IDEX Paris-Saclay APPEL A PROJETS RECHERCHE 2014 Titre du Projet : OPT2X Responsable du projet : Nom : Dowek Prénom : Danielle Etablissement/laboratoire : ISMO – CNRS – Université Paris-Sud Courriel : danielle.dowek@u-psud.fr Tél : 0169157672 Résumé du projet (15 lignes maximum) : This project aims at OPTimizing OPTical pulses for XUV ultrafast science (OPT2X). It will provide the Paris-Saclay scientific community with the necessary resources to fully exploit the exceptional potential of its laser-based sources in the extreme-ultraviolet (XUV 1nm-100 nm) domain. OPT2X will enhance the capabilities and the attractiveness of facilities like ATTOLAB and LASERIX, providing essential and presently missing advanced instrumentation at the interface between sources and user stations, and will be crucially important for a new generation of projects like LUNEX5. This instrumentation will make it possible to fully manipulate the temporal/spectral and spatial properties of XUV light beams according to the experimental needs, while preserving their unique characteristics (ultra-broadband coherence and high peak brightness). This synergetic effort will make optimal use of existing knowhow and resources, providing a broad scientific community with instruments and technological solutions otherwise non accessible to small research groups, will increase the visibility of the Campus and will train young scientist in a rapidly developing field. 1 Table des matières IDEX Paris-Saclay ..................................................................................................................................... 1 APPEL A PROJETS RECHERCHE 2014........................................................................................................ 1 Introduction – overall presentation of the project ................................................................................. 5 1 2 Ultrafast Science with XUV light (J.M. Mestdagh, A. Klisnick, + ....) ................................................ 5 1.1 Physics, chemistry and biology in the gas phase ....................................................................... 5 1.2 Physics, chemistry and biology in the condensed phase ........................................................... 5 1.3 Plasmas ...................................................................................................................................... 5 1.4 The XUV sources - characteristics : HHG, XRL, FEL .................................................................... 5 1.4.1 High harmonic sources ....................................................................................................... 6 1.4.2 X-ray laser (Sophie) ............................................................................................................. 6 1.4.3 Free Electron Laser (David) ................................................................................................. 7 State-of-the art ................................................................................................................................. 8 2.1 2.1.1 International – National (Marino - Rodrigo) ....................................................................... 8 2.1.2 Local (Franck instrumentation) ........................................................................................... 9 2.2 3 Existing Tools and User communities ........................................................................................ 8 What is missing and needed in Paris-Saclay campus (Danielle) .............................................. 15 2.2.1 Structuring and maintaining high level expertise ............................................................. 15 2.2.2 Technical needs ................................................................................................................ 15 2.2.3 Needs in training ............................................................................................................... 15 Objectives ....................................................................................................................................... 16 3.1 Structuring objectives in the perspective of UPS (Marino) ..................................................... 17 3.2 Technological objectives (Marino)........................................................................................... 17 3.3 Training (Sophie K) ................................................................................................................... 17 3.3.1 Maintaining expertise ....................................................................................................... 17 3.3.2 Existing involvement/actions in training .......................................................................... 17 3.3.3 Future actions in training .................................................................................................. 17 3.4 Academic dissemination (Danielle).......................................................................................... 17 3.4.1 existing actions ................................................................................................................. 17 3.4.2 Interest and future actions ............................................................................................... 18 3.5 industrial dissemination : technological transfer .................................................................... 18 3.5.1 Existing joint actions and projects .................................................................................... 18 3.5.2 Interest and future actions ............................................................................................... 18 3.6 Scientific benchmark studies (all) ............................................................................................ 18 3.6.1 atto time-resolved study in gas phase (Bertrand C, …) .................................................... 18 3.6.2 PI and polarization control – chirality (Danielle D, L. Nahon, T. Ruchon) ......................... 19 3.6.3 atto time-resolved study in solid (Marino) ....................................................................... 20 3.6.4 as-fs Ultrafast Phenomena at a nanometer scale (Hamed M) ......................................... 20 2 3.6.5 fs-ps timescale WDM (Annie K) ........................................................................................ 22 3.6.6 application bio (Philippe Z. to be discussed and selected) ............................................... 22 3.7 4 3.7.1 Technical ........................................................................................................................... 23 3.7.2 Training and Dissemination .............................................................................................. 23 Methodology and work plan........................................................................................................... 23 4.1 Overall technical objectives .............................................................................................. 28 4.1.2 2 year deliverables ............................................................................................................ 31 Overall technical objectives .............................................................................................. 32 4.2.2 2 year deliverable ............................................................................................................. 35 WP3: On-line diagnostics of spectro-temporal properties (A. Klisnick + D. Garzella +....) ...... 36 4.3.1 Overall technical objectives .............................................................................................. 36 4.3.2 2 year deliverables ............................................................................................................ 38 4.4 WP4: On-line diagnostics of spatial properties and polarization (Ph. Zeitoun + ...) ................ 39 4.4.1 Overall technical objectives .............................................................................................. 39 4.4.2 2 year deliverables ............................................................................................................ 42 4.5 WP5: Off-line optics metrology and detector development (F. Polack + F Mercier +...) ........ 43 4.5.1 technical objectives .......................................................................................................... 43 4.5.2 2 year deliverables ............................................................................................................ 43 4.6 WP6: Training (Sophie) ............................................................................................................ 43 4.6.1 Funding PhD theses, internships, ..................................................................................... 43 4.6.2 Training modules for students in the labs ........................................................................ 43 4.6.3 Website for training in XUV optics.................................................................................... 43 4.7 7 WP2: Control of spatial profile and polarization (F. Polack + ....) ............................................ 32 4.2.1 4.3 6 WP1: Control of the spectro-temporal profile (F. Delmotte + ...) ........................................... 28 4.1.1 4.2 5 2 year deliverables (Marino) .................................................................................................... 22 Gantt chart for WPs ................................................................................................................. 43 Consortium and financial request................................................................................................... 44 5.1 Consortium description (Danielle) ........................................................................................... 44 5.2 Governance (Danielle) ............................................................................................................. 44 5.3 financial request (Bertrand)..................................................................................................... 44 References ...................................................................................................................................... 48 6.1 External .................................................................................................................................... 48 6.2 OPT2X Consortium ................................................................................................................... 52 Annex .............................................................................................................................................. 59 7.1 XUV source characteristics ...................................................................................................... 59 7.2 French teams in ultrafast dynamics ......................................................................................... 59 7.3 XUV HHG sources ..................................................................................................................... 60 7.4 Funded projects ....................................................................................................................... 61 3 7.5 Training activity........................................................................................................................ 61 7.6 Industrial Partnership - letters of interest ............................................................................... 61 7.6.1 Horiba (FP) ........................................................................................................................ 61 7.6.2 Amplitude Techno (BC) ..................................................................................................... 61 7.6.3 Fastlite (BC) ....................................................................................................................... 61 7.6.4 EOTECH (FP) ...................................................................................................................... 61 7.6.5 Imagine Optics (HM) ......................................................................................................... 61 7.6.6 Phase view ?...................................................................................................................... 61 7.6.7 ............................................................................................................................................... 61 4 Introduction – overall presentation of the project 1 Ultrafast Science with XUV light (J.M. Mestdagh, A. Klisnick, + ....) 1.1 Physics, chemistry and biology in the gas phase 1.2 Physics, chemistry and biology in the condensed phase 1.3 Plasmas The scientific motivation of the proposed technical developments is to contribute to the understanding of matter heating induced by intense XUV radiation, and of the induced non-equilibrium transition phase from solids to the Warm Dense Matter (WDM) to dense strongly coupled plasmas (DSCP), through the investigation of the radiative emission .properties of the heated sample. The primary process for the energy deposition is direct photoionization of the solid by the incident XUV pulse, with a strong dependence with respect of the energy (wavelength) of the photons. Our particular interest is to investigate X-ray emission from hole states transitions rather than usual resonance lines. Due to the high autoionization probability associated with core hole states, emission originating from tcore holes is only possible on a femtosecond timescale. Therefore, it is not sensitive to low density recombining regimes that usually mask interesting high density features. We intend to use state-of-the art ASE XUV lasers operating at photon energies 89 eV and above, in a range of focused energy/duration that complements those already achieved with XUV Free Electron Lasers (see eg Dzeldzainis et al HEDP 6 (2010) 109; Zastrau et al Laser And Particle Beams 30 1 (2012) 45-56 ). Current ASE XUV lasers, delivering µJ, few ps pulses, will allow to investigate interaction in the 10 12 - 1013 W/cm2 range, while limiting the loss of density due to plasma expansion. Higher focused intensities (1014 W/cm2 and above) and shorter pulse duration (100 fs and below), approaching XUV FELs ones, are foreseen in a near future with the progress of seeded XUV lasers, which will be implemented at LASERIX and also investigated at the Apollon-CILEX facility. However the implementation of these experiments requires the development of specific advanced instrumentation to control and characterize the XUV intensity focused on the solid sample, on a single-shot basis. Namely, control of focusing with micrometer size (NB: we do not want very small focal spots, since we want to study the emission of the heated sample) Note: required parameters to reach a focused intensity of 1014 W/cm2 duration 1 ps: 100µJ in 10µm (diam) focal spot; 25µJ in 5µm (diam) focal spot duration 100 fs: 8µJ in 10µm (diam) focal spot; 2µJ in 5µm (diam) focal spot 1.4 The XUV sources - characteristics : HHG, XRL, FEL The XUV radiation which is considered in OPT2X has two main characteristics: It covers the extreme-UV spectral range between 100 nm (12 eV) and a few nm, including the water window (2.34 - 4.4nm / 280-530 eV), that we extrapolate to 1 nm (1200 eV) for the sake of definiteness. It has good temporal/spectral (longitudinal) and spatial coherences, respectively, in the following sense. If one component of the electric field is written as the complex quantity: ⃗ ⃗ , 𝝎)𝒆+𝒊(𝒌∙𝒓⃗−𝝎𝒕) 𝒅𝟑 ⃗𝒌𝒅𝝎, ̃𝑿𝑼𝑽 (𝒌 ⃗ , 𝒕) = |𝓔𝑿𝑼𝑽 (𝒓 ⃗ , 𝒕)|𝒆+𝒊𝝓(𝒓⃗,𝒕) = ∬ 𝓔 Eq 1 𝓔𝑿𝑼𝑽 (𝒓 ⃗ =𝒌 ⃗ (𝜔), the 𝝓(𝒓 ⃗ , 𝒕) phase in the space-time domain – and with the given dispersion relation 𝒌 ̃ ⃗ ⃗ ̃ equivalently the 𝝓(𝑘, 𝜔) phase of 𝓔𝑿𝑼𝑽 (𝒌, 𝝎) in the reciprocal wave vector-frequency, or spectral domain -, vary regularly enough with, respectively, space and time, wave vector and frequency over the full spectral bandwidth of the light field. As a result, amplitude and phase can be measured and, 5 