Chemical physics articles within Nature Chemistry

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  • News & Views |

    Surface heterogeneities lead to friction between droplets and solid surfaces, limiting the performance of the latter in a number of applications. A combination of friction force measurements and atomistic molecular dynamics simulations now sheds light on the influence of molecular scale heterogeneities on droplet friction.

    • Abhinav Naga
    •  & Doris Vollmer

  • Article |

    The design of open-shell nanographenes is commonly limited to systems featuring a single magnetic origin. Now a strategy that combines topological frustration and electron–electron interactions has been developed to generate a butterfly-shaped nanographene that hosts four highly entangled π-spins and exhibits both ferromagnetic and anti-ferromagnetic coupling.

    • Shaotang Song
    • , Andrés Pinar Solé
    •  & Jiong Lu

  • Article
    | Open Access

    Light-induced ultrafast switching between the molecular isomers norbornadiene and quadricyclane can reversibly store and release a substantial amount of chemical energy. Two competing pathways have now been identified by which electronically excited quadricyclane molecules relax to the electronic ground state, facilitating interconversion between the two isomers on different timescales.

    • Kurtis D. Borne
    • , Joseph C. Cooper
    •  & Daniel Rolles

  • Article
    | Open Access

    Single-atom alloys have emerged as highly active and selective catalysts that do not follow the traditional models of heterogeneous catalysis. Now it has been shown that the binding of adsorbates at their surface abides by a simple 10-electron count rule, which can identify promising catalysts for various applications.

    • Julia Schumann
    • , Michail Stamatakis
    •  & Romain Réocreux

  • Article |

    Light-induced azobenzene cis/trans isomerization has been extensively investigated, but the mechanical strength of its cis/trans structure is not well understood. Now it has been shown that cis azobenzene is mechanically less stable than the trans isomer due to its regiochemical structure, as revealed by single-molecule force spectroscopy.

    • Yiran Li
    • , Bin Xue
    •  & Yi Cao

  • Article |

    While aromaticity is a useful concept for assessing the reactivity of organic compounds, the connection between aromaticity and on-surface chemistry remains largely unexplored. Now, scanning probe experiments on cyclization reactions of porphyrins on Au(111) show that the peripheral carbon atoms outside of the aromatic 18-π electron pathway exhibit a higher reactivity.

    • Nan Cao
    • , Jonas Björk
    •  & Alexander Riss

  • Article |

    Wavepacket dynamics around conical intersections are influenced by geometric phase, which can affect chemical reaction outcomes but has only been observed through indirect signatures. Now, by engineering a controllable conical intersection in a trapped-ion quantum simulator, the destructive wavepacket interference caused by a geometric phase has been observed.

    • C. H. Valahu
    • , V. C. Olaya-Agudelo
    •  & I. Kassal

  • Article |

    Geometric phase interference has been predicted to appear around conical intersections but has been experimentally illusive owing to competing effects in molecular systems. Now, this effect has been demonstrated in chains of trapped ions using state-of-the-art quantum simulation and read-out techniques.

    • Jacob Whitlow
    • , Zhubing Jia
    •  & Kenneth R. Brown

  • Article |

    While chiral hybrid organic–inorganic perovskites are promising materials for optoelectronic applications, the synthesis of three-dimensional single crystals has proven challenging. Now, a general strategy has been shown to synthesize chiral, three-dimensional perovskites by heterogeneous nucleation. The single-crystalline materials contain no chiral component; their chiroptical activity arises from supercells formed by chiral patterns of the A-site cations.

    • Gaoyu Chen
    • , Xiaoyu Liu
    •  & Xun Wang

  • Research Briefing |

    Despite advances, understanding of the quantum state-to-state scattering dynamics between charged ions and neutral molecules at low collision energies remains limited. A high-resolution crossed-beam experiment with quantum state-selected ions prepared by laser photoionization and supporting trajectory surface-hopping calculations now provides insight into the quantum state-to-state collisional dynamics of a model charge-transfer reaction.

  • Article |

    Visualizing single-molecule reactions using electron microscopy can be difficult because of potential radiation damage from the electron beam. Now, however, it has been shown that a high-energy electron beam can be used to synthesize metallo-azafullerenes. Atomic-resolution, time-resolved transmission electron microscopy, with the help of computational calculations, is used to monitor the metal-encapsulation dynamics.

