Terahertz Spectroscopy Unambiguously Determines the Orientation of Guest Water Molecules in a Structurally Elusive Metal-Organic Framework.

Porous materials, particularly metal-organic frameworks (MOFs), hold great promise for advanced applications. MIL-53(Al) is an exceptionally well-studied MOF that exhibits a phase transition upon guest capture─in this case, water─resulting in a dramatic change in the pore volume. Despite extensive studies, the structure of the water-loaded narrow-pore phase, MIL-53(Al)-np, remains controversial, particularly with respect to the positions of the adsorbed water molecules. We use terahertz spectroscopy, coupled with powder X-ray diffraction and density functional theory simulations, to unambiguously resolve this controversy. We show that the low-frequency (<100 cm-1) vibrational spectrum depends on weak long-range forces that are extremely sensitive to the orientation of the adsorbed water molecules. This enables definitively determining the correct structure of MIL-53(Al)-np while highlighting the extreme sensitivity of terahertz spectroscopy to bulk structure, suggesting its potential as a robust complement to X-ray diffraction for precise characterization of host-guest complexes.

Propagation of THz radiation in air over a broad range of atmospheric temperature and humidity conditions.

As the need for higher data rates for communication increases, the terahertz (THz) band has drawn considerable attention. This spectral region promises a much wider bandwidth and the transmission of large amounts of data at high speeds. However, there are still challenges that need to be addressed before the THz telecommunications technology hits the consumer market. One of the recurring concerns is that THz radiation is greatly absorbed by atmospheric water-vapor. Although many studies have presented the attenuation of THz signals under different atmospheric conditions, these results analyze specific temperature or humidity values, leaving the need for a more comprehensive analysis over a wider range of climate conditions. In this work, we present the first study of the attenuation of THz radiation over a broad range of temperatures and humidity values. It is worth noticing that all of our measurements have been undertaken at atmospheric pressure unlike many previous studies where the pressure was not kept constant for various temperatures. Furthermore, we extend our analysis beyond the impact of absolute humidity on the bit error rate in THz communications. We also discuss the refractivity of the atmosphere, examining its variations across different temperatures and humidity levels. THz propagation is studied using two different measurement systems, a long-path THz time-domain spectrometer as well as a quasi-optic setup with vector network analyze. We also compare the results with the ITU-R P.676-13 propagation model. We conclude that the attenuation at the absorption peaks increases linearly with water content and has no dependence on the temperature, while the refractive index, away from absorption lines, namely at 300 GHz shows a sub-linear increase with humidity.

Real-time programmable metasurface for terahertz multifunctional wave front engineering.

Terahertz (THz) technologies have become a focus of research in recent years due to their prominent role in envisioned future communication and sensing systems. One of the key challenges facing the field is the need for tools to enable agile engineering of THz wave fronts. Here, we describe a reconfigurable metasurface based on GaN technology with an array-of-subarrays architecture. This subwavelength-spaced array, under the control of a 1-bit digital coding sequence, can switch between an enormous range of possible configurations, providing facile access to nearly arbitrary wave front control for signals near 0.34 THz. We demonstrate wide-angle beam scanning with 1° of angular precision over 70 GHz of bandwidth, as well as the generation of multi-beam and diffuse wave fronts, with a switching speed up to 100 MHz. This device, offering the ability to rapidly reconfigure a propagating wave front for beam-forming or diffusively scattered wide-angle coverage of a scene, will open new realms of possibilities in sensing, imaging, and networking.

Near-field terahertz nonlinear optics with blue light.

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.

Wireless communications sensing and security above 100 GHz.

The field of sub-terahertz wireless communications is advancing rapidly, with major research efforts ramping up around the globe. To address some of the significant hurdles associated with exploiting these high frequencies for broadband and secure networking, systems will require extensive new capabilities for sensing their environment and manipulating their broadcasts. Based on these requirements, a vision for future wireless systems is beginning to emerge. In this Perspective article, we discuss some of the prominent challenges and possible solutions which are at the forefront of current research, and which will contribute to the architecture of wireless platforms beyond 5G.