very importantly, controlled and shaped in order to control and possibly optimize the conditions of their interaction with the system under study. Although they may be intrinsically combined, it is usual and convenient to consider separately the temporal/spectral and spatial properties of the XUV radiation, and their subsequent control. This partition is adopted in the presentation and technical developments of the OPT2X project where, on the one hand, different types of XUV beamline with different properties are involved, and, on the other hand, the requirements of the scientific applications are different, addressing in priority either the temporal or the spatial characteristics of the XUV light. It is however central that an overall and consistent program of characterization and control be jointly supported in the project. Three types of XUV sources and radiation are considered in OPT2X. 1.4.1 High harmonic sources Laser-driven high harmonic generation (HHG) in either gas medium or plasma is today one of the main sources of coherent ultrashort light pulses in the XUV range. Based on laser-induced nonlinear polarization of bound electrons (atoms & molecules in gas medium) or free electrons (plasma), harmonic emission covers a large spectral range of which extension scale as the ponderomotive potential 𝑈𝑝 ∝ 𝐼𝐿 𝜆2𝐿 , where IL and λL are the driving field intensity and wavelength (at λL =800 nm (3µm) and IL =1014 W/cm2, Up~6 eV (90 eV)). In the time domain, when driven by a multi-cycle laser pulse, the emission takes the form of a train of attosecond pulses, of duration between a few 10 and 100 as. In the spectral domain, this corresponds to a discrete comb of odd harmonics (q-order “overtones”) of the driving frequency. One can produce isolated atto pulses either using a time gate [Baltuska03, Sola04] or exploiting spatial dispersion of attosecond emission in the attolighthouse scheme, proposed and demonstrated by the OPT2X partners [Vincenti12], in plasma [Wheeler12] and gas [Kim13] (in collab. with NRC Ottawa). One can use harmonic light in either the “femtosecond mode”, after appropriate selection of a narrow spectral width (ΔE/E~10-3 in the XUV range), or the attosecond mode, keeping a large spectral width (ΔE/E~1). In the NL process, the harmonic light inherits coherence properties of the driving field, however with important restriction and specific features. The XUV emission displays a temporal linear chirp (quadratic spectral phase) at the fs timescale (~100 meV bandwith, DE/E~10-3) and as timescale (~10 eV bandwith), due to a nonlinear dipole phase: ̃ (𝝎; 𝒓 ̃ 𝑳 (𝝎𝑳 ; 𝒓 ̃ 𝒅𝒊𝒑 (𝝎; 𝑰𝑳 ), ⃗ , 𝒕) = 𝒒𝝓 ⃗)+𝝓 Eq 2 𝝓 where ω=qωL, 𝜙̃𝐿 (𝜔𝐿 ; 𝑟, 𝑡) is the driving laser phase, 𝜙̃𝑑𝑖𝑝 (𝜔; 𝐼𝐿 ) the intensity-dependent nonlinear dipole phase (slow variations of 𝜙̃ phase with time and space, e.g., through 𝐼𝐿 (𝑟, 𝑡), are still described with (𝑟, 𝑡) variables rather than in the reciprocal space). Eq 2 illustrates that the phase properties of the XUV field are deterministically fixed by the generation conditions, that they can be partially controlled through the laser driving field, but that the key for control and shaping is the accurate characterization of phase in the spectral domain and in space. HHG emission is perfectly synchronized with the driving field at the attosecond optical cycle scale, at high repetition rate (1-10 kHz currently achieved, 1 MHz possible [Rothhardt]). 1.4.2 X-ray laser (Sophie) The X-ray laser (XRL) results of population inversion and lasing transition in either underdense plasma in gas target [Sebban] or overdense plasma on solid target [Laserix]. According to the high linear gain (>> 100 cm-1) at central frequency, the XRL has extremely narrow spectral width ΔE/E~105 in the XUV range, corresponding to pulse duration of ~1 ps close to Fourier limit. Several XRL schemes have been demonstrated. A very efficient one combines grazing incidence pumping (GRIP) (gain pumped by progressive wave in plasma on solid target) and XRL injection with a coherent XUV seed at the XRL wavelength, e.g., provided by narrow band harmonic emission. Injected XRL achieves high spatial coherence and high quality wavefront, as well as fs synchronization with an external laser source. The XRL in Ne-like and Ni-like metallic ions now densely covers the XUV range down to the water window, with output energy in the µJ range at 10 Hz repetition rate. Highly monochromatic 6 XRL is particularly adapted to time-resolved studies at high XUV intensity, e.g., in biological applications [Lacombe] and warm dense matter studies [xxx], time-resolved coherent imaging [xxx]. 1.4.3 Free Electron Laser (David) The Free Electron laser (FEL) has demonstrated extraordinary performances, e.g., at LCLS facility delivering pulses of 1 mJ energy and 5-20 fs duration at 200 eV-1 keV photon energy (Å wavelength range) and 100 Hz -1 kHz repetition rate (David, check). The FEL achieves high transverse (spatial) coherence which has been exploited in coherent imaging applications. In the SASE mode, the longitudinal (temporal) coherence is still limited. It can be drastically improved by seeding the FEL with an external source [xxx]. Seeding of FEL in the XUV range has been first demonstrated at 160 nm (5th harmonic of Ti:S laser generated in gas) at SCSS-Spring8 [Lambert08], and SPARC [Giannessi08], both experiment involving OPT2X partners. External seeding has been extended to 60 nm (13 th harmonic of Ti:S laser generated in gas [Togashi11]), and is currently implemented on several FEL (SFLASH, SACLA, … ?). Besides seeding, another crucial step will be reached with the injection of FEL by laser-accelerated electrons. Laser wake field acceleration (LWFA) of electrons in plasma, up to several GeV, constitutes one of the main programs of the CILEX Equipex to be installed on the ParisSaclay campus, in synergy with the LUNEX5 project (free electron Laser Using a New accelerator for the Exploitation of X-ray radiation of 5th generation). This scientific effort has been supported by three ERC advanced grants (V. Malka at LOA (2), M.-E. Couprie at SOLEIL). Basic characteristics of coherent XUV sources, HHG in gas and plasma, XRL, FEL are summarized in Table 1, as well as for standard SR beamline. Specifically, indicative numbers of photons delivered by HHG and XRL are plotted in Figure 1. HHG Plasma HHG Gas HHG Gas XRL SR FEL LOA Salle Noire SLIC ATTOLAB NIR SLIC ATTOLAB MIR LASERIX SOLEIL METROLOGY LUNEX5 lambda minmax (nm) Ephot min-max (eV) duration minmax (fs) Bandwith minmax (eV) Energy/pulse min-max (nJ) reprate 5-100nm 5-100nm 1-100nm 2-20nm 2-100nm 1-100nm 12-250 eV 12-250 eV 12-1200 eV 60-620 eV 12-620 eV 12-1200 eV 0,1-10fs 0,1-10fs 0,1-10fs 1ps 30ps 1-30fs 30meV-3eV 30meV-3eV 30meV-3eV 0,3meV 0,1meV 10-300meV 10nJ-10µJ 1nJ-1µJ 1nJ-1µJ 1µJ 1pJ 1µJ-1mJ 1,E+03 1,E+04 1,E+03 1,E+01 1,E+08 1,E+03 Nphot/sec minmax 3,E+11-5,E+15 3,E+11-5,E+15 5,E+09-5,E+14 1,E+11-1,E+12 1,E+12-5,E+13 5,E+14-5,E+16 Table 1 : Basic characteristics of coherent XUV sources, HHG in gas and plasma, XRL, FEL 7 12 15 10 10 Nb Photons / sec Nb Photons / pulse X-ray laser (10 Hz reprate) 9 10 HHG driving laser (10 kHz) wavelength / energy / duration 0.8 µm / 2 mJ / 20 fs 3.0 µm / 1 mJ / 40 fs 6 10 X-ray laser (10 Hz reprate) 12 10 HHG driving laser (10 kHz reprate) 9 10 wavelength / energy / duration 0.8 µm / 2 mJ / 20 fs 3.0 µm / 1 mJ / 40 fs 3 6 10 10 0 500 1000 1500 2000 0 Photon energy (eV) 500 1000 1500 2000 Photon energy (eV) Figure 1 : typical numbers of photons delivered, respectively, in 0,1% bandwidth (~100 meV) for HHG, in full BW for XRL, a) per pulse, b) per second. For HHG in the mid-IR (3µm), the numbers are extrapolated from [Popmintchev12] 2 State-of-the art 2.1 Existing Tools and User communities 2.1.1 International – National (Marino - Rodrigo) 2.1.1.1 HHG (Rodrigo) [LOA-Palaiseau] http://loa.ensta.fr/ [CLF-RAL-Oxford] http://www.clf.rl.ac.uk/Facilities/Artemis/12270.aspx [ETH-Zürich] http://www.ulp.ethz.ch/research/research_overview [IC-London] http://www.imperial.ac.uk/research/qols/ [ICFO-Barcelona] http://www.icfo.es/index.php?section=research5&lang=english [IMS-Ottawa] http://www.nrc-cnrc.gc.ca/eng/research/physics.html [JILA-Boulder] http://jila.colorado.edu/kmgroup/ [KAIST-Daejeon] http://www.kaist.ac.kr/english/03_academics/02_research.php [LLC-Lund] http://www-llc.fysik.lth.se/ [MPQ-Garching] http://www.attoworld.de/ [MPIK-Heidelberg] http://www.mpi-hd.mpg.de/ullrich/page.php?id=25 [MBI-Berlin] http://www.mbi-berlin.de/en/research/program/atoms/index.html [PoliMi-Milano] http://www.fisi.polimi.it/dip-fisica/page167.do [TUV-Vienna] http://atto.photonik.tuwien.ac.at [RIKEN-Tokyo] http://www.riken.jp/lab-www/mid-lab/untitled1-e.html [AMOLF-Amsterdam] http://www.amolf.nl/research/xuv-physics/ [ALLS-Toronto] http://lmn.emt.inrs.ca/EN/ALLS.htm [KSU-Kalamazoo] http://jrm.phys.ksu.edu/exp-research-grps.html [OSU-Colombus] http://www.physics.ohio-state.edu/~dimauro/ [IOPCAS-Beijing] http://english.iop.cas.cn/ 8 2.1.1.2 Laser X (Sophie K.) There are quite a few laser installations in the world dedicated to the applications of soft x-ray lasers. Among them: 1) Colorado state university, Rocca’s team 2 capillary discharges x-ray lasers 46 nm 1 Hz 1 mJ 1 ns (non seeded) 1 Ti:Sapph laser until 10 J pumping x-ray lasers down to 8 nm at 1 Hz (seeded) 1 XRL pumped by diode pumped laser with rep rate 100 Hz (non seeded) 2) PALS Inside the laserlab network offers a quasi steady state x-ray laser at 21,2 nm with the highest energy per pulse in the world (up to 10 mJ) relatively long pulse duration (100 ps) and no more than 3 pulses per hour. 3) APR Japan soft x ray laser at 13,9 nm, spatially coherent thanks to double target scheme (a first x-ray laser plays the role of an oscillator and is sent to a second amplifier one). These are the only installations open to users for applications to our knowledge. Otherwise LOA (Palaiseau France in the OFI scheme), Bern University, Tewallas (Roumania), MBI (Berlin Germany), GSI PHELIX (Darmstadt Germany), APRI GIST (Korea) develop their own source. 2.1.1.3 FEL (Marino – MEC – David G) LCLS FLASH SACLA FERMI LUNEX5 ? Swiss FEL 2.1.2 Local (Franck instrumentation) The large community of scientists involved in the research on sources, instrumentation and applications of XUV radiation positions the Paris-Saclay Campus as a national leader in these new technologies. The local interest is reinforced by the presence of large scientific facilities, such as SOLEIL, Equipex CILEX project and the future LUNEX5 project. The present project OPT2X aims at sharing of scientific and technological skills and equipment and will contribute significantly to strengthen the scientific impact of the Paris-Saclay community and the attractiveness for young French and foreign researchers in this field. We describe in the following paragraphs the state-of-theart of the ultrafast sources and XUV instrumentation already existing on Paris-Saclay campus. 2.1.2.1 Ultrafast XUV sources available in Paris-Saclay Campus Paris-Saclay campus gather in the same area a number of ultrafast coherent XUV sources that are internationally renowned and that have produced several high-impact scientific results in these last ten years. In 2001, SPAM was the first laboratory to observe and characterize an attosecond pulse train with a High Harmonics Generation source. [Paul2001] In 2004, the LOA produced the first highintensity highly coherent soft X-ray femtosecond laser seeded by a high harmonic beam. By combining the high optical quality available from high-harmonic laser sources (as a seed beam) with a highly energetic soft X-ray laser plasma amplifier, they produced a tabletop soft X-ray femtosecond 9 laser operating at 10 Hz and exhibiting full saturation, high energy, high coherence and full polarization. [Zeitoun2004] LASERiX -> The first XUV source facility fully dedicated to users… The LASERIX facility of the Paris South University is composed of a pettawatt class laser system fully dedicated to the development of advanced x-ray laser schemes and their applications. The installation is run by 4 assistant professors together with 4 engineers and technicians specialized in laser technology, electronics and computing. As a member of Laserlab network, LASERIX already offers beam-time directly using the XUV laser generated at 10 Hz from solid target (8 weeks per year). The visitor teams are concerned either by the soft x ray laser generation understanding and improvement or by the XUV beam as a pump or probe beam. As compared to high harmonic source, the XUV beam provided by soft x ray laser in transient collisional pumping is highly monochromatic, can range the microjoule energy level per pulse at 10 Hz and when seeded by harmonics has a regular spatial profile with low divergence (typically 1 mrad). Up to now, the pulse duration is close to 1 ps, of the order of the Fourier transform limit due to the spectral profile. Active research will be carried out to overcome this limit and reduce the pulse duration of soft x ray lasers, making them competitive sources as regards to advanced X-FEL sources. The XUV beam line that will be proposed to the user community will consist of a seeded x-ray laser at various wavelengths from 32,6 to 10 nm. An additive synchronized beam at the femtosecond scale will be proposed if required: femtosecond infrared up to 50 mJ per pulse or high harmonic beam. A large set of XUV imaging and focussing devices based on multilayer optics is proposed. The diagnostics already existing on the beam are: energy characterization with calibrated photodiode, near and far-field imaging, spectrum. The improvements that will be due to OPT2X project are temporal characterization, strong focussing. The development of ultrafast XUV sources within Paris-Saclay campus is supported by national and regional programs, as Equipex CILEX and ATTOLAB or SESAME ATTOLITE. These state-of-the-art sources, which are (or will be soon) available for Paris-Saclay scientific community, are listed in the table below, with their main characteristics and applications. Tableau à compléter/harmoniser avec la proposition de BC pour la partie 1.4 XUV Sources fs HHG gaz as HHG solid ASE XRL OFI seeded XRL solid ASE Spectral Energy per duration range pulse 10-40 LOA 1 à 50 nJ 20 fs nm 1 µJ 10 - 100 @32nm,20 SPAM 10 fs nm Hz 0.1µJ @1kHz 10 - 100 100 as SPAM few nJ nm (trains) 10 µJ 20 - 70 @60nm SPAM 10 fs nm expected 100µJ 30 - 40 LOA 30-40 nJ 5 ps nm 30 - 40 LOA 1 µJ 5 ps nm 10 - 30 LIXAM nm 1 µJ (prévu LASERI 1 - 10 ps (7-30 1-100 µJ) X nm) Loc. Rep. rate Spatial quality Main applications 1 kHz 10 Hz 1 kHz Div : 0.5mrad Source : 50µm 1 kHz qq Hz A compléter A compléter Div : 15-20 mrad Quasigaussien A compléter 10 Hz 10 Hz 10 Hz (0,1Hz) Div : qq mrad modulations A compléter 10 2.1.2.2 Optical components and systems for ultrafast XUV sources The study and the development of advanced XUV optical components (mirrors, detectors, filters, polarizers…) and systems (interferometers, imagers, monochromators, wavefront sensors…) for XUV ultrafast sources is essential in order to achieve XUV beamlines accessible to users. Moreover, the needs of these users give directions to the academic research required on the new materials and new technologies in order to achieve such instruments. We give below some examples of research and developments achieved by the Paris-Saclay scientific community related to optical components and systems for ultrafast studies in the XUV spectral range. These instrumental developments recently supported by local and national research networks (Triangle, PALM, ANR) illustrate the diversity and importance of this thematic within Paris-Saclay campus. They also show the huge amount of knowledge and knowhow existing in Paris-Saclay Campus that the OPT2X project aims at federate. XUV multilayer mirrors One of the pioneers in coatings for optics in the extreme ultraviolet (~ 10-60 nm), the "XUV Optics" team of Laboratoire Charles Fabry (LCF) studies and optimizes interferential mirrors based on multilayers since more than 25 years for several applications. A rather unique specificity of LCF is that