NANOPHOTONICS II Term 1 2006 Professor Derryck Reid

The following are highly cited papers in topics covered by the Nanophotonics II module.

Ultra-high-Q photonic double-heterostructure nanocavity

NATURE MATERIALS Vol 4, p207 (2005)
No abstract available

The use of nanocrystals in biological detection

NATURE BIOTECHNOLOGY Vol 22, p47 (2004)
In the coming decade, the ability to sense and detect the state of biological systems and living
organisms optically, electrically and magnetically will be radically transformed by developments in
materials physics and chemistry. The emerging ability to control the patterns of matter on the
nanometer length scale can be expected to lead to entirely new types of biological sensors. These new
systems will be capable of sensing at the single-molecule level in living cells, and capable of parallel
integration for detection of multiple signals, enabling a diversity of simultaneous experiments, as well
as better crosschecks and controls.

Subwavelength-diameter silica wires for low-loss optical wave guiding

NATURE Vol 426, p816 (2003)
Silica waveguides with diameters larger than the wavelength of transmitted light are widely used in
optical communications, sensors and other applications(1-3). Minimizing the width of the waveguides
is desirable for photonic device applications, but the fabrication of low-loss optical waveguides with
subwavelength diameters remains challenging because of strict requirements on surface roughness and
diameter uniformity(4-7). Here we report the fabrication of subwavelength-diameter silica 'wires' for
use as low-loss optical waveguides within the visible to near-infrared spectral range. We use a two-
step drawing process to fabricate long free-standing silicawires with diameters down to 50 nm that
show surface smoothness at the atomic level together with uniformity of diameter. Light can be
launched into these wires by optical evanescent coupling. The wires allow single-mode operation, and
have an optical loss of less than 0.1 dB mm(-1). We believe that these wires provide promising building
blocks for future microphotonic devices with subwavelength-width structures.

A revolution in optical manipulation

NATURE Vol 424, p810 (2003)
Optical tweezers use the forces exerted by a strongly focused beam of light to trap and move objects
ranging in size from tens of nanometres to tens of micrometres. Since their introduction in 1986, the
optical tweezer has become an important tool for research in the fields of biology, physical chemistry
and soft condensed matter physics. Recent advances promise to take optical tweezers out of the
laboratory and into the mainstream of manufacturing and diagnostics; they may even become
consumer products. The next generation of single-beam optical traps offers revolutionary new
opportunities for fundamental and applied research.

Surface plasmon subwavelength optics

NATURE Vol 424, p824 (2003)
Surface plasmons are waves that propagate along the surface of a conductor. By altering the structure
of a metal's surface, the properties of surface plasmons- in particular their interaction with light-can
be tailored, which offers the potential for developing new types of photonic device. This could lead to
miniaturized photonic circuits with length scales that are much smaller than those currently achieved.
Surface plasmons are being explored for their potential in subwavelength optics, data storage, light
generation, microscopy and bio-photonics.

Electrically induced optical emission from a carbon nanotube FET

SCIENCE Vol 300, p783 (2003)
Polarized infrared optical emission was observed from a carbon nanotube ambipolar field-effect
transistor (FET). An effective forward-biased p-n junction, without chemical dopants, was created in
the nanotube by appropriately biasing the nanotube device. Electrical measurements show that the
observed optical emission originates from radiative recombination of electrons and holes that are
simultaneously injected into the undoped nanotube. These observations are consistent with a nanotube
FET model in which thin Schottky barriers form at the source and drain contacts. This arrangement is
a novel optical recombination radiation source in which the electrons and holes are injected into a
nearly field-free region. Such a source may form the basis for ultrasmall integrated photonic devices.

Structure of optical vortices

PHYSICAL REVIEW LETTERS Vol 90, p133901 (2003)
Helical modes of light can be focused into toroidal optical traps known as optical vortices, which are
capable of localizing and applying torques to small volumes of matter. Measurements of optical
vortices created with the dynamic holographic optical tweezer technique reveal an unsuspected
dependence of their structure and angular momentum flux on their helicity. These measurements also
provide evidence for a novel optical ratchet potential in practical optical vortices.

The optical properties of metal nanoparticles: The influence of size, shape, and dielectric
environment
JOURNAL OF PHYSICAL CHEMISTRY B Vol 107, p668 (2003)
The optical properties of metal nanoparticles have long been of interest in physical chemistry, starting
with Faraday's investigations of colloidal gold in the middle 1800s. More recently, new lithographic
techniques as well as improvements to classical wet chemistry methods have made it possible to
synthesize noble metal nanoparticles with a wide range of sizes, shapes, and dielectric environments.
In this feature article, we describe recent progress in the theory of narroparticle optical properties,
particularly methods for solving Maxwell's equations for light scattering from particles of arbitrary
shape in a complex environment. Included is a description of the qualitative features of dipole and
quadrupole plasmon resonances for spherical particles; a discussion of analytical and numerical
methods for calculating extinction and scattering cross-sections, local fields, and other optical
properties for nonspherical particles; and a survey of applications to problems of recent interest
involving triangular silver particles and related shapes.

Efficient source of single photons: A single quantum dot in a micropost microcavity

PHYSICAL REVIEW LETTERS Vol 89, p233602 (2002)
We have demonstrated efficient production of triggered single photons by coupling a single
semiconductor quantum dot to a three-dimensionally confined optical mode in a micropost
microcavity. The efficiency of emitting single photons into a single-mode traveling wave is
approximately 38%, which is nearly 2 orders of magnitude higher than for a quantum dot in bulk
semiconductor material. At the same time, the probability of having more than one photon in a given
pulse is reduced by a factor of 7 as compared to light with Poissonian photon statistics.

