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Emission spectra and diagnostic spectral features of a diverse range of ablated meteorite samples with a known composition are presented. We aim to provide a reference spectral dataset to improve our abilities to classify meteoroid composition types from meteor spectra observations. The data were obtained by ablating meteorite samples in high-enthalpy plasma wind tunnel facilities recreating conditions characteristic of low-speed meteors. Near-UV to visible-range (320 - 800 nm) emission spectra of 22 diverse meteorites captured by a high-resolution Echelle spectrometer were analyzed to identify the characteristic spectral features of individual meteorite groups. The same dataset captured by a lower-resolution meteor spectrograph was applied to compare the meteorite data with meteor spectra observations. Spectral modeling revealed that the emitting meteorite plasma was characterized by temperatures of 3700 - 4800 K, similar to the main temperature component of meteors. The studied line intensity variations were found to trace the differences in the original meteorite composition and thus can be used to constrain the individual meteorite classes. We demonstrate that meteorite composition types, including ordinary chondrites, carbonaceous chondrites, various achondrites, stony-iron and iron meteorites, can be spectrally distinguished by measuring relative line intensities of Mg I, Fe I, Na I, Cr I, Mn I, Si I, H I, CN, Ni I, and Li I. Additionally, we confirm the effect of the incomplete evaporation of refractory elements Al, Ti, and Ca, and the presence of minor species Co I, Cu I, and V I.

Deep reinforcement learning has successfully been applied for molecular discovery as shown by the Molecule Deep Q-network (MolDQN) algorithm. This algorithm has challenges when applied to optimizing new molecules: training such a model is limited in terms of scalability to larger datasets and the trained model cannot be generalized to different molecules in the same dataset. In this paper, a distributed reinforcement learning algorithm for antioxidants, called DA-MolDQN is proposed to address these problems. State-of-the-art bond dissociation energy (BDE) and ionization potential (IP) predictors are integrated into DA-MolDQN, which are critical chemical properties while optimizing antioxidants. Training time is reduced by algorithmic improvements for molecular modifications. The algorithm is distributed, scalable for up to 512 molecules, and generalizes the model to a diverse set of molecules. The proposed models are trained with a proprietary antioxidant dataset. The results have been reproduced with both proprietary and public datasets. The proposed molecules have been validated with DFT simulations and a subset of them confirmed in public "unseen" datasets. In summary, DA-MolDQN is up to 100x faster than previous algorithms and can discover new optimized molecules from proprietary and public antioxidants.

Fragments of small solar system bodies entering Earth's atmosphere have possibly been important contributors of organic compounds to the early Earth. The cyano radical (CN) emission from meteors is considered as potentially one of the most suitable markers of organic compounds in meteoroids, however, its detection in meteor spectra has been thus far unsuccessful. With the aim to improve our abilities to identify CN emission in meteor observations and use its spectral features to characterize the composition of incoming asteroidal meteoroids, we present a detailed analysis of CN emission from high-resolution spectra of 22 laboratory simulated meteors including ordinary, carbonaceous, and enstatite chondrites, as well as a large diversity of achondrites (i.e., ureilite, aubrite, lunar, martian, howardite, eucrite, and diogenite), mesosiderite, and iron meteorites. We describe the variations of CN emission from different classes of asteroidal meteor analogues, its correlation and time evolution relative to other major meteoroid components. We demonstrate that CN can be used as a diagnostic spectral feature of carbonaceous and carbon-rich meteoroids, while most ordinary chondrites show no signs of CN. Our results point out strong correlation between CN and H emission and suggest both volatile features are suitable to trace contents of organic matter and water molecules present within meteoroids. For the application in lower resolution meteor observations, we demonstrate that CN can be best recognized in the early stages of ablation and for carbon-rich materials by measuring relative intensity ratio of CN band peak to the nearby Fe I-4 lines.

