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Volume 14 Issue 10, October 2022

Intermolecular Coulombic decay knows no bounds

During intermolecular Coulombic decay (ICD), photoexcited molecules relax while ionizing their neighbouring molecules. This is usually observed in weakly bound systems — such as clusters and hydrogen-bonded systems — because ICD is efficient when intermolecular interactions are active. Now Sajeev, Aravind and colleagues have shown that ICD can occur between unbound pyridine molecules excited at ambient-light intensities, implying that soft ionization could occur naturally in astrophysical environments that feature such molecules with π-electron systems. The cover depicts this process occurring.

See Barik et al.

Image: Hassan Tahini, ScienceBrush Design. Cover design: Tulsi Voralia


  • Decisions, decisions. There’s a lot to think about when moving on from a postdoctoral position and Shira Joudan takes us through the considerations that led to her ultimately taking a tenure-track position in a new city.

    • Shira Joudan


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News & Views

  • Aqueous organic redox flow batteries are promising for low-cost and large-scale energy storage, but the redox-active molecules they rely on degrade prematurely. Now, a facile electrochemical protocol to regenerate them has been proposed, resulting in extended battery lifetimes.

    • Antoni Forner-Cuenca
    News & Views
  • Amines with free N–H groups have long posed a tremendous challenge in transition metal-catalysed amination reactions. Now, use of a bidentate phosphorus ligand enables the palladium-catalysed oxidative amination of simple olefins with Lewis basic amines, with no prefunctionalization, forming both alkyl and aryl allylamines.

    • Logan E. Vine
    • Jennifer M. Schomaker
    News & Views
  • Quantitatively studying the partitioning of biomolecules and reaction equilibria in cellular systems is an enormous challenge. Now, a multiphase coacervate model system provides insight into this complex biological problem, illustrating how coexisting phases influence RNA partitioning and duplex dissociation.

    • Shuqi Wu
    • Liangfei Tian
    News & Views
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  • Intermolecular Coulombic decay (ICD) is a process whereby a photoexcited molecule relaxes while ionizing a neighbouring molecule. ICD is efficient when intermolecular interactions are active and consequently it is usually observed in weakly bound systems. Now, an efficient ICD is shown to occur even between unbound pyridine molecules excited at ambient-light intensities.

    • Saroj Barik
    • Saurav Dutta
    • G. Aravind
  • Aqueous organic redox flow batteries offer a safe and inexpensive solution to the problem of storing electricity produced from intermittent renewables. However, decomposition of the redox-active organic molecules that they rely on limits their lifetimes, preventing commercialization. Now it has been shown that these redox molecules can be electro-recomposed in situ, rejuvenating their function.

    • Yan Jing
    • Evan Wenbo Zhao
    • Michael J. Aziz
  • The biochemical roles and mechanisms of multiphase membraneless organelles are not yet well understood. Now, multiphase peptide droplets have been shown to sort RNA based on whether it is single- or double-stranded, as well as impact RNA duplexation through in-droplet thermodynamic equilibria. This work provides insight into possible primitive mechanisms for multicompartment intracellular condensates and can aid in the design of functional artificial membraneless organelles.

    • Saehyun Choi
    • McCauley O. Meyer
    • Christine D. Keating
  • Given the importance of amine compounds, methods for their synthesis continue to be in high demand. Now, a palladium-catalysed strategy has been developed for the selective oxidative amination of unactivated olefins with Lewis basic amines, via C(sp3)–H activation, forming architecturally versatile and functionally diverse allylamines in a single step.

    • Yangbin Jin
    • Yaru Jing
    • Huanfeng Jiang
  • The influence that liquid environments have on the ultrafast excited-state dynamics of molecules is poorly understood. Using time-resolved photoelectron spectroscopy, the dynamics of the photoisomerization of stilbene in the gas and liquid phases have now been shown to be qualitatively similar—including the observation of vibrational coherences—but the timescales are significantly longer in the liquid phase.