Nanowire resonant tunneling diodes

APPLIED PHYSICS LETTERS Vol 81, p4458 (2002)
Semiconductor heterostructures and their implementation into electronic and photonic devices have
had tremendous impact on science and technology. In the development of quantum nanoelectronics,
one-dimensional (1D) heterostructure devices are receiving a lot of interest. We report here functional
1D resonant tunneling diodes obtained via bottom-up assembly of designed segments of different
semiconductor materials in III/V nanowires. The emitter, collector, and the central quantum dot are
made from InAs and the barrier material from InP. Ideal resonant tunneling behavior, with peak-to-
valley ratios of up to 50:1 and current densities of 1 nA/mum(2) was observed at low temperatures. (C)
2002 American Institute of Physics.

Epitaxial core-shell and core-multishell nanowire heterostructures

NATURE Vol 420, p57 (2002)
Semiconductor heterostructures with modulated composition and/or doping enable passivation of
interfaces and the generation of devices with diverse functions(1). In this regard, the control of
interfaces in nanoscale building blocks with high surface area will be increasingly important in the
assembly of electronic and photonic devices(2-10). Core-shell heterostructures formed by the growth of
crystalline overlayers on nanocrystals offer enhanced emission efficiency 7, important for various
applications(8-10). Axial heterostructures have also been formed by a one-dimensional modulation of
nanowire composition(11-13) and doping(11). However, modulation of the radial composition and
doping in nanowire structures has received much less attention than planar 1 and nanocrystal(7)
systems. Here we synthesize silicon and germanium core-shell and multishell nanowire
heterostructures using a chemical vapour deposition method applicable to a variety of nanoscale
materials(14). Our investigations of the growth of boron-doped silicon shells on intrinsic silicon and
silicon-silicon oxide core-shell nanowires indicate that homoepitaxy can be achieved at relatively low
temperatures on clean silicon. We also demonstrate the possibility of heteroepitaxial growth of
crystalline germanium-silicon and silicon-germanium core-shell structures, in which band-offsets drive
hole injection into either germanium core or shell regions. Our synthesis of core-multi-shell structures,
including a high-performance coaxially gated field-effect transistor, indicates the general potential of
radial heterostructure growth for the development of nanowire-based devices.

Indistinguishable photons from a single-photon device

NATURE Vol 419, p594 (2002)
Single-photon sources have recently been demonstrated using a variety of devices, including
molecules(1-3), mesoscopic quantum wells(4), colour centres(5), trapped ions(6) and semiconductor
quantum dots(7-11). Compared with a Poisson-distributed source of the same intensity, these sources
rarely emit two or more photons in the same pulse. Numerous applications for single-photon sources
have been proposed in the field of quantum information, but most-including linear-optical quantum
computation(12)-also require consecutive photons to have identical wave packets. For a source based
on a single quantum emitter, the emitter must therefore be excited in a rapid or deterministic way, and
interact little with its surrounding environment. Here we test the indistinguishability of photons emitted
by a semiconductor quantum dot in a microcavity through a Hong-Ou-Mandel-type two-photon
interference experiment(13,14). We find that consecutive photons are largely indistinguishable, with a
mean wave-packet overlap as large as 0.81, making this source useful in a variety of experiments in
quantum optics and quantum information.

A nanoscale optical blosensor: Sensitivity and selectivity of an approach based on the localized
surface plasmon resonance spectroscopy of triangular silver nanoparticles
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Vol 124, p10596 (2002)
Triangular silver nanoparticles (similar to100 nm wide and 50 nm high) have remarkable optical
properties. In particular, the peak extinction wavelength, lambda(max) of their localized surface
plasmon resonance (LSPR) spectrum is unexpectedly sensitive to nanoparticle size, shape, and local
(similar to10-30 nm) external dielectric environment. This sensitivity of the LSPR lambda(max) to the
nanoenvironment has allowed us to develop a new class of nanoscale affinity biosensors. The essential
characteristics and operational principles of these LSPR nanobiosensors will be illustrated using the
well-studied biotin-streptavidin system. Exposure of biotin-functionalized Ag nanotriangles to 100 nM
streptavidin (SA) caused a 27.0 nm red-shift in the LSPR lambda(max). The LSPR lambda(max) shift,
DeltaR/DeltaR(max), versus [SA] response curve was measured over the concentration range 10(-15)
M < [SA] < 10(-6) M. Comparison of the data with the theoretical normalized response expected for
1:1 binding of a ligand to a multivalent receptor with different sites but invariant affinities yielded
approximate values for the saturation response, DeltaR(max) = 26.5 nm, and the surface-confined
thermodynamic binding constant K-a,K-surf = 10(11) M-1. At present, the limit of detection (LOD) for
the LSPR nanobiosensor is found to be in the low-picomolar to high-femtomolar region. A strategy to
amplify the response of the LSPR nanobiosensor using biotinylated Au colloids and thereby further
improve the LOD is demonstrated. Several control experiments were performed to define the LSPR
nanobiosensor's response to nonspecific binding as well as to demonstrate its response to the specific
binding of another protein. These include the following: (1) electrostatic binding of SA to a
nonbiotinylated surface, (2) nonspecific interactions of prebiotinylated SA to a biotinylated surface, (3)
nonspecific interactions of bovine serum albumin to a biotinylated surface, and (4) specific binding of
anti-biotin to a biotinylated surface. The LSPR nanobiosensor provides a pathway to ultrasensitive
biodetection experiments with extremely simple, small, light, robust, low-cost instrumentation that will
greatly facilitate field-portable environmental or point-of-service medical diagnostic applications.

