Nanocrystals are fundamental to modern science and technology. Mastery over the shape of a nanocrystal enables control of its properties and enhancement of its usefulness for a given application. Our aim is to present a comprehensive review of current research activities that center on the shape-controlled synthesis of metal nanocrystals. We begin with a brief introduction to nucleation and growth within the context of metal nanocrystal synthesis, followed by a discussion of the possible shapes that a metal nanocrystal might take under different conditions. We then focus on a variety of experimental parameters that have been explored to manipulate the nucleation and growth of metal nanocrystals in solution-phase syntheses in an effort to generate specific shapes. We then elaborate on these approaches by selecting examples in which there is already reasonable understanding for the observed shape control or at least the protocols have proven to be reproducible and controllable. Finally, we highlight a number of applications that have been enabled and/or enhanced by the shape-controlled synthesis of metal nanocrystals. We conclude this article with personal perspectives on the directions toward which future research in this field might take.

Shape‐Controlled Synthesis of Metal Nanocrystals: Simple Chemistry Meets Complex Physics?

We review the basic physics of surface-plasmon excitations occurring at metal/dielectric interfaces with special emphasis on the possibility of using such excitations for the localization of electromagnetic energy in one, two, and three dimensions, in a context of applications in sensing and waveguiding for functional photonic devices. Localized plasmon resonances occurring in metallic nanoparticles are discussed both for single particles and particle ensembles, focusing on the generation of confined light fields enabling enhancement of Raman-scattering and nonlinear processes. We then survey the basic properties of interface plasmons propagating along flat boundaries of thin metallic films, with applications for waveguiding along patterned films, stripes, and nanowires. Interactions between plasmonic structures and optically active media are also discussed.

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Plasmonics: Localization and guiding of electromagnetic energy in metal/dielectric structures

The history, fabrication, theory, numerical modeling, optical properties, guidance mechanisms, and applications of photonic-crystal fibers are reviewed

Photonic-Crystal Fibers

In this work, we use dark-field microscopy to observe a new plasmon resonance effect for a single silver nanocube in which the plasmon line shape has two distinct peaks when the particles are located on a glass substrate. The dependence of the resonance on nanocube size and shape is characterized, and it is found that the bluer peak has a higher figure of merit for chemical sensing applications than that for other particle shapes that have been studied previously. Comparison of the measured results with finite difference time domain (FDTD) electrodynamics calculations enables us to confirm the accuracy of our spectral assignments.

Localized surface plasmon resonance spectroscopy of single silver nanocubes

The absorption and emission properties of transition metal (TM)-doped zinc chalcogenides have been investigated to understand their potential application as room-temperature, mid-infrared tunable laser media. Crystals of ZnS, ZnSe, and ZnTe, individually doped with Cr/sup 2+/, Co/sup 2+/, Ni/sup 2+/, or Fe/sup 2+/ have been evaluated. The absorption and emission properties are presented and discussed in terms of the energy levels from which they arise. The absorption spectra of the crystals studied exhibit strong bands between 1.4 and 2.0 /spl mu/m which overlap with the output of strained-layer InGaAs diodes. The room-temperature emission spectra reveal wide-band emissions from 2-3 /spl mu/m for Cr and from 2.8-4.0 /spl mu/m for Co, Cr luminesces strongly at room temperature; Co exhibits significant losses from nonradiative decay at temperatures above 200 K, and Ni and Fe only luminesce at low temperatures, Cr/sup 2+/ is estimated to have the highest quantum yield at room temperature among the media investigated with values of /spl sim/75-100%. Laser demonstrations of Cr:ZnS and Cr:ZnSe have been performed in a laser-pumped laser cavity with a Co:MgF/sub 2/ pump laser. The output of both lasers were determined to peak at wavelengths near 2.35 /spl mu/m, and both lasers demonstrated a maximum slope efficiency of approximately 20%. Based on these initial results, the Cr/sup 2+/ ion is predicted to be a highly favorable laser ion for the mid-IR when doped into the zinc chalcogenides; Co/sup 2+/ may also serve usefully, but laser demonstrations yet remain to be performed.

Transition metal-doped zinc chalcogenides: Spectroscopy and laser demonstration of a new class of gain media

Spectroscopic properties and laser performance of Yb-doped tungstates at pulsed Ti:sapphire laser pumping are reported. Room-temperature lasing near 1025  nm is demonstrated in Yb:KY(WO4)2 and Yb:KGd(WO4)2, with a slope efficiency as great as 86.9%.

Pulsed laser operation of Yb-doped KY(WO 4 ) 2 and KGd(WO 4 ) 2

Efficient continuous-wave laser operation of Cr2+:ZnSe was demonstrated with an output power of 1400 mW at an absorbed pump power of 1900 mW from a Tm:YAG laser. Under continuous-wave diode pumping at 1.54 μm an output power of 15 mW was obtained from a Cr+2:ZnSe laser. Excited state absorption is shown to be negligible in the pump and laser spectral region.

Efficient laser operation and continuous-wave diode pumping of Cr2+:ZnSe single crystals

Passive Q switching of Er:glass lasers has been demonstrated with Cr2+:ZnSe and Co2+:ZnSe saturable absorbers. A pulse duration of ?50 ns and an output pulse energy of 5 mJ were obtained with both Co:ZnSe and Cr:ZnSe passive shutters. A Q-switched conversion efficiency of as much as 26% was obtained for Cr:ZnSe. Theoretical modeling exhibits satisfactory agreement with experimental data.

Cr(2+):ZnSe and Co(2+):ZnSe saturable-absorber Q switches for 1.54-mum Er:glass lasers.

Three-dimensional, permanent anisotropic modifications in glass containing spherical Ag nanoparticles are demonstrated using multicolor fs laser irradiation. The method can produce dichroism by deformation of nanoparticles to oblong shapes oriented parallel to the laser polarization. Using samples with a vertical gradient of the fill factor of Ag nanoparticles in the glass substrate and an accordingly inhomogeneous broadening of the surface plasmon band, modifications in various depths can be made using different excitation wavelengths. The induced modifications are reversible: heating to ≈600 °C restores the spherical shape of Ag nanoparticles. This technique could be used in manufacturing of different, 3D, polarization and wavelength selective micro-devices such as polarizers, filters, gratings, display and rewriting optical 3D data storage devices.

Femtosecond laser assisted production of dichroitic 3D structures in composite glass containing Ag nanoparticles

We present a spectrally decorrelated photon pair source bridging the visible and telecom wavelength regions. Tailored design and fabrication of a solid-core photonic crystal fiber (PCF) lead to the emission of signal and idler photons into only a single spectral and spatial mode. Thus no narrowband filtering is necessary and the heralded generation of pure photon number states in ultrafast wave packets at telecom wavelengths becomes possible.

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Alexander Podlipensky

Papers

Pulsed laser operation of Yb-doped KY(WO 4 ) 2 and KGd(WO 4 ) 2

Efficient laser operation and continuous-wave diode pumping of Cr2+:ZnSe single crystals

Cr(2+):ZnSe and Co(2+):ZnSe saturable-absorber Q switches for 1.54-mum Er:glass lasers.

Femtosecond laser assisted production of dichroitic 3D structures in composite glass containing Ag nanoparticles

Bridging visible and telecom wavelengths with a single-mode broadband photon pair source