Terahertz Conductivity of Free-Standing 3D Covalent Organic Framework Membranes Fabricated via Triple-Layer-Dual Interfacial Approach.

Processable covalent organic framework membranes (COFM) are emerging as potential semiconducting materials for device applications. Nevertheless, the fabrication of crystalline and free-standing 3D COFMs is challenging. In this work, a unique time and solvent-efficient triple-layer-dual interfacial (TLDI) approach for the simultaneous synthesis of two 3D COFMs from a single system is developed. Besides, for the first time, the optical conductivity of these free-standing 3D COFMs is analyzed using terahertz (THz) spectroscopy in transmission mode. Interestingly, these membranes show excellent transmittance at THz frequencies with very high intrinsic THz conductivities. The evaluated scattering time and plasma frequency of the free carriers of the COFMs are highly promising for future applications in optoelectronic devices in THz frequencies.

Critical slowing down near a magnetic quantum phase transition with fermionic breakdown.

When a system close to a continuous phase transition is subjected to perturbations, it takes an exceptionally long time to return to equilibrium. This critical slowing down is observed universally in the dynamics of bosonic excitations, such as order-parameter collective modes, but it is not generally expected to occur for fermionic excitations. Here using terahertz time-domain spectroscopy, we find evidence for fermionic critical slowing down in YbRh2Si2 close to a quantum phase transition between an antiferromagnetic phase and a heavy Fermi liquid. In the latter phase, the relevant quasiparticles are a quantum superposition of itinerant and localized electronic states with a strongly enhanced effective mass. As the temperature is lowered on the heavy-Fermi-liquid side of the transition, the heavy-fermion spectral weight builds up until the Kondo temperature TK ≈ 25 K, then decays towards the quantum phase transition and is, thereafter, followed by a logarithmic rise of the quasiparticle excitation rate below 10 K. A two-band heavy-Fermi-liquid theory shows that this is indicative of the fermionic critical slowing down associated with heavy-fermion breakdown near the quantum phase transition. The critical exponent of this breakdown could be used to classify this system among a wider family of fermionic quantum phase transitions that is yet to be fully explored.

Two-dimensional coherent spectroscopy of a THz quantum cascade laser: observation of multiple harmonics.

Two-dimensional spectroscopy is performed on a terahertz (THz) frequency quantum cascade laser (QCL) with two broadband THz pulses. Gain switching is used to amplify the first THz pulse and the second THz pulse is used to probe the system. Fourier transforms are taken with respect to the delay time between the two THz pulses and the sampling time of the THz probe pulse. The two-dimensional spectrum consists of three peaks at (ωτ = 0, ωt = ω0), (ωτ = ω0, ωt = ω0), and (ωτ = 2ω0, ωt = ω0) where ω0 denotes the lasing frequency. The peak at ωτ = 0 represents the response of the probe to the zero-frequency (rectified) component of the instantaneous intensity and can be used to measure the gain recovery.

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.

Broadband terahertz dispersion control in hybrid waveguides.

Dispersion control is a key objective in the field of photonics and spectroscopy, since it enhances non-linear effects by both enabling phase matching and offering slow light generation. In addition, it is essential for frequency comb generation, which requires a phase-lock mechanism that is provided by broadband compensation of group velocity dispersion (GVD). At optical frequencies, there are several well-established concepts for dispersion control such as prism or grating pairs. However, terahertz dispersion control is still a challenge, thus hindering further progress in the field of terahertz science and technology. In this work, we present a hybrid waveguide with both broadband, tuneable positive and more than octave-spanning negative terahertz GVD on the order of 10-22 s2/m, which is suitable for either intra- or extra cavity operation. This new terahertz device will enable ultra-short pulse compression, allow soliton propagation, improve frequency comb operation and foster the development of novel non-linear applications.

Ultrawide electrical tuning of light matter interaction in a high electron mobility transistor structure.

The interaction between intersubband resonances (ISRs) and metamaterial microcavities constitutes a strongly coupled system where new resonances form that depend on the coupling strength. Here we present experimental evidence of strong coupling between the cavity resonance of a terahertz metamaterial and the ISR in a high electron mobility transistor (HEMT) structure. The device is electrically switched from an uncoupled to a strongly coupled regime by tuning the ISR with epitaxially grown transparent gate. The asymmetric potential in the HEMT structure enables ultrawide electrical tuning of ISR, which is an order of magnitude higher as compared to an equivalent square well. For a single heterojunction with a triangular confinement, we achieve an avoided splitting of 0.52 THz, which is a significant fraction of the bare intersubband resonance at 2 THz.

Infrared transmission spectroscopy of charge carriers in self-assembled InAs quantum dots under surface electric fields.

We present a study on the intersublevel spacings of electrons and holes in a single layer of InAs self-assembled quantum dots. We use Fourier transform infrared transmission spectroscopy via a density chopping scheme for direct experimental observation of the intersublevel spacings of electrons without any external magnetic field. Epitaxial, complementary-doped and semi-transparent electrostatic gates are grown within the ultra high vacuum conditions of molecular beam epitaxy to voltage-tune the device, while a two dimensional electron gas (2DEG) serves as a back contact. Spacings of the hole sublevels are indirectly calculated from the photoluminescence spectrum by using a simple model given by Warburton et al [1]. Additionally, we observe that the intersubb and resonances of the 2DEG are enhanced due to the quantum dot layer on top of the device.