Motivation

 

Rapid developments in nanoscience and nanotechnology make it essential to be able to make spectroscopic measurements at the nanometer scale. The existence of quantum confinement effects in nanometer scale structures is a large part of what drives interest in this field; the strong dependence of these effects on individual structure sizes and the potential for strong coupling of levels from closely spaced structures renders the overall performance of assemblies of small structures complex, and difficult to predict.  In addition, segregation at interfaces, particularly those to nanostructures will dramatically affect both electronic and transport properties across them.  Many of the technologies earmarked for significant growth in the coming decades are critically dependent on credible nanometer-scale measurements and analysis.  These certainly include high-density electronics, biosensors, high throughput experimentation, separations, and catalysis.  Development of robust, nanoscale measurement tools is critically important if the full potential of these technologies is to be realized.

 

The spatial resolution available in a spectroscopic measurement depends both on the size of the probe beam, and on the spreading of the excited region due to either carrier diffusion or energy transfer through a system.  In the case of incident visible or UV light, the diffraction limit until recently seemingly prevented resolution at much below 0.1 um.  Focused x-ray sources provided insufficient incident flux to make nm scale spectroscopy possible.  Electron beams can be focused to sub-nm dimensions, but only at high energies, so that the electrons must undergo a large number of inelastic scatterings to drop into a bound energy level, again leading up until recently to resolution no better than 0.1 um.   A number of approaches have been invented in recent years to avoid these limitations.  Important examples are: Near-field scanning optical microscopy beats the diffraction limit through the use of an aperture.  The advent of ultra-bright third generation synchrotron sources now allows focusing of x-ray beams to a few tens of nm with exceedingly high incident fluxes.  The use of the scanning tunneling microscope allows injection of electrons or holes into a structure with 0.1 nm incident beam diameter, and at energies close to resonance with bound levels, greatly reducing their diffusion lengths.

 

Scope of the Workshops

 

The development of powerful new techniques and the modification of existing techniques for the measurement of spectroscopy with spatial resolution approaching the nanometer scale in recent years bring forth an unprecedented level of understanding as to the relationship between size/structure/composition/strain in nanometer sized structures, and the resultant electronic structure.  Briefly put, these techniques make possible the interrogation of individual nanostructures, or small numbers of coupled nanostructures, rather than ensembles, so that the above mentioned relationships and the coupling of energy levels between neighboring structures can be systematically studied.  These workshop serve as a forum for scientists from the US, Europe and Asia to present results demonstrating the capabilities of highly-spatially spectroscopic techniques to systems of scientific and technological interest. The scope of the third workshop included recent results from a variety of techniques, with sessions on spectroscopic photoemission microscopy and spectromicroscopy, near-field scanning optical microscopy, scanning tunneling microscopy-based techniques, and cathode luminescence.  In addition, we added sessions to address questions of critical nanomaterials science and technology interest, as discussed below.  The final program, abstracts and photos of the workshop are now available online.

 

One of the focus areas sessions at NSS3 was interfaces to nanostructures, and how to characterize them.  Presentations in this area described results of transport though nanotubes/metal, metal/molecule and semiconductor/metal interfaces, including vibrational spectroscopy derived from these measurements.  Measurements of this type contribute to our understanding of the nature of the transport across these interfaces. A crucial issue for application of nanostructures in logic, or sensing applications is our ability to produce reliable, low impedance contacts to these structures, to allow transport of signals into and out of them.  It has been recognized at least since the seminal work of Landauer  that transport through a nanoscale structure is determined not merely by its intrinsic conductance but also by the transmission probabilities across the interfaces bounding it.   Recent comparisons of measurements and calculations of the conductance profile for a simple case, that of single dithiol molecules between gold contacts show that these transmission probabilities can dominate the transport, resulting in measured values orders of magnitude below that for the molecule itself.  Measured electrical transport through carbon nanotubes has also indicated that the barriers formed at the contacts determine the electrical character of devices based upon these structures.  Indeed, this has led to a pronounced sensitivity the way in which the contacts are formed and subsequently processed, e.g. annealing in vacuum.  Direct measurement of the electrostatic potential across metallic nanowires by scanned gate microscopy in fact indicates that the resistance at the contacts can account for almost the entire potential drop across them.  This session included contributions both from experimentalists and from theorists doing first principles calculations of transport through these structures, and provided for a very lively discussion on this crucial issue.

