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The generation of monochromatic electromagnetic radiation in the terahertz (THz) frequency range has remained a challenging task for many decades. Here, the emission of monochromatic sub-THz radiation by optical phonons in the dielectric material KY(MoO 4 ) 2 is demonstrated. The layered crystal structure of KY(MoO 4 ) 2 causes infrared-active shear lattice vibrations to have energies below 3.7 meV, corresponding to frequencies lower than 900 GHz where solid-state-based monochromatic radiation sources are rare. Directly excited by a 5 ps long broadband THz pulse, infrared-active optical vibrations in KY(MoO 4 ) 2 re-emit narrowband sub-THz radiation as a time-varying dipole for tens of picoseconds, which is exceptionally long for oscillators with frequencies below 1 THz. Such a long coherent emission allows for the detection of more than 50 periods of radiation with frequencies of 568 and 860 GHz. The remarkably long decay time together with the chemical stability of the employed material suggests a variety of possible applications in THz technology., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Raman spectroscopy is among the top analytical techniques for ultra-low-dense organic matter, crucial to the search for life and analysis of celestial body surfaces in space exploration missions. Achieving the ultimate sensitivity of in-situ Raman spectroscopy necessitates a breakthrough in detecting inelastically scattered light. Single-photon detectors (SPDs) operating in photon counting mode, which can differentiate between Raman and luminescence responses, are promising candidates for the challenging scientific requirements. Since large SPD arrays are not yet commercially available, a dispersive element can be adapted to a single-pixel detector. By exploiting chromatic dispersion in optical fibers and picosecond-pulsed excitation, we delay the arrivals of different spectral components onto a single-pixel SPD. This method also separates weak Raman signals from stronger luminescence through correlated time-domain measurements. We study the impact of fiber properties and the excitation wavelength of a pulsed laser on the spectral resolution of the fiber-dispersive Raman spectrometer (FDRS). Additionally, we demonstrate the FDRS's potential for studying biomarkers and discuss its feasibility for analyzing inclusions in ice matrices., Competing Interests: Declaration of Conflicting InterestsThe authors declared no potential conflicts of interest with respect to the research, authorship, and/or publication of this article.

We present measurements of the coherence times of excited states of hydrogen-like arsenic impurities in germanium (Ge:As) using a table-top two-dimensional time-domain spectroscopy (2D-TDS) system. We show that this laboratory system is capable of resolving the coherence lifetimes of atomic-like excited levels of impurity centers in semiconductors, such as those used in solid-state quantum information technologies, on a subpicosecond time scale. By fitting the coherent nonlinear response of the system with the known intracenter transition frequencies, we are able to monitor coherent population transfer and decay of the transitions from the 2p 0 and 2p ± states for different low excitation pulse fields. Furthermore, by examining the off-diagonal resonances in the 2D frequency-domain map, we are able to identify coherences between excited electronic states that are not visible via conventional single-frequency pump-probe or Hahn-echo measurements., Competing Interests: The authors declare no competing financial interest., (© 2024 The Authors. Published by American Chemical Society.)

Atomic oxygen is a key species in the mesosphere and thermosphere of Venus. It peaks in the transition region between the two dominant atmospheric circulation patterns, the retrograde super-rotating zonal flow below 70 km and the subsolar to antisolar flow above 120 km altitude. However, past and current detection methods are indirect and based on measurements of other molecules in combination with photochemical models. Here, we show direct detection of atomic oxygen on the dayside as well as on the nightside of Venus by measuring its ground-state transition at 4.74 THz (63.2 µm). The atomic oxygen is concentrated at altitudes around 100 km with a maximum column density on the dayside where it is generated by photolysis of carbon dioxide and carbon monoxide. This method enables detailed investigations of the Venusian atmosphere in the region between the two atmospheric circulation patterns in support of future space missions to Venus., (© 2023. The Author(s).)

We demonstrate the frequency stabilization of a terahertz quantum-cascade laser (QCL) to the Lamb dip of the absorption line of a D 2 O rotational transition at 3.3809309 THz. To assess the quality of the frequency stabilization, a Schottky diode harmonic mixer is used to generate a downconverted QCL signal by mixing the laser emission with a multiplied microwave reference signal. This downconverted signal is directly measured by a spectrum analyzer showing a full width at half maximum of 350 kHz, which is eventually limited by high-frequency noise beyond the bandwidth of the stabilization loop.