Lasing from semiconductor quantum rods in a cylindrical microcavity

ADVANCED MATERIALS Vol 14, p317 (2002)
Lasers based on colloidal semiconductor nanostructures can benefit from the remarkable spectral
coverage afforded through the quantum confinement effect. The first observation of lasing for colloidal
CdSe/ZnS quantum rods in solution using a cylindrical microcavity is reported here (see also inside
front cover). Lasing in the same configuration was also observed for spherical nanocrystal quantum
dots. For the quantum dots lasing is not polarized, but in quantum rods the laser emission is highly
linearly polarized, a desirable feature for laser and photonic applications.

Electrically driven single-photon source

SCIENCE Vol 295, p102 (2002)
Electroluminescence from a single quantum dot within the intrinsic region of a p-i-n junction is shown
to act as an electrically driven single-photon source. At low injection currents, the dot
electroluminescence spectrum reveals a single sharp line due to exciton recombination, white another
tine due to the biexciton emerges at higher currents. The second-order correlation function of the diode
displays anti-bunching under a continuous drive current. Single-photon emission is stimulated by
subnanosecond voltage pulses. These results suggest that semiconductor technology can be used to
mass-produce a single-photon source for applications in quantum information technology.

Photoinduced conversion of silver nanospheres to nanoprisms

SCIENCE Vol 294, p1901 (2001)
A photoinduced method for converting large quantities of silver nanospheres into triangular
nanoprisms is reported. The photo-process has been characterized by time-dependent ultraviolet-
visible spectroscopy and transmission electron microscopy, allowing for the observation of several key
intermediates in and characteristics of the conversion process. This light-driven process results in a
colloid with distinctive optical properties that directly relate to the nanoprism shape of the particles.
Theoretical calculations coupled with experimental observations allow for the assignment of the
nanoprism plasmon bands and for the first identification of two distinct quadrupole plasmon
resonances for a nanoparticle. Unlike the spherical particles they are derived from that Rayleigh tight-
scatter in the blue, these nanoprisms exhibit scattering in the red, which could be useful in developing
multicolor diagnostic labels on the basis not only of nanoparticle composition and size but also of
shape.

Plasmonics - A route to nanoscale optical devices

ADVANCED MATERIALS Vol 13, p1501 (2001)
Plasmon waveguides, which are based on resonance between collective motions in noble-metal
nanoparticles and visible light, should be useful in building novel nanoscale optical devices;
calculations predict that corner. switch, and splitter elements are feasible. Experiments with
microwaves on macroscopic analogues confirm the guiding and splitting effects. The Figure shows a
corner element made of 50 nm circle divide, 75 nm spaced gold dots.

Highly polarized photoluminescence and photodetection from single indium phosphide

nanowires
SCIENCE Vol 293, p1455 (2001)
We have characterized the fundamental photoluminescence (PL) properties of individual, isolated
indium phosphide (InP) nanowires to define their potential for optoelectronics. Polarization-sensitive
measurements reveal a striking anisotropy in the PL intensity recorded parallel and perpendicular to
the long axis of a nanowire. The order-of-magnitude polarization anisotropy was quantitatively
explained in terms of the large dielectric contrast between these freestanding nanowires and
surrounding environment, as opposed to quantum confinement effects. This intrinsic anisotropy was
used to create polarization-sensitive nanoscale photodetectors that may prove useful in integrated
photonic circuits, optical switches and interconnects, near-field imaging, and high-resolution
detectors.

Some interesting properties of metals confined in time and nanometer space of different shapes
ACCOUNTS OF CHEMICAL RESEARCH Vol 34, p257 (2001)
The properties of a material depend on the type of motion its electrons can execute, which depends on
the space available for them (i.e., on the degree of their spatial confinement). Thus, the properties of
each material are characterized by a specific length scale, usually on the nanometer dimension. If the
physical size of the material is reduced below this length scale, its properties change and become
sensitive to its size and shape. In this Account we describe some of the observed new chemical, optical,
and thermal properties of metallic nanocrystals when their size is confined to the nanometer length
scale and their dynamical processes are observed on the femto- to picosecond time scale.

Triggered single photons from a quantum dot

PHYSICAL REVIEW LETTERS Vol 86, p1502 (2001)
We demonstrate a new method fur generating triggered single photons. After a laser pulse generates
excitons inside a single quantum dot, electrostatic interactions between them and the resulting spectral
shifts allow a single emitted photon to be isolated. Correlation measurements show a reduction of the
two-photon probability to 0.12 times the value for Poisson light. Strong antibunching persists when the
emission is saturated. The emitted photons are also polarized.
A quantum dot single-photon turnstile device
SCIENCE Vol 290, p2282 (2000)
Quantum communication relies on the availability of Light pulses with strong quantum correlations
among photons. An example of such an optical source is a single-photon pulse with a vanishing
probability for detecting two or more photons. Using pulsed laser excitation of a single quantum dot, a
single-photon turnstile device that generates a train of single-photon pulses was demonstrated. For a
spectrally isolated quantum dot, nearly 100% of the excitation pulses Lead to emission of a single
photon, yielding an ideal single-photon source.

Negative refraction makes a perfect lens

PHYSICAL REVIEW LETTERS Vol 85, p3966 (2000)
With a conventional lens sharpness of the image is always limited by the wavelength of light. An
unconventional alternative to a lens, a slab of negative refractive index material, has the power to
focus all Fourier components of a 2D image, even those that do not propagate in a radiative manner.
Such "superlenses" can be realized in the microwave band with current technology. Our simulations
show that a version of the lens operating at the frequency of visible light can be realized in the form of
a thin slab of silver. This optical version resolves objects only a few nanometers across.

