Suitable labels are at the core of Luminescence and fluorescence imaging and sensing. One of the most exciting, yet also controversial, advances in label technology is the emerging development of quantum dots (QDs)--inorganic nanocrystals with unique optical and chemical properties but complicated surface chemistry--as in vitro and in vivo fluorophores. Here we compare and evaluate the differences in physicochemical properties of common fluorescent labels, focusing on traditional organic dyes and QDs. Our aim is to provide a better understanding of the advantages and limitations of both classes of chromophores, to facilitate label choice and to address future challenges in the rational design and manipulation of QD labels.

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Quantum dots versus organic dyes as fluorescent labels

The rise time of intense radiation determines the maximum field strength atoms can be exposed to before their polarizability dramatically drops due to the detachment of an outer electron. Recent progress in ultrafast optics has allowed the generation of ultraintense light pulses comprising merely a few field oscillation cycles. The arising intensity gradient allows electrons to survive in their bound atomic state up to external field strengths many times higher than the binding Coulomb field and gives rise to ionization rates comparable to the light frequency, resulting in a significant extension of the frontiers of nonlinear optics and (nonrelativistic) high-field physics. Implications include the generation of coherent harmonic radiation up to kiloelectronvolt photon energies and control of the atomic dipole moment on a subfemtosecond $(1{\mathrm{f}\mathrm{s}=10}^{\mathrm{\ensuremath{-}}15}\mathrm{}\mathrm{s})$ time scale. This review presents the landmarks of the 30-odd-year evolution of ultrashort-pulse laser physics and technology culminating in the generation of intense few-cycle light pulses and discusses the impact of these pulses on high-field physics. Particular emphasis is placed on high-order harmonic emission and single subfemtosecond extreme ultraviolet/x-ray pulse generation. These as well as other strong-field processes are governed directly by the electric-field evolution, and hence their full control requires access to the (absolute) phase of the light carrier. We shall discuss routes to its determination and control, which will, for the first time, allow access to the electromagnetic fields in light waves and control of high-field interactions with never-before-achieved precision.

Intense few-cycle laser fields: Frontiers of nonlinear optics

We stabilized the carrier-envelope phase of the pulses emitted by a femtosecond mode-locked laser by using the powerful tools of frequency-domain laser stabilization. We confirmed control of the pulse-to-pulse carrier-envelope phase using temporal cross correlation. This phase stabilization locks the absolute frequencies emitted by the laser, which we used to perform absolute optical frequency measurements that were directly referenced to a stable microwave clock.

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Carrier-envelope phase control of femtosecond mode-locked lasers and direct optical frequency synthesis

We review the field of femtosecond pulse shaping, in which Fourier synthesis methods are used to generate nearly arbitrarily shaped ultrafast optical wave forms according to user specification. An emphasis is placed on programmable pulse shaping methods based on the use of spatial light modulators. After outlining the fundamental principles of pulse shaping, we then present a detailed discussion of pulse shaping using several different types of spatial light modulators. Finally, new research directions in pulse shaping, and applications of pulse shaping to optical communications, biomedical optical imaging, high power laser amplifiers, quantum control, and laser-electron beam interactions are reviewed.

Femtosecond pulse shaping using spatial light modulators

Ultrafast lasers, which generate optical pulses in the picosecond and femtosecond range, have progressed over the past decade from complicated and specialized laboratory systems to compact, reliable instruments. Semiconductor lasers for optical pumping and fast optical saturable absorbers, based on either semiconductor devices or the optical nonlinear Kerr effect, have dramatically improved these lasers and opened up new frontiers for applications with extremely short temporal resolution (much smaller than 10 fs), extremely high peak optical intensities (greater than 10 TW/cm2) and extremely fast pulse repetition rates (greater than 100 GHz).

Recent developments in compact ultrafast lasers

A system that expands and recompresses an ultrashort pulse by means of diffraction gratings is described. The expansion can be large enough to broaden the pulse to several nanoseconds. In this manner, as the signal and pump pulses have similar lengths, high-efficiency amplifiers can be designed. The expansion avoids inefficient energy storage in high-gain amplifiers and nonlinear effects in the amplifier medium, and the amplified spontaneous emission is drastically reduced by working in a saturated amplifier regime.

Design of high-power ultrashort pulse amplifiers by expansion and recompression

A matrix formalism for grating and prism compressors is introduced. It is an extension of the standard ABCD matrix formalism for Gaussian optics, but includes the possibility of considering dispersive elements such as gratings and prisms. The full formation on the frequency-dependent phase shift is obtained to compute the time delay dispersion. The formalism simplifies the design of compressors with focusing optics. Information on beam divergence and astigmatism is also acquired. >

Matrix formalism for pulse compressors

A detailed analysis of a method of phase measurement of ultrashort light pulses is performed. It is shown that the output pulse of a zero dispersion compressor with a mask consisting of a narrow slit is a wide pulse delayed an amount equal to the phase derivative of the field spectrum with respect to frequency. State criteria to determine whether the approximations are valid are presented. The method is not affected by artifacts coming from diffraction effects in the slit or by the fact that only correlations are measured. The effects of the errors in positioning the elements are considered and minimized in the construction of the experimental apparatus. A novel technique for measurement of the derivative of the cross correlation is described, and it is used to locate the delayed output pulse. >

Analysis of a method of phase measurement of ultrashort pulses in the frequency domain

We generate an observable which relates the interspike time statistics in a noise driven excitable system with its phase space global properties. Experimental results from a semiconductor laser with optical feedback are analyzed within this framework.

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Interspike Time Distribution in Noise Driven Excitable Systems

The properties of a liquid crystal television to be used as a spatial modulator of the polarization of a laser beam are studied. It is found that the model most commonly used for the display description does not adequately reproduce the transmission through crossed polarizers. A new model is proposed that takes into account additional birefringence effects resulting from border effects near the television windows. With this correction, the anomalous behavior of the television is explained and the throughput for different configurations is properly predicted.

Oscar E. Martínez

Papers

Design of high-power ultrashort pulse amplifiers by expansion and recompression

Matrix formalism for pulse compressors

Analysis of a method of phase measurement of ultrashort pulses in the frequency domain

Interspike Time Distribution in Noise Driven Excitable Systems

Characterization of a liquid crystal television as a programmable spatial light modulator