Energy transfer articles within Nature Chemistry

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  • Research Briefing |

    Radiation damage in biological systems by radicals and low-energy electrons formed from water ionization is a consequence of ultrafast processes that follow core-level ionization of hydrated metal ions. More details of the complex pathway are now revealed from the study of aluminium-ion relaxation through sequential electron-transfer-mediated decay.

  • News & Views |

    Scientists have been studying how polymers break in solutions for decades, but the mechanism by which chains are stretched to the point of covalent bond scission is not trivial. Now, an experiment series provides ample support for a dynamic model in which chains uncoil from end to middle, while concurrently relaxing.

    • Charles E. Diesendruck

  • Article |

    Quantum state-to-state understanding of collisional charge transfer is a long-time goal of chemical dynamics. Now, using high-resolution molecular-beam experiments with spin–orbit state-selected ions and surface-hopping calculations, a vibrational-state-specific mechanism has been observed for the reaction Ar+(2P3/2) + N2 → Ar + N2+(v′, J′). Besides the well-known long-range harpooning mechanism, a hard-collision glory scattering mechanism was also identified.

    • Guodong Zhang
    • , Dandan Lu
    •  & Hong Gao

  • Article |

    Hybrid structures made up of quantum dots functionalized with molecules are highly tunable platforms for light-driven applications; however, the interaction between their components is often weak. Now it has been shown that by connecting molecules to silicon quantum dots via p-conjugated tethers, strongly coupled exciton states can be generated that prove advantageous for photon upconversion.

    • Kefu Wang
    • , R. Peyton Cline
    •  & Ming Lee Tang

  • Article
    | Open Access

    Inelastic hydrogen atom scattering from surfaces provides a good benchmark for the validity of the Born–Oppenheimer approximation in surface chemistry. Now it has been shown that hydrogen atoms colliding with a semiconductor surface can efficiently excite electrons above the surface bandgap, representing a clear example of the failure of the approximation.

    • Kerstin Krüger
    • , Yingqi Wang
    •  & Oliver Bünermann

  • Article |

    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

  • 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 |

    Low-energy NO–He collisions have been studied and scattering resonances observed. By rotationally exciting NO before the collision, a controlled amount of angular momentum was added and its release in de-excitation collisions was monitored—additional quantum waves were imprinted in the angular distributions of the scattering products.

    • Tim de Jongh
    • , Quan Shuai
    •  & Sebastiaan Y. T. van de Meerakker

  • Article |

    In photosynthesis, photoenergy transfers through chromophore-containing proteins, which exhibit thermal fluctuations that change the positions of the chromophores. Now the ultrafast dynamics in allophycocyanin—a cyanobacterial light-harvesting protein—have been measured using single-molecule pump–probe spectroscopy. The data show that energy transfer precedes protein-induced photophysical heterogeneity, ensuring that light harvesting is robust to the heterogeneity.

    • Raymundo Moya
    • , Audrey C. Norris
    •  & Gabriela S. Schlau-Cohen

  • 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

  • News & Views |

    Transition metal complexes with metal-to-ligand charge transfer (MLCT) luminescence and photoactivity typically rely on precious metals such as ruthenium or iridium. Now, two complexes of the Earth-abundant 3d manganese have displayed room-temperature MLCT luminescence in solution and a unique excited-state reactivity.

    • Katja Heinze

  • Article |

    Manganese(i) is isoelectronic to iron(ii) but has typically been overlooked as a cheap Earth-abundant metal for the development of 3d6 metal-to-ligand charge transfer (MLCT) emitters and photosensitizers. Now, using chelating isocyanide ligands, air-stable manganese(i) complexes have been obtained that exhibit MLCT luminescence, as well as energy- and electron-transfer photoreactivity.

    • Patrick Herr
    • , Christoph Kerzig
    •  & Oliver S. Wenger

  • News & Views |

    Energy transfer from one molecule to another over a distance of nanometres is a fundamental process of widespread relevance. Now, scanning probe techniques have been used to include an intermediary third molecule and to watch how energy flows through it.

