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The dynamics of chemical bonds by ultrafast electron diffraction

English title The dynamics of chemical bonds by ultrafast electron diffraction
Applicant Carbone Fabrizio
Number 128269
Funding scheme SNSF Professorships
Research institution Institut des sciences et ingénierie chimiques EPFL - SB - ISIC
Institution of higher education EPF Lausanne - EPFL
Main discipline Condensed Matter Physics
Start/End 01.09.2010 - 31.08.2014
Approved amount 1'664'021.00
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All Disciplines (2)

Discipline
Condensed Matter Physics
Physical Chemistry

Keywords (14)

Femtosecond electron-diffraction; organic thin-films; superconductor; streak camera; electron-phonon coupling; quantum criticality; bulk helium; graphene; femtosecond; electron diffraction; ultrafast; nanostructures; superconductivity; quantum solids

Lay Summary (English)

Lead
Lay summary
The static structure of molecules and solids determines their ground state properties. The investigation of chemical reactions and phase transitions, requires the direct observation of the steps and structural changes through which they occur. Such changes take place on different time scales. Collective behaviors of ions in complex systems and solids can take from fs to microseconds (3-5). In this project, we propose to investigate the structural dynamics of low dimensional systems and superconductors with a novel apparatus based on Ultrafast Electron Crystallography (UEC). Time-resolved electron diffraction is a unique tool for providing information on the structural dynamics of solids, nano-sized materials, and atomically thin layers, thanks to the high scattering cross section of electrons. Fs lasers are used to generate ultrashort light and electron pulses. Light initiates a process in the sample and by recording snapshots of the electrons diffracted from the sample in a stroboscopic fashion, one can image the photo-induced motion of the structure. Here we propose a new experimental configuration based on a radiofrequency streak camera, which should provide a better time-resolution than what is currently available. Thanks to this new apparatus, the physics of phase transitions in low-dimensional solids will be accessible. In fact, the sensitivity to mono-layers of light elements will allow us to study Carbon based thin films and the interface between graphene and other materials, in particular Helium. A new class of molecular solids called diamondoids combine diamond-like properties such as great rigidity and strength, with the chemistry of hydrocarbon molecules and thus have the potential for precise construction and assembly via derivatization strategies. Information about the structural dynamics of these systems is necessary both for fundamental and practical reasons. Another subject of investigation will be superconductivity. Whether the structural changes occurring at the superconducting transition temperature cause superconductivity, or are a consequence of the modified electronic structure below Tc is currently under intense debate. The temporal evolution of these effects can be accessible to modern time-resolved techniques, capable of fs (femtosecond) time-resolution, the time-scale of Cooper pair formation and electron-phonon coupling. UEC provides a unique tool for investigating the electron-phonon coupling in High-Tc`: In a cold superconductor, the initial excitation is used to drive the electronic structure in the normal state, the structural motions are followed in time while the electrons reach their equilibrium with the lattice.
Direct link to Lay Summary Last update: 21.02.2013

