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arXiv:2108.13943 · The Journal of Physical Chemistry A

Which Way Does Stimulated Emission Go?

J. David Wong-Campos, J. V. Porto, Adam E. Cohen

Published Nov 3, 2021• 7 citations
arXivHTMLPDF

Abstract

Is it possible to form an image using light produced by stimulated emission? Here we study light scatter off an assembly of excited chromophores. Due to the Optical Theorem, stimulated emission is necessarily accompanied by excited state Rayleigh scattering. Both processes can be used to form images, though they have different dependencies on scattering direction, wavelength and chromophore configuration. Our results suggest several new approaches to optical imaging using fluorophore excited states.

DOI
10.1021/acs.jpca.1c07713

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Is it possible to form an image using light produced by stimulated emission? Here we study light scatter off an assembly of excited chromophores. Due to the Optical Theorem, stimulated emission is necessarily accompanied by excited state Rayleigh scattering. Both processes can be used to form images, though they have different dependencies on scattering direction, wavelength and chromophore configuration. Our results suggest several new approaches to optical imaging using fluorophore excited states.
Stimulated emission into optical whispering modes of a spherical sample of CaF2{\mathrm{F}}_{2}F2​: Sm++{\mathrm{Sm}}^{++}Sm++ has been observed. Light produced by the stimulated emission is radiated tangentially form each point on the surface of the sphere. The experimental results have been interpreted in terms of the electromagnetic analog of the Rayleigh theory of the whispering gallery.
Stimulated emission (StE) remains relatively unused as an image-forming signal despite having potential advantages over fluorescence in speed, coherence, and ultimately resolution. Several ideas for the radiation pattern and directionality of StE remain prevalent, namely, whether a single molecule would radiate StE itself in a pure dipole pattern, or whether its emission direction depends on the driving field. Previous StE imaging has been carried out in transmission, which would collect signal either way. Here, we introduce the StE driving field (the probe) at an angle, using total internal reflection to avoid incident probe light and its specular reflections in our detection path. In this non-collinear detection configuration that also collects some fluorescence from the sample, we observe fluorescence depletion even in the spectral window where an increase in detected signal from StE would be expected if StE radiated like a simple classical dipole. Because simultaneous direct measurement of the fluorescence represents a calibration of the potential size of StE were it spatially patterned like a classical dipole emitter, our study clarifies a critical characteristic of StE for optimal microscope design, optical cooling, and applications using small arrays of emitters.
Zenodo hosts the archival version of this document; for convenient viewing, please visit andrewgyork.github.io/stimulated_emission_imaging Abstract Stimulated emission is often described as indistinguishable from the stimulating beam, sharing the same phase, frequency, polarization, and direction of travel. What direction does stimulated emission travel when the emitter is pointlike? Pointlike sources typically emit in all directions (a spherical wave), but if the stimulating beam is nearly monodirectional (a plane wave), will the stimulated emission propagate in all directions, or just one? We perform simple experiments to explore this apparent paradox, with an eye towards technological utility. In particular, does stimulated emission encode information about an emitter's location? Can lenses use this stimulated emission to form images of emitter distributions? If so, this suggests a way to combine the high signal rates of transmitted light microscopy with the specificity of fluorescence microscopy.
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.
The temporal dynamics of stimulated emission is studied, with particular emphasis on stimulated emission induced by x-ray pulses interacting with nuclei. In typical nuclear forward scattering experiments, the short incident x-ray pulse is accompanied by a huge number of off-resonant background photons. This prompts the question of whether stimulated emission can be observed in the delayed nuclear scattering signal which is emitted after the incident pulse has passed. We find that the stimulated photons essentially overlap with the stimulating pulse. To overcome this problem, we identify the reduction of the delayed scattered light intensity as an alternative signature for the stimulated emission. We further study a phase-sensitive variant of stimulated emission in the low-excitation regime, which provides convenient control parameters to facilitate the detection. Finally, we analyze the possibility of observing stimulated emission in nuclei driven by free electron lasers or synchrotron radiation sources.