NIRT: Full SpatioTemporal Coherent Control on Nanoscale

1
Full Spatio-Temporal Coherent Control on
Nanoscale (NSF NIRT Grant CHE-0507147) Mark
Stockman1, Keith Nelson2, and Hrvoje
Petek3 1Department of Physics and Astronomy,
Georgia State University 2Department of
Chemistry, MIT 3Department of Physics and
Astronomy, University of Pittsburgh
Nanoconcentration of Terahertz Radiation in
Plasmonic Waveguides
Nanoplasmonic Renormalization of Coulomb
Interactions
Motivation and Goals
Optical processes on the nanoscale are of great
importance both fundamentally and for
applications in science, engineering, technology,
and defense. Among the fundamental problems of
the nanoscale optics and nanoplasmonics is
delivery of the optical fields to the nanoscale
and their control with nanoscale precision. The
conventional methods with tapered optical fibers
and sharp metal tips can produce high enough
enhancements of the local optical field by the
price of a very efficiency of the energy
transfer. A goal of this project is to find much
more efficient ways to transfer energy to the
nanoscale using tapered nanoplasmonic structures.
The concentration of the optical energy in the
nanoplasmonic structures is coherently controlled
using spatio-temporal pulse shapers.
Near a metal nanoparticle carriers exchange a
surface plasmon quantum, which can be represented
as a modification of Coulomb interaction between
carriers. We obtain renormalized interaction near
an arbitrary metal nanostructure
We establish the principal limits for the
nanoconcentration of the THz radiation in
metal/dielectric waveguides and determine their
optimum shapes required for this
nanoconcentration. We predict that the adiabatic
compression of THz radiation from the initial
spot size of R0?0 to the final size of R 100-
250 nm can be achieved, while the THz radiation
intensity is increased by a factor of 10 to
250.
Interaction near Metal-Dielectric Nanoshell
Terahertz wave in dielectric slab covered with
metal
Thick slab
Thin slab
Control of surface plasmons with phase-correlated
femtosecond light fields
Properties of Plasmonic-Renormalized Interaction
(ii) It is highly resonant. Near resonance
s(?)sn, W is increased by quality factor Q
(i) It is long-ranged
Eigenmodes are composed of hot spots separated
by distances on the scale of the entire plasmonic
nanostructure
The physical process that limits the extent of
spatial concentration is the skin effect, i.e.,
penetration of the radiation into the metal that
causes the losses the THz field penetrates the
depth of ls 30-60 nm of the metal, which
determines the ultimum localization radius.
PEEM Imaging of Surface Plasmon Polaritons
Q100-150 innear-IR for silver
Simulation
Experiment
(iii) It affects a wide range of many-body
phenomena near metal nanostructures (a)
scattering between charge carriers, the carriers
and ions, (b) ion-ion interactions, (c) exciton
formation (d) chemical reactions and catalysis
Interferometric time-resolved photoemission
electron microscopy ITR-PEEM image 10-fs,
single pulse
Adiabatic Concentration of Terahertz Energy in
Graded Waveguides
Spectroscopic Microscopy by means of
Time-of-flight-PEEM
Plasmonic-Renormalized Energy Transfer
Förster rate near metal nanostructure
Dyadic Greens function
J is spectral overlap integral
Time-of-flight PEEM Dx70 nm, DE100 meV
Energy Transfer near Metal-Dielectric Nanoshells
Control of SPPs in nano-optics is available by
using phase-correlated fs-optical pulses.
(1) FRET across nanoshell
Fields in tapered silver wedge cavity, 1 THz
Fields in tapered silver coaxial cable, 1 THz
?F
Adiabatic Nanoconcentration of Terahertz Energy
in Funnel Waveguides
The SPP and light interferes on the screen
To provide for the optimum guiding of the THz
wave and its concentration on the nanoscale, the
terminating (nanoscopic) part of the waveguide
should be tapered in a funnel-like manner.
Light SPP Coupling
Off-centered focusing of SPP by Circular-arc
lenses
(2) FRET averaged over acceptor position
Interference control
d
?F
?m
?r
(4) Radiation
Competing processes
(3) Energy transfer to the metal
Although near thick nanoshells FRET quantum
efficiency is small, FRET in the vicinity of the
nanoshells with high aspect ratios has quantum
efficiency around 50
Fields in curved silver wedge cavity, 1 THz
Fields in curved silver coaxial cable, 1 THz

• M. I. Stockman, in Plasmonic  Nanoguides and
  Circuits, edited by S. I. Bozhevolny, Adiabatic
  Concentration and Coherent Control in
  Nanoplasmonic Waveguides (World Scientific
  Publishing, Singapore, 2008).
• M. I. Stockman, Attosecond Physics - an Easier
  Route to High Harmony, Nature 453, 731-733
  (2008).
• M. I. Stockman, Spasers Explained, Nature
  Photonics 2, 327-329 (2008).
• M. I. Stockman, Ultrafast Nanoplasmonics under
  Coherent Control, New J. Phys. 10 025031-1-20
  (2008).
• A. Rusina, M. Durach, K. A. Nelson, and M. I.
  Stockman, Nanoconcentration of Terahertz
  Radiation in Plasmonic Waveguides, Opt. Expr. 16,
  18576-18589 (2008).
• K. F. MacDonald, Z. L. Samson, M. I. Stockman,
  and N. I. Zheludev, Ultrafast Active Plasmonics
  Transmission and Control of Femtosecond Plasmon
  Signals, arXiv0807.2542 (2008).
• 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).
• D. K. Gramotnev, M. W. Vogel, and M. I.
  Stockman, Optimized Nonadiabatic Nanofocusing of
  Plasmons by Tapered Metal Rods, J. Appl. Phys.
  104, 034311-1-8 (2008).

• M. Durach, A. Rusina, V. I. Klimov, and M. I.
  Stockman, Nanoplasmonic Renormalization and
  Enhancement of Coulomb Interactions, New J. Phys.
  10, 105011-1-14 (2008).
• J. Dai, F. Cajko, I. Tsukerman, and M. I.
  Stockman, Electrodynamic Effects in Plasmonic
  Nanolenses, Phys. Rev. B 77, 115419-1-5 (2008).
• M. I. Stockman, M. F. Kling, U. Kleineberg, and
  F. Krausz, Attosecond Nanoplasmonic Field
  Microscope, Nature Photonics 1, 539-544 (2007).
• A. Kubo and H. Petek, Femtosecond Time-resolved
  Photoemission Electron Microscope Studies of
  Surface Plasmon Dynamics, J. Vac. Soc. Jap. 51,
  368 (2008) (in Japanese).
• H. Petek and A. Kubo, Ultrafast photoemission
  electron microscopy imaging light with electrons
  on the femto-nano scale, in Ultrafast Phenomena
  XVI. E. Riedle and R. Schoenlein,
  Springer-Verlag, Berlin (in press invited).
• M. Durach, A. Rusina, M. I. Stockman, and K.
  Nelson, Toward Full Spatiotemporal Control on the
  Nanoscale, Nano Lett. 7, 3145-3149 (2007).

Interference pattern reversal is achievedby SPP
excitation with different phase-correlated
pulse pairs
In-phase pair of pulses
Out-of-phase pair of pulses