Frontiers of Optical SpectroscopyInvestigating Extreme Physical Conditions with Advanced Optical Techniques

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Series II: Mathematics, Physics and Chemistry – Vol. 168

Frontiers of Optical SpectroscopyInvestigating Extreme Physical Conditions with Advanced OpticalTechniques

edited by

Baldassare Di BartoloBoston College,Chestnut Hill, MA, U.S.A.

and

Ottavio ForteRaytheon Command, Control, Communications and Information Systems,Sudbury, MA, U.S.A.

Kluwer Academic Publishers

Dordrecht / Boston / London

Published in cooperation with NATO Scientific Affairs Division

Proceedings of the NATO Advanced Study Institute onFrontiers of Optical SpectroscopyInvestigating Extreme Physical Conditions with Advanced Optical TechniquesErice, Italy16 May–1 June 2003

A C.I.P. Catalogue record for this book is available from the Library of Congress.

ISBN 1-4020-2750-8 (PB)ISBN 1-4020-2749-4 (HB)ISBN 1-4020-2751-6 (e-book)

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© 2005 Kluwer Academic Publishers

CONTENTS

PREFACE xix

LIST OF PAST INSTITUTES xxi

LECTURES

1. INVESTIGATING PHYSICAL SYSTEMS WITH OPTICALSPECTROSCOPY 1(Baldassare Di Bartolo)Abstract 11. Introduction 12. Interaction of Radiation with Atoms and Molecules 2

Acknowledgements 28References 28

2. LIGHT-MATTER INTERACTIONS ON THE FEMTO SECONDTIME SCALE 29(Chris A.D. Roeser and Eric Mazur)Abstract 291. Light-matter Interactions 292. Ultrafast Dynamics of Solids under Intense Photoexcitation 363. Nonlinear Optical Properties 414. Ultrafast Materials Science 435. Summary 49

Notes 50References 51

3. PHOTONS AND PHOTON STATISTICS: FROM INCANDESCENTLIGHT TO LASERS 55(Ralph v. Baltz)

1. Introduction 552. Nature of Light 553. Classical Description of the EMF: Waves 554. Quantum Theory of Light: Photons 645. Optical Devices and Measurements 756. Outlook 90

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7. Acknowledgements 90References 91Solutions of the Problems 92

4. CARRIER-WAVE NONLINEAR OPTICS 93(Martin Wegener)1. Introduction 932. Some Aspects of Few-Cycle Laser Pulses From Mode-Locked

Oscillators 953. How Intense is the Light Field? 1094. Carrier-Wave Rabi Flopping of Electrons in Semiconductors 1195. “Off-Resonant” Carrier-Wave Nonlinear Optics of Electrons

in Semiconductors 1416. Attosecond Pulses and Interaction of Intense Laser Fields with

Atoms, Electrons and the Vacuum 1537. Summary 1708. Acknowledgements 1719. References 172

10. Solutions of Exercises 17611. Important Symbols and Constants 17912. Appendices 181

5. CAROTENOID EXCITED STATES-PHOTOPHYSICS,ULTRAFAST DYNAMICS AND PHOTOSYNTHETICFUNCTIONS 187(Tomáš Polívka and Villy Sundström)1. Introduction 1872. Excited State Structure of Carotenoid Molecules 188

195Acknowledgements 204References 214

6. SPECTROSCOPY OF QUANTUM WELLS ANDSUPERLATTICES 221(Claus Klingshirn)Abstract 2211. Prolog 2212. Introduction to Electronic Properties 2223. Quantum Wells and Superlattices 2294. Interband Spectroscopy 2335. Intersubband Transitions 2386. Phonons in Bulk Semiconductors 2407. Phonons in Superlattices 243

3. Excited States of Carotenoids in Pigment Protein Complexes

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8. Conclusions and Outlook 248Acknowledgements 248References 249

7. LASERS FOR FRONTIER SPECTROSCOPY 251(Giuseppe Baldacchini)Abstract 2511. Introduction 2512. The Rise of Lasers 2523. Spectroscopy with Lasers 2614. Advances of Laser and Spectroscopy 2705. Conclusions 284

Acknowledgements 285References 286

8. COHERENT SPECTROSCOPY OF STRATIFIED SEMI-CONDUCTOR MICRO- AND NANOSTRUCTURES 289(Vadim Lyssenko)1. Introduction 2892. Maxwell’s Equations 2903. Transmission and Reflectivity 2924. Multiple-beam Interference 2935. Refraction and Reflection at the Surface of an Absorptive

