Anomalous Temperature Effect in Weakly Coupled Superlattices: Carrier Transport in a THz Quantum Cascade Laser.

We present an investigation into the vertical transport through 13 different superlattice structures, where the well and barrier widths, doping concentration, dopant position, and contact layers were varied. Although superlattices have been extensively studied since 1970, there is a lack of publications on transport through superlattices similarly low doped as THz quantum cascade lasers (QCLs), for which the doping is in the 3-5×10^{10} cm^{-2} range. The superlattices presented are doped in the same range as THz QCLs, with contact layers and fabrication comparable to high-temperature THz QCLs. The temperature-dependent current-voltage characteristics were measured starting from 5 K and an anomalous temperature effect was observed at the first plateau. The measured current through the superlattice first decreases before increasing again with increasing temperature, resulting in the lowest current occurring at 75-110 K. This behavior is also observed in some THz QCLs. The effect disappears for thinner barriers, higher quantum well doping, or modified contact layers, indicating a strong dependency on band bending, due to the large difference in the doping of the contact layers and the superlattice, which is confirmed with multiscattering Büttiker simulations.

Deep learning control of THz QCLs.

Artificial neural networks are capable of fitting highly non-linear and complex systems. Such complicated systems can be found everywhere in nature, including the non-linear interaction between optical modes in laser resonators. In this work, we demonstrate artificial neural networks trained to model these complex interactions in the cavity of a Quantum Cascade Random Laser. The neural networks are able to predict modulation schemes for desired laser spectra in real-time. This radically novel approach makes it possible to adapt spectra to individual requirements without the need for lengthy and costly simulation and fabrication iterations.

Thermoelectric-cooled terahertz quantum cascade lasers.

We demonstrate the first lasing emission of a thermo-electrically cooled terahertz quantum cascade laser (THz QCL). A high temperature three-well THz QCL emitting at 3.8 THz is mounted to a novel five-stage thermoelectric cooler reaching a temperature difference of ΔT = 124 K. The temperature and time-dependent laser performance is investigated and shows a peak pulse power of 4.4 mW and a peak average output power of 100 µW for steady-state operation.

Suppression of axial growth by boron incorporation in GaAs nanowires grown by self-catalyzed molecular beam epitaxy.

The addition of boron to GaAs nanowires grown by self-catalyzed molecular beam epitaxy was found to have a strong effect on the nanowire morphology, with axial growth greatly reduced as the nominal boron concentration was increased. Transmission electron microscopy measurements show that the Ga catalyst droplet was unintentionally consumed during growth. Concurrent radial growth, a rough surface morphology and tapering of nanowires grown under boron flux suggest that this droplet consumption is due to reduced Ga adatom diffusion on the nanowire sidewalls in the presence of boron. Modelling of the nanowire growth puts the diffusion length of Ga adatoms under boron flux at around 700-1000 nm. Analyses of the nanowire surfaces show regions of high boron concentration, indicating the surfactant nature of boron in GaAs.

Room-Temperature Quantum Ballistic Transport in Monolithic Ultrascaled Al-Ge-Al Nanowire Heterostructures.

Conductance quantization at room temperature is a key requirement for the utilizing of ballistic transport for, e.g., high-performance, low-power dissipating transistors operating at the upper limit of "on"-state conductance or multivalued logic gates. So far, studying conductance quantization has been restricted to high-mobility materials at ultralow temperatures and requires sophisticated nanostructure formation techniques and precise lithography for contact formation. Utilizing a thermally induced exchange reaction between single-crystalline Ge nanowires and Al pads, we achieved monolithic Al-Ge-Al NW heterostructures with ultrasmall Ge segments contacted by self-aligned quasi one-dimensional crystalline Al leads. By integration in electrostatically modulated back-gated field-effect transistors, we demonstrate the first experimental observation of room temperature quantum ballistic transport in Ge, favorable for integration in complementary metal-oxide-semiconductor platform technology.

Spectrally resolved far-fields of terahertz quantum cascade lasers.

