| 1. |
- Acharya, B. S., et al.
(författare)
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Introducing the CTA concept
- 2013
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Ingår i: Astroparticle physics. - : Elsevier BV. - 0927-6505 .- 1873-2852. ; 43, s. 3-18
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Tidskriftsartikel (övrigt vetenskapligt/konstnärligt)abstract
- The Cherenkov Telescope Array (CTA) is a new observatory for very high-energy (VHE) gamma rays. CTA has ambitions science goals, for which it is necessary to achieve full-sky coverage, to improve the sensitivity by about an order of magnitude, to span about four decades of energy, from a few tens of GeV to above 100 TeV with enhanced angular and energy resolutions over existing VHE gamma-ray observatories. An international collaboration has formed with more than 1000 members from 27 countries in Europe, Asia, Africa and North and South America. In 2010 the CTA Consortium completed a Design Study and started a three-year Preparatory Phase which leads to production readiness of CTA in 2014. In this paper we introduce the science goals and the concept of CTA, and provide an overview of the project. (C) 2013 Elsevier B.V. All rights reserved.
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| 2. |
- Adcox, K, et al.
(författare)
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PHENIX detector overview
- 2003
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Ingår i: Nuclear Instruments & Methods in Physics Research. Section A: Accelerators, Spectrometers, Detectors, and Associated Equipment. - 0167-5087. ; 499:2-3, s. 469-479
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Tidskriftsartikel (refereegranskat)abstract
- The PHENIX detector is designed to perform a broad study of A-A, p-A, and p-p collisions to investigate nuclear matter under extreme conditions. A wide variety of probes, sensitive to all timescales, are used to study systematic variations with species and energy as well as to measure the spin structure of the nucleon. Designing for the needs of the heavy-ion and polarized-proton programs has produced a detector with unparalleled capabilities. PHENIX measures electron and muon pairs, photons, and hadrons with excellent energy and momentum resolution. The detector consists of a large number of subsystems that are discussed in other papers in this volume. The overall design parameters of the detector are presented. (C) 2002 Elsevier Science B.V. All rights reserved.
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| 3. |
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| 4. |
- Chen, F., et al.
(författare)
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Reply to "comment on 'Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3 ' "
- 2018
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Ingår i: Physical Review B. - 2469-9950. ; 97:22
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Tidskriftsartikel (refereegranskat)abstract
- In this reply to S. Durbin's comment on our original paper "Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3," we concur that his final equations 8 and 9 more accurately describe the change in diffracted intensity as a function of Ti displacement. We also provide an alternative derivation based on an ensemble average over unit cells. The conclusions of the paper are unaffected by this correction.
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| 5. |
- Chen, F., et al.
(författare)
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Ultrafast terahertz-field-driven ionic response in ferroelectric BaTiO3
- 2016
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Ingår i: Physical Review B. - 1098-0121. ; 94:18
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Tidskriftsartikel (refereegranskat)abstract
- The dynamical processes associated with electric field manipulation of the polarization in a ferroelectric remain largely unknown but fundamentally determine the speed and functionality of ferroelectric materials and devices. Here we apply subpicosecond duration, single-cycle terahertz pulses as an ultrafast electric field bias to prototypical BaTiO3 ferroelectric thin films with the atomic-scale response probed by femtosecond x-ray-scattering techniques. We show that electric fields applied perpendicular to the ferroelectric polarization drive large-amplitude displacements of the titanium atoms along the ferroelectric polarization axis, comparable to that of the built-in displacements associated with the intrinsic polarization and incoherent across unit cells. This effect is associated with a dynamic rotation of the ferroelectric polarization switching on and then off on picosecond time scales. These transient polarization modulations are followed by long-lived vibrational heating effects driven by resonant excitation of the ferroelectric soft mode, as reflected in changes in the c-axis tetragonality. The ultrafast structural characterization described here enables a direct comparison with first-principles-based molecular-dynamics simulations, with good agreement obtained.
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| 6. |
- Gray, A. X., et al.
