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At least 127 records · Page 7

Terahertz Dirac Hyperbolic Metamaterial

Hyperbolic metamaterials (HMMs) are engineered materials with a hyperbolic isofrequency surface, enabling a range of interesting phenomena and applications including negative refraction, enhanced sensing, and subdiffraction imaging, focusing, and waveguiding. Existing HMMs primarily work in the visible and infrared spectral range due to the inherent properties of their constituent materials. Here, we demonstrate a THz-range Dirac HMM using topological insulators as the building blocks. Here, we find that the structure houses up to three high-wavevector volume plasmon polariton (VPP) modes, consistent with transfer matrix modeling and effective medium theory calculations. The VPPs have mode indices greater than 100, significantly larger than observed for VPP modes in HMMs made from metals or doped semiconductors while maintaining comparable quality factors. We attribute these properties to the two-dimensional Dirac nature of the electrons occupying the topological insulator surface states. Because these are van der Waals materials, these structures can be grown at a wafer-scale on a variety of substrates, allowing them to be integrated with existing THz structures and enabling next-generation THz optical devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stimulated Rayleigh Scattering Enhanced by a Longitudinal Plasma Mode in a Periodically Driven Dirac Semimetal Cd 3 As 2

Using broadband (12–45 THz) multi-terahertz spectroscopy, we show that stimulated Rayleigh scattering dominates the transient optical conductivity of cadmium arsenide, a Dirac semimetal, under an optical driving field at 30 THz. Here, the characteristic dispersive line shape with net optical gain is accounted for by optical transitions between light-induced Floquet subbands, strikingly enhanced by the longitudinal plasma mode. Stimulated Rayleigh scattering with an unprecedentedly large refractive index change may pave the way for slow light generation in conductive solids at room temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Wavelength conversion through plasmon-coupled surface states

Surface states generally degrade semiconductor device performance by raising the charge injection barrier height, introducing localized trap states, inducing surface leakage current, and altering the electric potential. We show that the giant built-in electric field created by the surface states can be harnessed to enable passive wavelength conversion without utilizing any nonlinear optical phenomena. Photo-excited surface plasmons are coupled to the surface states to generate an electron gas, which is routed to a nanoantenna array through the giant electric field created by the surface states. The induced current on the nanoantennas, which contains mixing product of different optical frequency components, generates radiation at the beat frequencies of the incident photons. We utilize the functionalities of plasmon-coupled surface states to demonstrate passive wavelength conversion of nanojoule optical pulses at a 1550 nm center wavelength to terahertz regime with efficiencies that exceed nonlinear optical methods by 4-orders of magnitude.

42 ENGINEERING↗

Design Considerations for Compact High-Average Power Free-Electron Lasers/Masers at Terahertz Frequencies

Interest is increasing in high-power terahertz (THz) sources of radiation. The terminology is fluid, but researchers in the field typically refer to frequencies ranging from about 300 GHz to 10 THz as THz radiation. In this article, we present a description of design considerations for a compact, high-average power free-electron laser. At present, THz radiation is generated by a variety of mechanisms, including laser-based sources and electron-beam-based sources. Here, we provide a short description of current THz source technology to give background against which to compare the present concept; however, this should not be considered a comprehensive discussion of such technologies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Monolithic Kerr and electro-optic hybrid microcombs

Microresonator-based soliton generation promises chip-scale integration of optical frequency combs for applications spanning from time keeping to frequency synthesis. Access to the soliton repetition rate is a prerequisite for those applications. While miniaturized cavities harness Kerr nonlinearity and enable terahertz soliton repetition rates, such high rates are not amenable to direct electronic detection. Here, we demonstrate hybrid Kerr and electro-optic microcombs using a lithium niobate thin film that exhibits both Kerr and Pockels nonlinearities. By interleaving the high-repetition-rate Kerr soliton comb with the low-repetition-rate electro-optic comb on the same waveguide, wide Kerr soliton mode spacing is divided within a single chip, allowing for direct electronic detection and feedback control of the soliton repetition rate. Our work establishes an integrated approach to electronically access terahertz solitons, paving the way for building chip-scale referenced comb sources.

