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Applied Physics Letters

Excitation of a single molecule on the surface of a spherical microcavity

David J. Norris, Makoto Kuwata‐Gonokami, W. E. Moerner

Published Jul 21, 1997• 46 citations
Publisher

Abstract

We use the optical resonance of a spherical microcavity (quality factor ∼106) to excite a single molecule. By attaching a p-terphenyl crystal doped with pentacene and terrylene molecules to a dielectric sphere, we detect individual molecules excited by the near field of the cavity. A low-temperature optical microscope is utilized to image the emission from the single molecule, determine its position on the sphere surface, and measure its absorption linewidth. These results demonstrate the feasibility of single-molecule cavity quantum electrodynamics.

DOI
10.1063/1.119554

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We use the optical resonance of a spherical microcavity (quality factor ∼106) to excite a single molecule. By attaching a p-terphenyl crystal doped with pentacene and terrylene molecules to a dielectric sphere, we detect individual molecules excited by the near field of the cavity. A low-temperature optical microscope is utilized to image the emission from the single molecule, determine its position on the sphere surface, and measure its absorption linewidth. These results demonstrate the feasibility of single-molecule cavity quantum electrodynamics.
We describe recent results of experiments probing single molecules in the surface of spherical microcavities. Effects of spatial photoselection have been recently observed through changes in the single-molecule fluorescence photon statistics. In addition to being a sensitive probe of the highly interesting boundary region between classical and quantum mechanics, cavity-modified spontaneous emission and the possibility of single-molecule stimulated emission hold exciting promise as a means of exceeding sensitivity limitations such as photobleaching and absorption saturation in single molecule fluorescence detection. Ongoing efforts such as fluorescence imaging of single molecules on the surface of microspheres and attempts to observe single- molecule stimulated emission will also be described.
Single terrylene molecules embedded in microscopic p-terphenyl crystals are identified with the technique of fluorescence excitation spectroscopy. By use of the architecture of a scanning-probe microscope at T = 1.4 K , a single molecule is scanned through an excitation laser beam while the fluorescence signal is recorded. In this manner we have mapped the intensity distribution in a one-dimensional optical standing wave, demonstrating the potential of a single molecule as a nanometric probe. We discuss future experiments aimed at combining the high spatial and spectral sensitivity of a single molecule.
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.
Small volumes of a pentacene-doped p-terphenyl crystal are studied by fluorescence excitation. Excitation lines of single molecules of impurities are resolved, as is shown by the features of the single molecule lines and confirmed by the autocorrelation properties of the emitted light. Following the excitation lines as the temperature is changed, we observe various behaviors. In particular, one behavior is most simply explained by postulating a coupled two-level system in the molecule’s neighborhood.
Single molecules in suitable host crystals have been demonstrated to be useful single-photon emitters both at liquid-helium temperatures and at room temperature. The low-temperature source achieved controllable emission of single photons from a single terrylene molecule in p -terphenyl by an adiabatic rapid passage technique. In contrast with almost all other single-molecule systems, terrylene single molecules show extremely high photostability under continuous, high-intensity irradiation. A room-temperature source utilizing this material has been demonstrated, in which fast pumping into vibrational sidebands of the electronically excited state achieved efficient inversion of the emissive level. This source yielded a single-photon emission probability p (1) of 0.86 at a detected count rate near 300 000 photons s −1 , with very small probability of emission of more than one photon. Thus, single molecules in solids can be considered as contenders for applications of single-photon sources such as quantum key distribution.
The number density and orientation of molecules at the surface of a total-internal-reflection-ring minicavity are probed with extremely high sensitivity in a novel realization of the cavity ring-down optical absorption experiment. The modes of the ultralow-loss cavity, which are excited by photon tunneling, have long lifetimes that are sensitive to the presence of absorbing species in the evanescent field near a cavity facet. The total-internal-reflection-ring cavity extends cavity ring-down spectroscopy to surfaces and condensed matter, permitting a wide range of novel fundamental studies and applications. Routine single molecule detection may ultimately be feasible.