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Center of Research Excellence in
Ultrafast Science: !
Building on Strength at MSU
• initiated in 2009 by Professor Phil Duxbury
• initiated in 2009 by Professor Phil Duxbury
• initial commitment of 5 years at $500,000/year
• initiated in 2009 by Professor Phil Duxbury
• initial commitment of 5 years at $500,000/year
• focus on infrastructure development, promotion and support for interdisciplinary research teams across Chemistry, Physics, and Engineering, and increase the visibility of materials research at MSU
• initiated in 2009 by Professor Phil Duxbury
• initial commitment of 5 years at $500,000/year
• focus on infrastructure development, promotion and support for interdisciplinary research teams across Chemistry, Physics, and Engineering, and increase the visibility of materials research at MSU
• over 25 faculty affiliated with CORE-CM, including 10 new faculty hires
• initiated in 2009 by Professor Phil Duxbury
• initial commitment of 5 years at $500,000/year
• focus on infrastructure development, promotion and support for interdisciplinary research teams across Chemistry, Physics, and Engineering, and increase the visibility of materials research at MSU
• over 25 faculty affiliated with CORE-CM, including 10 new faculty hires
• > $17M in external funding for multi-PI grants generated by projects initiated through CORE-CM to date
• initiated in 2009 by Professor Phil Duxbury
• initial commitment of 5 years at $500,000/year
• focus on infrastructure development, promotion and support for interdisciplinary research teams across Chemistry, Physics, and Engineering, and increase the visibility of materials research at MSU
• over 25 faculty affiliated with CORE-CM, including 10 new faculty hires
• > $17M in external funding for multi-PI grants generated by projects initiated through CORE-CM to date
• has supported multiple national and international symposia, funded seminar programs within the colleges of Natural Science and Engineering, and created new courses in energy science (among others)
• initiated in 2009 by Professor Phil Duxbury
• initial commitment of 5 years at $500,000/year
• focus on infrastructure development, promotion and support for interdisciplinary research teams across Chemistry, Physics, and Engineering, and increase the visibility of materials research at MSU
• over 25 faculty affiliated with CORE-CM, including 10 new faculty hires
• > $17M in external funding for multi-PI grants generated by projects initiated through CORE-CM to date
• has supported multiple national and international symposia, funded seminar programs within the colleges of Natural Science and Engineering, and created new courses in energy science (among others)
• helped establish MSU’s presence in SOFI, a Solar Fuels Institute created by Northwestern University and Uppsala University in Sweden
In-house Excellence in Ultrafast Science
• seminar program in Spring 2014 highlighted the unique strength MSU currently has in ultrafast science
In-house Excellence in Ultrafast Science
• seminar program in Spring 2014 highlighted the unique strength MSU currently has in ultrafast science
• >10 faculty across Chemistry and Physics have active, well-funded research programs in ultrafast science
In-house Excellence in Ultrafast Science
• seminar program in Spring 2014 highlighted the unique strength MSU currently has in ultrafast science
• >10 faculty across Chemistry and Physics have active, well-funded research programs in ultrafast science
• represents one of the fastest growing areas of research in the physical sciences
In-house Excellence in Ultrafast Science
• seminar program in Spring 2014 highlighted the unique strength MSU currently has in ultrafast science
• >10 faculty across Chemistry and Physics have active, well-funded research programs in ultrafast science
• represents one of the fastest growing areas of research in the physical sciences
• ties in to a significant number of so-called Grand Challenges that are funding targets for several agencies…
In-house Excellence in Ultrafast Science
Grand Challenges
Grand Challenges
• Grand Challenges identified by the Office of Science at DOE (above) and the White House office of Science and Policy (left)
Grand Challenges
• Grand Challenges identified by the Office of Science at DOE (above) and the White House office of Science and Policy (left)
Grand Challenges
• Grand Challenges identified by the Office of Science at DOE (above) and the White House office of Science and Policy (left)
