DOCSLIB.ORG

Nonlinear Optics of Semiconductor and Molecular Nanostructures; a Common Perspective

Total Page：16

File Type：pdf, Size：1020Kb

Download full-text PDF Read full-text
Nonlinear Optics of Semiconductor and Molecular Nanostructures; a Common Perspective Nonlinear optics of semiconductor and molecular nanostructures; a common perspective V. M. Axt and S. Mukamel Department of Chemistry, University of Rochester, Rochester, New York 14627 A unified microscopic theoretical framework for the calculation of optical excitations in molecular and semiconductor materials is presented. The hierarchy of many-body density matrices for a pair-conserving many-electron model and the Frenkel exciton model is rigorously truncated to a given order in the radiation field. Closed equations of motion are derived for five generating functions representing the dynamics up to third order in the laser field including phonon degrees of freedom as well as all direct and exchange-type contributions to the Coulomb interaction. By eliminating the phonons perturbatively the authors obtain equations that, in the case of the many-electron system, generalize the semiconductor Bloch equations, are particularly suited for the analysis of the interplay between coherent and incoherent dynamics including many-body correlations, and lead to thermalized exciton (rather than single-particle) distributions at long times. A complete structural equivalence with the Frenkel exciton model of molecular materials is established. [S0034-6861(98)00201-3] CONTENTS 1963; Stahl and Balslev, 1987; Haug and Koch, 1993). Intermediate charge-transfer excitons exist in mixed I. Introduction 145 donor-acceptor crystals (Merrifield, 1961; Pope and II. The Microscopic Many-Electron Model 147 Swenberg, 1982; Haarer and Phillpott, 1983; Petelenz, III. Generating Functions for Coupled Exciton-Phonon 1989; Dubovsky and Mukamel, 1992) and in conjugated Variables 150 molecules (Mukamel and Wang, 1992; Hartmann and IV. Coherent Dynamics of the Purely Electronic System 151 Mukamel, 1993; Mukamel et al., 1994; Takahashi and V. Phonon-Induced Incoherent Dynamics 154 Mukamel, 1994; Chernyak and Mukamel, 1995a, 1996a; VI. Comparison with the Semiconductor Bloch Hartmann et al., 1995; Bulovic´ et al., 1996; Bulovic´ and Equations 156 Forrest, 1996). VII. Comparison with the Frenkel Exciton Model 160 VIII. Concluding Remarks 163 Apart from the Coulomb interaction, which is mainly Acknowledgments 164 responsible for correlations, the interaction of the carri- Appendix A: Equations for Electron-Hole ers with phonons is also crucial for a detailed under- Generating Functions 164 standing of the dynamics of these systems. A variety of Appendix B: Generating Functions for Frenkel Excitons 166 theoretical methods has been developed to address Appendix C: Exciton Representation of Two-Exciton these issues, including the conventional sum-over-states Variables and Coupling Constants 167 approach,1 multiconfiguration self-consistent field Appendix D: Phonon-Induced Self-Energies theories,2 Bogoliubov transformations,3 the Bethe- for the Many-Electron System 168 Salpeter equation,4 ‘‘dressed’’-exciton theories,5 semi- Appendix E: Phonon-Induced Self-Energies phenomenological few-level models,6 nonequilibrium for Frenkel Excitons 170 Appendix F: Contraction Relations 170 1For the sum-over-states approach, see Soos and Ramasesha, 1984, 1988; Yaron and Silbey, 1992; Abe et al., 1993; Soos I. INTRODUCTION et al., 1993; Soos et al., 1994; Chen and Mukamel, 1995; Chen et al., 1996; and Mukamel and Chemla, 1996. Optical measurements provide a tremendous insight 2For multiconfiguration self-consistent field theories, see into the electronic structure of various materials (Muka- Olsen and Jo”rgensen, 1985; Meyer et al., 1990; and Jaszun´ ski mel and Chemla, 1996). At moderate excitation densi- et al., 1993. ties, the basic physics tested by such experiments per- 3For the Bogoliubov transformations, see Comte and Mahler, formed on semiconductors, conjugated polymers, and 1986, 1988. 