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Plasma Physics

Nonthermal Plasma Nonthermal Plasma


Chemistry and Physics Chemistry and Physics
edited by
In addition to introducing the basics of plasma physics, Nonthermal Plasma
Chemistry and Physics is a comprehensive presentation of recent develop-
Jürgen Meichsner
ments in the rapidly growing field of nonthermal plasma chemistry. The book Martin Schmidt
offers a detailed discussion of the fundamentals of plasma chemical reactions
and modeling, nonthermal plasma sources, relevant diagnostic techniques, Ralf Schneider
and selected applications.
Hans-Erich Wagner
Features

• Includes a compact introduction in the nonthermal plasma


physics and plasma–surface interaction
• Classifies the plasma sources and chemical plasma reactors,
and provides important similarity parameters
• Overviews experimental methods in plasma diagnostics and
surface (thin film) analysis
• Presents detailed research results with modeling and applications
• Promotes strategies in plasma modeling and provides specific
methods, including examples

Elucidating interconnections and trends, the book focuses on basic princi-


ples and illustrations across a broad field of applications. Expert contributors
address environmental aspects of plasma chemistry. The book also includes
selected plasma conditions and specific applications in volume plasma
chemistry and treatment of material surfaces such as plasma etching in
microelectronics, chemical modification of polymer surfaces and deposition
of functional thin films. Designed for students of plasma physics, Nonthermal
Plasma Chemistry and Physics is a concise resource also for specialists
in this and related fields of research.

59165
ISBN: 978-1-4200-5916-8
90000

9 781420 059168

59165_Cover_mech.indd 1 9/28/12 10:20 AM


Nonthermal Plasma
Chemistry and Physics

© 2013 by Taylor & Francis Group, LLC


© 2013 by Taylor & Francis Group, LLC
Nonthermal Plasma
Chemistry and Physics
edited by
Jürgen Meichsner
Martin Schmidt
Ralf Schneider
Hans-Erich Wagner

Boca Raton London New York

CRC Press is an imprint of the


Taylor & Francis Group, an informa business

© 2013 by Taylor & Francis Group, LLC


Cover design by Sascha Meichsner and Carsten Desjardins.

CRC Press
Taylor & Francis Group
6000 Broken Sound Parkway NW, Suite 300
Boca Raton, FL 33487-2742
© 2013 by Taylor & Francis Group, LLC
CRC Press is an imprint of Taylor & Francis Group, an Informa business

No claim to original U.S. Government works


Version Date: 20121207

International Standard Book Number-13: 978-1-4200-5921-2 (eBook - PDF)

This book contains information obtained from authentic and highly regarded sources. Reason-
able efforts have been made to publish reliable data and information, but the author and publisher
cannot assume responsibility for the validity of all materials or the consequences of their use. The
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© 2013 by Taylor & Francis Group, LLC


Contents
Preface . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . vii
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ix
Editors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xi
Contributors. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . xiii

Chapter 1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1

Chapter 2 Nonthermal Plasma Chemical Processes of General Interest . . . . . . . . . . 7

Chapter 3 Physics of Nonthermal Plasmas . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15

Chapter 4 Nonthermal Plasma Chemical Reactors . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 137

Chapter 5 Elementary Processes on Surfaces in


Plasma–Wall Interaction. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 163

Chapter 6 Plasma Diagnostics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187

Chapter 7 Surface and Thin Film Analysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 255

Chapter 8 Selected Applications. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 285

Chapter 9 Modeling and Simulation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 407

Chapter 10 Trends and New Concepts . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 469

References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 473
Index . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 539