Responsible applicant and co-applicants

Employees

Publications

Publication
Order/Disorder Dynamics in a Dodecanethiol-Capped Gold Nanoparticles Supracrystal by Small-Angle Ultrafast Electron Diffraction
G. F. Mancini T. Latychevskaia F. Pennacchio J. Reguera Francesco St (2016), Order/Disorder Dynamics in a Dodecanethiol-Capped Gold Nanoparticles Supracrystal by Small-Angle Ultrafast Electron Diffraction, in NanoLetters, 16(4), 2705-2713.
Coupling of a high-energy excitation to superconducting quasiparticles in a cuprate from coherent charge fluctuation spectroscopy
B. Mansart, J. Lorenzana, A. Mahn, A. Odeh, M. Scarongella, M. Chergui, F. Carbone (2013), Coupling of a high-energy excitation to superconducting quasiparticles in a cuprate from coherent charge fluctuation spectroscopy, in PNAS, 110, 4539.
Investigating pairing interactions with coherent charge fluctuation spectroscopy
J. Lorenzana, B. Mansart, A. Mann, A. Odeh, M. CHergui, F. Carbone (2013), Investigating pairing interactions with coherent charge fluctuation spectroscopy, in The European Physical Journal Special Topics, , 222, 1223.
Quantitative imaging of flux vortices in the type-II superconductor MgB2 using cryo-Lorentz transmission electron microscopy
M.J.G. Cottet et al (2013), Quantitative imaging of flux vortices in the type-II superconductor MgB2 using cryo-Lorentz transmission electron microscopy, in Phys. Rev. B, 88, 014505.
Temperature-dependent electron-phonon coupling in La2−xSrxCuO4 probed by femtosecond x-ray diffraction
B. Mansart et al (2013), Temperature-dependent electron-phonon coupling in La2−xSrxCuO4 probed by femtosecond x-ray diffraction, in Phys. Rev. B, 88, 054507.
A perspective on novel sources of ultrashort electron and X-ray pulses
Carbone Fabrizio (2012), A perspective on novel sources of ultrashort electron and X-ray pulses, in Chemical Physics, 392, 1-9.
Design and implementation of a flexible beamline for fs electron diffraction experiments
Mancini G.F., Mansart B., Pagano S., van der Geer B., de Loos M., Carbone F. (2012), Design and implementation of a flexible beamline for fs electron diffraction experiments, in Nuclear Instruments and Methods in Physics Research Section A, 691, 113-122.
Evidence for a Peierls phase-transition in a three-dimensional multiple charge-density waves solid.
B. Mansart, M. J. G. Cottet, Thomas J. Penfold, Stephen B. Dugdalee, Riccardo Tediosi, Majed Chergui, Fabrizio Carbone (2012), Evidence for a Peierls phase-transition in a three-dimensional multiple charge-density waves solid., in PNAS, 109, 5603-5608.
Femtosecond carrier dynamics in bulk graphite and graphene paper
Carbone Fabrizio et al. (2011), Femtosecond carrier dynamics in bulk graphite and graphene paper, in Chemical Physics Letters, 504, 37-41.
Modern electron microscopy resolved in space, energy and time
Carbone Fabrizio (2011), Modern electron microscopy resolved in space, energy and time, in E. Phys. J.-Appl. Phys., 54, 33503-33514.

Collaboration

Group / person Country
Types of collaboration
University of Munich Germany (Europe)
- Research Infrastructure
University of Rome Italy (Europe)
- in-depth/constructive exchanges on approaches, methods or results
University of Eindhoven Netherlands (Europe)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure
University of California Los Angeles United States of America (North America)
- in-depth/constructive exchanges on approaches, methods or results
- Research Infrastructure