Medium 2966. Absorptive Fabry-Pérot Interferometer 3027. Basic Physics of Microcavities 3028. Angle-dependent Properties 3129. Electron Envelope Wavefunctions �(z) 322

10. Acknowledgements 33211. References 332

9. CONSEQUENCES OF EXTREME PHOTON CONFINEMENTIN MICRO-CAVITIES: I. ULTRA-SENSITIVE DETECTIONOF PERTURBATIONS BY BIO-MOLECULES 337(Stephen Arnold, Mayumi Noto, and Frank Vollmer)Abstract 3371. Introduction 3382. Simple Considerations 3393. Theoretical Approach 3404. Experimental Insights which Grow Out of the Fig. 3 3435. First Order Perturbation Theory: Spherically Symmetric

Layer 3456. Experimental Setup 349

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7. Experimental Results 351Acknowledgements 356References 357

10. LUMINESCENCE PROPERTIES OF VERY SMALL SEMI-CONDUCTOR PARTICLES 359(Cees Ronda)

1. Introduction 3592. Some Possible Application Areas of Very Small Semi-conductor

Quantum Dots 3593. Elementary Quantum Mechanics 3624. Electrons in a Crystal 3735. Density of States in Low Dimensional Structures 3786. Electrons, Holes and Excitons 3807. Low Dimensional Structures 3818. Quantum Confinement in Action 3839. Outlook 392

10. References 392

11. AN INTRODUCTION TO THE PHYSICS OF ULTRACOLDATOMIC GASES 395(C.J. Pethick, H. Smith)

1. Energy and Length Scales 3962. Bose-Einstein Condensation 4003. Interatomic Interactions 4034. Equilibrium Properties of a Trapped Gas 4065. Dynamics of Condensates 4106. Potential Flow and Quantized Vortices 4147. Other Topics 4168. Concluding Remarks 422

References 422

12. LASER COOLING AND TRAPPING OF NEUTRAL ATOMSTO ULTRALOW TEMPERATURES 427(Kristian Helmerson)

1. Introduction 4272. Radiative Forces 4293. Deceleration and Cooling of an Atomic Beam 4294. Traps for Neutral Atoms 4455. Sub-Doppler Laser Cooling 4546. Optical Lattices 460

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7. Manipulating Bose-Einstein Condensates with Light 468References 489

13. ULTRAFAST STRUCTURAL DYNAMICS IN THECONDENSED PHASE 497(Majed Cherqui)Abstract 4971. Introduction 4972. Historical Background: From Kinetics to Dynamics 4983. Basic Quantum Mechanics 4994. Wave Packets Dynamics in Isolated Systems 5015. Wave Packets Dynamics in Solids 5036. Wave Packet Dynamics in Biological Systems 5107. New Frontiers of Ultrafast Structural Dynamics 513

Acknowledgements 518References 518

14. LANTHANIDE SERIES SPECTROSCOPY UNDER EXTREMECONDITIONS 521(Norman P. Barnes)Abstract 5211. Introduction 5212. Absorption Saturation 5223. Amplified Spontaneous Emission 5244. Energy Transfer 5255. Self Quenching 5336. Up Conversion 5357. Excited State Absorption 5368. Summary 5389. References 538

15. EXCITING BOSE-EINSTEIN CONDENSATION VERSUSELECTRON-HOLE PLASMA FORMATION 539(Claus Klingshirn)Abstract 5391. Introduction 5392. The Electron-Hole Plasma 5413. Excitonic Bose-Einstein Condensation and Superfluidity 5534. Conclusion and Outlook 566

Acknowledgements 566References 567

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16. DYNAMICS OF SOLID-STATE COHERENT LIGHT SOURCES 571(Markus Pollnau)1. Introduction 5712. Spectroscopic Processes of Rare-Earth Ions in Solid-State

Laser Materials 5713. Upconversion Dynamics 5774. Impact of Energy-Transfer Upconversion on Solid-State

Laser Performance 5825. Conclusions 585

Acknowledgements 585References 585

17. SOME NOVEL ASPECTS OF INTRAMOLECULARELECTRONIC ENERGY TRANSFER PROCESSES 591(Shammai Speiser)Abstract 5911. Introduction 5912. The Naphthalene-Anthracene Bichromomorphic

