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Register a new userToward atomic resolution diffractive imaging of isolated molecules with x-ray free-electron lasers
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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.
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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.
Observing the motion of the nuclear wavepackets during a molecular reaction, in both space and time, is crucial for understanding and controlling the outcome of photoinduced chemical reactions. We have imaged the motion of a vibrational wavepacket in isolated iodine molecules using ultrafast electron diffraction with relativistic electrons. The time-varying interatomic distance was measured with a precision 0.07 {AA} and temporal resolution of 230 fs full-width at half-maximum (FWHM). The method is not only sensitive to the position but also the shape of the nuclear wavepacket.
We report experimental results on the diffractive imaging of three-dimensionally aligned 2,5-diiodothiophene molecules. The molecules were aligned by chirped near-infrared laser pulses, and their structure was probed at a photon energy of 9.5 keV ($lambdaapprox130 text{pm}$) provided by the Linac Coherent Light Source. Diffracted photons were recorded on the CSPAD detector and a two-dimensional diffraction pattern of the equilibrium structure of 2,5-diiodothiophene was recorded. The retrieved distance between the two iodine atoms agrees with the quantum-chemically calculated molecular structure to within 5 %. The experimental approach allows for the imaging of intrinsic molecular dynamics in the molecular frame, albeit this requires more experimental data which should be readily available at upcoming high-repetition-rate facilities.
We study the perspectives of measuring the phenomenon of vacuum birefringence predicted by quantum electrodynamics using an x-ray free-electron laser (XFEL) alone. We devise an experimental scheme allowing the XFEL beam to collide with itself under a finite angle, and thus act as both pump and probe field for the effect. The signature of vacuum birefringence is encoded in polarization-flipped signal photons to be detected with high-purity x-ray polarimetry. Our findings for idealized scenarios underline that the discovery potential of solely XFEL-based setups can be comparable to those involving optical high-intensity lasers. For currently achievable scenarios, we identify several key details of the x-ray optical ingredients that exert a strong influence on the magnitude of the desired signatures.
The single-pulse spectrum of self-amplified spontaneous emission (SASE) free electron lasers (FELs) is characterized by random fluctuations in frequency. The typical spectrum bandwidth for a hard x-ray FEL is in the range of 10-20 eV and is comparable with the distance between energy levels of valence electrons in atoms an molecules. We calculate the rate of transitions in a quantum three-level system with the energy difference of several eV caused by such radiation and show that for x-ray intensities in the range of $10^{20}$ W/cm$^2$ the probability of the transition over the duration of the x-ray pulse is large. We argue that this effect can be used to modify the spectrum of a SASE FEL potentially making it more narrow.
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