    • Klaus Kuhnke

  • Article |

    Energy funnelling within multichromophoric assemblies is key to the conversion of solar energy by plants. Now, energy transport between phthalocyanine-based chromophores has been monitored at the submolecular level using scanning tunnelling microscopy, focusing on the role of ancillary, passive and blocking chromophores in promoting and directing energy transfer between distant donor and acceptor units.

    • Shuiyan Cao
    • , Anna Rosławska
    •  & Guillaume Schull

  • Article |

    Quantum dots functionalized with energy-accepting dyes hold promise for converting low-energy photons into higher-energy visible light for bioimaging, catalysis and solar energy harvesting. Now, it has been shown that non-toxic silicon quantum dots can be used in these systems; the transfer of spin-triplet excitons to molecules at their surface has been observed.

    • Pan Xia
    • , Emily K. Raulerson
    •  & Sean T. Roberts

  • 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

  • Article |

    Although ubiquitous throughout chemistry and biology, the structure and transport mechanism of the aqueous proton in solution remain elusive. Through advances in ultrafast broadband 2D IR spectroscopy, the structure of the aqueous proton is revealed to have a charge-delocalized H5O2+ Zundel-like core arrangement with surprisingly persistent structural heterogeneity.

    • Joseph A. Fournier
    • , William B. Carpenter
    •  & Andrei Tokmakoff

  • News & Views |

    Molecular vibrations can be highly effective promoters of gas-phase chemistry. Now, measurements show that excited vibrational states can survive on metal surfaces far longer than expected — reshaping our understanding of how vibrational excitation might also promote or modify heterogeneously catalysed chemistry on metals.

    • Arthur L. Utz

  • Article |

    The implications of coherence signals for the transfer of energy within the Fenna–Matthews–Olson complex of photosynthetic green sulfur bacteria is a well debated topic. Now, polarization-controlled 2D spectroscopy — aided by vibronic exciton modelling — has enabled the characterization of all such coherences and determination of their physical origins; while electronic coherences dephase extremely rapidly, ground- and excited-state vibrational coherences dominate.

    • Erling Thyrhaug
    • , Roel Tempelaar
    •  & Donatas Zigmantas

  • Article |

    Collision-induced spin–orbit transitions involve multiple interaction potentials and are by nature non-adiabatic, complicating both their experimental and theoretical study. Crossed-beam experiments and non-Born–Oppenheimer quantum calculations for inelastic collisions of carbon atoms with helium atoms, down to energies corresponding to temperatures below 10 K, have now been performed. Quantum-dynamical resonances predicted by theory were experimentally detected.

    • Astrid Bergeat
    • , Simon Chefdeville
    •  & François Lique

  • Article |

    The vibrational relaxation of molecules adsorbed at metal surfaces is considered to be relatively fast and thus examples of vibrationally induced chemistry at surfaces are rare. The adsorption and subsequent desorption of long-lived vibrationally excited CO molecules from a gold surface have now been observed, suggesting that vibrational promotion of surface chemistry might be more prevalent than currently thought.

    • Pranav R. Shirhatti
    • , Igor Rahinov
    •  & Alec M. Wodtke

  • Article |

    Collisions between atoms and molecules are largely understood; however, our understanding of collisions between two molecules is lacking because they are significantly harder to study, Now, correlated rotational excitations have been observed in inelastic collisions between NO and O2 molecules. It is shown that the energy-gap law that governs atom–molecule collisions does not generally apply to bimolecular excitation processes.

    • Zhi Gao
    • , Tijs Karman
    •  & Sebastiaan Y. T. van de Meerakker

  • Article |

    Singlet fission may one day allow solar cells to produce two excited electrons with one photon. Now, by comparison of the time-resolved photoluminescence and sensitized triplet–triplet annihilation of a tetracene derivative, it has been shown that—contrary to previous reports—the excimer state is a trap, and not a necessary intermediate for singlet fission.

