Quantum optics and metamaterials. Janne Ruostekoski Mathematics & Centre for Photonic Metamaterials University of Southampton

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1 Quantum optics and metamaterials Janne Ruostekoski Mathematics & Centre for Photonic Metamaterials University of Southampton

2 Motivation Quantum optics a well-developed field for studying interaction of light with atoms Analogies of metamaterials systems to atomic and molecular scatterers Analogous phenomena to quantum coherence and semiclassical effects in atomic gases Nanostructured resonators interacting strongly with EM fields Less emphasis on microscopic approach Cooperative response in large system Start with a two-level system interacting with EM fields Quantum coherence phenomena, slow light, nanaofabricated analogs Collective effects in large systems

3 Standard quantum optics: Light propagation in polarization medium Weak interactions between scatterers in the medium (no free charges) (no free currents) Assume no magnetization

4 Plane wave propagation Slowly varying envelope approximation

5 slowly varying envelope approximation steady-state solution for electric field in linear medium real and imaginary parts of electric susceptibility absorption

6 Two-level medium 1 Interaction between dipole and electric field 0 quantum state see e.g. Meystre, Sargent, Elements of quantum optics

7 Introduce new slowly varying amplitude Rabi frequency; detuning here

8 Relaxation terms density matrix 1 0 choose closed two-state system

9 longitudinal and transverse relaxation times Steady-state solutions, conserved population

10 Optical response electric dipole excitation electric susceptibility

11 Laser Absorption

12 Laser Coherence may be expressed in terms of population difference usually positive and propagating light is absorbed One can also arrange (usually in multi-level system) so that atoms are transferred to and depleted from Inversion Light coupling to transition is amplified

13 Electromagnetically induced transparency & ultra slow light Three-level system see e.g.

14 Probe and coupling fields, nonlinear response dressed level picture (eigenstates) Autler-Townes splitting Quantum interference of different excitation paths

15 Electromagnetically induced transparency Ω p 1> 3 > 3 > Ω c 2> Three-level system Two ground states coupled to excited state Dark state : Absorbing state : D Ω A Ω ( 1 Ω 2 ) c ( 1 + Ω 2 ) p p c Ω p Ω c D> A> Dark state decoupled from light (quantum interference) Atoms driven to dark state via spontaneous emission Electromagnetically induced transparency (EIT) Otherwise opaque medium made transparent

16 EIT response Narrow resonance at which opaque medium transparent Steep anomalous dispersion has changed to normal dispersion with controllable steepness (by coupling laser) Steep and linear dispersion where absorption small Constructive interference of the nonlinear processes

17 Dark and bright states 3 > D> A>

18 Ultra-slow light propagation D> 3 > A> Atoms adiabatically follow dark state Small perturbations from D> lead to coherent driving between ground states with no absorption Reversible process Coherent driving and the associated exchange of photons between two light beams result in slow group velocity for light Hau, Harris, Dutton, Behroozi, Nature 397, 594 (1999) Liu, Dutton, Behroozi, Hau, Nature 409, 490 (2001)

19 Ultra-slow and stopped light Linear dependence of susceptibility close to the absorption dip extreme pulse compression

20 light pulses Dutton, Hau, Phys. Rev. A 70, (2004) Dutton, Ruostekoski, Phys. Rev. Lett 93, (2004) population transfer from 1 to 2 dark state switch coupling off Also probe pulse goes to zero Revive the probe pulse later on by switching the coupling field on

21 Nanostructures Hybridization model of plasmons supported by nanostructures of elementary geometries Analog of molecular orbital theory [Prodan et al., Science 302, 419 (2003)]

22 Hybridisation of metal nanoshell from interaction of sphere and cavity plasmons Split ring resonator r d r µ electric magnetic

23 Quantum optics and metamaterials Janne Ruostekoski Mathematics & Centre for Photonic Metamaterials University of Southampton

24 Electromagnetically induced transparency and slow light 3 > D> A>

25 EIT in metamaterials Instead of coupling atomic transitions to obtain quantum interference of transition amplitudes, create the interference using plasmonic structures Plasmonic structures allow large field strengths in small volumes

26

27 Interference of layered copper patterns Shifted double fish-scale copper pattern currents oscillate pi out of phase Papasimakis et al., PRL 101, (2008)

28

29

30 Coupling of a rod to two wires Coupled dipole and quadrupole antennas Liu et al., Nature Materials 8, 758 (2009) Two layers: gold rod on top two gold wires below h=70nm; g=220nm; w=80nm