42 ENGINEERING↗

Nanotechnology for catalysis and solar energy conversion

This roadmap on Nanotechnology for Catalysis and Solar Energy Conversion focuses on the application of nanotechnology in addressing the current challenges of energy conversion: 'high efficiency, stability, safety, and the potential for low-cost/scalable manufacturing' to quote from the contributed article by Nathan Lewis. This roadmap focuses on solar-to-fuel conversion, solar water splitting, solar photovoltaics and bio-catalysis. It includes dye-sensitized solar cells (DSSCs), perovskite solar cells, and organic photovoltaics. Smart engineering of colloidal quantum materials and nanostructured electrodes will improve solar-to-fuel conversion efficiency, as described in the articles by Waiskopf and Banin and Meyer. Semiconductor nanoparticles will also improve solar energy conversion efficiency, as discussed by Boschloo et al in their article on DSSCs. Perovskite solar cells have advanced rapidly in recent years, including new ideas on 2D and 3D hybrid halide perovskites, as described by Spanopoulos et al 'Next generation' solar cells using multiple exciton generation (MEG) from hot carriers, described in the article by Nozik and Beard, could lead to remarkable improvement in photovoltaic efficiency by using quantization effects in semiconductor nanostructures (quantum dots, wires or wells). These challenges will not be met without simultaneous improvement in nanoscale characterization methods. Terahertz spectroscopy, discussed in the article by Milot et al is one example of a method that is overcoming the difficulties associated with nanoscale materials characterization by avoiding electrical contacts to nanoparticles, allowing characterization during device operation, and enabling characterization of a single nanoparticle. Besides experimental advances, computational science is also meeting the challenges of nanomaterials synthesis. The article by Kohlstedt and Schatz discusses the computational frameworks being used to predict structure–property relationships in materials and devices, including machine learning methods, with an emphasis on organic photovoltaics. The contribution by Megarity and Armstrong presents the 'electrochemical leaf' for improvements in electrochemistry and beyond. In addition, biohybrid approaches can take advantage of efficient and specific enzyme catalysts. These articles present the nanoscience and technology at the forefront of renewable energy development that will have significant benefits to society.

14 SOLAR ENERGY↗

Modeling of Optoelectronic Devices

Ultrafast modulation of semiconductor quantum well (QW) laser is of technological importance for information technology. Improvement by order(s) of magnitude in data transfer rate is possible as terahertz (THz) radiation is available for heating the laser at picosecond time scale. Optical gain modulation in the QW is achieved via temperature modulation of electron-hole plasma (EHP). Applications include free-space THz communication, optical switching, and pulse generation. The EHP in the semiconductor QW is described with a two-band model. Semiconductor Bloch equations with many-body effects are used to derive a hydrodynamical model for the active QW region. Because of ultrafast carrier-carrier scatterings in the order of 50 fs, EHP follows quasiequilibrium Fermi-Dirac distributions and THz field interacts incoherently with it. Carrier-longitudinal optical (LO) phonon scatterings and coherent laser-EHP interaction are treated microscopically in our physical model. A set of hydrodynamical equations for plasma density, temperature, and laser envelop amplitude are derived and Runge-Kutta method is adopted for numerical simulation. A typical 8 nm GaAs/Al(0.3)Ga(0.7) As single QW at 300 K is used. Additional information is contained in the original extended abstract.

Li, Jian-Zhong↗

On-Chip Power-Combining for High-Power Schottky Diode Based Frequency Multipliers

A novel MMIC on-chip power-combined frequency multiplier device and a method of fabricating the same, comprising two or more multiplying structures integrated on a single chip, wherein each of the integrated multiplying structures are electrically identical and each of the multiplying structures include one input antenna (E-probe) for receiving an input signal in the millimeter-wave, submillimeter-wave or terahertz frequency range inputted on the chip, a stripline based input matching network electrically connecting the input antennas to two or more Schottky diodes in a balanced configuration, two or more Schottky diodes that are used as nonlinear semiconductor devices to generate harmonics out of the input signal and produce the multiplied output signal, stripline based output matching networks for transmitting the output signal from the Schottky diodes to an output antenna, and an output antenna (E-probe) for transmitting the output signal off the chip into the output waveguide transmission line.