Colloidal Au-enhanced surface plasmon resonance for ultrasensitive detection of DNA

hybridization
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Vol 122, p9071 (2000)
A new approach to ultrasensitive detection of DNA hybridization based on nanoparticle-amplified
surface plasmon resonance (SPR) is described. Use of the Au nanoparticle tags leads to a greater than
10-fold increase in angle shift, corresponding to a more than 1000-fold improvement in sensitivity for
the target oligonucleotide as compared to the unamplified binding event. This enhanced shift in SPR
reflectivity is a combined result of greatly increased surface mass, high dielectric constant of Au
particles, and electromagnetic coupling between An nanoparticles and the Au film. DNA melting and
digestion experiments further supported the feasibility of this approach in DNA hybridization studies;
The extremely large angle shifts observed in particle-amplified SPR make it possible to conduct SPR
imaging experiments on DNA arrays.:ln the present work, macroscopic 4 x 4 arrays; were employed,
and a similar to 10 pM limit of quantitation. was achieved for 24-mer oligonucleotides (surface density
less than or equal to 8 x 10(8) molecules/cm(2)). Even without further optimization, the sensitivity of
this technique begins to approach that of traditional fluorescence-based methods for DNA
hybridization. These results illustrate the potential of particle-amplified SPR for array-based DNA
analysis and ultrasensitive detection of oligonucleotides.

Quantum correlation among photons from a single quantum dot at room temperature
NATURE Vol 406, p968 (2000)
Maxwell's equations successfully describe the statistical properties(1,2) of fluorescence from an
ensemble of atoms or semiconductors in one or more dimensions. But quantization of the radiation
field is required to explain the correlations of light generated by a single two-level quantum emitter,
such as an atom, ion or single molecule(3-6). The observation of photon antibunching in resonance
fluorescence from a single atom unequivocally demonstrated the non-classical nature of radiation(3).
Here we report the experimental observation of photon antibunching from an artificial system-a single
cadmium selenide quantum dot at room temperature. Apart from providing direct evidence for a solid-
state non-classical light source, this result proves that a single quantum dot acts like an artificial atom,
with a discrete anharmonic spectrum. In contrast, we rnd the photon-emission events from a cluster of
several dots to be uncorrelated.

Entropic attraction and repulsion in binary colloids probed with a line optical tweezer
PHYSICAL REVIEW LETTERS Vol 82, p4352 (1999)
The long-range entropic forces that arise between two micrometer-sized colloidal spheres in a fluid of
much smaller colloidal spheres were directly measured using a line-scanned optical tweezer. This new
technique allowed us to measure the functional form of the potential with sub-k(B)T energy and 15 nm
spatial resolution. At the lowest small sphere concentrations, the potential was monotonically
attractive, while at higher concentrations an oscillatory potential was observed, due to the liquid
structure of the small spheres. Surprisingly, the large spheres came together only rarely at the higher
concentrations, suggesting a new means for stabilizing suspensions using entropy alone. [S0031-
9007(99)09246-7].
Photonic wires of nanometric dimensions. Electronic energy transfer in rigid rodlike
Ru(bpy)(3)(2+)-(ph)(n)-Os(bpy)(3)(2+) compounds (ph=1,4-phenylene; n=3, 5, 7)
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Vol 121, p4207 (1999)
We have synthesized nine rodlike compounds of nanometric dimension with general formula
[M(bpy)(3)- (ph)(n)-M'(bpy)(3)](4+) (M = M' = Ru(II); M = M' = Os(II); M = Ru(II), M' = Os(II); bpy
= 2,2'-bipyridine; ph = 1,4-phenylene; n = 3, 5, 7; the central phenylene unit bears two alkyl chains
for solubility reasons; the metal-to metal distance is 4.2'nm for the longest spacer). The absorption
spectra and the luminescence properties (emission spectra, quantum yields, and excited-state lifetimes)
of the nine dinuclear complexes have been investigated in acetonitrile solution at 293 K and in
butyronitrile rigid matrix at 77 K. The results obtained have been compared with those found for the
separated chromophoric units ([RU(bpy)(3)](2+), [Os(bpy)(3)](2+), and oligophenylene derivatives).
The absorption spectrum of each dinuclear complex is essentially equal to the sum of the spectra of the
component species, showing that intercomponent electronic interactions are weak. In the
homodinuclear compounds, the strong fluorescence of the oligophenylene spacers is completely
quenched by energy transfer to the metal-based units, which exhibit their characteristic metal-to-ligand
charge-transfer (MLCT) phosphorescence. In the heterodinuclear compounds, besides complete
quenching of the fluorescence of the oligophenylene spacers, a quenching of the phosphorescence of
the [Ru(bpy)(3)](2+) chromophoric unit and a parallel sensitization of the phosphorescence of the
[Os(bpy)(3)](2+) chromophoric unit are observed, indicating the occurrence of electronic energy
transfer. The rate of the energy-transfer process from the [Ru(bpy)(3)](2+) to the [Os(bpy)(3)](2+)
unit is practically temperature independent and decreases with increasing length of the oligophenylene
spacer tin acetonitrile solution at 293 K, k(en) = 6.7 x 10(8) s(-1) for n = 3; k(en) = 1.0 x 10(7) s(-1)
for n = 5; k(en) = 1.3 x 10(6) s(-1) for n = 7). It is shown that such an energy-transfer process takes
place via a Dexter-type mechanism (superexchange interaction) with an attenuation coefficient of 0.32
per Angstrom, and 1.5 per interposed phenylene unit.

Squeezing the optical near-field zone by plasmon coupling of metallic nanoparticles

PHYSICAL REVIEW LETTERS Vol 82, p2590 (1999)
We report on the experimental observation of near-field optical effects close to Au nanoparticles using
a photon scanning tunneling microscope (PSTM). Constant height operation of the PSTM allowed an
unprecedented direct comparison with theoretical computations of the distribution of the optical near-
field intensity. An unexpected squeezing of the optical near field due to plasmon coupling was observed
above a chain of Au nanoparticles. [S0031-9007(99)08708-6].