4 molecular aggregates is the dynamics of photogenerated For the Bethe-Salpeter equation, see Schmitt-Rink and Chemla, 1986; Chernyak et al., 1995. carriers forming correlated structures such as excitons or 5 biexcitons in either bound or unbound states. In ideal For the dressed-exciton theories, see Combescot and Comb- escot, 1989; Combescot and Betbeder-Matibet, 1990; Combes- molecular crystals, intermolecular charge transfer is not cot, 1992. possible and each molecule retains its own electrons. 6For the semi-phenomenological few-level models, see Dixit The elementary excitations in this case are tightly bound et al., 1990; Bar-Ad and Bar-Joseph, 1991, 1992; Lucht et al., electron-hole pairs known as Frenkel excitons (Davy- 1992; Mazumdar et al., 1992; Wu et al., 1992; Guo et al. 1993; dov, 1971). The loosely bound pairs in semiconductors Luo et al., 1993; Bott et al., 1993; Finkelstein et al., 1993; Guo, form hydrogen-atom-like Wannier excitons (Haken, 1994; Mayer et al., 1994). Reviews of Modern Physics, Vol. 70, No. 1, January 1998 0034-6861/98/70(1)/145(30)/$21.00 © 1998 The American Physical Society 145 146 Axt and Mukamel: Nonlinear optics of semiconductor... Green’s functions,7 and density-matrix theory.8 Density- In the present paper we consider a general model of matrix theory has become the method of choice in the many-electron systems whose Hamiltonian conserves treatment of experiments with ultrashort pulses because the number of electron-hole pairs and whose ground dealing with dynamic variables that are directly related state is therefore given by the Hartree-Fock ground to observables and that depend only on a single time state (a single Slater determinant). The system is further argument provides a very intuitive picture of the time- linearly coupled to a phonon bath. This model provides dependent material response. a unified treatment of semiconductors, molecules with The simplest level of theory is based on equations of weakly correlated electronic structure, and molecular motion for the reduced single-particle (two-point) den- aggregates. We introduce a hierarchy of exciton-phonon sity matrix. The optical polarization may be calculated generating functions, each representing a given exciton using this density matrix, which constitutes the minimal density matrix, and constituting a wave packet in pho- level of necessary information. The semiconductor non coordinates. We shall show that, to third order in Bloch equations (Haug and Koch, 1993), which are at the radiation field, the hierarchy can be truncated at the the heart of semiconductor optics, are derived within six-point-density-matrix level. We derive closed equa- this framework. The treatment of intermediate (charge- tions of motion for the relevant generating functions, transfer) excitons in conjugated polymers using the representing a formally rigorous description of the opti- single-particle density matrix allowed the interpolation cal response up to third order in the laser field including between molecular (Frenkel) limits (Mukamel, 1994) phonons. Taking these equations as a starting point, we and semiconductor (Wannier) limits (Mukamel and work out a reduced scheme, based on eliminating the Wang, 1992; Hartmann and Mukamel, 1993; Mukamel phonon degrees of freedom perturbatively. et al., 1994; Takahashi and Mukamel, 1994; Chernyak Optical excitations of molecular crystals, superlattices, and Mukamel, 1995a, 1995b, 1996b; Hartmann et