Department of Physics and Astronomy

Support: Georgia State University

Atlanta, GA 30303-3083, USA
US Israel
Binational Science
Foundation
German Science Foundation (DFG) through
the Cluster of Excellence Munich Center for
Advanced Photonics; EU reintegration
grant and the DFG Emmy-Noether program.

Nanoplasmonics from Attoseconds

‡ to Terahertz
Mark Stockman
Department of Physics and Astronomy,
Georgia State University, Atlanta, GA 30302, USA

FRISNO-10 (French-Israeli Symposium on

Web: http://www.phy-astr.gsu.edu/stockman Tuesday, February 10,
Nonlinear and Quantum Optics),
E-mail: mstockman@gsu.edu 2009 11:20-11:50 am, p.1
Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

CONTENTS
•Brief Introduction
•SPASER
•Attosecond Nanoplasmonic Field Microscope
•Time-Reversal Coherent Control of Nanoplasmonic
Systems
•Adiabatic Nanoconcentration of THz Radiation

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
MIS’s Collaborators:
•David J. Bergman, Department of Physics, Tel Aviv University, Israel
•Sophie Brasselet, Institut Fresnel, Marseilles, France
•Maxim Durach, Georgia State University, Atlanta, GA 30340, USA
•Anastasia Rusina, Georgia State University, Atlanta, GA 30340, USA
•Sergey V. Faleev, Sandia National Laboratories, Livermore, CA, USA
•Takayoshi Kobayashi, University of Tokyo, Japan
•Victor Klimov, Los Alamos National Laboratory, Los Alamos, New Mexico, USA
•Ferenc Krausz, Max Plank Institute for Quantum Optics, Garching, Germany
•Ulf Kleineberg, Ludwig Maximilian University, Munich, Germany
•Matthias Kling, Max Plank Institute for Quantum Optics, Garching, Germany
•Kuiru Li, Georgia State University, Atlanta, GA 30340, USA
•Ivan Larkin, Georgia State University, Atlanta, GA 30340, USA
•Keith Nelson, MIT, Boston, USA
•Hrvoje Petek, University of Pittsburgh, USA
•Peter Nordlander, Rice University, Houston, Texas, USA
•Misha Ivanov, Femtosecond Science Program, National Research Council of Canada
•Paul Corkum, Femtosecond Science Program, National Research Council of Canada
•Nikolay Zheludev, University of Southampton, UK
•Igor Tsukerman, University of Akron, OH 44325, USA
•Joseph Zyss, Ecole Normale Supérieure de Cachan, 94235 Cachan, France
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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

FRISNO-10 (French-Israeli Symposium on

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Nonlinear and Quantum Optics),
TheIsrael
Ein Gedi, most beautiful nanoplasmonicE-mail:colors of the world: La Sainte2009
mstockman@gsu.edu Chapelle, Paris
11:20-11:50 am, p.4
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

REUBEN ASHER DAN

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Applications of Nanoplasmonics:
• Ultrasensitive and express sensing and detection; NSOMs
• Coupling of light to semiconductor devices: extraction of light from
LEDs and nanostructured antennas for photodetectors and solar cells
• Photo- and chemically stable labels and probes for biomedical
research and medicine
• Nanoplasmonic-based immunoassays; home pregnancy test (in mass
production); heart attack test (in clinical trials) and HIV test.
• Near perspective: Generation of EUV and XUV pulses
• Thermal cancer therapy (stage 3 clinical trials):
L. R. Hirsch, R. J. Stafford, J. A. Bankson, S. R. Sershen, B. Rivera, R. E. Price, J. D.
Hazle, N. J. Halas, and J. L. West, Nanoshell-Mediated Near-Infrared Thermal
Therapy of Tumors under Magnetic Resonance Guidance, Proc. Natl. Acad. Sci. USA
100, 13549-13554 (2003).
C. Loo, A. Lowery, N. Halas, J. West, and R. Drezek, Immunotargeted Nanoshells for
Integrated Cancer Imaging and Therapy, Nano Lett. 5, 709-711 (2005).
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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

Nanoplasmonics is intrinsically ultrafast:

Spectrally, surface
plasmon resonances in
n (fs) complex systems occupy
Best area for a very wide frequency
plasmonics band
Δω ≈ ω p 2 ≈ 3.5 eV
Corresponding rise
time of plasmonic
n (eV)
responses ~ 100 as

Surface plasmon relaxation times are in

~10-100 fs range
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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

Quantum Nanoplasmonics: Surface

Plasmon Amplification by Stimulated
Emission of Radiation (SPASER)
D. J. Bergman and M. I. Stockman, Surface Plasmon
Amplification by Stimulated Emission of Radiation: Quantum
Generation of Coherent Surface Plasmons in Nanosystems,
Phys. Rev. Lett. 90, 027402-1-4 (2003).