Molecular System 5913. Towards Molecular Scale Devices Based on Controlled

Intramolecular Interactions 603Acknowledgements 617References 617

18. STIMULATED RAMAN SCATTERING SPECTROSCOPY OFFRONTIER NONLINEAR-LASER MATERIALS: ORGANICCRYSTALS AND NANOCRYSTALLINE CERAMICS 619(Alexander A. Kaminskii)Abstract 6191. Introduction 6192. The Steady-State Stimulated Raman Scattering 6213. Stimulated Raman Spectroscopy of Nonlinear-Laser Organic

Crystals and Nanocrystalline Ceramics 6244. Conclusion 627

Acknowledgements 627References 644

INTERDISCIPLINARY LECTURE

19. STRANGE PROPERTIES OF QUANTUM SYSTEMS ANDPOSSIBLE INTERPRETATIONS 647(Giovanni Costa)Abstract 647

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1. Introduction 6472. Resumé of the Main Ingredients of Quantum Mechanics 6483. Entangled States and the EPR Argument 6534. Bell’s Inequality 6565. Experimental Tests 6596. An Application of the EPR Theorem 6607. Macroscopic Quantum Superposition and the Measurement

Problem 662Acknowledgement 666References 666

LONG SEMINARS

20. MODULATION SPECTROSCOPY REVISITED 669(George J. Goldmith)

1. Introduction 6692. The Dielectric Function and Reflectivity 6703. Modulations Methods 6764. Some Applications 680

References 685

21. ADVANCES IN SOLID STATE LASERS AT NASA LANGLEYRESEARCH CENTER 687(James Barnes)Abstract 687

22. COMBINATORIAL CHEMISTRY TO GROW SINGLECRYSTALS AND ANALYSIS OF CONCENTRATIONQUENCHING PROCESSES: APPLICATION TO Yb3+-DOPEDLASER CRYSTALS 689(Georges Boulon)Abstract 6891. Introduction 6892. Fibre Crystal Growth 6913. Illustration of Our Approach for Yb3+ 6934. Analysis of Concentration Quenching Processes 7015. Model to Interpret Radiation Self-Trapping and Self-Quenching

Mechanisms in Yb3+ 7116. Conclusion 713

Acknowledgements 713References 714

-doped Crystals

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23. TABLE-TOP SOFT X-RAY LASERS AND THEIRAPPLICATIONS 715(Giuseppe Tomassetti)Abstract 7151. Introduction 7152. Pumping Techniques 716

References 719

24. RARE EARTH ION DOPED CERAMIC LASER MATERIALS 721(Xuesheng Chen)1. Introduction 7212. Nd doped Ceramic YA 7213. New Lead-based Ceramic Laser Materials 7244. Summary 731

References 731

25. SHORT SEMINARS

CONFOCAL FLUORESCENCE AND RAMAN MICROSCOPY OFFEMTOSECOND LASER-MODIFIED FUSED SILICA 733

Wilbur J. Reichman, James W. Chan, and Denise M. Krol

OPTICAL CHARACTERIZATION OF QUANTUM DOTS 733Francisco Rafael Leon, Denis M. Krol, and Thomas Huser

NEW PHOSPHORS FOR ULTRAVIOLET EXCITATION 734P. Vergeer and A. Meijerink

MAIN TOPICS OF INTERESTS IN THE AREA OFLUMINESCENCE MATERIALS 734

Artur Bednarkiewicz and Dariusz Hreniak

INTERACTION OF FEMTOSECOND PULSES WITHTRANSPARENT MATERIALS 735

Rafael Gattass and Iva Maxwell

ULTRAFAST PHASE TRANSITIONS IN SOLIDS 735Maria Kandyla

RELAXATION PATHWAYS FROM ELECTRONIC EXCITEDSTATES OF OXYGEN DEFICIENT CENTERS IN GE-DOPEDSILICA 736

A. Cannizzo and M. Leone

DETECTING QUANTUM SIGNATURES IN THE DYNAMICS OFTRAPPED IONS 737

B. Militello, A. Napoli and A. Messina

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NON-EQUILIBRIUM POLARIZATION IN DIELECTRICS ANDRELATED PHENOMENA 738

