Absolute frequency referencing in the long wave infrared using a quantum cascade laser frequency comb.

Optical frequency combs (OFCs) based on quantum cascade lasers (QCLs) have transformed mid-infrared spectroscopy. However, QCL-OFCs have not yet been exploited to provide a broadband absolute frequency reference. We demonstrate this possibility by performing comb-calibrated spectroscopy at 7.7 µm (1305 cm-1) using a QCL-OFC referenced to a molecular transition. We obtain 1.5·10-10 relative frequency stability (100-s integration time) and 3·10-9 relative frequency accuracy, comparable with state-of-the-art solutions relying on nonlinear frequency conversion. We show that QCL-OFCs can be locked with sub-Hz-level stability to a reference for hours, thus promising their use as metrological tools for the mid-infrared.

Coherently-averaged dual comb spectrometer at 7.7†µm with master and follower quantum cascade lasers.

We demonstrate coherent averaging of the multi-heterodyne beat signal between two quantum cascade laser frequency combs in a master-follower configuration. The two combs are mutually locked by acting on the drive current to control their relative offset frequency and by radio-frequency extraction and injection locking of their intermode beat signal to stabilize their mode spacing difference. By implementing an analog common-noise subtraction scheme, a reduction of the linewidth of all heterodyne beat notes by five orders of magnitude is achieved compared to the free-running lasers. We compare stabilization and post-processing corrections in terms of amplitude noise. While they give similar performances in terms of signal-to-noise ratio, real-time processing of the stabilized signal is less demanding in terms of computational power. Lastly, a proof-of-principle spectroscopic measurement was performed, showing the possibility to reduce the amount of data to be processed by three orders of magnitude, compared to the free-running system.

The fingerprint of the 2018 drought in Europe on ground-based atmospheric CO2 measurements.

During the summer of 2018, a widespread drought developed over Northern and Central Europe. The increase in temperature and the reduction of soil moisture have influenced carbon dioxide (CO2) exchange between the atmosphere and terrestrial ecosystems in various ways, such as a reduction of photosynthesis, changes in ecosystem respiration, or allowing more frequent fires. In this study, we characterize the resulting perturbation of the atmospheric CO2 seasonal cycles. 2018 has a good coverage of European regions affected by drought, allowing the investigation of how ecosystem flux anomalies impacted spatial CO2 gradients between stations. This density of stations is unprecedented compared to previous drought events in 2003 and 2015, particularly thanks to the deployment of the Integrated Carbon Observation System (ICOS) network of atmospheric greenhouse gas monitoring stations in recent years. Seasonal CO2 cycles from 48 European stations were available for 2017 and 2018. Earlier data were retrieved for comparison from international databases or national networks. Here, we show that the usual summer minimum in CO2 due to the surface carbon uptake was reduced by 1.4 ppm in 2018 for the 10 stations located in the area most affected by the temperature anomaly, mostly in Northern Europe. Notwithstanding, the CO2 transition phases before and after July were slower in 2018 compared to 2017, suggesting an extension of the growing season, with either continued CO2 uptake by photosynthesis and/or a reduction in respiration driven by the depletion of substrate for respiration inherited from the previous months due to the drought. For stations with sufficiently long time series, the CO2 anomaly observed in 2018 was compared to previous European droughts in 2003 and 2015. Considering the areas most affected by the temperature anomalies, we found a higher CO2 anomaly in 2003 (+3 ppm averaged over 4 sites), and a smaller anomaly in 2015 (+1 ppm averaged over 11 sites) compared to 2018. This article is part of the theme issue 'Impacts of the 2018 severe drought and heatwave in Europe: from site to continental scale'.

Intermittent operation of QC-lasers for mid-IR spectroscopy with low heat dissipation: tuning characteristics and driving electronics.

Intermittent scanning for continuous-wave quantum cascade lasers is proposed along with a custom-built laser driver optimized for such operation. This approach lowers the overall heat dissipation of the laser by dropping its drive current to zero between individual scans and holding a longer pause between scans. This allows packaging cw-QCLs in TO­3 housings with built-in collimating optics, thus reducing cost and footprint of the device. The fully integrated, largely analog, yet flexible laser driver eliminates the need for any external electronics for current modulation, lowers the demands on power supply performance, and allows shaping of the tuning current in a wide range. Optimized ramp shape selection leads to large and nearly linear frequency tuning (>1.5 cm−1). Experimental characterization of the proposed scheme with a QCL emitting at 7.7 µm gave a frequency stability of 3.2×10−5 cm−1 for the laser emission, while a temperature dependence of 2.3×10−4 cm−1/K was observed when the driver electronics was exposed to sudden temperature changes. We show that these characteristics make the driver suitable for high precision trace gas measurements by analyzing methane absorption lines in the respective spectral region.

Fossil and biogenic CO2 from waste incineration based on a yearlong radiocarbon study.

We describe the first long-term implementation of the radiocarbon (¹4C) method to study the share of biogenic (%Bio C) and fossil (%Fos C) carbon in combustion CO2. At five Swiss incinerators, a total of 24 three-week measurement campaigns were performed over 1 year. Temporally averaged bag samples were analyzed for ¹4CO2 by accelerator mass spectrometry. Significant differences between the plants in the share of fossil CO2 were observed, with annual mean values from 43.4 ± 3.9% to 54.5 ± 3.1%. Variations can be explained by the waste composition of the respective plant. Based on our dataset, an average value of 48 ± 4%Fos C was determined for waste incineration in Switzerland. No clear annual trend in %Fos C was observed for four of the monitored incinerators, while one incinerator showed considerable variations, which are likely due to the separation and temporary storage of bulky goods.

Determination of biogenic and fossil CO(2) emitted by waste incineration based on (14)CO(2) and mass balances.

A field application of the radiocarbon ((14)C) method was developed to determine the ratio of biogenic vs. fossil CO(2) emissions from waste-to-energy plants (WTE). This methodology can be used to assign the Kyoto relevant share of fossil CO(2) emissions, which is highly relevant for emission budgets and emission trading. Furthermore, heat and electricity produced by waste incinerators might be labelled depending on the fossil or biogenic nature of the primary energy source. The method development includes representative on-site CO(2) absorption and subsequent release in the laboratory. Furthermore, a reference value for the (14)C content of pure biogenic waste (f(M,bio)) was determined as 1.130+/-0.038. Gas samples for (14)CO(2) analysis were taken at three WTEs during one month each. Results were compared to an alternative approach based on mass and energy balances. Both methods were in excellent agreement and indicated a fraction of biogenic CO(2) slightly above 50%.