We demonstrate a convenient and fast method to measure the spectrally resolved far-fields of multimode terahertz quantum cascade lasers by combining a microbolometer focal plane array with an FTIR spectrometer. Far-fields of fundamental TM0 and higher lateral order TM1 modes of multimode Fabry-Pérot type lasers have been distinguished, which very well fit to the results obtained by a 3D finite-element simulation. Furthermore, multimode random laser cavities have been investigated, analyzing the contribution of each single laser mode to the total far-field. The presented method is thus an important tool to gain in-depth knowledge of the emission properties of multimode laser cavities at terahertz frequencies, which become increasingly important for future sensing applications.

Advanced gas sensors based on substrate-integrated hollow waveguides and dual-color ring quantum cascade lasers.

This study shows the first combination of a ring-shaped vertically emitting quantum cascade laser (riQCL) providing two distinct emission wavelengths combined with a substrate-integrated hollow waveguide (iHWG). This ultra-compact riQCL-iHWG gas sensing device enables the simultaneous detection of two vapor phase species - here, furan and 2-methoxyethanol - providing distinctive absorption features at the emission wavelengths of the riQCL (i.e., 1144 and 1170 cm-1). Hence, multianalyte gas sensing via a unique mid-infrared (MIR) sensor concept is demonstrated.

Subwavelength micropillar array terahertz lasers.

We report on micropillar-based terahertz lasers with active pillars that are much smaller than the emission wavelength. These micropillar array lasers correspond to scaled-down band-edge photonic crystal lasers forming an active photonic metamaterial. In contrast to photonic crystal lasers which use significantly larger pillar structures, lasing emission is not observed close to high-symmetry points in the photonic band diagram, but in the effective medium regime. We measure stimulated emission at 4 THz for micropillar array lasers with pillar diameters of 5 µm. Our results not only demonstrate the integration of active subwavelength optics in a terahertz laser, but are also an important step towards the realization of nanowire-based terahertz lasers.

Grating-based far field modifications of ring quantum cascade lasers.

We present methods for beam modifications of ring quantum cascade lasers emitting around λ = 9µm, which are based on novel distributed feedback grating designs. This includes the creation of a rotationally symmetric far field with a central intensity maximum using an off-center grating as well as the generation of partial radially polarized emission beams induced by a rotation of the grating slits.

Quantum cascade lasers with a tilted facet utilizing the inherent polarization purity.

We report on quantum cascade lasers (QCLs) with a tilted facet utilizing their polarization property. Contrary to diode lasers, QCLs generate purely TM polarized light due to the intersubband selection rules. This property enables the utilization of reflectivity in terms of only TM polarized light (TM reflectivity). The TM reflectivity is reduced by tilting the front facet, resulting in enhanced light output power from the tilted facet. The peak output power of a QCL with a facet angle of 12° are increased by 31 %. The slope efficiency of a QCL with a facet angle of 17° are increased by 43 %. Additionally, a peculiar property of TM reflectivity, the Brewster angle, is investigated by using COMSOL simulations to find its availability in QCLs.

Enhanced light output power of quantum cascade lasers from a tilted front facet.

We present a technique for enhancing the light output power of quantum cascade lasers (QCLs) by tilting of the front facet, which leads to a change of the modal reflectivity, resulting in an asymmetric light intensity distribution along the laser cavity. This asymmetry provides most of the light being emitted through one facet of the laser. An experimental study of threshold current, slope efficiency and light output power as a function of the front facet angles were performed and compared to conventional QCLs. The lasers with a front facet angle of 8° shows a 20% improved power output from the front facet.

Probing scattering mechanisms with symmetric quantum cascade lasers.

A characteristic feature of quantum cascade lasers is their unipolar carrier transport. We exploit this feature and realize nominally symmetric active regions for terahertz quantum cascade lasers, which should yield equal performance with either bias polarity. However, symmetric devices exhibit a strongly bias polarity dependent performance due to growth direction asymmetries, making them an ideal tool to study the related scattering mechanisms. In the case of an InGaAs/GaAsSb heterostructure, the pronounced interface asymmetry leads to a significantly better performance with negative bias polarity and can even lead to unidirectionally working devices, although the nominal band structure is symmetric. The results are a direct experimental proof that interface roughness scattering has a major impact on transport/lasing performance.

Monolithically integrated mid-infrared quantum cascade laser and detector.

