Laboratoire Interdisciplinaire Carnot de Bourgogne

The HITRAN database is a compilation of molecular spectroscopic parameters. It was established in the early 1970s and is used by various computer codes to predict and simulate the transmission and emission of light in gaseous media (with an emphasis on terrestrial and planetary atmospheres). The HITRAN compilation is composed of five major components: the line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, experimental infrared absorption cross-sections (for molecules where it is not yet feasible for representation in a line-by-line form), collision-induced absorption data, aerosol indices of refraction, and general tables (including partition sums) that apply globally to the data. This paper describes the contents of the 2020 quadrennial edition of HITRAN. The HITRAN2020 edition takes advantage of recent experimental and theoretical data that were meticulously validated, in particular, against laboratory and atmospheric spectra. The new edition replaces the previous HITRAN edition of 2016 (including its updates during the intervening years). All five components of HITRAN have undergone major updates. In particular, the extent of the updates in the HITRAN2020 edition range from updating a few lines of specific molecules to complete replacements of the lists, and also the introduction of additional isotopologues and new (to HITRAN) molecules: SO, CH3F, GeH4, CS2, CH3I and NF3. Many new vibrational bands were added, extending the spectral coverage and completeness of the line lists. Also, the accuracy of the parameters for major atmospheric absorbers has been increased substantially, often featuring sub-percent uncertainties. Broadening parameters associated with the ambient pressure of water vapor were introduced to HITRAN for the first time and are now available for several molecules. The HITRAN2020 edition continues to take advantage of the relational structure and efficient interface available at www.hitran.org and the HITRAN Application Programming Interface (HAPI). The functionality of both tools has been extended for the new edition.

The HITRAN database is a compilation of molecular spectroscopic parameters. It was established in the early 1970s and is used by various computer codes to predict and simulate the transmission and emission of light in gaseous media (with an emphasis on terrestrial and planetary atmospheres). The HITRAN compilation is composed of five major components: the line-by-line spectroscopic parameters required for high-resolution radiative-transfer codes, experimental infrared absorption cross-sections (for molecules where it is not yet feasible for representation in a line-by-line form), collision-induced absorption data, aerosol indices of refraction, and general tables (including partition sums) that apply globally to the data. This paper describes the contents of the 2020 quadrennial edition of HITRAN. The HITRAN2020 edition takes advantage of recent experimental and theoretical data that were meticulously validated, in particular, against laboratory and atmospheric spectra. The new edition replaces the previous HITRAN edition of 2016 (including its updates during the intervening years). All five components of HITRAN have undergone major updates. In particular, the extent of the updates in the HITRAN2020 edition range from updating a few lines of specific molecules to complete replacements of the lists, and also the introduction of additional isotopologues and new (to HITRAN) molecules: SO, CH3F, GeH4, CS2, CH3I and NF3. Many new vibrational bands were added, extending the spectral coverage and completeness of the line lists. Also, the accuracy of the parameters for major atmospheric absorbers has been increased substantially, often featuring sub-percent uncertainties. Broadening parameters associated with the ambient pressure of water vapor were introduced to HITRAN for the first time and are now available for several molecules. The HITRAN2020 edition continues to take advantage of the relational structure and efficient interface available at www.hitran.org and the HITRAN Application Programming Interface (HAPI). The functionality of both tools has been extended for the new edition.

It is control that turns scientific knowledge into useful technology: in physics and engineering it provides a systematic way for driving a dynamical system from a given initial state into a desired target state with minimized expenditure of energy and resources. As one of the cornerstones for enabling quantum technologies, optimal quantum control keeps evolving and expanding into areas as diverse as quantum-enhanced sensing, manipulation of single spins, photons, or atoms, optical spectroscopy, photochemistry, magnetic resonance (spectroscopy as well as medical imaging), quantum information processing and quantum simulation. In this communication, state-of-the-art quantum control techniques are reviewed and put into perspective by a consortium of experts in optimal control theory and applications to spectroscopy, imaging, as well as quantum dynamics of closed and open systems. We address key challenges and sketch a roadmap for future developments.