Fluorescence spectroscopy of single biomolecules

SCIENCE Vol 283, p1676 (1999)
Recent advances in single-molecule detection and single-molecule spectroscopy at room temperature
by Laser-induced fluorescence offer new tools for the study of individual macromolecules under
physiological conditions. These tools relay conformational states, conformational dynamics, and
activity of single biological molecules to physical observables, unmasked by ensemble averaging.
Distributions and time trajectories of these observables can therefore be measured during a reaction
without the impossible need to synchronize all the molecules in the ensemble. The progress in applying
these tools to biological studies with the use of fluorophores that are site-specifically attached to
macromolecules is reviewed.

An approach for recording and readout beyond the diffraction limit with an Sb thin film
APPLIED PHYSICS LETTERS Vol 73, p2078 (1998)
A technique for recording and retrieving small marks beyond the optical diffraction limit was
proposed. The basic experiment with this technique was also carried out at a constant linear velocity of
2.0 m/s, rotating a disk with a multi-layered structure of Sb and GeSbTe, which were separated by a
thin film of SiN. By use of the optically nonlinear property of the Sb thin film, carrier to noise ratio of
more than 10 dB was obtained from recorded marks of 90 nm, using an optical system with the laser
wavelength of 686 nm and a numerical aperture of 0.6. (C) 1998 American Institute of Physics.
[S0003-6951(98)02141-X].

Quantum dot bioconjugates for ultrasensitive nonisotopic detection

SCIENCE Vol 281, p2016 (1998)
Highly luminescent semiconductor quantum dots (zinc sulfide-capped cadmium selenide) have been
covalently coupled to biomolecules for use in ultrasensitive biological detection. In comparison with
organic dyes such as rhodamine, this class of luminescent labels is 20 times as bright, 100 times as
stable against photobleaching, and one-third as wide in spectral linewidth. These nanometer-sized
conjugates are water-soluble and biocompatible, Quantum dots that were labeled with the protein
transferrin underwent receptor-mediated endocytosis in cultured HeLa cells, and those dots that were
labeled with immunomolecules recognized specific antibodies or antigens.

Optical tweezer arrays and optical substrates created with diffractive optics
REVIEW OF SCIENTIFIC INSTRUMENTS Vol 69, p1974 (1998)
We describe a simple method for creating multiple optical tweezers from a single laser beam using
diffractive optical elements. As a demonstration of this technique, we have implemented a 4x4 square
array of optical tweezers-the hexadeca tweezer. Not only will diffractively generated optical tweezers
facilitate many new experiments in pure add applied physics, but they also will be useful for fabricating
nanocomposite materials and devices, including photonic bandgap materials and optical circuit
elements. (C) 1998 American Institute of Physics.

Surface-plasmon resonances in single metallic nanoparticles

PHYSICAL REVIEW LETTERS Vol 80, p4249 (1998)
Using a near-field optical antenna effect, we measure the homogeneous line shape of the surface-
plasmon resonance in single gold nanoparticles. The surface-plasmon dephasing times extracted from
the near-field spectra of the individual particles vary around 8 fs. This mean value agrees with
calculations based on Mie theory, which neglect surface effects. Deviations of individual particles from
this value an interpreted as being due to variations in the local nanoenvironment. We also observe
double-peaked line shapes caused by electromagnetic coupling between close-lying particles.

Supernormal vision and high-resolution retinal imaging through adaptive optics

JOURNAL OF THE OPTICAL SOCIETY OF AMERICA A-OPTICS IMAGE SCIENCE AND
VISION Vol 14, p2884 (1997)
Even when corrected with the best spectacles or contact lenses, normal human eyes still. suffer from
monochromatic aberrations that blur vision when the pupil is large. We have successfully corrected
these aberrations using adaptive optics, providing normal eyes with supernormal optical quality.
Contrast sensitivity to fine spatial patterns was increased when observers viewed stimuli through
adaptive optics. The eye's aberrations also limit the resolution of images of the retina, a limit that has
existed since the invention of the ophthalmoscope. We have constructed a fundus camera equipped with
adaptive optics that provides unprecedented resolution, allowing the imaging of microscopic structures
the size of single cells in the living human retina. (C) 1997 Optical Society of America.

Epitaxial growth of highly luminescent CdSe/CdS core/shell nanocrystals with photostability and
electronic accessibility
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Vol 119, p7019 (1997)
The synthesis of epitaxially grown, wurtzite CdSe/CdS core/shell nanocrystals is reported. Shells of up
to three monolayers in thickness were grown on cores ranging in diameter from 23 to 39 Angstrom.
Shell growth was controllable to within a tenth of a monolayer and was consistently accompanied by a
red shift of the absorption spectrum, an increase of the room temperature photoluminescence quantum
yield (up to at least 50%), and an increase in the photostability. Shell growth was shown to be uniform
and epitaxial by the use of X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), high
resolution transmission electron microscopy (HRTEM), and optical spectroscopy. The experimental
results indicate that in the excited state the hole is confined to the core and the electron is delocalized
throughout the entire structure. The photostability can be explained by the confinement of the hole,
while the delocalization of the electron results in a degree of electronic accessibility that makes these
nanocrystals attractive for use in optoelectronic devices.