it controls all the skills required for the development of optical components in the XUV spectral range: aspherization of super-polished surfaces, multilayer design, nanometric and sub-nanometric layer deposition and interferometric characterization. These skills have been applied in the past for the production of solar observation telescopes embedded in programs of ESA and NASA ( SOHO mission in 1992 and STEREO in 2003 ), [Howard] to achieve the unique Fourier-transform spectrometer that operates down to wavelengths as short as 40 nm (collaboration with SOLEIL) [DeOliveira] and more recently to provide X-ray diagnostics based on aperiodic multilayer mirrors for Laser MegaJoule plasma imaging and spectrometry [Maury, Bridou]. Concerning optics for ultrafast XUV sources, several specific multilayer components have been designed and produced in these last years: - Narrowband multilayers with enhanced spectral purity in order to select on harmonics in the HHG spectrum and to reject the VUV light. These optics provided for the RTRA project DYNELEC (LCAM‐LIXAM‐SPAM), have required the design of a specific XUV anti-reflection coatings on top of the multilayer [Billaud]. (see figure below) - XUV beamsplitters for Michelson interferometry. Due to material absorption in the XUV, efficient beamsplitters have been produced by deposition of multilayers on very thin silicon nitride membrane (about 80 nm thick) (collaboration LCF-LOA) [Delmotte2002] - Multilayer Optics for attosecond pulses. The first broadband multilayer mirrors for attosecond sources have been designed and produced in Paris-Saclay campus (coll. LOA-LCF) in 2006 [Morlens]. More recently, mirrors with control dispersion phase have been developed in order to transport or compress attosecond pulses. [Bourassin2011] This research has been supported by ANR project “Attomix” (coll. LCF-LCPMR) and RTRA project “Atto-Optique” (coll. LCF-SPAM). We have demonstrated that Pulse compression down to 50 as can be reached with broadband multilayer mirrors [Bourassin2012] 11 Figure 2: (a) Scheme of high-order harmonic generation (HHG) (b) Illustration of the spectral selectivity of the multilayers mirrors: HHG wavelength spectra measured without mirror (black full line), measured with one mirror (pink full line) and deduced for two mirrors (violet full line). (from [Billaud]) EUV Polarizer and Polarimeter The control and the characterization of the polarization of EUV ultrafast pulses are essential for many applications. For instance, the study of ultrafast demagnetization dynamics by using XUV magnetic microscopy required circularly polarized light whereas the HHG process in rare gas generates linearly polarized light. In order to overcome this difficulty, the LOA has designed and developed an EUV polarizer based on a four mirror setup (see figure below). Each mirror introduces a phase-shift between the s and p component of the electromagnetic wave. By adjusting the direction of polarization of the incoming wave and by optimizing the angles of incidence on the mirrors, one can get the s and p components with equal intensity and dephased by pi/2. This system has been optimized for a 20 nm wavelength. They have demonstrated a degree of circular polarization equal or close to 100 % for harmonics in the wavelength range on 18 to 26 nm and a total efficiency around 4 %. [Vodungbo] The setup is also equipped with an analyzer that consists of a multilayer mirror working at Brewster angle (i.e. close to 45° in the EUV spectral range) and a detector. Thus, the all setup can be used as a polarimeter in order to characterize the ultrafast pulse polarization state. This development has been supported by RTRA project IMMAGE (col. LOA-SPAM) and by ANR project FEMTO-X-MAG (col. LOA-SPAM-SOLEIL-LCPMR). Figure 3: Setup layout showing the production of the harmonics in a neon filled gas cell, the polarizer, the spectrometer, the analyzer and the CCD camera. From [Vodungbo] XUV interferometers Fresnel bi-mirror A compléter : principe -> FD 12 Applications -> AK ? Wavefront sensors (à compléter par PZ ?) 2.1.2.3 The CEMOX platform The CEMOX platform (Centrale d’Elaboration et de Métrologie d’Optiques XUV) has been created ten years ago as a join equipment between LIXAM (now ISMO) and LCF with several other partners: LURE (and then SOLEIL), CEA SPAM, CEA DAM, LOA. The main objective was to provide the community with state-of-the-art XUV optics. The initial platform included magnetron sputtering deposition systems (implanted in the LCF clean room) and a EUV plasma source reflectometer (implanted at ISMO). In 2008, CEMOX becomes a platform af LUMAT federation. In 2010, a new X-ray reflectometer, financially supported by Conseil Général de l’Essonne and ANR, was added to the platform. The different partners have used the CEMOX platform in a large number of research projects, including 3 ANR projects and 4 projects RTRA Triangle de la Physique. In total, more than 100 multilayer optics have been designed and deposited for specific applications. In addition to the project related to ultrafast XUV sources that we have already mentioned before, multilayer optics for other applications have also been produced. The main projects are the following: - Projets RTRA “Multicouche2D” (LCF‐SOLEIL): study and optimization of a new type of monochromator based on alternate multilayer grating. [Polack] - Design and production of aperiodic multilayer coatings for imaging diagnostics on LMJ (CEA DAM – LCF) [Maury] - Design and development of aperiodic multilayer coatings for spectrometry diagnostics on LMJ (CEA DAM – LCF) [Bridou] - ANR blanc “TPLUS”: Design and development of a tunable EUV laboratory source (LCPMR‐LCF) - Coating and calibration of multilayer optics at 17.5nm for SWAP instrument (Sun Watcher using Active pixel detector and imaging Processing) onboard PROBA‐2 satellite (ESA mission, collaboration CSL). - Coating and calibration of multilayer optics at 30.4nm for HECOR instrument (Helium Coronograph) onboard Herschel sounding rocket mission (NASA mission, collaboration NRL and IAS). - Coating of multilayer mirrors for ondulator diagnostic DIAGON for synchrotrons SOLEIL, DIAMOND and ALBA. [Desjardins] In 2014, the CEMOX platform will benefit from a new localization (in Institute d’Optique building at Palaiseau) and a new deposition facility for multilayer coating on large optics. This new plateform project is supported by region Ile de France (SESAME project CeMOX) and Equipex projects ATTOLAB and MORPHOSCOPE. 2.1.2.4 Simulation tools for optical design Several laboratories in Paris-Saclay have developed specific skills in the use of commercial simulation and optimization tools for optical design or thin film design: Thin Film Calculation, ... à compléter. Due to some particularities of the XUV spectral range, specific codes have been developed: - ROSA software: “Reflective Optical Systems for Attopulses”. 3D simulation of attosecond pulses after reflection on an optical component, by Charles Bourassin-Bouchet. - CARPEM : à completer par FP ? - … à completer par TOUS 13 2.1.2.5 Metrology for XUV components Metrology : SOLEIL – Optic Group The national synchrotron light source is both a research laboratory and a large research equipment welcoming 2,500 scientists per year over the 20 lines currently operating light, and employing 350 people. SOLEIL claims a dual purpose: to provide users with experimental devices at the highest international level and to conduct advanced scientific and technological research around the synchrotron source. Since 2002, the Optic Group of SOLEIL is responsible of all synchrotron beamlines. Its skills cover all the sequence from the general design of the beamline to the final instrument settings. The Optic group has developed its own simulation tools for instrumental design and a metrology lab in a clean room at controlled temperature for the control of optical surfaces. The main equipment available for the metrology of XUV optical component are : − phase‐shift interferometric microscopes for optical surface characterization − Atomic force microscpy (AFM) for atomic level surface characterization and metrology of etched patterns (e.g. gratings). − Reflectometer in the wavelength range 1 to 40 nm (Metrology beamline, XUV branch) Other facilities are also accessible in the other laboratories of Paris-Saclay: − Reflectometer in the wavelength range 10 to 50 nm (CEMOX EUV Reflectometer) - … à compléter: [Howard] R. A. Howard et al., “Sun Earth Connection Coronal and Heliospheric Investigation (SECCHI)”, Space Science Reviews 136, 67 (2008). [Maury] Maury H., Bridou F., Troussel P., Meltchakov E., Delmotte F., “Design and fabrication of supermirrors for (2-10 keV) high resolution X-ray plasmas diagnostic imaging”, Nucl. Instr. and Meth. in Phys. Res. A 621, 242-246 (2010) [Bridou] F. Bridou, F. Delmotte, Ph. Troussel, B. Villette, “Design and fabrication of X-ray non-periodic multilayer mirrors: Apodization and shaping of their spectral response”, Nucl. Instr. and Meth. in Phys. Res. A 680, 69-74 (2012) [Delmotte2002] F. Delmotte; MF. Ravet; F. Bridou; F. Varniere; P. Zeitoun; S. Hubert; L. Vanbostal; G. Soullie, “X-ray-ultraviolet beam splitters for the Michelson interferometer”, Appl. Opt. 41, 5905 (2002). [Morlens] A.S. Morlens, R. Lopez-Martens, O. Boyko, P. Zeitoun, P. Balcou, K. Varju, E. Gustafsson, T.Remetter, A. L’Huiller, S. Kazamias, J. Gautier, F. Delmotte and M.F. Ravet, “Design and characterization of extreme ultraviolet broadband mirrors for attosecond science”, Optics Letters 31, 1558-1560 (2006). [Bourassin2011] Bourassin-Bouchet C., Diveki Z., De Rossi S., English E., Meltchakov E., Gobert O., Guénot D., Carre B., Delmotte F., Salières P. and Ruchon T., “Control of the attosecond synchronization of XUV radiation with phase-optimized mirrors”, Optics Express 19, 3809 (2011) [Bourassin2012] Bourassin-Bouchet C., De Rossi S., Wang J., Meltchakov E., Giglia A., Mahne N., Nannarone S., Delmotte F., “Shaping of single-cycle sub-50-attosecond pulses with multilayer mirrors”, New J. Phys. 14, 023040 (2012) 14 [Vodungbo] B. Vodungbo, A. Barszczak Sardinha, J. Gautier, G. Lambert, C. Valentin, M. Lozano, G. Iaquaniello, F. Delmotte, S. Sebban, J. Lüning, and P. Zeitoun, “Polarization control of high order harmonics in the EUV photon energy range”, Optics Express 19, 4346-4356 (2011) [Dobosz] S. Dobosz, H. Stabile, A. Tortora, P. Monot, F. Reau, M. Bougeard, H. Merdji, B. Carre, Ph. Martin, D. Joyeux, D. Phalippou, F. Delmotte, J. Gautier, and R. Mercier, “Internal frequency conversion extreme ultraviolet interferometer using mutual coherence properties of two high-orderharmonic sources”, Rev. Sci. Instrum. 80, 113102 (2009) [Zeitoun2004] Ph. Zeitoun et al., Nature 431, 426-429 (2004) 2.2 What is missing and needed in Paris-Saclay campus (Danielle) 2.2.1 - Structuring and maintaining high level expertise positionnement et enjeux stratégiques au niveau national et international The advent of ultrafast science has made it possible to study the properties of matter in out of equilibrium conditions, opening new pathways for the study and the control of basic phenomena governing the behaviour of atoms, molecules, plasma and condensed matter. The Paris-Saclay campus presents an intense activity in this domain, with a strong presence of world-class research groups active in these fields and a concentration of ultrafast light sources which is second to none at the international level, for the number, variety and quality of its installations. Nevertheless, a gap needs to be bridged between the laser-based sources and the extended community of their users, in particular in the XUV domain. Ultrafast science requires ultra-steep gradients in time – down to the fs and as time scale – and in space – down to the Å scale – to coherently excite electronic/nuclear wave packets in a controlled manner, and to probe their temporal evolution. These gradients are ideally provided by fully controlled photon beams, from the mid-IR to the XUV range: the manipulation of light pulses is therefore an essential component of ultrafast science. While in the optical wavelength region light manipulation can be performed with methods accessible to individual researchers, in the XUV domain it requires a very specific and intense effort that is usually beyond the possibilities of small groups. Namely, it requires entirely new techniques of metrology and shaping; much more expensive, custom designed optical elements; and a more sophisticated and diverse knowhow. The OPT2X proposal aims at filling this gap by creating a synergetic effort to optimise the XUV ultrafast pulses available at the advanced facilities present in the Paris-Saclay campus – in particular at the recently funded AttoLab Equipex, at the recently completed Laserix sources, and at the LUNEX5 project. This effort will provide strongly needed and still missing advanced instrumentation between the XUV ultrafast sources and the user stations, to fully exploit the potential of the facilities and to reaffirm the international visibility of Paris-Saclay in a highly competitive field. The scientific and technological knowhow necessary to undertake this task is present on the Paris-Saclay campus ; nevertheless, it needs additional resources to have access to advanced technological elements and to realize efficient and reliable instruments, with the main goal of delivering usable and well characterized photons to the experimental stations. 2.2.2 Technical needs 2.2.3 Needs in training 15 3 Objectives Our main goal is the establishment of a transversal technical and scientific group capable of designing and implementing optimized beamlines for XUV ultrafast sources. This will be achieved thanks to a joint effort of the light source and user communities, together with expert groups in XUV optics active in technological platforms, and it will be constituted by an “OPT2X team”, mixing scientist and engineers that will keep cooperating - in continuous interaction with the ultrafast science community - well beyond the duration of this IDEX project. The specific, immediate objectives are the conception, design, construction and implementation of a few advanced photon manipulation instruments. These elements will be the first realizations of the OPT2X team: they will be able to be tested and operated as parts of novel and/or existing XUV beamlines on the Paris-Saclay campus; in this way, they will provide the user community with state-of-the-art instruments as soon as in 2016, allowing experiments at the forefront of the domain of ultrafast science. The design and implementation of these prototype instruments will help establishing a “working method” for our community and will pave the way for the realization of future similar beamlines in our campus, providing a long term answer to an urgent and growing need of a wide scientific community. Preproject This project aims at OPTimising OPTical pulses for eXtreme ultraviolet ultrafast science (OPT2X), providing the Paris-Saclay scientific community with the resources necessary to fully exploit the exceptional potential of its laser-based sources in the XUV domain. Within a 2- to 4-year period of stepwise development, the XUV sources on ATTOLAB and LASERIX will be equipped with advanced instrumentation at the interface with the user stations; these instruments will also be available for the first experiments on more innovative sources like LUNEX5. This investment will thus maintain its value in the long term: it will be used well beyond 2016 (for instance, we can recall that phase 2 of the ATTOLAB Equipex guarantees operating funds until 2020), and will enhance the capability of the facilities to find new funding. Since time gradient is the essential parameter in ultrafast science, the community of users of these facilities must be able to characterize, shape and control the temporal properties of the XUV light field (its spectral amplitude and phase properties), adapting their characteristics to each specific study. Besides controlling the XUV pulse generation by acting on the driving laser, pulse manipulation includes special