Abstract: Terahertz time-domain-spectroscopy (THz-TDS) has emerged as a versatile spectroscopic technique, and an alternative to powder X-ray diffraction in the characterization of molecular crystals. We tested the ability of terahertz spectroscopy to distinguish between chiral and racemic hydrogen-bonded cocrystals that are similar in molecular and supramolecular structure. Terahertz spectroscopy readily distinguished between the isostructural cocrystals of theophylline with chiral and racemic forms of malic acid which are almost identical in molecular structure and supramolecular architecture. Similarly, the cocrystals of theophylline with chiral and racemic forms of tartaric acid, which are similar at the molecular level but dissimilar in crystal packing, were distinguished unequivocally. The investigation of the same cocrystals using X-ray powder diffraction and Raman spectroscopy suggested that THz-TDS is comparable in sensitivity to diffraction methods and more sensitive than Raman spectroscopy to changes in cocrystal architecture. The differences in spectra acquired by THz-TDS could be further enhanced by cooling the samples to 109 K.

Abstract: We demonstrate for the first time the closure of an electronic phase lock loop for a continuous–wave quantum cascade laser (QCL) at 1.5 THz. The QCL is operated in a closed cycle cryo cooler. We achieved a frequency stability of better than 100 Hz, limited by the resolution bandwidth of the spectrum analyser. The PLL electronics make use of the intermediate frequency (IF) obtained from a hot electron bolometer (HEB) which is downconverted to a PLL IF of 125 MHz. The coarse selection of the longitudinal mode and the fine tuning is achieved via the bias voltage of the QCL. Within a QCL cavity mode, the free-running QCL shows frequency fluctuations of about 5 MHz, which the PLL circuit is able to control via the Stark–shift of the QCL gain material. Temperature dependent tuning is shown to be nonlinear, and of the order of -16 MHz/K. Additionally we have used the QCL as local oscillator (LO) to pump an HEB and perform, again for the first time at 1.5 THz, a heterodyne experiment, and obtain a receiver noise temperature of 1741 K.

Abstract: We present the results of direct measurements of the temperature resolution of an HEB receiver operating at 810 GHz, in both continuum and spectroscopic modes. In the continuum mode, the input of the receiver was switched between black bodies with different physical temperatures. With a system noise temperature of around 1100 K, the receiver was able to resolve loads which differed in temperature by about 1 K over an integration time of 5 seconds. This resolution is significantly worse than the value of 0.07 K given by the radiometer equation. In the spectroscopic mode, a gas cell filled with carbonyl sulphide (OCS) gas was used and the emission line at 813.3537060 GHz was measured using the receiver in conjunction with a digital spectrometer. From the observed spectra, we determined that the measurement uncertainty of the equivalent emission temperature was 2.8 K for an integration time of 0.25 seconds and a spectral resolution of 12 MHz, compared to a 1.4 K temperature resolution given by the radiometer equation. This relative improvement is due to the fact that at short integration times the contribution from 1/f noise and drift are less dominant. In both modes, the temperature resolution was improved by about 40% with the use of a feedback loop which adjusted the level of an injected microwave radiation to maintain a constant operating current of the HEB mixer. This stabilization scheme has proved to be very effective to keep the temperature resolution of the HEB receiver to close to the theoretical value given by the radiometer equation.