• ultrafast science plays a key role in virtually all of these efforts
A Center for Ultrafast Science
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
• serve as a nexus for ultrafast science in the Midwest, eventually coupling with the University of Michigan (a Michigan Ultrafast Sciences Corridor) and several large-scale user facilities worldwide
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
• serve as a nexus for ultrafast science in the Midwest, eventually coupling with the University of Michigan (a Michigan Ultrafast Sciences Corridor) and several large-scale user facilities worldwide
• new faculty hires in both existing and emerging areas (e.g., energy science, heterogeneous catalysis, natural and artificial photosynthesis)
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
• serve as a nexus for ultrafast science in the Midwest, eventually coupling with the University of Michigan (a Michigan Ultrafast Sciences Corridor) and several large-scale user facilities worldwide
• new faculty hires in both existing and emerging areas (e.g., energy science, heterogeneous catalysis, natural and artificial photosynthesis)
• envisioned to consist of three parts:
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
• serve as a nexus for ultrafast science in the Midwest, eventually coupling with the University of Michigan (a Michigan Ultrafast Sciences Corridor) and several large-scale user facilities worldwide
• new faculty hires in both existing and emerging areas (e.g., energy science, heterogeneous catalysis, natural and artificial photosynthesis)
• envisioned to consist of three parts:
✓ A CORE to serve as a catalyst for interdisciplinary efforts
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
• serve as a nexus for ultrafast science in the Midwest, eventually coupling with the University of Michigan (a Michigan Ultrafast Sciences Corridor) and several large-scale user facilities worldwide
• new faculty hires in both existing and emerging areas (e.g., energy science, heterogeneous catalysis, natural and artificial photosynthesis)
• envisioned to consist of three parts:
✓ A CORE to serve as a catalyst for interdisciplinary efforts
✓ a user facility (staffed by a Ph.D.-level scientist with expertise in ultrafast spectroscopy) to allow researchers across campus to advance their research
A Center for Ultrafast Science• builds on existing strengths at Michigan State University
• serve as a nexus for ultrafast science in the Midwest, eventually coupling with the University of Michigan (a Michigan Ultrafast Sciences Corridor) and several large-scale user facilities worldwide
• new faculty hires in both existing and emerging areas (e.g., energy science, heterogeneous catalysis, natural and artificial photosynthesis)
• envisioned to consist of three parts:
✓ A CORE to serve as a catalyst for interdisciplinary efforts
✓ a user facility (staffed by a Ph.D.-level scientist with expertise in ultrafast spectroscopy) to allow researchers across campus to advance their research
✓ a center for ultrafast source development that will leverage already established expertise (e.g., Dantus and Ruan) and place MSU at the forefront of new developments in ultrafast technology
Acc. Chem. Res. 2003, 36, 876
Ultrafast Dynamics of Transition Metal Complexes
✴ interest in the earliest stages of excited-state evolution in transition metal-containing systems
Acc. Chem. Res. 2003, 36, 876
Ultrafast Dynamics of Transition Metal Complexes
✴ interest in the earliest stages of excited-state evolution in transition metal-containing systems
Nuclear coordinate (Q)
Ener
gy
hν
Excited States
hν'
Acc. Chem. Res. 2003, 36, 876
Ultrafast Dynamics of Transition Metal Complexes
✴ interest in the earliest stages of excited-state evolution in transition metal-containing systems
Nuclear coordinate (Q)
Ener
gy
hν
Excited States
hν'
Acc. Chem. Res. 2003, 36, 876
✴ What is the time scale of excited-state evolution?
Ultrafast Dynamics of Transition Metal Complexes
✴ interest in the earliest stages of excited-state evolution in transition metal-containing systems
Nuclear coordinate (Q)
Ener
gy
hν
Excited States
hν'
Acc. Chem. Res. 2003, 36, 876
✴ What is the time scale of excited-state evolution?
✴ Mechanistic details?
Ultrafast Dynamics of Transition Metal Complexes
✴ interest in the earliest stages of excited-state evolution in transition metal-containing systems
Nuclear coordinate (Q)
Ener
gy
hν
Excited States
hν'
Acc. Chem. Res. 2003, 36, 876
✴ What is the time scale of excited-state evolution?
✴ Mechanistic details?
