Lecture Juraj Darmo - IR-On
Transcription
Lecture Juraj Darmo - IR-On
TECHNISCHE UNIVERSITAT WIEN VIENNA UNIVERSITY OF TECHNOLOGY Time-Domain Spectroscopy of THz Quantum Cascade Structures J. Darmo Photonics Institute Vienna University of Technology, Vienna, Austria IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Outline 1. Time domain THz spectroscopy 2. Interaction of THz-QCL and few-cycle THz pulse - theory - technical issues 3. THz-QCL data - transmission through QCL (gain) - role of design and waveguide - gain recovery (MIR QCL) - advanced concepts based on TDS - advances in electro-optic detection 4. Outlook Acknowledgement for contribution J. Kröll, M. Martl, D. Dietze, D. Bachmann, W. Parz, K. Unterrainer Photonics Institute Vienna University of Technology, Austria M.A. Andrews, H. Detz, P. Klang, W. Schrenk, G. Strasser. E. Gornik Institute of Solid-State Electronics & ZMNS Vienna University of Technology, Austria S. Barbieri and C. Sirtori University Paris Diderot, Paris 7, France S.S. Dhillon, N. Jukam Ecole Normale Superier, Paris, France Q. Hu, D. Burghoff MIT, Cambridge, U.S.A. G. Scalari and J. Faist Institute of Quantum Electronics ETH Zurich, Switzerland M. Kuhn, T. Elsaesser MBI for Nonlinear Optics, Berlin, Germany J. W. Cockburn University of Sheffield, U.K. M.S. Vitiello Scuola Normale Superiore, Pisa, Italy Funding: FWF (ADLIS,PLATON,QOCUS) & GMe Austria, EC (POISE,TERANOVA) Brief history of THz-TDS ... triggered by the advent of femtosecond laser emitters: photoconductive switches with ultrafast recovery time (Auston, LT-GaAs) optical rectification and DFG in NLOC – broadband coherent THz pulses – typical average power ~ uW detectors: photoconductive antenna (LT GaAs, Fe doped InP) free space electro-optic detection (X.-C. Zhang) - instant electric field vector can be measured with time resolution as high as 10 fs – gated detection: excellent SNR with respect to detected THz power Terahertz time-domain spectroscopy applied to THz-QCL (transmission measurement) … first attempts in 2005 J. Kroell et al., Nature 449, 698 (2007) TU Wien - SPWG, BTC design N. Jukam (S.S. Dhillon) ENS Paris - SPWG, BTC & RPD design, latter DMWG D. Burghoff (Q. Hu) MIT - DMWG, RPD & Co. accessible information on - absorption/gain in active/passive THz waveguides - real temperature in the THz-QCL active region - gain dynamics, mode dynamics IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria THz time-domain spectroscopy 6.0 Amplitude EO signal 4.0 2.0 0.0 -2.0 -4.0 100 80 60 40 20 0 0 -6.0 35 40 45 50 55 60 time delay (ps) Free induction decay of coherently excited H2O molecules 2 3 5 4 5 Frequency (THz) 100 80 60 40 20 0 0 1 2 3 Frequency (THz) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 4 Amplitude 30 1 F.I.D. of coherently excited H2O molecules Main pulse First coherences Parasitic reflections 0 frequency 1.5 3.0 4.5 6.0 0 2 4 6 time (ps) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 8 10 THz time-domain spectroscopy applied to THz-QCLs THz-TDS of THz QCL NIR 80 MHz THz emitter QCL High repetition fs-system (80 MHz): Ti:sapphire at 800 nm, < 80 fs pulses EOC Photoconductive THz emitter Electro-optic detection: - gated detection - detection bandwidth of 7 THz ( with 300 um GaP) double