31 Broad and narrow resonances dipole with large radiative damping (rod on top) quadrupole almost non-radiative (two wires below) Coupling between the two layers no coupling for s=0 due to symmetry for non-zero s the coupling induced

32 Level structure dipole excitation in the top rod quadrupole excitation in the bottom wires can be excited due to structural asymmetry non-radiative due to ohmic losses transition rate between dipole and quadrupole excitations

33 Resonances At s=0, there is a single resonance at No coupling between layers At s=10nm resonance properties change Transmittance peak at 173THz frequency difference between dipole and quadrupole resonances

34 Interference of transitions destructive interference between excitation paths Almost no excitation in dipole rod

35 image: Tassin etc. Analytic model

36

37

38 Dipole-quadrupole vs dipole-dipole Two single rods on top of each other

39 Circuit analog

40 Strong interactions to EM fields collective response Nanostructured resonators interacting strongly with EM fields Cooperative response in large system Analogies of metamaterials systems to molecular scatterers Analogous phenomena to quantum coherence effects in atomic gases Treatment of resonators as discrete scatterers

41 Natural medium and light propagation Electric dipole moment of the atom Electric displacement field

42 Nanofabricated resonators split-ring resonator (SSR) current electric polarization Net electric dipole Net magnetic dipole

43 Co-operative light scattering Coherent back-scattering Simplest manifestation of coherence in multiple scattering Enhanced scattering intensity in back-scattering direction Co-operative response Strong scattering Interference between different scattering paths Localisation of light (observed in semiconductor GaAs powder) Wiersma et al., Nature 390, 671 (1997) Analogous to Anderson localisation of electrons Localisation achievable in atomic condensates

44 Simple model of oscillating current in meta-molecule constituents Jenkins, Ruostekoski PRB meta-atom ensemble

45 Lagrangian description Coulomb gauge, Power-Zienau-Woolley transformation (Cohen-Tannoudji, Dupont-Roc, Grynberg, Photons and atoms) conjugate momentum for vector potential conjugate momentum for charges

46 Hamiltonian Introduce normal modes for the EM field sum over transverse polarizations and wavevectors kinetic energy + quadratic term (diamagnetic energy)

47 Radiated fields Total EM fields = incident field + scattered fields from all meta-atoms Jackson, Classical electrodynamics magnetic (electric) field from oscillating electric (magnetic) dipole electric (magnetic) field from oscillating electric (magnetic) dipole

48 Integral representation of Maxwell s wave equations in magnetodielectric medium (in freq space)

49 Resonator dynamics Charges driven by net magnetic flux their conjugate momenta driven by net electromotive force Interaction with self-radiated fields results in radiative damping electric radiative emission depends on self-capacitance magnetic depends on self-inductance resonance frequency fl Simple LC circuit include also ohmic losses

50 Coupled system for resonators Strong coupling mediated by scattered fields

51 Quantization Photon plane-wave mode amplitudes, replace photon annihilation and creation operators Resonators format

52 Quantum features illuminate by quantum light Nonlinear resonators (SQUID circuits)

53 Split ring resonator: Simple model of oscillating current single mode of current oscillation in each half of the unit-cell resonator dynamics variable charge Q polarization and magnetization densities

54 Single split ring resonator

55 Unit-cell resonator current excitations Symmetric oscillation 1 c( t ) = r + l 2 [ b ( t) b ( t) ] (eigenmodes) Antisymmetric oscillation 1 d( t ) = r l 2 [ b ( t) b ( t) ] Net electric dipole Net magnetic dipole Dipole Approximation r r r r Pj d j ( t) δ ( j ) r d ( t) = Q ( t) h pˆ j j j j µ r j d r j r r r r r M j (, t) µ j ( t) δ ( j ) r µ ( t) = I ( t) A qˆ j j j j

56 Metamaterial samples Unit-cell resonators (and their sub-elements) interact strongly Long-range coupling due to electric & magnetic radiation from current excitations Recurrent scattering: Wave is scattered more than once by the same resonator Metamaterial sample responds to EM fields cooperatively Exhibits collective excitation eigenmodes, resonance linewidths, frequencies

57 Cooperative response Uniform eigenmode model breaks down due to boundary effects, dislocations, defects, inhomogeneous sample, disorder Advantages of the discrete model Computationally efficient model for large systems Physically tractable providing insight and understanding Can be build up to more complex systems