al., and aggregates are usually formulated taking Frenkel 1995; Tretiak et al., 1996a). One of the major obstacles excitons rather than fermions as the basic entities. How- for a microscopic comparison of various materials is that ever, we shall demonstrate that the resulting dynamic molecular systems are usually discussed using the global equations can be recast in a form structurally equivalent (many-electron) eigenstates in real space, whereas semi- to the dynamics of the many-electron model, thus re- conductors are analyzed using elementary excitations vealing most clearly the fundamental similarities be- (quasiparticles) in k space. Treating all systems accord- tween the underlying physics of molecular and semicon- ing to the same basic strategy yields equations of motion ductor materials. The Frenkel exciton model is simpler, whose structural similarities most clearly reflect the since each exciton is represented by a single degree of common aspects of the underlying physics and thus al- freedom related to the center-of-mass motion of the lows for a systematic comparison of the remaining dif- pair. In semiconductors we need an additional coordi- ferences. An improved level of theory is obtained by nate representing the pair’s relative motion. The formal retaining higher-order (four-point, six-point, etc.) den- equivalence of the underlying dynamics provides a sim- sity matrices. This extension is essential in order to treat pler view of semiconductor optics and allows the clear two-exciton dynamics properly. Using a model Hamil- interpretation of many effects and levels of reduction tonian that conserves the number of electron-hole pairs, using the Frenkel exciton Hamiltonian, which is consid- it has been shown that for both Frenkel excitons erably simpler. Higher levels of modeling, which are (Dubovsky and Mukamel, 1991; Knoester and Muka- very tedious for semiconductors, are quite workable for mel, 1991; Leegwater and Mukamel, 1992; Mukamel, molecular systems. Consequently theoretical studies of 1994; Chernyak et al., 1995) and Wannier excitons (Axt molecular materials are more advanced than their semi- and Stahl, 1994a, 1994b; Lindberg et al., 1994; Maialle conductor counterparts. Experimental studies of semi- and Sham, 1994; Victor et al., 1995; Axt, Victor, and conductor nanostructures
Load more

Recommended publications
  • General Formalism for Excitonic Absorption Edges in Confined Systems with Arbitrary Dimensionality P
    General formalism for excitonic absorption edges in confined systems with arbitrary dimensionality P. Lefebvre, Philippe Christol, H. Mathieu To cite this version: P. Lefebvre, Philippe Christol, H. Mathieu. General formalism for excitonic absorption edges in confined systems with arbitrary dimensionality. Journal de Physique IV Proceedings, EDP Sciences, 1993, 03 (C5), pp.C5-377-C5-380. 10.1051/jp4:1993579. jpa-00251666 HAL Id: jpa-00251666 https://hal.archives-ouvertes.fr/jpa-00251666 Submitted on 1 Jan 1993 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. JOURNAL DE PHYSIQUE IV Colloque C5,supplement au Journal de Physique 11, Volume 3, octobre 1993 General formalism for excitonic absorption edges in confined systems with arbitrary dimensionality P. LEFEBVRE, l? CHRISTOL and H. MATHIEU Groupe d'Etudes des Semiconducteurs, CNRS, Universitk Montpellier I& Case coum'er 074, 34095 Montpellier cedex 5, France A metric space with a noninteger dimension a (1 < a) is used to describe bound and unbound states of strongly anisotropic Wannier-Mott excitons, such as those confined in semiconductor superlattices, quantum wells and quantum-well wires. Indeed, the relative motion of the electron- hole pair which constitutes such excitons can never be considered strictly ID, 2D or 3D.