The project Lunar Volatiles Mobile Instrumentation-Extended (LUVMI-X) developed an initial system design as well as payload and mobility breadboards for a small, lightweight rover dedicated for in situ exploration of the lunar south pole. One of the proposed payloads is the Volatiles Identification by Laser Analysis instrument (VOILA), which uses laser-induced breakdown spectroscopy (LIBS) to analyze the elemental composition of the lunar surface with an emphasis on sampling regolith and the detection of hydrogen for the inference of the presence of water. It is designed to analyze targets in front of the rover at variable focus between 300 mm and 500 mm. The spectrometer covers the wavelength range from 350 nm to 790 nm, which includes the hydrogen line at 656.3 nm as well as spectral lines of most major rock-forming elements. We report here the scientific input that fed into the concept and design of the VOILA instrument configuration for the LUVMI-X rover. Moreover, we present the measurements performed with the breadboard laboratory setup for VOILA at DLR Berlin that focused on verifying the performance of the designed LIBS instrument in particular for the detection and quantification of hydrogen and other major rock forming elements in the context of in situ lunar surface analysis.

The analysis of human breath is a very active area of research, driven by the vision of a fast, easy, and non-invasive tool for medical diagnoses at the point of care. Millimeter-wave gas spectroscopy (MMWGS) is a novel, well-suited technique for this application as it provides high sensitivity, specificity and selectivity. Most of all, it offers the perspective of compact low-cost systems to be used in doctors' offices or hospitals. In this work, we demonstrate the analysis of breath samples acquired in a medical environment using MMWGS and evaluate validity, reliability, as well as limitations and perspectives of the method. To this end, we investigated 28 duplicate samples from chronic obstructive lung disease patients and compared the results to gas chromatography-mass spectrometry (GC-MS). The quantification of the data was conducted using a calibration-free fit model, which describes the data precisely and delivers absolute quantities. For ethanol, acetone, and acetonitrile, the results agree well with the GC-MS measurements and are as reliable as GC-MS. The duplicate samples deviate from the mean values by only 6% to 18%. Detection limits of MMWGS depend strongly on the molecular species. For example, acetonitrile can be traced down to 1.8 × 10 -12 mol by the MMWGS system, which is comparable to the GC-MS system. We observed correlations of abundances between formaldehyde and acetaldehyde as well as between acetonitrile and acetaldehyde, which demonstrates the potential of MMWGS for breath research., (Creative Commons Attribution license.)

The two major challenges in Raman spectroscopy are the low intensity of spontaneous Raman scattering and often accompanying luminescence. We overcome these two issues with a novel fiber-dispersive Raman spectrometer utilizing pulsed excitation and a superconducting nanowire single-photon detector (SNSPD). By exploiting chromatic dispersion in the fiber material, we stretched propagation times of Raman photons and performed correlated measurements in the time domain, where the two emission processes, Raman scattering and luminescence, can be effectively separated. The spectrometer greatly benefits from SNSPD metrics, i.e. broad spectral sensitivity (from UV to near-IR wavelength range) on a single-photon level and high timing resolution (small timing jitter), which outperform those of competing avalanche single-photon detectors. The spectral resolution achievable with a fiber-dispersive spectrometer for the optimized components is estimated to be as good as 3 - 10 cm -1 over the Stokes shifted range up to 4400 cm -1 with an excitation wavelength of 785 nm and below 5 cm -1 covering the same range with an excitation wavelength of 532 nm.

We present an optically pumped terahertz gas laser, which is based on a mid-infrared quantum-cascade laser as a pump source, a transversely pumped standing wave resonator, and 15 NH 3 as a gain medium. We observe several laser lines around 4.5 THz, corresponding to rotational transitions in the ν 2 band of ammonia. So far, these are the highest frequencies obtained from a QCL-pumped THz gas laser. The involved molecular transitions are unambiguously identified by high-resolution spectroscopy.

We demonstrate a technique to simultaneously stabilize the frequency and output power of a terahertz quantum-cascade laser (QCL). This technique exploits frequency and power variations upon near-infrared illumination of the QCL with a diode laser. It does not require an external terahertz optical modulator. By locking the frequency to a molecular absorption line, we obtain a long-term (one-hour) linewidth of 260 kHz (full width at half maximum) and a root-mean-square power stability below 0.03%. With respect to the free-running case, this stabilization scheme improves the frequency stability by nearly two orders of magnitude and the power stability by a factor of three.

Breath gas analysis is a promising tool for medical research and diagnosis. A particularly powerful technological approach is millimeter-wave/terahertz (mmW/THz) spectroscopy, because it is a very sensitive and highly selective technique. In addition, it offers the potential for compact and affordable sensing systems for wide use. In this work, we demonstrate the capability of a mmW/THz spectrometer for breath analysis. Samples from three volunteers and a sample from ambient air were analyzed with respect to 31 different molecular species. High-resolution absorption spectra were measured by scanning two absorption lines from each species. Out of the 31, a total of 21 species were detected. The results demonstrate the potential of mmW/THz spectroscopy for breath analysis.