(författare)
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Ultrafast terahertz field control of electronic and structural interactions in vanadium dioxide
- 2018
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Ingår i: Physical Review B. - : AMER PHYSICAL SOC. - 2469-9950 .- 2469-9969. ; 98:4
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Tidskriftsartikel (refereegranskat)abstract
- Vanadium dioxide (VO2), an archetypal correlated-electron material, undergoes an insulator-metal transition near room temperature that exhibits electron-correlation-driven and structurally driven physics. Using ultrafast temperature- and fluence-dependent optical spectroscopy and x-ray scattering, we show that multiple interrelated electronic and structural processes in the nonequilibrium dynamics in VO2 can be disentangled in the time domain. Specifically, following intense subpicosecond terahertz (THz) electric-field excitation, a partial collapse of the insulating gap occurs within the first picosecond. At temperatures sufficiently close to the transition temperature and for THz peak fields above a threshold of approximately 1 MV/cm, this electronic reconfiguration initiates a change in lattice symmetry taking place on a slower timescale. We identify the kinetic energy increase of electrons tunneling in the strong electric field as the driving force, illustrating a promising method to control electronic and structural interactions in correlated materials on an ultrafast timescale.
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| 7. |
- Henighan, T., et al.
(författare)
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Generation mechanism of terahertz coherent acoustic phonons in Fe
- 2016
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Ingår i: PHYSICAL REVIEW B. - 2469-9950. ; 93:22
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Tidskriftsartikel (refereegranskat)abstract
- We use femtosecond time-resolved hard x-ray scattering to detect coherent acoustic phonons generated during ultrafast laser excitation of ferromagnetic bcc Fe films grown on MgO(001). We observe the coherent longitudinal-acoustic phonons as a function of wave vector through analysis of the temporal oscillations in the x-ray scattering signal. The width of the extracted strain wave front associated with this coherent motion is similar to 100 fs. An effective electronic Gruneisen parameter is extracted within a two-temperature model. However, ab initio calculations show that the phonons are nonthermal on the time scale of the experiment, which calls into question the validity of extracting physical constants by fitting such a two-temperature model.
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| 8. |
- Rettig, L., et al.
(författare)
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Disentangling transient charge order from structural dynamics contributions during coherent atomic motion studied by ultrafast resonant x-ray diffraction
- 2019
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Ingår i: Physical Review B. - 2469-9950. ; 99:13
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Tidskriftsartikel (refereegranskat)abstract
- We report on the ultrafast dynamics of charge order and structural response during the photoinduced suppression of charge and orbital order in a mixed-valence manganite. Employing femtosecond time-resolved resonant x-ray diffraction below and at the Mn K absorption edge, we present a method to disentangle the transient charge order and structural dynamics in thin films of Pr0.5Ca0.5MnO3. Based on the static resonant scattering spectra, we extract the dispersion correction of charge-ordered Mn3+ and Mn4+ ions, allowing us to separate the transient contributions of purely charge order from structural contributions to the scattering amplitude after optical excitation. Our finding of a coherent structural mode at around 2.3THz, which primarily modulates the lattice but does not strongly affect the charge order, supports the picture of the charge order being the driving force of the combined charge, orbital, and structural transition.
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| 9. |
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| 10. |
- Biasin, Elisa, et al.
(författare)
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Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated[Co(terpy)2]2$
- 2016
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Ingår i: Physical Review Letters. - : American Physical Society (APS). - 1079-7114 .- 0031-9007. ; 117:1
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Tidskriftsartikel (refereegranskat)abstract
- We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ∼7 ps.
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| 11. |
- Fuller, Franklin D, et al.
(författare)
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Drop-on-demand sample delivery for studying biocatalysts in action at X-ray free-electron lasers
- 2017
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Ingår i: Nature Methods. - : Macmillan Publishers Ltd.. - 1548-7091 .- 1548-7105. ; 14, s. 443-449
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Tidskriftsartikel (refereegranskat)abstract
- X-ray crystallography at X-ray free-electron laser sources is a powerful method for studying macromolecules at biologically relevant temperatures. Moreover, when combined with complementary techniques like X-ray emission spectroscopy, both global structures and chemical properties of metalloenzymes can be obtained concurrently, providing insights into the interplay between the protein structure and dynamics and the chemistry at an active site. The implementation of such a multimodal approach can be compromised by conflicting requirements to optimize each individual method. In particular, the method used for sample delivery greatly affects the data quality. We present here a robust way of delivering controlled sample amounts on demand using acoustic droplet ejection coupled with a conveyor belt drive that is optimized for crystallography and spectroscopy measurements of photochemical and chemical reactions over a wide range of time scales. Studies with photosystem II, the phytochrome photoreceptor, and ribonucleotide reductase R2 illustrate the power and versatility of this method.
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| 12. |
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| 13. |
- Lemke, Henrik T., et al.
(författare)
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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
- 2017
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
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Tidskriftsartikel (refereegranskat)abstract
- The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy) 3 ] 2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.