    • Helen Hoelzel
    • , Sol Lee
    •  & Dominik Lungerich

  • Article |

    Exciton–exciton annihilation is conventionally assumed to be limited by diffusion. Now, using time-resolved photoluminescence microscopy to determine exciton diffusion constants and annihilation rates in two substituted perylene diimide aggregates, along with a microscopic model, it has been shown that annihilation can be suppressed through quantum interference of the spatial phase of delocalized excitons.

    • Sarath Kumar
    • , Ian S. Dunn
    •  & Libai Huang

  • Article |

    Trihydrogen cations are abundant in interstellar space and play a vital role in both star and organic molecule formation. Now it has been shown that D3+ cations can be directly produced through photoionization of molecular D2–D2 dimers.

    • Yonghao Mi
    • , Enliang Wang
    •  & André Staudte

  • Article
    | Open Access

    Protein solutions can undergo liquid–liquid phase separation, by condensing into a dense phase that often resembles liquid droplets, which coexist with a dilute phase. Now it is shown that hydrophobic interactions, specifically at interfaces, can trigger a liquid–solid phase separation of a protein solution.

    • Daria Maltseva
    • , Sayantan Chatterjee
    •  & Mischa Bonn

  • Article |

    In situ chirality identification for single-molecule systems is not a straightforward task. Now, real-time chirality identification during a Michael addition reaction has been realized by continuous measurements of spin-polarized currents through a single-molecule junction, providing a promising method for studying symmetry-breaking reactions.

    • Chen Yang
    • , Yanwei Li
    •  & Xuefeng Guo

  • News & Views |

    An organic quantum magnet has been prepared in short chains of porphyrin derivatives through a combination of on-surface synthesis and atom manipulation using the tip of a scanning probe microscope.

    • P. Jelínek

  • Article |

    The transition state, a transient species where bond transformation occurs, fundamentally controls reaction dynamics. This important species can be probed through the photodetachment of an anionic precursor, as has now been shown in the F + NH3 reaction. A combination of theory and experiment reveals resonances that span the transition state.

    • Mark C. Babin
    • , Martin DeWitt
    •  & Daniel M. Neumark

  • News & Views |

    The study of rare isotopes, including many in the f-block, is a key step to advancing our fundamental understanding of these elements, but their scarcity poses challenges. Now, minute amounts of such materials have been isolated and characterized through complexation with polyoxometalate clusters.

    • Kristina O. Kvashnina

  • Article |

    Quantum nanomagnets, which display collective quantum behaviours, serve as important components in modern quantum technologies, but their fabrication has remained challenging. Quantum nanomagnets have now been constructed spin by spin in metal-free porphyrin chains, using on-surface synthesis and hydrogen manipulation using a scanning tunnelling microscope, and their collective quantum behaviours have been clearly resolved.

    • Yan Zhao
    • , Kaiyue Jiang
    •  & Shiyong Wang

  • Article |

    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

  • News & Views |

    How electric fields generated by enzyme active sites push and pull on substrates is important to their chemistry, but measuring them is difficult. Now, the electric field within an active site has been measured along two directions using a vibrational probe, revealing that the field effect in enzymes is different compared with that in bulk solvents.

    • Anuj Pennathur
    •  & Jahan Dawlaty

  • Article
    | Open Access

    Ions in salt solutions perturb the hydrogen bonding between the surrounding water molecules, altering the properties of water, but how ion polarity affects this is not fully understood. By monitoring the dissipation of terahertz energy in salt solutions, it has now been shown that intermolecular rotational-to-translational energy transfer is enhanced by highly charged cations and reduced by highly charged anions.

    • Vasileios Balos
    • , Naveen Kumar Kaliannan
    •  & Mohsen Sajadi

  • Article |

    HCN and its isomer HNC are both observed in the interstellar medium and inelastic collisions with helium and other species strongly influence their derived abundances. Now it has been shown experimentally and theoretically that HNC is much more strongly excited than HCN in collisions with helium at the low temperatures of interstellar space.

    • Brian M. Hays
    • , Divita Gupta
    •  & Ian R. Sims

  • Article |

    The collision dynamics between a pair of aligned molecules in the presence of a scattering resonance provide the most sensitive probe of the long-range anisotropic forces important to chemistry. By simultaneously controlling the collision temperature and geometry between a pair of aligned D2 molecules, we unravel the anisotropic dynamics of a cold scattering process.