The development of diffractive lenses for the upper terahertz (THz) frequency range above 1 THz was successfully demonstrated by employing a direct laser ablation (DLA) technology. Two types of samples such as the Soret zone plate lens and the multi-level phase-correcting Fresnel lens were fabricated of a metal foil and crystalline silicon, respectively. The focusing performance along the optical axis of a 4.745 THz quantum cascade laser beam with respect to the positioning angle of the sample was studied by using a real-time microbolometric camera. A binary-phase profile sample demonstrated the values of the focusing gain and focused beam size up to 25 dB and 0.15 mm (2.4 λ ), respectively. The increase of the phase quantization level to eight led to higher (up to 29 dB) focusing gain values without a measurable increase of optical losses. All the samples were tolerant to misalignment as large as 10 deg of oblique incidence with a focusing power drop no larger than 10%. The results pave the way for new applications of industry-ready DLA technology in the entire THz range.

Near-infrared optical excitation enables wideband frequency tuning of terahertz quantum-cascade lasers. In this work, we demonstrate the feasibility of the approach for molecular laser absorption spectroscopy. We present a physical model which explains the observed frequency tuning characteristics by the optical excitation of an electron-hole plasma. Due to an improved excitation configuration as compared to previous work, we observe a single-mode continuous-wave frequency coverage of as much as 40 GHz for a laser at 3.1 THz. This represents, for the same device, a ten-fold improvement over the usually employed tuning by current. The method can be readily applied to a large class of devices.

BIOMEX (BIOlogy and Mars EXperiment) is an ESA/Roscosmos space exposure experiment housed within the exposure facility EXPOSE-R2 outside the Zvezda module on the International Space Station (ISS). The design of the multiuser facility supports-among others-the BIOMEX investigations into the stability and level of degradation of space-exposed biosignatures such as pigments, secondary metabolites, and cell surfaces in contact with a terrestrial and Mars analog mineral environment. In parallel, analysis on the viability of the investigated organisms has provided relevant data for evaluation of the habitability of Mars, for the limits of life, and for the likelihood of an interplanetary transfer of life (theory of lithopanspermia). In this project, lichens, archaea, bacteria, cyanobacteria, snow/permafrost algae, meristematic black fungi, and bryophytes from alpine and polar habitats were embedded, grown, and cultured on a mixture of martian and lunar regolith analogs or other terrestrial minerals. The organisms and regolith analogs and terrestrial mineral mixtures were then exposed to space and to simulated Mars-like conditions by way of the EXPOSE-R2 facility. In this special issue, we present the first set of data obtained in reference to our investigation into the habitability of Mars and limits of life. This project was initiated and implemented by the BIOMEX group, an international and interdisciplinary consortium of 30 institutes in 12 countries on 3 continents. Preflight tests for sample selection, results from ground-based simulation experiments, and the space experiments themselves are presented and include a complete overview of the scientific processes required for this space experiment and postflight analysis. The presented BIOMEX concept could be scaled up to future exposure experiments on the Moon and will serve as a pretest in low Earth orbit.

We present the results of the first systematic "round-robin" comparison of far-infrared transmittance spectra measurements, which was performed by five laboratories and piloted by Physikalisch-Technische (PTB). The transmittance spectra of four different samples were measured by the participating laboratories in the 600 cm -1 to 10 cm -1 range (16.67 µm to 1000 µm) in a blind comparison. Different types of instruments, Fourier transform infrared (FT-IR) spectrometers of Michelson type and a laser radiation-based system were used for the transmittance measurements. FT-IR spectrometers are the most popular and commonly used instruments for the spectral characterization of materials in the infrared spectral range, and are well established for quantitative measurements in the mid- and near-infrared spectral ranges. However, obtaining quantitative transmittance measurements in the far-infrared spectral range by means of these instruments is challenging, because it involves weaker radiation sources, stronger diffraction effects, significant radiation originating from the sample itself and temperature gradients inside the spectrometer that may not be given proper consideration. Therefore, this comparison was initiated to test the actual capability of and identify problems with FT-IR transmittance measurements in this spectral region. We discuss the results and the possible reasons for the observed discrepancies.