Optical absorption spectra of nanocrystal gold molecules

JOURNAL OF PHYSICAL CHEMISTRY B Vol 101, p3706 (1997)
The optical absorption spectra of a series of nanocrystal gold molecules-larger, crystalline Au clusters
that are passivated by a compact monolayer of n-alkylthiol(ate)s-have been measured across the
electronic range (1.1-4.0 eV) in dilute solution at ordinary temperature. Each of the similar to 20
samples, ranging in effective core diameter from 1.4 to 3.2 nm (similar to 70 to similar to 800 Au
atoms), has been purified by fractional crystallization and has undergone a separate compositional
and structural characterization by mass spectrometry and X-ray diffraction. With decreasing core mass
(crystallite size) the spectra uniformly show a systematic evolution, specifically (i) a broadening of the
so-called surface-plasmon band until it is essentially unidentifiable for crystallites of less than 2.0 nm
effective diameter, (ii) the emergence of a distinct onset for strong absorption near the energy (similar
to 1.7 eV) of the interbandgap (5d --> 6sp), and (iii) the appearance in the smallest crystallites of a
weak steplike structure above this onset, which is interpreted as arising from a series of transitions
from the i continuum d-band to the discrete level structure of the conduction band just above the Fermi
level. The classical electrodynamic (Mie) theory, based on bulk optical properties, can reproduce this
spectral evolution-and thereby yield a consistent core-sizing-only by making a strong assumption about
the surface chemical interaction. Quantitative agreement with the spectral line shape requires a size-
dependent offset of the frequency-dependent dielectric function, which may be explained by a transition
in electronic structure just below 2.0 nm (similar to 200 atoms), as proposed earlier.

Single optical photon detection with a superconducting tunnel junction

NATURE Vol 381, p135 (1996)
THE charge-coupled device (CCD) has become the detector of choice in optical astronomy, CCDs
provide a very linear response to detected photons, are very efficient at some wavelengths, and can
now provide coverage of a relatively wide field of view(1-3). But they become quite inefficient with
decreasing wavelength, and they lack intrinsic wavelength and time resolution, The only way to select
specific wavelengths is to place filters in front of the detector, which makes the total system less
efficient, Time resolution can be achieved only,vith short exposures, which are possible only with very
bright sources. Here we report a superconducting device that can overcome these limitations, and
which has performance characteristics far superior to existing photon counting systems(4-7). Our
superconducting tunnel junction can detect individual photons at rates up to 2.5 kHz in the wavelength
range 200-500 nm, with an intrinsic spectral resolution of 45 mn and a quantum efficiency estimated to
be about 50 per cent, The theoretical resolution of the present device is similar to 20 nm, but use of
superconductors with lower transition temperature could improve that to 8 nm.

Surface plasmon spectroscopy of nanosized metal particles

LANGMUIR Vol 12, p788 (1996)
The use of optical measurements to monitor electrochemical changes on the surface of nanosized metal
particles is discussed within the Drude model. The absorption spectrum of a metal sol in water is
shown to be strongly affected by cathodic or anodic polarization, chemisorption, metal adatom
deposition, and alloying. Anion adsorption leads to strong damping of the free electron absorption.
Cathodic polarization leads to anion desorption. Underpotential deposition (upd) of electropositive
metal layers results in dramatic blue-shifts of the surface plasmon band of the substrate. The
deposition of just 0.1 monolayer can be readily detected by eye. In some cases alloying occurs
spontaneously during upd. Alloy formation can be ascertained from the optical absorption spectrum in
the case of gold deposition onto silver sole. The underpotential deposition of silver adatoms onto
palladium leads to the formation of a homogeneous silver shell, but the mean free path is less than
predicted, due to lattice strain in the shell.

QUANTUM CONFINEMENT AND LIGHT-EMISSION IN SIO2/SI SUPERLATTICES

NATURE Vol 378, p258 (1995)
Photonic devices are becoming increasingly important in information and communication
technologies. But attempts to integrate photonics with silicon-based microelectronics are hampered by
the fact that silicon has an indirect band gap, which prevents efficient electron-photon energy
conversion. Light-emitting silicon-based materials have been made using band-structure engineering
of SiGe and SiC alloys and Si/Ge superlattices, and by exploiting quantum-confinement effects in
nanoscale particles and crystallites(1-3). The discovery(4,5) that silicon can be etched
electrochemically into a highly porous form that emits light with a high quantum yield has opened up
the latter approach to intensive study(6-12). Here we report the fabrication, by molecular-beam
epitaxy, of well-defined superlattices of silicon and SiO2, which emit visible light through
photoluminescence. We show that this light emission can be explained in terms of quantum confinement
of electrons in the two-dimensional silicon layers. These superlattice structures are robust and
compatible with standard silicon technology.

PHOTONIC-WIRE LASER
PHYSICAL REVIEW LETTERS Vol 75, p2678 (1995)
We have achieved lasing in a strongly guided semiconductor waveguide with mode area as small as
0.02 mu m(2) (lambda = 1.4 mu m). The lasing action takes advantage of the large enhancement of
stimulated emission in the waveguide and its suppression of unwanted dipole emission. We call the
waveguide a photonic wire. The laser cavity is a high-Q microcavity ring resonator formed by the
photonic wire and has a small cavity mode volume of 0.27 mu m(3). The lasing behaviors are
consistent with theory. Laser outputs can be obtained via photon tunneling to adjacent waveguides.
The laser realized will allow us to study spontaneous emission and lasing in nanofabricated waveguide
structures.

