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.

Compact terahertz harmonic generation in the Reststrahlenband using a graphene-embedded metallic split ring resonator array.

Harmonic generation is a result of a strong non-linear interaction between light and matter. It is a key technology for optics, as it allows the conversion of optical signals to higher frequencies. Owing to its intrinsically large and electrically tunable non-linear optical response, graphene has been used for high harmonic generation but, until now, only at frequencies < 2 THz, and with high-power ultrafast table-top lasers or accelerator-based structures. Here, we demonstrate third harmonic generation at 9.63 THz by optically pumping single-layer graphene, coupled to a circular split ring resonator (CSRR) array, with a 3.21 THz frequency quantum cascade laser (QCL). Combined with the high graphene nonlinearity, the mode confinement provided by the optically-pumped CSRR enhances the pump power density as well as that at the third harmonic, permitting harmonic generation. This approach enables potential access to a frequency range (6-12 THz) where compact sources remain difficult to obtain, owing to the Reststrahlenband of typical III-V semiconductors.

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.

Self-Induced Mode-Locking in Electrically Pumped Far-Infrared Random Lasers.

Mode locking, the self-starting synchronous oscillation of electromagnetic modes in a laser cavity, is the primary way to generate ultrashort light pulses. In random lasers, without a cavity, mode-locking, the nonlinear coupling amongst low spatially coherent random modes, can be activated via optical pumping, even without the emission of short pulses. Here, by exploiting the combination of the inherently giant third-order χ(3) nonlinearity of semiconductor heterostructure lasers and the nonlinear properties of graphene, the authors demonstrate mode-locking in surface-emitting electrically pumped random quantum cascade lasers at terahertz frequencies. This is achieved by either lithographically patterning a multilayer graphene film to define a surface random pattern of light scatterers, or by coupling on chip a saturable absorber graphene reflector. Intermode beatnote mapping unveils self-induced phase-coherence between naturally incoherent random modes. Self-mixing intermode spectroscopy reveals phase-locked random modes. This is an important milestone in the physics of disordered systems. It paves the way to the development of a new generation of miniaturized, electrically pumped mode-locked light sources, ideal for broadband spectroscopy, multicolor speckle-free imaging applications, and reservoir quantum computing.

Detection of Strong Light-Matter Interaction in a Single Nanocavity with a Thermal Transducer.

The concept of strong light-matter coupling has been demonstrated in semiconductor structures, and it is poised to revolutionize the design and implementation of components, including solid state lasers and detectors. We demonstrate an original nanospectroscopy technique that permits the study of the light-matter interaction in single subwavelength-sized nanocavities where far-field spectroscopy is not possible using conventional techniques. We inserted a thin (∼150 nm) polymer layer with negligible absorption in the mid-infrared range (5 µm < λ < 12 µm) inside a metal-insulator-metal resonant cavity, where a photonic mode and the intersubband transition of a semiconductor quantum well are strongly coupled. The intersubband transition peaks at λ = 8.3 µm, and the nanocavity is overall 270 nm thick. Acting as a nonperturbative transducer, the polymer layer introduces only a limited alteration of the optical response while allowing to reveal the optical power absorbed inside the concealed cavity. Spectroscopy of the cavity losses is enabled by the polymer thermal expansion due to heat dissipation in the active part of the cavity, and performed using atomic force microscopy (AFM). This innovative approach allows the typical anticrossing characteristic of the polaritonic dispersion to be identified in the cavity loss spectra at the single nanoresonator level. Results also suggest that near-field coupling of the external drive field to the top metal patch mediated by a metal-coated AFM probe tip is possible, and it enables the near-field mapping of the cavity mode symmetry including in the presence of a strong light-matter interaction.

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.

Terahertz quantum cascade laser under optical feedback: effects of laser self-pulsations on self-mixing signals.

