Quartz-Enhanced Photoacoustic Sensor Based on a Multi-Laser Source for In-Sequence Detection of NO2, SO2, and NH3.

In this work, we report on the implementation of a multi-quantum cascade laser (QCL) module as an innovative light source for quartz-enhanced photoacoustic spectroscopy (QEPAS) sensing. The source is composed of three different QCLs coupled with a dichroitic beam combiner module that provides an overlapping collimated beam output for all three QCLs. The 3λ-QCL QEPAS sensor was tested for detection of NO2, SO2, and NH3 in sequence in a laboratory environment. Sensitivities of 19.99 mV/ppm, 19.39 mV/ppm, and 73.99 mV/ppm were reached for NO2, SO2, and NH3 gas detection, respectively, with ultimate detection limits of 9 ppb, 9.3 ppb, and 2.4 ppb for these three gases, respectively, at an integration time of 100 ms. The detection limits were well below the values of typical natural abundance of NO2, SO2, and NH3 in air.

Efficient Second-Harmonic Generation from Dielectric Inter-subband Polaritonic Metasurfaces Coupled to Lattice Resonance.

Nonlinear optical metasurfaces offer a possibility to perform frequency mixing without the phase-matching constraints of bulk nonlinear crystals and with control of the local nonlinear response at a sub-wavelength scale. Nonlinear inter-subband polaritonic metasurfaces created by combining the semiconductor heterostructures with quantum-engineered inter-subband nonlinear response and electromagnetically engineered metal-clad nanoresonators offer by far the largest second-order nonlinear response of all condensed matter systems reported to date. However, the nonlinear optical response of these metasurfaces is limited by optical intensity saturation in the nanoresonator hot spots that prevented the achievement of power conversion efficiencies over 0.2% in three-wave mixing experiments. In this study, we propose and experimentally demonstrate dielectric inter-subband polaritonic metasurfaces for second-harmonic generation that achieve 0.37% power conversion efficiency. Our structure is created by a new design approach that combines dielectric resonators inducing Mie resonant modes with a lattice resonance to achieve a uniform and high field enhancement throughout the meta-atom volume.

Electrical Phase Modulation Based on Mid-Infrared Intersubband Polaritonic Metasurfaces.

Electrically reconfigurable metasurfaces that overcome the static limitations in controlling the fundamental properties of scattered light are opening new avenues for functional flat optics. This work proposes and experimentally demonstrates electrically phase-tunable mid-infrared metasurfaces based on the polaritonic coupling of Stark-tunable intersubband transitions in semiconductor heterostructures and electromagnetic modes in plasmonic nanoresonators. In the applied voltage range of -3 to +3 V, the local phase tuning of the light reflects from the metasurface, which enables the electrical control of the polarization state and wavefront of the reflected wave. Electrical beam polarization control, electrical beam diffraction control, and electrical beam steering are experimentally demonstrated as applications for local phase tunability. The proposed electrically tunable metasurfaces can easily tune the operating wavelength and function at relatively low voltages, which will enable various applications in the mid-infrared region.

Terahertz difference-frequency-generation quantum cascade lasers on silicon with wire grid current injectors.

We propose the concept and experimentally verify the operation of terahertz quantum cascade laser sources based on intra-cavity Cherenkov difference-frequency generation on a silicon substrate with the current injection layer configured as a metal wire grid. Such a current injector configuration enables high transmission of TM-polarized terahertz radiation into the silicon substrate while simultaneously providing a low-resistivity metal contact for current injection.

Control of second-harmonic generation in all-dielectric intersubband metasurfaces by controlling the polarity of χ(2).

All-dielectric metasurfaces have recently led to a paradigm shift in nonlinear optics as they allow for circumventing the phase matching constraints of bulk crystals and offer high nonlinear conversion efficiencies when normalized by the light-matter interaction volume. Unlike bulk crystals, in all-dielectric metasurfaces nonlinear conversion efficiencies primarily rely on the material nonlinearity, field enhancements, and the modal overlaps, therefore most efforts to date have only focused on utilizing these degrees of freedom. In this work, we demonstrate that for second-harmonic generation in all-dielectric metasurfaces, an additional degree of freedom is the control of the polarity of the nonlinear susceptibility. We demonstrate that semiconductor heterostructures that support resonant nonlinearities based on quantum-engineered intersubband transitions provide this new degree of freedom. We can flip and control the polarity of the nonlinear susceptibility of the dielectric medium along the growth direction and couple it to the Mie-type photonic modes. Here we demonstrate that engineering the χ(2) polarity in the meta-atom enables the control of the second-harmonic radiation pattern and conversion efficiency. Our results therefore open a new direction for engineering and optimizing second-harmonic generation using all-dielectric intersubband nonlinear metasurfaces.