Scientific events

Active participation

Title Type of contribution Title of article or contribution Date Place Persons involved
IMC 2014 Talk given at a conference Fs-imaging of plasmon polaritons 01.09.2014 Prague, CZech Republic, Slovakia Carbone Fabrizio;
ECRYS summer school Talk given at a conference Ultrafast imaging of plasmons 18.08.2014 Cargese, Corsica, France Carbone Fabrizio;
SPS meeting Talk given at a conference Simultanoues observation of the wave-particle duality of a plasmonic field 02.07.2014 Fribourg, Switzerland Carbone Fabrizio;
Nobel Metals Nanoparticles, Gordon conference Talk given at a conference Ultrafast diffractive imaging from 2D self-assembled gold nano particles 15.06.2014 Boston, United States of America Mancini Giulia Fulvia;
Photo-induced phase transitions PIPT Talk given at a conference Photo-induced ordering phenomena in functionalized nanoparticles by Ultrafast Electron Diffractive Imaging 08.06.2014 Bled, Slovenia Carbone Fabrizio;
FEIS 2013 Talk given at a conference Time-domain observation of coherent phenomena in solids and nano-structures 09.12.2013 Key West, United States of America Carbone Fabrizio;
Physics colloquium Individual talk Ultrafast investigation of high temperature superconductors 06.11.2013 Fribourg, Switzerland Carbone Fabrizio;
The new generation in strongly correlated systems Talk given at a conference Introduction to the session "Coherent control of superconductivity" 01.07.2013 Sestri Levante, Italy Carbone Fabrizio; Mansart Barbara Laurence Paulette;
Superstripes Talk given at a conference Real-time oscillations of the superconducting condensate in a high-Tc superconductor 26.05.2013 Ischia, Italy Carbone Fabrizio;
Summer school "Quantitative Electron Microscopy" Talk given at a conference Ultrafast transmission electron microscopy 20.05.2013 Saint Aygulf, France Carbone Fabrizio; Mansart Barbara Laurence Paulette;
Cold beams, workshop Talk given at a conference Vortex dynamics in MgB2 01.10.2012 Nimes, France, France Mancini Giulia Fulvia; Carbone Fabrizio;
Electron Microscopy Conference Talk given at a conference Design and implementation of a fs TEM 21.09.2012 Manchester, UK, Great Britain and Northern Ireland Carbone Fabrizio;
LEES 2012 Talk given at a conference Coherent oscillations of Cooper pairs in LSCO 24.07.2012 Napa Valley, USA, United States of America Mancini Giulia Fulvia; Mansart Barbara Laurence Paulette;
Ultrafast phenomena, conference Talk given at a conference Coherent oscillations of Cooper pairs in LSCO 09.07.2012 Lausanne, Switzerland Mancini Giulia Fulvia; Carbone Fabrizio; Mansart Barbara Laurence Paulette;
SPS meeting Talk given at a conference Ultrafast optical spectroscopy of strongly correlated solids 21.06.2012 Zurich, Switzerland Carbone Fabrizio;
From biology to condensed matter physics Talk given at a conference Ultrafast spectroscopy of high temperature superconductors 09.06.2012 Dubrovnik, Croatia, Croatia Carbone Fabrizio;
SSOM Talk given at a conference Ultrafast EELS of graphite films 04.04.2012 Les Diablerets, CH, Switzerland Carbone Fabrizio;
"froniters in condensed matter physics" Talk given at a conference Ultrafast spectroscopy of superconductors 20.03.2012 Zermatt, CH, Switzerland Carbone Fabrizio;
MUST meeting Talk given at a conference Presentation of the Laboratory for Ultrafast microscopy and electron scattering 09.01.2012 Lenk, Switzerland Carbone Fabrizio;
PSI summer school 2011 Talk given at a conference Ultrafast science, tools and methods 15.08.2011 Zug, Switzerland Carbone Fabrizio;
SFMu Conference, plenary speaker Talk given at a conference Ultrafast electron microscopy of graphite and related materials 27.06.2011 Strasbourg, France Carbone Fabrizio;
Quantum workshop, invited speaker Talk given at a conference The perspective of novel X-rays and electron sources 18.05.2011 Leysin, CH, Switzerland Carbone Fabrizio;
Ultrafast Dynamics of Strongly Correlated Solids. Workshop, invited speaker Talk given at a conference Ultrafast Dynamics of Strongly Correlated Solids 05.04.2011 Zurich, Switzerland Carbone Fabrizio;
Invited seminar at the physics colloquium, University of Bern Talk given at a conference The dynamics of charge ordering in LuIrSi 10.03.2011 Bern, Switzerland Carbone Fabrizio;
Monochromatic ion and electron beams: new sources and applications. Workshop, invited speaker Talk given at a conference Ultrafast electron diffraction technology 16.02.2011 Paris, France Carbone Fabrizio;
ECOSS Conference, invited speaker Talk given at a conference Coherent oscillations of the superconducting condensate in LSCO 01.09.2010 Groningen, Netherlands Carbone Fabrizio; Mansart Barbara Laurence Paulette;


Awards

Title Year
Prize for excellent teaching performance 2013

Associated projects

Number Title Start Funding scheme
126409 Real-time structural investigation of superconductors 01.11.2009 Ambizione
159219 Femtosecond control of topological magnetic patterns 01.04.2015 Project funding (Div. I-III)
165560 Light-induced control of the Metal Insulator Transition in Magnetite 01.04.2016 Project funding (Div. I-III)
117088 Proposition d'éxperiences de Diffraction Ultra-rapide d'électrons sur des couches minces organiques au Caltech 01.04.2007 Fellowships for prospective researchers
121300 Functional protein dynamics via non-linear spectroscopy in the UV 01.07.2009 R'EQUIP

