X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser

We report experimental results on x-ray diffraction of quantum-state-selected and strongly aligned ensembles of the prototypical asymmetric rotor molecule 2,5-diiodobenzonitrile using the Linac Coherent Light Source. The experiments demonstrate first steps toward a new approach to diffractive imaging of distinct structures of individual, isolated gas-phase molecules. We confirm several key ingredients of single molecule diffraction experiments: the abilities to detect and count individual scattered x-ray photons in single shot diffraction data, to deliver state-selected, e.g., structural-isomer-selected, ensembles of molecules to the x-ray interaction volume, and to strongly align the scattering molecules. Our approach, using ultrashort x-ray pulses, is suitable to study ultrafast dynamics of isolated molecules.

• Publication year

  2013

• Venue

  Physical Review Letters

• Publication date

  2013-07-17

• Fields of study

  Materials Science, Physics, Chemistry

• Identifiers
  DOI 10.1103/PhysRevLett.112.083002arXiv 1307.4577
• External record

  Open on Semantic Scholar

• Source metadata

  Semantic Scholar

• No claims are published for this paper.

• No concepts are published for this paper.

• Molecular imaging using X-ray free-electron lasers.

  2018influential reference
• Mixed-field orientation of molecules without rotational symmetry.

  2013cited by this paper
• Femtosecond photoelectron diffraction on laser-aligned molecules: Towards time-resolved imaging of molecular structure

  2013cited by this paper
• Ultra-fast and ultra-intense x-ray sciences: first results from the Linac Coherent Light Source free-electron laser

  2013influential reference
• Ultrafast charge rearrangement and nuclear dynamics upon inner-shell multiple ionization of small polyatomic molecules.

  2013influential reference
• Spatially separated polar samples of the cis and trans conformers of 3-fluorophenol

  2013cited by this paper
• Nanoplasma dynamics of single large xenon clusters irradiated with superintense x-ray pulses from the linac coherent light source free-electron laser.

  2012cited by this paper
• Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight

  2012cited by this paper
• Impact of ultrafast electronic damage in single-particle x-ray imaging experiments.

  2012cited by this paper
• Spatial separation of state- and size-selected neutral clusters

  2012cited by this paper
• CASS - CFEL-ASG software suite

  2012cited by this paper
• Ultra-efficient ionization of heavy atoms by intense X-ray free-electron laser pulses

  2012cited by this paper
• Imaging of isolated molecules with ultrafast electron pulses.

  2012cited by this paper
• Limitations of coherent diffractive imaging of single objects due to their damage by intense x-ray radiation

  2012cited by this paper
• Single mimivirus particles intercepted and imaged with an X-ray laser

  2011cited by this paper
• Femtosecond x-ray pulse length characterization at the Linac Coherent Light Source free-electron laser

  2011cited by this paper
• Femtosecond X-ray protein nanocrystallography

  2011cited by this paper
• Self-terminating diffraction gates femtosecond X-ray nanocrystallography measurements

  2011cited by this paper
• Large-format, high-speed, X-ray pnCCDs combined with electron and ion imaging spectrometers in a multipurpose chamber for experiments at 4th generation light sources

  2010cited by this paper
• Time-resolved pump-probe experiments at the LCLS.

  2010influential reference
• State- and conformer-selected beams of aligned and oriented molecules for ultrafast diffraction studies.

  2010influential reference
• Ultrafast extreme ultraviolet induced isomerization of acetylene cations.

  2010cited by this paper
• First lasing and operation of an ångstrom-wavelength free-electron laser

  2010influential reference
• Femtosecond electronic response of atoms to ultra-intense X-rays

  2010cited by this paper
• Computational studies of x-ray scattering from three-dimensionally-aligned asymmetric-top molecules

  2009cited by this paper
• Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields.

  2009cited by this paper
• Pure samples of individual conformers: the separation of stereoisomers of complex molecules using electric fields.

  2009cited by this paper
• Laser-induced 3D alignment and orientation of quantum state-selected molecules.

  2009cited by this paper
• Laser-induced alignment and orientation of quantum-state-selected large molecules.