An All-Dielectric Polaritonic Metasurface with a Giant Nonlinear Optical Response.

Enhancing the efficiency of second-harmonic generation using all-dielectric metasurfaces to date has mostly focused on electromagnetic engineering of optical modes in the meta-atom. Further advances in nonlinear conversion efficiencies can be gained by engineering the material nonlinearities at the nanoscale, however this cannot be achieved using conventional materials. Semiconductor heterostructures that support resonant nonlinearities using quantum engineered intersubband transitions can provide this new degree of freedom. By simultaneously optimizing the heterostructures and meta-atoms, we experimentally realize an all-dielectric polaritonic metasurface with a maximum second-harmonic generation power conversion factor of 0.5 mW/W2 and power conversion efficiencies of 0.015% at nominal pump intensities of 11 kW/cm2. These conversion efficiencies are higher than the record values reported to date in all-dielectric nonlinear metasurfaces but with 3 orders of magnitude lower pump power. Our results therefore open a new direction for designing efficient nonlinear all-dielectric metasurfaces for new classical and quantum light sources.

Strong Coupling in All-Dielectric Intersubband Polaritonic Metasurfaces.

Mie-resonant dielectric metasurfaces are excellent candidates for both fundamental studies related to light-matter interactions and for numerous applications ranging from holography to sensing to nonlinear optics. To date, however, most applications using Mie metasurfaces utilize only weak light-matter interaction. Here, we go beyond the weak coupling regime and demonstrate for the first time strong polaritonic coupling between Mie photonic modes and intersubband (ISB) transitions in semiconductor heterostructures. Furthermore, along with demonstrating ISB polaritons with Rabi splitting as large as 10%, we also demonstrate the ability to tailor the strength of strong coupling by engineering either the semiconductor heterostructure or the photonic mode of the resonators. Unlike previous plasmonic-based works, our new all-dielectric metasurface approach to generate ISB polaritons is free from ohmic losses and has high optical damage thresholds, thereby making it ideal for creating novel and compact mid-infrared light sources based on nonlinear optics.

Giant Nonlinear Circular Dichroism from Intersubband Polaritonic Metasurfaces.

Nonlinear metasurfaces are advancing into a new paradigm of "flat nonlinear optics" owing to the ability to engineer local nonlinear responses in subwavelength-thin films. Recently, attempts have been made to expand the design space of nonlinear metasurfaces through nonlinear chiral responses. However, the development of metasurfaces that display both giant nonlinear circular dichroism and significantly large nonlinear optical response is still an unresolved challenge. Herein, we propose a method that induces giant nonlinear responses with near-unity circular dichroism using polaritonic metasurfaces with optical modes in chiral plasmonic nanocavities coupled with intersubband transitions in semiconductor heterostructures designed to have giant second and third order nonlinear responses. A stark contrast between effective nonlinear susceptibility elements for the two spin states of circularly polarized pump beams was seen in the hybrid structure. Experimentally, near-unity nonlinear circular dichroism and conversion efficiencies beyond 10-4% for second- and third-harmonic generation were achieved simultaneously in a single chip.

Quantum Confinement in Oxide Heterostructures: Room-Temperature Intersubband Absorption in SrTiO3/LaAlO3 Multiple Quantum Wells.

The Si-compatibility of perovskite heterostructures offers the intriguing possibility of producing oxide-based quantum well (QW) optoelectronic devices for use in Si photonics. While the SrTiO3/LaAlO3 (STO/LAO) system has been studied extensively in the hopes of using the interfacial two-dimensional electron gas in Si-integrated electronics, the potential to exploit its giant 2.4 eV conduction band offset in oxide-based QW optoelectronic devices has so far been largely ignored. Here, we demonstrate room-temperature intersubband absorption in STO/LAO QW heterostructures at energies on the order of hundreds of meV, including at energies approaching the critically important telecom wavelength of 1.55 µm. We demonstrate the ability to control the absorption energy by changing the width of the STO well layers by a single unit cell and present theory showing good agreement with experiment. A detailed structural and chemical analysis of the samples via scanning transmission electron microscopy and electron energy loss spectroscopy is presented. This work represents an important proof-of-concept for the use of transition metal oxide QWs in Si-compatible optoelectronic devices.

Spectral purity and tunability of terahertz quantum cascade laser sources based on intracavity difference-frequency generation.

