2D Time-Domain Spectroscopy for Determination of Energy and Momentum Relaxation Rates of Hydrogen-Like Donor States in Germanium.

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 2p0 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.

Near-field detection of gate-tunable anisotropic plasmon polaritons in black phosphorus at terahertz frequencies.

Polaritons in two-dimensional layered crystals offer an effective solution to confine, enhance and manipulate terahertz (THz) frequency electromagnetic waves at the nanoscale. Recently, strong THz field confinement has been achieved in a graphene-insulator-metal structure, exploiting THz plasmon polaritons (PPs) with strongly reduced wavelength (λp ≈ λ0/66) compared to the photon wavelength λ0. However, graphene PPs propagate isotropically, complicating the directional control of the THz field, which, on the contrary, can be achieved exploiting anisotropic layered crystals, such as orthorhombic black-phosphorus. Here, we detect PPs, at THz frequencies, in hBN-encapsulated black phosphorus field effect transistors through THz near-field photocurrent nanoscopy. The real-space mapping of the thermoelectrical near-field photocurrents reveals deeply sub-wavelength THz PPs (λp ≈ λ0/76), with dispersion tunable by electrostatic control of the carrier density. The in-plane anisotropy of the dielectric response results into anisotropic polariton propagation along the armchair and zigzag crystallographic axes of black-phosphorus. The achieved directional subwavelength light confinement makes this material system a versatile platform for sensing and quantum technology based on nonlinear optics.

Terahertz microscopy using laser feedback interferometry based on a generalised phase-stepping algorithm.

In this paper we report an improved method of coherent sensing through the use of a generalized phase-stepping algorithm to extract magnitude and phase information from interferometric fringes acquired by laser feedback interferometry (LFI). Our approach allows for significantly reduced optical sampling and acquisition times whilst also avoiding the need for fitting to complex models of lasers under optical feedback in post-processing. We investigate theoretically the applicability of this method under different levels of optical feedback, different laser parameters, and for different sampling conditions. We furthermore validate its use experimentally for LFI-based sensing using a terahertz (THz)-frequency laser in both far-field and near-field sensing configurations. Finally we demonstrate our approach for two-dimensional nanoscale imaging of the out-of-plane field supported by individual micro-resonators at THz frequencies. Our results show that fully coherent sensing can be achieved reliably with as little as 4 sampling points per imaging pixel, opening up opportunities for fast coherent sensing not only at THz frequencies but across the visible and infra-red spectrum.

Electrically Tunable Nonlinearity at 3.2 Terahertz in Single-Layer Graphene.

Graphene is a nonlinear material in the terahertz (THz) frequency range, with χ(3) ∼ 10-9 m2/V2 ∼ 15 orders of magnitude higher than that of other materials used in the THz range, such as GaAs or lithium niobate. This nonlinear behavior, combined with ultrafast dynamic for excited carriers, proved to be essential for third harmonic generation in the sub-THz and low (<2.5 THz) THz range, using moderate (60 kV/cm) fields and at room temperature. Here, we show that, for monochromatic high peak power (1.8 W) input THz signals, emitted by a quantum cascade laser, the nonlinearity can be controlled using an ionic liquid gate that tunes the graphene Fermi energy up to >1.2 eV. Pump and probe experiments reveal an intense absorption nonlinearity at 3.2 THz, with a dominant 3rd-order contribution at EF > 0.7 eV, hence opening intriguing perspectives per engineering novel architectures for light generation at frequencies > 9 THz.

Coherent terahertz laser feedback interferometry for hydration sensing in leaves.

The response of terahertz to the presence of water content makes it an ideal analytical tool for hydration monitoring in agricultural applications. This study reports on the feasibility of terahertz sensing for monitoring the hydration level of freshly harvested leaves of Celtis sinensis by employing a imaging platform based on quantum cascade lasers and laser feedback interferometry. The imaging platform produces wide angle high resolution terahertz amplitude and phase images of the leaves at high frame rates allowing monitoring of dynamic water transport and other changes across the whole leaf. The complementary information in the resulting images was fed to a machine learning model aiming to predict relative water content from a single frame. The model was used to predict the change in hydration level over time. Results of the study suggest that the technique could have substantial potential in agricultural applications.

Terahertz imaging of human skin pathologies using laser feedback interferometry with quantum cascade lasers.

