When fluorescence from electronically excited states follows the absorption of radiation, the emission spectrum is often a key to identification of the excited species. It now emerges that passing off-resonant laser light through such an electronically excited system may enhance or suppress the fluorescent emission. This report establishes the mechanism and theory for this optical control of spontaneous fluorescence, derived by quantum electrodynamical analysis. Experimental techniques to detect the enhanced signal are also proposed.
When fluorescence from electronically excited states follows the absorption of radiation, the emission spectrum is often a key to identification of the excited species. It now emerges that passing off-resonant laser light through such an electronically excited system may enhance or suppress the fluorescent emission. This report establishes the mechanism and theory for this optical control of spontaneous fluorescence, derived by quantum electrodynamical analysis. Experimental techniques to detect the enhanced signal are also proposed.
We present a quantum electrodynamical procedure to demonstrate the all-optical control of molecular fluorescence. The effect is achieved on passage of an off-resonant laser beam through an optically activated system; the presence of a surface is not required. Following the derivation and analysis of the all-optical control mechanism, calculations are given to quantify the significant modification of spontaneous fluorescent emission with input laser irradiance. Specific results are given for molecules whose electronic spectra are dominated by transitions between three electronic levels, and suitable laser experimental methods are proposed. It is also shown that the phenomenon is sensitive to the handedness of circularly polarized throughput, producing a conferred form of optical activity.
In the optical excitation of many nanoscale systems, the primary result of photon absorption is an electronic excitation that is typically followed by ultrafast relaxation processes. The losses associated with such relaxation generally produce a partial degradation of the optical energy acquired, before any ensuing photon emission occurs. Recent work has shown that the intensity and directional character of such emission may be significantly influenced through engagement with a completely off-resonant probe laser beam of sufficient intensity: the mechanism for this optical coupling is a secondorder nonlinearity. It is anticipated that the facility to actively control fluorescent emission in this way may lead to new opportunities in a variety of applications where molecular chromophores or quantum dots are used. In the latter connection it should prove possible to exploit the particle size dependence of the nonlinear optical dispersion, as well as that of the emission wavelength. Specific characteristics of the effect are calculated, and suitable experimental implementations of the mechanism are proposed. We anticipate that this all-optical control device may introduce significant new perspectives to fluorescence imaging techniques and other analytical applications.
The ability to modify the character of fluorescent emission by a laser-controlled, optically nonlinear process has recently been shown theoretically feasible, and several possible applications have already been identified. In operation, a pulse of off-resonant probe laser beam, of sufficient intensity, is applied to a system exhibiting fluorescence, during the interval of excited-state decay following the initial excitation. The result is a rate of decay that can be controllably modified, the associated changes in fluorescence behavior affording new, chemically specific information. In this paper, a two-level emission model is employed in the further analysis of this all-optical process; the results should prove especially relevant to the analysis and imaging of physical systems employing fluorescent markers, these ranging from quantum dots to green fluorescence protein. Expressions are presented for the laser-controlled fluorescence anisotropy exhibited by samples in which the fluorophores are randomly oriented. It is also shown that, in systems with suitably configured electronic levels and symmetry properties, fluorescence emission can be produced from energy levels that would normally decay nonradiatively.
Multiphoton fluorescence microscopy is now a well-established technique, currently attracting much interest across all fields of biophysics - especially with regard to enhanced focal resolution. The fundamental mechanism behind the technique, identified and understood through the application of quantum theory, reveals new optical polarization features that can be exploited to increase the information content of images from biological samples. In another development, based on a newly discovered, fundamentally related mechanism, it emerges the passage of off-resonant probe laser pulses may characteristically modify the intensity of single-photon fluorescence, and its associated optical polarization behavior. Here, the probe essentially confers optical nonlinearity on the decay transition, affording a means of optical control over the fluorescent emission. Compared to a catalogue of other laser-based techniques widely used in the life sciences, most suffer limitations reflecting the exploitation of specifically lifetime-associated features; the new optical control mechanism promises to be more generally applicable for the determination of kinetic data. Again, there is a prospect of improving spatial resolution, non-intrusively. It is anticipated that tight directionality can be imposed on single-photon fluorescence emission, expediting the development of new imaging applications. In addition, varying the optical frequency of the probe beam can add another dimension to the experimental parameter space. This affords a means of differentiating between molecular species with strongly overlapping fluorescence spectra, on the basis of their differential nonlinear optical properties. Such techniques significantly extend the scope and the precision of spatial and temporal information accessible from fluorescence studies.
Spontaneous emission can be modified if the atom is driven by an external coherent field. Such modification include the three-peak spectrum of resonance fluorescence from a two level atom. The spectral line elimination and cancellation of spontaneous emission is possible under conditions that the spontaneous emission from an excited atom can be trapped in the upper states without decaying. The amount of fluorescence in this case as well as the population of the upper levels can be controlled. If spontaneous emission along with atomic transition is suppressed, it is possible to create a population in version on this transition by using a very weak incoherent pumping.
Introduction Previous discussions (see Section 10.4) suggested that stimulated emission can be used to generate optical gain, that is, to amplify radiation. The reader certainly has experience in the amplification of electronic signal. For example, radio receivers capture faint radio waves and turn them into a signal that is powerful enough to drive large speakers. This electronic amplification increases the amplitude of the signal while faithfully preserving its acoustic frequencies and modulation characteristics. Similarly, optical amplification is expected to increase the amplitude of an optical signal while preserving its frequency, its modulation characteristics, and its coherence. The latter requirement is of particular significance for optical radiation, where the coherence of naturally occurring radiation rarely exceeds one micrometer. Lasers are the primary source for coherent radiation. They depend on stimulated emission for amplification and for the generation of coherent radiation (the word laser is the acronym of Light Amplification by Stimulated Emission of Radiation). For amplification, an atomic system that is part of the laser medium must be prepared with a sufficiently large number of particles in the excited state. (The term atomic system is used here to describe all microscopic systems including molecules and free electrons.) Radiation passing through that excited medium encounters multiple events of stimulated emission, each event contributing one photon that is added coherently to the propagating beam. When the number of events of stimulated emission exceed all losses by absorption or scattering, the incident radiation is amplified.