We demonstrate the monolithic integration of a mid-infrared laser and detector utilizing a bi-functional quantum cascade active region. When biased, this active region provides optical gain, while it can be used as a detector at zero bias. With our novel approach we can measure the light intensity of the laser on the same chip without the need of external lenses or detectors. Based on a bound-to-continuum design, the bi-functional active region has an inherent broad electro-luminescence spectrum of 200 cm⁻¹, which indicates its use for single mode laser arrays. We have measured a peak signal of 191.5 mV at the on-chip detector, without any amplification. The room-temperature pulsed emission with an averaged power consumption of 4 mW and the high-speed detection makes these devices ideal for low-power sensors. The combination of the on-chip detection functionality, the broad emission spectrum and the low average power consumption indicates the potential of our bi-functional quantum cascade structures to build a mid-infrared lab-on-a-chip based on quantum cascade laser technology.

Microcavity-integrated graphene photodetector.

There is an increasing interest in using graphene (1, 2) for optoelectronic applications. (3-19) However, because graphene is an inherently weak optical absorber (only ≈2.3% absorption), novel concepts need to be developed to increase the absorption and take full advantage of its unique optical properties. We demonstrate that by monolithically integrating graphene with a Fabry-Pérot microcavity, the optical absorption is 26-fold enhanced, reaching values >60%. We present a graphene-based microcavity photodetector with responsivity of 21 mA/W. Our approach can be applied to a variety of other graphene devices, such as electro-absorption modulators, variable optical attenuators, or light emitters, and provides a new route to graphene photonics with the potential for applications in communications, security, sensing and spectroscopy.

Beyond Karl Fischer titration: a monolithic quantum cascade sensor for monitoring residual water concentration in solvents.

Quality control of liquids is an important part of analytical chemistry. The gold standard for measuring residual water in organic solvents and pharmaceutical applications is Karl Fischer titration. It has a high sensitivity, selectivity and accuracy. The downsides are a time-consuming offline analysis, together with the need for toxic reagents producing waste, and it suffers from poor inter-laboratory reproducibility. In this work, we present a high-performance lab-on-a-chip sensor exploiting mid-IR spectroscopy for liquid sensing. It is operating at 6.1 µm wavelength and is suitable for robust and flexible real-time in situ analysis of the residual water concentration in isopropyl alcohol. This is demonstrated in two experiments. A custom-made 60 µL flow cell is employed to measure only minute amounts of analyte in an inline configuration. In a second approach, the whole sensor is immersed into the analyte to demonstrate sensitive and rapid in situ operation on the millisecond time scale. This is confirmed by the ability for time resolved single water-droplet monitoring, while they are mixed into the liquid sample. We obtain a limit of detection between 120 ppm and 150 ppm with a concentration coverage spanning three orders of magnitude from 1.2 × 10-2%vol to 25%vol for the flow cell and 1.5 × 10-2%vol to 19%vol in the in situ configuration, respectively.

Mesoporous Zirconia Coating for Sensing Applications Using Attenuated Total Reflection Fourier Transform Infrared (ATR FT-IR) Spectroscopy.

Mid-infrared attenuated total reflection (ATR) spectroscopy is a powerful tool for in situ monitoring of various processes. Mesoporous silica, an extensively studied material, has already been applied in sensing schemes due to its high surface area and tunable surface chemistry. However, its poor chemical stability in aqueous solutions at pH values higher than 8 and strong absorption below 1250 cm-1 limits its range of applications. To circumvent these problems, a mesoporous zirconia coating on ATR crystals was developed. Herein, the synthesis, surface modification, and characterization of ordered mesoporous zirconia films on Si wafers and Si-ATR crystals are presented. The modified coating was applied in sensing schemes using aromatic and aliphatic nitriles in aqueous solution as organic pollutants. The mesoporous zirconia coating shows strong chemical resistance when kept in alkaline solution for 72 h. The success of surface modification is confirmed using Fourier transform infrared (FT-IR) spectroscopy and contact angle measurements. Benzonitrile and valeronitrile in water are used as model analytes to evaluate the enrichment performance of the film. The experimental results are fitted using Freundlich isotherms, and enrichment factors of 162 and 26 are calculated for 10 mg L-1 benzonitrile and 25 mg L-1 valeronitrile in water, respectively. Limits of detection of 1 mg L-1 for benzonitrile and 11 mg L-1 for valeronitrile are obtained. The high chemical stability of this coating allows application in diverse fields such as catalysis with the possibility of in situ monitoring using FT-IR spectroscopy.

