Near-field fluorescence microscopy of cells.

We demonstrate the surface sensitivity of near-field scanning optical microscopy by fluorescence imaging of membrane and bulk proteins in cells. We discuss instrument design considerations for successful cell-biology work with NSOM and show that the technique is most suited for studying membrane proteins.

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). We attribute the observed ultrafast collective ordering to the p-d exchange interaction between photoexcited holes and Mn spins, leading to a correlation-induced peak around 20 K and a transient increase in T(c).

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. Using a microscopic theory, we show that these are due to many-particle coherences created by interactions between photoexcited carriers and collective excitations of the 2D electron gas. We extract quantitative information about the dephasing and interference of these coherences.

Kilohertz-rate continuum generation by amplification of femtosecond pulses near 1.5 microm.

A NaCl color-center amplifier is used to amplify femtosecond pulses from an additive-pulse mode-locked laser at wavelengths between 1.52 and 1.60 microm. Pulse energies of several microjoules are obtained with pulse widths as short as 100 fs at kilohertz repetition rates. These pulses have been used to generate a continuum in a variety of solid and liquid media for hours without optical damage. The continuum generated in BaF(2) covers the wavelength range of 400 nm < lambda < 3.5 microm.

Mechanism for enhanced optical nonlinearities and bistability by combined dielectric-electronic confinement in semiconductor microcrystallites.

We propose a new type of mechanism for enhanced optical nonlinearities and intrinsic optical bistability that relies on the combination of intrinsic feedback due to local field effects and excitonic resonances in semiconductor crystallites. These effects will be further enhanced by quantum confinement in small crystallites.

Ultrafast dynamics of many-body processes and fundamental quantum mechanical phenomena in semiconductors.

The large dielectric constant and small effective mass in a semiconductor allows a description of its electronic states in terms of envelope wavefunctions whose energy, time, and length scales are mesoscopic, i.e., halfway between those of atomic and those of condensed matter systems. This property makes it possible to demonstrate and investigate many quantum mechanical, many-body, and quantum kinetic phenomena with tabletop experiments that would be nearly impossible in other systems. This, along with the ability to custom-design semiconductor nanostructures, makes semiconductors an ideal laboratory for experimental investigations. We present an overview of some of the most exciting results obtained in semiconductors in recent years using the technique of ultrafast nonlinear optical spectrocopy. These results show that Coulomb correlation plays a major role in semiconductors and makes them behave more like a strongly interacting system than like an atomic system. The results provide insights into the physics of strongly interacting systems that are relevant to other condensed matter systems, but not easily accessible in other materials.

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. For example, studies over the past decade have shown that Coulomb correlations between quasiparticles dominate the nonlinear optical response of semiconductors, in marked contrast to the behaviour of atomic systems. These Coulomb correlations and other many-body interactions are important not only for semiconductors, but also for all condensed-matter systems.

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. At low densities, excitons are Bose-particles, and at low temperatures, of the order of a few kelvin, excitons can form a quantum liquid -- that is, a statistically degenerate Bose gas or even a Bose-Einstein condensate. Here we report photoluminescence measurements of a quasi-two-dimensional exciton gas in GaAs/AlGaAs coupled quantum wells and the observation of a macroscopically ordered exciton state. Our spatially resolved measurements reveal fragmentation of the ring-shaped emission pattern into circular structures that form periodic arrays over lengths up to 1 mm.

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. Oscillatory spectral features below the excitonic resonance are observed in the response for counterpolarized beams. Comparison with model calculations shows that in this case the coherent nonlinearity is dominated by biexciton-exciton interactions beyond the Hartree-Fock approximation.

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. This effect originates from the many-body electron-hole correlations which determine the dynamical response of the Fermi sea.

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. Our results are the first rigorous solution concerning formation and decay of four-particle correlations in semiconductors. They are in excellent agreement with experimental data.

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. Understanding the formation mechanisms of these degenerate exciton systems can open new opportunities for the realization of Bose-Einstein condensation in the solid state.

Optical Stark effect on excitons in GaAs quantum wells.

We describe the first reported experimental observation of an extremely fast shift of the n = 1 exciton transition energy in GaAs quantum-well heterostructures. The shift is produced by optical pumping below the band gap and is not associated with a carrier or exciton population. We interpret the shift in terms of an optical Stark effect. We present a model for the Stark effect on the ground-state exciton in quantum wells and find good agreement between the predictions of the model and our experimental results.

Membrane specific mapping and colocalization of malarial and host skeletal proteins in the Plasmodium falciparum infected erythrocyte by dual-color near-field scanning optical microscopy.