    • Haowen Zhou
    • , William E. Perreault
    •  & Richard N. Zare

  • News & Views |

    Electron spin relaxation, important in quantum information science, can be slowed down at clock transitions — which are insensitive to magnetic noise. It has now been shown that such transitions can be tuned, to high frequency, in rare-earth coordination complexes through control of s- and d-orbital mixing.

    • Eric J. L. McInnes

  • Article |

    Influencing the products of a reaction through controlling the state of the reactants is a notable goal for chemists. It has now been shown that the reactivity of a pair of Fermi-coupled vibrational states of CH3D(v1-I and v1-II) with a chlorine atom depends not only on the constituent basis modes, but also on the relative phase of the two modes in their wave-functions.

    • Huilin Pan
    •  & Kopin Liu

  • Article |

    Molecular energy transfer is thought to follow a simple rule of thumb: high energy transfer requires hard collisions that result in backscattering. However, now it has been observed that an unexpected forward scattering occurs in NO–CO and NO–HD collisions even for high energy transfer. This is attributed to ‘hard-collision glory scattering’, a mechanism that appears to be ubiquitous in molecule–molecule collisions.

    • Matthieu Besemer
    • , Guoqiang Tang
    •  & Tijs Karman

  • Article |

    The s-orbital mixing into the spin-bearing d orbital associated with a molecular Lu(II) complex is shown to both reduce spin–orbit coupling and increase electron–nuclear hyperfine interactions, which substantially improves electron spin coherence. Combined with the potential to tune interactions through coordination chemistry, it makes this system attractive for quantum information applications.

    • Krishnendu Kundu
    • , Jessica R. K. White
    •  & Stephen Hill

  • News & Views |

    Why do bulky anions solubilize macromolecules in water but precipitate out the corresponding monomers? The answer lies in the differences in local water structure. Polymers have now been shown to disrupt water structure more than their monomers, leading to an accumulation of anions near the polymers that increases their solubility.

    • Aniket U. Thosar
    •  & Amish J. Patel

  • Article |

    Aromatic systems that interact non-covalently are important in many settings, such as base-pair stacking and DNA–drug interactions; however, their excited-state molecular dynamics are not fully understood. Now, intermolecular Coulombic decay in benzene dimers has been observed. The process is initiated by electron-impact ionization and proceeds through ultrafast energy transfer between the benzene molecules.

    • Xueguang Ren
    • , Jiaqi Zhou
    •  & Alexander Dorn

  • Article |

    Electron spin resonance spectroscopy has traditionally been used to study large ensembles of spins, but its combination with scanning tunnelling microscopy recently enabled measurements on single adatoms. Now, individual iron phthalocyanine complexes adsorbed on a surface have been probed. Their spin distribution partially extends on the phthalocyanine, leading to a strong geometry-dependent exchange coupling interaction.

    • Xue Zhang
    • , Christoph Wolf
    •  & Taeyoung Choi

  • News & Views |

    Charged nanoparticles can behave as large ions or as small colloids. Their interaction with multivalent ions has now been shown to reflect this dichotomy, providing new paths to large, self-assembled nanoparticle superstructures.

    • Tobias Kraus

  • News & Views |

    Excited anion states provide doorways for molecular electron capture. Now, two-dimensional photoelectron spectroscopy of cluster anions has been shown to be a powerful tool for revealing the role of the local environment in facilitating the process.

    • C. Annie Hart
    •  & Richard Mabbs

  • Article |

    Although electron-driven chemistry is ubiquitous, how molecular electron capture is altered by solvent remains poorly understood. Now, using anion two-dimensional photoelectron spectroscopy, it is shown that the presence of water molecules can enhance electron capture and that considering the mechanism from the perspective of the anion offers further understanding.

    • Aude Lietard
    • , Golda Mensa-Bonsu
    •  & Jan R. R. Verlet

  • News & Views |

    Controlling reactions between molecules is a major fundamental goal in chemistry and doing so on the level of individual quantum states is very challenging. Now, control over the reactant state and full characterization of the product-state distribution of an ultracold bimolecular reaction has been demonstrated.

    • Andreas Osterwalder

  • Article |

    Analysis of the thermodynamics of protein–N-glycan interactions perturbed by mutations has revealed an enthalpy–entropy compensation that depends on the electronics of the interacting side chains. Machine-learned and statistical models showed that protein–N-glycan interactions highly correlate with stereoelectronic effects, and that a major part of protein–N-glycan interactions can be explained using the energetic rules of frontier molecular orbital interactions.

