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
State-of-the art ................................................................................................................................ 5
2.1
2.1.1
International – National (Marino - Rodrigo).................................................................... 5
2.1.2
Local (Franck instrumentation) ....................................................................................... 6
2.2
3
Existing Tools and User communities ...................................................................................... 5
What is missing and needed in Paris-Saclay campus (Danielle) .............................................. 7
2.2.1
Structuring and maintaining high level expertise............................................................ 7
2.2.2
Technical needs ............................................................................................................... 7
2.2.3
Needs in training ............................................................................................................. 7
Objectives ........................................................................................................................................ 8
3.1
Structuring objectives in the perspective of UPS (Marino) ..................................................... 9
3.2
Technological objectives (Marino) .......................................................................................... 9
3.3
Training (Sophie K) .................................................................................................................. 9
3.3.1
Maintaining expertise...................................................................................................... 9
3.3.2
Existing involvement/actions in training ......................................................................... 9
3.3.3
Future actions in training ................................................................................................ 9
3.4
Academic dissemination (Danielle) ......................................................................................... 9
3.4.1
existing actions ................................................................................................................ 9
3.4.2
Interest and future actions ............................................................................................ 10
3.5
industrial dissemination : technological transfer .................................................................. 10
3.5.1
Existing joint actions and projects ................................................................................. 10
3.5.2
Interest and future actions ............................................................................................ 10
3.6
Scientific benchmark studies (all) .......................................................................................... 10
3.6.1
atto time-resolved study in gas phase (Bertrand C, …) ................................................. 10
3.6.2
PI and polarization control – chirality (Danielle D, L. Nahon, T. Ruchon) ..................... 11
3.6.3
atto time-resolved study in solid (Marino).................................................................... 11
3.6.4
as-fs Ultrafast Phenomena at a nanometer scale (Hamed M) ...................................... 11
3.6.5
fs-ps timescale WDM (Annie K) ..................................................................................... 14
3.6.6
application bio (Philippe Z. to be discussed and selected) ............................................ 14
3.7
2 year deliverables (Marino) ................................................................................................. 14
2
4
3.7.1
Technical ........................................................................................................................ 14
3.7.2
Training and Dissemination ........................................................................................... 14
Methodology and work plan. ........................................................................................................ 15
4.1
4.1.1
Overall technical objectives........................................................................................... 19
4.1.2
2 year deliverables......................................................................................................... 21
4.2
Overall technical objectives........................................................................................... 21
4.2.2
2 year deliverable .......................................................................................................... 23
Overall technical objectives........................................................................................... 24
4.3.2
2 year deliverables......................................................................................................... 25
WP4: On-line diagnostics of spatial properties and polarization (Ph. Zeitoun + ...) ............. 25
4.4.1
Overall technical objectives........................................................................................... 25
4.4.2
2 year deliverables......................................................................................................... 29
4.5
WP5: Off-line optics metrology and detector development (F. Polack + F Mercier +...) ...... 29
4.5.1
technical objectives ....................................................................................................... 29
4.5.2
2 year deliverables......................................................................................................... 29
4.6
WP6: Training (Sophie) .......................................................................................................... 31
4.6.1
Funding PhD theses, internships, .................................................................................. 31
4.6.2
Training modules for students in the labs ..................................................................... 31
4.6.3
Website for training in XUV optics ................................................................................ 31
4.7
7
WP3: On-line diagnostics of spectro-temporal properties (A. Klisnick + D. Garzella +....) .... 24
4.3.1
4.4
6
WP2: Control of spatial profile and polarization (F. Polack + ....) ......................................... 21
4.2.1
4.3
5
WP1: Control of the spectro-temporal profile (F. Delmotte + ...) ......................................... 19
Gantt chart for WPs ............................................................................................................... 31
Consortium and financial request ................................................................................................. 32
5.1
Consortium description (Danielle) ........................................................................................ 32
5.2
Governance (Danielle) ........................................................................................................... 32
5.3
financial request (Bertrand) .................................................................................................. 32
References ..................................................................................................................................... 36
6.1
External.................................................................................................................................. 36
6.2
OPT2X Consortium ................................................................................................................ 39
Annex ............................................................................................................................................. 43
7.1
Funded projects ..................................................................................................................... 43
7.2
Training activity ..................................................................................................................... 43
7.3
Industrial Partnership - letters of interest............................................................................. 43
7.3.1
Horiba (FP) ..................................................................................................................... 43
7.3.2
Amplitude Techno (BC).................................................................................................. 43
7.3.3
Fastlite (BC).................................................................................................................... 43
7.3.4
EOTECH (FP)................................................................................................................... 43
3
7.3.5
Imagine Optics (HM) ...................................................................................................... 43
7.3.6
Phase view ? .................................................................................................................. 43
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
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
5
[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/
2.1.1.2 Laser X (Sophie K.)
Rocca
Korea
GSI ?
MBI
PALS
Romania
2.1.1.3 FEL (Marino – MEC – David G)
LCLS
FLASH
SACLA
FERMI
LUNEX5 ?