Terahertz sources based on intracavity difference-frequency generation in mid-infrared quantum cascade lasers (THz DFG-QCLs) have recently emerged as the first monolithic electrically pumped semiconductor sources capable of operating at room temperature across the 1- to 6-THz range. Despite tremendous progress in power output, which now exceeds 1 mW in pulsed and 10 µW in continuous-wave regimes at room temperature, knowledge of the major figure of merits of these devices for high-precision spectroscopy, such as spectral purity and absolute frequency tunability, is still lacking. By exploiting a metrological grade system comprising a terahertz frequency comb synthesizer, we measure, for the first time, the free-running emission linewidth (LW), the tuning characteristics, and the absolute center frequency of individual emission lines of these sources with an uncertainty of 4 × 10-10. The unveiled emission LW (400 kHz at 1-ms integration time) indicates that DFG-QCLs are well suited to operate as local oscillators and to be used for a variety of metrological, spectroscopic, communication, and imaging applications that require narrow-LW THz sources.

Electrical tuning of the polarization state of light using graphene-integrated anisotropic metasurfaces.

Plasmonic metasurfaces have been employed for moulding the flow of transmitted and reflected light, thereby enabling numerous applications that benefit from their ultra-thin sub-wavelength format. Their appeal is further enhanced by the incorporation of active electro-optic elements, paving the way for dynamic control of light's properties. In this paper, we realize a dynamic polarization state generator using a graphene-integrated anisotropic metasurface (GIAM) that converts the linear polarization of the incident light into an elliptical one. This is accomplished by using an anisotropic metasurface with two principal polarization axes, one of which possesses a Fano-type resonance. A gate-controlled single-layer graphene integrated with the metasurface was employed as an electro-optic element controlling the phase and intensity of light polarized along the resonant axis of the GIAM. When the incident light is polarized at an angle to the resonant axis of the metasurface, the ellipticity of the reflected light can be dynamically controlled by the application of a gate voltage. Thus accomplished dynamic polarization control is experimentally demonstrated and characterized by measuring the Stokes polarization parameters. Large changes of the ellipticity and the tilt angle of the polarization ellipse are observed. Our measurements show that the tilt angle can be changed from positive values through zero to negative values while keeping the ellipticity constant, potentially paving the way to rapid ellipsometry and other characterization techniques requiring fast polarization shifting.This article is part of the themed issue 'New horizons for nanophotonics'.

Thermopile detector of light ellipticity.

Polarimetric imaging is widely used in applications from material analysis to biomedical diagnostics, vision and astronomy. The degree of circular polarization, or light ellipticity, is associated with the S3 Stokes parameter which is defined as the difference in the intensities of the left- and right-circularly polarized components of light. Traditional way of determining this parameter relies on using several external optical elements, such as polarizers and wave plates, along with conventional photodetectors, and performing at least two measurements to distinguish left- and right-circularly polarized light components. Here we theoretically propose and experimentally demonstrate a thermopile photodetector element that provides bipolar voltage output directly proportional to the S3 Stokes parameter of the incident light.

Experimental Demonstration of Phase Modulation and Motion Sensing Using Graphene-Integrated Metasurfaces.

Strong interaction of graphene with light accounts for one of its most remarkable properties: the ability to absorb 2.3% of the incident light's energy within a single atomic layer. Free carrier injection via field-effect gating can dramatically vary the optical properties of graphene, thereby enabling fast graphene-based modulators of the light intensity. However, the very thinness of graphene makes it difficult to modulate the other fundamental property of the light wave: its optical phase. Here we demonstrate that considerable phase control can be achieved by integrating a single-layer graphene (SLG) with a resonant plasmonic metasurface that contains nanoscale gaps. By concentrating the light intensity inside of the nanogaps, the metasurface dramatically increases the coupling of light to the SLG and enables control of the phase of the reflected mid-infrared light by as much as 55° via field-effect gating. We experimentally demonstrate graphene-based phase modulators that maintain the amplitude of the reflected light essentially constant over most of the phase tuning range. Rapid nonmechanical phase modulation enables a new experimental technique, graphene-based laser interferometry, which we use to demonstrate motion detection with nanoscale precision. We also demonstrate that by the judicious choice of a strongly anisotropic metasurface the graphene-controlled phase shift of light can be rendered polarization-dependent. Using the experimentally measured phases for the two orthogonal polarizations, we demonstrate that the polarization state of the reflected light can be by modulated by carrier injection into the SLG. These results pave the way for novel high-speed graphene-based optical devices and sensors such as polarimeters, ellipsometers, and frequency modulators.

Spectroscopic Study of Terahertz Generation in Mid-Infrared Quantum Cascade Lasers.