Due to its high energy efficiency and environmental friendliness, solid-state cooling based on the barocaloric (BC) effect represents a promising alternative to traditional refrigeration technologies relying on greenhouse gases. Plastic crystals displaying orientational order-disorder solid-solid phase transitions have emerged among the most gifted materials on which to realize the full potential of BC solid-state cooling. However, a comprehensive understanding of the atomistic mechanisms on which order-disorder BC effects are sustained is still missing, and rigorous and systematic methods for quantitatively evaluating and anticipating them have not been yet established. Here, we present a computational approach for the assessment and prediction of BC effects in orientationally disordered materials that relies on atomistic molecular dynamics simulations and emulates quasi-direct calorimetric BC measurements. Remarkably, the proposed computational approach allows for a precise determination of the partial contributions to the total entropy stemming from the vibrational and molecular orientational degrees of freedom. Our BC simulation method is applied on the technologically relevant material CH$_{3}$NH$_{3}$PbI$_{3}$ (MAPI), finding giant BC isothermal entropy changes ($|\Delta S_{\rm BC}| \sim 10$ J K$^{-1}$ kg$^{-1}$) under moderate pressure shifts of $\sim 0.1$ GPa. Intriguingly, our computational analysis of MAPI reveals that changes in the vibrational degrees of freedom of the molecular cations, not their reorientational motion, have a major influence on the entropy change that accompanies the order-disorder solid-solid phase transition., Comment: 13 pages, 8 figures

In the pursuit of sustainable lubricant materials, the conversion of common organic molecules into graphitic material has been recently shown to effectively reduce friction of metallic interfaces. Aromatic molecules are perfect candidates due to their inertness and possibility to form carbon-based tribofilms. Among many promising possibilities, we selected a group of common aromatic compounds and we investigated their capability to reduce the adhesion of iron interface. Ab initio molecular dynamic simulations of the sliding interface show that hypericin, a component of St. John's wort, effectively separates the mating iron surfaces better than graphene. This phenomenon is due to the size of the molecule, the reactivity of the moieties at its edges and the possibility to stack several of these structures that can easily slide on top of each other. The decomposition of the lateral groups of hypericin observed in the dynamic simulations suggests that the clustering of several molecules is possible, offering innovative paths to lubricate sliding contacts with compounds not typically employed in tribology.

Molybdenum dithiocarbamates (MoDTCs) are lubricant additives very efficient in reducing the friction of steel and they are employed in a number of industrial applications. The functionality of these additives is ruled by the chemical interactions occurring at the buried sliding interface, which are of key importance for the improvement of the lubrication performance. Yet, these tribochemical processes are very difficult to monitor in real time. Ab initio molecular dynamics simulations are the ideal tool to shed light into such a complicated reactivity. In this work we perform ab initio simulations, both in static and tribological conditions, to understand the effect of surface oxidation on the tribochemical reactivity of MoDTC and we find that when the surfaces are covered by oxygen, the first dissociative steps of the additives are significantly hindered. Our preliminary tribological tests on oxidized steel discs support these results. Bare metallic surfaces are necessary for a stable adsorption of the additives, their quick decomposition, and the formation of a durable MoS$_2$ tribolayer. This work demonstrates the importance of the catalytic role of the substrate and confirms the full capability of the computational protocol in the pursuit of materials and compounds more efficient in reducing friction.

Context. The existence of meteor clusters has long since been a subject of speculation and so far only seven events have been reported, among which two involve less than five meteors, and three were seen during the Leonid storms. Aims. The 1995 outburst of Comet 73P/Schwassmann-Wachmann was predicted to result in a meteor shower in May 2022. We detected the shower, proved this to be the result of this outburst, and detected another meteor cluster during the same observation mission. Methods. The {\tau}-Herculids meteor shower outburst on 31 May 2022 was continuously monitored for 4 hours during an airborne campaign. The video data were analyzed using a recently developed computer-vision processing chain for meteor real-time detection. Results. We report and characterize the detection of a meteor cluster involving 38 fragments, detected at 06:48 UT for a total duration of 11.3 s. The derived cumulative size frequency distribution index is relatively shallow: s = 3.1. Our open-source computer-vision processing chain (named FMDT) detects 100% of the meteors that a human eye is able to detect in the video. Classical automated motion detection assuming a static camera was not suitable for the stabilized camera setup because of residual motion. Conclusions. From all reported meteor clusters, we crudely estimate their occurrence to be less than one per million observed meteors. Low heliocentric distance enhances the probability of such meteoroid self-disruption in the interplanetary space., Comment: 6 pqges, 5 figures

