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Atomistic Interactions in Stm Atom Manipulation A ATOMISTIC INTERACTIONS IN STM ATOM MANIPULATION A dissertation presented to the faculty of the College of Arts and Sciences of Ohio University In partial fulfillment of the requirements for the degree Doctor of Philosophy Aparna Deshpande March 2007 This dissertation entitled ATOMISTIC INTERACTIONS IN STM ATOM MANIPULATION by APARNA DESHPANDE has been approved for the Department of Physics and Astronomy and the College of Arts and Sciences by Saw-Wai Hla Associate Professor of Physics and Astronomy Benjamin M. Ogles Dean, College of Arts and Sciences Abstract DESHPANDE, APARNA, Ph.D., March 2007, Physics ATOMISTIC INTERACTIONS IN STM ATOM MANIPULATION (125 pp.) Director of Dissertation: Saw-Wai Hla This thesis describes the study of two diverse systems, a cluster of silver atoms, and individual silver and bromine atoms, deposited on a metallic single crystal Ag(111) substrate, in the domain of atomic and molecular manipulation techniques, using a custom-built ultrahigh vacuum low temperature scanning tunneling microscope. A cluster of silver atoms was created by a controlled tip-sample contact. Single atoms were extracted from the cluster by using STM tip induced lateral manipulation. To investigate the mechanism of extraction in detail, atom extraction was carried out for different values of manipulation voltage and current. The threshold distance to pull an atom out from the cluster was determined. The tip-cluster distance proved to be the governing factor for the atom extraction mechanism. Lateral manipulation of a metal atom, silver, and a halogen atom, bromine, was carried out on a silver substrate with a silver coated tip apex. Silver atoms were extracted from a cluster of atoms, and bromine atoms were extracted from a cobalt porphyrin molecule using tunneling electron-induced bond dissociation technique. The threshold distance necessary to manipulate the silver atom and the bromine atom was determined. The lateral manipulation signals provided a value of the angle made by the tip with the surface at the first jump of the atom during manipulation. The interaction energy curves for these atoms were calculated using density functional theory. From a combination of all these results, a numerical value of force was obtained. This force corresponds to the threshold force necessary to move a silver atom and a bromine atom on the surface. The values of force provide an insight into the ionic and metallic interactions on the surface at the single atom level. The manipulation capability of the scanning tunneling microscope to build nanostructures was demonstrated by constructing a parabolic corral using locally extracted atoms. Since the surface vacancies and defects created during construction can be sealed off with the atoms and clusters after construction, this procedure resembles an atomic scale analog of a macroscale construction site. Approved: Saw-Wai Hla Associate Professor of Physics and Astronomy Acknowledgments I am grateful to my advisor for his mentorship. His crucial input at every stage of my projects, his wisdom, scientific and otherwise, and his pedagogy have helped me all along. Thank you for your patience and for the opportunity to be involved in the construction of a sophisticated system. My thesis committee members for devoting a share of their precious time to read my thesis. A special note of thanks to Prof. Elizabeth who was willing to be on the committee at a late notice. Dr. Kai-Felix Braun for his help with the STM instrumentation, standing wave pattern calculation program, and insightful discussions. For all the physics classes and the professors who gave them, thank you. Prof. Sergio for letting me participate in the theory group meetings and the chance to broaden my physics and world outlook. Prof. Nancy for being a friend and a great listener. Ennice, Ruth, Tracy, Chris and Roger for all their help over the years. Violeta for the enriching friendship. To all my team mates in the Hla group for the camaraderie. Swati for the good times, Deepshikha for the fun get togethers and the fantastic Indian food, Anand for sharing the passion for movies and music. Collins for the love, friendship and the stoic support that I have always counted on. My Kaku and Kaka for making me a part of their family and for their continued love and affection. My Baba for always being there. Thank you for being a great parent, for instilling the value of education and for letting me follow my dreams. My Tai for the love and emotional support, Tejas for the wonderful growing up years. Suhita for being my pillar of strength. Dedicated to Suhita 8 Table of Contents Page Abstract……………………………………………………………………………………3 Acknowledgments…………………………………………………………………………5 Dedication…………………………………………………………………………………7 List of Table..................................................................................................................….11 List of Figures……………………………………………………………………………12 Chapter 1. Introduction..................................................................................................... 19 Chapter 2. Instrumentation ............................................................................................... 24 2.1 Operating Principle of STM ...................................................................... 24 2.2 UHV-LT-STM System ...............................................................................31 2.2.1 UHV System ......................................................................................32 2.2.2 STM Unit ...........................................................................................34 2.2.3 STM Hardware and Software ............................................................36 Chapter 3. Background ..................................................................................................... 38 3.1 STM Manipulation Techniques ................................................................. 38 3.1.1 Lateral Manipulation..........................................................................39 3.1.2 Vertical Manipulation ........................................................................43 3.1.3 Inelastic Tunneling Electron Induced Excitations .............................46 3.2 Atomistic Interactions................................................................................ 48 3.2.1 Types of Interactions..........................................................................48 3.2.2 Interactions in STM Manipulation.....................................................51 9 3.3 Materials ......................................................................................................52 3.3.1 Substrate..............................................................................................53 3.3.2 Molecule .............................................................................................55 Chapter 4. Atom Extraction by Controlled Tip-Cluster Interaction ................................. 57 4.1 Introduction.................................................................................................57 4.2 Experimental Details...................................................................................60 4.3 Atom Extraction..........................................................................................60 4.3.1 Lateral Manipulation for Extraction ................................................. 61 4.3.2 Threshold Resistance .........................................................................64 4.4 Modeling......................................................................................................67 4.5 Discussion....................................................................................................70 Chapter 5. Atomistic Constructions.................................................................................. 72 5.1 Construction Scheme .................................................................................. 72 5.2 Reconstruction Scheme............................................................................... 78 5.3 Discussion....................................................................................................79 Chapter 6. Atom Selective Force Measurement ............................................................... 81 6.1 Introduction……………………………………………. …………………81 6.2 Force Measurement Strategy .......................................................................82 6.3 Experimental Details....................................................................................84 6.4 Br Atoms......................................................................................................87 6.4.1 Extraction of Br Atoms.......................................................................87 6.4.2 Threshold Resistance Measurement of Br Atoms ...............................90 6.4.3 Lateral Manipulation for Angle Measurement ....................................94 10 6.4.4 Height Correction for Br Atoms ..........................................................96 6.4.5 Numerical Value of Force....................................................................97 6.5 Ag Atoms...................................................................................................100 6.5.1 Extraction of Ag Atoms.....................................................................100 6.5.2 Threshold Resistance Measurements for Ag Atoms..........................101 6.5.3 Lateral Manipulation for Angle Measurement ..................................104 6.5.4 Numerical
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