Siles Perez, Jose Vicente↗

Analytical WKB theory for high-harmonic generation and its application to massive Dirac electrons

Here we propose an analytical approach to high-harmonic generation (HHG) for nonperturbative low-frequency and high-intensity fields based on the (Jeffreys-)Wentzel-Kramers-Brillouin (WKB) approximation. By properly taking into account Stokes phenomena of WKB solutions, we obtain wave functions that systematically include the repetitive dynamics of production and acceleration of electron-hole pairs and quantum interference due to phase accumulation between different pair production times (Stückelberg phase). Using the obtained wave functions without relying on any phenomenological assumptions, we explicitly compute electric current (including intra- and interband contributions) as the source of HHG for a massive Dirac system in (1+1) dimensions under an ac electric field. We demonstrate that the WKB approximation agrees well with numerical results obtained by solving the time-dependent Schrödinger equation and point out that the quantum interference is important in HHG. We also predict in the deep nonperturbative regime that (1) harmonic intensities oscillate with respect to electric-field amplitude E 0 and frequency Ω with a period determined by the Stückelberg phase, (2) the cutoff order of HHG is determined by 2eE 0 ℏΩ 2 , with e being the electron charge, and that (3) noninteger harmonics, controlled by the Stückelberg phase, appear as a transient effect. Our WKB theory is particularly suited for a parameter regime, where the Keldysh parameter γ = (Δ/2)Ω/eE 0 ,with Δ being the gap size, is small. This parameter regime corresponds to intense lasers in the terahertz regime for realistic massive Dirac materials. Our analysis implies that the so-called HHG plateau can be observed at the terahertz frequency within the current technology.

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↗

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↗

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↗

Dynamic magneto-chiral instability in photoexcited tellurium

In systems of charged chiral fermions out of equilibrium, an electric current parallel to a magnetic field can generate a dynamic instability that amplifies electromagnetic waves. Whether this mechanism also operates in chiral solid-state systems has remained uncertain. Here we observe signatures of a dynamic magneto-chiral instability in elemental tellurium, a structurally chiral crystal, using time-domain terahertz emission spectroscopy. Under transient photoexcitation in a moderate magnetic field, we observe terahertz radiation with coherent modes that grow in amplitude over time. We present a theoretical model that describes this behaviour based on a dynamic instability of electromagnetic waves interacting with infrared-active oscillators of acceptor states in tellurium, giving rise to an amplifying polariton. These results demonstrate that magneto-chiral instabilities can emerge in solid-state systems and establish a mechanism for terahertz-wave amplification in chiral materials.

42 ENGINEERING↗

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↗

Star & Planet Formation Studies and Opportunities with SOFIA

Star formation, the most fundamental process in the universe, is linked to planet formation and thus to the origin and evolution of life. We have a general outline of how planets and stars form, yet unraveling the details of the physics and chemistry continues to challenge us. The infrared and submillimeter part of the spectrum hold the most promise for studying the beginnings of star formation. The observational landscape recently shaped by Spitzer, Herschel and ALMA, continues to challenge our current theories. SOFIA, the Stratospheric Observatory for Infrared Astronomy, equipped with state-of-the-art infrared instrumentation to a vantage point at 45,000 feet (13.7 kilometers) flight altitude that is above 99.9 percent of the Earth's water vapor, enables observations in the infrared through terahertz frequencies not possible from the ground. SOFIA is a community observatory, about to start its sixth annual observing cycle. My talk will focus on recent results in advancing star and planet formation processes using SOFIAʼs imaging and polarimetric capabilities, and the upcoming science enabled by the 3rd generation instrument High-Resolution Mid-Infrared Spectrometer (HIRMES) to be commissioned in 2019. I will show how mid-infrared imaging is used to test massive star formation theories, how far-infrared polarimetry on sub-parsec scales is directly testing the role of magnetic fields in molecular clouds, and how velocity-resolved high-resolution spectroscopy will push forward our understanding of proto-planetary disk science. I will also summarize upcoming opportunities with the SOFIA observatory. For the latest news about your flying observatory, see https://sofia.usra.edu/.

Star formation↗

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↗

DC electrical conductivity measurements of warm dense matter using ultrafast THz radiation

We describe measurements of the DC electrical conductivity of warm dense matter using ultrafast terahertz (THz) pulses. THz fields are sufficiently slowly varying that they behave like DC fields on the timescale of electron–electron and electron–ion interactions and hence probe DC-like responses. Using a novel single-shot electro-optic sampling technique, the electrical conductivity of the laser-generated warm dense matter was determined with <1 ps temporal resolution. We present the details of the single-shot THz detection methodology as well as considerations for warm dense matter experiments. We, then, provide proof-of-concept studies on aluminum driven to the warm dense matter regime through isochoric heating and shock compression. Our results indicate a decrease in the conductivity when driven to warm dense matter conditions and provide a platform for future warm dense matter studies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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↗