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Optics Communications

On separation of diffusive broadening and homogeneous linewidth in spectrum of single molecule in solids

Taras Plakhotnik

Published Jan 1, 1996• 9 citations
Publisher
DOI
10.1016/0030-4018(95)00531-5

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The extraordinarily short optical dephasing time of organic dye molecules in polymer hosts is known to be under 20 fs between 100 and 200 K. Short dephasing times suggest enormously broadened homogeneous linewidths on the order of 10 nm. Direct observation of single dye molecule fluorescence spectra shows a similarly broadened line, giving comparable dephasing times for room temperature measurements. While this single molecule linewidth agrees with that of the bulk sample, it is inaccurate to attribute this broadening to homogeneous mechanisms. Repeated single molecule fluorescence measurements permit determination of the homogeneous nature of this linewidth, as distinct from the inhomogeneous nature of dispersion in bulk samples. Spectral diffusion in single molecule spectra is evidenced by multiple peaks, visible despite broad spectra lines at room temperature. In the particular experiment discussed in this thesis, fluorescence from single organic dye molecules in thin polymethyl methacrylate films was studied with scanning confocal microscopy. Photon antibunching exhibited by the photon-pair correlation function g(2) (τ) at τ = 0 confirms that single molecule emission spectra were obtained.

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Experimental data on Photon Echoes (PE) in the system terrylene/poly(isobutylene) in the temperature range 0.4–8K are presented and compared with Single Molecule Spectroscopy (SMS) results. From this comparison we conclude that the linewidth distribution in SMS is caused mainly by a large T 2-dispersion (but not slow spectral diffusion). The temperature line broadening is discussed.

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Inhomogeneous broadening of local vibrations in spectra of organic molecules in solid matrices

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Linewidths In Spectra Of Terrylene In Polyethylene Probed By Incoherent Photon Echo. Comparison With Single Molecule Spectroscopy Data

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The concept of the homogeneous spectral linewidth of an impurity center is more complicated in disordered media such as organic glasses and polymers than it is in crystals. In amorphous media the local environments for impurity centers are continuously changing with time. As a result transition frequencies of individual centers diffuse within the inhomogeneous broadened spectral contour, which is called spectral diffusion. When the timescale for spectral diffusion processes is much longer than the dephasing time, it is possible to distinguish homogeneous dephasing from spectral diffusion. On the other hand, when the timescales of spectral diffusion and dephasing processes are comparable these phenomena become indistinguishable.

Spectral Hole-Burning and Related Spectroscopies: Science and Applications•Jan 1, 1994•0 citations

On the radiative linewidth in single molecule spectroscopy

Inna Rebane

Optics and Spectroscopy•Oct 1, 1999•2 citations
The extraordinarily short optical dephasing time of organic dye molecules in polymer hosts is known to be under 20 fs between 100 and 200 K. Short dephasing times suggest enormously broadened homogeneous linewidths on the order of 10 nm. Direct observation of single dye molecule fluorescence spectra shows a similarly broadened line, giving comparable dephasing times for room temperature measurements. While this single molecule linewidth agrees with that of the bulk sample, it is inaccurate to attribute this broadening to homogeneous mechanisms. Repeated single molecule fluorescence measurements permit determination of the homogeneous nature of this linewidth, as distinct from the inhomogeneous nature of dispersion in bulk samples. Spectral diffusion in single molecule spectra is evidenced by multiple peaks, visible despite broad spectra lines at room temperature. In the particular experiment discussed in this thesis, fluorescence from single organic dye molecules in thin polymethyl methacrylate films was studied with scanning confocal microscopy. Photon antibunching exhibited by the photon-pair correlation function g(2) (τ) at τ = 0 confirms that single molecule emission spectra were obtained.
The concept of the homogeneous spectral linewidth of an impurity center is more complicated in disordered media such as organic glasses and polymers than it is in crystals. In amorphous media the local environments for impurity centers are continuously changing with time. As a result transition frequencies of individual centers diffuse within the inhomogeneous broadened spectral contour, which is called spectral diffusion. When the timescale for spectral diffusion processes is much longer than the dephasing time, it is possible to distinguish homogeneous dephasing from spectral diffusion. On the other hand, when the timescales of spectral diffusion and dephasing processes are comparable these phenomena become indistinguishable.