Fluorescence provides a mechanism for achieving contrast in biological imaging that enables investigations of molecular structure, dynamics, and function at high spatial and temporal resolution. Small-molecule organic fluorophores have proven essential for such efforts and are widely used in advanced applications such as single-molecule and super-resolution microscopy. Yet, organic fluorophores, like all fluorescent species, exhibit instabilities in their emission characteristics, including blinking and photobleaching that limit their utility and performance. Here, we review the photophysics and photochemistry of organic fluorophores as they pertain to mitigating such instabilities, with a specific focus on the development of stabilized fluorophores through derivatization. Self-healing organic fluorophores, wherein the triplet state is intramolecularly quenched by a covalently attached protective agent, exhibit markedly improved photostabilities. We discuss the potential for further enhancements towards the goal of developing “ultra-stable” fluorophores spanning the visible spectrum and how such fluorophores are likely to impact the future of single-molecule research.

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Ultra-stable organic fluorophores for single-molecule research

Organic solid-state lasers are reviewed, with a special emphasis on works published during the last decade. Referring originally to dyes in solid-state polymeric matrices, organic lasers also include the rich family of organic semiconductors, paced by the rapid development of organic light emitting diodes. Organic lasers are broadly tunable coherent sources are potentially compact, convenient and manufactured at low-costs. In this review, we describe the basic photophysics of the materials used as gain media in organic lasers with a specific look at the distinctive feature of dyes and semiconductors. We also outline the laser architectures used in state-of-the-art organic lasers and the performances of these devices with regard to output power, lifetime, and beam quality. A survey of the recent trends in the field is given, highlighting the latest developments in terms of wavelength coverage, wavelength agility, efficiency and compactness, or towards integrated low-cost sources, with a special focus on the great challenges remaining for achieving direct electrical pumping. Finally, we discuss the very recent demonstration of new kinds of organic lasers based on polaritons or surface plasmons, which open new and very promising routes in the field of organic nanophotonics.

Recent advances in solid-state organic lasers

Various models of a passively mode-locked quasi-continuous laser are discussed and the evolution of pulses in various cavity configurations is traced. In certain circumstances, the combined action of amplifier and absorber saturation is shown to lead to rapid pulse compression even when the pulse duration is far shorter than the relaxation time of either nonlinear component. The results are in good agreement with recent streak- camera measurements involving the pulsed Rhodamine 6G dye laser and satisfactorily explain the efficient generation of picosecond pulses in CW dye-laser systems. The same pulse-compression mechanism can probably be used to generate ultrashort pulses in other quasi-continuous lasers.

Pulse evolution in mode-locked quasi-continuous lasers

Organic solid-state lasers are reviewed, with a special emphasis on works published during the last decade. Referring originally to dyes in solid-state polymeric matrices, organic lasers also include the rich family of organic semiconductors, paced by the rapid development of organic light-emitting diodes. Organic lasers are broadly tunable coherent sources, potentially compact, convenient and manufactured at low cost. In this review, we describe the basic photophysics of the materials used as gain media in organic lasers with a specific look at the distinctive features of dyes and semiconductors. We also outline the laser architectures used in state-of-the-art organic lasers and the performances of these devices with regard to output power, lifetime and beam quality. A survey of the recent trends in the field is given, highlighting the latest developments in terms of wavelength coverage, wavelength agility, efficiency and compactness, and towards integrated low-cost sources, with a special focus on the great challenges remaining for achieving direct electrical pumping. Finally, we discuss the very recent demonstration of new kinds of organic lasers based on polaritons or surface plasmons, which open new and very promising routes in the field of organic nanophotonics. Copyright © 2011 Society of Chemical Industry

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Recent advances in solid‐state organic lasers

Fluorescence Behaviour of Highly Concentrated Rhodamine 6G Solutions

This paper describes the results of an investigation of the interrelated physical parameters that determine laser threshold for three organic dyes: rhodamine B, rhodamine 6G, and fluorescein. Not only are these dyes (rhodamine 6G in particular) among the most widely used and important laser dyes, but insights into the threshold condition derived from our studies of these particular dyes should be generally applicable to future dye laser research. Our detailed characterization of threshold for these dyes and our novel insights result from the use of triplet state spectral data in a thorough and quantitative way for the first time, coupled with the physically realistic approximation that the triplet population is proportional to the singlet excited state population. For the case of self‐tuning of the laser emission wavelength, solutions to the threshold equations are presented that establish relations between all the parameters affecting lasing: critical inversion, emission wavelength, extrinsic losses, dye concentration, length of active medium, and triplet to excited singlet population ratio. For reasonably high extrinsic cavity losses, the critical inversion is a simple power law function of extrinsic loss, and the emission wavelength is self‐tuned in such a manner that the ratio of extrinsic losses to intrinsic singlet absorption losses is substantially constant. There exists a region of low, but still physically realizable, cavity losses, where laser action is determined exclusively by intrinsic characteristics of the dyes (triplet absorption, singlet emission, and absorption). Asymptotic limits on the maximum wavelength of emission and on the minimum critical inversion appear in this region, beyond which there is no point in reducing extrinsic cavity losses. The fraction of triplet state molecules also determines long wavelength cutoffs for an externally tuned laser. Methods are outlined for measuring the ratio of triplet state to excited singlet state populations for dyes with known triplet absorption spectra and for determining semiquantitatively the triplet effects in dyes where this information is not known. A final interesting conclusion is that molecular modifications of rhodamine 6G cannot be expected to improve its threshold characteristics as a laser dye by much more than a factor of 4.

Organic Dye Laser Threshold

Triplet state kinetics for rhodamine 6G in alcohol have been studied. The singlet‐to‐triplet intersystem crossing rate kST and triplet lifetime τT have been determined in air‐saturated alcohol, where the spin‐forbidden decay from the triplet manifold into the singlet ground state is enhanced by collision with oxygen molecules dissolved in the solution. Values of the kinetic parameters for air‐saturated ethanol solutions at room temperature were determined to be τT = 250 ± 40nsec and kST = (3.4 ± 1.3) × 106sec−1.

J. P. Webb

Papers

Organic Dye Laser Threshold

Intersystem Crossing Rate and Triplet State Lifetime for a Lasing Dye