modulation used Coupling optics IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Electro-optic detection photodetectors λ/2 plate & Wollaston prism electro-‐opFc crystal THz wave ellipFcally polarized NIR probe Δϕ ∝ 2π ⋅ LEOC ⋅ r41 ⋅ n 3 ⋅ ETHz λ linearly polarized NIR probe response funcFon of single layer EOS exp[i ⋅ Δk (ω, Ω)⋅ L] − 1 Ω NIR g (ω, Ω) = (ω ) − nTHz Δk (ω , Ω ) = ⋅ [ngroup phase (Ω )] i ⋅ Δk (ω , Ω) c IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria n3 no ≈ n − ⋅ ETHz ⋅ r41 2 n3 ne ≈ n + ⋅ ETHz ⋅ r41 2 G.Gallot, J.Opt.Soc.Am. B16, 1204 (1999) P. Planken, J. Opt. Soc. Am. B18, 313 (2001) van der Valk, J.Opt.Soc.Am. B21, 622 (2004) Electro-optic detection probe light intensity aYer polarizer, waveplate and PBS probe light intensity aYer two crossed polarizers I (φ0 , Δφ ) = I 0 sin (φ0 + Δφ ) I0 I (φ0 , Δφ ) = ⋅ [1 − cos(φ0 + Δφ )] 2 Taylor expansion ... 1 1 cos(φ0 + Δφ ) = cos(φ0 ) − sin (φ0 ) ⋅ Δφ − cos(φ0 ) ⋅ Δφ 2 + sin (φ0 ) ⋅ Δφ 3 + … 2 6 1 1 sin (φ0 + Δφ ) = sin (φ0 ) + cos(φ0 ) ⋅ Δφ − sin (φ0 ) ⋅ Δφ 2 − cos(φ0 ) ⋅ Δφ 3 + … 2 6 selected terms gives ... I (ϕ 0 , Δϕ ) ∝ Δϕ = Δϕ THz ⋅ cos ( Ωmod ⋅t ) I0 cos (ϕ 0 ) ⋅ Δϕ THz 2 ... signal (instant THz field) modulated at Ωmod IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria I (ϕ 0 , Δϕ ) ∝ I0 2 cos (ϕ 0 ) ⋅ Δϕ THz 4 ... signal (instant THz power) modulated at 2 ⋅Ωmod THz-TDS in QCL: Travel-wave amplification I < Ith THz QCL spontaneous emission – few photons with random timing and phase injected photons – trigger photon emission with correct timing and phase I > Ith THz QCL stimulated emission – photons with random timing and phase injected photons – trigger photon emission with correct timing and phase (long/short coherence time) I > Ith THz QCL stimulated emission –photons with correct timing and phase with respect to injected photons (even mode-locked laser) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Time-domain response of gain medium THz-QCL: two-level system rin rdep b hν ω ab a rsp ωa rout Density matrix if (tobserve > 1/rin, 1/rout, 1/rdep ) then interacting system if (tobserve < 1/rin, 1/rout, 1/rdep) then insulated system (standard) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria ⎛ ρaa ⎜ ⎜⎝ ρba ρaa , ρbb ρab , ρba ωb ρab ⎞ ⎟ ρbb ⎟⎠ ~ population ~ coherence Two-level system: time domain response standard spectroscopy – sensitive to probe intensity changes 2,0 E(t) E (~t )rabρab el. field (a.u.) 1,5 el. field (a.u.) 15 10 5 0 2 E ∫ dt ~ ρaa − ρbb 1,0 0,5 0,0 -0,5 -1,0 -5 1 -10 2 3 4 5 6 7 8 9 10 11 12 time (ps) -15 2 3 4 5 6 7 8 9 10 11 12 time (ps) 1,5 el. field (a.u.) 1 1,0 0,5 0,0 -0,5 -1,0 -1,5 1 IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 2 3 4 5 6 7 time (ps) 8 9 10 11 12 Two-level system: time domain response 16 4 reference 2-level system 3 x20 2 1 0 0.0 1.0 2.0 3.0 0.5ω 0.67ω 0.8ω 12 amplitude spectral density 5 4.0 frequency (THz) 1.05ω 1.3ω 4 0 0.0 5.0 ω 8 1.0 2.0 3.0 4.0 5.0 frequency (THz) Two response components - instant & resonant - stronger for higher frequency overlap - effect of strong driving field (Rabi oscillations) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria amplitude 30 E0 1.5E0 3E0 5E0 10E0 20 10 0 0.0 1.0 2.0 3.0 4.0 5.0 frequency (THz) 6.0 Technical issues