Early detection of skin pathologies with current clinical diagnostic tools is challenging, particularly when there are no visible colour changes or morphological cues present on the skin. In this study, we present a terahertz (THz) imaging technology based on a narrow band quantum cascade laser (QCL) at 2.8 THz for human skin pathology detection with diffraction limited spatial resolution. THz imaging was conducted for three different groups of unstained human skin samples (benign naevus, dysplastic naevus, and melanoma) and compared to the corresponding traditional histopathologic stained images. The minimum thickness of dehydrated human skin that can provide THz contrast was determined to be 50 µm, which is approximately one half-wavelength of the THz wave used. The THz images from different types of 50 µm-thick skin samples were well correlated with the histological findings. The per-sample locations of pathology vs healthy skin can be separated from the density distribution of the corresponding pixels in the THz amplitude-phase map. The possible THz contrast mechanisms relating to the origin of image contrast in addition to water content were analyzed from these dehydrated samples. Our findings suggest that THz imaging could provide a feasible imaging modality for skin cancer detection that is beyond the visible.

Comparison of Physical and System Factors Impacting Hydration Sensing in Leaves Using Terahertz Time-Domain and Quantum Cascade Laser Feedback Interferometry Imaging.

To reduce the water footprint in agriculture, the recent push toward precision irrigation management has initiated a sharp rise in photonics-based hydration sensing in plants in a non-contact, non-invasive manner. Here, this aspect of sensing was employed in the terahertz (THz) range for mapping liquid water in the plucked leaves of Bambusa vulgaris and Celtis sinensis. Two complementary techniques, broadband THz time-domain spectroscopic imaging and THz quantum cascade laser-based imaging, were utilized. The resulting hydration maps capture the spatial variations within the leaves as well as the hydration dynamics in various time scales. Although both techniques employed raster scanning to acquire the THz image, the results provide very distinct and different information. Terahertz time-domain spectroscopy provides rich spectral and phase information detailing the dehydration effects on the leaf structure, while THz quantum cascade laser-based laser feedback interferometry gives insight into the fast dynamic variation in dehydration patterns.

Resonant two-photon terahertz quantum cascade laser.

Lasers that can emit two photons from a single electron relaxation between two states of the same parity have been discussed since the early days of the laser era. However, such lasers have seen only limited success, mainly due to a lack of suitable gain medium. We propose that terahertz (THz) frequency quantum cascade lasers (QCLs) are an ideal semiconductor structure to realize such two-photon emissions. In this work, we present a THz QCL heterostructure designed to emit two resonant photons from each electronic relaxation between two same-parity states in the active region. We present coupled Maxwell-Bloch equations that describe the dynamics of such a two-photon laser and find analytical solutions for the steady-state light intensity, the steady-state energy-resolved carrier densities, and the total threshold carrier density. Due to the two-photon emission from each excited state relaxation and an increased photon-driven carrier transport rate, our simulations predict a significant enhancement of light intensity in our designed resonant two-photon THz QCL when compared to an exemplar conventional THz QCL structure.

Self-Induced Phase Locking of Terahertz Frequency Combs in a Phase-Sensitive Hyperspectral Near-Field Nanoscope.

Chip-scale, electrically-pumped terahertz (THz) frequency-combs (FCs) rely on nonlinear four-wave-mixing processes, and have a nontrivial phase relationship between the evenly spaced set of emitted modes. Simultaneous monitoring and manipulation of the intermode phase coherence, without any external seeding or active modulation, is a very demanding task for which there has hitherto been no technological solution. Here, a self-mixing intermode-beatnote spectroscopy system is demonstrated, based on THz quantum cascade laser FCs, in which light is back-scattered from the tip of a scanning near-field optical-microscope (SNOM) and the intracavity reinjection monitored. This enables to exploit the sensitivity of FC phase-coherence to optical feedback and, for the first time, manipulate the amplitude, linewidth and frequency of the intermode THz FC beatnote using the feedback itself. Stable phase-locked regimes are used to construct a FC-based hyperspectral, THz s-SNOM nanoscope. This nanoscope provides 160 nm spatial resolution, coherent detection of multiple phase-locked modes, and mapping of the THz optical response of nanoscale materials up to 3.5 THz, with noise-equivalent-power (NEP) ≈400 pW √Hz-1 . This technique can be applied to the entire infrared range, opening up a new approach to hyper-spectral near-field imaging with wide-scale applications in the study of plasmonics and quantum science, inter alia.

Micro-homology intermediates: RecA's transient sampling revealed at the single molecule level.

Recombinase A (RecA) is central to homologous recombination. However, despite significant advances, the mechanism with which RecA is able to orchestrate a search for homology remains elusive. DNA nanostructure-augmented high-speed AFM offers the spatial and temporal resolutions required to study the RecA recombination mechanism directly and at the single molecule level. We present the direct in situ observation of RecA-orchestrated alignment of homologous DNA strands to form a stable recombination product within a supporting DNA nanostructure. We show the existence of subtle and short-lived states in the interaction landscape, which suggests that RecA transiently samples micro-homology at the single RecA monomer-level throughout the search for sequence alignment. These transient interactions form the early steps in the search for sequence homology, prior to the formation of stable pairings at >8 nucleotide seeds. The removal of sequence micro-homology results in the loss of the associated transient sampling at that location.