    [Show full text]
  • Nanoplatelets As Material System Between Strong Confinement And
    Nanoplatelets as material system between strong confinement and weak confinement Marten Richter1, ∗ 1Institut f¨urTheoretische Physik, Nichtlineare Optik und Quantenelektronik, Technische Universit¨atBerlin, Hardenbergstr. 36, EW 7-1, 10623 Berlin, Germany (Dated: October 18, 2018) Recently, the fabrication of CdSe nanoplatelets became an important research topic. Nanoplatelets are often described as having a similar electronic structure as 2D dimensional quantum wells and are promoted as colloidal quantum wells with monolayer precision width. In this paper, we show, that nanoplatelets are not ideal quantum wells, but cover depending on the size: the strong confinement regime, an intermediate regime and a Coulomb dominated regime. Thus, nanoplatelets are an ideal platform to study the physics in these regimes. Therefore, the exciton states of the nanoplatelets are numerically calculated by solving the full four dimensional Schr¨odingerequation. We compare the results with approximate solutions from semiconductor quantum well and quan- tum dot theory. The paper can also act as review of these concepts for the colloidal nanoparticle community. In quantum dots the wave function of the electron and is the correct approach, if confinement dominates com- hole, that form the optically created exciton are con- pared to Coulomb interaction. Treatments with a chem- fined in all three dimensions resulting in a quasi zero ical background22 used a Frenkel exciton ansatz, which dimensional system with discrete states1{5. The chemi- does not reflect the properties of the more Wannier type cal synthesis of colloidal quantum dots is a very active excitons in the nanoplatelets. research field6{9, since the controlled growths of these A detailed look at the typical model ansatz wavefunc- materials lead to many real life applications like dyes for tions for platelets, previously known from quantum wells e.g.
    [Show full text]
  • Modeling of Interlayer Excitons in Van Der Waals Heterostructures
    Modeling of interlayer excitons in van der Waals heterostructures Simon Ovesen Department of Physics CHALMERS UNIVERSITY OF TECHNOLOGY Gothenburg, Sweden 2017 Master’s thesis 2017 Modeling of interlayer excitons in van der Waals heterostructures Simon Ovesen Department of Physics Division of Condensed Matter Theory Chalmers University of Technology Gothenburg, Sweden 2017 Modeling of interlayer excitons in van der Waals heterostructures Author: Simon Ovesen © Simon Ovesen, 2017. Supervisor: Ermin Malic, Department of Physics, Division of Condensed Matter Theory Examiner: Ermin Malic, Department of Physics, Division of Condensed Matter Theory Master’s Thesis 2017 Department of Physics Chalmers University of Technology SE-412 96 Gothenburg Telephone +46 31 772 1000 Cover: Illustration of the formation and radiative decay of interlayer excitons. Taken from [1]. Typeset in LATEX Gothenburg, Sweden 2017 iv Modeling of interlayer excitons in van der Waals heterostructures Simon Ovesen Department of Physics Chalmers University of Technology Abstract The field of TMD (Transition Metal Dichalcogenide) monolayers is an active one due to certain interesting properties such as a direct band gap, strong spin-orbit coupling and a remarkably large Coulomb interaction leading to strongly bound excitons. For technical applications heterostructures composed of stacked monolayers are also a huge topic of interest. Recent experimental studies of the photoluminescence of these structures show evidence of the existence of interlayer excitons. The aim of this thesis is to propose a mechanism for the formation and dynamics of these interlayer excitons in a bilayer heterostructure. For this purpose the second quantization formalism and tight binding approach are employed. Aside from the free, optical, carrier-photon, carrier-phonon and Coulomb interactions that have already been studied for monolayers, a tunneling interaction that couples the two layers is also included.
    [Show full text]
  • Deviations of the Exciton Level Spectrum in Cuprous Oxide from The
    Deviations of the exciton level spectrum in Cu2O from the hydrogen series F. Sch¨one,S.-O. Kr¨uger,P. Gr¨unwald, H. Stolz, and S. Scheel Institut f¨urPhysik, Universit¨atRostock, Albert-Einstein-Strasse 23, D-18059 Rostock, Germany M. Aßmann, J. Heck¨otter,J. Thewes, D. Fr¨ohlich, and M. Bayer Experimentelle Physik 2, Technische Universit¨atDortmund, D-44221 Dortmund, Germany Recent high-resolution absorption spectroscopy on excited excitons in cuprous oxide [Nature 514, 343 (2014)] has revealed significant deviations of their spectrum from that of the ideal hydrogen- like series. Here we show that the complex band dispersion of the crystal, determining the kinetic energies of electrons and holes, strongly affects the exciton binding energies. Specifically, we show that the nonparabolicity of the band dispersion is the main cause of the deviation from the hydrogen series. Experimental data collected from high-resolution absorption spectroscopy in electric fields validate the assignment of the deviation to the nonparabolicity of the band dispersion. PACS numbers: 71.35.Cc, 78.20.-e, 32.80.Ee, 33.80.Rv I. INTRODUCTION the band dispersion. Fluorescence spectra of atomic systems are an ex- II. VALENCE BAND DISPERSIONS IN tremely rich source of information about the interactions CUPROUS OXIDE of electrons and the nuclei, and their study laid the foun- dations of the development of quantum mechanics. The Cuprous oxide (Cu O) was historically the first ma- basic hydrogen dependence of the electron binding ener- 2 2 terial in which excitons were observed [7{9]. Their dis- gies of 1=n already turns out to be insufficient for al- covery, combined with the availability of exceptionally kali, i.e.
