Time-gated biological imaging by use of colloidal quantum dots.

The long (but not too long) fluorescence lifetime of CdSe semiconductor quantum dots was exploited to enhance fluorescence biological imaging contrast and sensitivity by time-gated detection. Significant and selective reduction of the autofluorescence contribution to the overall image was achieved, and enhancement of the signal-to-background ratio by more than an order of magnitude was demonstrated.

Ultrafast enhancement of ferromagnetism via photoexcited holes in GaMnAs.

We report on the observation of ultrafast photoenhanced ferromagnetism in GaMnAs. It is manifested as a transient magnetization increase on a 100 ps time scale, after an initial subpicosecond demagnetization. The dynamic magnetization enhancement exhibits a maximum below the Curie temperature T(c) and dominates the demagnetization component when approaching T(c).

Ultrabroadband 50-130 THz pulses generated via phase-matched difference frequency mixing in LiIO(3).

We report the generation of ultrabroadband pulses spanning the 50-130 THz frequency range via phase-matched difference frequency mixing within the broad spectrum of sub-10 fs pulses in LiIO(3). Model calculations reproduce the octave-spanning spectra and predict few-cycle THz pulse durations less than 20 fs. The broad applicability of this scheme is demonstrated with 9-fs pulses from a Ti:sapphire oscillator and with 7-fs amplified pulses from a hollow fiber compressor as pump sources.

Ultrafast dynamics of coherences in a quantum Hall system.

Using three-pulse four-wave-mixing optical spectroscopy, we study the ultrafast dynamics of the quantum Hall system. We observe striking differences as compared to an undoped system, where the 2D electron gas is absent. In particular, we observe a large off-resonant signal with strong oscillations.

Stimulated terahertz emission from intraexcitonic transitions in Cu2O.

We report the first observation of stimulated emission of terahertz radiation from internal transitions of excitons. The far-infrared electromagnetic response of Cu2O is monitored via broadband terahertz pulses after ultrafast resonant excitation of three-dimensional 3p excitons. Stimulated emission from the 3p to the energetically lower 2s bound level occurs at a photon energy of 6.

Formation mechanism and low-temperature instability of exciton rings.

The macroscopic rings observed in the photoluminescence patterns of excitons in coupled quantum wells are explained by a mechanism of carrier imbalance, transport, and recombination. The rings originate from the spatial separation of p and n carriers, and occur at the interface of the p and n domains, where excitons are generated. We explore the states of excitons in the ring over a range of temperatures down to 380 mK and report a transition of the ring into a periodic array of aggregates, a new low-temperature ordered exciton state.

Phase diagram of degenerate exciton systems.

Degenerate exciton systems have been produced in quasi-two-dimensional confined areas in semiconductor coupled quantum well structures. We observed contractions of clouds containing tens of thousands of excitons within areas as small as (10 micron)2 near 10 kelvin. The spatial and energy distributions of optically active excitons were determined by measuring photoluminescence as a function of temperature and laser excitation and were used as thermodynamic quantities to construct the phase diagram of the exciton system, which demonstrates the existence of distinct phases.

Ultrafast terahertz probes of transient conducting and insulating phases in an electron-hole gas.

Many-body systems in nature exhibit complexity and self-organization arising from seemingly simple laws. For example, the long-range Coulomb interaction between electrical charges has a simple form, yet is responsible for a plethora of bound states in matter, ranging from the hydrogen atom to complex biochemical structures. Semiconductors form an ideal laboratory for studying many-body interactions of electronic quasiparticles among themselves and with lattice vibrations and light.

Dynamics of inter-landau-level excitations of a two-dimensional electron gas in the quantum Hall regime.

The femtosecond inter-Landau-level dynamics of a two-dimensional electron gas in a large magnetic field is investigated by degenerate four-wave mixing on modulation doped quantum wells. We observe a large transfer of oscillator strength to the lowest Landau level, and unusual dynamics due to Coulomb correlation. We interpret the effects using a model based on shakeup of the electron gas.

Macroscopically ordered state in an exciton system.

There is a rich variety of quantum liquids -- such as superconductors, liquid helium and atom Bose-Einstein condensates -- that exhibit macroscopic coherence in the form of ordered arrays of vortices. Experimental observation of a macroscopically ordered electronic state in semiconductors has, however, remained a challenging and relatively unexplored problem. A promising approach for the realization of such a state is to use excitons, bound pairs of electrons and holes that can form in semiconductor systems.

Towards Bose-Einstein condensation of excitons in potential traps.

An exciton is an electron-hole bound pair in a semiconductor. In the low-density limit, it is a composite Bose quasi-particle, akin to the hydrogen atom. Just as in dilute atomic gases, reducing the temperature or increasing the exciton density increases the occupation numbers of the low-energy states leading to quantum degeneracy and eventually to Bose-Einstein condensation (BEC).

Far-infrared optical conductivity gap in superconducting MgB2 films.

We report the first study of the optical conductivity of MgB2 covering the range of its lowest-energy superconducting gap. Terahertz time-domain spectroscopy is utilized to determine the complex, frequency-dependent conductivity sigma(omega) of thin films. The imaginary part reveals an inductive response due to the emergence of the superconducting condensate.

Observation of magnetically induced effective-mass enhancement of quasi-2D excitons.

We present the first measurements of the dispersion relation of a quasi-2D magnetoexciton. We demonstrate that the magnetoexciton effective mass is determined by the coupling between the center-of-mass motion and internal structure and becomes overwhelmingly larger than the sum of the electron and hole masses in high magnetic fields.