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| 14. |
- Chollet, M., et al.
(författare)
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Public Speaking Training with a Multimodal Interactive Virtual Audience Framework
- 2015
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Ingår i: ICMI '15 Proceedings of the 2015 ACM on International Conference on Multimodal Interaction. - New York, NY, USA : ACM Digital Library. ; , s. 367-368
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Konferensbidrag (refereegranskat)abstract
- We have developed an interactive virtual audience platform for public speaking training. Users' public speaking behavior is automatically analyzed using multimodal sensors, and ultimodal feedback is produced by virtual characters and generic visual widgets depending on the user's behavior. The flexibility of our system allows to compare different interaction mediums (e.g. virtual reality vs normal interaction), social situations (e.g. one-on-one meetings vs large audiences) and trained behaviors (e.g. general public speaking performance vs specific behaviors).
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| 15. |
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| 16. |
- Faundez-Zanuy, M, et al.
(författare)
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The COST-277 European action : An overview
- 2005
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Ingår i: NONLINEAR ANALYSES AND ALGORITHMS FOR SPEECH PROCESSING. ; , s. 1-9
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Konferensbidrag (refereegranskat)abstract
- This paper summarizes the rationale for proposing the COST-277 "nonlinear speech processing" action, and the work done during these last four years. In addition, future perspectives are described.
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| 17. |
- Kjær, Kasper S., et al.
(författare)
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Ligand manipulation of charge transfer excited state relaxation and spin crossover in [Fe(2,2'-bipyridine)2(CN)2]
- 2017
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Ingår i: Structural Dynamics. - : AIP Publishing. - 2329-7778. ; 4:4
-
Tidskriftsartikel (refereegranskat)abstract
- We have used femtosecond resolution UV-visible and Kβ x-ray emission spectroscopy to characterize the electronic excited state dynamics of [Fe(bpy)2(CN)2], where bpy=2,20-bipyridine, initiated by metal-to-ligand charge transfer (MLCT) excitation. The excited-state absorption in the transient UV-visible spectra, associated with the 2,20-bipyridine radical anion, provides a robust marker for the MLCT excited state, while the transient Kβ x-ray emission spectra provide a clear measure of intermediate and high spin metal-centered excited states. From these measurements, we conclude that the MLCT state of [Fe(bpy)2(CN)2] undergoes ultrafast spin crossover to a metalcentered quintet excited state through a short lived metal-centered triplet transient species. These measurements of [Fe(bpy)2(CN)2] complement prior measurement performed on [Fe(bpy)3]2+ and [Fe(bpy)(CN)4]2- in dimethylsulfoxide solution and help complete the chemical series [Fe(bpy)N(CN)6-2N]2N-4, whereN=1-3. The measurements confirm that simple ligand modifications can significantly change the relaxation pathways and excited state lifetimes and support the further investigation of light harvesting and photocatalytic applications of 3d transition metal complexes.
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| 18. |
- Mojtahid, M., et al.
(författare)
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Assessing the impact of different carbonate system parameters on benthic foraminifera from controlled growth experiments
- 2023
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Ingår i: Chemical Geology. - : Elsevier BV. - 0009-2541. ; 623
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Tidskriftsartikel (refereegranskat)abstract
- Insights into past marine carbon cycling and water mass properties can be obtained by means of geochemical proxies calibrated through controlled laboratory experiments with accurate seawater carbonate system (C-system) manipulations. Here, we explored the use of strontium/calcium ratio (Sr/Ca) of the calcite shells of benthic foraminifera as a potential seawater C-system proxy through a controlled growth experiment with two deep-sea species (Bulimina marginata and Cassidulina laevigata) and one intertidal species (Ammonia T6). To this aim, we used two experimental set-ups to decouple as much as possible the individual components of the carbonate system, i.e., changing pH at constant dissolved inorganic carbon (DIC) and changing DIC at constant pH. Four climatic chambers were used with different controlled concentrations of atmospheric pCO2 (180 ppm, 410 ppm, 1000 ppm, 1500 ppm). Our results demonstrated that pH did not influence the survival and growth of the three species. However, low DIC conditions (879 μmol kg−1) negatively affected B. marginata and C. laevigata through reduced growth, whereas no effect was observed for Ammonia T6. Our results also showed that Sr/Ca was positively correlated with total Alkalinity (TA), DIC and bicarbonate ion concentration ([HCO3 −]) for Ammonia T6 and B. marginata; i.e., DIC and/or [HCO3 −] were the main controlling factors. For these two species, the regression models were coherent with published data (existing so far only for Ammonia T6) and showed overall similar slopes but different intercepts, implying species-specific effects. Furthermore, the Sr/Ca - C-system relationship was not impacted by ontogenetic trends between chamber stages, which is a considerable advantage for paleo-applications. This applied particularly to Ammonia T6 that calcified many chambers compared to the two other species. However, no correlation with any of the C-system parameters was observed for Sr/Ca in C. laevigata. This might imply either a strong species-specific effect and/or a low tolerance to laboratory conditions leading to a physiological stress, thereby impacting the Sr incorporation into the calcite lattice of C. laevigata.