new optical elements (multilayer mirrors for amplitude/phase shaping, monochromators, focusing optics, XUV waveplates, interferometers, etc.): they will be designed and characterized by means of “all-optical” specific set-ups implemented on the existing facilities available at the LCF, the SOLEIL synchrotron, LOA and CEA laser laboratories . Moreover, XUV field characterization involves advanced techniques based on photoemission and quantum interferometry, which will be implemented on dedicated stations. The final goal is to complement the XUV sources with flexible and user friendly optical systems, to obtain a control of the optical pulses similar to what is achieved (in a cw mode) at synchrotron radiation sources. If fully controlling the XUV field properties is the key concept of the project, the effective goal of OPT2X is to realize two types of XUV beamlines, i) one based on multilayer mirrors with different bandwidths, and ii) one based on dispersive gratings. The two types of beamlines will be implemented on both LASERIX and ATTOLAB facilities. The beamlines will incorporate at least one microfocusing system, polarizing elements and a complete set of diagnostics to allow real time 16 characterisation of the XUV pulses delivered to the user stations. These crucial issues will be developed while taking into account stringent conditions of excellent mechanical stability, differential pumping, precise optical delay lines, etc. - impact au niveau de Paris-Saclay By making it possible to fully exploit the potential of its XUV sources for ultrafast science, the OPT2X project will significantly enhance the scientific activity on Paris-Saclay; furthermore, it will reinforce the role of these facilities as scientific crossover centers, facilitating the access for future possible users. An important facet of the project will be the training of Ph.D. students and postdocs in an open scientific context, at the intersection of laser technology, optics and basic sciences: the project will host a number of young scientists motivated by its rich interdisciplinary content. The results of this effort will make it possible for the Paris-Saclay campus to confirm and strengthen its leading international role in ultrafast science, and to cope with a fierce competition from other campuses in Europe, US and Asia. 3.1 Structuring objectives in the perspective of UPS (Marino) Structuring and strengthening the considerable existing know-how in XUV optics, on the mid to long term at UPS Training young scientists and students in the field of XUV-optics and applications Associating the strong industrial environment in joint R&D 3.2 Technological objectives (Marino) Realization of advanced instruments for the controlled transport of XUV photons to the user stations, preserving the unique properties of XUV atto-femto-picosecond pulses in space, time, energy and polarization. Establishment of a platform for off-line development and characterization of novel instruments (optics, detectors, etc), to characterize instruments before their implementation on the beamlines Conception and realization of optimized on-line diagnostic tools, to provide the users the necessary real time characterization of the XUV pulses during the experiments. 3.3 Training (Sophie K) 3.3.1 Maintaining expertise Preparing future recruitment 3.3.2 Existing involvement/actions in training 3.3.3 Future actions in training See 4.6 Demande bourses Site web pour offre thèses et stages 3.4 Academic dissemination (Danielle) 3.4.1 existing actions See list in Annex EQUIPEX 17 LUMAT LABEX ANR 3.4.2 Interest and future actions Spatial research (FD) 3.5 industrial dissemination : technological transfer 3.5.1 Existing joint actions and projects See list in Annex 3.5.2 Interest and future actions CEA, LOA have established a partnership with Imagine Optic Company. They have obtained in 2013 a 1Meuros grant from the French ministry of research (ANR) to develop lensless microscopy at an industrial level with sub micrometer spatial resolution and a moderate cost. Images are obtained by recording coherent diffraction pattern without using any lens. It is based on the use of phaseretrieval algorithms and holograms. Since few years, it became a very active area of research for lensless imaging at X-ray wavelengths. This technique having the potential to reach high resolution at low cost, there is a growing interest in using it in the visible or UV range with targeted resolution on the order of a few 100’s nanometers. Indeed, the extreme spatial resolution can reach half the illumining wavelength motivating the use short wavelength radiation. Moreover the technique does not suffer from any aberration due to the limited quality of optics. Whatever the wavelength is, high quality, high aperture optics are hardly impacting the cost of microscopes. The consortium will start by building a prototype using a compact UV laser diode. Our constraint is to have a 2D/3D microscope, called the Nanoscope, with an ultimate resolution of 200 nm with a cost lower than 20 Keuros. To achieve this goal we will work on the process of 2D and 3D image formation from multiple to single diffraction pattern. We will push the basic knowledge in coherent imaging exploiting and speeding up algorithms and image processing techniques. In parallel of building this prototype, the partners will prepare the second class of instrument, the 20 nm resolution instrument. This instrument is more prospective. It makes use of an intense coherent X-ray source with a wavelength down to 10 nm. Innovative demonstration applications of The R-Nanoscopes will be performed in Biology and Material science. To realize this program, state of the art wave front sensing and corrections developed by Imagine Optic Inc. will be used to push the spatial resolutions at its extreme. Finally, an important goal is to stimulate at all level the development and implementation of the Nanoscope instruments with potential commercial value. We will look for any potential market from biophotonics, medicine to nanosciences. 3.6 Scientific benchmark studies (all) Within the two-year project, the technical developments aim at making – partially or fully – possible a series of benchmark studies in the gas phase, the solid-state and plasmas. These studies are representative of the scientific objectives and generic needs of research in the field of ultrafast dynamics and XUV optics. 3.6.1 atto time-resolved study in gas phase (Bertrand C, …) One of the main tasks of ultrafast dynamics is the study of coherent electronic wavepackets (EWP) localized in space and time. As an example, recent efforts have been focused on measuring a socalled “photoemission delay” in atoms and molecules [Haessler09, Schultze10, Klünder11, Caillat11] and solids [Cavalieri07]. In photoionization in the gas phase, let us recall that the free photoelectron wavepacket, produced in single photon ionization of the initial bound state |𝜓0 ⟩ by the ℰ𝑋𝑈𝑉 XUV 18 field, expresses as a coherent superposition of scattering eigenstates |𝜀⟩𝑒 𝑖𝜂(𝜀) at 𝜀 energy in the continuum: +∞ (𝜺−𝜺𝟎 ) (𝒕−𝝉𝑾 ) ℏ ⃗ 𝑿𝑼𝑽 (𝜺)|𝝍𝟎 ⟩𝒆−𝒊 ⃗ , 𝒕) ∝ ∫𝟎 |𝜺⟩⟨𝜺|𝒓 ⃗ ∙𝓔 𝝍𝒆 (𝒓 𝒅𝜺, (E1) where 𝜀0 is the central energy of the electronic wavepacket (EWP). The photoemission delay or the 𝑑𝜂 Wigner time [Wigner55, Caillat11] appears as a group delay 𝜏𝑊 = 𝑑𝜀 | , i.e., the derivative of the 𝜀0 scattering phase with respect to energy. In isolated systems, the photoemission delay corresponds to the formation of the free EWP from the valence shell out of the core region, therefore depending on the ionized bound state, potential shape and electron correlations. In solids, it is rather related to the transport time of the EWP from the bulk where photon is absorbed to the solid surface. Variation of the photoemission delay from one to another initial bound state is as short as a few 10 as [Schultze10, Klünder11]. These measurements, though they are still discussed theoretically, undoubtedly shed light on electronic dynamics at the finest timescale, in one of the most fundamental processes in physics, physicalchemistry and biology. To achieve characterization of the EWP and photoemission delay measurements in (E1), FROG type techniques are particularly adapted. They involve production of the EWP in the presence of a strong coherent field, e.g., a laser field in the mid-IR/IR range. The strong field acts as an “optical gate” inducing modulation of the EWP quantum phase and energy. From the measured spectrogram, i.e., the photoelectron yield as a function of energy and XUV/laser delay, one can retrieve amplitude and quantum phase of the EWP. Note that, in (E1), only the combination of the XUV field and EWP properties is addressed and the latter not resolved. However, the XUV field spectral amplitude and phase are determined as soon as those of the EWP are known or can be reliably calculated, as this is the case for 𝑑𝜂 photoionization into a “flat” continuum ( 𝑑𝜀 ≈ 0). Conversely, photoionization with a fully characterized XUV field gives access to the intrinsic properties of the system, e.g., photoemission delay in autoionizing resonance [Haessler09]. The general frame of the above FROG type (FROG-CRAB) technique has been proposed at SPAM [Mairesse05], whereas variants were already successfully used, such as attosecond streaking [Drescher02, Uiberacker, Goulielmakis, Yakovlev10, Schultze13] and RABBIT [Paul01, Mairesse03, Mauritsson, Boutu09, Haessler10]. The OPT2X project will implement, among others, the FROG type techniques as standard tools for the users, for the two complementary purposes of, i) complete determination of the XUV field, and ii) complete characterization of EWP. This requires that stringent conditions are reached: In order to get well defined of quantum interferences in PI, the XUV and laser wavefronts should be well defined. XUV/IR superposition perfectly controlled. 3.6.2 PI and polarization control – chirality (Danielle D, L. Nahon, T. Ruchon) CELIA The importance of chiral configuration determination through chiroptical diagnostics such as circular birefringences and dichroisms (CD*) is enormous in biology and chemistry, especially in the 3-6eV range. Indeed, a great deal of molecules used and synthesized by living organisms are chiral, and elementary bricks of life such as amino-acids are found homochiral* in the biosphere. In the drug industry, usually only one of the enantiomers* is useful, the other one being potentially harmful. However, at variance with magnetic circular dichroism which is a routine diagnostic on synchrotron beam lines, CD values are excessively small compared to regular absorption (∼10-3-10-5). Their study thus requires the use of lock in detection techniques, requiring the modulation of the light source’s polarization. In the XUV domain only a slow modulation of a few tens of Hertz is achieved on the undulators of about five synchrotron radiation (SR) beam lines worldwide (e.g. [Nah2012,Tur2004]). Alternatively, PhotoElectron Circular Dichroism (PECD: excess of forward/backward photoionization 19 of chiral species by a circularly polarized XUV light beam) is much larger than regular CD. It has been studied on SR soon after its prediction in the 2000’s and proved to be excessively sensitive to the photon energy [Nah2006], static [Pow2008] and dynamical molecular structures [Gar2013]. Along with synchrotron sources, the currently commissioned XFEL’s include this capability of delivering circular polarization [e.g. All2012], extending the synchrotron static measurements to dynamical ones with a resolution of 10 to 500 fs with significant jitter. In view of this state of the art, there is a clear scientific case for temporally short XUV beams of modulated circular polarization. The Opt2X project will implement i. ii. HHG beam lights with high modulation rate of circular polarization through the use of smart combinations of driving fields for the study of PECD. Polarization characterization devices (reflective polarizers) for the study of XCD 3.6.3 atto time-resolved study in solid (Marino) as-fs ARPES Time, space Switching between as/broadband and ps/narrow band 3.6.4 as-fs Ultrafast Phenomena at a nanometer scale (Hamed M) Ultrafast phenomena at a nanometer scale merge two large and highly successful fields of modern research: ultrafast science and nanoscale physics. Ultrafast science, which produces and analyzes events as short as attoseconds, is often explored through studies of atoms and molecules, while nanoscale research focuses on condensed matter. Joining these two fields is only natural because their intrinsic time and length scales match almost perfectly. In fact, all important electronic processes in solids take place on attosecond to femtosecond time scales as determined by the spectral bandwidths and electron interaction (collision) times. In space, important phenomena in condensed matter such as plasmonic energy localization, electron scattering, the skin effect as well as the steering of electronic matter waves, etc. take place over distances of around 10 nm. Researchers in the Plateau de Saclay have started to investigate ultrafast processes at a nanoscale using coherent X-ray diffraction and small angle scattering. Ultrafast coherent diffraction using soft and hard X-rays is actually revolutionizing imaging science thanks to new sources recently available (HHG, FELs in particular). This powerful technique extends standard X-ray diffraction towards imaging of non-crystalline objects and leads actually to a strong impact in physics, chemistry and biology. Atto/femto-second coherent X-rays from high harmonic generation available in our lab allow watching matter evolving with unprecedented space and time resolution. We have demonstrated single shot (20 femtoseconds) nanoscale imaging using either a phase retrieval approach or a new holographic scheme. This has required a lot of effort to achieve state-of-the art X-ray beamlines with few micron focusing, wavefront and coherence optimization. Indeed, measuring accurately the spatial configuration of an isolated nanometric object may turn difficult in multi-shot acquisition. The difficulty even increases in dynamical imaging, where space and time configurations should be repeated. Hence, real time imaging of single object requires that the parameters of the source are well known. Accuracy means that the beam parameters have to be carefully controlled and that the highest intensity is available on the sample. As above mentioned, we have already obtained at LOA and CEA single shot diffraction pattern from isolated object using tabletop harmonics lasers [Ravasio09, Gauthier10, Ge13]. Further progresses can be made by using innovative approaches to transport and condition the beam and to focus the coherent beam. LOA and Imagine Optic have been developing jointly optical systems that would match our requirements. Further developments are however needed. In particular, a Shack Hartmann wavefront sensor would help in improving the beam quality and the focusing of the XUV beam. 20 We propose to explore the limits of these coherent imaging techniques in space (nanometer to atomic) and in time in a “pump-probe” experiment (femtosecond down to attosecond). We are interested in following at a nanometer scale different dynamical processes such as laser-induced nano-plasmas, magnetic nanoscale phase transition and nanoplasmonic field enhancement. Imaging magnetic nanodomains properties Magnetism properties of nano-objects is known to be different from bulk structures. Such tiny magnetic elements will be commercially available in every computer within less than 10 years for enhanced data storage capacity or for flash memories. Today, study of magnetic nano-objects is mainly achieved on huge facilities [Wang12] (free-electron lasers) that are ranging from 200 m to 3 km, with cost from 200 M€ to 1B€. In parallel, since about 6 years LOA and CEA collaborate with two French laboratories, LCPMR and LPS, specialized in magnetic nano-systems to transfer the imaging technics from these huge machine to compact high harmonic sources. This work is now far beyond the demonstration with