4 eV, can be linked to excitations of different kinds of multifold fermions. The characteristic features of the CPGE, which displays a sign change at 0.4 eV and a large non-quantized response peak of around 160 μA/V 2 at 0.7 eV, are explained by assuming that the chemical potential crosses a flat hole band at the Brillouin zone center. Our theory predicts that, in order to observe a quantized CPGE in RhSi, it is necessary to increase the chemical potential as well as the quasiparticle lifetime. More broadly, our methodology, especially the development of the broadband terahertz emission spectroscopy, could be widely applied to study photogalvanic effects in noncentrosymmetric materials and in topological insulators in a contact-less way and accelerate the technological development of efficient infrared detectors based on topological semimetals.

Materials Science↗

Distinct Optical Excitation Mechanisms of a Coherent Magnon in a van der Waals Antiferromagnet

The control of antiferromagnets with ultrashort optical pulses has emerged as a prominent field of research. Tailored laser excitation can launch coherent spin waves at terahertz frequencies, yet a comprehensive description of their generation mechanisms is still lacking despite extensive efforts. Using terahertz emission spectroscopy, we investigate the generation of a coherent magnon mode in the van der Waals antiferromagnet NiPS 3 under a range of photoexcitation conditions. By tuning the pump photon energy from transparency to resonant with a 𝑑−𝑑 transition, we reveal a striking change in the coherent magnon’s dependence on the pump polarization, indicating two distinct excitation mechanisms. Furthermore, our findings provide a strategy for the manipulation of magnetic modes via photoexcitation around subgap electronic states.

Light-induced magnetic effects↗

Disorder and diffuse scattering in single-chirality (TaSe 4 ) 2 ⁢I crystals

The quasi-one-dimensional chiral compound (TaSe 4 ) 2 I has been extensively studied as a prime example of a topological Weyl semimetal. Upon crossing its phase transition temperature $T$ CDW ≈263K, (TaSe 4 ) 2 I exhibits incommensurate charge density wave (CDW) modulations described by the well-defined propagation vector ∼(0.05,0.05,0.11), oblique to the TaSe 4 chains. Although optical and transport properties greatly depend on chirality, there is no systematic report about chiral domain size for (TaSe 4 ) 2 I. In this study, our single-crystal scattering refinements reveal a bulk iodine deficiency, and Flack parameter measurements on multiple crystals demonstrate that separate (TaSe 4 ) 2 I crystals have uniform handedness, supported by direct imaging and helicity-dependent terahertz emission spectroscopy. Our single-crystal x-ray scattering and calculated diffraction patterns identify multiple diffuse features and create a real-space picture of the temperature-dependent (TaSe 4 ) 2 I crystal structure. Further, the short-range diffuse features are present at room temperature and decrease in intensity as the CDW modulation develops. These transverse displacements, along with electron pinning from the iodine deficiency, help explain why (TaSe 4 ) 2 I behaves as an electronic semiconductor at temperatures above and below $T$ CDW , despite a metallic band structure calculated from density functional theory of the ideal structure.

36 MATERIALS SCIENCE↗

Ultrafast THz emission spectroscopy of spin currents in the metamagnet FeRh

Heterostructures of ferromagnetic (FM) and noble metal (NM) thin films have recently attracted considerable interest as viable platforms for the ultrafast generation, control, and transduction of light-induced spin currents. In such systems, an ultrafast laser can generate a transient spin current in the FM layer, which is then converted to a charge current at the FM/NM interface due to strong spin–orbit coupling in the NM layer. Whether such conversion can happen in a single material and how the resulting spin current can be quantified are open questions under active study. Here, we report ultrafast THz emission from spin–charge conversion in a bare FeRh thin film without any NM layer. Our results highlight that the magnetic material by itself can enable spin–charge conversion in the same order as that in a FM/NM heterostructure. We further propose a simple model to estimate the light-induced spin current in FeRh across its metamagnetic phase transition temperature. Our findings have implications for the study of the ultrafast dynamics of magnetic order in quantum materials using THz emission spectroscopy.

