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Electromagnetically Induced Transparency (EIT) via Spin Coherences in Semiconductor Hailin Wang Oregon Center for Optics, University of Oregon, USA Students: Shannon O Leary Susanta Sarkar Yumin Shen Phedon Palinginis Mark Phillips Tao Li Collaborations: C. Chang-Hasnain UC Berkeley R. Binder Univ. of Arizona J. Prineas Univ. of Iowa R.T. Cox CNRS, France Supported by DARPA, NSF, ARO

Outline Introduction EIT: Destructive interference via quantum coherence Why we are interested in EIT? Challenges for realizing EIT in semiconductors Experimental realization of EIT in semiconductors Exciton spin coherence Electron spin coherence Future work

Quantum Coherence Coherent superposition with well-defined relative phase between probability amplitudes b> a> Dipole optical transition Two-level system: ψ >= C a > + C b a b e.g. atoms, spins > Quantum coherence can be induced and manipulated via optical processes.

Nonradiative Quantum Coherence Nonradiative coherence: C b > + C c > b c a> b> and c> are not directly coupled by a dipole optical transition. b> c> Quantum interference: Total optical transition rate depends on the relative phase of the probability amplitudes.

Electromagnetically Induced Transparency (EIT) a> 2 Ca = Cb a + Cc a 2 = 0 b> c> Harris, Physics Today 50 (7), 36 (1997); Scully & Zubairy, Quantum Optics. ψ >= C b > + C c b c > Population trapped state: A special superposition state with C b a = C c a EIT: Vanishing optical absorption due to complete destructive quantum interference

EIT: Quantum Interference Induced Transparency a> a> b> c> b> c> Absorption Destructive quantum interference Absorption Refractive Index Frequency Refractive Index Frequency

Manipulating Light with EIT Slow and stored light Entangled photon pairs Light-matter quantum interface Lasing without inversion Nonlinear optics with single photons Stimulated Raman adiabatic passage For a review, see for example, Lukin, Rev. Mod. Phys. 75, 457 (2003).

Slow Light v dω c g = = dk dn n + ω dω b> a> c> Group velocity ~ c /10 7 Hau et al., Nature 397, 594 (1999). Kash et al., Phys. Rev. Lett. 82, 5229 (1999). Budker et al., Phys. Rev. Lett. 83, 1767 (1999). Application: e.g., Optical buffers (Chang-Hasnain, UC Berkeley) Refractive Index Frequency

Spin-Photon Correlation a> > > Duan et al., Nature 414, 413 (2001). Emission of a photon via the spontaneous Raman transition is correlated with a spin flip. Application Quantum state transfer, entangled photon pairs, quantum repeaters, and long distance quantum communication

Quantum Control of Single Photons with EIT Functional quantum nodes for entanglement distribution over scalable quantum networks, Science 316, 1316 (2006). Kimble group Generation of narrow-bandwidth paired photons: use of a single driving laser, Phys. Rev. Lett. 97, 113602 (2006). Harris group Storage and retrieval of single photons transmitted between remote quantum memories, Nature 438, 833 (2005). Kuzmich group Electromagnetically induced transparency with tunable singlephoton pulses, Nature 438, 837 (2005). Lukin group

Challenges for EIT in Semiconductors Short decoherence time Solution 1: Pursuing quantum interference in a transient regime Solution 1: Using robust quantum coherence. Manybody Coulomb interactions Fundamentally affect optical processes in semiconductors. Solution: Understand and harness manybody interactions for EIT.

Optical Excitations in Semiconductors: Excitons ω c> v> Absorption GaAs Excitons: Bound states of an e-h pair E B ~ 10 mev r B ~ 10 nm 1.51 1.52 Energy (ev) Very loosely bound e-h pairs! Collective excitation of the crystal Manybody interactions between excitons

Three Types of EIT Systems a control 3> 2> probe 1> b control probe 3> 2> 1> c control 3> 1> probe 2> Demonstrated EIT using analogous systems in semiconductors: a) Exciton spin coherence [Phys. Rev. Lett. 89, 186401 (2002)] b) Biexciton coherence [Phys. Rev. Lett. 91, 183602 (2003)] c) Electron spin coherence [Phys. Rev. B 70, 153307 (2004); Phys. Rev. B 72, 035343 (2005); Opt. Lett. 32, 569 (2007).]

Outline Introduction EIT: Destructive interference via quantum coherence Why we are interested in EIT? Challenges for realizing EIT in semiconductors Experimental realization of EIT in semiconductors Exciton spin coherence Electron spin coherence Summary

Exciton Spin Coherence s z = 1/2 s z =+1/2 AlGaAs GaAs AlGaAs σ+ k σ k j z = 3/2 j z =+3/2 GaAs quantum well Exciton spin coherence: coherent superposition of spinup and spin-down exciton states The two transitions share no common state. No exciton spin coherence can be induced in a noninteracting exciton system.