58 Quantum optics and metamaterials Janne Ruostekoski Mathematics & Centre for Photonic Metamaterials University of Southampton

59 Polarization Computational model for collective interactions Assume each meta-atom supports a single mode of current oscillation: 1 dynamic variable per meta-atom Calculate the scattered electric and magnetic fields from each meta-atom Magnetization Scattered fields mediate interactions between meta-atom dynamic variables. The incident field drives the system Meta-material supports collective modes of oscillation: each with a distinct resonance frequency and decay rate

60 Cooperative response Uniform eigenmode model breaks down due to boundary effects, dislocations, defects, disorder Recurrent scattering: Wave is scattered more than once by the same scatterer

61 retrieving effective material parameters can fail

62 Single split ring resonator Symmetric oscillation 1 c( t ) = r + l 2 [ b ( t) b ( t) ] Antisymmetric oscillation 1 d( t ) = r l 2 [ b ( t) b ( t) ] Net electric dipole Net magnetic dipole

63 Collective excitation eigenmodes Split ring resonator (SRR): Two eigenmodes per unit-cell array = 2178 modes An isolated one half of a SRR would radiate at the rate Γ Collective resonance linewidthsγ lattice spacing 0.5 wavelength lattice spacing 1.4 wavelength Sensitive to lattice spacing Strongly subradiant modes 5 10 Γ

64 Eigenmodes with uniform phase profiles All magnetic dipoles oscillating in phase All electric dipoles oscillating in phase Subradiant 0.02Γ

65 Subradiance and superradiance 5 Most subradiant 10 Γ checkerboard pattern of electric dipoles Most superradiant 11 Γ antisymmetric pattern of magnetic dipoles Phase-matched with field propagating in the x-direction

66 Asymmetric split-ring resonators m p Symmetric oscillation 1 c( t ) = br ( t) + bl ( t) 2 [ ] r d Antisymmetric oscillation 1 d( t ) = [ br ( t) bl ( t) ] 2 r µ electric magnetic l - left half ring r right half ring

67 V. Fedotov et al, PRL 104, (2010).

68 Symmetric case r d ω l ω = ω = ω0 r 0 Γ E r µ ω 0 Γ M eigenstates typically only electric dipole mode driven r ( r E, ) in t r ( r B, ) in t

69 Asymmetric case r d ω = ω δω ω r = ω 0 + δω l 0 Γ E r µ ω 0 Γ M Coupling between states by asymmetry electric dipole mode drives the magnetic dipole mode r ( r E, ) in t r ( r B, ) in t

70 Collective response by phase-matched E k H uniform modes weak radiation on the plane electric dipoles radiate strongly out of the plane fl change in transmission Uniform collective electric dipole mode phase-matched with incident plane-wave Split-ring asymmetry drives weakly radiating uniform collective magnetic dipole mode fl over 98% of excitation can be driven to the magnetic mode

71 Lifetime of the phase-matched magnetic mode and system size Inverse decay rate of the phase matched magnetic mode Lattice spacing λ λ Linewidth narrowing Number of split rings in the lattice λ λ

72 Q-factor: Theory vs experiment Saturation is due to ohmic losses Transmission Resonance Quality Factor Quality factor of collective mode Number of metamolecules Experimentally measured quality factor: V. A. Fedotov et al, Phys. Rev. Lett. 104, (2010) Theoretical quality factor of collective phase matched mode calculated from model

73 Excitation probability of magnetic mode Phase-coherent magnetic collective mode Phase-matched with incident plane-wave Split-ring asymmetry drives weakly radiating collective magnetic dipole mode 98% overlap with target mode

74 Collective mode

75 Exploiting collective interactions Coupling between the collective modes EIT-like but not a single-resonator effect Excitations in the presence of disorder in the positions of the resonators exhibit complex structure Excitation of a superposition of collective modes that exhibit subwavelength structures coherent control Highly localized excitation can transfer energy to a collective excitation and subsequently to a low-divergence free-space light beam

76 Collective phase-matched modes: Cooperative Asymmetry Induced Transparency

77 When the collective magnetic mode decays slowly, the magnetic mode can be excited at the expense of the electric mode Collective mode decay rates Incident field driving Mode coupling due to asymmetry Energy in phase matched electric mode Energy in phase matched magnetic mode Phase matched magnetic mode resonance solid dashed Detuning from phase matched electric mode resonance = Single metaatom decay rate