of THz-TDS THz waveguides for QCL Coupling of THz waves into laser waveguide THz optics THz pulse aperture THz-QCL chip + leaky laser cavity - low coupling efficiency (<10%) ω1 ω2 NIR pulse THz-emitter chip IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria THz-QCL chip - coupled cavities + high coupling efficiency (>60%) Optics: Coupling of THz Waves into WG HR-Si lens THz-QCL IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Towards integrated THz Coupling THz emitter Approach Waveguide Emitter (WGE) Facet-Excitation on THz QCLs M. Martl et al., IRMMW-THz 2008 S.S. Dhillon et al., APL 96, 061107 (2010) SI-GaAs Emitter section on THz QCLs THz QCL Micro Chip Emitter (MCE) M. Martl et al., unpublished SI-GaAs • semi-insulating GaAs • broadband THz pulse generation at the facet of a waveguide IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria - QW structure of THz QCL - waferbonding-technique - WG thickness defined by AR - THz emitter (section A) - active QCL (section B) M. Martl et al., Opt. Expr. 19, 733 (2011) D. Burghoff et al., APL 98, 061112 (2011) J. Maysonnave et al., Opt. Lett. 37, 731 (2012) Gain in THz-QCL THz QCL – Design & Parameters Design: • GaAs/AlGaAs system • band-to-continuum • transition energy: 2.0, 2.9 THz and 3.4 THz Waveguide: • surface plasmon (n+-GaAs buried confinement layer) • ridge type (110 – 200 um wide) S: Barbieri et al., APL85(10), 2004 Ch. Worral et al., OE14(1), 2005 B. Williams et al., EL40, 2004 IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria band structure THz QCL – THz pulse transmission (2.9 THz) 0 100 50 0 -50 -100 10 2 ETHz (V/cm) (a) 6 8 10 Reference pulse waveform Eoff(t) (b) 5 4 Δ E(t)=Eon(t)-Eoff(t) Modulation observed 0 ETHz (arb. units) -5 Comparison of experimental data and model (red line) (c) -5 0 5 0 2 4 6 8 10 time delay (ps) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 12 J. Kroell et al., Nature 449, 698 (2007) Gain spectrum: current dependence 0 2 4 6 8 10 0 10 J=45 A/cm 5 2 3 4 4 2 2 0 -5 0 -10 10 J=113 A/cm 5 4 2 2 0 -5 0 -10 10 J=170 A/cm 5 4 2 2 0 -5 spectral intensity (arb. units) THz electric field (arb. units) 1 0 -10 0 2 4 6 8 time delay (ps) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 10 0 1 2 3 4 frequency (THz) J. Kroell et al., Nature 449, 698 (2007) Gain peak region: 2.9 THz-QCL 100 150 200 250 spectral intensity 30 50 (a) laser losses 20 WG loss 10 0 8 (b) 6 120 model 100 80 60 40 II. I. 20 III. 0 0 100 200 300 400 500 current 4 2 0 6 25 (c) 20 15 4 10 2 5 0 0 50 100 150 200 2 current density (A/cm ) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 0 250 I. diff. resistance (Ω ) laser bias (V) THz output power (arb. units) single pass gain (1/cm) 0 Cascades aligned: gain increases with current I. spatial hole burning – reduced gain slope III. gradual disalignment of cascades J. Kroell et al., Nature 449, 698 (2007) Probing THz-QCL with DMWG Mini-broadband THz-QCL THz-QCL with RPD design: spectral gain IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Mini-broadband THz-QCL THz-QCL with RPD design: gain IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Mini-broadband THz-QCL THz-QCL with RPD design: gain IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Mini-broadband THz-QCL THz-QCL