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Laser Physics

The single-molecule dye laser

Zhen Wang, HERSCHEL A. RABITZ, Marlan O. Scully

Published Jan 1, 2005• 4 citations
OpenAlex

Abstract

This work explores the feasibility of inducing lasing action in a single dye molecule using an optical microcavity. A single-molecule light source is proposed, in which a microcavity-coupled dye molecule is pumped by multiple energy donors via an intermolecular resonance energy transfer mechanism. A quantitative model based on realistic parameters for microcavities and for organic dyes shows that stimulated emission may become dominant over spontaneous fluorescence under optimal yet technically reachable conditions, suggesting the likelihood of achieving a single-molecule lasing photon source with the proposed device. Lasing of a single dye molecule generates signals much brighter than spontaneous fluorescence, and may find applications in a wide range of fields from physics and chemistry to biology.

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Science•Oct 27, 2000•355 citations
This work explores the feasibility of inducing lasing action in a single dye molecule using an optical microcavity. A single-molecule light source is proposed, in which a microcavity-coupled dye molecule is pumped by multiple energy donors via an intermolecular resonance energy transfer mechanism. A quantitative model based on realistic parameters for microcavities and for organic dyes shows that stimulated emission may become dominant over spontaneous fluorescence under optimal yet technically reachable conditions, suggesting the likelihood of achieving a single-molecule lasing photon source with the proposed device. Lasing of a single dye molecule generates signals much brighter than spontaneous fluorescence, and may find applications in a wide range of fields from physics and chemistry to biology.
Motivated by the recent progresses in one-atom laser and single-molecule manipulation, this work presents the model and simulations of a single dye molecule laser device, which consists of a single dye molecule as an acceptor in a microcavity pumped by multiple donors via the intermolecular resonance energy transfer mechanism. The photon intensity is calculated at the emission peaks of donor and acceptor dyes for different pump rates and donor numbers. Finally, it is demonstrated that stimulated emission gains a distinct advantage over spontaneous emission under appropriate conditions. This work would have many important applications in a wide range of fields from physics and chemistry to nanotechnology in future.
A significant limitation in the detection and spectroscopy of individual dye molecules in liquid room temperature samples is the loss of fluorescence signal through chromophore photobleaching. Although often considered a fundamental restriction on sensitivity, it has been shown that the probability per excitation cycle of photobleaching may be reduced by enhancing the spontaneous emission rate of the chromophore located inside a microdroplet, which acts as a optical cavity. Studies of glycerol microdroplets containing R6G dye molecules, and levitated in a three-dimensional electrodynamic trap, have demonstrated a significant enhancement of both the fluorescence decay rate [1] and the total fluorescence yield [2] of the chromophore. Modification of the emission rate is greatest for molecules located near the surface of small (< 10 μm) microdroplets, where the influence of the droplet cavity modes of the droplet is most significant. To exploit this surface sensitivity, surfactant forms of rhodamine dyes were recently studied [3]. Fluorescence emission of the dye molecules, constrained to the droplet surface and with fixed transition moments perpendicular to the surface normal, were shown to be significantly enhanced at small droplet sizes. Additionally, at larger droplet sizes corresponding to higher droplet Q’s, preferential emission into the cavity modes was observed, however the detection of fluorescence photons was delayed by the storage time of the cavity, which may be on the same order as the fluorescence lifetime. These measurements, performed on relatively concentrated dye solutions, suggest that microcavity effects may be exploited to greatly enhance single molecule detection sensitivity in glycerol microdroplets. Furthermore, the large cavity storage time of the high-Q droplets opens the possibility for re-excitation of the molecule following emission into the droplet resonance, and subsequent stimulated emission, that is, single-molecule lasing.
The spontaneous emission from a thin layer of a dilute solution of fluorescent dye molecules within an optical microcavity has been studied. Strong fluctuations in fluorescence intensity are observed when the average number of molecules in the measurement volume is small. We have performed experiments that simultaneously characterize these fluctuations over nine orders of magnitude of time, from ns to s. These measurements have identified photon antibunching characteristic of single-molecule emission, along with triplet-state shelving and diffusion driven number fluctuations. The results give fundamental information on the kinetics of dye molecules and allow one to speculate about the prospect of using single molecules as sources of single photons for quantum optics.
We investigate experimentally and theoretically the fluorescence emitted by molecular ensembles as well as spatially isolated, single molecules of an organic dye immobilized in a quasi-planar optical microresonator at room temperature. The optically excited dipole emitters couple simultaneously to on- and off-axis cavity resonances of the microresonator. The multi-spectral radiative contributions are strongly modified with respect to free (non-confined) space due to enhancement and inhibition of the molecular spontaneous emission (SpE) rate. By varying the mirror spacing of the microresonator on the nanometer-scale, the SpE rate of the cavity-confined molecules and, consequently, the spectral line width of the microresonator-controlled broadband fluorescence can be tuned by up to one order of magnitude. Stepwise reducing the optical confinement, we observe that the microresonator-controlled molecular fluorescence line shape converges towards the measured fluorescence line shape in free space. Our results are important for research on and application of broadband emitters in nano-optics and -photonics as well as microcavity-enhanced (single molecule) spectroscopy.
Dynamic structural changes of macromolecules undergoing biochemical reactions can be studied using a novel single pair fluorescence resonance energy transfer (sp-FRET) tool which can be used as a nanoscale spectroscopic ruler. Although recent advances in applying such a nanoscale ruler to biological systems have been made, improvements in photon detectors and photophysical properties of the single FRET pair are still being studied. Motivated by the recent progresses in single-atom laser, we have investigated the ability to use the optical microcavity to amplify the sp-FRET signal. When the single FRET pair and the attached macromolecule of interest are placed inside an optical cavity with the emission mode of the acceptor dye in resonance with the cavity mode, quantitative modeling shows that, when adjusting the acceptor-cavity coupling parameters to be appropriate values, the acceptor fluorescence emission signal amplified by the cavity coupling mode would reach a significant value, leading to a much brighter sp-FRET spectroscopic signal. Possible applications to sp-FRET measurement of biological molecules are quantitatively examined.
By studying the transfer of excitation energy between dye molecules confined within an optical microcavity, we demonstrate experimentally that Förster energy transfer is influenced by the local photonic mode density. Locating donor and acceptor molecules at well-defined positions allows the transfer rate to be determined as a function of both mutual separation and cavity length. The results show that the Förster transfer rate depends linearly on the donor emission rate and hence photonic mode density, providing the potential to control energy transfer by modification of the optical environment.