36 MATERIALS SCIENCE↗

Ultrafast Inverse Chirality-Induced Spin Selectivity Observed by THz Emission

Chirality-induced spin selectivity (CISS) phenomena arise from an interplay among structural chirality, electron spin orientation, and charge current. Steady-state observations such as magnetoresistance offer little insight into the timescales that govern the spin-charge interconversion and often conflate interfacial and bulk phenomena. By contrast, inverse CISS involves the conversion of spin to a charge current. Using terahertz (THz) emission spectroscopy, we directly measured an ultrafast charge current due to inverse CISS with picosecond time resolution. Polarity and polarization analysis of the THz emission map the induced charge current direction upon spin injection. We found that a charge current is generated along the spin orientation that changes direction with stereochemical configuration. These observations directly demonstrate the inherent coupling between spin and charge currents in chiral systems, offering key insights into their fundamental dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗

Lightwave-driven electron emission for polarity-sensitive terahertz beam profiling

The full exploitation of advanced light sources in the terahertz (THz) frequency range requires versatile experimental tools to fully characterize the spatial, temporal, and spectral shapes of the THz electric field. Several techniques for passive THz beam profiling exist that offer information about the temporally integrated intensity. Thus, any information about the electric field itself is lost. Here, we show that a UV–visible light emission produced via a lightwave-driven field emission from single-layer metasurfaces can be used to visualize the peak electric field distribution of THz beams in real time. Our technique is scalable up to frequencies approaching the plasma frequency of the metal used for the metasurface. Uniquely, our device is sensitive to the absolute polarity of the THz lightwave. These findings demonstrate a general pathway to designing metamaterial-based field-sensitive optical detectors suitable for the entire THz and IR spectral region.

42 ENGINEERING↗

Light-Induced Currents at Domain Walls in Multiferroic BiFeO3.

Multiferroic BiFeO3 (BFO) films with spontaneously formed periodic stripe domains can generate above-gap open circuit voltages under visible light illumination; nevertheless the underlying mechanism behind this intriguing optoelectronic response has not been understood to date. Here, we make contact-free measurements of light-induced currents in epitaxial BFO films via detecting terahertz radiation emanated by these currents, enabling a direct probe of the intrinsic charge separation mechanisms along with quantitative measurements of the current amplitudes and their directions. In the periodic stripe samples, we find that the net photocurrent is dominated by the charge separation across the domain walls, whereas in the monodomain samples the photovoltaic response arises from a bulk shift current associated with the non-centrosymmetry of the crystal. The peak current amplitude driven by the charge separation at the domain walls is found to be 2 orders of magnitude higher than the bulk shift current response, indicating the prominent role of domain walls acting as nanoscale junctions to efficiently separate photogenerated charges in the stripe domain BFO films. These findings show that domain-wall-engineered BFO thin films offer exciting prospects for ferroelectric-based optoelectronics, as well as bias-free strong terahertz emitters.

36 MATERIALS SCIENCE↗

Light-driven nanoscale vectorial currents

Controlled charge flows are fundamental to many areas of science and technology, serving as carriers of energy and information, as probes of material properties and dynamics and as a means of revealing or even inducing broken symmetries. Emerging methods for light-based current control offer particularly promising routes beyond the speed and adaptability limitations of conventional voltage-driven systems. However, optical generation and manipulation of currents at nanometre spatial scales remains a basic challenge and a crucial step towards scalable optoelectronic systems for microelectronics and information science. Here we introduce vectorial optoelectronic metasurfaces in which ultrafast light pulses induce local directional charge flows around symmetry-broken plasmonic nanostructures, with tunable responses and arbitrary patterning down to subdiffractive nanometre scales. Local symmetries and vectorial currents are revealed by polarization-dependent and wavelength-sensitive electrical readout and terahertz (THz) emission, whereas spatially tailored global currents are demonstrated in the direct generation of elusive broadband THz vector beams 17 . We show that, in graphene, a detailed interplay between electrodynamic, thermodynamic and hydrodynamic degrees of freedom gives rise to rapidly evolving nanoscale driving forces and charge flows under the extremely spatially and temporally localized excitation. These results set the stage for versatile patterning and optical control over nanoscale currents in materials diagnostics, THz spectroscopies, nanomagnetism and ultrafast information processing.