The hydrogen emission from meteors is assumed to originate mainly from the meteoroid composition, making it a potential tracer of H$_{2}$O molecules and organic compounds. H$\alpha$ line was previously detected in individual fireballs, but its variation in a larger meteor dataset and dependency on the dynamical origin and physical properties have not yet been studied. Here we investigate the relative intensity of H$\alpha$ within 304 meteor spectra observed by the AMOS network. We demonstrate that H$\alpha$ emission is favored in faster meteors ($v_i >>$ 30 km s$^{-1}$) which form the high-temperature spectral component. H$\alpha$ was found to be a characteristic spectral feature of cometary meteoroids with $\sim$ 92% of all meteoroids with detected H$\alpha$ originating from Halley-type and long-period orbits. Our results suggest that hydrogen is being depleted from meteoroids with lower perihelion distances (q $<$ 0.4 au). No asteroidal meteoroids with detected H emission were found. However, using spectral data from simulated ablation of different meteorite types, we show that H emission from asteroidal materials can occur, and apparently correlates with their water and organic matter content. Strongest H emission was detected from carbonaceous chondrites (CM and CV) and achondrites (ureilite and aubrite), while it was lacking in most ordinary chondrites. The detection of H$\alpha$ in asteroidal meteoroids could be used to identify meteoroids of carbonaceous or achondritic composition. Overall, our results suggest that H$\alpha$ emission correlates with the emission of other volatiles (Na and CN) and presents a suitable tracer of water and organic matter in meteoroids.

The fragmentation of two aerospace aluminum alloys is investigated in a ground testing facility including mechanical loads as occurring due to aerodynamic forces in a real atmospheric entry event at three trajectory points. The emission spectroscopic analysis shows that these materials fail after distinct alkali metal features are observed in the spectra. The two alloys feature characteristic emissions of the different alkali metals. The presence of lithium lines that have previously been exclusively attributed to battery failure in observation campaigns may be considered as a marker for aluminum breakup. This is particularly interesting for future entry observations because it allows a new insight into the structural failure processes of the demising spacecraft. The lack of emission of alloying elements points to these spectra being a candidate for the determination of spacecraft demise. The identification of such features in ground testing will allow a more certain identification of specific break-up events, Comment: submitted to Journal of Spacecraft and Rockets

Landau suggested that the low-temperature properties of metals can be understood in terms of long-lived quasiparticles with all complex interactions included in Fermi-liquid parameters, such as the effective mass $m^{\star}$. Despite its wide applicability, electronic transport in bad or strange metals and unconventional superconductors is controversially discussed towards a possible collapse of the quasiparticle concept. Here we explore the electrodynamic response of correlated metals at half filling for varying correlation strength upon approaching a Mott insulator. We reveal persistent Fermi-liquid behavior with pronounced quadratic dependences of the optical scattering rate on temperature and frequency, along with a puzzling elastic contribution to relaxation. The strong increase of the resistivity beyond the Ioffe-Regel-Mott limit is accompanied by a `displaced Drude peak' in the optical conductivity. Our results, supported by a theoretical model for the optical response, demonstrate the emergence of a bad metal from resilient quasiparticles that are subject to dynamical localization and dissolve near the Mott transition., Comment: Main part: 8 pages, 4 figures; Supplement: 8 pages, 11 figures

Canonical instanton theory is a widespread approach to describe the dynamics of chemical reactions in low temperature environments when tunneling effects become dominant. It is a semiclassical theory which requires locating classical periodic orbits on the upside-down potential energy surface, so-called instantons, and the computation of second order quantum corrections. The calculation of these corrections usually involves a matrix diagonalization. In this paper we present an alternative approach, which requires to solve only linear systems of equations involving sparse matrices. Furthermore, the proposed method provides a reliable and numerically stable way to obtain stability parameters in multidimensional systems, which are of particular interest in the context of microcanonical instanton theory.

Microcanonical instanton theory offers the promise of providing rate constants for chemical reactions including quantum tunneling of atoms over the whole temperature range. We discuss different rate expressions, which require the calculation of stability parameters of the instantons. The traditional way of obtaining these stability parameters is shown to be numerically unstable in practical applications. We provide three alternative algorithms to obtain such stability parameters for non-separable systems, i.e., systems in which the vibrational modes perpendicular to the instanton path couple to movement along the path. We show the applicability of our algorithms on two molecular systems: H$_2$ + OH $\rightarrow$ H$_2$O + H using a fitted potential energy surface and HNCO + H $\rightarrow$ NH$_2$CO using a potential obtained on-the-fly from density functional calculations.

