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Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecular liquids, thus providing a promising probe of their local structure. However, the capabilities of these spectroscopies are still largely unexplored due to experimental limitations and inherently weak nonlinear signals. Here, through a combination of equilibrium-nonequilibrium molecular dynamics (MD) and a tailored spectrum decomposition scheme, we identify a relationship between the tetrahedral order of liquid water and its two-dimensional IR-IR-Raman (IIR) spectrum. The structure-spectrum relationship can explain the temperature dependence of the spectral features corresponding to the anharmonic coupling between low-frequency intermolecular and high-frequency intramolecular vibrational modes of water. In light of these results, we propose new experiments and discuss the implications for the study of tetrahedrality of liquid water. Direct spectroscopic probes of the impact of structure on dynamical processes in liquids remain scarce. Here, the authors use molecular dynamics simulations to show that the correlation between vibrational coupling and the local tetrahedral structure of liquid water can be studied via hybrid terahertz- and infrared-Raman spectroscopy.

We use the C/N ratio as a monitor of the delivery of key ingredients of life to nascent terrestrial worlds. Total elemental C and N contents, and their ratio, are examined for the interstellar medium, comets, chondritic meteorites, and terrestrial planets; we include an updated estimate for the bulk silicate Earth (C/N = 49.0 ± 9.3). Using a kinetic model of disk chemistry, and the sublimation/condensation temperatures of primitive molecules, we suggest that organic ices and macromolecular (refractory or carbonaceous dust) organic material are the likely initial C and N carriers. Chemical reactions in the disk can produce nebular C/N ratios of ∼1–12, comparable to those of comets and the low end estimated for planetesimals. An increase of the C/N ratio is traced between volatile-rich pristine bodies and larger volatile-depleted objects subjected to thermal/accretional metamorphism. The C/N ratios of the dominant materials accreted to terrestrial planets should therefore be higher than those seen in carbonaceous chondrites or comets. During planetary formation, we explore scenarios leading to further volatile loss and associated C/N variations owing to core formation and atmospheric escape. Key processes include relative enrichment of nitrogen in the atmosphere and preferential sequestration of carbon by the core. The high C/N bulk silicate Earth ratio therefore is best satisfied by accretion of thermally processed objects followed by large-scale atmospheric loss. These two effects must be more profound if volatile sequestration in the core is effective. The stochastic nature of these processes hints that the surface/atmospheric abundances of biosphere-essential materials will likely be variable. With the rapid pace at which exoplanets are being discovered, many efforts have now been dedicated to identifying which planets are expected to have the ingredients necessary for the development of life. In this work we explore the relative disposition of the essential elements carbon and nitrogen in each stage of star and planet formation, using the Earth and our solar system as grounding data. Our results suggest that planets like the Earth are readily supplied with these key elements, but their relative amounts on the surface and in the atmosphere will be highly variable.

Life on Earth relies on chiral molecules—that is, species not superimposable on their mirror images. This manifests itself in the selection of a single molecular handedness, or homochirality, across the biosphere. We present the astronomical detection of a chiral molecule, propylene oxide (CH₃CHCH₂O), in absorption toward the Galactic center. Propylene oxide is detected in the gas phase in a cold, extended molecular shell around the embedded, massive protostellar clusters in the Sagittarius B2 star-forming region. This material is representative of the earliest stage of solar system evolution in which a chiral molecule has been found.

Planets form in the disks around young stars. Their formation efficiency and composition are intimately linked to the protoplanetary disk locations of \"snow lines\" of abundant volatiles. We present chemical imaging of the carbon monoxide (CO) snow line in the disk around TW Hya, an analog of the solar nebula, using high spatial and spectral resolution Atacama Large Millimeter/Submillimeter Array observations of diazenylium (N 2 H + ), a reactive ion present in large abundance only where CO is frozen out. The N 2 H + emission is distributed in a large ring, with an inner radius that matches CO snow line model predictions. The extracted CO snow line radius of ∼30 astronomical units helps to assess models of the formation dynamics of the solar system, when combined with measurements of the bulk composition of planets and comets.

We present 2D terahertz-terahertz-Raman (2D TTR) spectroscopy, the first technique, to our knowledge, to interrogate a liquid with multiple pulses of terahertz (THz) light. This hybrid approach isolates nonlinear signatures in isotropic media, and is sensitive to the coupling and anharmonicity of thermally activated THz modes that play a central role in liquid-phase chemistry. Specifically, by varying the timing between two intense THz pulses, we control the orientational alignment of molecules in a liquid, and nonlinearly excite vibrational coherences. A comparison of experimental and simulated 2D TTR spectra of bromoform (CHBr₃), carbon tetrachloride (CCl₄), and dibromodichloromethane (CBr₂Cl₂) shows previously unobserved off-diagonal anharmonic coupling between thermally populated vibrational modes.

