Y. V. G. S. Murti C. Vijayan Physics of Nonlinear Optics Second Edition Physics of Nonlinear Optics Y. V. G. S. Murti C. Vijayan (cid:129) Physics of Nonlinear Optics Second Edition 123 Y.V.G.S.Murti C. Vijayan Formerly, atDepartment of Physics Department ofPhysics Indian Institute of Technology Madras Indian Institute of Technology Madras Chennai, Tamil Nadu,India Chennai, Tamil Nadu,India ISBN978-3-030-73978-2 ISBN978-3-030-73979-9 (eBook) https://doi.org/10.1007/978-3-030-73979-9 JointlypublishedwithANEBooksIndia ISBNoftheCo-Publisher’sedition:978-9-383-65663-9 1stedition:©AneBooksPvt.Ltd.2016 2ndedition:©TheEditor(s)(ifapplicable)andTheAuthor(s),underexclusivelicensetoSpringerNature SwitzerlandAG2021 Thisworkissubjecttocopyright.AllrightsaresolelyandexclusivelylicensedbythePublisher,whether thewholeorpartofthematerialisconcerned,specificallytherightsoftranslation,reprinting,reuseof illustrations, recitation, broadcasting, reproduction on microfilms or in any other physical way, and transmissionorinformationstorageandretrieval,electronicadaptation,computersoftware,orbysimilar ordissimilarmethodologynowknownorhereafterdeveloped. The use of general descriptive names, registered names, trademarks, service marks, etc. in this publicationdoesnotimply,evenintheabsenceofaspecificstatement,thatsuchnamesareexemptfrom therelevantprotectivelawsandregulationsandthereforefreeforgeneraluse. Thepublishers,theauthors,andtheeditorsaresafetoassumethattheadviceandinformationinthis book are believed to be true and accurate at the date of publication. Neither the publishers nor the authorsortheeditorsgiveawarranty,expressorimplied,withrespecttothematerialcontainedhereinor for any errors or omissions that may have been made. The publishers remain neutral with regard to jurisdictionalclaimsinpublishedmapsandinstitutionalaffiliations. ThisSpringerimprintispublishedbytheregisteredcompanySpringerNatureSwitzerlandAG Theregisteredcompanyaddressis:Gewerbestrasse11,6330Cham,Switzerland “...Jyotirgamaya...” (Lead, kindly, to light !) BrhadAraNyaka Upanishad Preface to Second Edition Thefirsteditionofthisbook,publishedin2014,waswelcomedenthusiasticallyand appreciatedbystudents,researchers,andteachersofnonlinearoptics.Asthereisa demand for thenextedition, it isquite naturalto take note of theseveral advances that have occurred in the subject over the past five years and to decide which of these are appropriate for inclusion at the textbook level, in view of the funda- mentalnatureandthesignificanceofthesubjectarea.Thisistheprimemotivation of bringing out a revised second edition. Among the newer mechanisms and materials, we introduce supercontinuum generation, which arises from an excellent interplay of the various mechanisms of opticalnonlinearity,mostofwhichwereincludedinthefirstedition.So,itisquite naturaltoincludethistopicintherequireddetailinthesecondedition.Anotherarea of optical nonlinearity, owing origin to basic nonlinear light–matter interaction, is that of multi-photon microscopy, which has demonstrated the potential to revolu- tionize applications in medical imaging and materials characterization. So, a full chapter has been added on this important emerging area of nonlinear optics. Our sincerehope isthat themodifications and new additions will render thebook even more useful to the beginner in nonlinear optics. Several colleagues and students have helped in shaping up the second edition of the book, and feedback on the first edition from many readers was a valuable input indeed. In addition, I am particularly grateful to my Ph.D. student Ms. Gayathri Radhakrishnan for contributing the newly added part on supercon- tinuum generation and for designing the cover page of this book. Chennai, India Y. V. G. S. Murti C. Vijayan vii Preface to First Edition Nonlinearopticalinteractionofmatterwithintenseopticalfieldsformsthebasisof Photonics and holds the key to a deep and comprehensive understanding of light-matter interaction as well as to the development of several significant facets of the technology of tomorrow. Training of students equipped with a clear understandingofthebasic Physicsinvolvedandenthusiasticawarenessofthevast scopeofthefieldappeartobemoreessentialthaneverinviewoftherequirements for the delineation of the basic physical mechanisms as well as the optimal exploitation of the application potential in areas such as control, communication, and