    [Show full text]
  • Optical Properties of Yellow Excitons in Cuprous Oxide
    Optical Properties of yellow Excitons in Cuprous Oxide Dissertation zur Erlangung des akademischen Grades doctor rerum naturalium (Dr. rer. nat.) der Mathematisch-Naturwissenschaftlichen Fakultät der Universität Rostock vorgelegt von Dipl.-Phys. Florian Schöne, geboren am .. in Rostock Rostock, den .. ii Gutachter: Prof. Dr. Heinrich Stolz (Universität Rostock, Institut für Physik) Prof. Dr. Frank Jahnke (Universität Bremen, Institut für Theoretische Physik) Datum der Einreichung: .. Datum der Verteidigung: .. iii Abstract Cuprous oxide (Cu2O) has proven historically as well as contemporarily to be one of the most suitable materials for the research of excitons in bulk semiconductors. This thesis concerns itself with the theoretical description of some optical properties of the yellow exciton series in Cu2O and is divided into two parts. The first part aims at the determination of the basic excitonic properties by considering central-cell corrections. For large principal quan- tum numbers n the nonparabolicity of the highest valence band is treated and the concept of quantum defects is introduced. For the analysis of the yellow 1S paraexciton the additional coupling to LO phonons is addressed. The second part examines the absorption edge of the Γ3− phonon-assisted transition into the 1S yellow orthoexciton and determines the correspond- ing deformation potential. The deformation potential is further utilised to calculate the Auger coefficient of the phonon-assisted decay mechanism. Zusammenfassung Kupferoxydul (Cu2O) zeigte sowohl historisch als auch in der Neuzeit, dass es eines der am besten geeigneten Materialien für die Untersuchung von Exzitonen in Halbleitern ist. Die vorliegende Dissertation untersucht einige optische Eigenschaften der gelben Exzitonenserie in Cu2O und lässt sich in zwei Teile unterteilen.
    [Show full text]
  • Optical Near Field Interaction of Spherical Quantum Dots
    OPTICAL NEAR FIELD INTERACTION OF SPHERICAL QUANTUM DOTS A THESIS SUBMITTED TO THE DEPARTMENT OF PHYSICS AND THE GRADUATE SCHOOL OF ENGINEERING AND SCIENCE OF BILKENT UNIVERSITY IN PARTIAL FULLFILMENT OF THE REQUIREMENTS FOR THE DEGREE OF MASTER OF SCIENCE By Togay Amirahmadov July, 2012 I certify that I have read this thesis and that in my opinion it is fully adequate, in scope and in quality, as a thesis for the degree of Master of Science. Assoc. Prof. Hilmi Volkan Demir (Supervisor) I certify that I have read this thesis and that in my opinion it is fully adequate, in scope and in quality, as a thesis for the degree of Master of Science. Prof. Oğuz Gülseren I certify that I have read this thesis and that in my opinion it is fully adequate, in scope and in quality, as a thesis for the degree of Master of Science. Assoc. Prof. Azer Kerimov Approved for the Graduate School of Engineering and Sciences: Prof. Levent Onural Director of Graduate School of Engineering and Sciences ii ABSTRACT OPTICAL NEAR FIELD INTERACTION OF SPHERICAL QUANTUM DOTS Togay Amirahmadov M.S. in Physics Supervisor: Assoc. Prof. Hilmi Volkan Demir July, 2012 Nanometer-sized materials can be used to make advanced photonic devices. However, as far as the conventional far-field light is concerned, the size of these photonic devices cannot be reduced beyond the diffraction limit of light, unless emerging optical near-fields (ONF) are utilized. ONF is the localized field on the surface of nanometric particles, manifesting itself in the form of dressed photons as a result of light-matter interaction, which are bound to the material and not massless.