PROGRESS OF HIGH-RESOLUTION PHOTON SCANNING-TUNNELING-MICROSCOPY

DUE TO A NANOMETRIC FIBER PROBE
JOURNAL OF LIGHTWAVE TECHNOLOGY Vol 13, p1200 (1995)
The present status of a photon scanning tunneling microscope (PSTM) and its application are
reviewed. In order to realize a nanometric apertured fiber probe, a highly reproducible chemical
etching process was developed to realize a sharpened fiber with the cone angle and tip diameter as
small as 14 degrees and 3 mn, respectively. The possibility of tailoring the shapes of the sharpened
fibers was presented. Chemical etching and nanometric photolithography were developed to fabricate
a metallic aperture with a diameter of 30 nm (or even smaller) on the Sharpened fiber tip. Imaging
experiments with biological specimens were carried out by operating the PSTM in the collection mode
and illumination mode geometries. Dependencies of these images on the polarization state of the
incident light were found, and a resolution of 10 mn or even smaller was achieved, Nondestructive
inspection of dielectric optical waveguides with subwavelength resolution was proposed by presenting
the diagnosed results of a proton-exchanged LiTaO3 waveguide, Possibilities of diagnosing
nanometric active photonic devices were also demonstrated through imaging experiments of
semiconductor quantum dots. Experiments on fluorescence detection from dye-doped nanometric
polystyrene spheres confirmed the enhanced efficiency of coupling of the fluorescence to the fiber tip,
and this was attributed to the spatially inhomogeneous spontaneous emission due to the-short-range
electromagnetic interaction between the sphere and probe tip. To demonstrate the possibilities of
nanometric fabrication, high density optical storage, especially the photon-mode storage, was
demonstrated to realize a stored circular pit of 100 mm diameter on an organic thin film. As an
ultimate goal of fabrication to explore the future technology of atomic-level material processing, an
atom guide using a hollow fiber and atom trapping by the illumination mode PSTM were proposed to
control the thermal motion of freely flying atoms in vacuum. The concept of a virtual photon based on
an intuitive modeling of the localized evanescent light was introduced to provide a semiclassical theory
of the PSTM. Transfer functions of the PSTM were calculated by using this model, which agreed
qualitatively with the experimental results.

SHARP-LINE PHOTOLUMINESCENCE AND 2-PHOTON ABSORPTION OF ZERO-

DIMENSIONAL BIEXCITONS IN A GAAS/ALGAAS STRUCTURE
PHYSICAL REVIEW LETTERS Vol 73, p1138 (1994)
Using a micron-sized photoluminescence (PL) probe enables us to study single islandlike interface
defects of a thin GaAs/AlGaAs quantum well. The bound exciton ground state locally emits a distinct
sharp line. With increasing excitation of this quantum dot level additional transition lines emerge at
lower energy. They are attributed to localized biexciton states. The biexciton correlation energy is
about 4 meV. A distinct two-photon resonant absorption peak of the biexciton ground state is observed
in PL excitation spectroscopy. Its linewidth is only about 30 mueV. The spectra and their polarization
properties are discussed on the basis of a discrete level scheme and the Pauli exclusion principle.

LIGHT-PROPAGATION THROUGH NANOMETER-SIZED STRUCTURES - THE 2-

DIMENSIONAL-APERTURE SCANNING NEAR-FIELD OPTICAL MICROSCOPE
JOURNAL OF THE OPTICAL SOCIETY OF AMERICA A-OPTICS IMAGE SCIENCE AND
VISION Vol 11, p1768 (1994)
The propagation of light through nanometer-sized structures is studied computationally by use of
multiple-multipole method. A two-dimensional scanning near-field optical microscope structure is
chosen as an example. The relevant near and far fields as well as some imaging properties are
determined for the two principal polarizations. Strikingly different results are obtained for the two
principal polarizations: for 8 polarization, strong field confinement in the gap region, high sensitivity
of the radiation pattern to the presence of an object, and high contrast; for p polarization, higher
signal level with low contrast. At small gap widths a substantial amount of radiation is coupled into the
substrate at angles larger than the critical angle. Line scan simulations for lambda = 488 nm indicate
a resolution of approximately two times the optical slit width. Resolution and contrast can be optimized
by the appropriate choice of detector orientation and angle of acceptance. Coherent superposition of
the radiation emitted into different directions permits further improvements.
SINGLE MOLECULES OBSERVED BY NEAR-FIELD SCANNING OPTICAL
MICROSCOPY
SCIENCE Vol 262, p1422 (1993)
Individual carbocyanine dye molecules in a sub-monolayer spread have been imaged with near-field
scanning optical microscopy. Molecules can be repeatedly detected and spatially localized (to
approximately lambda/50 where lambda is the wavelength of light) with a sensitivity of at least 0.005
molecules/(Hz)1/2 and the orientation of each molecular dipole can be determined. This information is
exploited to map the electric field distribution in the near-field aperture with molecular spatial
resolution.

MEASUREMENT OF THE SINGLE-PHOTON TUNNELING TIME

PHYSICAL REVIEW LETTERS Vol 71, p708 (1993)
Using a two-photon interferometer, we have measured the time delay for a photon to tunnel across a
barrier consisting of a 1.1-mum-thick 1D photonic band-gap material. The peak of the photon wave
packet appears on the far side of the barrier 1.47 +/- 0.21 fs earlier than it would if it were to travel at
the vacuum speed of light c. Although the apparent tunneling velocity (1.7 +/- 0.2)c is superluminal,
this is not a genuine signal velocity, and Einstein causality is not violated. The measured tunneling time
is consistent with the group delay (''phase time''), but not with the semiclassical time.

NEAR-FIELD MAGNETOOPTICS AND HIGH-DENSITY DATA-STORAGE

APPLIED PHYSICS LETTERS Vol 61, p142 (1992)
Near-field scanning optical microscopy (NSOM) has been used to image and record domains in thin-
film magneto-optic (MO) materials. In the imaging mode, resolution of 30-50 nm has been consistently
obtained, whereas in the recording mode, domains down to approximately 60 nm have been written
reproducibly. Data densities of approximately 45 Gbits/in.2 have been achieved, well in excess of
current magnetic or MO technologies. A brief analysis of speed and other issues indicates that the
technique may represent a viable alternative to these and other methods for anticipated high density
data storage needs.