Excitons: A Interacting Many-Particle System Exchange interaction: r B ~ 10 nm Exciton wave-functions start to overlap at relatively low densities. 2 ψ X e h e h e h e h h e h e h e h e Coulomb correlation: For nearby excitons, charge fluctuations are strongly correlated. Attractive correlations can lead to the formation of exciton molecules or biexcitons. e-h h-e biexciton

Exciton Spin Coherence via Biexcitons Coupling exciton spin states via biexcitonic transitions: Biexciton > B Exciton σ+ σ > > ψ >= C > + C > Taking advantage of manybody interactions between excitons to induce quantum coherence and realize EIT.

EIT with Ultrafast Pulses > B Probe Pump > > Intensity probe pump A long pump pulse and a short probe induce a spin coherence. Re { ρ + } -5 0 5 Spin coherence γt Re(ρ +- )<0: Phased for destructive interference.

Experimental Configuration 6 ps 800 nj/cm 2 GaAs QW Probe > B Pump 150 fs 8 nj/cm 2 > > Prepulse 3 ps 100 nj/cm 2 Prepulse g> The prepulse pulse arrives 10 ps before the pump to inject spin-down excitons.

Biexciton Resonance > B Absorption (αl) 1 T=10 K biexciton Probe > > Prepulse 0 1.536 1.540 1.544 Energy (ev) g> 10 nm GaAs/AlGaAs QW Dashed curve: Absorption spectrum without prepulse. Solid curve: Absorption spectrum with prepulse.

EIT from Exciton Spin Coherence > B 1 τ =-3 ps Probe Pump EIT > > 10 nm GaAs QW T=10 K Absorption (αl) 0 1 τ = 6 ps t Phys. Rev. Lett. 89, 186401 (2002). 0 1.536 1.540 1.544 Energy (ev) t

EIT from Spin Coherence > B Probe Pump > > Absorption Theoretical calculation based on a 3-level model. -5 0 5 δ/γ Dashed line: Absorption spectrum when the spin coherence is artificially turned off.

Two-Exciton States e-h xx> ////////// bx> x> e-h h-e e-h biexciton Axt and Stahl, Z. Phys. B 93, 195 (1994). Östreich et al., Phys. Rev. Lett. 74, 4698 (1995). Kner et al., Phys. Rev. Lett. 81, 5386 (1998). Sieh et al., Phys. Rev. Lett. 82, 3112 (1999). g> e-h The two-exciton states play an essential role in coherent optical processes in semiconductors. Only 1s exciton states are inlcuded.

Spin Coherence via Two-Exciton Scattering States ////////// > U > B Inducing spin coherence via twoexciton scattering states? > > Experiment: The pump pulse excites excitons directly: no prepulse is needed. g> EIT occurs at the energy of the exciton resonance.

EIT via Exciton spin Coherence Phys. Rev. Lett. 89, 186401 (2002). -1/2> 1/2> Absorption (αl) 1 T=10 K Probe Pump -3/2> 3/2> 10 nm GaAs QW 0 1.535 1.540 Energy (ev) The pump and probe couple to transitions that share no common states. Exciton spin coherence induced via two-exciton continuum states can also lead to EIT.

EIT from Biexciton Coherence Two pathways to drive the system to state x>: g> to x> & bx> to x> bx> Pump x> Probe g> biexciton exciton Biexciton coherence: Coherent superposition of g> and x>. The probe and pump couple to the exciton and biexciton transitions, respectively. The EIT dip occurs at the exciton absorption resonance.

EIT from Biexciton Coherence 3 τ =-1 ps biexciton The pump is tuned slightly above the biexciton resonance. Absorption (αl) 0 3 τ = 10 ps The absorption dip occurs at the exciton resonance. Delay dependence shows the coherent nature of the dip. 0 1.526 1.528 Energy (ev) Phys. Rev. Lett. 91, 183602 (2003).

Outline Introduction EIT: Destructive interference via quantum coherence Why we are interested in EIT? Challenges for realizing EIT in semiconductors Experimental realization of EIT in semiconductors Exciton spin coherence Electron spin coherence Future work

Electron Spin Coherence in Semiconductors Electron spin coherence is exceptionally robust. can last as long as 0.1 μs and remain robust at room temperature. 300K Kikkawa et al, Science 277, 1284 (1997). Faraday Rotation (Arb. U.) 200K 100K 50K 20K GaAs QW Suitable three-level systems? 10K 0 100 200 300 400 Delay (ps)

Band Structure s z = 1/2 s z =+1/2 AlGaAs GaAs AlGaAs σ+ k σ k j z = 3/2 j z =+3/2 GaAs quantum well The lowest energy interband transitions in a GaAs QW are characterized by two heavy-hole (HH) transitions. The two transitions share no common state. No electron spin coherence can be induced.

