Large Blue Shift of the Biexciton State in Tellurium Doped CdSe Colloidal Quantum Dots

The exciton−exciton interaction energy of tellurium doped CdSe colloidal quantum dots is experimentally investigated. The dots exhibit a strong Coulomb repulsion between the two excitons, which results in a huge measured biexciton blue shift of up to 300 meV. Such a strong Coulomb repulsion implies a very narrow hole wave function localized around the defect, which is manifested by a large Stokes shift. Moreover, we show that the biexciton blue shift increases linearly with the Stokes shift. This result is highly relevant for the use of colloidal QDs as optical gain media, where a large biexciton blue shift is required to obtain gain in the single exciton regime

Broadband Near-Infrared to Visible Upconversion in Quantum Dot–Quantum Well Heterostructures

Upconversion is a nonlinear process in which two, or more, long wavelength photons are converted to a shorter wavelength photon. It holds great promise for bioimaging, enabling spatially resolved imaging in a scattering specimen and for photovoltaic devices as a means to surpass the Shockley–Queisser efficiency limit. Here, we present dual near-infrared and visible emitting PbSe/CdSe/CdS nanocrystals able to upconvert a broad range of NIR wavelengths to visible emission at room temperature. The synthesis is a three-step process, which enables versatility and tunability of both the visible emission color and the NIR absorption edge. Using this method, one can achieve a range of desired upconverted emission peak positions with a suitable NIR band gap

Optical properties of spherulite opals

Spherulites are birefringent sturctures with spherical symmetry, which are typically observed in crystallized polymers. We compute the band structure of opals made of close-packed assemblies of highly birefringent spherulites. We demonstrate that spherulitic birefringence of constituent spheres does not affect the symmetries of an opal, and yet significantly affects the dispersion of eigenmodes, leading to new pseudogaps in sections of the band structure, and consequently enhanced reflectivity

Noninvasive linear fluorescence imaging through scattering media via wavefront shaping

We demonstrate focusing and imaging through a scattering medium noninvasively by using wavefront shaping. Our concept is based on utilizing the spatial fluorescence contrast which naturally exists in the hidden target object. By scanning the angle of incidence of the illuminating laser beam and maximizing the variation of the detected fluorescence signal from the object, as measured by a bucket detector at the front of the scattering medium, we are able to generate a tightly focused excitation spot. Thereafter, an image is obtained by scanning the focus over the object. The requirements for applicability of the method are discussed

Low Frequency Collinear Pre-Resonant Impulsive Stimulated Raman Spectroscopy

In this work we extend low frequency impulsive stimulated Raman microspectroscopy to the pre-electronic resonance regime. We use a broadband two color collinear pump probe scheme which can be readily extended to imaging. We discuss the difficulties unique to this type of measurements in the form of competing resonant two-photon processes and the means to overcome them. We successfully reduce the noise which arises due to those competing processes by eliminating the detected spectral components which do not contribute to the vibrational signature of the sample though introduce most of the noise. Finally, we demonstrate low-frequency spectroscopy of crystalline samples under near-resonant pumping showing both enhancement and spectral modification due to coupling with the electronic degree of freedom

How Quickly Does a Hole Relax into an Engineered Defect State in CdSe Quantum Dots

Intraband hole relaxation of colloidal Te-doped CdSe quantum dots is studied using state-selective transient absorption spectroscopy. The dots are excited at the band edge, and the defect band bleach caused by state filling of the hole is probed. Close to the defect energy, the hole relaxation is substantially slowed down, indicating a gap separating the defect state from the CdSe band edge. A clear dependence of the relaxation time with the QD’s size is presented, implying that the hole relaxation is mediated by longitudinal optical (LO) phonon modes of the CdSe host. In addition, we find that overcoating the quantum dots by two monolayers of a ZnS shell extends the hole relaxation time by a factor of 2, suggesting a combined effect of LO phonons and surface effects governing intraband hole relaxation

Media 1: Scanningless depth-resolved microscopy

Originally published in Optics Express on 07 March 2005 (oe-13-5-1468

Media 2: Scanningless depth-resolved microscopy

Originally published in Optics Express on 07 March 2005 (oe-13-5-1468

Temperature Dependence of Optical Gain in CdSe/ZnS Quantum Rods

We studied the optical gain characteristics of CdSe/ZnS core/shell colloidal quantum rods, investigated their temperature dependence, and compared the gain properties with quantum dots (QD). The gain was measured systematically for close-packed films of rods and dots under quasi-CW nanosecond optical pumping, using the variable stripe length method measuring the amplified spontaneous emission (ASE). Tunable ASE can be achieved by changing the rod diameter. Optical gain factors of up to 350 cm-1 at a temperature range of 10−120 K were measured for quantum rods. Above 120 K, the gain decreased sharply, but by increasing the pump power, ASE was easily achieved also at room temperature. The temperature dependence was assigned to the Auger heating process and phonon assisted thermal relaxation. QD of similar diameters as the rods showed much smaller gain values (∼50 cm-1) and a sharp decrease in gain at lowered temperatures (∼50 K), and ASE could not be detected at room temperature even at high pump powers. The significantly improved gain values in quantum rods as compared with dots were attributed to the slower Auger relaxation rates, the higher absorption cross-section, and the reduced self-absorption due to the larger Stokes shift. The temperature dependence of the threshold power for the quantum rods, used to characterize the thermal insensitivity of the system, showed two distinct temperature regions. In the low-temperature region, a very high T0 value of 3500 K was measured, as predicted for a low-dimensional quantum confined system