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by: Deondre Ullrich


Deondre Ullrich
Rice University
GPA 3.54


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Class Notes
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This 17 page Class Notes was uploaded by Deondre Ullrich on Monday October 19, 2015. The Class Notes belongs to ELEC 603 at Rice University taught by Staff in Fall. Since its upload, it has received 61 views. For similar materials see /class/224980/elec-603-rice-university in Electrical Engineering & Computer Science at Rice University.

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Date Created: 10/19/15
RICE UNIVERSITY Fluorescence Near Metal Tips The roles of energy transfer and surface plasmon polaritons Nader A Issa and Reinhard Guckenberger Mark Knight Laboratory for Nanophoz onics LQNF LAEIG IAJCAHV NAMDPHOTDNICB RICE UNIVERSITY Model Geometry a Axis of rotational symmetvy f39fII f fffffjjffff Medium Ail IIIm I Vert ocall j H I elecuk I RICE UNIVERSITY Paper Summary Paper based on FEM simulations using dipole metal tip Results are independent of molecular excitation method When tip enters near eld ef cient SPP creation increases Radiative rate Nonradiative rate Enhancements brighten molecular uorescence Tip molecule separations less than 5 nm result in quenching RICE UNIVERSITY Decay Rate y Assumptions Molecule is represented by classical electrical dipole p Magnitude of dipole unchanged by environment YYrYian yr 2 Radiative decay ratephotons Can calculate by integrating Poynting vector over sphere surrounding molecule yl IIntrinsicintra molecularenergyloss ynr I Nonradiative EM dissipation to surroundings Includes thermal dissipation of SPP in metals RICE UNIVERSITY Excitation amp Detection For a single molecule ydet E N yr g detection efficiency of instruments N probability of finding molecule in excited state y decay rate y Phv W Far Below Saturation Nltlt1 UnCommon Most common case Ydet E Yr Ydet E Yexc q yexc excitation rate q quantum ef ciency RICE UNIVERSITY Model Limitations Excludes effects of nonlocality Ignores surface electron scattering May underestimate nonradiative rates for distances between 05 10 nm Mean free path of electrons is 10 nm for infrared wavelengths RICE UNIVERSITY Model Geometry a Axis of rotational symmetry Vontat I vE elecmt I dipote I 39 39 39 l Fig 1 3 Example solution ReHe with diagram overlay of the model geometry This cross section view is symmetric about indicated axis of rotation In this gure the tip silver is at a distance D100nm from the dipole and 1550mn The metal tip supports a propagating SPP that is clearly visible The power in propagating SPPs remaining at the top of the tip is measured prior to the top PML and is counted as nonradiative b Example FEM meshing near the up showing adaptation and ne mesh near panescale features D10nm 0 Diagram illustrating different pans of the tip where the integrated resistive losses are attributed to SPP losses volume I and local energy transfer volume 2 RICE UNIVERSITY Model notes Solved Maxwell s equations in frequency domain using COMSOL multiphysics Used experimental dielectric constants 31 P B Johnson and R W Cbirsty quotOptical constants of the noble metalsquot Phys Rev B 6 4370 4379 1972 32 D R Lide ed CRC handbook of chemistry and physics CRC press London 1996 2 iterations of adaptive meshing used Accuracy of model better than 3 Degrees of freedom O106 Rmolewle lt 2 x 10392 nm RICE UNIVERSITY Nonradiative Rate yr an YSPP YLEr YSPP rate at which surface plasmons are dissipated as heat in an infinite length tip LET nonradiative energy transfer to apex of tip Length scale for LET 7 nm y LET calculated by integrating heat losses over 10 nm radius sphere 100000 0 Numerical solution 10000 Y 1000 A Numerical solution Y 100 Analytic solution 10 E 6 N A Q y 1 m Y W 5 My 0 1 100 071 001 D nm Fig 2 Comparison of the numerical solution of 715147 with the analytic solution Eq6 that neglects retardation effects The numerical solution is for a silver tip using the geometry of Fig 1a without glass substrate and 1550nm The analytic solution assumes the molecule is at distance D from a at silver substrate no tip For comparison the normalized total nonradiative rate 71 2 is shown RICE UNIVERSITY Origin of LET Quenching Distance scale lt 5 nm Quantum view nearfield of molecule penetrates metal excites excitons electronhole pairs Classical view Lossy surface waves Induced chargedensity oscillations Interpret as dipoledipole energy transfer to volume of dipoles comprising metal RICE UNIVERSITY Movie Crosssection of rumian symmei c solution Magnetic eld IREfHJI DQGEJJEnm RICE UNIVERSITY Quantum Efficiency Silver tip 7 550nm 8 mm l29 043i 1 101 1 qa 0 08 W99 uni 0394 1 04 02 02 0 H r 01 01 1 10 100 1000 01 D mm D rim q Yfv Yepv vimY Fig 5 Comparison of ef ciencies for two different initial quantum efficiencies The curves are nearly identical for D lt 10nn1see text RICE UNIVERSITY Spectra Gold lip Air D 30 nm 1 1 Water 8medium l 1 Emcdium 134 1 08 J I 08 I 06 06 A k A 630nm MA A 560nm X 04 3 51 04 5 4 04 06 00 10 12 14 16 04 I 05 08 Hi i 1 1 3911 AHm 101m 4 YfY stPY rmy Fig 9 Spectra for gold tips in air and water surrounding medium With xed D30nm RICE UNIVERSITY Paper Summary Paper based on FEM simulations using dipole metal tip Results are independent of molecular excitation method When tip enters near eld ef cient SPP creation increases Radiative rate Nonradiative rate Enhancements brighten molecular uorescence Tip molecule separations less than 5 nm result in quenching RICE UNIVERSITY Nod to the Past General effects were summed up in 1984 ELECTROMAGNETIC INTERACTIONS OF MOLECULES WITH METAL SURFACES GW FORD Physics Department The University pf Michigan Ann Arbor MI 48109 USA and WM WEBER Phyxiar DemImam Research Staff Ford Man Company Dearbam M14812 USA by several authors 26 29 At distances of order d 50 500 A ie much larger than atomic dimen sions but somewhat le than ength the uorescing molecule couples strongly to the Mahmudquot I l 30 31 This decay into surface plasmons has been observed direct 39 plers to conve these surfa e waves 39nto photons 32 36 H 39 t 7 7 7 7 7 7 7 77 7 7 7 and these nterband absorption electron scattering losses and electron hole excitations Which of these mechanisms is most important in a given RICE UNIVERSITY Playing with COMSOL RICE UNIVERSITY Dipole above Nanoshell InmbanwahtIPkJ Max SVDUb surface Magnellcheld pm nmpunanAm1 0 xm 7 5 4 4 3 a 2 2 I u 1 71 n 72 71 73 2 4 gt4 3 2 1 0 1 2 3 4 5 a 7 s 077 Mm fungi


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