  2008cited by this paper
• Ultrafast single-shot diffraction imaging of nanoscale dynamics

  2008cited by this paper
• An x-ray probe of laser-aligned molecules

  2008cited by this paper
• Selector for structural isomers of neutral molecules.

  2008cited by this paper
• Femtosecond diffractive imaging with a soft-X-ray free-electron laser

  2006cited by this paper
• Diffraction and imaging from a beam of laser-aligned proteins: resolution limits.

  2005cited by this paper
• XCOM : Photon Cross Sections Database

  2005cited by this paper
• Single molecule diffraction.

  2004cited by this paper
• Colloquium: Aligning molecules with strong laser pulses

  2003cited by this paper
• Elements of Modern X-ray Physics

  2001cited by this paper
• Three dimensional alignment of molecules using elliptically polarized laser fields

  2000cited by this paper
• First observation of self-amplified spontaneous emission in a free-electron laser at 109 nm wavelength

  2000cited by this paper
• Potential for biomolecular imaging with femtosecond X-ray pulses

  2000influential reference
• Cooling of large molecules below 1 K and He clusters formation

  2000cited by this paper
• Conformation of Macromolecules in the Gas Phase: Use of Matrix-Assisted Laser Desorption Methods in Ion Chromatography

  1995cited by this paper
• Alignment and trapping of molecules in intense laser fields.

  1995cited by this paper
• New analytical scattering‐factor functions for free atoms and ions

  1995cited by this paper
• Direct Hartree-Fock calculation of multiple Xei+ ion production through inner shell vacancy de-excitations

  1994cited by this paper
• X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92

  1993cited by this paper
• General atomic and molecular electronic structure system

  1993cited by this paper

• Stability Enhancement of a Self-Amplified Spontaneous Emission Free-electron Laser with Bunching Containment

  2025cites this paper
• Geometry Change of 1,3-Dicyanobenzene upon Electronic Excitation from a Franck–Condon Fit of Several Fluorescence Emission Spectra

  2025cites this paper
• Controlled molecule injector for cold, dense, and pure molecular beams at the European x-ray free-electron laser.

  2024cites this paper
• Correlated rotational alignment spectroscopy: a new tool for high-resolution spectroscopy and the analysis of heterogeneous samples.

  2024cites this paper
• Pushing the limits of ultrafast diffraction: Imaging quantum coherences in isolated molecules

  2024cites this paper
• Tracking the Electron Density Changes in Excited States: A Computational Study of Pyrazine.

  2024cites this paper
• Time‐resolved x‐ray spectroscopy of nucleobases and their thionated analogs

  2024cites this paper
• A versatile and transportable endstation for controlled molecule experiments.

  2024cites this paper
• Partial orientation retrieval of proteins from X-ray free-electron-laser induced explosions for single particle imaging

  2024cites this paper
• Molecular influence on nuclear-quadrupole-coupling effects in laser induced alignment.

  2024cites this paper
• Laser-induced alignment of nanoparticles and macromolecules for single-particle-imaging applications

  2023cites this paper
• The contribution of Compton ionization to ultrafast x-ray scattering.

  2023cites this paper
• Unraveling the ultrafast dynamics of thermal-energy chemical reactions.

  2023cites this paper
• X-ray multiphoton-induced Coulomb explosion images complex single molecules

  2022cites this paper
• Ultrafast isolated molecule imaging without crystallization

  2022influential citation
• Ultrafast coherent photoexcited dynamics in a trimeric dendrimer probed by X-ray stimulated-Raman signals

  2022cites this paper
• Resolving vibrations in a polyatomic molecule with femtometer precision via x-ray spectroscopy

  2022cites this paper
• Time-resolved experiments on gas-phase atoms and molecules with XUV and X-ray free-electron lasers

  2022cites this paper
• Perspectives of Gas Phase Ion Chemistry: Spectroscopy and Modeling

  2022cites this paper
• Perspective: Ultrafast Imaging of Molecular Dynamics Using Ultrafast Low-Frequency Lasers, X-ray Free Electron Laser and Electron Pulses

  2022influential citation
• Femtosecond Rotational Dynamics of D_{2} Molecules in Superfluid Helium Nanodroplets.