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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 D. J. Bergman and M. I. Stockman, Surface Plasmon Amplification by
Department
Stimulated ofofPhysics
Emission andQuantum
Radiation: Astronomy
Generation of Coherent Surface
Georgia State University
Plasmons in Nanosystems,
Atlanta, Phys. Rev.
GA 30303-3083, USALett. 90, 027402-1-4 (2003).

Avalanche of surface plasmon

stimulated emission will
develop within an ultrashort
time of
τ
~ 5 fs
αn
This dimensionless gain
shows how many times the
Calculated gain for thin (three net rate of SP emission
monolayers of quantum dots) exceeds the rate of their
active medium decay due to dissipation

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 D. J. Bergman and M. I. Stockman, Surface Plasmon Amplification by
Department
Stimulated ofofPhysics
Emission andQuantum
Radiation: Astronomy
Generation of Coherent Surface
Georgia State University
Plasmons in Nanosystems,
Atlanta, Phys. Rev.
GA 30303-3083, USALett. 90, 027402-1-4 (2003).

Eigenmodes with highest yields for the spectral maximum at 1.2 eV

=ω = 1.15 eV =ω = 1.18 eV
—wn=1.15 eV —wn=1.18 eV
αann=12., 5 ×103−3
= 12, f nfn==5.E- α = 11, ffn n==3.E-
a nn=11.,
−12
3 ×1012
Luminous eigenmode Dark eigenmode

5.E7 7.E7
E
EH0L
⎛ VVn ⎞
H0L
En E
⎛HVV ⎞ ⎜H €€€€⎟L
⎜ m€€L⎟
€€
⎝ mm ⎠
⎝ m ⎠ 30 30
x z x z
30 30
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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Strong pumping
NSP
100

Above the threshold 50

NSP =ω (eV)

20 1.1 1.2 1.3

Pumping at the threshold =ω (eV)

NSP
20 1.1 1.2 1.3

=ω (eV)
1.1 1.2 1.3

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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 M.A. Noginov et al., Observation of Spaser, NanoMeta 2009 Conference, Seefeld,
Department of Physics and Astronomy
Austria Georgia State University
Atlanta, GA 30303-3083, USA

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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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 Department of Physics and Astronomy
Support: Georgia State University
Atlanta, GA 30303-3083, USA

Nature Photonics 1, 539-544 (2007)

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Schematic of Attosecond
PEEM Electron Nanoplasmonic Field
Optics Imaging
Microscope
with Energy
Resolution XUV-emitted
photoelectrons
are accelerated
by enhanced IR
nanoplasmonic
local fields

With respect to XUV pulses, metal

nanosystem is non-resonant.
An XUV pulse excites all parts of
the nanosystem non-selectively
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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

Energy of the Fermi-edge

photoelectron is (~100±10)
eV. The local potential of
the instantaneous plasmonic
fields at the instant of the
attosecond pulse arrival
adds to the kinetic energy
of electrons, acting as a
local electrostatic (van de
Graaf) accelerator. This
provides direct access to
the nanoplasmonic local
field magnitude at any
given instance
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 z

Department of Physics and Astronomy 60

Georgia State University
Atlanta, GA 30303-3083, USA
40

1. Excitation field 20

0 x
t (fs) 0 20 40 60

0. ttX==
Plasmonic 14 fs fspotential
64.13
surface
100 200 (V) at the maximum
10

−1. Local optical electric field

5
0ϕ
20 at the “hottest spot” in (nm) −5
time 60 −10
t (fs) 40
0 z
60
20
100 200 40
20 x (nm)
−FRISNO-10
20 (French-Israeli Symposium Attosecond pulse
applied within
on a period
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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Energy shift (eV) of electrons emitted by a 95 eV XUV attosecond
pulse as a function of the as pulse excitation instant with respect to
the infrared excitation field (frames are in 200 as) as observed in
Photoemission Electron Microscope (PEEM).
Experiment directly measures potential of nanoplasmonic
oscillations with nm spatial and ~100 as temporal resolution
z
Energy change (eV)
60
of 90 eV XUV
40
photoelectrons from
silver nanosystem for
20 10 GW/cm2 800 nm
IR power; × 1015
0 x slowed down
0 20 40 60
Nanosystem is 60x60 nm random silver film (50% filling factor)
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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

CONCLUSIONS
• Nanoplasmonics is intrinsically ultrafast with ~10-50 fs relaxation times and
~100 as coherent dynamics times
• We have proposed attosecond nanoplasmonic field microscope to study
spatiotemporal dynamics of local optical fields in nanosystems with a
nanometer-scale spatial resolution and ~100 attosecond temporal resolution
• This method is based on the use of attosecond XUV pulses produced from
and synchronized with waveform-stabilized optical pulses. The electrons
produced by the XUV pulses are imaged in energy-resolving PEEM
• This is a direct method of measurements in the real space/real time domain,
which is non-invasive (non-perturbing). It provides the maximum
information of the nanometer-femtosecond dynamics of the nanoplasmonic
local fields