Terahertz (THz) radiation meaning electromagnetic radiation in the range from 0.1 (3) to 10 (30) has the unique advantage of easily penetrating many obstructions while being non-hazardous to organic tissue since it is non-ionizing. A shortcoming of this domain is the limited availability of high-sensitivity detector arrays respective THz cameras with >1k pixels. To overcome the imaging limitations of the THz domain, compressive imaging in combination with an optically controllable THz spatial light modulator is a promising approach especially when used in a single-pixel imaging modality. The imaging fidelity, performance and speed of this approach depend crucially on the imaging patterns also called masks and their properties used in the imaging process. Therefore, in this paper, it is investigated how the image quality after reconstruction is specifically influenced by the different mask types and their properties in a compressive imaging modality. The evaluation uses an liquid-crystal display based projector as spatial light modulator to derive specific guidelines for the use of binary and true greyscale masks in THz single-pixel imaging setups respective THz single-pixel cameras when used in far-field applications e.g. stand-off security imaging.

We report on the Doppler-free saturation spectroscopy of a molecular transition at 3.3 THz based on a quantum-cascade laser and an absorption cell in a collinear pump-probe configuration. A Lamb dip with a sub-Doppler linewidth of 170 kHz is observed for a rotational transition of HDO. We found that a certain level of external optical feedback is tolerable as long as the free spectral range of the external cavity is large compared to the width of the absorption line.

We report on real-time gas sensing with a terahertz quantum-cascade laser (QCL). The method is solely based on the modulation of the external cavity length, exploiting the intermediate optical feedback regime. While the QCL is operated in continuous-wave mode, optical feedback results in a change of the QCL frequency as well as its terminal voltage. The first effect is exploited to tune the lasing frequency across a molecular absorption line. The second effect is used for the detection of the self-mixing signal. This allows for fast measurement times on the order of 10 ms per spectrum and for real-time measurements of gas concentrations with a rate of 100 Hz. This technique is demonstrated with a mixture of D 2 O and CH 3 OD in an absorption cell.

We report on a high-spectral-resolution terahertz imaging system operating with a multi-mode quantum-cascade laser (QCL), a fast scanning mirror, and a sensitive Ge:Ga detector. By tuning the frequency of the QCL, several spectra can be recorded in 1.5 s during the scan through a gas cell filled with methanol (CH 3 OH). These experiments yield information about the local absorption and the linewidth. Measurements with a faster frame rate of up to 3 Hz allow for the dynamic observation of CH 3 OH gas leaking from a terahertz-transparent tube into the evacuated cell. In addition to the relative absorption, the local pressure is mapped by exploiting the effect of pressure broadening.

We describe a spectrometer consisting of a vector network analyzer, a gas absorption cell, and a quasi-optical bench that acquires terahertz spectra of gaseous substances and mixtures. We tested volatile organic compounds that are medical biomarkers or chemicals which can be found on the US Environment Protection Agency list of harmful substances. Absorption spectra at gas pressures between 10 Pa and 5000 Pa were recorded. A subsequent multivariate data analysis demonstrated excellent qualitative and quantitative identification of pure substances and complex mixtures. The applied multivariate algorithms are principal components analysis, partial least square regression and soft independent modelling of class analogy.

We report on a terahertz spectrometer for high-resolution molecular spectroscopy based on a quantum-cascade laser. High-frequency modulation (up to 50 MHz) of the laser driving current produces a simultaneous modulation of the frequency and amplitude of the laser output. The modulation generates sidebands, which are symmetrically positioned with respect to the laser carrier frequency. The molecular transition is probed by scanning the sidebands across it. In this way, the absorption and the dispersion caused by the molecular transition are measured. The signals are modeled by taking into account the simultaneous modulation of the frequency and amplitude of the laser emission. This allows for the determination of the strength of the frequency as well as amplitude modulation of the laser and of molecular parameters such as pressure broadening.

Laboratory spectroscopy of atomic hydrogen in a magnetic flux density of 10(5) T (1 gigagauss), the maximum observed on high-field magnetic white dwarfs, is impossible because practically available fields are about a thousand times less. In this regime, the cyclotron and binding energies become equal. Here we demonstrate Lyman series spectra for phosphorus impurities in silicon up to the equivalent field, which is scaled to 32.8 T by the effective mass and dielectric constant. The spectra reproduce the high-field theory for free hydrogen, with quadratic Zeeman splitting and strong mixing of spherical harmonics. They show the way for experiments on He and H(2) analogues, and for investigation of He(2), a bound molecule predicted under extreme field conditions.