 

A second focus area addressed critical issues in quantum dots, including characterization of size, shape, composition and correlation to electronic and optical properties, requiring advanced nanoscale spectroscopies such as optical near-field spectroscopy.  Knowledge gained from such measurements is needed to feed back into the development of functionalized quantum dot materials that can enable new technologies such as spintronics and quantum computing. Additional important issues involve achieving electronic control of individual quantum dots using local external fields, for example, with an STM tip or an optical laser pulse.  Coherent optical control of the wavefunction of individual quantum dots using nano-optical techniques could eventually enable solid state quantum computing.

 

A third focus area was single molecule spectroscopies (SMS), which are of great interest at present.   From a scientific viewpoint, the greatest strength of single molecule spectroscopy lies in our ability to resolve structural and dynamic heterogeneity masked by conventional ensemble measurements.  SMS methods are particularly suited for the investigation of complex kinetic processes, determination of structural heterogeneity of complex systems, and materials characterization on molecular length scales.  SMS techniques can be applied in a host of sample matrices from glassy materials to living cells and promise to be important in addressing unanswered questions such as the origin of the observed “blinking” phenomenon in quantum dots and the molecular nature of "hot spots" in surface enhanced Raman scattering

 

The development of new techniques which allow probing of individual nanostructures or small numbers of nanostructures continues to shed new experimental light on the interrelationship between synthesis, structure and properties of materials, enhancing our understanding and driving further development of theoretical models to explain unexpected observations.  At the heart of the excitement of nanoscience is the fact that it provides working models in which one of the great intellectual feats of the twentieth century, the development of quantum mechanics, can be tested.  The goal of research in nanoscale spectroscopy is to extend our understanding of fundamental issues in nanoscale science.  These include the relationship between structure and electronic energy levels at the nanoscale, the coupling of energy levels in neighboring mesoscale structures, the mechanisms which limit the coherence length in coupled structures, and how transport occurs across interfaces between nanostructures. NSS3 provided a forum for discussion of new experimental observations, how these can be understood within a theoretical framework, and how they require the modification of existing models of phenomena at the nanoscale. 

 

Program

 

Participation was from approximately 70 scientists and students from the United States, Europe and Japan, including a number of key researchers working on the development and application of nanometer scale spectroscopy and related techniques.  Invited speakers as well as titles/topics for their presentations are listed below.  A brief summary of the results presented, session by session is available on line. A number of the presentations were given by young faculty, postdoctoral researchers and graduate students working in this exciting field. 

 

Stefan Eisebitt

Bessy II

Lensless X-ray Imaging

Hendrik Ohldag

SSRL, Stanford

XPEEM from Antiferromagnets

Barry Barker

Lab for Physical Sciences

STS at and Below 4K

Harald Ade

NC State University

Soft X-ray characterization in real and reciprocal space

Saw-Wai Hla

University of Ohio

Single Atom Manipulation

Markus Morgenstern

RWTH Aachen

Wavefunction Mapping in different dimensions

Adrian Wetzel

University of Basel

Time of flight SPM

Jun Cheng

University of Michigan

Coherent Optical Spectroscopy of single quantum dots

Allan Bracker

Naval Research Labs

Optical pumping of spin in single charged quantum dots

David Fromm

Stanford University

Optical Properties of Nanoscale Metallic Structures

Bernd Kabius

Argonne National Lab

Energy-Filtered TEM, and the TEAM instrument 

Andy Lupini

Oak Ridge National Lab

STEM-based EELS and Applications to Nanoscience

Vladimir Oleshko

University of Virginia

PEEL Spectroscopy and EFTEM

Chris Davis

University of Maryland

Optical Properties of Nanohole arrays

Igor Smolyaninov

University of Maryland

Far field microscope with nm resolution

Lukas Novotny

University of Rochester

Nanoscale Optical

 Spectroscopy

Bennett Goldberg

Boston University

Resonant microRaman and light spectroscopy from Nanotubes

Paul Barbara

Univ. of Texas-Austin

Single Molecule

 Spectroscopy

Ken Shih

Univ. of Texas-Austin

Rabi flopping on a single quantum dot

James Kushmerick

Naval Research Labs

Understanding Charge Transport in Molecular Electronics and Vibrational Spectroscopy