Terahertz Frequency Combs Exploiting an On-Chip, Solution-Processed, Graphene-Quantum Cascade Laser Coupled-Cavity.

The ability to engineer quantum-cascade-lasers (QCLs) with ultrabroad gain spectra, and with a full compensation of the group velocity dispersion, at terahertz (THz) frequencies, is key for devising monolithic and miniaturized optical frequency-comb-synthesizers (FCSs) in the far-infrared. In THz QCLs four-wave mixing, driven by intrinsic third-order susceptibility of the intersubband gain medium, self-locks the optical modes in phase, allowing stable comb operation, albeit over a restricted dynamic range (∼20% of the laser operational range). Here, we engineer miniaturized THz FCSs, comprising a heterogeneous THz QCL, integrated with a tightly coupled, on-chip, solution-processed, graphene saturable-absorber reflector that preserves phase-coherence between lasing modes, even when four-wave mixing no longer provides dispersion compensation. This enables a high-power (8 mW) FCS with over 90 optical modes, through 55% of the laser operational range. We also achieve stable injection-locking, paving the way to a number of key applications, including high-precision tunable broadband-spectroscopy and quantum-metrology.

Ultrafast terahertz saturable absorbers using tailored intersubband polaritons.

Semiconductor heterostructures have enabled a great variety of applications ranging from GHz electronics to photonic quantum devices. While nonlinearities play a central role for cutting-edge functionality, they require strong field amplitudes owing to the weak light-matter coupling of electronic resonances of naturally occurring materials. Here, we ultrastrongly couple intersubband transitions of semiconductor quantum wells to the photonic mode of a metallic cavity in order to custom-tailor the population and polarization dynamics of intersubband cavity polaritons in the saturation regime. Two-dimensional THz spectroscopy reveals strong subcycle nonlinearities including six-wave mixing and a collapse of light-matter coupling within 900 fs. This collapse bleaches the absorption, at a peak intensity one order of magnitude lower than previous all-integrated approaches and well achievable by state-of-the-art QCLs, as demonstrated by a saturation of the structure under cw-excitation. We complement our data by a quantitative theory. Our results highlight a path towards passively mode-locked QCLs based on polaritonic saturable absorbers in a monolithic single-chip design.

Modeling and improving the output power of terahertz master-oscillator power-amplifier quantum cascade lasers.

A model based on carrier rate equations is proposed to evaluate the gain saturation and predict the dependence of the output power of a terahertz master-oscillator power-amplifier quantum cascade laser (THz-MOPA-QCL) on the material and structure parameters. The model reveals the design rules of the preamplifier and the power extractor to maximize the output power and the wall-plug efficiency. The correction of the model is verified by its agreement with the experiment results. The optimized MOPA devices exhibit single-mode emission at ∼ 2.6 THz with a side mode suppression ratio of 23 dB, a pulsed output power of 153 mW, a wall-plug efficiency of 0.22%, and a low divergence angle of ∼6°×16°, all measured at an operation temperature of 77 K. The model developed here is helpful for the design of MOPA devices and semiconductor optical amplifiers, in which the active region is based on intersubband transitions.

Optomechanical response with nanometer resolution in the self-mixing signal of a terahertz quantum cascade laser.

Owing to their intrinsic stability against optical feedback (OF), quantum cascade lasers (QCLs) represent a uniquely versatile source to further improve self-mixing interferometry at mid-infrared and terahertz (THz) frequencies. Here, we show the feasibility of detecting with nanometer precision, the deeply subwavelength ($ \lt \lambda /6000 $<λ/6000) mechanical vibrations of a suspended $ {{\rm Si}_3}{{\rm N}_4} $Si3N4 membrane used as the external element of a THz QCL feedback interferometer. Besides representing an extension of the applicability of vibrometric characterization at THz frequencies, our system can be exploited for the realization of optomechanical applications, such as dynamical switching between different OF regimes and a still-lacking THz master-slave configuration.

Tunable and compact dispersion compensation of broadband THz quantum cascade laser frequency combs.

