High-resolution microscope for tip-enhanced optical processes in ultrahigh vacuum.

An optical microscope based on tip-enhanced optical processes that can be used for studies on adsorbates as well as thin layers and nanostructures is presented. The microscope provides chemical and topographic informations with a resolution of a few nanometers and can be employed in ultrahigh vacuum as well as gas phase. The construction involves a number of improvements compared to conventional instruments. The central idea is to mount, within an UHV system, an optical platform with all necessary optical elements to a rigid frame that also carries the scanning tunneling microscope unit and to integrate a high numerical aperture parabolic mirror between the scanning probe microscope head and the sample. The parabolic mirror serves to focus the incident light and to collect a large fraction of the scattered light. The first experimental results of Raman measurements on silicon samples as well as brilliant cresyl blue layers on single crystalline gold and platinum surfaces in ultrahigh vacuum are presented. For dye adsorbates a Raman enhancement of approximately 10(6) and a net signal gain of up to 4000 was observed. The focus diameter ( approximately lambda2) was measured by Raman imaging the focal region on a Si surface. The requirements of the parabolic mirror in terms of alignment accuracy were experimentally determined as well.

[1]  A. Meixner,et al.  Confocal microscopy with a high numerical aperture parabolic mirror. , 2001, Optics express.

[2]  Quang Nguyen,et al.  Simple model for the polarization effects in tip-enhanced Raman spectroscopy , 2007 .

[3]  J. Jersch,et al.  Calculation of the field enhancement on laser-illuminated scanning probe tips by the boundary element method , 1998 .

[4]  A. Demming,et al.  Plasmon resonances on metal tips: understanding tip-enhanced Raman scattering. , 2005, The Journal of chemical physics.

[5]  Olivier J. F. Martin,et al.  Controlling and tuning strong optical field gradients at a local probe microscope tip apex , 1997 .

[6]  Nir Davidson,et al.  High-numerical-aperture focusing of radially polarized doughnut beams with a parabolic mirror and a flat diffractive lens. , 2004, Optics letters.

[7]  G. Ertl,et al.  Surface-enhanced and STM tip-enhanced Raman spectroscopy of CN− ions at gold surfaces , 2003 .

[8]  B. Ren,et al.  Preparation of gold tips suitable for tip-enhanced Raman spectroscopy and light emission by electrochemical etching , 2004 .

[9]  Markus B. Raschke,et al.  Scanning-probe Raman spectroscopy with single-molecule sensitivity , 2006 .

[10]  J. Maguire,et al.  Nano-Raman spectroscopy with side-illumination optics , 2005 .

[11]  Lukas Novotny,et al.  Nanoscale vibrational analysis of single-walled carbon nanotubes. , 2005, Journal of the American Chemical Society.

[12]  Nicholas A. Klymyshyn,et al.  Finite Element Method Simulation of the Field Distribution for AFM Tip-Enhanced Surface-Enhanced Raman Scanning Microscopy , 2003 .

[13]  Satoshi Kawata,et al.  Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode , 2006 .

[14]  Lukas Novotny,et al.  High-resolution near-field Raman microscopy of single-walled carbon nanotubes. , 2003, Physical review letters.

[15]  A. Meixner,et al.  A high numerical aperture parabolic mirror as imaging device for confocal microscopy. , 2001, Optics express.

[16]  Gerd Leuchs,et al.  Generation of a radially polarized doughnut mode of high quality , 2005 .

[17]  Kathleen S. Youngworth,et al.  Focusing of high numerical aperture cylindrical-vector beams. , 2000, Optics express.

[18]  S. Kawata,et al.  Metallized tip amplification of near-field Raman scattering , 2000 .

[19]  Gerd Leuchs,et al.  Focusing light to a tighter spot , 2000 .

[20]  R. Zenobi,et al.  Nanoscale chemical analysis by tip-enhanced Raman spectroscopy , 2000 .

[21]  S. Kawata,et al.  Tip-enhanced coherent anti-stokes Raman scattering for vibrational nanoimaging. , 2004, Physical review letters.

[22]  S. Kawata,et al.  Polarization measurements in tip-enhanced Raman spectroscopy applied to single-walled carbon nanotubes , 2005 .

[23]  A. Meixner,et al.  Probing highly confined optical fields in the focal region of a high NA parabolic mirror with subwavelength spatial resolution , 2003, Journal of microscopy.

[24]  I. Notingher,et al.  Effect of sample and substrate electric properties on the electric field enhancement at the apex of SPM nanotips. , 2005, The journal of physical chemistry. B.

[25]  Lukas Novotny,et al.  Theory of Nanometric Optical Tweezers , 1997 .

[26]  T. Witting,et al.  On the Field Enhancement at Laser‐illuminated Scanning Probe Tips , 2002 .

[27]  Hans Peter Herzig,et al.  Propagation of the electromagnetic field in fully coated near-field optical probes , 2003 .

[28]  Gerhard Ertl,et al.  Surface Enhanced Raman Spectroscopy: Towards Single Molecule Spectroscopy , 2000 .

[29]  Jürgen Popp,et al.  On the way to nanometer-sized information of the bacterial surface by tip-enhanced Raman spectroscopy. , 2006, Chemphyschem : a European journal of chemical physics and physical chemistry.

[30]  Jürgen Popp,et al.  Towards a detailed understanding of bacterial metabolism--spectroscopic characterization of Staphylococcus epidermidis. , 2007, Chemphyschem : a European journal of chemical physics and physical chemistry.

[31]  G Leuchs,et al.  Sharper focus for a radially polarized light beam. , 2003, Physical review letters.

[32]  Gerhard Ertl,et al.  Tip‐enhanced Raman spectroscopy (TERS) of malachite green isothiocyanate at Au(111): bleaching behavior under the influence of high electromagnetic fields , 2005 .