We present a novel chemical database for gas-phase astrochemistry. Named the KInetic Database for Astrochemistry
\n(KIDA), this database consists of gas-phase reactions with rate coefficients and uncertainties that will be vetted
\nto the greatest extent possible. Submissions of measured and calculated rate coefficients are welcome, and will
\nbe studied by experts before inclusion into the database. Besides providing kinetic information for the interstellar
\nmedium, KIDA is planned to contain such data for planetary atmospheres and for circumstellar envelopes. Each
\nyear, a subset of the reactions in the database (kida.uva) will be provided as a network for the simulation of the
\nchemistry of dense interstellar clouds with temperatures between 10 K and 300 K. We also provide a code, named
\nNahoon, to study the time-dependent gas-phase chemistry of zero-dimensional and one-dimensional interstellar
\nsources.

This paper provides an update on research in the relatively new and fast-moving field of decadal climate prediction, and addresses the use of decadal climate predictions not only for potential users of such information but also for improving our understanding of processes in the climate system. External forcing influences the predictions throughout, but their contributions to predictive skill become dominant after most of the improved skill from initialization with observations vanishes after about 6–9 years. Recent multimodel results suggest that there is relatively more decadal predictive skill in the North Atlantic, western Pacific, and Indian Oceans than in other regions of the world oceans. Aspects of decadal variability of SSTs, like the mid-1970s shift in the Pacific, the mid-1990s shift in the northern North Atlantic and western Pacific, and the early-2000s hiatus, are better represented in initialized hindcasts compared to uninitialized simulations. There is evidence of higher skill in initialized multimodel ensemble decadal hindcasts than in single model results, with multimodel initialized predictions for near-term climate showing somewhat less global warming than uninitialized simulations. Some decadal hindcasts have shown statistically reliable predictions of surface temperature over various land and ocean regions for lead times of up to 6–9 years, but this needs to be investigated in a wider set of models. As in the early days of El Niño–Southern Oscillation (ENSO) prediction, improvements to models will reduce the need for bias adjustment, and increase the reliability, and thus usefulness, of decadal climate predictions in the future.

A combined experimental and theoretical study is reported on the vibrational properties of tenorite CuO and paramelaconite Cu4O3. The optically active modes have been measured by Raman scattering and infrared absorption spectroscopy. First-principles calculations have been carried out with the LDA+U approach to account for strong electron correlation in the copper oxides. The vibrational properties have been computed ab initio using the so-called direct method. Excellent agreement is found between the measured Raman and infrared peak positions and the calculated phonon frequencies at the Brillouin zone center, which allows the assignment of all prominent peaks of the Cu4O3 spectra. Through a detailed analysis of the displacement eigenvectors, it is shown that a close relationship exists between the Raman modes of CuO and Cu4O3.

Real-time access to the internal ultrafast dynamics of complex dissipative optical systems opens new explorations of pulse-pulse interactions and dynamic patterns. We present the first direct experimental evidence of the internal motion of a dissipative optical soliton molecule generated in a passively mode-locked erbium-doped fiber laser. We map the internal motion of a soliton pair molecule by using a dispersive Fourier-transform imaging technique, revealing different categories of internal pulsations, including vibrationlike and phase drifting dynamics. Our experiments agree well with numerical predictions and bring insights to the analogy between self-organized states of lights and states of the matter.

Platinum is the most versatile element in catalysis, but it is rare and its high price limits large-scale applications, for example in fuel-cell technology. Still, conventional catalysts use only a small fraction of the Pt content, that is, those atoms located at the catalyst's surface. To maximize the noble-metal efficiency, the precious metal should be atomically dispersed and exclusively located within the outermost surface layer of the material. Such atomically dispersed Pt surface species can indeed be prepared with exceptionally high stability. Using DFT calculations we identify a specific structural element, a ceria "nanopocket", which binds Pt(2+) so strongly that it withstands sintering and bulk diffusion. On model catalysts we experimentally confirm the theoretically predicted stability, and on real Pt-CeO2 nanocomposites showing high Pt efficiency in fuel-cell catalysis we also identify these anchoring sites.

