We present an experimental and theoretical study of the fluorescence rate of a single molecule as a function of its distance to a laser-irradiated gold nanoparticle. The local field enhancement leads to an increased excitation rate whereas nonradiative energy transfer to the particle leads to a decrease of the quantum yield (quenching). Because of these competing effects, previous experiments showed either fluorescence enhancement or fluorescence quenching. By varying the distance between molecule and particle we show the first experimental measurement demonstrating the continuous transition from fluorescence enhancement to fluorescence quenching. This transition cannot be explained by treating the particle as a polarizable sphere in the dipole approximation.

https://www.photonics.ethz.ch/fileadmin/user_upload/FILES2SHARE/anger06a.pdf

Enhancement and quenching of single-molecule fluorescence.

Cavity quantum electrodynamics, a central research field in optics and solid-state physics, addresses properties of atom-like emitters in cavities and can be divided into a weak and a strong coupling regime. For weak coupling, the spontaneous emission can be enhanced or reduced compared with its vacuum level by tuning discrete cavity modes in and out of resonance with the emitter. However, the most striking change of emission properties occurs when the conditions for strong coupling are fulfilled. In this case there is a change from the usual irreversible spontaneous emission to a reversible exchange of energy between the emitter and the cavity mode. This coherent coupling may provide a basis for future applications in quantum information processing or schemes for coherent control. Until now, strong coupling of individual two-level systems has been observed only for atoms in large cavities. Here we report the observation of strong coupling of a single two-level solid-state system with a photon, as realized by a single quantum dot in a semiconductor microcavity. The strong coupling is manifest in photoluminescence data that display anti-crossings between the quantum dot exciton and cavity-mode dispersion relations, characterized by a vacuum Rabi splitting of about 140 microeV.

/pdf/strong-coupling-in-a-single-quantum-dot-semiconductor-48bgjfnp5v.pdf

Strong coupling in a single quantum dot–semiconductor microcavity system

Optical approaches for observing the dynamics of single molecules have required pico- to nanomolar concentrations of fluorophore in order to isolate individual molecules. However, many biologically relevant processes occur at micromolar ligand concentrations, necessitating a reduction in the conventional observation volume by three orders of magnitude. We show that arrays of zero-mode waveguides consisting of subwavelength holes in a metal film provide a simple and highly parallel means for studying single-molecule dynamics at micromolar concentrations with microsecond temporal resolution. We present observations of DNA polymerase activity as an example of the effectiveness of zero-mode waveguides for performing single-molecule experiments at high concentrations.

/pdf/zero-mode-waveguides-for-single-molecule-analysis-at-high-1u8cepddlv.pdf

Zero-Mode Waveguides for Single-Molecule Analysis at High Concentrations

The techniques of optical trapping and manipulation of neutral particles by lasers provide unique means to control the dynamics of small particles. These new experimental methods have played a revolutionary role in areas of the physical and biological sciences. This paper reviews the early developments in the field leading to the demonstration of cooling and trapping of neutral atoms in atomic physics and to the first use of optical tweezers traps in biology. Some further major achievements of these rapidly developing methods also are considered.

/pdf/optical-trapping-and-manipulation-of-neutral-particles-using-4qf0uymz6l.pdf

Optical trapping and manipulation of neutral particles using lasers

https://link.aps.org/pdf/10.1103/RevModPhys.70.721

Nobel Lecture: Laser cooling and trapping of neutral atoms

The radiative properties of an atom in a cavity differ fundamentally from the atom's radiative properties in free space. Spontaneous emission is inhibited if the cavity has characteristic dimensions which are small compared to the radiation wavelength, and enhanced if the cavity is resonant. The cavity causes slight shifts in the energies of the atom, analogous to radiative shifts. Experiments are proposed for observing these effects.

Inhibited Spontaneous Emission

The population of a beam of lithium atoms has been transferred from a low angular momentum Rydberg state to a state with $|m|=n\ensuremath{-}1$, with nearly 100% efficiency. Selective field ionization is employed to detect the high $|m|$ state. Transfer occurs by a series of adiabatic rapid passages; it can also occur by a single multiphoton process.

/pdf/rydberg-atoms-in-circular-states-33mf11fxu2.pdf

Rydberg Atoms in "Circular" States

We have confined over 5\ifmmode\times\else\texttimes\fi{}${10}^{12}$ atoms of hydrogen in a static magnetic trap. The atoms are loaded into the trap by precooling with a dilution refrigerator. At operating densities near 1\ifmmode\times\else\texttimes\fi{}${10}^{13}$ ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}3}$ the gas is observed to be electron and nuclear polarized in the uppermost hyperfine state. The long lifetime of the trapped gas (over 20 min) suggests that it is thermally decoupled from the wall and has evaporatively cooled to a temperature of about 40 mK. The residual decay of the gas density is consistent with spin relaxation induced by dipolar interactions between atoms.

Magnetic trapping of spin-polarized atomic hydrogen.

Atomic physics 7

We have measured the blackbody photoionization rate from the $17d$ state of sodium as a function of temperature from 90 to 300 K. The experimental rates, which vary by a factor greater than one hundred over this temperature range, are in good agreement with our theoretical values.

Daniel Kleppner

Papers

Inhibited Spontaneous Emission

Rydberg Atoms in "Circular" States

Magnetic trapping of spin-polarized atomic hydrogen.

Atomic physics 7

Photoionization by blackbody radiation