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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)
Energy
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)
Energy
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)
Energy
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)
Energy
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)
Energy
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-
N
N
e- injection
Ru
N
N
(S+/S)
O
O
(S+/S*)
NCS
NCS
counterelectrodeTiO2 particle
chromophore shifts
energy required for
photoconduction
into 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-
N
N
e- injection
Ru
N
N
(S+/S)
O
O
(S+/S*)
NCS
NCS
counterelectrodeTiO2 particle
chromophore shifts
energy required for
photoconduction
into 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
dantus@msu.edu
dantus@msu.eduCOI 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 CommunicationsEnergy
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
Figure S3.6. Epi-detected i3PF imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat.
Figure S3.14. Epi-detected tri-mode SHG/THG/CARS-2850cm-1
imaging of unstained rat mammary tumor from a 15-
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
PhotochemistryMaterial science/
Nano-electronics
Biological scienceNanoscience
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 S
U LT R A FA S T B I O L O G Y
Warren F. Beck

Department 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
Complexity
Benjamin 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-Keldysh
contour 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 scattering
Nuclear scattering
Nuclear reactions
At high ion energy
most 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
MSU
U of M
MSU
U of M
MSU
U of M
APS at ANL
MSU
U of M
APS at ANL
MSU
U of M
APS at ANL
LCLS at SLAC
MSU
U of M
APS at ANL
LCLS at SLAC

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Center of Reserach Excellence in Ultrafast Science

  • 1. Center of Research Excellence in Ultrafast Science: ! Building on Strength at MSU
  • 2.
  • 3.
  • 4. • initiated in 2009 by Professor Phil Duxbury
  • 5. • initiated in 2009 by Professor Phil Duxbury • initial commitment of 5 years at $500,000/year
  • 6. • 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
  • 7. • 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
  • 8. • 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
  • 9. • 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)
  • 10. • 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
  • 11. In-house Excellence in Ultrafast Science
  • 12. • seminar program in Spring 2014 highlighted the unique strength MSU currently has in ultrafast science In-house Excellence in Ultrafast Science
  • 13. • 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
  • 14. • 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
  • 15. • 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
  • 17. Grand Challenges • Grand Challenges identified by the Office of Science at DOE (above) and the White House office of Science and Policy (left)
  • 18. Grand Challenges • Grand Challenges identified by the Office of Science at DOE (above) and the White House office of Science and Policy (left)
  • 19. 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
  • 20. A Center for Ultrafast Science
  • 21. A Center for Ultrafast Science • builds on existing strengths at Michigan State University
  • 22. 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
  • 23. 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)
  • 24. 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:
  • 25. 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
  • 26. 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
  • 27. 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
  • 28. Acc. Chem. Res. 2003, 36, 876 Ultrafast Dynamics of Transition Metal Complexes
  • 29. ✴ 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
  • 30. ✴ interest in the earliest stages of excited-state evolution in transition metal- containing systems Nuclear coordinate (Q) Energy hν Excited States hν' Acc. Chem. Res. 2003, 36, 876 Ultrafast Dynamics of Transition Metal Complexes
  • 31. ✴ interest in the earliest stages of excited-state evolution in transition metal- containing systems Nuclear coordinate (Q) Energy 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
  • 32. ✴ interest in the earliest stages of excited-state evolution in transition metal- containing systems Nuclear coordinate (Q) Energy 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
  • 33. ✴ interest in the earliest stages of excited-state evolution in transition metal- containing systems Nuclear coordinate (Q) Energy 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
  • 34. ✴ interest in the earliest stages of excited-state evolution in transition metal- containing systems Nuclear coordinate (Q) Energy 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
  • 35. Acc. Chem. Res. 2003, 36, 876 Ultrafast Dynamics of Transition Metal Complexes
  • 36. TiO2-Based Photovoltaics:The Grätzel Cell hν e-e- load e- (R/R-) e- O O e- e- N N e- injection Ru N N (S+/S) O O (S+/S*) NCS NCS counterelectrodeTiO2 particle chromophore shifts energy required for photoconduction into 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
  • 37. TiO2-Based Photovoltaics:The Grätzel Cell hν e-e- load e- (R/R-) e- O O e- e- N N e- injection Ru N N (S+/S) O O (S+/S*) NCS NCS counterelectrodeTiO2 particle chromophore shifts energy required for photoconduction into 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
  • 38. 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
  • 39. 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
  • 40. 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
  • 41. 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
  • 42. Ultrafast Lasers: A universal light source perspective Marcos Dantus dantus@msu.edu dantus@msu.eduCOI Disclosure: Dantus is the Founder and CTO of 1   Ultrafast TED at MSU, October 23, 2015
  • 43. Why ultrafast lasers? •  Faster than nuclear motion: Femtochemistry, Nobel Prize 1999 •  High peak power: •  Broad bandwidth:
  • 44. 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
  • 45. 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 CommunicationsEnergy Physics Chemistry Biology Sensing Measuring Cutting Imaging Enabling and Transforming Processing Information/Materials
  • 46. 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
  • 47. 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.
  • 48. Opt.  Express    19,  12074  (2011)   Fiber  laser  oscillators  capable  of  genera>ng  35fs  pulses   Development of new ultrafast laser sources at MSU
  • 49. 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
  • 50. 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 Figure S3.6. Epi-detected i3PF imaging of unstained rat mammary tumor from a 15-week-old carcinogen-injected rat. Figure S3.14. Epi-detected tri-mode SHG/THG/CARS-2850cm-1 imaging of unstained rat mammary tumor from a 15-
  • 51. Temporal dephasing from individual nanoparticles
  • 52. 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.  
  • 53. (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
  • 54. Material Imaging at Space-Time Limit Based on SPG/NSF-MRI/DOE seed (2009-2015) Chong-Yu Ruan, Department of Physics & Astronomy
  • 55. 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
  • 56. 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
  • 57. Current Capabilities and Development PhotochemistryMaterial science/ Nano-electronics Biological scienceNanoscience 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
  • 58. 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
  • 59. 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!
  • 60. C H E M I C A L B I O D Y N A M I C S U LT R A FA S T B I O L O G Y Warren F. Beck
 Department of Chemistry
  • 61. 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
  • 62. 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
  • 63. 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
  • 64. Theory of Ultrafast Processes: Dissecting Complexity Benjamin G. Levine Department of Chemistry
  • 65. 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
  • 66. 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?
  • 67. 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
  • 68. 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
  • 69. Creation of fs Electron pulse with millions of electrons: Accelerator physics with intense beams Experiment
  • 70. 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
  • 71. Keldysh contour • Single-particle Green’s function along the Kadanoff-Baym-Keldysh contour is defined as: Calculating NEQ electron dynamics
  • 72. 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 scattering Nuclear scattering Nuclear reactions At high ion energy most of the energy transferred to electrons
  • 73. 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)
  • 74.
  • 75. MSU
  • 78. MSU U of M APS at ANL
  • 79. MSU U of M APS at ANL
  • 80. MSU U of M APS at ANL LCLS at SLAC
  • 81. MSU U of M APS at ANL LCLS at SLAC