Parity-forbidden excitations of Sr(2)CuO(2)Cl(2) revealed by optical third-harmonic spectroscopy.

We present the first study of nonlinear optical third-harmonic generation (THG) in the strongly correlated charge-transfer insulator Sr(2)CuO(2)Cl(2). For fundamental excitation in the near infrared, the THG spectrum reveals a strongly resonant response for photon energies near 0.7 eV.

Monitoring the conformational fluctuations of DNA hairpins using single-pair fluorescence resonance energy transfer.

We present single-pair fluorescence resonance energy transfer (spFRET) observations of individual opening and closing events of surface-immobilized DNA hairpins. Two glass-surface immobilization strategies employing the biotin-streptavidin interaction and a third covalent immobilization strategy involving formation of a disulfide bond to a thiol-derivatized glass surface are described and evaluated. Results from image and time-trace data from surface-immobilized molecules are compared with those from freely diffusing molecules, which are unperturbed by surface interactions.

Many-body and correlation effects in semiconductors.

Solids consist of 1022-1023 particles per cubic centimetre, interacting through infinite-range Coulomb interactions. The linear response of a solid to a weak external perturbation is well described by the concept of non-interacting 'quasiparticles' first introduced by Landau. But interactions between quasiparticles can be substantial in dense systems.

Ratiometric single-molecule studies of freely diffusing biomolecules.

We outline recent developments in biological single-molecule fluorescence detection with particular emphasis on observations by ratiometric fluorescence resonance energy transfer (FRET) of biomolecules freely diffusing in solution. Single-molecule-diffusion methodologies were developed to minimize perturbations introduced by interactions between molecules and surfaces. Confocal microscopy is used in combination with sensitive detectors to observe bursts of photons from fluorescently labeled biomolecules as they diffuse through the focal volume.

From coherently excited highly correlated states to incoherent relaxation processes in semiconductors.

Recent theories of highly excited semiconductors are based on two formalisms, referring to complementary experimental conditions, the real-time nonequilibrium Green's function techniques and the coherently controlled truncation of the many-particle problem. We present a novel many-particle theory containing both of these methods as limiting cases. As a first example of its application, we investigate four-particle correlations in a strong magnetic field including dephasing resulting from the growth of incoherent one-particle distribution functions.

Ultrahigh-resolution multicolor colocalization of single fluorescent nanocrystals.

A new method for and possibly ultrahigh-resolution colocalization and distance measurement between biomolecules is described, based on semiconductor nanocrystal probes. This ruler bridges the gap between FRET and far-field (or near-field scanning optical microscope) imaging and has a dynamic range from few nanometers to tens of micrometers. The ruler is based on a stage-scanning confocal microscope that allows the simultaneous excitation and localization of the excitation point-spread-function (PSF) of various colors nanocrystals while maintaining perfect registry between the channels.

Unified picture of polariton propagation in bulk GaAs semiconductors.

High-resolution amplitude and phase linear spectroscopy of high-quality bulk GaAs are reported. The detailed structure of the observed full complex transmission is consistently explained by polariton effects on the basis of microscopic calculations. The coupled equations for the excitonic polarization and the light field in the slab configuration are evaluated using appropriate boundary conditions for the electromagnetic field and the excitonic wave function without reference to additional boundary conditions for the macroscopic polarization.

Femtosecond coherent dynamics of the fermi-edge singularity and exciton hybrid.

We study theoretically the coherent nonlinear optical response of doped quantum wells with several subbands. When the Fermi energy approaches the exciton level of an upper subband, the absorption spectrum acquires a characteristic double-peak shape originating from the interference between the Fermi-edge singularity and the exciton resonance. We demonstrate that, for off-resonant pump excitation, the pump-probe spectrum undergoes a striking transformation, with a time-dependent exchange of oscillator strength between the Fermi-edge singularity and exciton peaks.

Polariton-biexciton transitions in a semiconductor microcavity.

The influence of four-particle correlations on the nonlinear optics of a semiconductor microcavity is determined by a pump-and-probe investigation. Experiments are performed on a nonmonolithic microcavity which contains a ZnSe quantum well. In this system the biexciton binding energy exceeds both the normal-mode splitting between exciton and cavity mode and all damping constants.

Demonstration of sixth-order coulomb correlations in a semiconductor single quantum well.

Six-wave mixing in a ZnSe quantum well is investigated and compared with microscopic theory. We demonstrate that sixth-order Coulomb correlations have a significant qualitative impact on the nonlinear optical response. Six-wave mixing is shown to be a uniquely sensitive tool for investigation of correlations beyond the four-point level.

Ultrahigh-resolution multicolor colocalization of single fluorescent probes.

An optical ruler based on ultrahigh-resolution colocalization of single fluorescent probes is described in this paper. It relies on the use of two unique families of fluorophores, namely energy-transfer fluorescent beads (TransFluoSpheres) and semiconductor nanocrystal quantum dots, that can be excited by a single laser wavelength but emit at different wavelengths. A multicolor sample-scanning confocal microscope was constructed that allows one to image each fluorescent light emitter, free of chromatic aberrations, by scanning the sample with nanometer scale steps with a piezo-scanner.

Single-molecule protein folding: diffusion fluorescence resonance energy transfer studies of the denaturation of chymotrypsin inhibitor 2.

We report single-molecule folding studies of a small, single-domain protein, chymotrypsin inhibitor 2 (CI2). CI2 is an excellent model system for protein folding studies and has been extensively studied, both experimentally (at the ensemble level) and theoretically. Conformationally assisted ligation methodology was used to synthesize the proteins and site-specifically label them with donor and acceptor dyes.