The detected Na/Mg ratio in a sample of 17 Na-enhanced and Na-rich meteors is investigated based on obtained spectral, orbital and structural data. We utilize the meteor observations of the AMOS network obtained within a survey of medium-sized meteoroids supplemented by higher-resolution spectra observed on the Canary Islands. Ground-based meteor observations are then compared with high-resolution Echelle spectra of simulated ablation of known meteorite samples in a high-enthalpy plasma wind tunnel. It was found that most Na-enhanced and Na-rich spectra can be explained by the effect of low meteor speed related to low ablation temperatures and generally do not reflect real meteoroid composition. Spectra obtained by the laboratory experiment simulating low meteor speeds show corresponding Na-rich profiles irrespectively of the meteorite composition. We estimate that for an H-type ordinary chondrite with speed of $\approx$ 10 km/s, the Na line intensity is increased by a factor of 40 to 95. The dynamical analysis has revealed that all Na-rich meteors originated on Apollo-type orbits and exhibit consistent chondritic material strengths. For more clarity in the classification of Na-enhanced and Na-rich meteoroids, we propose new speed-dependent boundaries between the spectral classes. Real compositional Na enhancement was confirmed in five cometary meteoroids: two Perseids, an $\alpha$-Capricornid, $\nu$-Draconid and a sporadic. The two Na-enhanced Perseids were linked with increased material strength suggesting that the detected increase of volatile content has implications for the meteoroid structure.

The dimer Mott insulator $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ can be tuned into a metallic and superconducting state upon applying pressure of 1.5 kbar and more. We have performed dielectric spectroscopy measurements (7 kHz to 5 MHz) on $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$ single crystals as a function of temperature (down to $T=8$ K) and pressure (up to $p=4$ kbar). At ambient conditions, a relaxor-like dielectric behavior develops below 50 K that shifts toward lower temperatures as the crystal is pressurized. Interestingly, a second peak emerges in $\varepsilon_{1}(T)$ around $T=15$ K, which becomes strongly enhanced with pressure and is attributed to a small volume fraction of metallic puddles in the insulating host phase. When approaching the phase boundary, this peak diverges rapidly reaching $\varepsilon_{1} \approx 10^{5}$. Our dynamical mean-field theory calculations substantiate that the dielectric catastrophe at the Mott transition is not caused by closing the energy gap, but due to the spatial coexistence of correlated metallic and insulating regions. We discuss the percolative nature of the first-order Mott insulator-to-metal transition in all details.

The electronic properties of molecular conductors can be readily varied via physical or chemical pressure as it increases the bandwidth W; this enables crossing the Mott insulator-to-metal phase transition by reducing electronic correlations U/W. Here we introduce an alternative path by increasing the molecular orbitals when partially replacing sulfur by selenium in the constituting bis-(ethylenedithio)-tetrathiafulvalene (BEDT-TTF) molecules of the title compound. We characterize the tuning of the insulating quantum spin liquid state via a Mott transition to the metallic Fermi-liquid state by transport, dielectric, and optical measurements. At this first-order phase transition, metallic regions coexist in the insulating matrix leading to pronounced percolative effects most obvious in a strong enhancement of the dielectric constant at low temperatures.

The correlation-driven Mott transition is commonly characterized by a drop in resistivity across the insulator-metal phase boundary; yet, the complex permittivity provides a deeper insight into the microscopic nature. We investigate the frequency- and temperature-dependent dielectric response of the Mott insulator $\kappa$-(BEDT-TTF)$_{2}$-Cu$_2$(CN)$_3$ when tuning from a quantum spin liquid into the Fermi-liquid state by applying external pressure and chemical substitution of the donor molecules. At low temperatures the coexistence region at the first-order transition leads to a strong enhancement of the quasi-static dielectric constant $\epsilon_1$ when the effective correlations are tuned through the critical value. Several dynamical regimes are identified around the Mott point and vividly mapped through pronounced permittivity crossovers. All experimental trends are captured by dynamical mean-field theory of the single-band Hubbard model supplemented by percolation theory., Comment: 6 pages, 4 figures