    • Cameron B. Dover
    • , Joseph K. Gallaher
    •  & Timothy W. Schmidt

  • Article |

    Singlet fission — the splitting of a singlet exciton into two triplets — is a process that could be exploited to improve the power conversion efficiency of solar cells. Spectroscopic data now suggest that coherent and incoherent mechanisms for singlet fission in crystalline hexacene coexist and occur on different timescales.

    • Nicholas R. Monahan
    • , Dezheng Sun
    •  & X.-Y. Zhu

  • Article |

    Stereodynamics describes how the vector properties of molecules affect the probabilities of specific processes in molecular collisions. Measurements of irregular diffraction patterns for NO radicals colliding with rare-gas atoms reveal a previously unrecognized type of quantum stereodynamics and a ‘propensity rule’ for the magnetic quantum number (m) of the molecules.

    • Jolijn Onvlee
    • , Sean D. S. Gordon
    •  & Sebastiaan Y. T. van de Meerakker

  • Article |

    Difficulties in experimentally achieving simultaneous structural sensitivity and time resolution have hindered the real-time mapping of the vibrational energy relaxation pathways in biomacromolecules. Now, using ultrashort light pulses to locally deposit excess energy in a protein-bound haem, the temporal evolution of the subsequent energy flow has been monitored, unravelling vibrational couplings that lead to mode-specific temperature changes.

    • C. Ferrante
    • , E. Pontecorvo
    •  & T. Scopigno

  • Article |

    Effective light capture in photosynthetic organisms depends on the efficiency of all energy-transfer steps in the photosynthetic unit. Two-dimensional electronic spectroscopy has now been used on intact cells in situ to reveal and characterize the functional connectivity between individual complexes in the photosynthetic apparatus of green sulfur bacteria.

    • Jakub Dostál
    • , Jakub Pšenčík
    •  & Donatas Zigmantas

  • Article |

    Metal centres play an important role in the damage to biomolecules caused by radiation, but the respective microscopic mechanisms are unknown. Now it is shown that the absorption of X-rays by a metal ion leads to an intricate chain of ultrafast relaxation steps that results in the complete degradation of the metal's local environment.

    • V. Stumpf
    • , K. Gokhberg
    •  & L. S. Cederbaum

  • Article |

    Singlet fission, a spin-allowed conversion of a spin-singlet state into a pair of spin-triplet excitons, may be useful for the development of next-generation photovoltaics. Ultrafast coherence measurements now show that vibrational motions play a critical role in fission as they facilitate the mixing of triplet-pair states with singlet excitons.

    • Artem A. Bakulin
    • , Sarah E. Morgan
    •  & Akshay Rao

  • Article |

    Long-lived molecular collision complexes — or ‘resonances’ — are difficult to identify experimentally. Now crossed-beam experiments and quantum calculations are reported for rotationally inelastic CO−He collisions at energies corresponding to temperatures as low as 4 K. Quantum dynamical resonances that are predicted by theory were detected and fully characterized.

    • Astrid Bergeat
    • , Jolijn Onvlee
    •  & Michel Costes

  • Article |

    Understanding the process of exciton fission, which occurs in certain organic materials, could lead to the development of more efficient photovoltaic devices. Here, an expression derived from first principles is used to accurately characterize the singlet fission rate of a wide array of materials, reproducing a transition from weak to strong coupling as a function of molecular separation.

    • Shane R. Yost
    • , Jiye Lee
    •  & Troy Van Voorhis

  • Article |

    When molecules collide with atoms or other molecules their quantum mechanical character can lead to the diffraction of matter waves. Making use of advances in molecular beam technology, such diffraction oscillations have now been observed with unprecedented sharpness and angular resolution in the benchmark NO + He, Ne, or Ar systems.