A mid-infrared lab-on-a-chip for dynamic reaction monitoring.

Mid-infrared spectroscopy is a sensitive and selective technique for probing molecules in the gas or liquid phase. Investigating chemical reactions in bio-medical applications such as drug production is recently gaining particular interest. However, monitoring dynamic processes in liquids is commonly limited to bulky systems and thus requires time-consuming offline analytics. In this work, we show a next-generation, fully-integrated and robust chip-scale sensor for online measurements of molecule dynamics in a liquid solution. Our fingertip-sized device utilizes quantum cascade technology, combining the emitter, sensing section and detector on a single chip. This enables real-time measurements probing only microliter amounts of analyte in an in situ configuration. We demonstrate time-resolved device operation by analyzing temperature-induced conformational changes of the model protein bovine serum albumin in heavy water. Quantitative measurements reveal excellent performance characteristics in terms of sensor linearity, wide coverage of concentrations, extending from 0.075 mg ml-1 to 92 mg ml-1 and a 55-times higher absorbance than state-of-the-art bulky and offline reference systems.

Higher order modes in photonic crystal slabs.

We present a detailed investigation of higher order modes in photonic crystal slabs. In such structures the resonances exhibit a blue-shift compared to an ideal two-dimensional photonic crystal, which depends on the order of the slab mode and the polarization. By fabricating a series of photonic crystal slab photo detecting devices, with varying ratios of slab thickness to photonic crystal lattice constant, we are able to distinguish between 0th and 1st order slab modes as well as the polarization from the shift of resonances in the photocurrent spectra. This method complements the photonic band structure mapping technique for characterization of photonic crystal slabs.

Terahertz active photonic crystals for condensed gas sensing.

The terahertz (THz) spectral region, covering frequencies from 1 to 10 THz, is highly interesting for chemical sensing. The energy of rotational and vibrational transitions of molecules lies within this frequency range. Therefore, chemical fingerprints can be derived, allowing for a simple detection scheme. Here, we present an optical sensor based on active photonic crystals (PhCs), i.e., the pillars are fabricated directly from an active THz quantum-cascade laser medium. The individual pillars are pumped electrically leading to laser emission at cryogenic temperatures. There is no need to couple light into the resonant structure because the PhC itself is used as the light source. An injected gas changes the resonance condition of the PhC and thereby the laser emission frequency. We achieve an experimental frequency shift of 10(-3) times the center lasing frequency. The minimum detectable refractive index change is 1.6 × 10(-5) RIU.

d-Glucose Adsorption on the TiO2 Anatase (100) Surface: A Direct Comparison Between Cluster-Based and Periodic Approaches.

Titanium dioxide (TiO2) has been extensively studied as a suitable material for a wide range of fields including catalysis and sensing. For example, TiO2-based nanoparticles are active in the catalytic conversion of glucose into value-added chemicals, while the good biocompatibility of titania allows for its application in innovative biosensing devices for glucose detection. A key process for efficient and selective biosensors and catalysts is the interaction and binding mode between the analyte and the sensor/catalyst surface. The relevant features regard both the molecular recognition event and its effects on the nanoparticle electronic structure. In this work, we address both these features by combining two first-principles methods based on periodic boundary conditions and cluster approaches (CAs). While the former allows for the investigation of extended materials and surfaces, CAs focus only on a local region of the surface but allow for using hybrid functionals with low computational cost, leading to a highly accurate description of electronic properties. Moreover, the CA is suitable for the study of reaction mechanisms and charged systems, which can be cumbersome with PBC. Here, a direct and detailed comparison of the two computational methodologies is applied for the investigation of d-glucose on the TiO2 (100) anatase surface. As an alternative to the commonly used PBC calculations, the CA is successfully exploited to characterize the formation of surface and subsurface oxygen vacancies and to determine their decisive role in d-glucose adsorption. The results of such direct comparison allow for the selection of an efficient, finite-size structural model that is suitable for future investigations of biosensor electrocatalytic processes and biomass conversion catalysis.