several high impact articles already published [Vodu11, Vodu12]. Figure 4: Schematic description of pump-probe experiment (a) achieved at LOA aiming to study the temporal evolution of magnetic nano-objects (b and c). Image b has been obtained with Magnetic Force microscope showing the magnetic nano-structures. Up to now LOA and CEA have performed scattering experiment. We are now on the path to realize images of magnetic nanodomains. Moreover the ultrashort pulses (femtosecond) allow tracking the dynamical properties of such systems. More generally, OPT2X beamlines at CEA and LOA will offer to every industrial laboratory the capacity to do at-home experiments and inspections on their future magnetic nano-systems. Ultrafast Nanoplasmonics: Recently, IDEX researchers have proposed to study generation of coherent EUV pulse from HHG assisted by plasmonic resonances. Bowtie nano-antenna will be used to generate high-harmonic radiation at a repetition rate of 75 MHz as proposed by Kim et al. [Kim et al. Nature 2008]. It is clear that the scientific and industrial outcome of this research is more than timely and extremely valuable for the IDEX scientific community. The low cost of this new generation of coherent XUV light will stimulate the wide diffusion of these new EUV ultrafast sources for novel academic and industrial applications. The developments proposed in the OPT2X project will support those progresses. In particular, coherent diffractive imaging will be used to characterize the coherence properties of the 21 radiation. Wave front sensing and spatial coherence will additionally help in characterizing the beamline. Nanoplasmas It has been recently shown that it is possible to confine relativistic fields in nanostructured gold targets [Purvis et al. Nature Photonics 2013] in order to reach ultra-hot and dense plasmas regimes. Typically, densities two orders of magnitude above the critical density and temperatures exceeding few thousand of keV can be obtained using moderated laser energy (below 1 joule). In parallel, researchers have shown that it is possible to amplify locally a laser field using plasmonic structures. IDEX researcher will combine both knowledge in plasmas physics, ultrafast lasers and plasmonics to generate relativistic fields (1018 W/cm²) from few 1014 W/cm² classical laser field obtained using very modest laser (few 10 mJ range). The target will be designed at CSNSM in Orsay and the experiments will be conducted at CEA in collaboration with LOA. The generated relativistic nanoplasmas will be diagnosed using ultrafast nanoscale imaging already in hand at Saclay. We will benefit from OPT2X developments, in particular broadband attosecond optics and few micrometers XUV focusing optics are mandatory for the success of the experiment. 3.6.5 fs-ps timescale WDM (Annie K) The scientific motivation of the proposed technical developments is to contribute to the understanding of matter heating induced by intense XUV radiation, and of the induced non-equilibrium transition phase from solids to the Warm Dense Matter (WDM) to dense strongly coupled plasmas (DSCP), through the investigation of the radiative emission .properties of the heated sample. The primary process for the energy deposition is direct photoionization of the solid by the incident XUV pulse, with a strong dependence with respect of the energy (wavelength) of the photons. Our particular interest is to investigate X-ray emission from hole states transitions rather than usual resonance lines. Due to the high autoionization probability associated with core hole states, emission originating from core holes is only possible on a femtosecond timescale. Therefore, it is not sensitive to low density recombining regimes that usually mask interesting high density features. We intend to use state-of-the art ASE XUV lasers operating at photon energies 89 eV and above, in a range of focused energy/duration that complements those already achieved with XUV Free Electron Lasers (see eg Dzeldzainis et al HEDP 6 (2010) 109; Zastrau et al Laser And Particle Beams 30 1 (2012) 45-56 ). Current ASE XUV lasers, delivering µJ, few ps pulses, will allow to investigate interaction in the 10 12 - 1013 W/cm2 range, while limiting the loss of density due to plasma expansion. Higher focused intensities (1014 W/cm2 and above) and shorter pulse duration (100 fs and below), approaching XUV FELs ones, are foreseen in a near future with the progress of seeded XUV lasers, which will be implemented at LASERIX and also investigated at the Appollon-CILEX facility. However the implementation of these experiments requires the development of specific advanced instrumentation to control and characterize the XUV intensity focused on the solid sample, on a single-shot basis. Namely, control of focusing with micrometer size (NB: we do not want very small focal spots, since we want to study the emission of the heated sample) Note: required parameters to reach a focused intensity of 1014 W/cm2 duration 1 ps: 100µJ in 10µm (diam) focal spot; 25µJ in 5µm (diam) focal spot duration 100 fs: 8µJ in 10µm (diam) focal spot; 2µJ in 5µm (diam) focal spot 3.6.6 application bio (Philippe Z. to be discussed and selected) 3.7 2 year deliverables (Marino) The following technical objectives have been identified by the partners as strategic and requiring a cooperative effort to be realized by 2016: 22 3.7.1 Technical - Pulse shaping monochromating system based on dispersive gratings; - Pulse shaping bandpass control system based on multilayers; - Microfocusing optical systems with relative mechanical components etc - XUV polarization control - Real time XUV diagnostics, with relative detectors etc 3.7.2 Training and Dissemination - Training of young scientists and engineers 4 Methodology and work plan. We have identified 5 work packages (WP’s) to organize the cooperative action among the partners. This work plan will make it possible to achieve the specific goals (described in 2.4), delivering novel instruments that will be tested and operated on the existing XUV facilities at Paris-Saclay, and will be a basis to continue the operation of the OPT2X team also beyond 2016. WP1 – WP2 – WP3 – WP4 – WP5 – Manipulation of the spectro-temporal profile Manipulation of spatial profile and polarization On-line diagnostics of spectro-temporal properties On-line diagnostics of spatial properties and polarization Off-line optics metrology and detector development The WP coordinators, together with the users present in the OPT2X team, will collect specific technical needs from the wide user community supporting this proposal, to define the specifications and the choices for the instruments. All the main choices/ decisions will be communicated to the user community (for instance with topical one-day workshops). When the instruments will be available on the various XUV sources, the source managers will inform in detail the user community on the new performance levels attained by the facilities thanks to the contribution of OPT2X. The OPT2X team will continuously interact and exchange information with the user community. 23 OPT2 X LASERIX ATTOLAB LOA SOLEIL 2016 User Platform Future projects WP1 WP2 WP3 WP4 WP5 Each of the 5 technical workpackages is presented as a two-step effort. First, we present the generic long term development. Second, we focus on the 2-year deliverables of the project. 24 Generic beamlines (Annex ?) Figure 5 : Generic atto-fs HHG-based beamline 25 Figure 6 : Generic fs-ps XRL beamline 26 Topic D1.1 Time Control Space Control Temporal Characterization Spatial Characterization WP1 WP2 WP3 WP4 Metrology WP5 Training WP6 D1.2 Deliverable monochromatizing system based on multilayer optics (switchable between “10 fs – single harmonic” mode and “as – broadband” mode) monochromator based on “off plane mount approach” (switchable between “30 fs – narrow bandpass”, “10 fs – single harmonic” and “as–broadband” mode) D1.3 Multicolor (XUV/IR) and XUV/XUV time and space (focusing) superposition system (Marie G, Bertrand C) D2.1 as-fs / fs-ps : Focusing system grazing-incidence to achieve few micron focal spot (PhZ) D2.2 as-fs / fs-ps: “User polarization control system: de-phaser” D2.3 as-fs : multicolor XUV/IR and XUV/XUV focusing system (Marie G.) D3.1 Shot-to-shot measurement of pulse intensity D3.2 As-fs/fs-ps : Shot-to-shot (almost) on line spectrum (recorded/stored during data acquisition) with absolute monitoring of pulse intensity (time & space) D3.3 as-fs : complete characterization time profile : FROG-CRAB or 2nd order autoco (Thierry R) D3.4 Online, single-shot characterization of XUV pulse by THz streaking D4.1 on-line measurement of spatial profile D4.2 Wavefront sensor D4.3 complete determination of all Stokes numbers (Danielle D, Laurent N) D5.1 Metrology Table 2 : 2-year Deliverables 27 4.1 WP1: Control of the spectro-temporal profile (F. Delmotte + ...) 4.1.1 Overall technical objectives 4.1.1.1 as-fs: Multilayer optics for (broadband) spectral selection and spectral phase shaping (F. Delmotte, ....) The rapid progress in ultrafast science applications induces new requirements on multilayer optics: not only higher reflectivity, but also a better control of the spectral shape (narrowband or broadband mirrors, enhanced spectral purity by rejection of unwanted spectral lines, etc.)… In order to efficiently reflect ultrashort pulses off a multilayer mirror, the latter must have a bandpass broader than the pulse spectrum and a well-controlled phase. Thus, there is a distinction between the design of a multilayer stack for pico/femtosecond pulses, and for attosecond pulses. In the first case, the pulse spectrum never exceeds a few tenths of electron-volts, which always fits in the Bragg’s peak of a periodic multilayer stack. Moreover, the phase of such a mirror being always linear throughout the reflectivity peak, the pulse can be efficiently reflected off a simple periodic stack. In the case of attosecond pulses, the XUV spectrum is at least a few ten-eV large, i.e. much larger than the Bragg’s peak of a periodic multilayer stack. Therefore specific multilayer designs are required to obtain structures exhibiting a broadband reflectivity and a controlled phase. Concerning fs pulses, the design of multilayer mirror turns out to be very challenging if one wants to select one harmonic from a HHG spectrum. As usual, the mirror peak reflectance is an essential parameter but, in this case, more critical is the spectral selectivity. On one hand, the bandwidth of usual multilayer is not narrow enough to efficiently reject the neighbor harmonics. One the other hand, usual multilayer mirrors exhibit high reflectance at low energy due to metallic surface reflection. During these last years, both kinds of multilayer components (broadband & phase controlled mirrors on one side and selective multilayers on the other side) have been successfully designed, produced and used for applications in Paris-Saclay laboratories. One main objective of OPT2X project is to combine these two functions in one single instrument to be inserted in-line on Paris-Saclay ultrafast beamlines. It will offer to the users a very versatile way to control the spectro-temporal profile and thus enable multi-timescale studies of one sample in the same environment. The user will have the possibility to select one harmonic (fs duration) or few harmonics (as duration) just by translation of multilayer mirrors with specific design. As one of the two functions concerns the manipulation of attosecond pulses, we will take special care about mechanical stability issues in the design of the instrument. Currently, this opportunity does not exist, inside or even outside Paris-Saclay campus. It will be an actual contribution of OPT2X project to the users community. 4.1.1.2 as-fs : Attosecond delay lines with active control (Marie G – Willem B) It is worth to recall that the major motivation for studies in the time domain is to track the – usually coherent - motion of electronic and nuclear wavepackets in real time, in the two cases of: i) initial excitation by a pump pulse followed by the free motion of the WP under action of internal driving forces alone [Haessler10, Goulielmakis, Wörner11, Ruf12], and ii) initial excitation and motion under action of internal and time-dependent external pump forces, e.g., in the presence of a strong field [Sansone10, Schultze13]. 28 In the simpler first case i), through coherent excitation with light pulse of duration tL ~ 1 fs and ℏ bandwidth EL ~0.5 eV (∆𝑡𝐿 ∆𝐸𝐿 = 2), it is possible to produce electronic/nuclear wavepacket ℏ localized in space: the spatial extension of the wave packet, ∆𝑥0 = 2∆𝑝 = 𝑣∆𝑡𝐿 where v is the group (classical) velocity, intrinsically ranges at the Angström scale of a molecule or solid lattice. The WP then coherently evolves in time, its quantum coherences changing over the ∆𝑡𝐿 timescale, its spatial extension changing over the 𝑡𝑠 = 2 𝑚Δ𝑥02 ⁄ℏ “uncertainty” timescale [Zewail01], over which the WP may be considered as a “classically localized” object; since it depends on mass, the uncertainty time is typically in the as-fs (fs-ps) range for an electronic (nuclear) WP. Both cases i) and ii) imply that multiple – at least two - ultrashort pulses, including attosecond XUV ones, are combined in pump/probe experiments, that is spatially overlapped with accurate control of intensity and wave fronts, and temporally delayed with attosecond accuracy, i.e., nm scale control of optical path . At given frequency ω, propagation into material of refractive index 𝑛𝜔 over distance d 𝑑 𝑑𝑛 𝑑 introduce phase shift 𝜙𝜔 = 𝑛𝜔 𝜔 𝑐 and group delay 𝑡𝜔 ≈ (𝑛𝜔 + 𝜔 𝑑𝜔𝜔 ) 𝑐 ; in vacuum, d=3 nm corresponds to 10 as group delay. In experiments, the time delay between the pump and probe pulses has to be controlled with an accuracy better than 100 as and a setup to adjust the delay has to have a stability of at least 30 nm to reach the required temporal resolution. Two pump-probe schemes, and thus two types of delay lines, are required, combining respectively XUV/laser (IR-vis-UV) and XUV/XUV pulses. 1) In the XUV/laser (IR-vis-UV) scheme, since the XUV source is coherently driven by and therefore perfectly synchronized with the laser driving field (DF), the delay can be more easily introduced between the DF and pump/probe laser field (PF) (before the generation process), in the IR-vis-UV range where accurate transmissive optics (wedge) are available. However, this usually results in long arms interferometer (m length) with critical stability, especially on the long run period (several hours or even days) required for data acquisition. In this scheme an active stabilization of the optical path difference is mandatory [Böttcher2008, Ruchon2010]. Alternately, the delay can be introduced between the XUV and PF (after generation). This requires that highly specific optics are designed which reflect either broadband or selectively narrow band XUV - using multilayer mirrors - together with laser (IR), focus the two beams in the same region with attosecond control of the delay. A commercial device derived from lab research is shown in Figure 7 2) [UltrafastInnov]. This arrangement is also available as a narrow band XUV/XUV delay line, then including two multilayer mirrors. Figure 7 : a) Example of XUV/IR pulse delay unit for attosecond streaking, from UltraFast Innovations company [UltrafastInnov]. The central mirror reflects the XUV and the surrounding silver mirror the IR beam. The two-segment mirror is mounted on independent piezo-actuated translations and tilts. The translation of the inner segment is feedback controlled in a scan range of 300 fs, with a resolution reaching less than 3 as. b) interferometric scheme for active time and 2D space stabilization of the coaxial delay line [Böttcher08]. 