✴ To what extent do factors such as electronic and/or geometric structure, solvation, etc. play a role?
Ultrafast Dynamics of Transition Metal Complexes
✴ interest in the earliest stages of excited-state evolution in transition metal-containing systems
Nuclear coordinate (Q)
Ener
gy
hν
Excited States
hν'
Acc. Chem. Res. 2003, 36, 876
✴ What is the time scale of excited-state evolution?
✴ Mechanistic details?
✴ To what extent do factors such as electronic and/or geometric structure, solvation, etc. play a role?
✴ Can we control these various factors in such a way as to influence energy redistribution?
Ultrafast Dynamics of Transition Metal Complexes
Acc. Chem. Res. 2003, 36, 876
Ultrafast Dynamics of Transition Metal Complexes
TiO2-Based Photovoltaics: The Grätzel Cell
hν
e-e-
load
e-(R/R-)
e-
O
O
e-
e-
NN
e- injection
Ru
NN
(S+/S)
O
O
(S+/S*)
NCS
NCS
counterelectrodeTiO2 particle
chromophore shiftsenergy required for
photoconductioninto visible
ΔV
TiO2
• introduced by O‘Regan and Gratzel in 1991
• extended previously known concept of semiconductor sensitization
• inexpensive and easy to manufacture
• highest overall conversion efficiency currently reported is ca. 12%
O’Regan, B.; Gratzel, M. Nature 1991, 335, 737
TiO2-Based Photovoltaics: The Grätzel Cell
hν
e-e-
load
e-(R/R-)
e-
O
O
e-
e-
NN
e- injection
Ru
NN
(S+/S)
O
O
(S+/S*)
NCS
NCS
counterelectrodeTiO2 particle
chromophore shiftsenergy required for
photoconductioninto visible
ΔV
TiO2
• introduced by O‘Regan and Gratzel in 1991
• extended previously known concept of semiconductor sensitization
• inexpensive and easy to manufacture
• highest overall conversion efficiency currently reported is ca. 12%
• broad-based utility tied to cost reductions, significant improvements in overall efficiency, and scalability
O’Regan, B.; Gratzel, M. Nature 1991, 335, 737
First-row Sensitizers
LF
CTCT
CB
VB
Ru,Os Fe
LF
• Potential benefits:
substantial reduction in cost (particularly for multi-component cells)
expands palette of possible chromophores
scalable
• Scientific issues:
‣ potential for low-lying excited states to impact injection dynamics
First-row Sensitizers
LF
CTCT
CB
VB
Ru,Os Fe
LF
• Potential benefits:
substantial reduction in cost (particularly for multi-component cells)
expands palette of possible chromophores
scalable
• Scientific issues:
‣ potential for low-lying excited states to impact injection dynamics
First-row Sensitizers
LF
CTCT
CB
VB
Ru,Os Fe
LF
• Potential benefits:
substantial reduction in cost (particularly for multi-component cells)
expands palette of possible chromophores
scalable
• Scientific issues:
‣ potential for low-lying excited states to impact injection dynamics
‣ qualitatively explains low efficiency of Fe-based DSSCs
First-row Sensitizers
LF
CTCT
CB
VB
Ru,Os Fe
LF
• Potential benefits:
substantial reduction in cost (particularly for multi-component cells)
expands palette of possible chromophores
scalable
• Scientific issues:
‣ potential for low-lying excited states to impact injection dynamics
‣ qualitatively explains low efficiency of Fe-based DSSCs
‣ need to elucidate factors controlling ultrafast dynamics
Ultrafast Lasers: A universal light source perspective
Marcos Dantus [email protected]
[email protected] COI Disclosure: Dantus is the Founder and CTO of 1
Ultrafast TED at MSU, October 23, 2015
Why ultrafast lasers?
• Faster than nuclear motion: Femtochemistry, Nobel Prize 1999
• High peak power:
• Broad bandwidth:
Why ultrafast lasers?
• Faster than nuclear motion: Femtochemistry, Nobel Prize 1999
• High peak power:
• Broad bandwidth:
• Ultrahigh resolution metrology: 10-18s, Physics Nobel Prize 2005
• Gateway to attosecond and zeptosecond science
Why ultrafast lasers?
