Frequency stabilization of a terahertz quantum-cascade laser to the Lamb dip of a molecular absorption line.

We demonstrate the frequency stabilization of a terahertz quantum-cascade laser (QCL) to the Lamb dip of the absorption line of a D2O rotational transition at 3.3809309 THz. To assess the quality of the frequency stabilization, a Schottky diode harmonic mixer is used to generate a downconverted QCL signal by mixing the laser emission with a multiplied microwave reference signal. This downconverted signal is directly measured by a spectrum analyzer showing a full width at half maximum of 350 kHz, which is eventually limited by high-frequency noise beyond the bandwidth of the stabilization loop.

Fiber-dispersive Raman spectrometer with single-photon sensitivity.

The two major challenges in Raman spectroscopy are the low intensity of spontaneous Raman scattering and often accompanying luminescence. We overcome these two issues with a novel fiber-dispersive Raman spectrometer utilizing pulsed excitation and a superconducting nanowire single-photon detector (SNSPD). By exploiting chromatic dispersion in the fiber material, we stretched propagation times of Raman photons and performed correlated measurements in the time domain, where the two emission processes, Raman scattering and luminescence, can be effectively separated. The spectrometer greatly benefits from SNSPD metrics, i.e. broad spectral sensitivity (from UV to near-IR wavelength range) on a single-photon level and high timing resolution (small timing jitter), which outperform those of competing avalanche single-photon detectors. The spectral resolution achievable with a fiber-dispersive spectrometer for the optimized components is estimated to be as good as 3 - 10 cm-1 over the Stokes shifted range up to 4400 cm-1 with an excitation wavelength of 785 nm and below 5 cm-1 covering the same range with an excitation wavelength of 532 nm.

Frequency and power stabilization of a terahertz quantum-cascade laser using near-infrared optical excitation.

We demonstrate a technique to simultaneously stabilize the frequency and output power of a terahertz quantum-cascade laser (QCL). This technique exploits frequency and power variations upon near-infrared illumination of the QCL with a diode laser. It does not require an external terahertz optical modulator. By locking the frequency to a molecular absorption line, we obtain a long-term (one-hour) linewidth of 260 kHz (full width at half maximum) and a root-mean-square power stability below 0.03%. With respect to the free-running case, this stabilization scheme improves the frequency stability by nearly two orders of magnitude and the power stability by a factor of three.

Wideband, high-resolution terahertz spectroscopy by light-induced frequency tuning of quantum-cascade lasers.

Near-infrared optical excitation enables wideband frequency tuning of terahertz quantum-cascade lasers. In this work, we demonstrate the feasibility of the approach for molecular laser absorption spectroscopy. We present a physical model which explains the observed frequency tuning characteristics by the optical excitation of an electron-hole plasma. Due to an improved excitation configuration as compared to previous work, we observe a single-mode continuous-wave frequency coverage of as much as 40 GHz for a laser at 3.1 THz. This represents, for the same device, a ten-fold improvement over the usually employed tuning by current. The method can be readily applied to a large class of devices.

Doppler-free spectroscopy with a terahertz quantum-cascade laser.

We report on the Doppler-free saturation spectroscopy of a molecular transition at 3.3 THz based on a quantum-cascade laser and an absorption cell in a collinear pump-probe configuration. A Lamb dip with a sub-Doppler linewidth of 170 kHz is observed for a rotational transition of HDO. We found that a certain level of external optical feedback is tolerable as long as the free spectral range of the external cavity is large compared to the width of the absorption line.

Intercomparison of far-infrared transmittance measurements.

We present the results of the first systematic "round-robin" comparison of far-infrared transmittance spectra measurements, which was performed by five laboratories and piloted by Physikalisch-Technische (PTB). The transmittance spectra of four different samples were measured by the participating laboratories in the 600 cm-1 to 10 cm-1 range (16.67 µm to 1000 µm) in a blind comparison. Different types of instruments, Fourier transform infrared (FT-IR) spectrometers of Michelson type and a laser radiation-based system were used for the transmittance measurements. FT-IR spectrometers are the most popular and commonly used instruments for the spectral characterization of materials in the infrared spectral range, and are well established for quantitative measurements in the mid- and near-infrared spectral ranges. However, obtaining quantitative transmittance measurements in the far-infrared spectral range by means of these instruments is challenging, because it involves weaker radiation sources, stronger diffraction effects, significant radiation originating from the sample itself and temperature gradients inside the spectrometer that may not be given proper consideration. Therefore, this comparison was initiated to test the actual capability of and identify problems with FT-IR transmittance measurements in this spectral region. We discuss the results and the possible reasons for the observed discrepancies.

Terahertz gas-phase spectroscopy: chemometrics for security and medical applications.

We describe a spectrometer consisting of a vector network analyzer, a gas absorption cell, and a quasi-optical bench that acquires terahertz spectra of gaseous substances and mixtures. We tested volatile organic compounds that are medical biomarkers or chemicals which can be found on the US Environment Protection Agency list of harmful substances. Absorption spectra at gas pressures between 10 Pa and 5000 Pa were recorded. A subsequent multivariate data analysis demonstrated excellent qualitative and quantitative identification of pure substances and complex mixtures. The applied multivariate algorithms are principal components analysis, partial least square regression and soft independent modelling of class analogy.

Si:P as a laboratory analogue for hydrogen on high magnetic field white dwarf stars.