We measured the optical reflectivity of the Dirac material Au$_{2}$Pb in a broad frequency range (30 - 48 000 cm$^{-1}$) for temperatures between 9 and 300 K. The optical conductivity, computed from the reflectivity, is dominated by free-carrier contributions from topologically trivial bulk bands at all temperatures. The temperature-independent total plasma frequency of these carriers is 3.9 $\pm$ 0.2 eV. Overall, optical response of Au$_{2}$Pb is typically metallic with no signs of localization and bad-metal behavior., Comment: 10 pages, IOP style

The optical properties of (001)-oriented NbP single crystals have been studied in a wide spectral range from 6 meV to 3 eV from room temperature down to 10 K. The itinerant carriers lead to a Drude-like contribution to the optical response; we can further identify two pronounced phonon modes and interband transitions starting already at rather low frequencies. By comparing our experimental findings to the calculated interband optical conductivity, we can assign the features observed in the measured conductivity to certain interband transitions. In particular, we find that transitions between the electronic bands spilt by spin-orbit coupling dominate the interband conductivity of NbP below 100 meV. At low temperatures, the momentum-relaxing scattering rate of the itinerant carriers in NbP is very small, leading to macroscopic characteristic length scales of the momentum relaxation of approximately 0.5 $\mu$m., Comment: 7.5 pages

Determining the source regions of meteorites is one of the major goals of current research in planetary science. Whereas asteroid observations are currently unable to pinpoint the source regions of most meteorite classes, observations of meteors with camera networks and the subsequent recovery of the meteorite may help make progress on this question. The main caveat of such an approach, however, is that the recovery rate of meteorite falls is low, implying that the meteoritic analogues of at least 80% of the observed falls remain unknown. Aims: Spectroscopic observations of bolides may have the potential to mitigate this problem by classifying the incoming material. Methods: To probe the use of spectroscopy to determine the meteoritic analogues of bolides, we collected emission spectra in the visible range (320-880nm) of five meteorite types (H,L,LL,CM,eucrite) acquired in atmospheric entry-like conditions in a plasma wind tunnel at the University of Stuttgart (Germany). A detailed spectral analysis including line identification and mass ratio determinations (Mg/Fe,Na/Fe) was subsequently performed on all spectra. Results: Spectroscopy, via a simple line identification, allows us to distinguish the main meteorite classes (chondrites, achondrites and irons) but does not have the potential to distinguish for example an H from a CM chondrite. Conclusions: The source location within the main belt of the different meteorite classes (H, L, LL, CM, etc.) should continue to be investigated via fireball observation networks. Spectroscopy of incoming bolides only marginally helps precisely classify the incoming material (iron meteorites only). To reach a statistically significant sample of recovered meteorites along with accurate orbits (>100) within a reasonable time frame (10-20 years), the optimal solution may be the spatial extension of existing fireball observation networks.

The Widom line identifies the locus in the phase diagram where a supercritical gas crosses over from gas-like to a more liquid-like behavior. A similar transition exists in correlated electron liquids, where the interplay of Coulomb repulsion, bandwidth and temperature triggers between the Mott insulating state and an incoherent conduction regime. Here we explore the electrodynamic response of three organic quantum spin liquids with different degrees of effective correlation, where the absence of magnetic order enables unique insight into the nature of the genuine Mott state down to the most relevant low-temperature region. Combining optical spectroscopy with pressure-dependent dc transport and theoretical calculations, we succeeded to construct a phase diagram valid for all Mott insulators on a quantitative scale. In the vicinity of the low-temperature phase boundary, we discover metallic fluctuations within the Mott gap, exhibiting enhanced absorption upon cooling that is not present in antiferromagnetic Mott insulators. Our findings reveal the phase coexistence region and Pomeranchuk-like anomaly of the Mott transition, previously predicted but never observed., Comment: Supplementary information after Acknowledgements