• Faster than nuclear motion: Femtochemistry, Nobel Prize 1999
• High peak power:
• Broad bandwidth:
• Ultrahigh resolution metrology: 10-18s, Physics Nobel Prize 2005
• Gateway to attosecond and zeptosecond science
Defense Medicine Industry Communications Energy
Physics Chemistry Biology
Sensing Measuring Cutting Imaging
Enabling and Transforming
Processing Information/Materials
MIIPS over 20 issued patents
Technology commercialized, over 130 systems worldwide.
MIIPS characterizes and corrects femtosecond pulses
A Breakthrough at MSU
MSU laser
4 fs pulses
Extreme Light Sources U. Michigan: Hercules Ohio State U: Scarle7 U. Nebraska: Diocles UT Aus>n: Texas Petawa7 Laser European Union ELI project Osaka Japan LFEX
Need for spatial and temporal shaping to achieve highest
focused intensities.
Opt. Express 19, 12074 (2011) Fiber laser oscillators capable of genera>ng 35fs pulses
Development of new ultrafast laser sources at MSU
25 um 25 um
100 um 100 um
140 um 140 um
800 nm 1060 nm
800 nm
1060 nm
Sub-40 fs 1060 nm Yb-fiber laser enhances penetration depth in non-linear optical microscopy of human skin
Label-free chemical imaging of cancer with programmable light
Figure S3.2. Epi-detected CARS-3050 cm-1 imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. Water-rich regions and an area of protein granules are revealed. One water-rich area (delineated by blue solid line) indicates a region of dense collagen (see Fig. S3.5), while another marked area (delineated by green broken line) reveals several FAD-rich microparticles (see Fig. S3.4).
Figure S3.3. Epi-detected CARS-2850 cm-1 imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. The unconfirmed nerve and blood cells resemble those reported nerve (Fig. 2A in Ref. 12) and blood cells (Fig. 11f in Ref. 13). A marked lipid-poor area (delineated by solid line) indicates a region of dense collagen (see Fig. S3.5), while another marked area (delineated by broken line) reveals several FAD-rich microparticles (see Fig. S3.4).
Figure S3.4. Epi-detected i2PF imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. The image reveals a region of thin elastin fibers, 2 interstitial cells among adipocytes (see Fig. 3.3 for positive contrast of adipocytes), 5 cells on adipocyte boundaries, 5 free cells in various stromal regions, 2 tumor cells on a tumor boundary (confirmed by bright-field imaging), and several FAD-rich microparticles inside the corresponding solid tumor. A marked area of no obvious structure (delineated by red solid line) indicates a region of dense collagen (see Fig. S3.5). A natural question arises whether the visible elongated features are of the same origin, which can be answered by the dual-modal i2PF/i3PF image analysis (see Fig. S3.10).
Figure S3.5. Epi-detected SHG imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. One marked area (delineated by red solid line) indicates a region of dense collagen, while another area forms a collagen fiber tube. A natural question arises why collagen forms a tube structure, which can be answered by the dual-modal SHG/i3PF image analysis (see Fig. S3.11). Another question arises why collagen forms a large-scale strand-like structure, which can be answered by the tri-modality CARS-2850 cm-1/SHG/THG image analysis (see Fig. S3.14).
Figure S3.6. Epi-detected i3PF imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. Lipid microparticles and adipocytes in CARS imaging (see Fig. S3.3) also show up. One marked area (delineated by broken yellow line) reveals several FAD-rich microparticles (see Fig. S3.4). Other areas with scattered fluorescent microparticles (delineated by solid orange lines) are described in the THG image (see Fig. S3.7). A natural question arises why most of the fluorescent microparticles are distributed in tubular formations rather than the random formations of the marked areas (yellow rectangles), which can be answered by the dual-modal i3PF/CARS-2850 cm-1 image analysis (see Fig. S3.9).
Figure S3.14. Epi-detected tri-mode SHG/THG/CARS-2850cm-1 imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. Collagen attains the large-scale strand-like structure in Fig. S3.5 to enclose and protect the confirmed nerve.