The nonlinear Schrödinger equation (NLSE) is a central model of nonlinear science, applying to hydrodynamics, plasma physics, molecular biology and optics. The NLSE admits only few elementary analytic solutions, but one in particular describing a localized soliton on a finite background is of intense current interest in the context of understanding the physics of extreme waves. However, although the first solution of this type was the Kuznetzov-Ma (KM) soliton derived in 1977, there have in fact been no quantitative experiments confirming its validity. We report here novel experiments in optical fibre that confirm the KM soliton theory, completing an important series of experiments that have now observed a complete family of soliton on background solutions to the NLSE. Our results also show that KM dynamics appear more universally than for the specific conditions originally considered, and can be interpreted as an analytic description of Fermi-Pasta-Ulam recurrence in NLSE propagation.

Rare events of extremely high optical intensity are experimentally recorded at the output of a mode-locked fiber laser that operates in a strongly dissipative regime of chaotic multiple-pulse generation. The probability distribution of these intensity fluctuations, which highly depend on the cavity parameters, features a long-tailed distribution. Recorded intensity fluctuations result from the ceaseless relative motion and nonlinear interaction of pulses within a temporally localized multisoliton phase.

Chemical models used to study the chemical composition of the gas and the ices in the interstellar medium are based on a network of chemical reactions and associated rate coefficients. These reactions and rate coefficients are partially compiled from data in the literature, when available. We present in this paper kida.uva.2014, a new updated version of the kida.uva public gas-phase network first released in 2012. In addition to a description of the many specific updates, we illustrate changes in the predicted abundances of molecules for cold dense cloud conditions as compared with the results of the previous version of our network, kida.uva.2011.

Frequency combs are optical spectra composed of a set of discrete equally spaced lines. Such spectra can be generated by diverse sources such as mode-locked lasers, resonators, or electro-optic modulators. This last possibility has shown a growing interest in the recent years for its advantageous features in providing high repetition rates, intrinsic mutual coherence, or high power per comb lines. Moreover, applications of electro-optic modulator-based combs have flourished in fundamental physics, spectroscopy, or instrumental calibrations. In this paper, we present the most recent progresses made on frequency combs generated by electro-optic modulators, along with the applications where these combs have shown a particular interest.

Ultrashort optical pulses propagating in a dissipative nonlinear system can interact and bind stably, forming optical soliton molecules. Soliton molecules in ultrafast lasers are under intense research focus and present striking analogies with their matter molecules counterparts. The recent development of real-time spectral measurements allows probing the internal dynamics of an optical soliton molecule, mapping the dynamics of the pulses' relative separations and phases that constitute the relevant internal degrees of freedom of the molecule. The soliton-pair molecule, which consists of two strongly bound optical solitons, has been the most studied multi-soliton structure. We here demonstrate that two soliton-pair molecules can bind subsequently to form a stable molecular complex and highlight the important differences between the intra-molecular and inter-molecular bonds. The dynamics of the experimentally observed soliton molecular complexes are discussed with the help of fitting models and numerical simulations, showing the universality of these multi-soliton optical patterns.