RPD design: gain curve Time-domain response of MIR-QCL amplitude (arb. units) MIR QCL: time domain analysis 0% 1 200 % of Jth x 50 0 measurement -1 0.0 amplitude (arb. units) 100 % 3.8 4.0 4.2 time (ps) 0% 1 100 % 4.4 4.6 200 % of Jth x 50 good agreement with the response function of a 2D waveguide calculation for the TM00 mode. 0 calculation -1 0.0 3.8 4.0 4.2 4.4 4.6 time (ps) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria W. Parz et al, APL 93, 091105 (2008) 0 MIR QCL: gain curve 0.5 2 0 40 0.0 s -40 as se -120 0 50 100 % 200 % 100 150 current (% of JTh) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria 24 26 28 frequency (THz) 3p -80 50 % of JTh -100 22 -1 gain (cm ) gain after 3 passes -200 s s 1 pa 0 0 gain (cm-1) 4 optical power (arb. u.) voltage (V) 6 100 150 200 current (% of IThreshold) 8 1.0 50 200 - gain clamps above threshold - stark shift to red when full gain is present, in agreement with calculations - no stark shift when gain builds up - sign for individual alignment of the cascades W. Parz et al, APL 93, 091105 (2008) Comparison of gain curves Mini-broadband THz-QCL THz-QCL gain bandwidth comparison N.Jukam et al., APL94 251108 (2009) RPD + SPWG N. Jukam et al., APL93 101115 (2008) BTC + SPWG IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria M.Martl et al., OE19 733 (2011) RPD + DMWG D. Burghoff et al., APL98 061112 (2011) RPD + DMWG Mini-broadband THz-QCL gain curveTHz-QCL comparison N.Jukam et al., APL94 251108 (2009) RPD + SPWG N. Jukam et al., APL93 101115 (2008) BTC + SPWG IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria M.Martl et al., OE19 733 (2011) RPD + DMWG D. Burghoff et al., APL98 061112 (2011) RPD + DMWG Active region temperature Mini-broadband THz-QCL THz-QCL with RPD design: gain Tmax IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Device Real Temperature RPD M.S. Vitiello et al., APL86 111115 (2005) BTC DMWG SPWG M.S. Vitiello et al., APL89 021111 (2006) BTC DMWG SPWG M.S. Vitiello et al., APL89 131114 (2006) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria Gain dynamics Pump/probe spectroscopy of MIR QCL • pump & probe electric field strength: >6 kVcm-1 Kühn et. al, APL 93, 151106 (2008) W. Parz et al, APL 93, 091105 (2008) 0,4 FFT Power (arb. u.) Transmission change ΔT / T0 Pump/probe spectroscopy of MIR QCL 0,2 0,0 0,8 1,2 1,6 2,0 frequency (THz) 0 mA 150 mA 400 mA 650 mA 0,6 0,4 0,2 0,0 4 2 0 0 2 4 6 Delay τ (ps) 8 10 Time shift (fs) Phase shift (rad) -0,2 • below threshold relaxation time constant ~3 ps • above threshold relaxation time constant <1 ps • observation of relaxation oscillations @ 0.8 THz Kühn et. al, APL 93, 151106 (2008) W. Parz et al, APL 93, 091105 (2008) Pump/probe spectroscopy of MIR QCL injection barrier extraction barrier 1 1 THz 25 THz 2, g 1 2, g ~ 50 ps gain recovery Fme for MIR QCL from pulse autocorrelaFon (V.M. Gkortsas et al., OE18 13616 (2010)) ~ 50 ps gain recovery Fme for THz QCL from autocorrelaFon of photocurrent pulses (FEL) for BTC QCL @ 3.2 THz (P.R. Green et al., PRB80 075303 (2009)) H. Choi et al, phys. stat. sol. (c) 5, 225 (2008), APL 92, 122114 (2008), Phys. Rev. Le^. 