Temporal dephasing from individual nanoparticles
Figure S3.14. Epi-detected tri-mode SHG/THG/CARS-2850cm-1 imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. Collagen attains the large-scale strand-like structure in Fig. S3.5 to enclose and protect the confirmed nerve.
Current Collabora4ons Manooch Koochesfahani (MSU, Engineering, Fluid dynamics) Benjamin Levine (MSU, ab ini4o and MD simula4ons) Ned Jackson (MSU, organic chemistry) Gavin Reid (MSU, Chemistry, Proteomics) Chong-‐Yu Ruan (MSU, ultrafast electron diffrac4on) Warren Beck (MSU, Mul4dimensional Microscopy) Arnoczky, Steven (MSU, Chair of Vet. Surgery) Shaul Mukamel (UC Irvine, NLO pathway assignment) Bruce Tromberg (UC Irvine, Beckman Laser Ins4tute) Sunney Xie (Harvard, SRS microscopy) Conor Evans (Harvard, Biomedical imaging) Frank Wise (Cornell, fiber laser design) Stephen Boppart (UIUC, femtosecond endoscopy) Jim Gord (Air Force Research Lab, CARS) Sukesh Roy (Spectral Engines LLC, CARS, Machining)
Addi4onal collabora4ons through Biophotonic Solu4ons Inc.
(a) Next generation biomedical/plant imaging (b) Next generation laser sources
• Time Resolved Broadband XAFS Element sensitivity for materials research
• Ultra-short and Ultra-intense in Vis and Mid-IR Gateway for relativistic optics Gateway for attosencond and zeptosecond pulse generation
Ultrafast Science, Sources and Applications Next Sources and Grand Challenges
3 cm
Material Imaging at Space-Time Limit
Based on SPG/NSF-MRI/DOE seed (2009-2015)
Chong-Yu Ruan, Department of Physics & Astronomy
High-brightness ultrafast electron microscope (UEM) technology
Key areas: Photonics RF accelerator technology Beam dynamics Laser-RF synchronization Laser pulse shaping Material science Photocathods Electron microscopy
MSU has the foundation for the key technologies to be combined and developing a mature UEM system
New Frontiers in Science Enabled by fs-EM
High-Tc superconductor
Key areas
Laser machining
Water splitting
Photo-catalysis
Nano-electronics
Photo-voltaics
Protein-folding
Current Capabilities and Development
Photochemistry Material science/ Nano-electronics
Biological science Nanoscience
Advanced capabilities at MSU • Femtosecond high-brightness electron probe • Ultrafast electron diffractive imaging • Ultrafast electron microdiffraction
Already demonstrated as a proof of principle in areas of .. (* work implemented at MSU)
* Nano letters 7, 1290 (2007) * Phys. Rev. Lett. 101, 077401 (2008)
Science 291, 458 (2001) Proc. Natl. Aca. Sci. 98, 7117 (2001) Phys. Rev. Lett. 109, 133202 (2012)
* Phys Rev Lett 109, 166406 (2012) Science 318, 788 (2007) Science 304, 80 (2004)
Quantum physics
UEM
UED
*Science Advances 1, e1400173 (2015)
Before
After
VO2 20 nm
Charge density waves Interfacial water
Next-generation instruments at MSU Combining imaging and spectroscopy with high sensitivity
•300 fs to 3 ps; 0.3 eV to 0.05 eV •Core level spectroscopy, near-edge EELS •Element sensitivity •Imaging 3D electronic structures
Ultrafast electron microdiffraction (Current beamline, Upgrade optics and environment control) •300 fs high-brightness beam; e dose > 10 e/um2
•Coherence length > 30 nm •Spatial resolution < 0.1 angstrom
Substituting ultrafast ARPES Complementary to ultrafast XAS
(Develop new spectrometer)
Ultrafast angle-resolved ultrafast electron spectroscopy
Ultrafast electron imaging and spectroscopy technology can play a part in broader MSU’s efforts for center and facility development
Collaboration leads to new opportunities!