Accurate localization of proteins within the substructure of cells and cellular organelles enables better understanding of structure-function relationships, including elucidation of protein-protein interactions. We describe the use of a near-field scanning optical microscope (NSOM) to simultaneously map and detect colocalized proteins within a cell, with superresolution. The system we elected to study was that of human red blood cells invaded by the human malaria parasite Plasmodium falciparum. During intraerythrocytic growth, the parasite expresses proteins that are transported to the erythrocyte cell membrane. Association of parasite proteins with host skeletal proteins leads to modification of the erythrocyte membrane. We report on colocalization studies of parasite proteins with an erythrocyte skeletal protein. Host and parasite proteins were selectively labeled in indirect immunofluorescence antibody assays. Simultaneous dual-color excitation and detection with NSOM provided fluorescence maps together with topography of the cell membrane with subwavelength (100 nm) resolution. Colocalization studies with laser scanning confocal microscopy provided lower resolution (310 nm) fluorescence maps of cross sections through the cell. Because the two excitation colors shared the exact same near-field aperture, the two fluorescence images were acquired in perfect, pixel-by-pixel registry, free from chromatic aberrations, which contaminate laser scanning confocal microscopy measurements. Colocalization studies of the protein pairs of mature parasite-infected erythrocyte surface antigen (MESA) (parasite)/protein4.1(host) and P. falciparum histidine rich protein (PfHRP1) (parasite)/protein4.1(host) showed good real-space correlation for the MESA/protein4.1 pair, but relatively poor correlation for the PfHRP1/protein4.1 pair. These data imply that NSOM provides high resolution information on in situ interactions between proteins in biological membranes. This method of detecting colocalization of proteins in cellular structures may have general applicability in many areas of current biological research.

Nonlinear optics with a diode-laser light source.

We report results of cw degenerate four-wave mixing experiments on room-temperature GaAs-GaAlAs multiple quantum-well material using a commercial semiconductor diode laser as the sole light source. With cw powers of ~3 mW and intensities of ~13 W/cm(2), we observe diffraction efficiencies of ~10(-4), corresponding to an effective nonlinear coefficient of chi(3)~6 x 10(-2) esu.

How fast is excitonic electroabsorption?

Many semiconductor light modulators rely on changes in excitonic absorption induced by electric fields. We study their temporal response in the framework of a one-dimensional model, for which we solve exactly the timedependent Schrödinger equation. For a homogeneously broadened system, the electroabsorption response time is found to be simply the inverse of the (field-induced) exciton linewidth, which can be as short as 50 fsec.

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. Oppositely charged electron and hole quasiparticles can coexist in an ionized but correlated plasma, or form bound hydrogen-like pairs called excitons. The pathways between such states, however, remain elusive in near-visible optical experiments that detect a subset of excitons with vanishing centre-of-mass momenta. In contrast, transitions between internal exciton levels, which occur in the far-infrared at terahertz (1012 s(-1)) frequencies, are independent of this restriction, suggesting their use as a probe of electron-hole pair dynamics. Here we employ an ultrafast terahertz probe to investigate directly the dynamical interplay of optically-generated excitons and unbound electron-hole pairs in GaAs quantum wells. Our observations reveal an unexpected quasi-instantaneous excitonic enhancement, the formation of insulating excitons on a 100-ps timescale, and the conditions under which excitonic populations prevail.

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. The resulting spots are accurately localized by fitting them to the known shape of the excitation point-spread function of the microscope. We present results of two-dimensional colocalization of TransFluoSpheres (40 nm in diameter) and of nanocrystals (3-10 nm in diameter) and demonstrate distance-measurement accuracy of better than 10 nm using conventional far-field optics. This ruler bridges the gap between fluorescence resonance energy transfer, near- and far-field imaging, spanning a range of a few nanometers to tens of micrometers.

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). Because the exciton mass is small--even smaller than the free electron mass--exciton BEC should occur at temperatures of about 1 K, many orders of magnitude higher than for atoms. However, it is in practice difficult to reach BEC conditions, as the temperature of excitons can considerably exceed that of the semiconductor lattice. The search for exciton BEC has concentrated on long-lived excitons: the exciton lifetime against electron-hole recombination therefore should exceed the characteristic timescale for the cooling of initially hot photo-generated excitons. Until now, all experiments on atom condensation were performed on atomic gases confined in the potential traps. Inspired by these experiments, and using specially designed semiconductor nanostructures, we have collected quasi-two-dimensional excitons in an in-plane potential trap. Our photoluminescence measurements show that the quasi-two-dimensional excitons indeed condense at the bottom of the traps, giving rise to a statistically degenerate Bose gas.

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.