© 2013 by Taylor & Francis Group, LLC


© 2013 by Taylor & Francis Group, LLC
Preface
Plasma processing is one of the key technologies worldwide, especially using non-
thermal, low-temperature plasmas. Recently, the situation is characterized by the
fast-growing interest in the optimization of existing applications as well as the
development of new ones.
This book provides a basic introduction to nonthermal plasma chemistry and
physics for students of plasma physics, PhD students, and scientists. The fundamen-
tals of plasma chemical reactions and its modeling, most importantly nonthermal
plasma sources, relevant diagnostic techniques, as well as selected applications, are
presented and discussed in a systematic manner. Interconnections are shown; trends
and new concepts are illustrated. The chapters discuss the basic principles and pro-
vide exemplary illustrations of the wide field of applications. Therefore, it is not the
aim of this book to give a complete overview of the state of the art in the research
areas. For this, the readers can refer to already existing excellent monographs and
topical reviews given in the references.
The book is based on contributions from internationally known experts in their
research fields, using examples from their own scientific activities to illustrate the
basic principles with applications.
After a short introduction to the field of nonthermal plasma chemistry with some
historical notes and its specific characteristics, topics of general interest in this field are
briefly presented, which illustrate the broad spectrum of applications. Dry air plasma
chemistry with ozone generation or lacquer stripping and ashing reactions are briefly
discussed. Plasma etching presents a key technology in integrated circuit production.
Methane gas reformation as well as diamond deposition are important topics of
hydrocarbon plasma chemistry. The formation of pre-biochemical compounds is also
observed in nonthermal plasmas. Thin film generation of plasma polymers, of metallic
compounds, and silicone-based cells are products of plasma chemical processes.
The fundamentals, sources, and diagnostics of nonthermal plasmas are discussed
next. The basic concepts of plasma physics for thermal and nonthermal plasmas,
including collisional processes, plasma kinetics, and macroscopic transport equations,
are introduced. Due to the importance of surface processes in many applications, the
plasma-wall boundary is also considered. The basic physics of different nonthermal
plasmas of electric discharges and the realizations for technical plasma sources are
presented at the end of this chapter.
Nonthermal plasma reactors are characterized in terms of the principles of
chemical quasi-equilibria, macroscopic kinetics, and plasma chemical similarity.
Plasma–surface interaction is one of the fastest-growing branches in plasma
physics and has got an important issue in the field of applied surface science. Its basic
question concerns the mastering of an old problem: the contact of different states
of matter. The investigation and application of plasma–surface interaction plays an
essential role in low-temperature plasma processing such as etching, deposition, or
modification of surfaces as well as in fusion research. Therefore, such elementary
processes on surfaces in contact with plasmas are discussed. The particle and energy
balance at the surface determine the importance of the different mechanisms.
vii

© 2013 by Taylor & Francis Group, LLC


viii Preface

According to the broad spectrum of plasma components, different tasks exist


for the investigation of the plasma to understand the processes and to control
chemical reactions characteristic of the various applications. Therefore, the funda-
mentals of probe measurements, microwave interferometry, emission and absorption
spectroscopy, laser-induced fluorescence spectroscopy, and gas chromatography are
discussed.
Complementary techniques needed for surface and thin film analysis are
presented next.
The first part of the next chapter presents examples of applications of volume
plasma chemistry. The reactions take place in the volume, as pure gas phase reac-
tions, or in heterogeneous processes with participation of the surface of substrates,
electrodes, or walls, sometimes assisted by catalytic effects. The second part con-
cerns applications of surface chemistry. Here the plasma chemical reactions result in
changes in surface properties. The reactions may involve volume processes, but the
essential reactions take place at the surface. Etching and thin film deposition as well
as surface functionalization up to plasma medical applications are presented.
Modeling and simulation provide an increasing number of tools to improve the
basic understanding of nonthermal plasmas and allow predictive studies for optimiza-
tion of processes. The hierarchy of plasma models is explained at the beginning of the
next chapter, followed by a discussion of theoretical concepts for elementary volume
and surface processes in gas discharges. The chapter concludes with an example
of modeling, namely, the spatiotemporal dynamics in radio-frequency discharges of
oxygen and its comparison with experimental results.
The book concludes with a discussion of trends and new concepts in this
fascinating and dynamic research area.