  2022cites this paper
• Diffraction pattern degradation driven by intense ultrafast X-ray pulse for H2+

  2021cites this paper
• Real-space inversion and super-resolution of ultrafast scattering

  2021cites this paper
• A new route for enantio-sensitive structure determination by photoelectron scattering on molecules in the gas phase.

  2021cites this paper
• Ultrafast light-induced dynamics in the microsolvated biomolecular indole chromophore with water

  2021cites this paper
• Conical Intersection Passages of Molecules Probed by X-ray Diffraction and Stimulated Raman Spectroscopy.

  2021cites this paper
• Machine learning for laser-induced electron diffraction imaging of molecular structures

  2021cites this paper
• In-situ measurement of aligning intensity and rotational temperature in field-free molecular alignment via white light generation

  2021cites this paper
• Three dimensional orientation of small polyatomic molecules excited by two-color femtosecond pulses

  2021cites this paper
• Unveiling the spatial distribution of molecular coherences at conical intersections by covariance X-ray diffraction signals

  2021cites this paper
• Field-free molecular orientation induced by a four-color laser pulse

  2021cites this paper
• Probing molecular dynamics with ultrafast electron diffraction

  2021cites this paper
• Ultrafast light-induced dynamics in solvated biomolecules: The indole chromophore with water

  2021cites this paper
• CMInject: Python framework for the numerical simulation of nanoparticle injection pipelines

  2021cites this paper
• Imaging conical intersection dynamics during azobenzene photoisomerization by ultrafast X-ray diffraction

  2021cites this paper
• Spatiotemporal rotational dynamics of laser-driven molecules

  2020cites this paper
• Study of molecular orientation steered by few-cycle terahertz pulse

  2020cites this paper
• Scattering of adiabatically aligned molecules by nonresonant optical standing waves

  2020cites this paper
• Time-resolved x-ray scattering from impulsively aligned or oriented molecules

  2020cites this paper
• X-ray scattering signatures of early-time accelerations in iodine dissociation

  2020cites this paper
• Ultrafast electron diffraction imaging of gas-phase molecules

  2020cites this paper
• Studies of H2 photoionization by a strong ultrashort x-ray pulse on base of a trajectory method

  2020cites this paper
• Comparative studies of the degrees of orientation of CO molecules pumped by intense femtosecond two-color pulses based on high-order harmonic generation and Coulomb explosion imaging

  2020cites this paper
• Time-resolving the UV-initiated photodissociation dynamics of OCS.

  2020cites this paper
• Picosecond pulse-shaping for strong three-dimensional field-free alignment of generic asymmetric-top molecules

  2020cites this paper
• Imaging of Objects by Coherent Diffraction of X-Ray Free-Electron Laser Pulses

  2020cites this paper
• Spatial separation of 2-propanol monomer and its ionization-fragmentation pathways

  2020cites this paper
• Molecular Physics and Gas-Phase Chemistry with Free-Electron Lasers

  2020cites this paper
• Controlling rotation in the molecular frame with an optical centrifuge

  2020cites this paper
• Spatial Separation of the Conformers of Methyl Vinyl Ketone.

  2020cites this paper
• Spectroscopic and Structural Probing of Excited-State Molecular Dynamics with Time-Resolved Photoelectron Spectroscopy and Ultrafast Electron Diffraction

  2020cites this paper
• Atomic-resolution imaging of carbonyl sulfide by laser-induced electron diffraction.

  2019cites this paper
• Capturing the photo-induced dynamics of nano-molecules by X-ray free electron laser induced Coulomb explosion.

  2019cites this paper
• Recipe for preparing a molecular ensemble with macroscopic threefold symmetry

  2019cites this paper
• Real-time observation of X-ray-induced intramolecular and interatomic electronic decay in CH2I2

  2019cites this paper
• Direct imaging of molecular rotation with high-order-harmonic generation

  2019cites this paper
• Plasma channel formation in NIR laser-irradiated carrier gas from an aerosol nanoparticle injector

  2019cites this paper
• Ultrafast X-ray scattering reveals vibrational coherence following Rydberg excitation

  2019cites this paper
• Probing Electronic Fluxes via Time-Resolved X-Ray Scattering.