V.A. Trepakov

OPTICAL TRANSITIONS IN QUANTUM NANOSTRUCTURESBASED ON IONIC MATERIALS 739

O. Proshina, I. Ipatova, and A. Maslov

LEDS MAKE THINGS BETTER 740Cees Ronda

26. POSTERS

PHOTOREFLECTANCE AND LUMINESCENCE MEASUREMENTSOF GAINNAS/GAAS MULTIPLE QUANTUM WELLSTRUCTURES 741

Andreas Grau, Michael Hetterich, and Claus Klingshirn

SELF-CONSISTENT CALCULATION OF GROUND AND EXCITEDENERGY LEVELS OF A DOPED QUANTUM DOT BY AQUANTUM GENERIC ALGORITHM 741

Mehmet Sahin, Ulfet Atav, and Mehmet Tomak

THE WIRES DIRECTION PHOTOCONDUCTIVITY OFGAAS/ALGAAS QUANTUM WIRES MEASURED ALONG 742

Miroslav Saraydarov

HIGHER EXCITATION SPECTROSCOPY OF ZnO 742H. Priller, J. Brückner, Th. Gruber, C. Klingshirn, H. Kalt, and A. Waag

PROPERTIES OF PECVD a-SiOX:H FILMS 743A.O. Kodolbas, A. Bacioglu, and O. Oktu

OPTICAL INVESTIGATION OF SPIN INJECTION INTOOPTICALLY ACTIVE NANOSTRUCTURES 743

Daniel Troendle, Robert Hauschild, Hendrik Burger, and Heinz Kalt

ULTRAFAST PHASE TRANSITIONS IN SOLIDS 743Maria Kandyla

STIMULATED EMISSION OF Nd0.5La0.5Al3(BO3)4 RANDOM LASERAND THE THRESHOLD CONDITIONS FOR LARGE ANDSMALL PUMPING REGIMES 744

K.J. Morris, M. Bahoura, G. Zhu, and M.A. Noginov

SPECTROSCOPY AND OPTICAL MICROSCOPY WITH NANO-LOCAL LIGHT SOURCES 745

Jinquan Liu, Andrea Callegari, Jerome Morville, Dino Tonti,Awos Alsalman, and Majed Chergui

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THE SIZE-EFFECT AND PHASE TRANSITIONS-EFFECT ONLUMINESCENCE PROPERTIES OF BaTiO3:Eu3+ NANO-CRYSTALLITES PREPARED BY THE SOL-GEL METHOD 745

D. Hreniak, W. Strek, G. Boulon, and R. Pa̧zik

ENERGY TRANSFER IN Nd3+ AND Yb3+ DOPOPED NANO-METRIC YAG CERAMICS 746

Artur Bednarkiewitz and Wieslaw Strek

ENVIRONMENT AND SHAPE EFFECTS ON DYNAMICS OF CdSeNANOCRYSTALS: COMPARING QUANTUM DOTS AND RODS 746

Camilla Bonati, Mona Mohamed, Dino Tonti, Jinquan Liu, and Majed Chergui

GAMMA AND PROTON IRRADIATION EFFECTS ON KU1QUARTZ GLASS 747

M. R. Nemtanu and B. Constantinescu

FEATURES OF FEMTOSECOND LASER ABLATION OF SOLIDTARGETS 747

M. Vitiello, S. Amoruso, R. Bruzzese, N. Spinelli, R. Velotta,X. Wang, C. Altucci, and C. de Lisio

STUDY OF THE SURFACE OF SrTiO3 SINGLE CRYSTALS BYOPTICAL SECOND HARMONIC GENERATION 748

G. Cerrone, L. Marrucci, F. Miletto, D. Paparo, and U. Scotti di Uccio

DLS MEASUREMENT OF NANOMETRIC CARBON CLUSTERSPRODUCED IN LAMINAR PREMIXED FLAMES 749

A. Bruno, D. Cecere, P. Minutolo, and A. D’Alessio

INDEX 751

00 H

t

t w H

%:

La nature de notre esprit nous porte a chercherl'essence ou le 'pourquois' des choses.L'experience nous apprend bientot que nousne devons pas aller au dela du 'comment'.

Claude Bernard

PREFACE

This book presents an account of the course "Frontiers of Optical Spectroscopy," held inErice, Sicily, Italy, from May 16 to June 1, 2003. This meeting was organized by theInternational School of Atomic and Molecular Spectroscopy of the "Ettore Majorana"Centre for Scientific Culture.

Advanced spectroscopic techniques allow the probing of very small systems and very fastphenomena, conditions that can be considered "extreme" at the present status of ourexperimentation and knowledge. Quantum dots, nanocrystals, and single molecules areexamples of the former and events on the femtosecond scale examples of the latter. Thepurpose of this institute was to examine the realm of phenomena of such extreme type andthe techniques that permit their investigations.