    • Chuncheng Wang
    • Max D. J. Waters
    • Hans Jakob Wörner
  • The β1-adrenergic receptor (β1AR) contains empty cavities in its preactive conformation, which disappear in the active one. Now, using X-ray crystallography of xenon-derivatized β1AR crystals, a cavity has been shown to be in contact with the cholesterol-binding pocket. Monitoring the binding of a cholesterol analogue in solution has explained the function of cholesterol as a negative allosteric modulator of β1AR.

    • Layara Akemi Abiko
    • Raphael Dias Teixeira
    • Stephan Grzesiek
  • The apparent disconnect between prebiotic aldehyde-based Strecker synthesis of amino acids and the α-ketoacid-based metabolism of extant biochemistry necessitates an evolutionary switch between these disparate chemistries. Now it has been shown that Bucherer–Bergs reactions of α-ketoacids produce α-amino acids and dihydroorotate, paralleling the biochemical synthesis of orotate and suggesting a more congruent evolutionary pathway from cyanide-based chemistries.

    • Sunil Pulletikurti
    • Mahipal Yadav
    • Ramanarayanan Krishnamurthy
  • Although neutral and anionic low-valent aluminium complexes are widespread, their cationic counterparts have remained rare. Now, a salt of [Al(AlCp*)3]+ featuring a formal low-valent Al+ cation has been isolated that dimerizes in concentrated solutions and the solid state, and also forms Al4 clusters on coordinating with Lewis bases.

    • Philipp Dabringhaus
    • Julie Willrett
    • Ingo Krossing
  • Supramolecular interactions play an essential role in organic electronic materials and biological systems. Now, it has been demonstrated that the σ–σ stacking interactions between neighbouring non-conjugated molecules can offer an efficient pathway for charge transport through supramolecular junctions, which provides a new guideline for the design and fabrication of organic materials and devices.

    • Anni Feng
    • Yu Zhou
    • Wenjing Hong
  • Most proteins must fold co-translationally on the ribosome to adopt biologically active conformations, yet structural, mechanistic descriptions are lacking. Using 19F NMR spectroscopy to study a nascent multi-domain protein has now enabled the identification of two co-translational folding intermediates that are significantly more stable than intermediates formed off the ribosome, suggesting that the ribosome may thermodynamically regulate folding.

    • Sammy H. S. Chan
    • Tomasz Włodarski
    • John Christodoulou
    Article Open Access
  • The majority of methods to prepare β-amino acid derivatives require metal-mediated multistep manipulations of pre-functionalized substrates. Now, a metal-free, energy-transfer enabled, highly regioselective aminocarboxylation reaction has been developed, for the single-step installation of both amine and ester functionalities into alkenes or (hetero)arenes. An oxime oxalate ester is used as a bifunctional reagent, supplying C-centred ester and N-centred iminyl radicals.

    • Guangying Tan
    • Mowpriya Das
    • Frank Glorius
  • Butafulvene is a constitutional isomer of benzene, comprising a cyclobutene skeleton bearing two exocyclic conjugated methylene units. Strategies for the synthesis of butafulvene compounds are currently limited due to its intrinsic high strain energy and anti-aromaticity. Now, palladium-catalysed couplings have been developed for the rapid assembly of symmetric and non-symmetric anti-aromatic butafulvene derivatives.

    • Xin Huang
    • Bing-Zhi Chen
    • Shengming Ma
  • In silico chemical prediction of a polyketide synthase gene cluster in the bacterium Gynuella sunshinyii has led to the discovery of a class of natural products called janustatins. The absolute configuration of the stereocentres in these compounds was determined by a combination of techniques including DFT calculations and 2D NMR experiments—and finally confirmed by total synthesis. Janustatins were found to cause delayed, synchronized cell death at subnanomolar concentrations.

    • Reiko Ueoka
    • Philipp Sondermann
    • Jörn Piel
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In Your Element

  • Madison Knapp and Jennifer Bridwell-Rabb explore the functions of chlorophyll and explain how our understanding of this green pigment has changed over time.

    • Madison Knapp
    • Jennifer Bridwell-Rabb
    In Your Element
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