computing. AninterestingobservationabouttheavailablebooksonNonlinearOpticstoday isthewidevarietyincontent,style,coverageofspecifictopics,relativeemphasisof areas and the depth of treatment. Excellent classics on this topic by Bloembergen, Boyd, Shen, Butcher and Cotter, Yariv are resources providing adequate coverage and for researchers. insight. The handbooks by Sutherland and Paras Prasad, Fischer,andZyssandChemlaandthebookonNonlinearFiberopticsbyAgrawal arealsoworthspecialmention.Worthyofspecialmentionisaveryusefulresource letter published recently, listing the details of all text books, reviews and other documents related to nonlinear optics with brief descriptions on each. Details of these and the recent books are given in the bibliography. However,whileteachingcoursesonnonlinearopticstostudentsofbothscience andengineeringduringthepasttwodecades,theauthorshavefeltastrongneedfor an introductory level book that caters to the requirements of students at the level of the bachelors and masters courses. This book is a humble attempt in this direction and is presented as a textbook designed at college/University level for undergraduate students of Science and Engineering and a one semester course can easilybedesignedbasedonthis.Carehasbeentakentoincluderigorouslyfeatures such as: (cid:129) elucidation of relevant basic principles of Physics. (cid:129) clear exposition of the ideas involved at the beginners’ level. (cid:129) coverage of the physical mechanisms of nonlinearity. ix x PrefacetoFirstEdition (cid:129) overview of physical processes in emerging photonic materials. (cid:129) exploratory questions and problems at the end of the chapters. The topics covered include a detailed formalism and phenomenology of non- linear wave mixing processes, quantum mechanics of nonlinear interaction of matter and radiation and an elucidation of specific processes as harmonic genera- tion, optical phase conjugation, selffocusing, self phase modulation and nonlinear absorption,leadingtoanappreciationoftheirapplicationpotentialinareassuchas tunable laser action, pulse modification, photonic switching and bistability. Major highlights of the book are detailed chapters on the symmetry aspects in nonlinear opticsandonthevariousspecificphysicalmechanismsofopticalnonlinearitywith examplesofmaterialsystemsinwhichtheseareoperative,takingcaretointroduce emerging trends as well. However, an exhaustive coverage of all nonlinear optical phenomenaisnotattemptedandtopicssuchasRamanandBaudouinscatteringare not included. The authors are pleased to place on record the beneficial interactions with stu- dents and fellow teachers in the evolution of this book. Specifically, inputs from Professors R. Vijaya, IIT, Kanpur, C. V. Krishnamurthy and Edamana Prasad, IIT Madras,RejiPhilip,IISc,Bangalore,MajlesAra,TTU,TeheranandP.Nandakumar, BITSGoaandaregratefullyacknowledged.Sincerethanksarealsoduetostudents Dileep,RadhikaV.Nair,JaisTomandRadhuandpostdoctoralfellowDr.AnitaR. Warrierforacarefulproofreadingofthemanuscript. The authors have been rather slow in putting the book together and the book could not have taken the shape but for the kind indulgence of the publishers, Ane Books Pvt Ltd, and particularly Mr. A. Rathinam. Chennai, India Y. V. G. S. Murti C. Vijayan Contents 1 From Optics to Photonics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1 1.1 The Charm and Challenge of Photonics . . . . . . . . . . . . . . . . . . . 1 1.2 The Nature of Optical Nonlinearity . . . . . . . . . . . . . . . . . . . . . . 3 1.3 Overcoming the Materials Bottleneck. . . . . . . . . . . . . . . . . . . . . 4 1.4 The Expanding Frontiers. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 5 1.5 Explorations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6 2 A Phenomenological View of Nonlinear Optics. . . . . . . . . . . . . . . . . 9 2.1 Optics in the Nonlinear World. . . . . . . . . . . . . . . . . . . . . . . . . . 9 2.1.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 9 2.1.2 First-Order Susceptibility . . . . . . . . . . . . . . . . . . . . . . . 11 2.1.3 Second-Order Susceptibility . . . . . . . . . . . . . . . . . . . . . 11 2.1.4 Third-Order Susceptibility. . . . . . . . . . . . . . . . . . . . . . . 12 2.2 Time Domain Response . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13 2.2.1 First-Order Polarization—Time Domain Response . . . . . 