    [Show full text]
  • Microscopic Theory of Coherent and Incoherent Optical Properties of Semiconductor Heterostructures
    Microscopic Theory of Coherent and Incoherent Optical Properties of Semiconductor Heterostructures Dissertation zur Erlangung des Doktorgrades der Naturwissenschaften (Dr. rer. nat.) dem Fachbereich Physik der Philipps-Universit¨at Marburg vorgelegt von Martin Sch¨afer aus Marburg Marburg(Lahn), 2008 Vom Fachbereich Physik der Philipps-Universit¨at Marburg als Dissertation angenommen am 25.08.2008 Erstgutachter: Prof. Dr. S.W. Koch Zweitgutachter: Prof. Dr. W. Stolz Tag der m¨undlichen Prfung: 02.09.2008 F¨ur Marianne Zusammenfassung W¨ahrend der letzten Jahrzehnte sind Halbleiter wegen ihrer interessanten elektrischen Eigenschaften zu einem wichtigen Grundmaterial f¨ur eine Vielzahl technologischer An- wendungen geworden. Halbleiter zeigen beispielsweise im Gegensatz zu Metallen eine mit der Temperatur ansteigende Leitf¨ahigkeit und es ist m¨oglich, die Leitf¨ahigkeit eines Halbleiters gezielt zu ver¨andern indem man ihn bewusst verunreinigt. Dieses soge- nannte Dotieren erlaubt es Bauteile mit genau definierten Leitf¨ahigkeitseigenschaften herzustellen. Beispiele f¨ur solche Bauteile sind Dioden und Transistoren. Letztere haben schließlich die Entwicklung moderner Computer erm¨oglicht. Ungl¨ucklicherweise f¨uhren dieselben physikalischen Prozesse, die eine gezielte Gestal- tung der elektronischen Charakteristika von Halbleiterbauelementen erlauben, dazu, dass Halbleitereigenschaften sehr sensitiv auf ungewollte Verunreinigungen reagieren. Deswegen bezeichnete Wolfgang Paul Anfang der 1920er Jahre die Halbleiterphysik als ”Dreckphysik”. Mit modernen Epitaxiemethoden ist es jedoch heute m¨oglich, Halblei- termaterialen auf einzelne Atomlagen genau zu wachsen und dabei eine sehr hohe Ma- terialreinheit zu erreichen [1]. Die interessanten elektrischen Eigenschaften von Halbleitern sind auf ihre spezielle Bandstruktur zur¨uckzuf¨uhren. Im Gegensatz zu Leitern und ¨ahnlich zu Isolatoren haben Halbleiter im Grundzustand ein g¨anzlich gef¨ulltes Valenzband und ein leeres Leitungs- band.