We report on the development of a compact, easy-to-use terahertz radiation source, which combines a quantum-cascade laser (QCL) operating at 3.1 THz with a compact, low-input-power Stirling cooler. The QCL, which is based on a two-miniband design, has been developed for high output and low electrical pump power. The amount of generated heat complies with the nominal cooling capacity of the Stirling cooler of 7 W at 65 K with 240 W of electrical input power. Special care has been taken to achieve a good thermal coupling between the QCL and the cold finger of the cooler. The whole system weighs less than 15 kg including the cooler and power supplies. The maximum output power is 8 mW at 3.1 THz. With an appropriate optical beam shaping, the emission profile of the laser is fundamental Gaussian. The applicability of the system is demonstrated by imaging and molecular-spectroscopy experiments., ((c) 2010 Optical Society of America.)

Transitions between the spin-rotational levels of the (14)NH(+) radical in the v = 0 levels of its X (2)Pi and a (4)Sigma(-) states have been studied by the technique of laser magnetic resonance at far-infrared wavelengths. The data have been combined with a previous zero-field measurement of the J = 1 1/2 - 1/2 transition frequencies at 1.01 THz to determine a much improved set of molecular parameters for NH(+) in the X (2)Pi state; the major parameters for the a (4)Sigma(-) state have also been determined. A full determination of the hyperfine parameters for both (14)N and (1)H nuclei has been achieved for the first time. Accurate predictions of the transition frequencies between the low-lying levels of the radical in the absence of a magnetic field have also been made, including lambda-doubling frequencies for use by radio astronomers.

Both AuGe based alloys and Ti/Au metal layer stacks are widely used as ohmic metal contacts for photoconductive THz antennas made of low temperature grown GaAs. Here, we present the first systematic comparison between these two metallization types. A series of antennas of both kinds is excited by femtosecond laser pulses and by the emission from two diode lasers, i.e. we test the structures as pulsed THz emitters and as photomixers. In both cases, coherent and incoherent detection schemes are employed. We find that the power emitted from the antennas with AuGe metallization is 50% higher than that of antennas with a Ti/Au metal layer. From a comparison with a photomixer model we conclude that the higher output power results from a lower contact resistance of the AuGe contacts leading to an increased current flow. However, Ti/Au contacts have a higher thermal stability which might be advantageous if high system stability is called for.

Stimulated Stokes emission has been observed from silicon crystals doped by antimony donors when optically excited by radiation from a tunable infrared free electron laser. The photon energy of the emission is equal to the pump photon energy reduced by the energy of the intervalley transverse acoustic (TA) g phonon in silicon (approximately 2.92 THz). The emission frequency covers the range of 4.6-5.8 THz. The laser process occurs due to a resonant coupling of the 1s(E) and 1s(A1) donor states (separation approximately 2.97 THz) via the g-TA phonon, which conserves momentum and energy within a single impurity center.

Terahertz quantum cascade lasers have been investigated with respect to their performance as a local oscillator in a heterodyne receiver. The beam profile has been measured and transformed in to a close to Gaussian profile resulting in a good matching between the field patterns of the quantum cascade laser and the antenna of a superconducting hot electron bolometric mixer. Noise temperature measurements with the hot electron bolometer and a 2.5 THz quantum cascade laser yielded the same result as with a gas laser as local oscillator.

We present a model describing high power stable broadband coherent synchrotron radiation (CSR) in the terahertz frequency region in an electron storage ring. The model includes distortion of bunch shape from the synchrotron radiation (SR), which enhances higher frequency coherent emission, and limits to stable emission due to an instability excited by the SR wakefield. It gives a quantitative explanation of several features of the recent observations of CSR at the BESSY II storage ring. We also use this model to optimize the performance of a source for stable CSR emission.

A new technology for generating steady state, brilliant, broadband, coherent, far-infrared (FIR) radiation in electron storage rings is presented, suitable for FIR spectroscopy. An FIR power increase of up to 100 000 compared to the normal, incoherent synchrotron radiation in the range of approximately 5 to approximately 40 cm(-1) could be achieved. The source is up to 1000 times more brillant compared to a standard Hg arc lamp. The coherent synchrotron radiation is produced in a "low alpha" optics mode of the synchrotron light source BESSY, by bunch shortening and non-Gaussian bunch deformation.

At BESSY II it is demonstrated that far-infrared coherent synchrotron radiation (CSR) can be generated by a controlled, steady-state process at storage rings. As an indication for coherent emission, the radiated power grows with the square of the beam current. The spectrum was analyzed by an interferometer in the 1-mm to 0.3-mm wavelength range. The CSR was enhanced more than 3000 times above background; the incoherent radiation remained below the background level. Steady-state and bursting CSR were discriminated by time resolved analysis from micro seconds to seconds.