© 2013 by Taylor & Francis Group, LLC


Acknowledgments
We would like to express our deep gratitude to all coauthors. They are the fundament
on which this work is based.
A very special thank you goes to Andrea Kleiber (Max-Planck-Institut für Plasma-
physik, Teilinstitut Greifswald, EURATOM Association, Greifswald) for her endless
patience and amazing support. The book would never have been completed with-
out her uncountable contributions and her careful attention. Bert Krames helped as
emergency support in the final processing and transformed the impossible into reality.
We would also like to gratefully acknowledge the work of Marcel Beu (Leibniz-
Institut für Plasmaforschung und Technologie e.V. (INP Greifswald)) for helping us
with the drawings.
This work was partly supported by the Deutsche Forschungsgemeinschaft, Son-
derforschungsbereich Transregio 24. One of the editors (M. S.) appreciates the support
of the INP Greifswald.
Very special thanks go to Lance Wobus of Taylor & Francis Group for his valuable
advice and his patience during the preparation of this book. We gave him a hard time
with this project, but he was always giving us a backup whenever problems appeared.

ix

© 2013 by Taylor & Francis Group, LLC


© 2013 by Taylor & Francis Group, LLC
Editors
Jürgen Meichsner
Institut für Physik der Ernst-Moritz-Arndt-Universität Greifswald, Felix-Hausdorff-
Str. 6, D-17489 Greifswald, Germany

Martin Schmidt
Leibniz-Institut für Plasmaforschung und Technologie e.V. (INP Greifswald) Felix-
Hausdorff-Str. 2, D-17489 Greifswald, Germany

Ralf Schneider
Recent address:
Institut für Physik der Ernst-Moritz-Arndt-Universität Greifswald, Felix-Hausdorff-
Str. 6, D-17489 Greifswald, Germany

Max-Planck-Institut für Plasmaphysik, Teilinstitut Greifswald, EURATOM Associ-


ation, Wendelsteinstr. 1, D-17491 Greifswald, Germany

Hans-Erich Wagner
Institut für Physik der Ernst-Moritz-Arndt-Universität Greifswald, Felix-Hausdorff-
Str. 6, D-17489 Greifswald, Germany

xi

© 2013 by Taylor & Francis Group, LLC


© 2013 by Taylor & Francis Group, LLC
Contributors
Name Institute Sections
Kurt H. Becker PU Brooklyna Section 8.3
Ronny Brandenburg INP Greifswaldb Section 8.2.2
Franz X. Bronold IfP Greifswaldc Section 9.2
Paul B. Davies DoC Cambridged Section 6.3
Andreas Dinklage IPP Greifswalde Section 6.4
Kristian Dittmann IfP Greifswaldc Section 9.4
Jörg Ehlbeck INP Greifswaldb Section 8.2.2
Holger Fehske IfP Greifswaldc Section 9.2
Rüdiger Foest INP Greifswaldb Sections 8.2.2 and 8.2.3.4
Mario Hannemann INP Greifswaldb Section 6.1
Hans-Jürgen Hartfuß IPP Greifswalde Section 6.2
Rainer Hippler IfP Greifswaldc Section 8.4
Holger Kersten IEAP Kielf Sections 5 and 8.4
Kirill V. Kozlov MSU Moscowg Section 8.1.1
Boris P. Lavrov FoP St.-Petersburgh Section 6.3
Detlef Loffhagen INP Greifswaldb Sections 8.1.3 and 9.1
Jürgen Meichsner IfP Greifswaldc Chapters 1, 10, Sections 3.1
through 3.7, 7.1
Siegfried Müller INP Greifswaldb Sections 8.1.2, 8.1.3, and
8.2.2.2
Andreas Ohl INP Greifswaldb Section 8.2.3.4
Abha Rai IPP Greifswalde Sections 8.2.4.1.1 and 9.3
Jürgen Röpcke INP Greifswaldb Section 6.3
Antoine Rousseau LPT Palaiseau Cedexi Section 6.3
Martin Schmidt INP Greifswaldb Chapters 1, 6, 10, Sections 3.8,
6.5, 7.3, 8.1, and 8.2
Ralf Schneider IfP Greifswaldc Chapters 1, 4, 10,
Sections 8.2.3.1.1, 9.3, and 9.4

