Plasmon enhanced UV electroluminescence in SiO 2 with percolating conduction sustained by free-exciton emitting SnO 2 nanoparticles
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1 Dipartimento di Scienza dei Materiali Università di Milano-Bicocca TITLE Plasmon enhanced UV electroluminescence in O 2 with percolating conduction sustained by free-exciton emitting SnO 2 nanoparticles Alberto Paleari XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
2 TITLE UV-LED Technological Goals Wide band gap QDs Origin of the idea O2 films, -technology compatibility excitons, hopping, plasmons Nanostructuring features Sol-gel deposition Thermally induced clustering structure role of electrodes and nanostructuring percolation mechanism nanoparticle charging and e function exciton emission surface plasmon enhancement S final achievements & thanks XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
3 Technological Goals UV light emitters Curing (adhesive, ink, polymer, resin) Photocatalysis for air and water purifier Lab-on-chip for bio applications Planar geometries Compactness licon-based technology XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
4 AlGaN Critical features Doping Crystallinity GaN AlN ZnO nm NanoWires Quantum Wells Quantum Dots XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
5 SnO2 OXIDE IN OXIDE oxide nanocrystals amorphous matrix Wide-band gap Stoichiometry doping Nanocrystallinity Chemical stability O2 Optical features compatibility Workability Chemical stability NANOSTRUCTURED SnO2:O2 FILMS XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
6 Nanofeatures XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
7 TITLE Main reaction: hydrolysis and condensation of TEOS (TetraEthylOrtolicate) Dopant precursors: Sn dibutyl diacetate (a well known silicon condensation cure agent) CH 3 CH 2 CH 2 CH 2 H 2 O Sn OOCCH 3 CH 3 CH 2 CH 2 CH 2 OOCCH 3 hydrolysis networking O O O O O R O Sn R O O O O O O O O R R Sn OH OH Self-condensation Thermally-activated densification nano-clustering XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
8 structure UV-emission V ~ 20 nm ~ 800 nm 1 mm Nanostructured O2 p-type silicon Metal Gate 10 nm 2 nm XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
9 - percolation process dead-ends f( D ) D 1/ 3 d c b a 1 0 dn v( r) dr dr 1/ 3 XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
10 hole/electron injection - Electrons + Holes SnO 2 phase (n-type) SnO interphase (p-type) XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
11 current/voltage response Warm Colours: - Rectifying film - Ohmic Conduction - Low oxygen - Fast heating rate - Doping Cold Colours: - Non-rectifying film - Thermoionic (Schottky) - High oxygen - Slow heating rate XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
12 Metal-like Semiconductor-like TITLE thermal behaviour Positive bias Negative bias Positive bias Negative bias XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
13 capacity/voltage response rectifying MOS (no NC) non-rectifying d d L DC=C 0 { (L/[L-d[L/(d+)]) - 1} DC/C 0 d/ XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
14 vs XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
15 h Light-emission yield enhancement e h h e e Q e/h e/h / z RAD RAD SP 0 Q SP / z RAD + NR RAD + NR + SPe Q SP /Q 0 e/h UV nonradiative decay h e h h e e surface plasmon e/h e/h e/h + e UV SP RAD XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
16 plasmon/exciton coupling PL Intensity (Arb. Units) Real Dielectric Constant e Ti -e d e Al Photon Energy (ev) SP Absorbance Surface-plasmon in Ti /O 2 Surface-plasmon in Al /O 2 k SP ENERGY RESONANCE h exciton 3.6 ev c 0 e de m e + e d e m SP m e d XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
17 NANOSTRUCTURED FILM SUBSTRATE TITLE plasmon/exciton coupling MOMENTUM CONSERVATION kexciton k SP 100 nm Interface patterning Nanosized refractive index patterning XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
18 plasmon/exciton cavity-modes Emitting dipole I( ) ξ l D=ξ+l D 0 r 1 Reflected Waves 2nξ 2nl=2n(D-ξ) 2 cos 2n + r Titanium electrode 2 R SP Coupling efficiency Q SP Exp(-ξ/Z) R licon substrate 2 cos 2n( D ) + / z RAD SP Q SP / z RAD + NR + SPe 2 Q + SP e ( ) d XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
19 plasmon/exciton cavity-modes Doubled FP Fabry Perot Fabry Perot Doubled FP XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
20 SP/Exciton-coupling enhanced UV emission Fabry Perot reflectivity Doubled structured EL Reflectance % Electro- Luminescence Photon Energy (ev) XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
21 THANKS PEOPLE Norberto Chiodini Alessandro Lauria Roberto Lorenzi Sergio Brovelli Marco Giussani Andrea Clementi synthesis design material and device fabrication experiment design and simulations measurements and interpretation electrical measurements optical measurements FUNDING Fondazione Cariplo 2-year funded project Fondazione lvio Tronchetti Provera 3-year PhD grant Consorzio CORIMAV UniMIB-Pirelli two 3-year PhD grants XCVI CONGRESSO NAZIONALE - SOCIETÀ ITALIANA DI FISICA - Bologna, Settembre /21
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