Cross-cutting Basic Research Needs for Solid-State Lighting from the DOE BES Workshop

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Cross-cutting Basic Research Needs for Solid-State Lighting from the DOE BES Workshop Jim Misewich Condensed Matter Physics and Materials Science Department Brookhaven National Lab

BES Basic Research Needs Workshops http://www.sc.doe.gov/bes/reports/list.html

Workshop on Basic Research Needs for SSL Chair: Julia Phillips, Sandia National Lab Co-Chair: Paul Burrows, Pacific Northwest National Lab Panel 1: LEDs Robert Davis (CMU) Jerry Simmons (Sandia) Panel 2: OLEDs George Malliaras (Cornell) Franky So (U. Florida) Panel 3: Cross-cutting Science, Novel Methods Jim Misewich (BNL) Arto Nurmikko (Brown) Darryl Smith (LANL)

Efficiency Heating: 70% Electric motors: 85-95% Lamps: much less! 1.5 Billion light bulbs sold/year (US) Incandescent lamp (19 th century): 5% Fluorescent lamp (20 th century): 20% Solid-state lighting (SSL): the direct conversion of electricity to white light using semiconducting materials 21 st century opportunities/needs efficiency Must have acceptable: Color quality, brightness, cost

Solid state lighting approaches LEDs OLEDs holes V electrons glass hole injection layer Hole electrode transporter ITO Blue emitter hole / exciton blocking layer cathode

Inefficiencies Accumulate Wall Plug Efficiency (E WP ) -- fraction of energy provided by power source that is converted to emitted light energy Injection Efficiency (E inj ) -- efficiency with which electrons & holes are injected into the active region Internal Quantum Efficiency (η int ) -- fraction of injected e-h pairs that become photons emitted inside the die Light Extraction Efficiency (C ext ) -- fraction of internally emitted photons that escape from the die E WP = E inj η int C ext Top Contact Other losses (for white SSL luminaire): Absorption by contacts, phosphors, encapsulants, etc. Phosphor Stokes shift Optical element losses Back Contact Active Layer

Chairs: Panelists: Panel 3: Cross-Cutting Science Jim Misewich (BNL) Arto Nurmikko (Brown U) Darryl Smith (LANL) Marc Achermann (U. Massachusetts at Amherst) Vladimir Agranovich (Russian Academy of Science) Len Buckley (NRL) Vladimir Bulovic (MIT) Francois Leonard (SNL) Tony Levi (USC) Shawn Lin (RPI) Lukas Novotny (U Rochester) Peter Littlewood (U of Cambridge) Garry Rumbles (NREL) Peidong Yang (UC Berkeley) Rashid Zia (Brown U) Identify priority research directions and grand challenges

Five Priority Research Directions Identified New functionality through heterogeneous nanostructures Innovative photon management Enhanced light-matter interaction Multiscale modelling for solid-state lighting Precision nanoscale characterization for SSL

Tunability: quantum confinement Nanoscale Materials

New Functionality Through Heterogeneous Nanostructures Overview Exploit new degrees of freedom in heterogeneous nanostructures to control fundamental physical processes important for SSL Develop new synthesis and assembly approaches for high quality nanostructured materials and heterostructures Explore the physics and chemistry of macroscopic area nanostructure arrays Integration of nanostructured materials in macroscopic SSL devices MOLECULES OPTIMIZED EXCITATION INTERACTION SPECTRAL TAILORING QUANTUM DOTS NANOSCALE CONTROL STRUCTURES NANOTUBES METAL ISLANDS Impact with success - High efficiency and color quality in solid state lighting through increased control of functionality at the nanoscale DIRECTED GROWTH ORDERED LAYERS

New Functionality Through Heterogeneous Nanostructures Science questions and opportunities Synthesis and Self-Assembly issues Size, composition, passivation and shape controlled synthesis of nanomaterials Environmentally acceptable nanomaterials (sustainable resources, scalable processes) Self-Assembly of nano-elements (organic, inorganic) into enhanced functional forms Understanding and Control of Radiative and Non-Radiative Processes What governs quantum efficiencies at the nanoscale? Manipulating and metering photons, excitons, polarons, phonons, and plasmons in nanostructures Coupled excitations in nanostructures (electron-photon, electron-phonon, ) Optical mode tailoring (directionality of emission, spectral tuning) Integration into SSL Structures Influence of nanostructures on the SSL device designs Array behavior of nanostructures (coupling, cross-talk, periodicity) Opportunities for thermal / mechanical management Enhanced operational stability Nanoscale materials in photonic structures

New Functionality Through Heterogeneous Nanostructures Recent advances illustrating promise of PRD Yang: dislocation-free nanowires enabled by the identical ETL,HTL,HBL for all QD-LEDs Cathode Electron Transport Hole Blocking Hole Transport Anode Glass Bulovic: organic/inorganic (QD) hybrid materials WHITE

Innovative Photon Management Overview Embedded emitter photonic nanostructures Control over final spectrum, polarization, and radiation pattern Bio-inspired optics and biomimetic approaches Tailoring the density of optical modes Nanostructured lens Photonic Downconverter Final spectrum & radiation pattern Impact with success Ultra-efficient, compact, high power light sources Paradigm shift in LED luminaire architectures Embedded & enhanced emitter

Innovative Photon Management Science questions and opportunities Ultra-high energy transfer into extracted light spectrum Spontaneous emission and thermal emission modification New luminaire concepts based on large-area nano-structured materials Photonic coupling to desirable down-conversion media Emitters with integrated lens capabilities Bio-inspired optics for large area illumination Potential research approaches Facile 3-D nanostructure fabrication techniques Full 3-D Maxwell solvers including photonics/plasmonics for efficient photon mgmt. Novel photothermally stable optical packaging materials