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| 19. |
- Van Driel, Tim B., et al.
(författare)
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Atomistic characterization of the active-site solvation dynamics of a model photocatalyst
- 2016
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 7
-
Tidskriftsartikel (refereegranskat)abstract
- The interactions between the reactive excited state of molecular photocatalysts and surrounding solvent dictate reaction mechanisms and pathways, but are not readily accessible to conventional optical spectroscopic techniques. Here we report an investigation of the structural and solvation dynamics following excitation of a model photocatalytic molecular system [Ir 2 (dimen) 4 ] 2+, where dimen is para-diisocyanomenthane. The time-dependent structural changes in this model photocatalyst, as well as the changes in the solvation shell structure, have been measured with ultrafast diffuse X-ray scattering and simulated with Born-Oppenheimer Molecular Dynamics. Both methods provide direct access to the solute-solvent pair distribution function, enabling the solvation dynamics around the catalytically active iridium sites to be robustly characterized. Our results provide evidence for the coordination of the iridium atoms by the acetonitrile solvent and demonstrate the viability of using diffuse X-ray scattering at free-electron laser sources for studying the dynamics of photocatalysis.
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| 20. |
- Zalden, Peter, et al.
(författare)
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Femtosecond x-ray diffraction reveals a liquid–liquid phase transition in phase-change materials
- 2019
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Ingår i: Science. - Washington, DC : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 364:6445, s. 1062-1067
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Tidskriftsartikel (refereegranskat)abstract
- In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process. We found a liquid–liquid phase transition in the phase-change materials Ag4In3Sb67Te26 and Ge15Sb85 at 660 and 610 kelvin, respectively. The transition is predominantly caused by the onset of Peierls distortions, the amplitude of which correlates with an increase of the apparent activation energy of diffusivity. This reveals a relationship between atomic structure and kinetics, enabling a systematic optimization of the memory-switching kinetics.
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| 21. |
- Zhang, Wenkai, et al.
(författare)
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Manipulating charge transfer excited state relaxation and spin crossover in iron coordination complexes with ligand substitution
- 2016
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Ingår i: Chemical Science. - 2041-6520. ; 8:1, s. 515-523
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Tidskriftsartikel (refereegranskat)abstract
- Developing light-harvesting and photocatalytic molecules made with iron could provide a cost effective, scalable, and environmentally benign path for solar energy conversion. To date these developments have been limited by the sub-picosecond metal-to-ligand charge transfer (MLCT) electronic excited state lifetime of iron based complexes due to spin crossover-the extremely fast intersystem crossing and internal conversion to high spin metal-centered excited states. We revitalize a 30 year old synthetic strategy for extending the MLCT excited state lifetimes of iron complexes by making mixed ligand iron complexes with four cyanide (CN-;) ligands and one 2,2′-bipyridine (bpy) ligand. This enables MLCT excited state and metal-centered excited state energies to be manipulated with partial independence and provides a path to suppressing spin crossover. We have combined X-ray Free-Electron Laser (XFEL) Kβ hard X-ray fluorescence spectroscopy with femtosecond time-resolved UV-visible absorption spectroscopy to characterize the electronic excited state dynamics initiated by MLCT excitation of [Fe(CN)4(bpy)]2-. The two experimental techniques are highly complementary; the time-resolved UV-visible measurement probes allowed electronic transitions between valence states making it sensitive to ligand-centered electronic states such as MLCT states, whereas the Kβ fluorescence spectroscopy provides a sensitive measure of changes in the Fe spin state characteristic of metal-centered excited states. We conclude that the MLCT excited state of [Fe(CN)4(bpy)]2- decays with roughly a 20 ps lifetime without undergoing spin crossover, exceeding the MLCT excited state lifetime of [Fe(2,2′-bipyridine)3]2+ by more than two orders of magnitude.
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