36 MATERIALS SCIENCE↗

Coherent emission from surface Josephson plasmons in striped cuprates

The interplay between charge order and superconductivity remains one of the central themes of research in quantum materials. In the case of cuprates, the coupling between striped charge fluctuations and local electromagnetic fields is especially important, as it affects transport properties, coherence, and dimensionality of superconducting correlations. Here, we study the emission of coherent terahertz radiation in single-layer cuprates of the La 2-x Ba x CuO 4 family, for which this effect is expected to be forbidden by symmetry. We find that emission vanishes for compounds in which the stripes are quasi-static but is activated when c-axis inversion symmetry is broken by incommensurate or fluctuating charge stripes, such as in La 1.905 Ba 0.095 CuO 4 and in La 1.845 Ba 0.155 CuO 4 . In this case, terahertz radiation is emitted by surface Josephson plasmons, which are generally dark modes, but couple to free space electromagnetic radiation because of the stripe modulation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

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↗

Circuits Enhance Scientific Instruments and Safety Devices

Since its founding in 1958, NASA has pioneered the use of different frequencies on the electromagnetic spectrum - including X-ray, microwave, and infrared wavelengths - to gather information about distant celestial bodies. During the 1962 Mariner 2 mission, NASA used microwave radiometers that operated in the range of 15-23 gigahertz (GHz) to assess the surface temperature of Venus and to determine the percentage of water vapor in its atmosphere. Today, there is another area on the spectrum proving uniquely useful to scientists: the terahertz (THz) range, spanning from about 100 GHz-10,000 GHz. (1 THz equals approximately 1,000 GHz.) Terahertz frequencies span the lesser-known gap on the electromagnetic spectrum between microwave radiation and infrared (and visible) light, falling within the spectral range where most simple molecules resonate. This molecular resonance makes terahertz particularly useful for chemical spectroscopy and the remote sensing of specific molecules. In the 1990s, NASA began using frequencies above 300 GHz (more than an order of magnitude higher than the instrumentation on Mariner 2) to perform spectral analysis of molecular clouds and planetary atmospheres. Instruments using these higher frequencies have included the Microwave Limb Sounder (MLS) on the Upper Atmosphere Research Satellite (UARS), deployed from 1991-2001, and the Microwave Instrument for the Rosetta Orbiter (MIRO), launched in 2004. With UARS-MLS, NASA used advanced terahertz receivers to measure the emission signatures from atmospheric molecules, providing researchers with valuable data about the changes in the Earth s protective ozone layer. MIRO, set to rendezvous with the comet 67P Churyumov-Gerasimenko in 2014, will use terahertz instrumentation to analyze the comet s dust and gases. Although NASA has been a driving force behind the development of terahertz technology, scientific equipment for terahertz research - including transmitters, receivers, and basic test and measurement equipment - is not widely available, making scientific experiments in this range between traditional electronics and quantum photonics more costly and greatly limiting commercial development in the field. Given NASA s interest in studying distant bodies in space as well as in improving life on Earth, the Agency has collaborated with private industry to develop terahertz technologies.

Source record↗

Cross-Cutting Metrology Tools for In Operando Characterization of Carrier Dynamics in Photovoltaic Devices (Final Technical Report)

