Fluorescence photon antibunching from single molecules on a surface

Abstract Fluorescence correlation spectroscopy of individual Rhodamine 6G (R6G) molecules immobilized on a silica surface is performed in air at room temperature using confocal laser scanning optical microscopy (CLSM). The high excitation irradiance in CLSM is used to saturate single R6G molecules, and to observe fluorescence photon antibunching. An experimental arrangement is described that improves the overall coincidence counting efficiency at high irradiance. Photophysical parameters obtained from the saturation data are used to model the antibunching behavior. This is the first reported example of photon antibunching from individual quantum systems on a surface.

[1]  W. Moerner,et al.  Examining Nanoenvironments in Solids on the Scale of a Single, Isolated Impurity Molecule , 1994, Science.

[2]  Louis E. Brus,et al.  Imaging and Time-Resolved Spectroscopy of Single Molecules at an Interface , 1996, Science.

[3]  Robert J. Chichester,et al.  Single Molecules Observed by Near-Field Scanning Optical Microscopy , 1993, Science.

[4]  Alfred J. Meixner,et al.  Super-resolution imaging and detection of fluorescence from single molecules by scanning near-field optical microscopy , 1995 .

[5]  Talon,et al.  Photon antibunching in the fluorescence of a single dye molecule trapped in a solid. , 1992, Physical review letters.

[6]  E. Betzig,et al.  Near-field spectroscopy of single molecules at room temperature , 1994, Nature.

[7]  J. Pawley,et al.  Handbook of Biological Confocal Microscopy , 1990, Springer US.

[8]  Mario Dagenais,et al.  Photon Antibunching in Resonance Fluorescence , 1977 .

[9]  Lloyd M. Davis,et al.  Single photon avalanche diode for single molecule detection , 1993, Optical Society of America Annual Meeting.

[10]  W. Lukosz.  Light emission by magnetic and electric dipoles close to a plane dielectric interface. III. Radiation patterns of dipoles with arbitrary orientation , 1979 .

[11]  Måns Ehrenberg,et al.  Rotational brownian motion and fluorescence intensify fluctuations , 1974 .

[12]  Walther,et al.  Nonclassical radiation of a single stored ion. , 1987, Physical review letters.

[13]  C. Reimann,et al.  Photochemical bleaching of adsorbed rhodamine 6G as a probe of binding geometries on a fused silica surface , 1991 .

[14]  De Martini F,et al.  Single-mode generation of quantum photon states by excited single molecules in a microcavity trap. , 1996, Physical review letters.

[15]  T. Basché,et al.  Measurement of Optical Dephasing of a Single Terrylene Molecule with Nanosecond Time Resolution , 1995 .

[16]  S. Garoff,et al.  Surface interactions of adsorbed molecules as probed by their optical properties , 1982 .

[17]  W. Lukosz,et al.  Optical-environment-dependent effects on the fluorescence of submonomolecular dye layers on interfaces , 1987 .

[18]  Tsuyoshi Hayakawa,et al.  Single-Molecule Detection by Laser-Induced Fluorescence Technique with a Position-Sensitive Photon-Counting Apparatus , 1994 .

[19]  A. H. Klahn,et al.  References and Notes , 2022 .

[20]  W. P. Ambrose,et al.  Alterations of Single Molecule Fluorescence Lifetimes in Near-Field Optical Microscopy , 1994, Science.

[21]  Alois Renn,et al.  Fluorescence Microscopy of Single Molecules , 1994 .

[22]  Kiwamu Saito,et al.  Imaging of single fluorescent molecules and individual ATP turnovers by single myosin molecules in aqueous solution , 1995, Nature.

[23]  J. J. Macklin,et al.  Time-resolved spectroscopy of single molecules using near-field and far-field optics , 1996 .

[24]  W. Moerner,et al.  Structure and Dynamics in Solids As Probed by Optical Spectroscopy , 1996 .

[25]  Ambrose,et al.  Single molecule detection and photochemistry on a surface using near-field optical excitation. , 1994, Physical review letters.