Swiss FEL
2.1.2 Local (Franck instrumentation)
Partner Laboratories and facilities (LOA, LaseriX, SPAM, Soleil, …)
- Experimental projects and stations supported by local research networks (Triangle, PALM)
- Sources supported by national programs Equipex CILEX, ATTOLAB,…
SOLEIL metrology
LaseriX XUV/XUV
XUV-IR
LOA Salle Rouge
Magnétisme
Optique cohérente
Métrology
6
Attolab FAB1 – FAB10
Matière condensée
LUCA
Sofockle
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
7
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 3-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
characterisation of the XUV pulses delivered to the user stations. These crucial issues will be
8
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
LUMAT
9
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 ℰ⃗𝑋𝑈𝑉 XUV
10
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
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
11
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 [Rava09, Gaut10, 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.
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].
12
Fig. ..: 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 with the 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
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
13
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 1012
- 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:
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
14
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.
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.
15
Generic beamlines (Annex ?)
Figure 1 : Generic atto-fs HHG-based beamline
16
Figure 2 : Generic fs-ps XRL beamline
17
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 1 : 2-year Deliverables
18
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, ....)
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].
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 = ), it is possible to produce electronic/nuclear wavepacket
2
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 (many hours or even days) required for data acquisition. In
this scheme an active stabilization control of the arms is mandatory [Böttcher2008,
Ruchon2010]. This can be implemented by the means of a data acquisition card piloted via a
servo-program developed in Labview at the lab. In the servo-program, a first step is
dedicated to the calibration of the system and a second step is dedicated to its operation.
The servo-loop is based on a PID algorithm: the PID compensate for the difference between
the measured value and the set point. Generally this program is working together with a
RABBIT data acquisition program.
2) 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
19
narrow band XUV 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
3) Figure 3 [UltrafastInnov].
In experiment requiring long acquisition time (several hours) at 1-10 kHz, active stabilization of the
time- and space overlap is mandatory. Figure 3b gives example of the interferometric scheme
adapted to the coaxial delay line [Böttcher08].
Figure 3 : 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].
Two-color parabolic mirror
4.1.1.3 as-fs : attolighthouse (FQuéré - B. Carré)
4.1.1.4 fs-ps : XUV/XUV (Willem ?)
Amplitude division beamsplitters are not readily available in the XUV domain because of the high
absorption of the materials. 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 one fixed half and one controlled half that can be moved along the beam position with a high
precision – see Figure 4c. However the scanning range is limited. Moreover, any modification of the
wavelength implies using a new set of mirrors. A more versatile option is to use a system that can be
inserted before the focusing optics. For instance, the 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 Figure 4a. 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.
20
Figure 4 : XUV beam splitters for XUV/XUV pump-probe experiments.
see e.g. systems developed in the fs regime for FELs experiments (Moshammer et al)
Danielle D OK pour discussions
4.1.1.5 as-fs: Diffractive optics (conical grating) for selecting single harmonic (DE ~100
meV, < 10 fs) (F. Polack, ...)
4.1.1.6 as-fs: Mechanical stability (LOA, SOLEIL)
4.1.2
4.1.2.1
2 year deliverables
monochromatizing system based on multilayer optics (easily switchable between a
“10 fs – single harmonic” mode and an “as – broadband” mode)
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)
see 4.1.1.2 and 0
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
21
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
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.
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 (J. Gautier LOA)
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 5. 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.
22
Figure 5 : 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.
4.2.1.4 as-fs / fs-ps: Simulations (F. Delmotte)
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.
Tele-microscope: 10 kE
Set of samples + motorized holder: 15 kE
Kirkpatrick-Baez bender: 110 kE
Vacuum chamber + optical table (to dump the vibrations): 35 kE
XUV wave front sensor: developed by LOA and Imagine optic. (see 4.3.1.2)
Filters, gas, samples, consumables for tests: 20 kE
23
Post-doc 1 year: 50 kE
4.2.2.2 as-fs / fs-ps: “User polarization control system: de-phaser” : if realistic and feasible,
otherwise medium term development
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.
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.
4.3 WP3: On-line diagnostics of spectro-temporal properties (A. Klisnick +
D. Garzella +....)
4.3.1
Overall technical objectives
4.3.1.1 As-fs : complete characterization of ultrashort pulses : Quantum interferometry &
FROG techniques (Thierry R)
XUV/XUV photoionization : 2nd order autocorrelation
Two-color XUV/IR Quantum interferometry (FROG-CRAB, RABBIT)
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:
 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)
24
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)
On line XUV spectro after interaction chamber (Willem B)
grating 1st order diffraction (Willem)
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 (when needed)
FROG-CRAB or 2nd order autoco (Thierry R)
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.
25
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.
Fig. 5.1. 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. 5.2. 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
26
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. 7. Principle of a Hartmann wavefront sensor.
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 IDEX 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.
27
(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.
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
28
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
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)
29
30
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
31
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
32
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
33
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
34
Table 2 : 2-year deliverables, planning and budget
35
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42
7 Annex
7.1 Funded projects
7.2 Training activity
7.3 Industrial Partnership - letters of interest
7.3.1
Horiba (FP)
7.3.2
Amplitude Techno (BC)
7.3.3
Fastlite (BC)
7.3.4
EOTECH (FP)
7.3.5
Imagine Optics (HM)
7.3.6
Phase view ?
7.3.7
43