Calcium silicate hydrate (C-S-H) is the main constituent of hydrated cement paste and determines its cohesive properties. Because of the environmental impact of cement industry, it is more and more common to replace a part of the clinker in cement by secondary cementitious materials (SCMs). These SCMs are generally alumina-rich and as a consequence some aluminum is incorporated into the C-S-H. This may have consequences on the cohesion and durability of the material, and it is thus of importance to know the amount and the location of Al in C-S-H and what the parameters are that control these features. The present paper reports the (29)Si and (27)Al MAS NMR analyses of well-characterized C-A-S-H samples (C-S-H containing Al). These samples were synthesized using an original procedure that successfully leads to pure C-A-S-H of controlled compositions in equilibrium with well-characterized solutions. The (27)Al MAS NMR spectra were quantitatively interpreted assuming a tobermorite-like structure for C-A-S-H to determine the aluminum location in this structure. For this purpose, an in-house written software was used which allows decomposing several spectra simultaneously using the same constrained spectral parameters for each resonance but with variable intensities. The hypothesis on the aluminum location in the C-A-S-H structure determines the proportion of each silicon site. Therefore, from the (27)Al NMR quantitative results and the chemical composition of each sample, the intensity of each resonance line in the (29)Si spectra was set. The agreement between the experimental and calculated (29)Si MAS NMR spectra corroborates the assumed C-A-S-H structure and the proposed Al incorporation mechanism. The consistency between the results obtained for all compositions provides another means to assess the assumptions on the C-A-S-H structure. It is found that Al substitutes Si mainly in bridging positions and moderately in pairing positions in some conditions. Al in pairing site is observed only for Ca/(Si+Al) ratios greater than 0.95 (equivalent to 4 mmol.L(-1) of calcium hydroxide). Finally, the results suggest that penta and hexa-coordinated aluminum are adsorbed on the sides of the C-A-S-H particles.

Rains of solitons constitute a class of nonlinear dynamics of dissipative soliton ensembles that we briefly reported in Opt. Express 17, 11776 (2009) from a fiber laser experiment. The existence of a relatively intense noisy background together with several tens of soliton pulses aggregated in a condensed soliton phase constitutes a necessary condition for their appearance. New soliton pulses form spontaneously from the background fluctuations and drift until they reach the condensed soliton phase. We here relate in detail the experimental conditions under which soliton rains manifest and their key features, describe related dynamics observed in their vicinity, and propose an explanation for soliton rain dynamics.

Spatiotemporal mode coupling in highly multimode physical systems permits new routes for exploring complex instabilities and forming coherent wave structures. We present here the first experimental demonstration of multiple geometric parametric instability sidebands, generated in the frequency domain through resonant space-time coupling, owing to the natural periodic spatial self-imaging of a multimode quasi-continuous-wave beam in a standard graded-index multimode fiber. The input beam was launched in the fiber by means of an amplified microchip laser emitting sub-ns pulses at 1064 nm. The experimentally observed frequency spacing among sidebands agrees well with analytical predictions and numerical simulations. The first-order peaks are located at the considerably large detuning of 123.5 THz from the pump. These results open the remarkable possibility to convert a near-infrared laser directly into a broad spectral range spanning visible and infrared wavelengths, by means of a single resonant parametric nonlinear effect occurring in the normal dispersion regime. As further evidence of our strong space-time coupling regime, we observed the striking effect that all of the different sideband peaks were carried by a well-defined and stable bell-shaped spatial profile.

The pioneering paper 'Optical rogue waves' by Solli et al (2007 Nature 450 1054) started the new subfield in optics. This work launched a great deal of activity on this novel subject. As a result, the initial concept has expanded and has been enriched by new ideas. Various approaches have been suggested since then. A fresh look at the older results and new discoveries has been undertaken, stimulated by the concept of 'optical rogue waves'. Presently, there may not by a unique view on how this new scientific term should be used and developed. There is nothing surprising when the opinion of the experts diverge in any new field of research. After all, rogue waves may appear for a multiplicity of reasons and not necessarily only in optical fibers and not only in the process of supercontinuum generation. We know by now that rogue waves may be generated by lasers, appear in wide aperture cavities, in plasmas and in a variety of other optical systems. Theorists, in turn, have suggested many other situations when rogue waves may be observed. The strict definition of a rogue wave is still an open question. For example, it has been suggested that it is defined as 'an optical pulse whose amplitude or intensity is much higher than that of the surrounding pulses'. This definition (as suggested by a peer reviewer) is clear at the intuitive level and can be easily extended to the case of spatial beams although additional clarifications are still needed. An extended definition has been presented earlier by N Akhmediev and E Pelinovsky (2010 Eur. Phys. J. Spec. Top. 185 1-4). Discussions along these lines are always useful and all new approaches stimulate research and encourage discoveries of new phenomena. Despite the potentially existing disagreements, the scientific terms 'optical rogue waves' and 'extreme events' do exist. Therefore coordination of our efforts in either unifying the concept or in introducing alternative definitions must be continued. From this point of view, a number of the scientists who work in this area of research have come together to present their research in a single review article that will greatly benefit all interested parties of this research direction. Whether the authors of this 'roadmap' have similar views or different from the original concept, the potential reader of the review will enrich their knowledge by encountering most of the existing views on the subject. Previously, a special issue on optical rogue waves (2013 J. Opt. 15 060201) was successful in achieving this goal but over two years have passed and more material has been published in this quickly emerging subject. Thus, it is time for a roadmap that may stimulate and encourage further research.