78 Phase-matched electric mode is unexcited in the transparency window Results from simplified two mode model dashed lines Results of numerical simulations of the full meta-material solid lines Energy in phase matched electric mode Energy in phase matched magnetic mode Energy in all other collective modes Phase matched magnetic mode resonance = Single metaatom decay rate

79 Changing geometry shifts the Square lattice transmission resonance Energy in phase matched electric mode Energy in phase matched magnetic mode Energy in all other collective modes Phase matched magnetic mode resonance Nanoelectromechanical switchable photonic metamaterials Every other column vertically shifted by 0.1 wavelengths K. Aydin et al, Optics Express 12, 5896 (2004)

80 Effects of disorder Displacing resonators by a Gaussian stochastic noise Increasing disorder leads to potential localization of collective modes. standard deviation lattice spacing = 0.05 Energy of excited magnetic modes Magnitude and phase of excited magnetic modes

81 Disorder standard deviation lattice spacing = 0.1 Comparison to disorder experiments by Papasimakis et al

82 Disorder

83 Subwavelength control Precise control and manipulation of optical fields on nanoscale one of the most important and challenging problems in nanophotonics Tailoring phase modulation of ultrashort optical pulses (Stockman etc.) Collective interactions and cw fields

84 Nanoscale field localization by exciting linear combinations of eigenmodes Plasmonic Metamaterials Phase, rad. π π 2 0 π 2 π Y Plane wave (constant amplitude) Gold unit cell: 440nm width: 25nm thickness: 50nm Sinusoidal phase profile ϕ = ϕ(r r ) X 1.32 Absorption,% Transmission,% ϕ ϕ 0. max = π ππ Y,μm Y-pol. 0 λ=880nm X FWHM ~133nm (~0.15λ) Y FWHM ~60nm (~0.07λ) Wavelength, nm X,μm e -9 0 Reflection, % Total energy intensity, J/m 3

85 Plasmonic metamaterials 80 Phase, rad. π π Sinusoidal phase profile r ϕ = ϕ (r ) 2 0 π 2 Total energy intensity, J/m Wavelength, nm ϕ max = π π 9e-9 Transmission,% Absorption,% 100 Reflection, % Nanoscale field localization with coherent control 60 Y 50 X λ=1150nm 50 0 Y, μm λ=700nm X,μm λ=880nm

86 see also Transfer of sub-diffraction evanescent fields to propagating fields by a resonator array

87 Experimental observation

88 Localized excitation by electron beam Highly localized excitation can transfer energy to a collective excitation and subsequently to a low-divergence free-space light beam Excite only 1-4 unit-cell resonators in an ASR metamaterial array The phase-uniform collective magnetic mode can assume dominant role of total excitation energy High degree of spatial coherence Highly directed emission pattern and narrow resonance linewidth

89 Role of phase-coherent magnetic mode Excite resonantly collective magnetic mode (a) Excite only a single resonator: 70% of steady-state response in collective magnetic mode (b) Excite four resonators: 85% of steady-state response in collective magnetic mode phase variance 2.2 degrees If detuned 8 linewidths off-resonant, 45% and 24 degree phase variance G Adamo et al.

90 Electron-Beam-Driven Metamaterial Light Sources e-beam Light emission Collective (coherent) light emission from plasmonic metamaterials 50 nm Au 100 nm Si 3 N 4 Smith-Purcell emission enhancement through Surface Plasmons ASRs in 1/e 2 source spot A Intensity Linewidth,nm B C Injection point H I J µm 0 6 x x 10 4 ϕ= 0 30 θ= Peak amplitude Total emission MM emission Ag Thickness, nm

91 Nonlinear and quantum systems

92 SQUID rings Suppress ohmic losses Introduce nonlinearity in the system Current through SQUID ring total external magnetic flux flux trapped in squid loop Nonlinear relationship for the flux

93 Optical lattice Atoms trapped in periodic optical potential AC Stark effect of off-resonant lasers Optical lattices as a platform to exploit collective interactions Atomic dipole-dipole interactions mediated by scattered EM fields

94 Quantum metamaterial Prepare a 2D optical lattice one atom per site Atoms can be reasonably well localized Positions of dipoles fluctuate due to zero-point vacuum fluctuations size of Wannier Function lattice spacing d

95 Cooperative localization constant intensity Modulated phase

96 Quantum effects and confinement size of Wannier Function lattice spacing d = 0 = 0.12 d single stochastic realization = 0.12 d Ensemble average of many realizations

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