Miniaturized frequency combs (FCs) can be self-generated at terahertz (THz) frequencies through four-wave mixing in the cavity of a quantum cascade laser (QCL). To date, however, stable comb operation is only observed over a small operational current range in which the bias-depended chromatic dispersion is compensated. As most dispersion compensation techniques in the THz range are not tunable, this limits the spectral coverage of the comb and the emitted output power, restricting potential applications in, for example, metrology and ultrashort THz pulse generation. Here, we demonstrate an alternative architecture that provides a tunable, lithographically independent, control of the free-running coherence properties of THz QCL FCs. This is achieved by integrating an on-chip tightly coupled mirror with the QCL cavity, providing an external cavity and hence a tunable Gires Tournois interferometer (GTI). By finely adjusting the gap between the GTI and the back-facet of an ultra-broadband, high dynamic range QCL, we attain wide dispersion compensation regions, where stable and narrow (~3 kHz linewidth) single beatnotes extend over an operation range that is significantly larger than that of dispersion-dominated bare laser cavity counterparts. Significant reduction of the phase noise is registered over the whole QCL spectral bandwidth (1.35 THz). This agile accommodation of a tunable dispersion compensator will help enable uptake of QCL-combs for metrological, spectroscopic and quantum technology-oriented applications.

Fully phase-stabilized quantum cascade laser frequency comb.

Miniaturized frequency comb sources across hard-to-access spectral regions, i.e. mid- and far-infrared, have long been sought. Four-wave-mixing based Quantum Cascade Laser combs (QCL-combs) are ideal candidates, in this respect, due to the unique possibility to tailor their spectral emission by proper nanoscale design of the quantum wells. We demonstrate full-phase-stabilization of a QCL-comb against the primary frequency standard, proving independent and simultaneous control of the two comb degrees of freedom (modes spacing and frequency offset) at a metrological level. Each emitted mode exhibits a sub-Hz relative frequency stability, while a correlation analysis on the modal phases confirms the high degree of coherence in the device emission, over different power-cycles and over different days. The achievement of fully controlled, phase-stabilized QCL-comb emitters proves that this technology is mature for metrological-grade uses, as well as for an increasing number of scientific and technological applications.

Coherent imaging using laser feedback interferometry with pulsed-mode terahertz quantum cascade lasers.

We report a coherent terahertz (THz) imaging system that utilises a quantum cascade laser (QCL) operating in pulsed-mode as both the source and detector. The realisation of a short-pulsed THz QCL feedback interferometer permits both high peak powers and improved thermal efficiency, which enables the cryogen-free operation of the system. In this work, we demonstrated pulsed-mode swept-frequency laser feedback interferometry experimentally. Our interferometric detection scheme not only permits the simultaneous creation of both amplitude and phase images, but inherently suppresses unwanted background radiation. We demonstrate that the proposed system utilising microsecond pulses has the potential to achieve 0.25 mega-pixel per second acquisition rates, paving the pathway to video frame rate THz imaging.

Frequency-tunable continuous-wave random lasers at terahertz frequencies.

Random lasers are a class of devices in which feedback arises from multiple elastic scattering in a highly disordered structure, providing an almost ideal light source for artefact-free imaging due to achievable low spatial coherence. However, for many applications ranging from sensing and spectroscopy to speckle-free imaging, it is essential to have high-radiance sources operating in continuous-wave (CW). In this paper, we demonstrate CW operation of a random laser using an electrically pumped quantum-cascade laser gain medium in which a bi-dimensional (2D) random distribution of air holes is patterned into the top metal waveguide. We obtain a highly collimated vertical emission at ~3 THz, with a 430 GHz bandwidth, device operation up to 110 K, peak (pulsed) power of 21 mW, and CW emission of 1.7 mW. Furthermore, we show that an external cavity formed with a movable mirror can be used to tune a random laser, obtaining continuous frequency tuning over 11 GHz.

Ultrafast two-dimensional field spectroscopy of terahertz intersubband saturable absorbers.

Intersubband (ISB) transitions in semiconductor multi-quantum well (MQW) structures are promising candidates for the development of saturable absorbers at terahertz (THz) frequencies. Here, we exploit amplitude and phase-resolved two-dimensional (2D) THz spectroscopy on the sub-cycle time scale to observe directly the saturation dynamics and coherent control of ISB transitions in a metal-insulator MQW structure. Clear signatures of incoherent pump-probe and coherent four-wave mixing signals are recorded as a function of the peak electric field of the single-cycle THz pulses. All nonlinear signals reach a pronounced maximum for a THz electric field amplitude of 11 kV/cm and decrease for higher fields. We demonstrate that this behavior is a fingerprint of THz-driven carrier-wave Rabi flopping. A numerical solution of the Maxwell-Bloch equations reproduces our experimental findings quantitatively and traces the trajectory of the Bloch vector. This microscopic model allows us to design tailored MQW structures with optimized dynamical properties for saturable absorbers that could be used in future compact semiconductor-based single-cycle THz sources.