Abstract

Ultrafast electron diffraction (UEC) is a unique tool for providing direct and detailed information on the structural dynamics of molecules, solids, nano-sized materials, and atomically thin layers, thanks to the high cross section for interaction between electron and matter. Femtosecond lasers are used to generate ultrashort light and electron pulses. Light initiates a process in the sample - a phase transition, an electronic excitation or simply a temperature jump - and by recording snapshots of the electrons diffracted from the sample in a stroboscopic fashion, one can image the photo-induced motion of the structure. By varying the experimental geometry, the probed thickness can be tuned, allowing to study bulk properties and interfaces.Here, we propose a new experimental configuration, which should provide a nearly 10 times better time-resolution than what is currently available. With a resolution around 100 fs, we want to understand the following physical phenomena: i) the structural dynamics of organic low-dimensional systems ii) the pairing mechanism in high temperature superconductors and its relation to the chemistry of the material.In recent years, there has been much interest in the properties of nano-sized materials, biological aggregates, atomically thin layers, and sub-picosecond phenomena in chemical reaction and solids. These systems, together with the need for ultra fast devices in modern electronics, have pushed experimentalists to develop techniques sensitive to minute amounts of material and capable of fs time resolution. The combination of microscopy and spectroscopy has appealed to researchers for many years.With time resolved X-ray diffraction, k-space microscopy and time resolution were successfully combined, and provided a unique tool for the investigation of many structural phenomena. Recently, it has been shown that ultrafast electron diffraction can be a valid alternative to X-ray diffraction. In fact, electrons have a million times higher cross section for interaction with matter then X-rays, which allows the investigation of atomically thin samples such as graphene, and systems made of light elements, relevant for biology.Currently, electron bunches containing up to 2000 e- per pulse are generated at the photo-cathode and accelerated up to several tens of kV, in order to limit the space charge effect and keep the time resolution below 1 ps. This solution requires rather long acquisition times when sub-ps resolution is needed. In the proposed scheme, we use long electron pulses, which can contain up to a million electrons in 10 - 30 ps. The diffracted electron pulses will then be detected by a combination of a streak camera, which transforms the time coordinate into a spatial coordinate, and an imaging CCD camera. In this configuration, the time resolution can be pushed to the laser pulse duration itself (50 to 100 fs), i.e. nearly 10 times better than what is currently available, and all the temporal evolution of one Bragg reflection can be acquired within one pulse. Moreover, it is not necessary to accelerate the electrons up to very high voltages, opening the possibility to detect inelastic processes. A new type of streak camera employing radiofrequency fields is able to deflect several microns particles separated by 50 fs. Such a device has been developed in UCLA by Dr. Pietro Musumeci and Prof. Jamie Rosenzweig for relativistic electron beams (i.e. electrons accelerated up to few MeV). This device demonstrated a resolution of 50 fs, on 300 fs relativistic electron pulses containing up to 100 millions electrons. A different design for “slow”, KeV electrons have been manufactured at UCLA within a collaboration between Dr Carbone and prof. Musumeci, and will be used in our experiments. Thanks to this apparatus we propose to investigate the following subjects:- The structural properties of organic thin films such as ultrathin graphite or diamondoids. New and unexpected structural phenomena in solids and nanostructures have been observed in prof. Zewail`s lab by means of UEC (for example an ultrafast compression of graphite`s lattice in response to laser excitation, and the nature of the structural phase transition in VO2). The extention of these studies to different organic nanostructures like thin films, nanotubes and diamondoids would give the unique possibility to observe photoinduced structural changes in atomically thin materials of interest for applications. Also, thanks to the control of graphite`s surface, we will be able to study the quantum critical phase transitions in Helium films deposited on graphite. -The pairing mechanism in high temperature superconductors; the reaction of the lattice to a laser pulse capable of driving a superconductor in the normal state helped clarifying the role of the lattice dynamics, in the formation of Cooper pairs. The first results obtained at Caltech by Dr Carbone demonstrated the ability of ultrafast electron diffraction in retrieving the electron-phonon coupling parameter and its symmetry in complex systems. An extensive study of the laser induced structural dynamics in different superconductors will allow us to understand the relation between the phase transition and the chemistry of the materials. This project would be carried out on samples grown in the group of Dirk van der Marel at the university of Geneva.
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