13 2.2.2 Higher-Order Polarizations—Time Domain Response. . . 14 2.3 Frequency Domain Response. . . . . . . . . . . . . . . . . . . . . . . . . . . 16 2.3.1 First-Order Susceptibility . . . . . . . . . . . . . . . . . . . . . . . 16 2.3.2 Second-Order Susceptibility . . . . . . . . . . . . . . . . . . . . . 17 2.3.3 General Order (n) Susceptibility . . . . . . . . . . . . . . . . . . 18 2.4 The nth-Order Polarization . . . . . . . . . . . . . . . . . . . . . . . . . . . . 18 2.5 Monochromatic Waves . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19 2.6 Calculation of the Factor K . . . . . . . . . . . . . . . . . . . . . . . . . . . . 21 2.6.1 Optical Rectification. . . . . . . . . . . . . . . . . . . . . . . . . . . 21 2.6.2 Second-Harmonic Generation . . . . . . . . . . . . . . . . . . . . 22 2.6.3 Pockels Effect . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22 2.6.4 Sum and Difference Frequency Generation . . . . . . . . . . 22 2.6.5 Third-Harmonic Generation. . . . . . . . . . . . . . . . . . . . . . 23 2.6.6 Non-degenerate Four-Wave Mixing. . . . . . . . . . . . . . . . 23 2.7 Explorations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24 xi xii Contents 3 Symmetry and Susceptibility Tensors . . . . . . . . . . . . . . . . . . . . . . . . 27 3.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27 3.2 Crystal Symmetry and Susceptibility Tensors . . . . . . . . . . . . . . . 28 3.2.1 Neumann Principle. . . . . . . . . . . . . . . . . . . . . . . . . . . . 32 3.2.2 Symmetry of Second-Order Susceptibility . . . . . . . . . . . 34 3.2.3 Second-Harmonic Generation . . . . . . . . . . . . . . . . . . . . 36 3.2.4 Kleinman Symmetry. . . . . . . . . . . . . . . . . . . . . . . . . . . 40 3.2.5 Symmetry of Third-Order Susceptibility . . . . . . . . . . . . 41 3.3 The Dielectric Permittivity Tensor . . . . . . . . . . . . . . . . . . . . . . . 43 3.4 The Refractive Index Ellipsoid . . . . . . . . . . . . . . . . . . . . . . . . . 45 3.5 Explorations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47 4 Calculation of Nonlinear Susceptibilities . . . . . . . . . . . . . . . . . . . . . . 49 4.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49 4.1.1 Physical Quantities in Quantum Physics . . . . . . . . . . . . 50 4.1.2 The Projection Operator . . . . . . . . . . . . . . . . . . . . . . . . 50 4.2 The Equation of Motion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 52 4.3 Ensembles of Particles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 54 4.4 Time-Dependent Perturbation . . . . . . . . . . . . . . . . . . . . . . . . . . 55 4.5 Dipolar Interaction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56 4.6 First-Order Density Matrix . . . . . . . . . . . . . . . . . . . . . . . . . . . . 58 4.7 Second-Order Density Matrix . . . . . . . . . . . . . . . . . . . . . . . . . . 58 4.8 Third-Order Density Matrix. . . . . . . . . . . . . . . . . . . . . . . . . . . . 60 4.9 Double Integrals in the Expressions for Density Matrix. . . . . . . . 61 4.10 Second-Harmonic Susceptibility. . . . . . . . . . . . . . . . . . . . . . . . . 62 4.11 Relaxation Effects. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 64 4.12 Applications to Color Centers . . . . . . . . . . . . . . . . . . . . . . . . . . 64 4.12.1 Third-Order Susceptibility. . . . . . . . . . . . . . . . . . . . . . . 64 4.12.2 Second-Order Susceptibility . . . . . . . . . . . . . . . . . . . . . 66 4.13 Explorations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 67 5 Nonlinear Wave Mixing Processes . . . . . . . . . . . . . . . . . . . . . . . . . . 69 5.1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 69 5.2 Elements of Electromagnetism. . . . . . . . . . . . . . . . . . . . . . . . . . 70 5.3 Traveling Electromagnetic Waves in Free Space. . . . . . . . . . . . . 72 5.3.1 Energy Density in the Traveling Wave . . . . . . . . . . . . . 74 5.4 Propagation of Electromagnetic Waves in Linear Materials . . . . . 75 5.5 Propagation of Electromagnetic Waves in Nonlinear Materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77 5.5.1 The Wave Equation . . . . . . . . . . . . . . . . . . . . . . . . . . . 77 5.5.2 Energy Transfer Rate . . . . . . . . . . . . . . . . . . . . . . . . . . 78 5.6 Three-Wave Mixing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80 5.6.1 An Approximation . . . . . . . . . . . . . . . . . . . . . . . . . . . . 81