NEAR-FIELD OPTICS - MICROSCOPY, SPECTROSCOPY, AND SURFACE

MODIFICATION BEYOND THE DIFFRACTION LIMIT
SCIENCE Vol 257, p189 (1992)
The near-field optical interaction between a sharp probe and a sample of interest can be exploited to
image, spectroscopically probe, or modify surfaces at a resolution (down to approximately 12 nm)
inaccessible by traditional far-field techniques. Many of the attractive features of conventional optics
are retained, including noninvasiveness, reliability, and low cost. In addition, most optical contrast
mechanisms can be extended to the near-field regime, resulting in a technique of considerable
versatility. This versatility is demonstrated by several examples, such as the imaging of nanometric-
scale features in mammalian tissue sections and the creation of ultrasmall, magneto-optic domains
having implications for high-density data storage. Although the technique may find uses in many
diverse fields, two of the most exciting possibilities are localized optical spectroscopy of
semiconductors and the fluorescence imaging of living cells.

QUANTUM CRYPTOGRAPHY USING ANY 2 NONORTHOGONAL STATES

PHYSICAL REVIEW LETTERS Vol 68, p3121 (1992)
Quantum techniques for key distribution-the classically impossible task of distributing secret
information over an insecure channel whose transmissions are subject to inspection by an
eavesdropper, between parties who share no secret initially-have been proposed using (a) four
nonorthogonally polarized single-photon states or low-intensity light pulses, and (b) polarization-
entangled or spacetime-entangled two-photon states. Here we show that in principle any two
nonorthogonal quantum states suffice, and describe a practical interferometric realization using low-
intensity coherent light pulses.

COMBINED SHEAR FORCE AND NEAR-FIELD SCANNING OPTICAL MICROSCOPY

APPLIED PHYSICS LETTERS Vol 60, p2484 (1992)
A distance regulation method has been developed to enhance the the reliability, versatility, and ease of
use of near-field scanning optical microscopy (NSOM). The method relies on the detection of shear
forces between the end of a near-field probe and the sample of interest. The system can be used solely
for distance regulation in NSOM, for simultaneous shear force and near-field imaging, or for shear
force microscopy alone. In the latter case, uncoated optical fiber probes are found to yield images
with consistently high resolution.

SEMICONDUCTOR QUANTUM-WIRE STRUCTURES DIRECTLY GROWN ON HIGH-

INDEX SURFACES
PHYSICAL REVIEW B Vol 45, p3507 (1992)
The direct synthesis of GaAs quantum-wire structures on (311) A oriented substrates by molecular-
beam epitaxy has been achieved due to the in situ formation of an array of nanometer-scale macrosteps
or facets with a periodicity determined by energy rather than growth-related parameters. These kinds
of macrosteps are formed by breaking up a flat surface with high surface energy into facets
corresponding to planes with lower surface energy. Reflection high-energy electron diffraction
(RHEED) directly reveals the formation of such macrosteps on the GaAs (311) A surface comprised of
two sets of {331} facets oriented along the [233BAR] direction. The lateral periodicity of 32 angstrom
is determined from the splitting of the zeroth-order streak observed along [233BAR] into sharp
satellites and the height of the steps of 10.2 angstrom from the splitting along its length. The RHEED
intensity dynamics during growth of GaAs/AlAs multilayer structures show a pronounced oscillation at
the onset of GaAs and AlAs, growth, respectively, due to a phase change of the surface corrugation
during the deposition of the first monolayers. The complete structure then contains alternating thicker
and thinner channels of GaAs and AlAs forming the quantum wires oriented along [233BAR], which is
confirmed by high-resolution transmission-electron microscopy. The GaAs quantum-wire structures
grown on (311) substrates exhibit a pronounced anisotropy of the electronic properties.
Photoluminescence and photoluminescence-excitation (PLE) measurements reveal distinct energy
shifts of the excitonic resonances and a strong polarization anisotropy in agreement with theory.
Confinement energies up to 90 meV are determined from the appearance of phonon-related lines in the
PLE spectra. A strong anisotropy in conductivity is observed in modulation-doped heterostructures.
The integrated luminescence of the GaAs quantum-wire structures does not degrade up to temperatures
as high as 400 K. This result is important for applications in light-emitting devices.

OPTICAL TRAPPING OF A METAL-PARTICLE AND A WATER DROPLET BY A

SCANNING LASER-BEAM
APPLIED PHYSICS LETTERS Vol 60, p807 (1992)
Laser trapping of a metal particle in water or a water droplet in liquid paraffin, which cannot be
attained by irradiation of a TEM00 mode focused laser beam, was experimentally confirmed based on
a scanning laser trapping technique. Although a metal particle or a water droplet experiences
repulsive radiation force from a laser beam (1064 nm, focused into a approximately 1-mu-m spot),
scanning of the laser beam circularly around the particle was successful to optically trap and tweezer
the particle. Water and ethylene glycol droplets dispersed in liquid paraffin were also shown to be
manipulated independently by scanning double laser-beam trapping.

BREAKING THE DIFFRACTION BARRIER - OPTICAL MICROSCOPY ON A

NANOMETRIC SCALE
SCIENCE Vol 251, p1468 (1991)
In near-field scanning optical microscopy, a light source or detector with dimensions less than the
wavelength (lambda) is placed in close proximity (< lambda/50) to a sample to generate images with
resolution better than the diffraction limit. A near-field probe has been developed that yields a
resolution of approximately 12 nm (approximately-lambda/43) and signals approximately 10(4)- to
10(6)-fold larger than those reported previously. In addition, image contrast is demonstrated to be
highly polarization dependent. With these probes, near-field microscopy appears poised to fulfill its
promise by combining the power of optical characterization methods with nanometric spatial
resolution.