Karsten Schröder INP Greifswaldb Sections 7.2 and 8.2.3.4
Hartmut Steffen INP Greifswaldb Sections 7.2 and 8.2.4.2
Dirk Uhrlandt INP Greifswaldb Section 9.1
Achim von Keudell RUB Bochumj Chapter 5
Th. von Woedtke INP Greifswaldb Section 8.2.3.5
Hans-Erich Wagner IfP Greifswaldc Chapters 1, 4, 10, Section 6.6
(continued)

xiii

© 2013 by Taylor & Francis Group, LLC


xiv Contributors

(continued)

Name Institute Sections


K.-D. Weltmann INP Greifswaldb Section 8.2.3.5
Harm Wulff IfB Greifswaldk Sections 7.3, 7.5, and 8.2.4.2
Rolf-Jürgen Zahn INP Greifswaldb Sections 8.1.2 and 8.2.3.3

a
Polytechnic Institute of New York University, Brooklyn, NY 11201, USA.
b
Leibniz-Institut für Plasmaforschung und Technologie e.V. (INP Greifswald), Felix-
Hausdorff-Str. 2, D-17489 Greifswald, Germany.
c
Institut für Physik der Ernst-Moritz-Arndt-Universität Greifswald, Felix-Hausdorff-
Str. 6, D-17489 Greifswald, Germany.
d
Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2
1EW, U.K.
e
Max-Planck-Institut für Plasmaphysik, Teilinstitut Greifswald, EURATOM Associa-
tion, Wendelsteinstr. 1, D-17491 Greifswald, Germany.
f
Institut für Experimentelle und Angewandte Physik der Christian-Albrechts-
Universität zu Kiel, Leibnizstr. 19, D-24118 Kiel, Germany.
g
Moscow State University, Department of Chemistry, 119991 Moscow, Russia.
h
Faculty of Physics, St.-Petersburg State University, Ulianovskaya 2, 198904
St.-Petersburg, Russia.
i
Laboratoire de Physique et Technologie des Plasmas, Ecole Polytechnique, Route de
Saclay, F-91128 Palaiseau Cedex, France.
j
Ruhr-Universität Bochum, Universitätsstraße 150, D-44801 Bochum, Germany.
k
Institut für Biochemie der Ernst-Moritz-Arndt-Universität Greifswald, Felix-
Hausdorff-Str. 4, D-17489 Greifswald, Germany.

Deceased.

© 2013 by Taylor & Francis Group, LLC


1 Introduction
CONTENTS
1.1 Plasma Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Historical Notes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.3 Thermal and Nonthermal Plasma Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
1.4 Specifics of Nonthermal Plasma Chemistry . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 3

1.1 PLASMA CHEMISTRY


The plasma state of matter (also named fourth state) is characterized by the exis-
tence of free electrons, positive and negative ions, as well as excited species and
radicals in mixture with the other neutrals of gaseous systems (atoms, molecules) or
liquids. Well-known examples for natural plasmas are the interstellar matter, stars,
the ionosphere, lightnings, and flames.
Plasmas are generated by the input of thermal energy, electric field energy, radi-
ation, or beams (lasers, UV photons, electrons, protons), respectively. The principles
of plasma generation are summarized in Figure 1.1. The focus of the book is on
technical plasmas in gaseous systems that are mostly initiated by applied electric
fields. Examples of such electrical gas discharges are the corona and barrier dis-
charge, sparks, arcs, and plasma torches, operating usually at atmospheric pressure.
Technically important low-pressure plasmas are the different kinds of glow discharges
driven by dc and rf voltages or microwaves.
Gas heating by thermal energy and/or collisions of neutrals with free electrons
and photons of sufficiently high energy initiate the production of free radicals and
further charged species. The generated particles are the source for various chemical
reactions in the volume as well as on the plasma interfaces, forming new compounds,
depositing layers, and modifying the properties of materials.

The science and application of chemical conversions in plasmas, including


reactive processes at interfaces, is the subject of plasma chemistry.

1.2 HISTORICAL NOTES


The existence of chemical reactions in plasmas, initiated by the input of electrical
energy in gaseous atmosphere, is a very old experience of mankind, with even Homer
describing the smell of sulfur∗ in the Iliad in air after lightning.


Sulfur was later identified as nitrogen oxides.

© 2013 by Taylor & Francis Group, LLC


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