The idea of using ultrashort X-ray pulses to obtain images of single proteins frozen in time has fascinated and inspired many.It was one of the arguments for building X-ray free-electron lasers.According to theory,the...The idea of using ultrashort X-ray pulses to obtain images of single proteins frozen in time has fascinated and inspired many.It was one of the arguments for building X-ray free-electron lasers.According to theory,the extremely intense pulses provide sufficient signal to dispense with using crystals as an amplifier,and the ultrashort pulse duration permits capturing the diffraction data before the sample inevitably explodes.This was first demonstrated on biological samples a decade ago on the giant mimivirus.Since then,a large collaboration has been pushing the limit of the smallest sample that can be imaged.The ability to capture snapshots on the timescale of atomic vibrations,while keeping the sample at room temperature,may allow probing the entire conformational phase space of macromolecules.Here we show the first observation of an X-ray diffraction pattern from a single protein,that of Escherichia coli GroEL which at 14 nm in diameter is the smallest biological sample ever imaged by X-rays,and demonstrate that the concept of diffraction before destruction extends to single proteins.From the pattern,it is possible to determine the approximate orientation of the protein.Our experiment demonstrates the feasibility of ultrafast imaging of single proteins,opening the way to single-molecule time-resolved studies on the femtosecond timescale.展开更多
Unraveling the exact nature of nonequilibrium and correlated interactions is paramount for continued progress in many areas of condensed matter science. Such insight is a prerequisite to develop an engineered approach...Unraveling the exact nature of nonequilibrium and correlated interactions is paramount for continued progress in many areas of condensed matter science. Such insight is a prerequisite to develop an engineered approach for smart materials with targeted properties designed to address standing needs such as efficient light harvesting, energy storage, or information processing. For this goal, it is critical to unravel the dynamics of the energy conversion processes between carriers in the earliest time scales of the excitation dynamics. We discuss the implementation and benefits of attosecond soft x-ray core-level spectroscopy up to photon energies of 600 eV for measurements in solid-state systems. In particular, we examine how the pairing between coherent spectral coverage and temporal resolution provides a powerful new insight into the quantum dynamic interactions that determine the macroscopic electronic and optical response. We highlight the different building blocks of the methodology and point out the important aspects for its application from condensed matter studies to materials as thin as 25 nm. Furthermore, we discuss the technological developments in the field of tabletop attosecond soft x-ray sources with time-resolved measurements at the near and extended edge simultaneously and investigate the exciting prospective of extending such technique to the study of 2-dimensional materials.展开更多
基金supported by the Universität Hamburg and DFG grant numbers(INST 152/772-1|152/774-1|152/775-1|152/776-1|152/777-1 FUGG)We acknowledge the support of funding from:Cluster of Excellence‘CUI:Advanced Imaging of Matter’of the Deutsche Forschungsgemeinschaft(DFG)-EXC 2056-project ID 390715994+7 种基金ERC-2013-CoG COMOTION 614507NFR 240770Fellowship from the Joachim Herz Stiftung(P.L.X.)P.L.X.and H.N.C.acknowledge support from the Human Frontiers Science Program(RGP0010/2017)J.H.acknowledges support from the European Development Fund:Structural dynamics of biomolecular systems(ELIBIO)(CZ.02.1.01/0.0/0.0/15_003/0000447)EMBO long-term fellowship(ALTF 356-2018)awarded to L.E.F.the Röntgen-Ångström Cluster(2015-06107 and 2019-06092)the Swedish Research Council(2017-05336,2018-00234 and 2019-03935)the Swedish Foundation for Strategic Research(ITM17-0455).
文摘The idea of using ultrashort X-ray pulses to obtain images of single proteins frozen in time has fascinated and inspired many.It was one of the arguments for building X-ray free-electron lasers.According to theory,the extremely intense pulses provide sufficient signal to dispense with using crystals as an amplifier,and the ultrashort pulse duration permits capturing the diffraction data before the sample inevitably explodes.This was first demonstrated on biological samples a decade ago on the giant mimivirus.Since then,a large collaboration has been pushing the limit of the smallest sample that can be imaged.The ability to capture snapshots on the timescale of atomic vibrations,while keeping the sample at room temperature,may allow probing the entire conformational phase space of macromolecules.Here we show the first observation of an X-ray diffraction pattern from a single protein,that of Escherichia coli GroEL which at 14 nm in diameter is the smallest biological sample ever imaged by X-rays,and demonstrate that the concept of diffraction before destruction extends to single proteins.From the pattern,it is possible to determine the approximate orientation of the protein.Our experiment demonstrates the feasibility of ultrafast imaging of single proteins,opening the way to single-molecule time-resolved studies on the femtosecond timescale.
基金J.B.acknowledges financial support from the European Research Council for ERC Advanced Grant"TRANSFORMER"(788218)ERC Proof of Concept Grant"miniX"(840010),FET-OPEN"PETACom"(829153),FET-OPEN"OPTOlogic"(899794)+5 种基金FET-OPEN"Twisted Nano(101046424),Laserlab-Europe(871124),Marie Sktodowska-Curie ITN"smart-X"(860553)MINECO for Plan Nacional PID2020-112664 GB-I00AGAUR for 2017 SGR 1639,MINECO for"Severo Ochoa"(CEX2019-000910-S)Fundacio Cellex Barcelona,the CERCA Programme/Generalitat de Catalunyathe Alexander von Humboldt Foundation for the Friedrich Wilhelm Bessel Prize.S.S.acknowledges Marie Sktodowska-Curie grant agreement no.713729(COFUND)M.R.and A.M.S.acknowledge Marie Sktodowska-Curie Grant agreement no.754510(PROBIST)。
文摘Unraveling the exact nature of nonequilibrium and correlated interactions is paramount for continued progress in many areas of condensed matter science. Such insight is a prerequisite to develop an engineered approach for smart materials with targeted properties designed to address standing needs such as efficient light harvesting, energy storage, or information processing. For this goal, it is critical to unravel the dynamics of the energy conversion processes between carriers in the earliest time scales of the excitation dynamics. We discuss the implementation and benefits of attosecond soft x-ray core-level spectroscopy up to photon energies of 600 eV for measurements in solid-state systems. In particular, we examine how the pairing between coherent spectral coverage and temporal resolution provides a powerful new insight into the quantum dynamic interactions that determine the macroscopic electronic and optical response. We highlight the different building blocks of the methodology and point out the important aspects for its application from condensed matter studies to materials as thin as 25 nm. Furthermore, we discuss the technological developments in the field of tabletop attosecond soft x-ray sources with time-resolved measurements at the near and extended edge simultaneously and investigate the exciting prospective of extending such technique to the study of 2-dimensional materials.