Understanding the nature of recombination and its dependence on defects and interfaces is essential for engineering materials and contacts for higher V oc and photovoltaic (PV) efficiency. Time-resolved photoluminescence (TRPL) has conventionally been used to evaluate recombination, but not all materials are strongly emissive or otherwise suitable. Time-resolved terahertz spectroscopy is a pump – probe method that presents valuable complementary information, wherein an optical pump pulse photoexcites carriers within the absorber and the transient photoconductivity is probed with a terahertz pulse. Until now, experimental constraints have prohibited the use of terahertz probes to interrogate full device stacks, and measurements were instead made on exfoliated films or films grown on unconventional substrates. However, interfaces are critical to the behavior of photoexcited carriers in solar cells, and the substrates themselves often influence the film growth and bulk properties. Therefore, it is important to probe the behavior of PV absorbers as close as possible to their normal operating conditions. Here we have developed cross-cutting metrology that enable in operando characterization of carrier dynamics and recombination mechanisms in working PV devices. Through a combination of complementary non-contact TRTS and TRPL experiments and modeling, we have obtained key parameters including photoexcited carrier bulk lifetime and interface and back surface recombination velocities with greater precision and accuracy than can be achieved with conventional TRPL alone. By varying pulsed photoexcitation conditions, the contributions of interface and bulk recombination mechanisms can be determined. We have developed and refined this characterization approach by investigating CdTe PVs, which is a well-established technology but with significant margin for further improvements in efficiency. Results were published in Journal of Applied Physics (DOI: 10.1063/5.0064730) and Proceedings of the IEEE PVSC (DOI: 10.1109/PVSC43889.2021.9518559). After validating the approach, we have applied it to correlate recombination rates to processing conditions and material properties, including composition and defects as well as interfaces and surface treatments. Such feedback can inform processing and design choices to enable higher PV efficiency, not only for CdTe, but also CdSe x Te 1-x , CIGS, perovskites, kesterites, and future technologies. A perspective on predicting solar cell performance from terahertz spectroscopy was published in Advanced Energy Materials (DOI: 10.1002/aenm.202102776). The cross-cutting metrology tools developed here will enable determination of the locus and mechanism of performance-limiting recombination in thin film PV devices. This feedback can guide the engineering of PV devices with higher V oc and efficiency, thereby leading to reductions in levelized cost of electricity to meet the SunShot 2030 target of $0.03/kWh for utility-scale PV. Lower costs will enable rapid expansion of renewable electricity generation that is nearly free of carbon emissions. Reducing carbon emissions of the electricity sector is one of the most important solutions to climate change. The project’s specific focus on CdTe PV can benefit First Solar, the US company that is the global leader in CdTe technology, through both technology and workforce development.

14 SOLAR ENERGY↗

Fabrication of a Cryogenic Terahertz Emitter for Bolometer Focal Plane Calibrations

A fabrication process is reported for prototype emitters of THz radiation, which operate cryogenically, and should provide a fast, stable blackbody source suitable for characterization of THz devices. The fabrication has been demonstrated and, at the time of this reporting, testing was underway. The emitter is similar to a monolithic silicon bolometer in design, using both a low-noise thermometer and a heater element on a thermally isolated stage. An impedance-matched, high-emissivity coat ing is also integrated to tune the blackbody properties. This emitter is designed to emit a precise amount of power as a blackbody spectrum centered on terahertz frequencies. The emission is a function of the blackbody temperature. An integrated resistive heater and thermometer system can control the temperature of the blackbody with greater precision than previous incarnations of calibration sources that relied on blackbody emission. The emitter is fabricated using a silicon- on-insulator substrate wafer. The buried oxide is chosen to be less than 1 micron thick, and the silicon device thickness is 1-2 microns. Layers of phosphorus compensated with boron are implanted into and diffused throughout the full thickness of the silicon device layer to create the thermometer and heater components. Degenerately doped wiring is implanted to connect the devices to wire-bondable contact pads at the edge of the emitter chip. Then the device is micromachined to remove the thick-handle silicon behind the thermometer and heater components, and to thermally isolate it on a silicon membrane. An impedance- matched emissive coating (ion assisted evaporated Bi) is applied to the back of the membrane to enable high-efficiency emission of the blackbody spectrum.

Chervenak, James↗

Coherent frequency combs from electrons colliding with a laser pulse

Highly coherent and powerful light sources capable of generating soft x-ray frequency combs are essential for high precision measurements and rigorous tests of fundamental physics. In this work, we derive the analytical conditions required for the emission of coherent radiation from an electron beam colliding with a laser pulse, modeled as a plane wave. These conditions are applied in a series of numerical simulations, where we show that a soft x-ray frequency comb can be produced if the electrons are regularly-spaced and sufficiently monoenergetic. High quality beams of this kind may be produced in the near future from laser-plasma interactions or linear accelerators. Furthermore, we highlight the advantageous role of employing few-cycle laser pulses in relaxing the stringent monoenergeticity requirements for coherent emission. The conditions derived here can also be used to optimize coherent emission in other frequency ranges, such as the terahertz domain.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