29 As mentioned above, in experiment requiring long acquisition time at 1-10 kHz repetition rate, active stabilization of the time- and space overlap is mandatory in case 1), and highly recommended in case 2°. Figure b gives example of the interferometric scheme adapted to the coaxial delay line [Böttcher08]. Active stabilization of the two pulses overlap in time and space (i.e., XUV/IR) can be obtained by means of an He-Ne laser (split in 2) which co-propagates collinearly to the IR beams through the interferometer. After recombination the two He-Ne beams produce a pattern of interference fringes, which is measured by multiple (4-quadrant) photodiodes. From the interference pattern, the optical path difference in the delay line is calculated and a PID loop acting on the piezoplate control allows stabilizing the delay within 60 as rms. Simultaneously, the 4-quadrant signal allows for continuous adjustment of the spatial overlap. 4.1.1.3 as-fs & fs-ps delay line for XUV pulses XUV/XUV pump/probe experiments raise specific problems for superimposing two XUV pulses and controlling their temporal and spatial overlap. If the two XUV pulses have the same spectral characteristics, it is natural to produce them from the same initial pulse by either amplitude or wavefront division. Because of the high absorption of the materials, amplitude division beamsplitters are complex devices requiring advanced design and fabrication, e.g., beamsplitter at λ=22 nm based on multilayer deposited on thin membrane and realized in the consortium [Morlens04]. Wavefront division offers more flexibility though the design should be specifically dedicated to either as-fs or fs-ps pulse control. Finally, in the case of HHG, the “attolighthouse” scheme offers an elegant and efficient way of producing multiple atto pulses separated in space which can be further recombined in a pump/probe arrangement. 4.1.1.3.1 optics for wavefront division (Willem Boutu) Wavefront division systems have been developed and demonstrated both on FELs and HHG beamlines. The most efficient solution consists in using a split focusing optics with a fixed part and a controlled part that can be moved along the beam position with a high precision. The arrangements in Figure 7 and Figure 8a give two examples of cylindrical and plane symmetry, respectively. The schematic in Figure 8b shows the relation between optical path difference (𝑐𝜏 ∝ 𝑑𝑐𝑜𝑠𝑖, where τ is the delay, d the mirror translation and i the incidence angle) and relative displacement of the beams (∝ 𝑑𝑠𝑖𝑛𝑖). In the as-fs regime at grazing incidence favoring broadband reflectivity (or in the fs-ps regime at usually close to normal incidence on wavelength specific multilayer mirrors), one should take care that scanning the delay over a few fs scale (a few 100 fs) does not shift the beam by more than the beam waist (µm size). Alternatively, a versatile option is to use a system that can be decoupled from the focusing, inserted before the focusing optics. For instance, CEA developed a system based on one prism that cuts the beam in two equal parts and subsequent grazing incidence mirrors that makes the two beams parallel – see Error! Reference source not found.9a. One of the mirrors can be adjusted to change the timing. An off-axis parabola is then used to both select the wavelength and focus the two beams on the same sample spot. A compact and moveable system will be developed. The micrometer precision needed for the delay line motion is a standard with vacuum compatible DC motors. The use of grazing incidence optics ensures a high transmission of the setup, even in the XUV range. 30 c= 2dcosi 2dsini i d Figure 8: a) XUV/XUV delay line using two-segment mirror with plane symmetry, b) schematic of the two-segment mirror with cylindrical symmetry, showing delay and central ray displacement as a function of incidence angle. (a) Figure 9 (a) and (b) : XUV beam splitters for XUV/XUV pump-probe experiments. 4.1.1.4 as-fs: Diffractive optics (conical grating) for selecting single harmonic (DE ~100 meV, < 10 fs) (F. Polack, ...) 4.1.1.5 as-fs: Mechanical stability (LOA, SOLEIL) 4.1.2 2 year deliverables 4.1.2.1 monochromatizing system based on multilayer optics (easily switchable between a “10 fs – single harmonic” mode and an “as – broadband” mode) Post-doc 1 year: 50 k€ Mirrors and precision mechanics: 20 k€ Motorized mirror holders: 20 k€ Mirror Coatings (incl. calibration & test): 20 k€ Vacuum chamber + optical table: 30 k€ Consumables for tests: 10 k€ 31 User interface (computer & electronics): 10 k€ 4.1.2.2 monochromator based on “off plane mount approach” (easily switchable among a “30 fs – narrow bandpass”, a “10 fs – single harmonic” and a “as–broadband” mode) 4.1.2.3 multicolor (XUV/IR) space-time superposition (Marie G, Bertrand C) One of the end-stations foreseen in ATTLOAB is a reaction microscope relying on the COLTRIMS technique. In order to perform experiments using an XUV source combined with this instrument, we must be able to: - focus the XUV/IR (respectively XUV/XUV) pulses in the ultrasonic jet of the target gas inside the reaction chamber at ultra-high vacuum, - monitor precisely the spatial overlap in time of the two XUV/IR (respectively XUV/XUV) foci, during the whole experiment duration (many hours, even days). Two schemes can be used, and thus two types of optics are required, combining XUV/laser (IR-visUV) (respectively XUV/XUV) pulses. 1) drilled silver mirrors combined to specific filtering system as metallic filters and multilayer mirrors allowing spectral selection of one or several harmonic in the XUV spectrum. 2) two-segment XUV/IR (respectively XUV/XUV) mirror. 4.2 WP2: Control of spatial profile and polarization (F. Polack + ....) 4.2.1 Overall technical objectives 4.2.1.1 as-fs / fs-ps : Focusing (Ph. Zeitoun, S. Kazamias, O. Guilbaud) In order to achieve high intensities or for coherent imaging it is necessary to focus the soft x-ray beams down to a spot of few micrometers in diameter, with a minimum loss of energy. Such focal spot has been achieved in LOA and CEA thanks to the use of normal incidence, multilayer-coated parabola or at SOLEIL with grazing-incidence optics. Parabola, either centered or off-axis, are relatively cheap optical element and relatively simple to align. From our experience, off-axis parabola may need the use of XUV wavefront sensor for fine alignment. Such sensor exists within the partners of the project. Normal incidence parabola has two main limitations. To efficiently reflect the XUV beam the parabola has to be coated with multilayer. So, first the reflectivity does not exceed 60% at best and often ranges at about 30%. Second, high reflectivity implies narrow bandwidth. Such coating is not compatible with attosecond beams. Also it requires a set of parabola for a facility like LASERIX. Warm Dense Matter experiment (see Science part) requires being able to easily change the wavelength of the XUV beam from above to below an atomic edge. LASERIX demonstrated their capacity to quickly modify the wavelength by changing the target. However, aligning a new parabola and searching for the position of the focal spot is a long work not compatible with user access. Finally, the cost associated to a large set of parabola is far from negligible and it might be relatively long to purchase these optics since each wavelength will require a specific coating. OPT2X policy consists in standardizing as much as possible the optical elements between the partners ensuring cost-reduction, knowledge and know-how sharing, and possibility to exceptionally borrow an optic. Consequently grazing-incidence optics are the most suitable for both attosecond and femtosecond focusing. There are two main kinds of optics: monolithic and active. We consider acquiring active optic and more specifically an optic so called “bender”. This is often a set of two flat mirrors placed at 90° from 32 each other and bent to form two ellipsoidal mirrors. Within elastic limit of the mirrors it is possible to slightly change the focal length by adjusting the bending. SOLEIL, LOA and CEA teams have good experience in using and actively aligning these optics on both synchrotron and free-electron lasers. Alignment is much easier and accurate if using a XUV wave front sensor as CEA and LOA demonstrated on FERMI@ELETRRA free-electron laser, in collaboration with Imagine Optic. As mentioned in 3.6, in XUV/XUV pump/probe experiment the signal does not only depend on the number of XUV photons but on the XUV intensity on target. This requires that the XUV beam be tightly focused – see 4.2.1.1. Technical objective (AK) - Microfocusing with grazing incidence (achromatic) optics to allow studies at several wavelengths with a single device Possible solutions (to be chosen in the early stage of the project): two-toroidal mirrors (see Poletto et al SPIE 2013): aberration corrected, long exit arms, cost-effective; but focal spot 5-15 µm (enough for our purpose ?) elliptical mirrors in a Kirkpatrick-Baez geometry (ref ?) other alternative choice: off-axis parabolas with multilayer coating; single wavelength, but several mirrors could be mounted on a single mount, to allow easy change when changing wavelength 4.2.1.2 as-fs / fs-ps : Polarization control (FD+L Nahon) The state-of-the-art undulator-based VUV beamline DESIRS at SOLEIL covers the 4-40 eV range (30030 nm) and is mainly dedicated to spectroscopy and photodynamics on dilute matter. [Nahon2012] It features very high spectral resolution, with resolving power of up to 106 on the Fourier-Transform spectroscopy branch for absorption and 2 x 105 on the monochromator branch, and high flux, typically in the 1012-1013 ph/sec/0.1%BW over most of the VUV range. In addition, owing to its variable polarization undulator, fully tailored polarization ellipses can be achieved, with in particular quasi-perfect horizontal and vertical linear polarization (s1= ± 0.99), as well left- and righ-circular polarization (s3= ±0.97 or better). Such polarizations have been calibrated owing to a home-made VUV 2x3 reflections-based polarimeter. [Nahon2004] Nevertheless, this instrument is implemented permanently on DESIR beamline (it is part of the beamline) and can not be move to another place. Concerning polarization control on ultrafast XUV sources, a polarizer based upon a four-mirror reflection setup has already been developed by the LOA (see part 2.1.2). This instrument has been successfully applied to generate circularly polarized HHG at wavelength around 20 nm. The fact that it was optimized for a precise wavelength and for a specific application (to transform linear polarized light to circular one) limits its usability and/or performances for other applications. In this project, we will develop a new polarizer system, based upon the same concept, but much more versatile and more compact, owing to variable angles of incidence and the use of various coatings. The objective is to reach an overall transmission higher than 10% in the spectral range 10 – 60 nm (20-120 eV), and an absolute circular polarization rate (s3) above 95 %. This in-line instrument will be designed to fit all Paris-Saclay beamlines (definition of mechanical standard). To design such instrument in the EUV range, it is very important to have access to the experimental response of each mirror, i.e. their complex reflectivity (including the phase), which is poorly known from the literature especially in the VUV range. As a matter of fact, surface effects (oxidation, carbon contamination) have a significant effect on the polarization that is not taken into account in theoretical models. In this project, several types of thin film coated mirrors will be characterized on the DESIRS beamline at SOLEIL in order to access their complex reflectivity, by using an already existing reflectometer chamber from CEMOX platform. This reflectometer, based on a pulsed laser plasma source, will be 33 adapted to receive the harmonic-free and linearly polarized photons from DESIRS. Based on these measurements, the best combination of mirrors will be chosen and implemented on four motorized rotation stages under vacuum. In addition, we will develop a user interface allowing to tune the optimal angles of the mirrors as a function of the state of polarization required for a given experiment. Then, the transmission of the whole instrument will be calibrated on the DESIRS beamline. The control of polarization of attosecond pulses is an actual technological challenge due to the large spectral bandwidth of such pulses. Innovative solutions will be studied by simulations and developed at medium term in the project. [Nahon2004] L. Nahon, and C. Alcaraz, "SU5: a calibrated variable-polarization synchrotron radiation beam line in the vacuum-ultraviolet range," Applied Optics 43, 1024-1037 (2004). [Nahon2012] L. Nahon, N. de Oliveira, G. Garcia, J. F. Gil, B. Pilette, O. Marcouille, B. Lagarde, and F. Polack, "DESIRS : a state-of-the-art VUV beamline featuring high resolution and variable polarization for spectroscopy and dichroism at SOLEIL " J. Synchrotron Rad. 19, 508-520 (2012). 4.2.1.3 as-fs : sub-micron target control - Multiple targets (Willem B) Coherent diffractive imaging and other applications are extremely sensitive to the beam spatial properties. It is therefore crucial to measure and control its characteristics in situ, at the exact sample position. For instance, measuring the coherence is done by using a specifically patterned mask at focus, and a beam focal spot size can be measured using a scanning razor blade across the beam profile. Being able to switch from the characterization configuration to the actual experiment without breaking the ultra-high vacuum environment is crucial. Moreover, when imaging samples with sub-100 nm details, the position of the beam in the few micrometer diameter XUV spot has to be controlled with the nanometer precision. Combining those requirements can be achieved using a specifically designed sample holder that can accommodate several samples and diagnostics – see Figure 10. Vacuum compatible motorized stages allow now for 10s cm travel range with sub-micrometer resolution, while new piezo-electric systems can achieve few nanometers steps over very long distances. Furthermore, long distance microscopes can be used to monitor the beam positioning with respect to the sample. This is especially useful in the case of pump-probe schemes in a non collinear configuration. Figure 10: Sample holder in the Matter in Extreme Conditions (MEC) endstation at LCLS. The holder is fixed on highly stable hexapod, long run translation stage and magnetic socket. It comprises four slots for sample and beam diagnostics. 34 4.2.1.4 as-fs : Simulation tool for XUV optical instruments (F. Delmotte) A Matlab code, called ROSA: “Reflective Optical Systems for Attopulses” has been developed by Charles Bourassin-Bouchet during his PhD at LCF [Bourassin-ROSA2010]. This software provides 3D simulations of attosecond pulses after reflection on an optical component (focusing mirror, multilayer mirrors…). It allows complex studies of the effect of optical aberrations on the pulse duration in experimental conditions, in particular the effect of spatiotemporal coupling in attosecond pulses. [Bourassin-ROSA2011] It is also a very efficient tool to simulate the quality of focusing of attosecond pulses [Bourassin-ROSA2013]. In this project, we propose to improve this code in order to take into account multiple optical reflections. This will allows the simulation and complete instruments and will facilitate the design of attosecond/femtosecond XUV beamlines. We would like also to make this simulation tool available for Paris-Saclay scientific community. For this, we plan to produce a user manual and some user training sessions. This new code would be also an efficient tool for the training of students at master level. [Bourassin-ROSA2013] How to focus an attosecond pulse, Charles Bourassin-Bouchet; Matthias Maximilian Mang; Franck Delmotte; Pierre Chavel; Sébastien De Rossi, Optics Express, 2013, 21, pp. 2506-2520 [Bourassin-ROSA2011] Duration of ultrashort pulses in the presence of spatio-temporal coupling Charles Bourassin-Bouchet; Michele Stephens; Sébastien De Rossi; Franck Delmotte; Pierre Chavel Optics Express, 2011, 19 (18), pp. 17357 [Bourassin-ROSA2010] Spatiotemporal dist ortions of attosecond pulses, Charles Bourassin-Bouchet; Sébastien De Rossi; Franck Delmotte; Pierre Chavel, Journal of the Optical Society of America A, 2010, 27 (6), pp. 1395 4.2.2 2 year deliverable 4.2.2.1 as-fs / fs-ps : Focusing KB system grazing-incidence to achieve few micron focal spot (PhZ) We plan to realize a focusing system aiming to achieve few micrometers focal spot with a focal distance of about 0.5 m. The system will work under grazing-incidence, around 2°, to ensure high reflectivity over a wide spectral range. With gold coating the reflectivity peaks around 80% per mirror from 10 eV to 185 eV then decreases to 60-70% for photon energy up to 1 keV. Even for two reflections, the total throughput will be around 60% for photon energy below 185 eV that is better than the reflectivity of most normal incidence multilayer coating. At higher photon energy, multilayers reflectivity drops dramatically to 20% or less while this optic maintains reflectivity around 40-50%. The optic will be based on the Kirkpatrick-Baez bender technology well-known at SOLEIL and widely used on large-scale facilities. The optic will be controlled by a dedicated XUV wave front sensor. We will also associate a monitoring system to control the focal spot after alignment. We will use the technic developed on free-electron laser consisting in inducing damage on a flat sample and measuring its shape and size in-line by the use of a tele-microscope. The full system will be built, then implemented in Salle Orange at LOA on the high harmonic beamline for test. Although the energy per pulse is low, LOA demonstrated the possibility to ablate samples meaning that the full system may be totally tested. After fully decommissioning, the system will be transferred to LASERIX for being implemented on its beamline. 