  2019cites this paper
• Alignment of the CS2 dimer embedded in helium droplets induced by a circularly polarized laser pulse

  2019cites this paper
• Improved molecular structure retrieval method for photoelectron holography

  2019cites this paper
• Molecular-Frame Angularly-Resolved Photoelectron Spectroscopy

  2019influential citation
• Edinburgh Research Explorer The photochemical ring-opening of 1,3-cyclohexadiene imaged by ultrafast electron diffraction

  2019cites this paper
• Robust and Accurate Computational Estimation of the Polarizability Tensors of Macromolecules.

  2019cites this paper
• X-ray diffractive imaging of controlled gas-phase molecules: Toward imaging of dynamics in the molecular frame.

  2019cites this paper
• Pure Molecular Beam of Water Dimer.

  2019cites this paper
• Laser-induced dynamics of molecules with strong nuclear quadrupole coupling.

  2019cites this paper
• Femtosecond gas-phase mega-electron-volt ultrafast electron diffraction

  2019cites this paper
• Imaging Electron Dynamics with Ultrashort Light Pulses: A Theory Perspective

  2018cites this paper
• Anisotropy enhanced X-ray scattering from solvated transition metal complexes.

  2018cites this paper
• RichMol: A general variational approach for rovibrational molecular dynamics in external electric fields.

  2018cites this paper
• All-optical field-free three-dimensional orientation of asymmetric-top molecules

  2018cites this paper
• Acetylacetone photodynamics at a seeded free-electron laser

  2018cites this paper
• Visualizing rotational wave functions of electronically excited nitric oxide molecules by using an ion imaging technique.

  2018cites this paper
• Spatially separating the conformers of the dipeptide Ac-Phe-Cys-NH 2

  2018cites this paper
• Laser-induced alignment of weakly bound molecular aggregates

  2018cites this paper
• Spatially Separating the Conformers of a Dipeptide.

  2018cites this paper
• CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser

  2018cites this paper
• Echo Spectroscopy in Multilevel Quantum-Mechanical Rotors.

  2018cites this paper
• Laser-induced acoustic desorption of thermally stable and unstable biomolecules

  2018cites this paper
• Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction

  2018cites this paper
• X-ray Emission Spectroscopy at X-ray Free Electron Lasers: Limits to Observation of the Classical Spectroscopic Response for Electronic Structure Analysis.

  2018cites this paper
• Spatial separation of pyrrole and pyrrole-water clusters

  2018cites this paper
• Spatially separating the conformers of the dipeptide Ac-Phe-Cys-NH$_\text{2}$

  2018cites this paper
• Imaging the Photochemical Ring-Opening of 1,3-Cyclohexadiene by Ultrafast Electron Diffraction

  2018cites this paper
• Räumliche Trennung der Konformere eines Dipeptids

  2018cites this paper
• Access to the ultrafast dynamics of molecules-laser interaction with high harmonic spectroscopy

  2018cites this paper
• Optimized cell geometry for buffer-gas-cooled molecular-beam sources

  2018cites this paper
• Quantum control of molecular rotation

  2018cites this paper
• Molecular Orbital Tomography Based on High-Order Harmonic Generation: Principles and Perspectives

  2018cites this paper
• Changes of Normal Coordinates and Geometrical Parameters of a Molecule in a Laser Field

  2018cites this paper
• Evaluation of the photoionization probability of H2+ by the trajectory semiclassical method

  2018cites this paper
• Developing Methods towards the Structure Determination of Biological Particles using Crystallographic and Single Particle Imaging Techniques

  2018cites this paper
• Multiple-orbital effects in laser-induced electron diffraction of aligned molecules

  2018cites this paper
• Advanced sample injection for serial diffraction at free-electron lasers

  2018cites this paper
• Optical and aerodynamic focusing of isolated particles for diffractive imaging experiments at X-ray free electron lasers

  2018cites this paper
• The LAMP instrument at the Linac Coherent Light Source free-electron laser.

  2018cites this paper
• Molecular movie of ultrafast coherent rotational dynamics of OCS

  2018influential citation
• DNA-based construction at the nanoscale: emerging trends and applications

  2018cites this paper
• Mapping the Complete Reaction Path of a Complex Photochemical Reaction.

  2018cites this paper