In this article, we explore the interplay between the self-pulsations (SPs) and self-mixing (SM) signals generated in terahertz (THz) quantum cascade lasers (QCLs) under optical feedback. We find that optical feedback dynamics in a THz QCL, namely, SPs, modulate the conventional SM interference fringes in a laser feedback interferometry system. The phenomenon of fringe loss in the SM signal - well known in interband diode lasers - was also observed along with pronounced SPs. With an increasing optical feedback strength, SM interference fringes transition from regular fringes at weak feedback (C ≤ 1) to fringes modulated by SPs under moderate feedback (1 < C ≤ 4.6), and then [under strong feedback (C > 4.6)] to a SM waveform with reduced number of fringes modulated by SP, until eventually (under even greater feedback) all the fringes are lost and only SPs are left visible. The transition route described above was identified in simulation when the SM fringes are created either by a moving target or a current modulation of the THz QCL. This SM signal transition route was successfully validated experimentally in a pulsed mode THz QCL with SM fringes created by current modulation during the pulse. The effects of SP dynamics in laser feedback interferometric system investigated in this work not only provides a further understanding of nonlinear dynamics in a THz QCL but also helps to understand the SM waveforms generated in a THz QCLs when they are used for various sensing and imaging applications.

Millimeter wave photonics with terahertz semiconductor lasers.

Millimeter wave (mmWave) generation using photonic techniques has so far been limited to the use of near-infrared lasers that are down-converted to the mmWave region. However, such methodologies do not currently benefit from a monolithic architecture and suffer from the quantum defect i.e. the difference in photon energies between the near-infrared and mmWave region, which can ultimately limit the conversion efficiency. Miniaturized terahertz (THz) quantum cascade lasers (QCLs) have inherent advantages in this respect: their low energy photons, ultrafast gain relaxation and high nonlinearities open up the possibility of innovatively integrating both laser action and mmWave generation in a single device. Here, we demonstrate intracavity mmWave generation within THz QCLs over the unprecedented range of 25 GHz to 500 GHz. Through ultrafast time resolved techniques, we highlight the importance of modal phases and that the process is a result of a giant second-order nonlinearity combined with a phase matched process between the THz and mmWave emission. Importantly, this work opens up the possibility of compact, low noise mmWave generation using modelocked THz frequency combs.

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.

Photoconductive arrays on insulating substrates for high-field terahertz generation.

We report on the design, fabrication and characterisation of large-area photoconductive THz array structures, consisting of a thin LT-GaAs active region transferred to an insulating substrate using a wafer-scale bonding process. The electrically insulating, transparent substrate reduces the parasitic currents in the devices, allowing peak THz-fields as high as 120 kV cm-1 to be generated over a bandwidth >5 THz. These results are achieved using lower pulse energies than demanded by conventional photoconductive arrays and other popular methods of generating high-field THz radiation. Two device sizes are fully characterised and the emission properties are compared to generation by optical rectification in ZnTe. The device can be operated in an optically saturated regime in order to suppress laser noise.

Highly efficient surface-emitting semiconductor lasers exploiting quasi-crystalline distributed feedback photonic patterns.

Quasi-crystal distributed feedback lasers do not require any form of mirror cavity to amplify and extract radiation. Once implemented on the top surface of a semiconductor laser, a quasi-crystal pattern can be used to tune both the radiation feedback and the extraction of highly radiative and high-quality-factor optical modes that do not have a defined symmetric or anti-symmetric nature. Therefore, this methodology offers the possibility to achieve efficient emission, combined with tailored spectra and controlled beam divergence. Here, we apply this concept to a one-dimensional quantum cascade wire laser. By lithographically patterning a series of air slits with different widths, following the Octonacci sequence, on the top metal layer of a double-metal quantum cascade laser operating at THz frequencies, we can vary the emission from single-frequency-mode to multimode over a 530-GHz bandwidth, achieving a maximum peak optical power of 240 mW (190 mW) in multimode (single-frequency-mode) lasers, with record slope efficiencies for multimode surface-emitting disordered THz lasers up to ≈570 mW/A at 78 K and ≈720 mW/A at 20 K and wall-plug efficiencies of η ≈ 1%.

Author Correction: Thermally and field-driven mobility of emergent magnetic charges in square artificial spin ice.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.