35 4.2.2.2 as-fs / fs-ps: “User polarization control system: de-phaser” Post-doc 1 year: 50 k€ Polarizer instrument Mirrors and coatings: 20 k€ 4 motorized mirror stages: 40 k€ Vacuum chamber + optical table: 35 k€ Consumables for tests: 20 k€ User interface (computer, control software, electronics) : 10 k€ Modification of CEMOX reflectometer : (à mettre dans WP5 ?) New detector with electronics: 10 k€ Upgrade for compatibility with SOLEIL: 20k€ Upgrade of user interface (computer, control software…): 10k€ 4.2.2.3 as-fs : multicolor XUV/IR and XUV/XUV focusing system (Marie G.) see 4.1.2.3 One of the end-stations foreseen in ATTLOAB is a reaction microscope relying on the COLTRIMS technique. In order to perform experiments using an XUV source combined with this instrument, we must be able to: - focus the XUV/IR (respectively XUV/XUV) pulses in the ultrasonic jet of the target gas inside the reaction chamber at ultra-high vacuum, - monitor precisely the spatial overlap in time of the two XUV/IR (respectively XUV/XUV) foci, during the whole experiment duration (many hours, even days). Two schemes can be used, and thus two types of optics are required, combining XUV/laser (IR-visUV) (respectively XUV/XUV) pulses. 3) drilled silver mirrors combined to specific filtering system as metallic filters and multilayer mirrors allowing spectral selection of one or several harmonic in the XUV spectrum. 4) two-segment XUV/IR (respectively XUV/XUV) mirror. 4.2.2.4 as-fs : Simulation tool for XUV optical instruments Post-doc 1 year: same person as 4.2.2.2 4.3 WP3: On-line diagnostics of spectro-temporal properties (A. Klisnick + D. Garzella +....) 4.3.1 Overall technical objectives Characterizing the temporal/spectral properties of the XUV light field, with component ℰ𝑋𝑈𝑉 (𝑡) = |ℰ𝑋𝑈𝑉 (𝑡)|𝑒 +𝑖𝜙(𝑡) (𝑟-dependence in Equation 1 has been skipped), is very challenging. One should recall that, for the studies of coherent processes excited/probed by XUV pulses, it is crucial that the amplitude and the phase of ℰ𝑋𝑈𝑉 (𝑡) are determined. At the as-fs scale, HHG pulses spectrally extend and show coherence over a broad spectral range of several tens eV. Throughout this range, an account of the strong absorption in matter, none of the powerful optical methods which serve in the IR-vis-UV directly applies. Conversely, at the ps timescale, XRL shows extremely narrow line width (ΔE/E~10-5) which cannot be measured using 36 conventional spectrometer. To face these challenges, XUV metrology has developed a number of specific innovative techniques, a number of which – XUV Fourier transform spectroscopy, FROG- and SPIDER-type techniques - has been proposed and demonstrated by the OPT2X partners. We briefly address some major tasks of temporal/spectral characterization which motivate long term effort in the OPT2X consortium, as well as 2-year realization of specific deliverables. 4.3.1.1 As-fs : complete characterization of ultrashort pulses : Quantum interferometry & FROG techniques (Thierry R, BC) Frequency-resolved optical gating (FROG) is a widely used technique for the full temporal characterization of visible pulses [Trebino00]. In FROG, to determine the ℰ(𝑡) complex field, one cuts “temporal slices” in the field by means of an movable optical time gate 𝐺(𝑡 + 𝜏), and gets its +∞ 2 spectrum 𝑆(𝜔, 𝜏) = |∫−∞ 𝐺(𝑡 + 𝜏)ℰ(𝑡)𝑒 𝑖𝜔𝑡 𝑑𝑡| . From algorithmic analysis of the so-called 𝑆(𝜔, 𝜏) spectrogram, one usually uniquely retrieves the ℰ(𝑡) field and the 𝐺(𝑡) gate. Y. Mairesse and F. Quéré have shown that FROG could be transposed in the XUV to achieve complete reconstruction of attosecond bursts (FROG-CRAB), and more generally of any ultrashort pulse at the as- fs time scale [Mairesse05]. FROG-CRAB offers the general frame which encompasses its former variants efficiently used in specific cases, such as Attosecond streaking [Uiberacker07, Goulielmakis07, Schultze13] and RABBIT [Véniard96, Paul01, Mairesse03]. FROG-CRAB is based on quantum interferometry : photoelectrons are produced from photoionization of atoms into a “flat” continuum (free of resonance, slow energy-dependence of the scattering phase), in the presence of a laser field. The optical field modulates in time the quantum phase of the EWP, i.e., its energy, and plays the role of the optical time gate in FROG. The photoelectron spectrum as a function of the XUV/laser delay takes the form of a S(ω,τ) spectrogram, from which the ℰ(𝑡) – and the optical field – can be fully retrieved – see numerical example from [Mairesse05] in Figure 11. Figure 11: from [Mairesse05] a) FROG- CRAB trace of a complex as field, whose spectrum (shaded curved and spectral phase - red line - are shown in panel b). The spectrum consists of discrete peaks spaced by <3 eV in its lower part, and a continuous component in its upper part. In (c) and (d), the exact intensity profile of the as field and the laser electric field (full lines) are compared to the ones retrieved from this trace (dots) after 300 iterations of PCGPA algorithm. 4.3.1.2 As-fs : complete characterization of ultrashort pulses : Optical interferometry (SPIDER, 2-sources) (Bertrand C) 4.3.1.3 as-fs : Single shot characterization of ultrashort pulse : THz streaking (Annie) - Online, single-shot characterization of the time-resolved intensity (power) of the XUV pulse Possible technical solutions: 37 THz streaking of XUV generated photoelectrons (U Fruhling et al Nat Phot 2009, I Grguras et al Nat Phot 2012) IR induced side-bands of XUV generated photoelectrons with spatial resolution (S Cunovic et al APL 2007) other methods ? 4.3.1.4 as-fs : Free Electron laser (D Garzella, P. Audebert, C. Miron) 4.3.1.5 fs-ps : X-ray laser (S. Kazamias, A. Klisnick) 4.3.2 2 year deliverables 4.3.2.1 Shot-to-shot (almost?) intensity of pulse fluence 4.3.2.2 As-fs/fs-ps : Shot-to-shot (almost) on line spectrum (recorded/stored during data acquisition) When performing gas phase measurements, in line spectrum measurement can be performed by installing a spectrometer after the interaction region. The system can consist of either an imaging photon spectrometer or an electron spectrometer. However, solid state samples usually absorb the XUV radiation, thus preventing a posteriori characterization. Two solutions can be envisioned. The first one, already implemented at CEA, consists in inserting a first independent photoelectron spectrometer upstream of the experiment interaction point. However, single shot spectrum measurement is then usually prevented due to the low photon number and ionization probabilities. Moreover, this implies using a second focusing optic to re-image that first focus, hence increasing the sources of optical aberrations. The second possibility is to introduce a transmission grating in the beam path. The zeroth order is sent to the experiment, while the first order, where the spectral components of the beam are dispersed, is sent to a XUV CCD camera. In that configuration, shot to shot spectrum acquisition becomes possible, within the limitation of the readout time of the CCD, usually longer than the laser period. The system main advantages are its small size and its minimum impact on the beam properties. The same diagnostic, once calibrated, can also be used to measure the intensity and spatial profile. However, the zeroth order transmission (a few 10s percent) may limit the applications. An alternative solution would be to use reflective gratings, at the expense of the compactness and movability of the system. 4.3.2.3 automatic analysis of (single pulse) spectral lineshape (to point out instabilities) 4.3.2.4 as-fs : time profile (Thierry Ruchon) When performing multiphoton experiments, not only the power spectrum of the excitation light comes into play, but also i) its spectral phase, to define a given temporal profile, and ii) the synchronization of the two or more fields involved. Envisioning XUV-XUV experiments is for now an experimental tour de force, and it is unlikely that we could, within two years, set up an online diagnosis about the synchronization of two XUV beams. We will alternatively focus on two linked objectives: monitoring XUV pulse profiles and servo-looping XUV/IR pulse synchronization within 20as. Both will make use of the FROG-CRAB protocol, implemented using a magnetic bottle electron spectrometer to enhance the collection efficiency and thus the acquisition time. Given the FAB1FAB10 anticipated fluxes, we will aim at a diagnosis within less than a minute, short enough to monitor long term drifts, and much shorter that typical acquisition times in solid state physics of COLTRIMS experiments. Special care will be taken to be able to run this diagnosis without stopping the experiments placed downstream, thus requiring a series of differential pumping stages to get 38 from typically 10-4 to 10-10 mbar, and a specifically shaped (probably annular) dressing beam. Special care will also be taken to design a user friendly software that will give a live update of the XUV temporal pulse profile and synchronization with the IR, the aim being to transfer the SPAM knowledge to a diagnosis run by non experts. 4.4 WP4: On-line diagnostics of spatial properties and polarization (Ph. Zeitoun + ...) 4.4.1 Overall technical objectives 4.4.1.1 single shot coherence measurement (Hamed) The beam spatial coherence is a key factor for all the coherent imaging techniques, as demonstrated recently at CEA (Ge et al. Optics Express 2013). However, the Young’s double slits experiment can only measure the spatial coherence at one given dimension of the harmonic beam in one acquisition. Therefore, to characterize the entire beam spot, one should combine the measurements of multiple acquisitions from a complete set of various size double-slits. This avoids a single shot characterization of the full beam. This last point is crucial as most of the available XUV sources, HHG, X-ray laser or XFELs will exhibits shot to shot fluctuations. To perform such measurement, one can use a nonredundant array of apertures (NRA), which can characterize the beam more completely in two dimensions with one interferogram (or hologram). The NRA, initially proposed and demonstrated with visible lasers in Ref. 1, is composed of nine pinholes (Fig…) in well-chosen positions to have a non-redundant superposition of the beam spot (Fig…) for interference measurement (Fig….). The spatial coherence of the beam (Fig…) can then be calculated at the localization of each spot. Therefore, a more complete characterization of the spatial coherence across the beam is achieved. Note that in both Young’s double slits and NRA measurements, the knowledge of the beam’s intensity distribution is necessary for calculating the spatial coherence, which is usually assumed to be uniform for simplification. Thus, single-shot measurement of the spatial coherence will always rely on the statistics of the intensity distribution introducing a systematic deviation in the measurements. At CEA, we are currently developing NRA-style patterns (Fig…), which are actually redundant and symmetric to retrieve both intensity and spatial coherence for all the pinhole positions from only one measurement. The only hypothesis is that the pinholes within a small area of the beam center (red circles) are identical in intensity and each pair has same spatial coherence. We will develop a code to retrieve the spatial coherence based only on this assumption. Additionally, the intensity distribution can be consistently checked using a phase retrieval of the recorded hologram. The principle will be tested first using HHG sources at LOA and CEA. The goal is to demonstrate the capability of a single shot mode. We propose to develop then specific instruments for the LASERIX and the FERMI X-ray free electron laser installations, for in situ full spatial coherence inspection. 39 Fig. 12. Principle and experimental demonstration of the NRA spatial coherent measurement. Pictures are extracted from Ref. 1. (a) The NRA is composed of nine pinholes whose autocorrelation (b) has equal amplitudes for all autocorrelation peaks (filled circles) except the center one (open circle). (c) is the measured interferogram of a diode laser (635 nm) and (d) is the deducted spatial coherence of the beam from (b). Fig. 13. SEM images of the NRA patterns that will be used for characterizing our harmonic beam. The white bars in each image is 1 μm. Note that the images are taken with a view angle of about 60 degrees. 4.4.1.2 - Wavefront sensing (Ph. Zeitoun, H. Merdji 2 contributions to be merged) (HM) Although not critical it remains important to achieve a small and homogeneous (aberration-free) focal spot with the XUV beam. Wavefront sensing and adaptive optics will be implemented to keep the wavefront down to the diffraction-limit. Another application of the wavefront sensor will be the optimization of the IDEX XUV beams transport and parameters. As a consequence, we will minimize fluctuations related to wavefront instabilities. Control over the source parameters is mandatory to adjust the micrometer to sub-micrometer focusing. The principle of a Hartmann wavefront sensor is illustrated below. A grid samples the beam. Each sub-beam is then illuminating a specific area of a CCD detector. The deviation of the sub-beams positions compared to references leads to the reconstruction of the phase front of the wave at the grid. As the intensity profile is also recorded, back propagation codes can be applied to calculate for instance the field at focus. In the context of imaging, one could inverse Fourier transform the field at the grid to reconstruct a sample image. However, due to both the reduced sampling (limited by the grid properties) and the limited numerical aperture, the spatial resolution that could be reached with our current detector is limited. Nevertheless, this first image could serve as a guide in the image reconstruction process (the initial guess in the phase retrieval algorithm). Fig. 14. Principle of a Hartmann wavefront sensor. 