A drop in the ocean Earth's bulk composition is similar to that of a group of oxygen-poor meteorites called enstatite chondrites, thought to have formed in the early solar nebula. This leads to the suggestion that proto-Earth was dry, and that volatiles including water were delivered by asteroid and comet impacts. The deuterium-to-hydrogen (D/H) ratios measured in six Oort cloud comets are much higher than on Earth, however, apparently ruling out a dominant role for such bodies. Now the Herschel Space Telescope has been used to determine the D/H ratio in the Kuiper belt comet 103P/Hartley 2. The ratio is Earth-like, suggesting that this population of comets may have contributed to Earth's ocean waters. For decades, the source of Earth's volatiles, especially water with a deuterium-to-hydrogen ratio (D/H) of (1.558 ± 0.001) × 10 −4 , has been a subject of debate. The similarity of Earth’s bulk composition to that of meteorites known as enstatite chondrites 1 suggests a dry proto-Earth 2 with subsequent delivery of volatiles 3 by local accretion 4 or impacts of asteroids or comets 5 , 6 . Previous measurements in six comets from the Oort cloud yielded a mean D/H ratio of (2.96 ± 0.25) × 10 −4 . The D/H value in carbonaceous chondrites, (1.4 ± 0.1) × 10 −4 , together with dynamical simulations, led to models in which asteroids were the main source of Earth's water 7 , with ≤10 per cent being delivered by comets. Here we report that the D/H ratio in the Jupiter-family comet 103P/Hartley 2, which originated in the Kuiper belt, is (1.61 ± 0.24) × 10 −4 . This result substantially expands the reservoir of Earth ocean-like water to include some comets, and is consistent with the emerging picture of a complex dynamical evolution of the early Solar System 8 , 9 .

Icy bodies may have delivered the oceans to the early Earth, yet little is known about water in the ice-dominated regions of extrasolar planet-forming disks. The Heterodyne Instrument for the Far-Infrared on board the Herschel Space Observatory has detected emission lines from both spin isomers of cold water vapor from the disk around the young star TW Hydrae. This water vapor likely originates from ice-coated solids near the disk surface, hinting at a water ice reservoir equivalent to several thousand Earth oceans in mass. The water's ortho-to-para ratio falls well below that of solar system comets, suggesting that comets contain heterogeneous ice mixtures collected across the entire solar nebula during the early stages of planetary birth.

We quantified eight parent volatiles (H₂O, C₂H₆, HCN, CO, CH₃OH, H₂CO, C₂H₂, and CH₄) in the Jupiter-family comet Tempel 1 using high-dispersion infrared spectroscopy in the wavelength range 2.8 to 5.0 micrometers. The abundance ratio for ethane was significantly higher after impact, whereas those for methanol and hydrogen cyanide were unchanged. The abundance ratios in the ejecta are similar to those for most Oort cloud comets, but methanol and acetylene are lower in Tempel 1 by a factor of about 2. These results suggest that the volatile ices in Tempel 1 and in most Oort cloud comets originated in a common region of the protoplanetary disk.

Recent advances in the understanding of the chemical processes that occur during all stages of the formation of stars, from the collapse of molecular clouds to the assemblage of icy planetesimals in protoplanetary accretion disks, are reviewed. Observational studies of the circumstellar material within 100-10,000 AU of the young star with (sub)millimeter single-dish telescopes, millimeter interferometers, and ground-based as well as space-borne infrared observatories have only become possible within the past few years. Results are compared with detailed chemical models that emphasize the coupling of gas-phase and grain-surface chemistry. Molecules that are particularly sensitive to different routes of formation and that may be useful in distinguishing between a variety of environments and histories are outlined. In the cold, low-density prestellar cores, radicals and long unsaturated carbon chains are enhanced. During the cold collapse phase, most species freeze out onto the grains in the high-density inner region. Once young stars ignite, their surroundings are heated through radiation and/or shocks, whereupon new chemical characteristics appear. Evaporation of ices drives a \"hot core\" chemistry rich in organic molecules, whereas shocks propagating through the dense envelope release both refractory and volatile grain material, resulting in prominent SiO, OH, and H 2 O emission. The role of future instrumentation in further developing these chemical and temporal diagnostics is discussed.

The initial mass distribution in the solar nebula is a critical input to planet formation models that seek to reproduce today’s Solar System 1 . Traditionally, constraints on the gas mass distribution are derived from observations of the dust emission from disks 2 , 3 , but this approach suffers from large uncertainties in dust opacity and gas-to-dust ratio 2 . On the other hand, previous observations of gas tracers only probe surface layers above the bulk mass reservoir 4 . Here we present the first partially spatially resolved observations of the 13 C 18 O J  = 3–2 line emission in the closest protoplanetary disk, TW Hydrae, a gas tracer that probes the bulk mass distribution. Combining it with the C 18 O J  = 3–2 emission and the previously detected HD J  = 1–0 flux, we directly constrain the mid-plane temperature and optical depths of gas and dust emission. We report a gas mass distribution with radius, R , of 13 − 5 + 8 × ( R / 20 .5 au ) − 0.9 − 0.3 + 0.4  g cm −2 in the expected formation zone of gas and ice giants (5–21 au). We find that the mass ratio of total gas to millimetre-sized dust is 140 in this region, suggesting that at least 2.4 M ⊕ of dust aggregates have grown to centimetre sizes (and perhaps much larger). The radial distribution of gas mass is consistent with a self-similar viscous disk profile but much flatter than the posterior extrapolation of mass distribution in our own and extrasolar planetary systems. ALMA observations of TW Hydrae in the 13C18O J = 3–2 molecular line probe the mid-plane of the circumstellar disk where giant planets are expected to form. With other lines, the gas mass distribution, temperature and the gas-to-dust ratio are determined.