100, 167401 (2008) ~ ps recovery, mulFcomponent Origin of gain oscillation: injector/active region wave packet oscillation F. Eickemeyer et al., APL76 3254 (2000) F. Eickemeyer et al., APL79, 165 (2001) F. Eickemeyer et al., PRL89 047402 (2002) -‐ first p/p results on MIR QCS Kühn et. al, APL 93, 151106 (2008) W. Parz et al, APL 93, 091105 (2008) Advanced concepts based on TDS Ultrafast gain switching • Ultrafast gain switching of QCL through Integrated Auston Switch • THz pulse amplification Auston Switch OFF Clamped Gain Auston Switch ON Unclamped Gain 1,5 1 1,0 5 3 7 0,5 0,0 -0,5 -1,0 -1,5 -2,0 0 20 40 60 80 100 120 140 Time (ps) 2,0 1,5 1,0 0,5 0,0 -0,5 -1,0 -1,5 -2,0 1 3 5 7 Electric Field (V/cm) Electric field (V/cm) 2,0 0 20 40 60 80 100 120 140 Time (ps) N. Jukam. et al. Nature Phot. 3, 715 (2009). (Integrated) Injection seeding gain switching of QCL • Injection seeding of QCL – Detection of QCL emission using coherent techniques 8 8 4 0 -4 RF OFF DC bias above threshold -8 0 Field (V/cm) Field (V/cm) Field (V/cm) • Ultrafast 100 200 Time (ps) 300 400 4 0 -4 -8 925 926 Time (ps) 927 928 8 4 0 -4 RF ON DC bias below threshold -8 0 100 200 300 400 500 600 700 800 900 1000 Time (ps) D. Oustinov et al., Nature Comm. DOI 10.1038 /ncomms (2010) J. Maysonnave et al., OL37, 4 (2012) Sampling of mode-locked THz QCL 1 Δfr ZnTe QCL frep1~10GHz l/4 l/2 1/frep2 Δfr = frep1 − n ⋅ frep2 fs-laser frep2 ~ 100MHz Down-converted THz spectrum Sampled pulse train -30 -40 -50 10 20 30 Frequency (MHz) 40 3mm ridge – surface plasmon Electric field (arb. units) QCL phase-locked to fs-laser rep rate Schematic of the asynchronous sampling setup 1/frep1 Measured Computed -100 -50 0 50 100 Time (ps) Barbieri et al. Nature Photon. 5, 306 (2011) Advances in electro-optic detection EOD: quasi phase matching A. B. C. vTHz @ t1 GaP (110) n′′ = n0 − n′ = n0 ph 2 3 n0 r41 ETHz 2 vNIRg vTHzph @ t2 GaP (110) n′′ = n0 − n′ = n0 2 3 n0 r41 ETHz 2 vNIRg vTHzph @ t2 GaP (110) GaP (-1-10) n′′ = n0 + n′ = n0 2 3 n0 r41 ETHz 2 vNIRg -‐ sensiFvity of the EOS can be increased by an increase of interacFon length without compromise if the mismatching between probe and THz pulses is handled J. Darmo et al. Elerctron Lett. 46, 788 (2010) EOD: quasi phase matching response funcFon of ... ... periodically inverted crystalline orientaFon of individual layers of EOS g (ω, Ω) = exp[i ⋅ Δk (ω, Ω)⋅ L] − 1 ⋅ {1 − exp[i ⋅ Δk (ω, Ω)⋅ L] + exp[i ⋅ Δk (ω, Ω)⋅ 2L] − exp[i ⋅ Δk (ω, Ω)⋅ NL]} i ⋅ Δk (ω, Ω) ... or exp[i ⋅ Δk (ω , Ω)⋅ L] − 1 1 − (− 1) ⋅ exp[i ⋅ Δk (ω , Ω)⋅ (N + 1)⋅ L] g (ω , Ω) = × i ⋅ Δk (ω , Ω) 1 + exp[i ⋅ Δk (ω , Ω)⋅ L] N +1 single layer responce ‚‚enhancement‘‘ factor (frequency dependent) J. Darmo et al. Elerctron Lett. 46, 788 (2010) EOD: quasi phase matching photodetectors l/2 plate & Wollaston prism electro-‐opFc crystal ellipFcally polarized NIR probe linearly polarized NIR probe EO signal (arb. units) THz wave 16 a/ 14 L = 1.5 mm L = 0.3 mm L = 5x0.3 mm 12 10 8 6 4 2 0 0 1 2 3 4 5 frequency (THz) IQCLSW 2012, 2.-6. Sept. 2012, Baden, Austria J. Darmo et al. Elerctron Lett. 46, 788 (2010) Outlook þ gain saturation and gain recovery dynamics (design impact) þ gain degradation mechanisms (temperature, heterogeneous active region) þ broadband THz laser/amplifier þ waveguide dispersion, mode locking þ mode-locked QCL for remote sensing þ large area surface emitting QCLs