Jamming a terahertz wireless link.

As the demand for bandwidth in wireless communication increases, carrier frequencies will reach the terahertz (THz) regime. One of the common preconceived notions is that, at these high frequencies, signals can radiate with high directivity which inherently provides more secure channels. Here, we describe the first study of the vulnerability of these directional links to jamming, in which we identify several features that are distinct from the usual considerations of jamming at low frequencies. We show that the receiver's use of an envelope detector provides the jammer with the ability to thwart active attempts to adapt to their attack. In addition, a jammer can exploit the broadband nature of typical receivers to implement a beat jamming attack, which allows them to optimize the efficacy of the interference even if their broadcast is detuned from the frequency of the intended link. Our work quantifies the increasing susceptibility of broadband receivers to jamming, revealing previously unidentified vulnerabilities which must be considered in the development of future wireless systems operating above 100 GHz.

The effect of angular dispersion on THz data transmission.

One of the key distinctions between legacy low-frequency wireless systems and future THz wireless transmissions is that THz links will require high directionality, to overcome the large free-space path loss. Because of this directionality, optical phenomena become increasingly important as design considerations. A key example lies in the strong dependence of angular radiation patterns on the transmission frequency, which is manifested in many different situations including common diffraction patterns and the emission from leaky-wave apertures. As a result of this effect, the spectral bandwidth at a receiver is nonlinearly dependent on the receiver's angular position and distance from the transmitter. In this work, we explore the implications of this type of effect by incorporating either a diffraction grating or a leaky wave antenna into a communication link. These general considerations will have significant implications for the robustness of data transmissions at high frequencies.

Bar code reader for the THz region.

We demonstrate a bar code sensing system for the THz region using leaky parallel plate waveguide and an off-axis parabolic mirror. The bars of the bar code are made from metal with air as gaps between them. We use up to 6 bars in the barcode system which can store up to 64 bits. Because the system employs coherent detection, we can further increase the bit density by adding Teflon strips to the barcode, encoding information in both amplitude and phase delay. These bar codes can be manufactured easily and inexpensively, offering a versatile alternative to RFID tags.

High-volume rapid prototyping technique for terahertz metallic metasurfaces.

Terahertz technology has greatly benefited from the recent development and generalization of prototyping technologies such as 3D printing and laser machining. These techniques can be used to rapidly fabricate optical devices for applications in sensing, imaging and communications. In this paper, we introduce hot stamping, a simple inexpensive and rapid technique to form 2D metallic patterns that are suitable for many terahertz devices. We fabricate several example devices to illustrate the versatility of the technique, including metasurfaces made of arrays of split-ring resonators with resonances up to 550 GHz. We also fabricate a wire-grid polarizer for use as a polarizing beam splitter. The simplicity and low cost of this technique can help in rapid prototyping and realization of future terahertz devices.

Anomalous contrast in broadband THz near-field imaging of gold microstructures.

THz scattering-type scanning near-field microscopy (s-SNOM) has become a powerful technique for measuring carrier dynamics in nanoscale materials and structures. Changes in a material's local THz reflection or transmission can be correlated to changes in electrical conductivity. Here, we perform tip-based THz nano-imaging of subwavelength gold nanostructures and demonstrate image contrast unrelated to any spatially varying material properties. We show that the specific physical configuration of the gold structures can have a strong influence on local excitations which can obscure the sample's true dielectric response, even in cases where the relevant structures are far outside of the spatial region probed by the AFM tip.

Broadband wide-angle terahertz antenna based on the application of transformation optics to a Luneburg lens.

