Cross Determination of Exciton Coherence Length in J-Aggregates.

The coherence length of the Frenkel excitons (Ncoh) is one of the most critical parameters governing many key features of supramolecular J-aggregates. Determining experimentally the value of Ncoh is a nontrivial task since it is sensitive to the technique/method applied, causing discrepancies in the literature data even for the same chemical compound and aggregation conditions. By using a combination of different experimental techniques including UV-vis-NIR, fluorescence emission, time-resolved photoluminescence, and transient absorption spectroscopies, we determined Ncoh values for J-aggregates of a cyanine dye. We found that the absorption spectroscopy alone - a widely used technique- fails in determining right value for Ncoh. The correct approach is based on the modification of photoluminescence lifetime and nonlinear response upon aggregation and careful analysis of the Stokes shift and electron-phonon coupling strength. This approach revealed that Ncoh of JC-1 J-aggregates ranges from 3 to 6.

Colloidal synthesis and optical properties of type-II CdSe-CdTe and inverted CdTe-CdSe core-wing heteronanoplatelets.

We developed colloidal synthesis to investigate the structural and electronic properties of CdSe-CdTe and inverted CdTe-CdSe heteronanoplatelets and experimentally demonstrate that the overgrowth of cadmium selenide or cadmium telluride core nanoplatelets with counterpartner chalcogenide wings leads to type-II heteronanoplatelets with emission energies defined by the bandgaps of the CdSe and CdTe platelets and the characteristic band offsets. The observed conduction and valence band offsets of 0.36 eV and 0.56 eV are in line with theoretical predictions. The presented type-II heteronanoplatelets exhibit efficient spatially indirect radiative exciton recombination with a quantum yield as high as 23%. While the exciton lifetime is strongly prolonged in the investigated type-II 2D systems with respect to 2D type-I systems, the occurring 2D giant oscillator strength (GOST) effect still leads to a fast and efficient exciton recombination. This makes type-II heteronanoplatelets interesting candidates for low threshold lasing applications and photovoltaics.

Resonance energy transfer in self-organized organic/inorganic dendrite structures.

Hybrid materials formed by semiconductor quantum dots and J-aggregates of cyanine dyes provide a unique combination of enhanced absorption in inorganic constituents with large oscillator strength and extremely narrow exciton bands of the organic component. The optical properties of dendrite structures with fractal dimension 1.7-1.8, formed from J-aggregates integrated with CdTe quantum dots (QDs), have been investigated by photoluminescence spectroscopy and fluorescence lifetime imaging microscopy. Our results demonstrate that (i) J-aggregates are coupled to QDs by Förster-type resonant energy transfer and (ii) there are energy fluxes from the periphery to the centre of the structure, where the QD density is higher than in the periphery of the dendrite. Such an anisotropic energy transport can be only observed when dendrites are formed from QDs integrated with J-aggregates. These QD/J-aggregate hybrid systems can have applications in light harvesting systems and optical sensors with extended absorption spectra.

The creation and annihilation of optical vortices using cascade conical diffraction.

Internal conical diffraction produces a superposition of orthogonally polarised zero- and first-order Bessel like beams from an incident circularly polarised Gaussian beam. For right-circularly polarised light, the first-order beam has an optical vortex of charge -1. Upon propagation of the first-order beam through a second biaxial crystal, a process which is termed cascade conical refraction, the generated beam is a superposition of orthogonally polarised fields of charge 0 and -1 or 0 and -2. This spin to orbital angular momentum conversion provides a new method for the generation and annihilation of optical vortices in an all-optical arrangement that is solely dependent on the incident polarisation and vortex handedness.

Generation of continuously tunable fractional optical orbital angular momentum using internal conical diffraction.

When a left-circularly polarised Gaussian light beam, which has spin angular momentum (SAM) J(sp) = sigmah = 1h per photon, is incident along one of the optic axes of a slab of biaxial crystal it undergoes internal conical diffraction and propagates as a hollow cone of light in the crystal. The emergent beam is a superposition of equal amplitude zero and first order Bessel like beams. The zero order beam is left-circularly polarised with zero orbital angular momentum (OAM) J(orb) = [see text]h = 0, while the first order beam is right-circularly polarized but carries OAM of J(orb) = 1h per photon. Thus, taken together the two beams have zero SAM and J(orb) = (1/2)h per photon. In this paper we examine internal conical diffraction of an elliptically polarised beam, which has fractional SAM, and demonstrate an all-optical process for the generation light beams with fractional OAM up to +/- 1h.

Conical diffraction of linearly polarised light controls the angular position of a microscopic object.

Conical diffraction of linearly polarised light in a biaxial crystal produces a beam with a crescent-shaped intensity profile. Rotation of the plane of polarisation produces the unique effect of spatially moving the crescent-shaped beam around a ring. We use this effect to trap microspheres and white blood cells and to position them at any angular position on the ring. Continuous motion around the circle is also demonstrated. This crescent beam does not require an interferometeric arrangement to form it, nor does it carry optical angular momentum. The ability to spatially locate a beam and an associated trapped object simply by varying the polarisation of light suggests that this optical process should find application in the manipulation and actuation of micro- and nano-scale physical and biological objects.

Conical diffraction and Bessel beam formation with a high optical quality biaxial crystal.

The manipulation of a Gaussian laser beam using conical diffraction in a high optical quality biaxial crystal of KGd(WO(4))(2) has been examined in detail with emphasis on the experimental techniques involved and intuitive explanations of the notable features. Two different optical arrangements were used to form the Pogendorff double-ring light pattern in the focal image plane. The formation of both diverging and non-diverging zeroth and first order Bessel beams was investigated. The various intensity distributions and polarization properties were measured and compared with the predictions of well-established theory.