Terahertz quantum cascade laser sources based on intra-cavity difference-frequency generation are currently the only room-temperature mass-producible diode-laser-like emitters of coherent 1-6 THz radiation. Device performance has improved dramatically over the past few years to reach milliwatt-level power output and broad tuning from 1.2 to 5.9 THz, all at room-temperature. Terahertz output in these sources originates from intersubband optical nonlinearity in the laser active region. Here we report the first comprehensive spectroscopic study of the optical nonlinearity and investigate its dependence on the mid-infrared pump frequencies. Our work shows that the terahertz generation efficiency can vary by a factor of 2 or greater depending on the spectral position of the mid-infrared pumps for a fixed THz difference-frequency. We have also measured for the first time the linewidth for transitions between the lower quantum cascade laser states, which is critical for determining terahertz nonlinearity and predicting optical loss in quantum cascade laser waveguides.

Gradient Nonlinear Pancharatnam-Berry Metasurfaces.

We apply the Pancharatnam-Berry phase approach to plasmonic metasurfaces loaded by highly nonlinear multiquantum-well substrates, establishing a platform to control the nonlinear wave front at will based on giant localized nonlinear effects. We apply this approach to design flat nonlinear metasurfaces for efficient second-harmonic radiation, including beam steering, focusing, and polarization manipulation. Our findings open a new direction for nonlinear optics, in which phase matching issues are relaxed, and an unprecedented level of local wave front control is achieved over thin devices with giant nonlinear responses.

Giant nonlinear response from plasmonic metasurfaces coupled to intersubband transitions.

Intersubband transitions in n-doped multi-quantum-well semiconductor heterostructures make it possible to engineer one of the largest known nonlinear optical responses in condensed matter systems--but this nonlinear response is limited to light with electric field polarized normal to the semiconductor layers. In a different context, plasmonic metasurfaces (thin conductor-dielectric composite materials) have been proposed as a way of strongly enhancing light-matter interaction and realizing ultrathin planarized devices with exotic wave properties. Here we propose and experimentally realize metasurfaces with a record-high nonlinear response based on the coupling of electromagnetic modes in plasmonic metasurfaces with quantum-engineered electronic intersubband transitions in semiconductor heterostructures. We show that it is possible to engineer almost any element of the nonlinear susceptibility tensor of these structures, and we experimentally verify this concept by realizing a 400-nm-thick metasurface with nonlinear susceptibility of greater than 5 × 10(4) picometres per volt for second harmonic generation at a wavelength of about 8 micrometres under normal incidence. This susceptibility is many orders of magnitude larger than any second-order nonlinear response in optical metasurfaces measured so far. The proposed structures can act as ultrathin highly nonlinear optical elements that enable efficient frequency mixing with relaxed phase-matching conditions, ideal for realizing broadband frequency up- and down-conversions, phase conjugation and all-optical control and tunability over a surface.

Broadly tunable monolithic room-temperature terahertz quantum cascade laser sources.

Electrically pumped room-temperature semiconductor sources of tunable terahertz radiation in 1-5 THz spectral range are highly desired to enable compact instrumentation for THz sensing and spectroscopy. Quantum cascade lasers with intra-cavity difference-frequency generation are currently the only room-temperature electrically pumped semiconductor sources that can operate in the entire 1-5 THz spectral range. Here we demonstrate that this technology is suitable to implementing monolithic room-temperature terahertz tuners with broadband electrical control of the emission frequency. Experimentally, we demonstrate ridge waveguide devices electrically tunable between 3.44 and 4.02 THz.

Broadly tunable terahertz generation in mid-infrared quantum cascade lasers.

Room temperature, broadly tunable, electrically pumped semiconductor sources in the terahertz spectral range, similar in operation simplicity to diode lasers, are highly desired for applications. An emerging technology in this area are sources based on intracavity difference-frequency generation in dual-wavelength mid-infrared quantum cascade lasers. Here we report terahertz quantum cascade laser sources based on an optimized non-collinear Cherenkov difference-frequency generation scheme that demonstrates dramatic improvements in performance. Devices emitting at 4 THz display a mid-infrared-to-terahertz conversion efficiency in excess of 0.6 mW W(-2) and provide nearly 0.12 mW of peak power output. Devices emitting at 2 and 3 THz fabricated on the same chip display 0.09 and 0.4 mW W(-2) conversion efficiencies at room temperature, respectively. High terahertz-generation efficiency and relaxed phase-matching conditions offered by the Cherenkov scheme allowed us to demonstrate, for the first time, an external-cavity terahertz quantum cascade laser source tunable between 1.70 and 5.25 THz.

Infrared absorption nano-spectroscopy using sample photoexpansion induced by tunable quantum cascade lasers.

We report a simple technique that allows obtaining mid-infrared absorption spectra with nanoscale spatial resolution under low-power illumination from tunable quantum cascade lasers. Light absorption is detected by measuring associated sample thermal expansion with an atomic force microscope. To detect minute thermal expansion we tune the repetition frequency of laser pulses in resonance with the mechanical frequency of the atomic force microscope cantilever. Spatial resolution of better than 50 nm is experimentally demonstrated.