Laboratory spectroscopy of atomic hydrogen in a magnetic flux density of 10(5) T (1 gigagauss), the maximum observed on high-field magnetic white dwarfs, is impossible because practically available fields are about a thousand times less. In this regime, the cyclotron and binding energies become equal. Here we demonstrate Lyman series spectra for phosphorus impurities in silicon up to the equivalent field, which is scaled to 32.8 T by the effective mass and dielectric constant. The spectra reproduce the high-field theory for free hydrogen, with quadratic Zeeman splitting and strong mixing of spherical harmonics. They show the way for experiments on He and H(2) analogues, and for investigation of He(2), a bound molecule predicted under extreme field conditions.

Frequency modulation spectroscopy with a THz quantum-cascade laser.

We report on a terahertz spectrometer for high-resolution molecular spectroscopy based on a quantum-cascade laser. High-frequency modulation (up to 50 MHz) of the laser driving current produces a simultaneous modulation of the frequency and amplitude of the laser output. The modulation generates sidebands, which are symmetrically positioned with respect to the laser carrier frequency. The molecular transition is probed by scanning the sidebands across it. In this way, the absorption and the dispersion caused by the molecular transition are measured. The signals are modeled by taking into account the simultaneous modulation of the frequency and amplitude of the laser emission. This allows for the determination of the strength of the frequency as well as amplitude modulation of the laser and of molecular parameters such as pressure broadening.

A compact, continuous-wave terahertz source based on a quantum-cascade laser and a miniature cryocooler.

We report on the development of a compact, easy-to-use terahertz radiation source, which combines a quantum-cascade laser (QCL) operating at 3.1 THz with a compact, low-input-power Stirling cooler. The QCL, which is based on a two-miniband design, has been developed for high output and low electrical pump power. The amount of generated heat complies with the nominal cooling capacity of the Stirling cooler of 7 W at 65 K with 240 W of electrical input power. Special care has been taken to achieve a good thermal coupling between the QCL and the cold finger of the cooler. The whole system weighs less than 15 kg including the cooler and power supplies. The maximum output power is 8 mW at 3.1 THz. With an appropriate optical beam shaping, the emission profile of the laser is fundamental Gaussian. The applicability of the system is demonstrated by imaging and molecular-spectroscopy experiments.

Impact of the contact metallization on the performance of photoconductive THz antennas.

Both AuGe based alloys and Ti/Au metal layer stacks are widely used as ohmic metal contacts for photoconductive THz antennas made of low temperature grown GaAs. Here, we present the first systematic comparison between these two metallization types. A series of antennas of both kinds is excited by femtosecond laser pulses and by the emission from two diode lasers, i.e. we test the structures as pulsed THz emitters and as photomixers. In both cases, coherent and incoherent detection schemes are employed. We find that the power emitted from the antennas with AuGe metallization is 50% higher than that of antennas with a Ti/Au metal layer. From a comparison with a photomixer model we conclude that the higher output power results from a lower contact resistance of the AuGe contacts leading to an increased current flow. However, Ti/Au contacts have a higher thermal stability which might be advantageous if high system stability is called for.

Stimulated terahertz stokes emission of silicon crystals doped with antimony donors.

Stimulated Stokes emission has been observed from silicon crystals doped by antimony donors when optically excited by radiation from a tunable infrared free electron laser. The photon energy of the emission is equal to the pump photon energy reduced by the energy of the intervalley transverse acoustic (TA) g phonon in silicon (approximately 2.92 THz). The emission frequency covers the range of 4.6-5.8 THz. The laser process occurs due to a resonant coupling of the 1s(E) and 1s(A1) donor states (separation approximately 2.97 THz) via the g-TA phonon, which conserves momentum and energy within a single impurity center.

A model describing stable coherent synchrotron radiation in storage rings.

We present a model describing high power stable broadband coherent synchrotron radiation (CSR) in the terahertz frequency region in an electron storage ring. The model includes distortion of bunch shape from the synchrotron radiation (SR), which enhances higher frequency coherent emission, and limits to stable emission due to an instability excited by the SR wakefield. It gives a quantitative explanation of several features of the recent observations of CSR at the BESSY II storage ring. We also use this model to optimize the performance of a source for stable CSR emission.

Brilliant, coherent far-infrared (THz) synchrotron radiation.

A new technology for generating steady state, brilliant, broadband, coherent, far-infrared (FIR) radiation in electron storage rings is presented, suitable for FIR spectroscopy. An FIR power increase of up to 100 000 compared to the normal, incoherent synchrotron radiation in the range of approximately 5 to approximately 40 cm(-1) could be achieved. The source is up to 1000 times more brillant compared to a standard Hg arc lamp. The coherent synchrotron radiation is produced in a "low alpha" optics mode of the synchrotron light source BESSY, by bunch shortening and non-Gaussian bunch deformation.

Steady-state far-infrared coherent synchrotron radiation detected at BESSY II.

At BESSY II it is demonstrated that far-infrared coherent synchrotron radiation (CSR) can be generated by a controlled, steady-state process at storage rings. As an indication for coherent emission, the radiated power grows with the square of the beam current. The spectrum was analyzed by an interferometer in the 1-mm to 0.3-mm wavelength range. The CSR was enhanced more than 3000 times above background; the incoherent radiation remained below the background level. Steady-state and bursting CSR were discriminated by time resolved analysis from micro seconds to seconds.