The design of antennas for terahertz systems remains a significant challenge. These antennas must provide very high gain to overcome significant free-space path loss, which limits their ability to broadcast or receive a beam over a wide angular range. To circumvent this limitation, here we describe a new device concept, based on the application of quasi-conformal transformation optics to the traditional Luneburg lens. This device offers the possibility for wide-angle beam steering and beam reception over a broad bandwidth, scalable to any frequency band in the THz range.

Terahertz smart dynamic and active functional electromagnetic metasurfaces and their applications.

The demand for smart and multi-functional applications in the terahertz (THz) frequency band, such as for communication, imaging, spectroscopy, sensing and THz integrated circuits, motivates the development of novel active, controllable and informational devices for manipulating and controlling THz waves. Metasurfaces are planar artificial structures composed of thousands of unit cells or metallic structures, whose size is either comparable to or smaller than the wavelength of the illuminated wave, which can efficiently interact with the THz wave and exhibit additional degrees of freedom to modulate the THz wave. In the past decades, active metasurfaces have been developed by combining diode arrays, two-dimensional active materials, two-dimensional electron gases, phase transition material films and other such elements, which can overcome the limitations of conventional bulk materials and structures for applications in compact THz multi-functional antennas, diffractive devices, high-speed data transmission and high-resolution imaging. In this paper, we provide a brief overview of the development of dynamic and active functional electromagnetic metasurfaces and their applications in the THz band in recent years. Different kinds of active metasurfaces are cited and introduced. We believe that, in the future, active metasurfaces will be combined with digitalization and coding to yield more intelligent metasurfaces, which can be used to realize smart THz wave beam scanning, automatic target recognition imaging, self-adaptive directional high-speed data transmission network, biological intelligent detection and other such applications. This article is part of the theme issue 'Advanced electromagnetic non-destructive evaluation and smart monitoring'.

Analysis of ancient ceramics using terahertz imaging and photogrammetry.

Imaging using terahertz time-domain spectroscopy is a valuable diagnostic tool for material inspection. However, in the case of samples with inhomogeneous shape and composition, the reliable extraction of spatially varying dielectric properties can be very challenging. Here, we demonstrate a new approach which combines THz-TDS with photogrammetric reconstruction. We show that this technique can be used to estimate the local refractive index of samples with a complex geometry. We employ this method to study samples of ancient pottery, and demonstrate that THz techniques can provide a valuable new tool for this branch of archaeological science.

Laser THz emission nanoscopy and THz nanoscopy.

We present an experimental and theoretical comparison of two different scattering-type scanning near-field optical microscopy (s-SNOM) based techniques in the terahertz regime; nanoscale reflection-type terahertz time-domain spectroscopy (THz nanoscopy) and nanoscale laser terahertz emission microscopy, or laser terahertz emission nanoscopy (LTEN). We show that complementary information regarding a material's charge carriers can be gained from these techniques when employed back-to-back. For the specific case of THz nanoscopy and LTEN imaging performed on a lightly p-doped InAs sample, we were able to record waveforms with detector signal components demodulated up to the 6th and the 10th harmonic of the tip oscillation frequency, and measure a THz near-field confinement down to 11 nm. A computational approach for determining the spatial confinement of the enhanced electric field in the near-field region of the conductive probe is presented, which manifests an effective "tip sharpening" in the case of nanoscale LTEN due to the alternative geometry and optical nonlinearity of the THz generation mechanism. Finally, we demonstrate the utility of the finite dipole model (FDM) in predicting the broadband scattered THz electric field, and present the first use of this model for predicting a near-field response from LTEN.

Real-time object tracking using a leaky THz waveguide.

We demonstrate a 2D radar system for the THz region using a leaky parallel-plate waveguide, which can support real-time object tracking. The system can track a target within 200 ms with an accuracy of 1 mm in range and 1.4° in angle. Because the system is based on broadband excitation, it can locate multiple objects simultaneously. The broadband excitation also enables sensing of objects for which there is no direct line-of-sight path to the waveguide, via detection of a non-line-of-sight path.

Single-shot link discovery for terahertz wireless networks.