    [Show full text]
  • Appendix a TWO-LEVEL SYSTEMS and RATE EQUATIONS
    Appendix A TWO-LEVEL SYSTEMS AND RATE EQUATIONS Chapters 2 and 3 show that for semiconductor laser purposes, the in­ teraction of light with a semiconductor medium can often be modeled in terms of electronic transitions between a valence and a conduction band. A spread of transition energies occur that depend on the value of the car­ rier momentum k. Elsewhere in physics such a range of transitions is known to occur, namely in ensembles of inhomogeneously broadened two­ level systems. These appear to good approximation in the interaction of light with atoms and with the magnetic dipoles of nuclear magnetic reso­ nance. Hence people have been led to model semiconductor laser media using the theory of two-level systems. In appropriate limits, the two-level approaches reduce to rate equation theory, also very popular in modeling aspects of semiconductor laser operation. On the other hand, Sec. 3-1 rev­ eals that the semiconductor medium is at the very least an inhomogene­ ously broadened four-level medium, all of whose levels have appreciable probability in a gain medium. Two of the four levels correspond to the levels in a two-level medium, but the other two are absent in the two-level medium. Hence the degree to which a two-level model can describe semi­ conductor response is disturbingly uncertain. One is really better off using a real semiconductor model, for which the approximations are well de­ fined. Nevertheless much of the physics of the two-level model has coun­ terparts in the semiconductor models and one can study this physics in a relatively simple context.
    [Show full text]
  • Quantum Confined Rydberg Excitons in Reduced Dimensions
    Journal of Physics B: Atomic, Molecular and Optical Physics PAPER • OPEN ACCESS Quantum confined Rydberg excitons in reduced dimensions To cite this article: Annika Konzelmann et al 2020 J. Phys. B: At. Mol. Opt. Phys. 53 024001 View the article online for updates and enhancements. This content was downloaded from IP address 141.58.18.93 on 08/02/2020 at 01:26 Journal of Physics B: Atomic, Molecular and Optical Physics J. Phys. B: At. Mol. Opt. Phys. 53 (2020) 024001 (7pp) https://doi.org/10.1088/1361-6455/ab56a9 Quantum confined Rydberg excitons in reduced dimensions Annika Konzelmann , Bettina Frank and Harald Giessen 4th Physics Institute and Research Center SCoPE, University of Stuttgart, D-70569 Stuttgart, Germany E-mail: [email protected] Received 7 August 2019, revised 30 September 2019 Accepted for publication 12 November 2019 Published 18 December 2019 Abstract In this paper we propose first steps towards calculating the energy shifts of confined Rydberg excitons in CuO2 quantum wells, wires, and dots. The macroscopic size of Rydberg excitons with high quantum numbers n implies that already μm sized lamellar, wire-like, or box-like structures lead to quantum size effects, which depend on the principal Rydberg quantum number n. Such structures can be fabricated using focused ion beam milling of cuprite crystals. Quantum confinement causes an energy shift of the confined object, which is interesting for quantum technology. We find in our calculations that the Rydberg excitons gain a potential energy in the μeV to meV range due to the quantum confinement. This effect is dependent on the Rydberg exciton size and, thus, the principal quantum number n.
    [Show full text]
  • Analytical Quantitative Semi-Classical Approach to the Losurdo-Stark Effect and Ionization in 2D Excitons
    Analytical Quantitative Semi-Classical Approach to the LoSurdo-Stark Effect and Ionization in 2D excitons J. C. G. Henriques1, Høgni C. Kamban2;3, Thomas G. Pedersen2;3, N. M. R. Peres1;4 1Department and Centre of Physics, and QuantaLab, University of Minho, Campus of Gualtar, 4710-057, Braga, Portugal 2Department of Materials and Production, Aalborg University, DK-9220 Aalborg Øst, Denmark 3 Center for Nanostructured Graphene (CNG), DK-9220 Aalborg Øst, Denmark and 4International Iberian Nanotechnology Laboratory (INL), Av. Mestre José Veiga, 4715-330, Braga, Portugal (Dated: April 27, 2020) Using a semi-classical approach, we derive a fully analytical expression for the ionization rate of excitons in two-dimensional materials due to an external static electric field, which eliminates the need for complicated numerical calculations. Our formula shows quantitative agreement with more sophisticated numerical methods based on the exterior complex scaling approach, which solves a non-hermitian eigenvalue problem yielding complex energy eigenvalues, where the imaginary part describes the ionization rate. Results for excitons in hexagonal boron nitride and the A−exciton in transition metal dichalcogenides are given as a simple examples. The extension of the theory to include spin-orbit-split excitons in transition metal dichalcogenides is trivial. I. INTRODUCTION linear Riccati equation. Also, using the same mapping, Dolgov and Turbiner devised a numerical perturbative The LoSurdo-Stark effect has a venerable history in method [9], starting from an interpolated solution of the both atomic, molecular, and condensed matter physics Riccati equation, for computing the ionization rate at [1]. This effect refers to the modification of the position strong fields.