Electron-doped Eu(Fe$_{0.93}$Rh$_{0.07}$)$_2$As$_2$ has been systematically studied by high pressure investigations of the magnetic and electrical transport properties, in order to unravel the complex interplay of superconductivity and magnetism. The compound reveals an exceedingly broad re-entrant transition to the superconducting state between $T_{\rm{c,on}} = 19.8$ K and $T_{\rm{c,0}} = 5.2$ K due to a canted A-type antiferromagnetic ordering of the Eu$^{2+}$ moments at $T_{\rm{N}} = 16.6$ K and a re-entrant spin glass transition at $T_{\rm{SG}} = 14.1$ K. At ambient pressure evidences for the coexistence of superconductivity and ferromagnetism could be observed, as well as a magnetic-field-induced enhancement of the zero-resistance temperature $T_{\rm{c,0}}$ up to $7.2$ K with small magnetic fields applied parallel to the \textit{ab}-plane of the crystal. We attribute the field-induced-enhancement of superconductivity to the suppression of the ferromagnetic component of the Eu$^{2+}$ moments along the \textit{c}-axis, which leads to a reduction of the orbital pair breaking effect. Application of hydrostatic pressure suppresses the superconducting state around $14$ kbar along with a linear temperature dependence of the resistivity, implying that a non-Fermi liquid region is located at the boundary of the superconducting phase. At intermediate pressure, an additional feature in the resistivity curves is identified, which can be suppressed by external magnetic fields and competes with the superconducting phase. We suggest that the effect of negative pressure by the chemical Rh substitution in Eu(Fe$_{0.93}$Rh$_{0.07}$)$_2$As$_2$ is partially reversed, leading to a re-activation of the spin density wave., Comment: 11 pages, 13 figures

$\alpha$-(BEDT-TTF)$_2$I$_3$ is a prominent example of charge ordering among organic conductors. In this work we explore the details of transport within the charge-ordered as well as semimetallic phase at ambient pressure. In the high-temperature semimetallic phase, the mobilities and concentrations of both electrons and holes conspire in such a way to create an almost temperature-independent conductivity as well as a low Hall effect. We explain these phenomena as a consequence of a predominantly inter-pocket scattering which equalizes mobilities of the two types of charge carriers. At low temperatures, within the insulating charge-ordered phase two channels of conduction can be discerned: a temperature-dependent activation which follows the mean-field behavior, and a nearest-neighbor hopping contribution. Together with negative magnetoresistance, the latter relies on the presence of disorder. The charge-ordered phase also features a prominent dielectric peak which bears a similarity to relaxor ferroelectrics. Its dispersion is determined by free-electron screening and pushed by disorder well below the transition temperature. The source of this disorder can be found in the anion layers which randomly perturb BEDT-TTF molecules through hydrogen bonds., Comment: 10 pages, 7 figures, submitted to Physical Review B

We investigated transport, magnetotransport, and broadband optical properties of the half-Heusler compound YbPtBi. Hall measurements evidence two types of charge carriers: highly mobile electrons with a temperature-dependent concentration and low-mobile holes; their concentration stays almost constant within the investigated temperature range from 2.5 to 300 K. The optical spectra (10 meV - 2.7 eV) can be naturally decomposed into contributions from intra- and interband absorption processes, the former manifesting themselves as two Drude bands with very different scattering rates, corresponding to the charges with different mobilities. These results of the optical measurements allow us to separate the contributions from electrons and holes to the total conductivity and to implement a two-channel-conduction model for description of the magnetotransport data. In this approach, the electron and hole mobilities are found to be around 50000 and 10 cm$^{2}$/Vs at the lowest temperatures (2.5 K), respectively., Comment: 6 pages

The Mott insulator $\kappa$-(BEDT-TTF)$_2$Ag$_2$(CN)$_3$ forms a highly-frustrated triangular lattice of $S=1/2$ dimers with a possible quantum-spin-liquid state. Our experimental and numerical studies reveal the emergence of a slight charge imbalance between crystallographically inequivalent sites, relaxor dielectric response and hopping dc transport. In a broader perspective we conclude that the universal properties of strongly-correlated charge-transfer salts with spin liquid state are an anion-supported valence band and cyanide-induced quasi-degenerate electronic configurations in the relaxed state. The generic low-energy excitations are caused by charged domain walls rather than by fluctuating electric dipoles. They give rise to glassy dynamics characteristic of dimerized Mott insulators, including the sibling compound $\kappa$-(BEDT-TTF)$_2$Cu$_2$(CN)$_3$., Comment: 5 pages, 6 figures, submitted to Physical Review B Rapid Communications