Considering the problem of the control of a two-state quantum system by an external field, we establish a general and versatile method allowing the derivation of smooth pulses which feature the properties of high fidelity, robustness, and low area. Such shaped pulses can be interpreted as a single-shot generalization of the composite pulse-sequence technique with a time-dependent phase.

The origin of the exceptionally high activity of (B, Ag)-codoped TiO(2) catalysts under solar-light irradiation has been investigated by XPS and (11)B solid-state NMR spectroscopy in conjunction with density functional theory (DFT) calculations. XPS experimental results demonstrated that a portion of the dopant Ag (Ag(3+)) ions were implanted into the crystalline lattice of (B, Ag)-codoped TiO(2) and were in close proximity to the interstitial B (B(int.)) sites, forming [B(int.)-O-Ag] structural units. In situ XPS experiments were employed to follow the evolution of the chemical states of the B and Ag dopants during UV-vis irradiation. It was found that the [B(int.)-O-Ag] units could trap the photoinduced electron to form a unique intermediate structure in the (B, Ag)-codoped TiO(2) during the irradiation, which is responsible for the photoinduced shifts of the B 1s and Ag 3d peaks observed in the in situ XPS spectra. Solid-state NMR experiments including (11)B triple-quantum and double-quantum magic angle spinning (MAS) NMR revealed that up to six different boron species were present in the catalysts and only the tricoordinated interstitial boron (T*) species was in close proximity to the substitutional Ag species, leading to formation of [T*-O-Ag] structural units. Furthermore, as demonstrated by DFT calculations, the [T*-O-Ag] structural units were responsible for trapping the photoinduced electrons, which prolongs the life of the photoinduced charge carriers and eventually leads to a remarkable enhancement in the photocatalytic activity. All these unprecedented findings are expected to be crucial for understanding the roles of B and Ag dopants and their synergistic effect in numerous titania-mediated photocatalytic reactions.

High- and ultrahigh-Q whispering-gallery mode resonators have the capability to trap photons by total internal reflection for a duration ranging from nanoseconds to milliseconds. These exceptionally long photon lifetimes enhance the light–matter interactions at all scales, namely at the electronic, molecular, and lattice levels. As a consequence, nonlinear photon scattering can be triggered with very low threshold powers, down to a few microwatts. The possibility to efficiently harness photon–photon interactions with a system optimizing size, weight, power, and cost constraints has created a new, quickly thriving research area in photonics science and technology. This topic is inherently cross-disciplinary, as it stands at the intersection of nonlinear and quantum optics, crystallography, optoelectronics, and microwave photonics. From a fundamental perspective, high-Q whispering-gallery mode resonators have emerged as an ideal platform to investigate light–matter interactions in nonlinear bulk materials. From an applied viewpoint, technological applications include time-metrology, aerospace engineering, coherent optical fiber communications, or nonclassical light generation, among others. The aim of this paper is to provide an overview of the most recent advances in this area, which is increasingly gaining importance in contemporary photonics.