    [Show full text]
  • Exciton Photon and Phonon Interactions in Semiconductor Quantum Dots
    EXCITON PHOTON AND PHONON INTERACTIONS IN SEMICONDUCTOR QUANTUM DOTS By Kaijie Xu A DISSERTATION Submitted to Michigan State University in partial ful¯llment of the requirements for the degree of DOCTOR OF PHILOSOPHY Physics 2012 ABSTRACT EXCITON PHOTON AND PHONON INTERACTIONS IN SEMICONDUCTOR QUANTUM DOTS By Kaijie Xu Excitons, photons, and phonons are elementary excitations that have been widely investi- gated in semiconductor systems. This thesis focuses on the exciton energy transfer between quantum dots, which is a physical process that involves all these elementary excitations. Exciton energy transfer is a common process in many arti¯cial systems such as solar cells, lasers, and quantum gates. In order to study the exciton energy transfer, we develop a full quantum theory to de- scribe the exciton-photon interaction and exciton-phonon interaction. We derive the exciton- photon interaction from the quantized ¯eld operator representing the electromagnetic ¯eld. In the derivation, the e®ect of a planar cavity, which modi¯es the photon density of states is considered. We also obtain the exciton-phonon interaction starting from the deforma- tion potential. With both types of interaction given, we study the dynamics of the exciton transfer in a cavity by solving the SchrÄodingerequation for the coupled system of excitons, photons and phonons. Both elastic and inelastic exciton energy transfer are simulated. We ¯nd that the coupling to phonons enhances the exciton energy transfer when two dots are o®-resonant. In addition to the theoretical and numerical study of the exciton energy trans- fer, two applications of the theory are discussed. As an application to quantum computing, phonon-assisted exciton energy transfer is proposed as the key ingredient in the implementa- tion of a Quantum Zeno gate.
    [Show full text]
  • Quantum Field Theory of Exciton Correlations and Entanglement in Semiconductor Structures
    60 Quantum Field Theory of Exciton Correlations and Entanglement in Semiconductor Structures M. Erementchouk, V. Turkowski and Michael N. Leuenberger NanoScience Technology Center and Department of Physics, University of Central Florida USA 1. Introduction The usual ideology when dealing with many-body systems using second quantization is to treat elementary excitations, say electrons, as the main entities determining the physical properties of the system: the states are enumerated by population numbers, the response is described using Green’s functions defined in terms of the elementary excitation, and so on. The situation changes drastically when interaction allows for the formation of bound states. The whole view of the system has to be revisited. Perhaps the most famous example is given by superconductors. In the normal state the material fits the canonical universal description when, roughly speaking, most of the properties are explained (at least qualitatively) by the position of the Fermi level. In the superconducting state, however, one has complete reconstruction of the ground state. Now properties of the material are defined by Cooper pairs with behavior qualitatively different from that of individual electrons. For one the exclusion principle has significantly diminished effect, so that pairs can even condense. Such change in the character of elementary excitations leads to significant consequences: resistivity drops practically to zero. In the present chapter we review the basic approaches to treating such new states in semiconductors, where elementary excitations, electrons and holes, have opposite charge and the Coulomb attraction leads to formation of excitons, bound states of electron-hole pairs. Excitons are the major factor determining the semiconductor optical response below the fundamental absorption edge: they are responsible for resonant absorption at these frequencies, where in the absence of excitons the material would be transparent.
    [Show full text]