Massimilliano DiVentra

Univ. of California-San Diego

First Principles Calculations of Transport across interfaces to molecules & nanostructures

Michael Fuhrer

University of Maryland

Probing Energy States of Molecules and Nanotubes through Transport

Igor Smolyninov

University of Maryland

Far-field optical microscope with nanometer-scale resolution

Yoichi Uehara

Tohoku University

Light Emission STM

Yoshio Watanabe

NTT-Japan

SPELEEM observation of individual single-walled carbon nanotubes

Emil Zolotoyabko

Technion

Stroboscopic X-Ray Imaging

 

Invited speakers who participated  in NSS3.

 

Organization

 

The local organization committee consisted of Ray Phaneuf, Dennis Drew, Doug English, and Janice Reutt-Robey (University of Maryland), Stephan Stranick (NIST), and Dan Gammon (NRL).The international program committee for the workshop consists of Ray Phaneuf, (University of Maryland), Doug English, (University of Maryland), Stephan Stranick, (NIST), Giancarlo Salviati (IMEM-CNR, Italy), Stefan Heun (Laboratorio TASC-INFM), Marcello Colocci (University of Firenze, Italy), and from Japan: Yoichi Uehara (Tohoku University, Japan), Takashi Sekiguchi (NIMS, Japan) and Yoshio Watanabe  (NTT, Japan).   

 

 

Photos from the Third International Workshop

(Click here for additional photos)

 

The workshop was held at the Laboratory for Physical Sciences (LPS), at the University of Maryland at College Park (UMCP), located just outside of Washington, DC.  The program included presentations from LPS researchers, as well as UMCP faculty and students from the departments of Physics, Chemistry, Materials Science and Engineering, and Electrical and Computer Engineering. 

 

Previous Workshops

 

The International Workshops on Nanoscale Spectroscopy were created to serve as a forum for the exchange of information about applications and new developments of these techniques in the rapidly growing field of nanoscience and technology.  The first workshop on Nanoscale Spectroscopy and its Applications to Semiconductor Research was held at the International Center for Theoretical Physics (ICTP) in Trieste, Italy, from December 11 - 14, 2000. It was the result of a joint initiative between the Italian National Research Council (CNR) and the Japanese Society for the Promotion of Science (JSPS), and was attended by 74 participants from 13 countries (Italy, Japan, Germany, Switzerland, Slovenia, Russia, Spain, Czech Republic, India, USA, UK, Poland, and Austria).  The second International Workshop on Nanoscale Spectroscopy and Nanotechnology was held in Tokyo, Japan, from November 25-29, 2002.  This workshop expanded the scope of the meetings to include work done investigating quantum wires and carbon nanotubes, identification of surface adsorbates, and dynamics of nanostructure formation.   The third workshop will be held in the United States, at the University of Maryland, College Park, and will further expand the scope of the meetings.

 

Acknowledgements

 

Support was generously provided by LPS, by a National Science Foundation Materials Research and Engineering Center (NSF-MRSEC), by the National Institute of Standards and Technology (NIST), by Omicron Nanotechnology, SPECS Corporation, and by the National Science Foundation.

 

 

 

 

For more information on NSS3, contact:

Ray Phaneuf

Department of Materials Science and Engineering

University of Maryland

College Park, MD 20742

Tel.: 1-301-935-6473

Fax: 1-301-935-6723

phaneuf@eng.umd.edu

Organizer, Third International Workshop on Nanoscale Spectroscopy and Nanotechnology