40 For wavelength lower than 300nm, Hartmann sensing is the most common method used to measure wavefronts. Above 300nm, the Shack Hartmann technique is preferred: Holes are replaced by microlenses. The accuracy and sensitivity of sensors are then increased. The new generation of Shack-Hartmann sensor should include some modifications of the existing algorithms as the expected spots shape on the CCD will be different than those obtained on visible light wavefront sensors. For wavelength under 160nm, the Shack-Hartmann technology is nearly impossible due to a limitation in the existing glass. CEA and LOA in synergy with Imagine Optic will design an optimized Hartmann sensor adapted to the Opt2X beamlines. All the experiment constraints (high resolution, number of available photons, field of view…) will be taken into account to optimize the grid parameters and the CCD choice. Principle of Hartmann or Shack Hartmann spatial resolution improvement The spatial resolution of these types of wavefront sensors is given by the micro lens or micro holes pitch. The lateral positions of the spots of each sub aperture gives the local slopes of the wavefront (i.e. the wavefront first derivative). The spatial resolution is then the sub-aperture pitch. An assumption is done in this analysis: the local wavefront in front of each aperture comprises only tilts. But, when there is some aberrations (except tilts) in the wavefront this assumption is not perfectly correct. There are some small aberrations in the local wavefront in front of each sub aperture. These aberrations change a little bit the shape of each spot (diffraction pattern). It is known that, in small aberration regime, it is possible to determine the aberrations thanks to the deformation of the diffraction pattern. If all the second orders of the aberrations (i.e. focus and astigmatisms) are determined for each sub aperture, the spatial resolution is improved by a factor of 2. If all the second and third orders aberrations are found for each sub aperture, the spatial resolution is 3 times better. OPT2X will use a complete new approach of the Shack-Hartmann technology. CEA will be in charge of these developments with the support of Imagine Optics Company who will commercialize the high resolution Shack Hartmann in the long term. (PhZ) Use of fully or partially coherent soft x-ray sources for application implies a much higher control of the beam quality than for incoherent beams. Within all the applications already developed, OPT2X is particularly interested in non-linear physic in soft x-ray range, coherent imaging and plasma creation with soft x-ray laser. These applications require tight focusing, on a few micrometer spot, with most of the energy contained in the main spot. Such problem has been widely studied for visible and infrared lasers that commonly use wave front sensor associated with an adaptive optics. From our past experience, we observed that the wave front of OPT2X sources (high harmonics and LASERIX) might have very good wave front at the diffraction-limit. The main problem remains in the beam transport and focusing. Also since the beams are propagating under vacuum there is no need of using adaptive optic. As described above we only consider active optic, i.e. an optic with slightly changeable focal length and where coma and astigmatism might be corrected in-line. Wave front sensor for KB focusing on Laserix The wave front sensor associated with such an optic may have relaxed constraints with the advantages of higher compactness, cheaper prize and faster calculation. Actual wave front sensors are based on expensive soft x-ray CCD camera with chip as large 2.5 cm. The sensor has typically 70*70 pupils for sampling the beam giving access to very high order aberration (up to the 36th Zernike polynomial). Since astigmatism at 0° and 45° are the 4th and 6th Zernike polynomial sand coma the 5th, one may understand that such sensor is of too high quality for our purpose. LOA will develop with Imagine Optic a specific wave front sensor having smaller detector and fewer pupils. Such sensor would have high commercial impact for Imagine Optic since it will be designed for active bender as installed on many large-scale facilities. 41 When developed the sensor will be used for optimizing the Kirkpatrick-Baez optic to be installed on LASERIX. The design of this sensor will be very fast. Calibration and test will be done on Salle Orange at LOA with the high harmonic source. We consider also to do some test at FERMI@ELETTRA on their Kirkpatrick-Baez optic. This will serve as final test and also to promote our technology to potential buyers. Wave front sensor for Holography and Coherent Diffraction Imaging Wave front sensing is also important for coherent imaging. Wave front impacts this technic along two issues. Holography and Coherent Diffraction Imaging require focusing the beam on a spot ranging from sub-µm to 10 µm. The spot size depends on the technic and the sample size. However, imaging requires always much better wave front than focusing process. As mentioned above, to achieve a good focusing the beam does not need to be sampled with high spatial resolution. However, on coherent imaging, a residual defect on the incident beam wave front will be encoded on the detector as a defect of the object. The only way to prevent it consists in measuring the wave front of the incident beam with a high spatial resolution and encoded on a high number of Zernike polynomials to subtract the aberrated wave front during the data treatment process (phase retrieval, inverse Fourier-transform …). Although, this problem affects differently the coherent diffraction imaging, the in-line holography or the Fourier-transform holography, it is always a limiting factor. CEA and LOA will work on that subject. Wave front sensor for large NA beam characterization CEA and LOA demonstrated already a spatial resolution of 60 nm using coherent X-ray diffraction imaging coupled with high harmonic beam. This means that the recorded diffraction beam had numerical aperture of nearly 0.5. Measurement of wave fronts at such high numerical aperture is extremely challenging and has never been done so far. CEA and LOA, in collaboration with Imagine Optics will work on the development of such sensor. Post- OPT2X, we consider to test different optics for sub-µm focusing. It will leads to intensity enhancement by one or two orders of magnitude of interest for soft x-ray non-linear physics. It will be also very beneficial for coherent diffraction imaging of very small biological samples 4.4.1.3 - Polarimetry (D. Dowek, J. Gautier, L. Nahon, F. Delmotte) 4.4.2 2 year deliverables 4.4.2.1 on-line measurement of spatial profile (who?) 4.4.2.2 Wavefront sensor (PhZ) Wave front sensor for KB focusing on Laserix Post-doc 1 year: same as for 4.1.2.2 Soft x-ray CCD: 25 kE Mechanics + Hartman plate + alignment system: 15 kE Filters, gas, small consumable: 10 kE Computer for the sensor: 2 kE Development, calculation, new design, tests and calibration by Imagine Optic: 25 kE Wave front sensor for Holography and Coherent Diffraction Imaging Post-doc 1 year: same person as for 4.1.2.2 Soft x-ray CCD: 25 kE Mechanics + Hartman plate + alignment system: 15 kE Filters, gas, small consumable: 10 kE Computer for the sensor: 1 kE Development, calculation, new design, tests and calibration by Imagine Optic: 15 kE 42 Wave front sensor for large NA beam characterization Post-doc 1 year: on high numerical aperture wave front sensing and coherent imaging Soft x-ray CCD: 40 kE Mechanics + Hartman plate + alignment system: 15 kE Filters, gas, small consumable: 10 kE Computer for the sensor: 1 kE Development, calculation, new design, tests and calibration by Imagine Optic: 25 kE 4.4.2.3 complete determination of Stokes numbers (Danielle D, Laurent N) 4.5 WP5: Off-line optics metrology and detector development (F. Polack + F Mercier +...) 4.5.1 technical objectives 4.5.1.1 - off line optics characterization 4.5.1.2 - detector development (specific aspects for XUV pulses? relevance also for WP3 and WP4) (SOLEIL) 4.5.2 2 year deliverables addition to existing infrastructures specific to OPT2X's needs ???? (SOLEIL, CEMOX) 4.6 WP6: Training (Sophie) 4.6.1 Funding PhD theses, internships, 4.6.2 Training modules for students in the labs 4.6.3 Website for training in XUV optics 4.7 Gantt chart for WPs See budget 43 5 Consortium and financial request 5.1 Consortium description (Danielle) Nom, prénom du responsable Dowek Danielle Klisnick Annie Mestdagh Jean-Michel Mons Michel Miron Catalin Polack François Marsi Marino Delmotte Franck Garzella David Carré Bertrand Ros David Lopez-Martens Rodrigo Statut Laboratoire, Etablissements de Taille Commentaires éventuels tutelle équipe (chercheurs et enseignants chercheurs) DR ISMO, CNRS-UPSUD 2 DR ISMO, CNRS-UPSUD 1 DR LFP, CEA-CNRS 2 DR LFP, CEA-CNRS 2 DR SOLEIL 4 DR SOLEIL 2 PR LPS, CNRS-UPSUD 3 MCF LCF - IOGS 3 DR SPAM, CEA 2 Laser and XUV secondary sources DR SPAM, CEA 3 ATTOLAB, high harmonic source MCF LASERIX, UPSUD 4 DR LOA – ENSTA-CNRS 2 5.2 Governance (Danielle) 5.3 financial request (Bertrand) Financial request to IDEX <=> Other funding sources for larger budget ??? Need breakdown per year: indicatively 680 K€ (year 1) and 630 K€ (year 2) WP WP1 WP2 WP3 WP4 Item kEuros Focusing system - few micron focal spot 60 multicolor XUV/IR focusing system 50 polarization control system 150 variable band selection broad band selection multicolor time overlap wavefront sensing polarimetry 230 150 40 100 150 single pulse intensity 30 44 single pulse (auto-analysis) spectrum? pulse time profile WP5 post-doc Ph-D. Student detectors TOTAL requested to Idex 30 30+40 100 90 60 1310 45 To be completed and validated - see excel file - Check compatibility with initial table Deliverable Topic Year1 Year2 cost Time Control WP1 D1.1 Time Control WP1 D1.2 monochromatizing system based on multilayer optics (switchable between “10 fs – single harmonic” mode and “as – broadband” mode) monochromator based on “off plane mount approach” (switchable between “30 fs – narrow bandpass”, “10 fs – single harmonic” and “as–broadband” mode) Time Control WP1 D1.3 Multicolor (XUV/IR) and XUV/XUV time and space (focusing) superposition system (Marie G, Bertrand C) Space Control WP2 D2.1 as-fs / fs-ps : Focusing system grazing-incidence to achieve few micron focal spot (PhZ) Space Control WP2 D2.2 as-fs / fs-ps: “User polarization control system: de-phaser” Space Control WP2 D2.3 as-fs : multicolor XUV/IR and XUV/XUV focusing system (Marie G.) - see D13 x 0 Temporal Characterization WP3 D3.1 Shot-to-shot measurement of pulse intensity x 0 Temporal Characterization WP3 D3.2 As-fs/fs-ps : Shot-to-shot (almost) on line spectrum (recorded/stored during data acquisition) with absolute monitoring of pulse intensity (time & space) x 80 Temporal Characterization WP3 D3.3 as-fs : complete characterization time profile : FROG-CRAB or 2nd order autoco (Thierry R) Temporal Characterization WP3 D3.4 Online, single-shot characterization of XUV pulse by THz streaking Spatial Characterization WP4 D4.1 on-line measurement of spatial profile x 0 Spatial Characterization WP4 D4.2 Wavefront sensor x 354 Spatial Characterization WP4 D4.3 complete determination of all Stokes numbers (Danielle D, Laurent N) x 50 Metrology WP5 D5.1 Metrology x 120 Metrology WP5 Training WP6 Total 640 X 100 x 100 x 107 x 240 x x x 30 59 50 650,5 1291 46 Table 3 : 2-year deliverables, planning and budget 47 6 References 6.1 External F. 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E 86, 026406 (2012) Wilson et al., 58 7 Annex 7.1 XUV source characteristics HHG Plasma HHG Gas (NIR) HHG Gas (MIR) XRL RS FEL LOA Salle Noire SLIC ATTOLAB SLIC ATTOLAB LASERIX SOLEIL METROLOGY LUNEX5 lambda max (m) 1,E-07 1,E-07 1,E-07 2,E-08 1,E-07 1,E-07 lambda min (m) 5,E-09 5,E-09 1,E-09 2,E-09 2,E-09 1,E-09 Ephot min (eV) 12 12 12 62 12 12 Ephot max (eV) 248 248 1239 620 620 1239 reprate 1,E+03 1,E+04 1,E+03 1,E+01 1,E+08 1,E+03 duration min (s) 1,E-16 1,E-16 1,E-16 1,E-12 3,E-11 1,E-15 duration max (s) 1,E-14 1,E-14 1,E-14 1,E-12 3,E-11 3,E-14 3,E-02 3,E-02 3,E-02 3,E-04 1,E-05 1,E-02 3,E+00 3,E+00 3,E+00 3,E-04 1,E-05 3,E-01 1,E-08 1,E-09 1,E-09 1,E-06 1,E-12 1,E-04 1,E-05 1,E-06 1,E-06 1,E-06 1,E-12 1,E-04 Nphot/sec min 3,E+11 3,E+11 5,E+09 1,E+11 1,E+12 5,E+14 Nphot/sec max 5,E+15 5,E+15 5,E+14 1,E+12 5,E+13 5,E+16 Bandwith min (eV) Bandwith max (eV) Energy/pulse min (J) Energy/pulse max (J) 7.2 French teams in ultrafast dynamics [FrenchUFD] (PSC means Paris-Saclay Campus) Gas Phase French laboratories hosting one or more UFD teams Laboratoire Charles Fabry de l'Institut d'Optique (LCFIO, PSC) http://iramis.cea.fr/spam/inde x.php x http://iramis.cea.fr/spam/ME C/?lang=ang&num=0&keyw= http://www.lcf.institutoptique .fr/ Institut des Sciences Moléculaires d’Orsay (ISMO, PSC) http://www.ismo.u-psud.fr/ Service des Photons, Atomes et Molécules (SPAM, PSC) http://www.synchrotronsoleil.fr/ http://wwwLaboratoire Francis Perrin (LFP, PSC) lfp.cea.fr/?lang=ang&num=0& keyw= Service de Physique et Chimie des Surfaces et Interfaces http://iramis.cea.fr/spcsi/inde (SPCSI, PSC) x.php SOLEIL (PSC) Condensed Plasma Phase s Biolog R&D y laser x x x x x x x x x Laboratoire de Physique des Solides (LPS, PSC) http://www.lps.u-psud.fr/ x Laboratoire des Solides Irradiés (LSI, PSC) http://www.lsi.polytechnique. fr/jsp/accueil.jsp?CODE=05322 973&LANGUE=1 x Laboratoire d’Optique Appliquée (LOA, PSC) http://loa.ensta-paristech.fr/ x x x 59 Centre de Physique Théorique (Marseille) Centre Lasers Intenses et Applications (CELIA, Bordeaux) Département Optique, Interaction MatièreRayonnement (OMR, Dijon) Institut de Physique de Rennes (IPR, Rennes) Institut de Physique et Chimie des Matériaux de Strasbourg (IPCMS, Strasbourg) Institut de Recherche sur les Systèmes Atomiques et Moléculaires Complexes (IRSAMC, Toulouse) Laboratoire Aimé Cotton (LAC, PSC) Laboratoire de Chimie Physique (LCP, PSC) Laboratoire de Chimie Physique Matière et Rayonnement (LCPMR) Laboratoire de Dynamique, Interactions et Réactivité (LADIR, Lille) Laboratoire de Physico-Chimie des Matériaux Luminescents (LPCML, Lyon) Laboratoire de Physique des Gaz et des Plasmas (LPGP, PSC) Laboratoire de Physique Théorique de la Matière Condensée (LPTMC, PSC)) Laboratoire de Spectrométrie Ionique et Moléculaire (LASIM, Lyon) Laboratoire Optique et Biosciences (LOB, PSC) Laboratoire pour l'Utilisation des Laser Intenses (LULI, PSC) Lasers, Plasmas and Photonic Processes (LP3 Marseille) Physique des Interactions Ioniques et Moléculaires (PIIM, Marseille) http://www.cpt.univ-mrs.fr/ http://www.celia.ubordeaux1.fr/ http://icb.ubourgogne.fr/OMR/ http://www.ipr.univrennes1.fr/FR/home http://www-ipcms.ustrasbg.fr/ x x x x x x x x http://www.irsamc.ups-tlse.fr/ x http://www.lac.u-psud.fr/x Laboratoryhttp://www.lcp.upsud.fr/rubrique.php3?id_rubr x ique=266/ http://www.lcpmr.upmc.fr/ x http://www.ladir.cnrs.fr/ x http://pcml.univ-lyon1.fr/ x x http://www.lpgp.upsud.fr/modeles/ind.php x http://www-lasim.univx lyon1.fr/ http://www.lob.polytechnique .fr/ http://www.luli.polytechnique .fr/ http://www.lp3.univmrs.fr/lp3-gb.htm http://www.piim.up.univmrs.fr/ Total 14 x x x x 11 5 x 2 7.3 XUV HHG sources [LOA-Palaiseau] http://loa.ensta.fr/ [CLF-RAL-Oxford] http://www.clf.rl.ac.uk/Facilities/Artemis/12270.aspx [ETH-Zürich] http://www.ulp.ethz.ch/research/research_overview [IC-London] http://www.imperial.ac.uk/research/qols/ [ICFO-Barcelona] http://www.icfo.es/index.php?section=research5&lang=english [IMS-Ottawa] http://www.nrc-cnrc.gc.ca/eng/research/physics.html [JILA-Boulder] http://jila.colorado.edu/kmgroup/ [KAIST-Daejeon] http://www.kaist.ac.kr/english/03_academics/02_research.php [LLC-Lund] http://www-llc.fysik.lth.se/ [MPQ-Garching] http://www.attoworld.de/ [MPIK-Heidelberg] http://www.mpi-hd.mpg.de/ullrich/page.php?id=25 [MBI-Berlin] http://www.mbi-berlin.de/en/research/program/atoms/index.html 60 5 [PoliMi-Milano] http://www.fisi.polimi.it/dip-fisica/page167.do [TUV-Vienna] http://atto.photonik.tuwien.ac.at [RIKEN-Tokyo] http://www.riken.jp/lab-www/mid-lab/untitled1-e.html [AMOLF-Amsterdam] http://www.amolf.nl/research/xuv-physics/ [ALLS-Toronto] http://lmn.emt.inrs.ca/EN/ALLS.htm [KSU-Kalamazoo] http://jrm.phys.ksu.edu/exp-research-grps.html [OSU-Colombus] http://www.physics.ohio-state.edu/~dimauro/ [IOPCAS-Beijing] http://english.iop.cas.cn/ 7.4 Funded projects 7.5 Training activity 7.6 Industrial Partnership - letters of interest 7.6.1 Horiba (FP) 7.6.2 Amplitude Techno (BC) 7.6.3 Fastlite (BC) 7.6.4 EOTECH (FP) 7.6.5 Imagine Optics (HM) 7.6.6 Phase view ? 7.6.7 61