C H E M I C A L B I O D Y N A M I C SU LT R A FA S T B I O L O G Y
Warren F. BeckDepartment of Chemistry
U LT R A FA S T B I O L O G Y H O W B I O L O G I C A L M O L E C U L E S W O R K
• Structures:Intermediates and Mechanisms
• Dynamics:Motion and Relaxation
• Energy: Conversion and Storage
• Information: Coherence and Correlation
U LT R A FA S T B I O L O G Y C H A R A C T E R I S T I C T I M E S C A L E S
• Vibrations: 10 fs–1ps
• Energy Transfer: 50 fs–100 ps
• Electron Transfer: ps–μs
• Protein Folding: μs−s
U LT R A FA S T B I O L O G Y C U T T I N G E D G E M E T H O D S
• Two-Dimensional Spectroscopies
• 2DES: Electronic
• 2DIR: Infrared
• 2DEV: Electronic–Vibrational
• Femtosecond X-ray Diffraction
Theory of Ultrafast Processes: Dissecting ComplexityBenjamin G. Levine
Department of Chemistry
Through Theory We Directly Model Complex Molecular Motions• Even modestly sized molecules are
composed of dozens or hundreds of particles which may react to light
• Ultrafast experiments provide time-resolved information in low dimension
The Three Big Questions
MSU has a strong footprint in all three areas (Chemistry: Cukier, Hunt, Levine, Merz, Piecuch, Wilson; Biochemistry: Dickson, Feig; Physics: Duxbury, Tomanek;
Engineering: Yue Qi; Math: Christlieb, Hirn, Liu, Promislow)
Electronic Structure: What
are the electrons doing?
Molecular Dynamics: How
do the nuclei move?
Nonadiabatic Dynamics: How do nuclear and
electronic motions influence
one another?
More Complex Experiments Need More Complex Theories• Complex materials and
biological macromolecules Multiscale modeling Quantum molecular dynamics in
complex environments High performance computing
• Shorter, stronger laser pulses Real-time electron dynamics Non-linear and relativistic effects
Ultrafast Physical processes
- Beam simulations for ultrafast electron microscopes
- Photo-induced phase transitions
- Simulation of swift heavy ion effects on materials
Three nuggets
Four grand challenges in ultrafast science that are interesting targets for MSU/physics
Creation of fs Electron pulse with millions of electrons:
Accelerator physics with intense beams
Experiment
Photo-induced phase transitions (PIPT) in TaS2, VO2 etc.
CCDW
NCCDW
ICCDW
VO2 : Tao et al. Phys. Rev. Letts. 109, 166406 (2012)
TaS2 : Han et al. Science Advances, June 26th (2015).
Non-adiabatic response
Keldysh contour • Single-particle Green’s
function along the Kadanoff-Baym-Keldyshcontour is defined as:
Calculating NEQ electron dynamics
Response of materials to radiation e.g. a single swift heavy ion passing through a material (FRIB)
J. Zhang et al. J. Mater. Res. 25, 1344 (2010)
Materials for FRIB- Titanium- Graphite- Diamond
Electron scatteringNuclear scatteringNuclear reactionsAt high ion energymost of the energy transferred to electrons
Ultrafast grand challenges• Design and build a functional transmission electron
microscope with ns to fs time resolution and micron to Angstrom spatial resolution (Ruan)
• Computationally solve the NEQ quantum dynamics of nuclei and electrons simultaneously, in complex materials and molecules (Levine, McCusker, Tomanek).
• Control photo-induced phase transitions and molecular switching at ultrafast timescales (Ruan, Dantus, McCusker).
• Develop ultrafast tabletop sources of x-rays, electrons and ions. (i) Sources to generate one particle at a time on demand at fs time resolution. (ii) Ultrafast, high intensity, low emittance, broadband sources. (Dantus, FRIB team)
MSU
MSUU of M
MSUU of M
MSUU of M
APS at ANL
MSUU of M
APS at ANL
MSUU of M
APS at ANL
LCLS at SLAC
MSUU of M
APS at ANL
LCLS at SLAC