Innovative Photon Management Recent advances illustrating promise of PRD Enhanced radiative emission through DOS engineering Photonic nanostructure radiation pattern control Wierer et. al., Appl. Phys. Lett. 84, 3885 (2004). NoPX PX1 PX2 PX3 PX4 120 90 60 150 30 PRL 96, 113002 (2006) 180 0

Exploit new degrees of freedom (enabled by strong coupling) Novel control of photon-exciton hybridization Enhanced light-matter interactions Enhanced quantum efficiency by resonant light-matter interaction Manipulation of collective radiative effects in dense multifluorophore nanoparticle arrays Control of electron-photon interaction Impact with success: leading to dramatic advances and innovations in nanomaterial configurations for high efficiency LEDs

Enhanced light-matter interactions Science questions and opportunities (research needs) Integrated photon generation/extraction New approaches to high performance Organic/inorganic hybrids 3D-Microcavity confinement Nanoplasmonic enhancement Enable giant oscillator strength Control Energy Pathways Near-field induced transitions Directed Forster energy pathways Incoherent vs. coherent Forster processes Collective effects in high density quantum confined arrays Potential research approaches: Chemical synthesis of ordered nanocomposites Optimally designed 3D photonic resonators Light emitters with quantum-engineered giant oscillator strength smart spectrally adaptive emitters

Enhanced light-matter interactions Recent advances illustrating promise of PRD Kasprzak et al (2006) Coherent Polaritons in CdTe microcavities (low-t) Atay et al (2005) Fluorescence enhancement of CdSe/ZnS QD-plasmon nanoparticle composite

Multiscale modelling for solid state lighting Overview Hierarchical approach From primary quantum excitations to continuum dynamics Adaptive quantum design Multidimensional optimization Integrated device design Experimental validation 0.5 nm Impact of success Predictive models enabling full exploitation of opportunities in new materials Rational design for advanced concepts in solid state lighting Bulovic et al MIT 50nm 1 mm

Multiscale modelling for solid state lighting Science questions and opportunities (research needs) Predictive models for solid state lighting devices Disordered molecular materials Integrated optical and electronic models Ab-initio methods for excited states Kinetics and non-equilibrium phenomena Transport (energy, charge, light and heat) Potential research approaches Quantum design from basic principles Discovery of new physical phenomena Hierarchical models Primary quantum excitations (e.g. ab-initio quantum chemistry, density functional theory, quantum Monte Carlo) Large-scale, inhomogeneous model Hamiltonians (e.g. optical modes, hopping transport) Semiclassical dynamics (e.g. coupling to external reservoirs, phonons, kinetics, pumping) Device level models (e.g. rate equations, drift-diffusion ) Integrated device design Carrier injection, transport and dynamics Interfaces Experimental validation

Multiscale modelling for solid state lighting Recent advance quantum coherence in a planar microcavity Coherent light-matter interaction Bose-Einstein condensation of entangled light and matter Kasprzak et al. (2006)

Precision Nanoscale Characterization for SSL Overview Develop new structurally sensitive tools with resolution from molecules to materials. Imaging structure and function in operating SSL devices allowing for the measurement of local (nanoscale) properties In situ x-ray characterization of MOCVD at the APS Impact with success Provide unprecedented feedback and control for improved growth/synthesis. - Simultaneous measurements of different physical properties (e.g. optical, structural, and electronic) allowing for evaluating strategies of generation and extraction of photons.

Precision Nanoscale Characterization for SSL Science questions and opportunities Simultaneous structure and function Subsurface/buried interface imaging Quantification of Impurities/dopants/defects Unprecedented spatial and temporal resolution Non-invasive Chemically-specific 3d reconstruction - Novel combinations Potential research approaches Xray techniques including in situ microscopy, ultrafast time resolved scattering and spectroscopies, and inelastic scattering. Single molecule (particle) optical techniques using new interaction mechanisms (nonlinear optical, Raman,.. ). Nanoscale chemically-specific imaging with scanning probes including nearfield optical spectroscopy (IR, Raman). Advanced imaging tools for spin degrees of freedom. Electron and ion beam techniques with enhanced energy and spatial resolution for improved sensitivities to avoid sample damage.

Precision Nanoscale Characterization for SSL Recent advances illustrating promise of PRD Novotny: Near-field Raman spectroscopy Barbara: Single molecule spectroscopy in a functioning device ωo ωo + ωn ω N

Grand Challenge Rational design of solid-state lighting systems

Rational design of solid-state lighting systems Control for ultimate efficiency through: Designed optical properties Charge or energy transfer to lumophore Color Quality Luminance Color temp Dynamic Exciton-light coupling Emission spectrum Radiative rate Minimized parasitic processes Designed transport properties High mobility Optimized contacts Multidimensional optimization Charge transport characteristics + - Robust or self-assembled/ self-healing components

Rational design of solid-state lighting systems Fundamental materials science needs Physics: ability to precisely tune basic physical properties New functionality through heterogeneous nanostructures Enhanced light-matter interaction Innovative photon management Discovery of design rules for robust photon conversion materials & matrices for use in the UV-Vis-IR Chemistry: high-quality materials, high precision placement Computational design and/or synthesis of unconventional light emitting materials with tailored properties Manage & exploit disorder in OLEDs Understand the origins of OLED degradation Theoretical understanding Multiscale modelling for solid-state lighting Understand & control highly polarized materials & heterojunctions Integrated approach to OLED design