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Optical Properties of Nanoscale
Optical Properties of Nanoscale
Materials
Materials
David G. Stroud
David G. Stroud
,
,
Department of Physics
Department of Physics
,
,
Ohio State University Columbus OH 43210
Ohio State University Columbus OH 43210
Work supported by NSF Grant DMR01-04987 and NSF DMR04-12295
Work supported by NSF Grant DMR01-04987 and NSF DMR04-12295
and by the Ohio Supercomputer Center
and by the Ohio Supercomputer Center
OUTLINE
OUTLINE
Introduction: Linear Optical Properties and Surface Plasmons
Introduction: Linear Optical Properties and Surface Plasmons
Liquid-Crystal Coated Nanoparticles
Liquid-Crystal Coated Nanoparticles
Surface Plasmons in Nanoparticle Chains
Surface Plasmons in Nanoparticle Chains
Composites of Gold Nanoparticles and DNA
Composites of Gold Nanoparticles and DNA
Conclusions
Conclusions
“
“
Labors of the Months” (Norwich, England, ca. 1480).
Labors of the Months” (Norwich, England, ca. 1480).
(The ruby color is probably due to embedded
(The ruby color is probably due to embedded
gold nanoparticles.)
gold nanoparticles.)
The Lycurgus Cup (glass; British
The Lycurgus Cup (glass; British
Museum; 4
Museum; 4
th
th
century A. D.)
century A. D.)
When illuminated from
outside, it appears
green. However, when
Illuminated from within
the cup, it glows red.
Red color is due to very
small amounts of gold
powder (about 40 parts
per million)
Lycurgus Cup illuminated from
Lycurgus Cup illuminated from
within
within
When illuminated from
within, the Lycurgus cup
glows red. The red color
is due to tiny gold
particles embedded in
the glass, which have an
absorption peak at
around 520 nm
What is the origin of the color?
What is the origin of the color?
Answer: ``surface plasmons’’
Answer: ``surface plasmons’’
An SP is a natural oscillation of the electron gas
An SP is a natural oscillation of the electron gas
inside a
inside a
gold
gold
nanosphere
nanosphere
.
.
SP frequency depends on the
SP frequency depends on the
dielectric
dielectric
function
function
of the gold, and the
of the gold, and the
shape
shape
of the nanoparticle.
of the nanoparticle.
electron
sphere
Ionic
background
Electron cloud oscillates with frequency of SP; ions provide restoring
force.
(not to
scale)
Sphere in an applied electric field
Sphere in an applied electric field
Surface plasmon is excited when a long-
Surface plasmon is excited when a long-
wavelength electromagnetic wave is incident on a
wavelength electromagnetic wave is incident on a
metallic sphere.
metallic sphere.
Metallic sphere
EM wave
Incident electric field
is E_0exp(-i w t)
Calculation of SP Frequency
Calculation of SP Frequency
0
0
0
2
3
EE
in
in
εε
ε
+
=
=
0
E
2
2
1
ω
ω
ε
p
in
−=
0
0
21
ε
ω
ω
+
=
applied electric field;
= Drude dielectric function
Surface plasmon
frequency is therefore:
=
0
ε
host dielectric function
(This assumes particle is small compared to wavelength.)
Extinction coefficient, dilute suspension of Au
Extinction coefficient, dilute suspension of Au
particles in acqueous solution
particles in acqueous solution
Crosses: experiment [Elghanian et al, Science 277, 1078 (1997);
Storhoff et al, JACS 120, 1959 (1998). Dashed and full curves:
calculated with and without quantum size corrections [Park and
Stroud, PRB 68, 224201 (2003)].
Control of Surface Plasmons Using
Control of Surface Plasmons Using
Nematic Liquid Crystals
Nematic Liquid Crystals
A nematic liquid crystal (NLC) is a liquid made up of rod-like
A nematic liquid crystal (NLC) is a liquid made up of rod-like
molecules, which can be oriented by an applied dc electric field.
molecules, which can be oriented by an applied dc electric field.
The axis of the NLC is known as the director.
The axis of the NLC is known as the director.
The dielectric tensor of the NLC is anisotropic, with different
The dielectric tensor of the NLC is anisotropic, with different
components parallel and perpendicular to the director.
components parallel and perpendicular to the director.
