Toward atomic resolution diffractive imaging of isolated molecules with X-ray free-electron lasers.

We give a detailed account of the theoretical analysis and the experimental results of an X-ray-diffraction experiment on quantum-state selected and strongly laser-aligned gas-phase ensembles of the prototypical large asymmetric rotor molecule 2,5-diiodobenzonitrile, performed at the Linac Coherent Light Source [Phys. Rev. Lett.112, 083002 (2014)]. This experiment is the first step toward coherent diffractive imaging of structures and structural dynamics of isolated molecules at atomic resolution, i.e., picometers and femtoseconds, using X-ray free-electron lasers.

[1]  G. Meijer,et al.  Selector for structural isomers of neutral molecules. , 2008, Physical review letters.

[2]  I. A. Vartanyants,et al.  Orientation determination in single-particle x-ray coherent diffraction imaging experiments , 2013, 1302.5730.

[3]  Georg Weidenspointner,et al.  Femtosecond X-ray protein nanocrystallography , 2011, Nature.

[4]  A. H. Walenta,et al.  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 , 2010 .

[5]  P. Bogdanovich,et al.  Atomic Data and Nuclear Data Tables , 2013 .

[6]  Anton Barty,et al.  CASS - CFEL-ASG software suite , 2012, Comput. Phys. Commun..

[7]  Ahmed H. Zewail,et al.  Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond† , 2000 .

[8]  M. Bandstra,et al.  Measurements of Fukushima fallout by the Berkeley Radiological Air and Water Monitoring project , 2011, 2011 IEEE Nuclear Science Symposium Conference Record.

[9]  A. Kirfel,et al.  New analytical scattering‐factor functions for free atoms and ions , 1995 .

[10]  S. T. Pratt,et al.  Femtosecond electronic response of atoms to ultra-intense X-rays , 2010, Nature.

[11]  J. Bozek AMO instrumentation for the LCLS X-ray FEL , 2009 .

[12]  H. Stapelfeldt,et al.  Molecular-frame 3D photoelectron momentum distributions by tomographic reconstruction. , 2012, Physical review letters.

[13]  Georg Weidenspointner,et al.  X-ray diffraction from isolated and strongly aligned gas-phase molecules with a free-electron laser , 2013, 1307.4577.

[14]  J. Jortner,et al.  Cooling of large molecules below 1 K and He clusters formation , 2000 .

[15]  Li Fang,et al.  Ultra-fast and ultra-intense x-ray sciences: first results from the Linac Coherent Light Source free-electron laser , 2013 .

[16]  A. Zewail,et al.  Ultrafast electron diffraction. Velocity mismatch and temporal resolution in crossed-beam experiments , 1993 .

[17]  Friedrich,et al.  Alignment and trapping of molecules in intense laser fields. , 1995, Physical review letters.

[18]  J. Küpper,et al.  Strongly aligned and oriented molecular samples at a kHz repetition rate , 2013, 1301.1826.

[19]  D. Ratner,et al.  First lasing and operation of an ångstrom-wavelength free-electron laser , 2010 .

[20]  Germán Sciaini,et al.  Femtosecond electron diffraction: heralding the era of atomically resolved dynamics , 2011 .

[21]  A. Ourmazd,et al.  Structure from Fleeting Illumination of Faint Spinning Objects in Flight with Application to Single Molecules , 2008, 0806.2341.

[22]  H. Chapman,et al.  State- and conformer-selected beams of aligned and oriented molecules for ultrafast diffraction studies. , 2010, Physical chemistry chemical physics : PCCP.

[23]  U. Even,et al.  Generation and propagation of intense supersonic beams. , 2011, The journal of physical chemistry. A.

[24]  A. Zewail,et al.  Electron and X-ray methods of ultrafast structural dynamics: advances and applications. , 2009, Chemphyschem : a European journal of chemical physics and physical chemistry.

[25]  Anton Barty,et al.  Molecular imaging using X-ray free-electron lasers. , 2018, Annual review of physical chemistry.

[26]  A Barty,et al.  Damped and thermal motion of laser-aligned hydrated macromolecule beams for diffraction. , 2005, The Journal of chemical physics.

[27]  Jochen Küpper,et al.  CMIstark: Python package for the Stark-effect calculation and symmetry classification of linear, symmetric and asymmetric top wavefunctions in dc electric fields , 2013, Comput. Phys. Commun..

[28]  J. L. Hansen,et al.  Pure samples of individual conformers: the separation of stereoisomers of complex molecules using electric fields. , 2009, Angewandte Chemie.

[29]  J. H. Hubbell,et al.  XCOM : Photon Cross Sections Database , 2005 .

[30]  J. Spence,et al.  Single molecule diffraction. , 2004, Physical review letters.

[31]  S. Stern,et al.  Spatial separation of state- and size-selected neutral clusters , 2012, 1208.4935.

[32]  Henry N. Chapman,et al.  Femtosecond x-ray photoelectron diffraction on gas-phase dibromobenzene molecules , 2014 .

[33]  H. Stapelfeldt,et al.  Aligning molecules with intense nonresonant laser fields , 1999 .