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Coherent Control by Shaped Pulses
Different spectral components of
the excitation pulse excite
resonant surface plasmon modes.
These excitations dynamically
interfere creating time-dependent
hot spots of local fields during
their coherence time
This interference can be directed
by choosing phases and
amplitudes of the different
frequency components of the
excitation pulse (pulse shaping)
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 Principles
Department of Physicsof coherent
and Astronomy(quantum) control
Georgia State University
D. J. Tannor andAtlanta,
S. A. Rice,
GA Control of Selectivity
30303-3083, USAof Chemical Reaction Via Control of Wave Packet
Evolution, The Journal of Chemical Physics 83, 5013-5018 (1985); P. Brumer and M. Shapiro, Principles of
the Quantum Control of Molecular Processes (Wiley, New York, 2003); R. S. Judson and H. Rabitz,
Teaching Lasers to Control Molecules, Phys. Rev. Lett. 68, 1500 (1992).
REFERENCES ON COHERENT CONTROL OF OPTICAL ENERGY
NANOLOCALIZATION
•M. I. Stockman, S. V. Faleev, and D. J. Bergman, Coherent Control of Femtosecond Energy
Localization in Nanosystems, Phys. Rev. Lett. 88, 67402-1-4 (2002).
•M. I. Stockman, D. J. Bergman, and T. Kobayashi, Coherent Control of Nanoscale Localization of
Ultrafast Optical Excitation in Nanosystems, Phys. Rev. B 69, 054202-10 (2004)
•A. Kubo, K. Onda, H. Petek, Z. Sun, Y. S. Jung, and H. K. Kim, Femtosecond Imaging of Surface
Plasmon Dynamics in a Nanostructured Silver Film, Nano Lett. 5, 1123-1127 (2005)
•M. I. Stockman and P. Hewageegana, Nanolocalized Nonlinear Electron Photoemission under
Coherent Control, Nano Lett. 5, 2325-2329 (2005)
•M. Aeschlimann, M. Bauer, D. Bayer, T. Brixner, F. J. G. d. Abajo, W. Pfeiffer, M. Rohmer, C.
Spindler, and F. Steeb, Adaptive Subwavelength Control of Nano-Optical Fields, Nature 446, 301-304
(2007).
•X. Li and M. I. Stockman, Highly Efficient Spatiotemporal Coherent Control in Nanoplasmonics on a
Nanometer-Femtosecond Scale by Time Reversal, Phys. Rev. B 77, 195109-1-10 (2008).
FRISNO-10 (French-Israeli Symposium on
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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
A. Kubo, K. Onda, H. Petek, Z. Sun, Y. S. Jung, and H. K. Kim,
Femtosecond Imaging of Surface Plasmon Dynamics in a
Nanostructured Silver Film, Nano Lett. 5, 1123-1127 (2005).
Delay
1
200 nm
0.5

-100 -50 50 100 150 200

-0.5

-1

Experiment: Distribution
of the two-photon electron
emission from rough silver
surface. Frames are taken
by electron microscopy
with 200 as periodicity in
delay
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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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Ein Gedi, Israel
Nanoplasmonic Energy
Department Localization,
of Physics Time Reversal, and Coherent
and Astronomy
Control Georgia State University
Atlanta, GA 30303-3083, USA
X. Li and M. I. Stockman, Highly efficient spatiotemporal coherent
control in nanoplasmonics on a nanometer-femtosecond scale by time
reversal, Phys. Rev. B 77, 195109 (2008); arXiv:0705.0553
Idea of time reversal for
subwavelength EM-wave
localization:
G. Lerosey, J. de Rosny, A. Tourin, and M.
Fink, Focusing Beyond the Diffraction
Limit with Far-Field Time Reversal,
Science 315, 1120-1122 (2007).
A. Derode, A. Tourin, J. de Rosny, M.
Tanter, S. Yon, and M. Fink, Taking
Advantage of Multiple Scattering to
Communicate with Time-Reversal
Antennas, Phys. Rev. Lett. 90, 014301
(2003).

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Ein Gedi, Israel
 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Time-averaged two-photon excitation Time-dependent local field intensity at the target points

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

M. I. Stockman,
Nanofocusing of Optical
Energy in Tapered Plasmonic
Waveguides, Phys. Rev. Lett.
93, 137404-1-4 (2004).
FRISNO-10 (French-Israeli Symposium on
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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
E. Verhagen, A. Polman, and L.
Kuipers, Nanofocusing in Laterally
Tapered Plasmonic Waveguides, Opt.
Express 16, 45-57 (2008)

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Nano Lett. 7, 2784-
2788 (2007).

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 Department of Physics and Astronomy
DOI 10.1021/nl801112e
Georgia State University
Atlanta, GA 30303-3083, USA

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Adiabatic Compression of THz Radiation in 2d Using TEM Modes
in Coaxial Geometry

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Adiabatic concentration:
Fields at 1 THz for conical
silver coax

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA
Adiabatic
concentration:
Fields at 1 THz for
adiabatically tapered
silver coax

δ ≈ const

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 Department of Physics and Astronomy
Georgia State University
Atlanta, GA 30303-3083, USA

THE END
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