    • Maziar S. Ardejani
    • , Louis Noodleman
    •  & Jeffery W. Kelly

  • Article |

    Reactions at the interface between water and other phases play important roles in various chemical settings. Now, ultrafast phase-sensitive interface-selective vibrational spectroscopy has revealed that the photoionization of phenol can occur four orders of magnitude faster at the water surface than in the bulk aqueous phase.

    • Ryoji Kusaka
    • , Satoshi Nihonyanagi
    •  & Tahei Tahara

  • Article |

    Energy scrambling in intermediate complexes—which form in many chemical reactions—presents a major challenge to state-to-state control. However, nuclear spin tends to remain unchanged throughout reactions and now, by manipulating the reactants’ nuclear spins using an external magnetic field, control over the product state distribution of a bimolecular reaction has been demonstrated.

    • Ming-Guang Hu
    • , Yu Liu
    •  & Kang-Kuen Ni

  • Article |

    Low-temperature scattering leads to the formation of quantum resonances or quasi-bound states, which are observable as peaks in the measured collision cross-sections. Now it has been shown that two different formation mechanisms, quantum tunnelling and quantum reflection, can be distinguished by measuring and comparing elastic and inelastic scattering, which probe the spatial localization of the resonance wavefunctions.

    • Prerna Paliwal
    • , Nabanita Deb
    •  & Edvardas Narevicius

  • Article |

    Scattering experiments in which two beams nearly co-propagate allow broadly tunable collision energies and can enable cold collisions. Now, such experiments have been combined with the preparation of NO molecules using stimulated emission to generate highly vibrationally excited states for state-to-state scattering studies, testing the theoretical gold standard in a regime not found in nature.

    • Chandika Amarasinghe
    • , Hongwei Li
    •  & Arthur G. Suits

  • Article |

    The broad infrared spectrum of water in the OH stretching region shows how significantly a water molecule is distorted when within a hydrogen-bonding network; it also raises the question of what the spectrum of a single OH oscillator would be. Now, the spectral signatures of isolated OH oscillators embedded in cold water cages have been measured using vibrational spectroscopy.

    • Nan Yang
    • , Chinh H. Duong
    •  & Mark A. Johnson

  • Article |

    Quantum coherence and dephasing in molecular motions determine the behaviour of many chemical reactions and are the fundamental basis for the concept of coherent control. Now, ultrafast X-ray scattering combined with a detailed structural determination analysis precisely measures the coherent vibrational motions of a polyatomic organic molecule following photoexcitation.

    • Brian Stankus
    • , Haiwang Yong
    •  & Peter M. Weber

  • News & Views |

    Light is often used to trigger reactions, energetically exciting the reactant(s) to kick them over the intrinsic reaction barrier. Now, however, the reaction between an excited atom and a charged molecule at very low temperatures has been shown not to adhere to this paradigm, instead undergoing a reaction blockading effect.

    • Roland Wester

  • News & Views |

    Intersystem crossing plays a role in the mechanism of many reactive collisions between atomic species and organic molecules, and has been generally observed when the reactants are still approaching one another. Now, intersystem crossing has been observed to also occur after their initial interaction.

    • Luis Bañares

  • Article |

    Intersystem crossing (ISC) is a radiationless process that is important in many photophysical systems. It has now been observed to take place in the exit channel for the reaction of ground-state atomic oxygen with alkylamines.

    • Hongwei Li
    • , Alexander Kamasah
    •  & Arthur G. Suits

  • News & Views |

    Magnetic or electric fields have long been used to align or orient atomic or molecular species in a molecular beam. Now, experiments in a merged beam apparatus show that an external magnetic field can be used to favour one particular reaction path.

    • Astrid Bergeat
    •  & Christian Naulin

  • Article |

    Steric effects in a fundamental energy-transfer reaction at collision energies from over 1,000 K down to 20 mK have now been studied. At high energies a pronounced dependence of the reactivity on the reactant orientation is observed, but this effect is not present at the lowest energies because of dynamic reorientation.

    • Sean D. S. Gordon
    • , Juan J. Omiste
    •  & Andreas Osterwalder

  • Article |

    Measurements of vector correlations provide insight into the forces acting during molecular collisions, and are a stringent test of electronic-structure calculations. Now, non-intuitive dynamics of molecular collisions have been revealed by measuring the correlation between the relative velocities of the colliders and the molecular rotational angular momentum—before and after the collision—for NO(A 2Σ+) + Ne.

    • Thomas R. Sharples
    • , Joseph G. Leng
    •  & Matthew L. Costen

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