The technical advances have enabled the observation of new phenomena such as high-harmonic generation in atoms, metrology using femtosecond lasers, observation ofentangled states in semiconductor quantum dots (a prerequisite for quantum computing),Bose-Einstein condensation, light as slow as a bicyclist, and many more. The fruitful cross-fertilization of optical techniques and phenomena in physical and chemical systems was themotivation of this Institute.

Each lecturer aimed at developing a coherent section of the program starting at a somewhatfundamental level and ultimately reaching the frontier of knowledge in the field in asystematic and didactic fashion. The formal lectures were complemented and illustrated byadditional seminars and discussions. The course was addressed to workers inspectroscopy-related fields from universities, laboratories, and industries. Senior scientistswere encouraged to participate.

The Institute provided the participants with an opportunity to present their research work inthe form of short seminars or posters.

The participants came from 15 different countries: Belarus, Bulgaria, Denmark, France,Germany, Israel, Italy, The Netherlands, Romania, Russia, Spain, Sweden, Switzerland,Turkey, and United States.

There were 18 formal lectures, one interdisciplinary lecture, and 5 long seminars. Inaddition, 11 short seminars and 16 posters were presented. Two round-table discussionswere held. The first round-table discussion took place during the first week of the school inorder to evaluate the work done and consider suggestions and proposals regarding theorganization, format and presentation of the lectures. The second round-table discussionwas held at the conclusion of the course, so that the participants could comment on the

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work done during the entire meeting and discuss various proposals for the next course ofthe International School of Atomic and Molecular Spectroscopy.

The full-text lectures/long seminars and the abstracts of short seminars and posters arereported in this book.

The secretary of the course was Ottavio Forte.

I wish to acknowledge the sponsorship of the meeting by NATO, NASA, the ENEAOrganization, Boston College, the Italian Ministry of University and Scientific Researchand Technology, the USA National Science Foundation, and the Sicilian RegionalGovernment.

I would like to thank the Co-Director of the Course, Academian Alexander Voitovich, themembers of the organizing committee (Prof. Martin Wegener, Dr. Giuseppe Baldacchini,Prof. Claus Klingshirn, Dr. Cees Ronda, Prof. Eric Mazur, Dr. James Barnes, Dr. NormanBarnes, Prof. Ralph von Baltz, and Prof. Steve Arnold), the secretary of the course (Mr.Ottavio Forte) and Prof. Xuesheng Chen for their help in organizing and running thecourse.

A special thank you goes to my brother Francesco who received all the participants in hishouse for a social gathering.

I am looking forward to our activities at the Majorana Centre in years to come, includingthe next 2005 meeting of the International School of Atomic and Molecular Spectroscopy.

Baldassare (Rino) Di BartoloDirector of the International School ofAtomic and Molecular Spectroscopy ofthe "Ettore Majorana" Center

NOTE: During the preparation of this volume we received the sad news of theuntimely death of Dr. James Barnes. The paper whose abstract appears on page 687will be his last contribution to our schools. We shall always remember hisenthusiastic participation in our meetings, his gentlemanly courtesy and his warmfriendship.

LIST OF PAST INSTITUTES

Advanced Study Institutes Held at the “Ettore Majorana” Centre in Erice, Sicily, Italy, Organizes by the International School of Atomic and Molecular Spectroscopy

1974 – Optical Properties of Ions in Solids 1975 – The Spectroscopy of the Excited State 1977 – Luminescence of Inorganic Solids 1979 – Radiationless Processes 1981 – Collective Excitations in Solids 1983 – Energy Transfer Processes in Condensed Matter 1985 – Spectroscopy of Solid-State Laser Type Materials 1987 – Disordered Solids: Structures and Processes 1989 – Advances in Nonradiative Processes 1991 – Optical Properties of Excited State in Solids 1993 – Nonlinear Spectroscopy of Solids: Advances and Applications 1995 – Spectroscopy and Dynamics of Collective Excitations in Solids 1996 – Workshop on Luminescence Spectroscopy 1997 – Ultrafast Dynamics of Quantum Systems: Physical Processes and Spectroscopic Techniques 1998 – Workshop on Advances in Solid State in Luminescence Spectroscopy 1999 – Advances in Energy Transfer Processes 2000 – Workshop on Advanced Topics in Luminescence Spectroscopy 2001 – Spectroscopy of Systems with Spatially Confined Structures 2002 – Workshop on the Status and Prospects of Luminescence Research

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