Of the many challenges in building a wireless network at terahertz frequencies, link discovery remains one of the most critical and least explored. In a network of mobile receivers using narrow directional beams, how do the nodes rapidly locate each other? This direction information is crucial for beam forming and steering, which are fundamental operations for maintaining link quality. As the carrier frequency increases into the terahertz range, the conventional methods used by existing networks become prohibitively time-consuming, so an alternative strategy is required. Using a leaky-wave antenna with a broadband transmitter, we demonstrate a single-shot approach for link discovery which can be accomplished much more rapidly. Our method relies on measurements of the width of a broad spectrum, and does not require any information about the phase of the received signal. This protocol, which relies on a detailed understanding of the radiation from leaky-wave devices, offers a realistic approach for enabling mobility in directional networks.

Broadband amplitude, frequency, and polarization splitter for terahertz frequencies using parallel-plate waveguide technology.

In this Letter, we report a broadband frequency/polarization demultiplexer based on parallel-plate waveguides (PPWGs) for terahertz (THz) frequencies. The fabrication and experimental validation of this polarization sensitive demultiplexer is demonstrated for the range from 0.2 to 1 THz. Upgrading the demultiplexer by adding a second demultiplexer stage, a fifty-fifty amplitude splitter is also demonstrated in the same frequency range. The multiplexer is based on a stainless-steel traveling-wave antenna, exhibiting strong mechanical robustness. This unique device exhibits three splitting mechanisms in the same device: amplitude, polarization, and frequency splitting. This is a significant improvement for the next generation of THz passive components for communication purposes.

Experimental measurement of the wake field in a plasma filament created by a single-color ultrafast laser pulse.

A laser plasma wake field in a single-color femtosecond laser filament determines the acceleration of ionized electrons, which affects the intensity and bandwidth of the emitted terahertz wave and is important for understanding the fundamental nonlinear process of THz generation. Since the THz wave generated by a laser wake field is extremely small and easily hidden by other THz generation mechanisms, no method exists to measure this wake field directly. In this paper, a simple and stable method for determining the amplitude of the laser plasma wake field is presented. Based on the cancellation of a positive laser plasma wake field and an external negative electric field, the "zero point" of the intensity of the generated THz wave at some frequency can be used to determine the exact amplitude of the corresponding laser plasma wake field. This finding opens an avenue toward the clarification of ultrafast electronic dynamic processes in laser-induced plasmas.

Characteristics of resonance-induced optical vortices and spatial reshaping.

The spatial profile of a beam can experience complicated reshaping after interacting with a planar resonator near resonant conditions. Previously, this phenomenon was recognized as the Goos-Hänchen effect, which only partially explains the experimental observations. In this Letter, we introduce a 2D model that can fully describe the resonance-induced spatial reshaping. The model predicts several general features of the output beam profile and suggests that optical phase or polarization vortices can be generated and manipulated by an arbitrary planar resonator. We validate our theoretical results with experimental measurements using terahertz spectroscopy.

Generation of spatiotemporally tailored terahertz wavepackets by nonlinear metasurfaces.

The past two decades have witnessed an ever-growing number of emerging applications that utilize terahertz (THz) waves, ranging from advanced biomedical imaging, through novel security applications, fast wireless communications, and new abilities to study and control matter in all of its phases. The development and deployment of these emerging technologies is however held back, due to a substantial lack of simple methods for efficient generation, detection and manipulation of THz waves. Recently it was shown that uniform nonlinear metasurfaces can efficiently generate broadband single-cycle THz pulses. Here we show that judicious engineering of the single-emitters that comprise the metasurface, enables to obtain unprecedented control of the spatiotemporal properties of the emitted THz wavepackets. We specifically demonstrate generation of propagating spatiotemporal quadrupole and few-cycles THz pulses with engineered angular dispersion. Our results place nonlinear metasurfaces as a new promising tool for generating application-tailored THz fields with controlled spatial and temporal characteristics.