[34]  Martin Centurion,et al.  Imaging of isolated molecules with ultrafast electron pulses. , 2012, Physical review letters.

[35]  Veit Elser,et al.  Reconstruction algorithm for single-particle diffraction imaging experiments. , 2009, Physical review. E, Statistical, nonlinear, and soft matter physics.

[36]  G. Meijer,et al.  Laser-induced alignment and orientation of quantum-state-selected large molecules. , 2008, Physical review letters.

[37]  Georg Weidenspointner,et al.  Ultra-efficient ionization of heavy atoms by intense X-ray free-electron laser pulses , 2012, Nature Photonics.

[38]  H. Chapman,et al.  Imaging molecular structure through femtosecond photoelectron diffraction on aligned and oriented gas-phase molecules. , 2014, Faraday discussions.

[39]  J. L. Hansen,et al.  Laser-induced 3D alignment and orientation of quantum state-selected molecules. , 2009, Physical chemistry chemical physics : PCCP.

[40]  C. Bostedt,et al.  Ultrafast charge rearrangement and nuclear dynamics upon inner-shell multiple ionization of small polyatomic molecules. , 2013, Physical review letters.

[41]  Hald,et al.  Three dimensional alignment of molecules using elliptically polarized laser fields , 2000, Physical review letters.

[42]  E. A. Schneidmiller,et al.  Generation of attosecond soft x-ray pulses in a longitudinal space charge amplifier , 2011 .

[43]  J. Als-Nielsen,et al.  Elements of Modern X-ray Physics , 2001 .

[44]  Henrik Stapelfeldt,et al.  Colloquium: Aligning molecules with strong laser pulses , 2003 .

[45]  J. L. Hansen,et al.  Mixed-field orientation of molecules without rotational symmetry. , 2013, The Journal of chemical physics.

[46]  P Emma,et al.  Measurements and simulations of ultralow emittance and ultrashort electron beams in the linac coherent light source. , 2009, Physical review letters.

[47]  J. Hajdu,et al.  Potential for biomolecular imaging with femtosecond X-ray pulses , 2000, Nature.

[48]  H. Chapman,et al.  Femtosecond protein nanocrystallography-data analysis methods. , 2010, Optics express.

[49]  I. Mclaren,et al.  TIME-OF-FLIGHT MASS SPECTROMETER WITH IMPROVED RESOLUTION , 1955 .

[50]  B. L. Henke,et al.  X-Ray Interactions: Photoabsorption, Scattering, Transmission, and Reflection at E = 50-30,000 eV, Z = 1-92 , 1993 .

[51]  E. Weckert,et al.  Impact of ultrafast electronic damage in single-particle x-ray imaging experiments. , 2012, Physical review. E, Statistical, nonlinear, and soft matter physics.

[52]  J. L. Hansen,et al.  Quantum-state selection, alignment, and orientation of large molecules using static electric and laser fields. , 2009, The Journal of chemical physics.

[53]  R. Weinkauf,et al.  Highly Efficient Charge Transfer in Peptide Cations in the Gas Phase: Threshold Effects and Mechanism , 1996 .

[54]  J. Kupper,et al.  Spatially separated polar samples of the cis and trans conformers of 3-fluorophenol , 2013, 1312.4417.

[55]  G Ruocco,et al.  Single-molecule imaging with x-ray free-electron lasers: dream or reality? , 2010, Physical review letters.

[56]  J S Wu,et al.  Diffraction and imaging from a beam of laser-aligned proteins: resolution limits. , 2005, Acta crystallographica. Section A, Foundations of crystallography.

[57]  C. Bostedt,et al.  Femtosecond photoelectron diffraction on laser-aligned molecules: Towards time-resolved imaging of molecular structure , 2013 .

[58]  Garth J. Williams,et al.  Single mimivirus particles intercepted and imaged with an X-ray laser , 2011, Nature.

[59]  I. Petrov,et al.  Direct Hartree-Fock calculation of multiple Xei+ ion production through inner shell vacancy de-excitations , 1994 .

[60]  T. Wyttenbach,et al.  Conformation of Macromolecules in the Gas Phase: Use of Matrix-Assisted Laser Desorption Methods in Ion Chromatography , 1995, Science.

[61]  Alan D. Martin,et al.  Review of Particle Physics , 2010 .

[62]  Mark S. Gordon,et al.  General atomic and molecular electronic structure system , 1993, J. Comput. Chem..

[63]  R. Rosenfeld Nature , 2009, Otolaryngology--head and neck surgery : official journal of American Academy of Otolaryngology-Head and Neck Surgery.

[64]  P Emma,et al.  Femtosecond x-ray pulse characterization in free-electron lasers using a cross-correlation technique. , 2012, Physical review letters.

[65]  C. Bostedt,et al.  Femtosecond x-ray pulse length characterization at the Linac Coherent Light Source free-electron laser , 2011 .

[66]  H. Chapman,et al.  Limitations of coherent diffractive imaging of single objects due to their damage by intense x-ray radiation , 2012 .