Schematic of experimental configuration
Experiment to show electric field control of surface plasmon
frequency of gold nanoparticles, using nematic liquid crystals
[J. Muller et al, Appl. Phys. Lett. 81, 171 (2002).]
[...]... energy flow around corners, etc Nanoparticle chain d a Surface plasmons can propagate along a periodic chain of metallic nanoparticles (above) Photon STM Image of a Chain of Au nanoparticles [from Krenn et al, PRL 82, 2590 (1999)] Individual particles: 100x100x40 nm, separated by 100 nm and deposited on an ITO substrate Sphere at end of waveguide is excited using the tip of near-field scanning optical... comparison of unlinked and aggregated Au nanoparticles Absorptance of unlinked and aggregated Au nanoparticles, as measured by Storhoff et al [J Am Chem Soc 120, 1959 (1998)] Description of Previous Slide Source: R Jin et al, J Am Chem Soc 125, 1643 (2003) Top two pictures show (a) samples under transmitted light before and after being exposed to the target (b) UV and visible extinction coefficients of. .. detected using fluorescent nanospheres Calculation of SP modes in nanoparticle chain In the dipole approximation, there are three SP modes on each sphere, two polarized perpendicular to chain, and one polarized parallel The propagating waves are linear combinations of these modes on different spheres In our calculation, we include all multipoles, not just dipoles Then there are a infinite number of. .. (Experimental splitting at zero applied field closest to “melon” morphology Maximum splitting in expt: 30 meV; in melon config, 22 mev) Propagating Waves of Surface Plasmons in Chains of Nanoparticles A chain of closely spaced metallic nanoparticles allows WAVES of surface plasmons to propagate down the chain The waves can be either transverse (T) or longitudinal (L) modes, and can have group velocities... volumes, each of which carry dipole moment Dipole moment due to local electric field from all the other dipoles Calculate total cross-section, using multipole-scattering approach Can be used for anisotropic, and absorbing, scatterers Connect polarizability of small volume to dielectric function, using Clausius-Mossotti approximation Calculated surface plasmon frequency as a function of metal particle... 2003a] Place Au nanoparticles on a simple cubic (SC) lattice Each Au particle has N single DNA strands, of which N/z point towards each of z nearest neighbors (z = 6 for SC) Two-state model for reaction converting two single strands into a double strand: S+S = D Probability of double-strand forming is p(T), determined by chemical equilibrium constant of reaction Probability that no...Measured deviation of surface plasmon resonance energy from mean value, vs angular position of polarization analyzer From Muller et al, Appl Phys Lett 81, 171 (2002) Maximum splitting: 30 mev (expt) Pictures (b) and © from D.R.Nelson, Nano Lett (2002) Plausible configurations of liquid crystal coating: (a) “uniform” (director always in same direction);... dispersion relations s(k) for L and T modes in a chain of nanoparticles, plotted vs k for (a-f) a/d=0.25,0.33,0.4,0.45, 0.49,0.5 (spheres touching) a=sphere radius, d=distance between sphere centers Open symbols: point dipole approx The symbol s = (1 − ε m / ε s ) −1 [Park and Stroud, PRB69, 125418 (2004)] Melting and Optical Properties of Gold/DNA Nanocomposites Linker DNA At high T, single Au particles... dehybridization of DNA duplexes, using T-dependent bond-breaking probability used for percolation model Repeat this aggregation/dehybridization process many times Result is a fractal cluster with a T-dependent fractal dimension Appropriate when aggregation process is non-equilibrium Once aggregation process is complete, calculate optical properties versus T, using DDA Discrete Dipole Approximation Melting of Au/DNA... particles on a cubic lattice (a): all bonds present; (b) 50% of bonds present; (c) 20% of bonds present (d) Low temperature cluster formed by reaction-limited cluster-cluster aggregation (RLCA) Extinction coefficient, dilute suspension Extinction coefficient per unit vol of Au,dilute suspension Crosses: experiment [Elghanian et al, Science (1997); Storhoff et al, JACS (1998) Dashed and full curves: calculated . metallic nanoparticles (above)
chain of metallic nanoparticles (above)
a
d
Photon STM Image of a Chain of
Photon STM Image of a Chain of
Au nanoparticles.
detected using fluorescent nanospheres.
detected using fluorescent nanospheres.
Calculation of SP modes in
Calculation of SP modes in
nanoparticle chain
nanoparticle
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