    • Alexander von Zastrow
    • , Jolijn Onvlee
    •  & Sebastiaan Y. T. van de Meerakker

  • News & Views |

    Radiation of sufficient energy can knock out a tightly bound core-electron from the inner shell of a water molecule, leaving behind a short-lived, highly excited state. Now, through electron spectroscopy and theoretical simulations, these states have been observed to undergo previously unconsidered proton-mediated processes in solution.

    • Lars G. M. Pettersson

  • Article |

    Previously unobserved types of reactive species formed on the core ionization of liquid water have been identified using a combination of liquid microjet photoemission spectroscopy and ab initio calculations. The charge-separated di-cationic species are formed within a few femtoseconds, through proton-transfer-mediated processes followed by autoionization.

    • Stephan Thürmer
    • , Milan Ončák
    •  & Bernd Winter

  • Article |

    Quantum beating has been observed in photosynthetic systems, suggesting that energy-transfer processes in natural light harvesting could involve quantum effects. Now, extensive beating is found in the light-harvesting protein of a cryptophyte alga, and shown to be electronic. The implications of these observations on the free-energy surfaces and exciton delocalization were investigated.

    • Cathy Y. Wong
    • , Richard M. Alvey
    •  & Gregory D. Scholes

  • Article |

    At water's surface, its network of hydrogen-bonds is abruptly interrupted, conferring distinct properties on interfacial water from bulk water. Understanding aqueous interfaces is essential for many environmental, technological and biophysical systems, and now the pathways and rates of energy transfer at the water/air interface are elucidated using a surface-specific ultrafast spectroscopic technique.

    • Zhen Zhang
    • , Lukasz Piatkowski
    •  & Mischa Bonn

  • Article |

    The flow of vibrational energy into reactants and out of products plays a critical role in nearly every chemical reaction. Here, a time-resolved ultrafast microscopic map of energy flow is provided for a thermal bimolecular chemical reaction that takes place in dichloromethane, a typical organic solvent.

    • David R. Glowacki
    • , Rebecca A. Rose
    •  & Jeremy N. Harvey

  • Review Article |

    Photosynthesis starts when light is absorbed and the associated excitation energy is directed to reaction centres by antenna complexes. The principles learned from studying these complexes are described in this Review, and provide the framework from which the authors suggest how to elucidate strategies for designing light-harvesting systems that route the flow of energy in sophisticated ways.

    • Gregory D. Scholes
    • , Graham R. Fleming
    •  & Rienk van Grondelle

  • News & Views |

    The collision of an atom and a diatomic molecule may sound like a simple process but it has long been studied to understand the inherent intricacies of collisional energy transfer. Now, experiments carried out in unprecedented detail on the scattering of NO by Ar have revealed further complexity: parity-dependent quantum interference effects.

    • David W. Chandler

  • Article |

    Differential cross sections for the rotationally inelastic scattering of NO by Ar are reported with unprecedented quantum-state resolution. The experiments give important details about the mechanism of this fundamental collisional process, providing evidence for a parity-dependent quantum-mechanical interference effect.

    • C. J. Eyles
    • , M. Brouard
    •  & S. Stolte

  • News & Views |

    There is a long history of gas-phase studies of bimolecular reactions, but the presence of surrounding molecules complicates analogous studies in solution. Now, advances in ultrafast laser technology have enabled the detailed study of vibrational energy release in a reaction in solution.

    • F. Fleming Crim

  • News & Views |

    Photosynthesis in plants converts energy from the Sun into chemical fuel in the form of glucose. Now, a strategy to combine carbon dioxide reduction and photochemical water splitting, using a recyclable hydrogen donor, offers the opportunity to develop non-biomimetic photosynthesis.

    • Josef Michl

  • News & Views |

    Controlled energy-transfer on a molecular scale is a goal in many areas of science, from artificial photosynthesis to molecular electronics. Now, DNA origami has been used to direct the transfer of energy from an excited input dye down one of two paths by precisely arranging a mediator dye.

    • Bo Albinsson

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