V-System in an External Magnetic Field Inducing spin coherence: Coupling electron spin states to a common valence band state via dipole transitions. s x = 1/2 s x =1/2 σ σ B x z Voigt configuration J z =3/2 GaAs QW Electron spins are aligned with the external magnetic field. In a weak magnetic field, J z remains approximately a good quantum number for the holes.

CW EIT Experiments Pump Differential transmission: Probe σ σ ΔT = T (pump-on) T (pump-off) J z =3/2 The pump and probe excite an electron spin coherence. Destructive interference induced by the spin coherence can lead to: Induced resonance in transmission (dip in the absorption).

Coherent Zeeman Resonance s x = 1/2 s x =1/2 ΔT = T Pump T on pump off σ σ T=10 K, 13 nm GaAs J z =3/2 0.5T Probe Pump B GaAs QW ΔT/T [arb. units] 2.0T 4.0T The sharp Zeeman resonance arises from destructive interference induced by the electron spin coherence. Phys. Rev. B 70, 153307 (2004). -15 0 15 Detuning [GHz]

Polarization Dependence T=10 K, 13 nm GaAs B=2.0T (σ σ ) s x = 1/2 s x =1/2 σ σ+ σ σ+ ΔT/T [arb. units] (σ+ σ ) (x, y) J z =3/2 s x = 1/2 x y J z =3/2 s x =1/2 y x (y, y) HH+ HH- -15 0 15 Detuning [GHz] Coherent Zeeman resonance in the crosslinear configuration can be viewed as EIT from the electron spin coherence.

V-System without External Magnetic Fields C> s z =-1/2 s z =1/2 Using light hole transitions in a waveguide. TM (z) LH> z z σ+ σ j z =-1/2 j z =1/2 k QW TE (σ+, σ-) 1 2 = 1/ 2 >= Y 11 > > + Y > > 3 3 j z 10 Key features: Spin-orbit coupling mixes the spin-up and spin-down states for the light-hole (LH) band: double-v system. Inducing electron spin coherence in the absence of an external magnetic field. The waveguide geometry enables long interaction length.

GaAs/AlGaAs QW Waveguide Transmission (Arb. Units) T = 20 K TE LH HH TM LH 795 800 805 810 Wavelength (nm) k TE TM (z) QW Sample: Single 17.5 nm GaAs QW AlGaAs Cladding Length ~ 100 μm For TM polarization, HH exciton resonance is nearly negligible, as expected from optical selection rules.

EIT in a QW Waveguide TM- Probe Light-Hole exciton transition k B s z =-1/2 s z =1/2 s z =-1/2 s z =1/2 z σ+ σ z TE-Pump (σ+, σ-) j z =-1/2 j z =1/2 ΔT (Arb. Units) GaAs QW B=0 T=50 K -5 0 5 Detuning (GHz) ΔT (Arb. Units) T = 50 K, B = 0.25 T -4-2 0 2 4 Detuning (GHz) Phys. Rev. B 72, 035343 (2005)

V-Type vs Λ-type Three-Level Systems a g V-System Spin decoherence is limited by radiative decay. Degree of transparency is limited. Λ-System Spin states are the ground states. Nearly complete transparency can be achieved.

Λ-type Three-Level System via Trions X Trion: An exciton bound to an electron (negatively charged exciton). Involves two electrons and one hole. Kheng et al., PRL 71, 1752 (1993). The formation of the Λ-system requires an excess electron population in the conduction band.

Mixed Type Quantum Well Structures 23Å GaAs 160Å GaAs X-valley 112Å AlAs Mixed type QW: The bottom of the conduction band in the narrow QW is higher than the X-valley in the AlAs barrier. Narrow well: type II Wide well: type I Galbraith et al., Phys. Rev. B 45, 013499 (1992). Electrons in narrow QW transfer via X-valley in the barrier to wide QW. Holes remain confined in the narrow QW. Advantage: Using optical injection to control the electron density in the wide QW.

Formation of Trions in a Mixed-Type QW PL Intensity X X With increasing number of electrons in the wide well, more excitons are converted into trions. Trion binding energy: 1.6 mev 1.528 1.530 1.532 1.534 Energy (ev) For black lines, the sample is excited by both the red and green laser beams. I= 0.5, 1, 2 mw/cm 2 I= 2 W/cm 2

Λ-type Three-Level System via Trions Trion states +3/2 z -3/2 z B x σ+ σ z Electron spin states +1/2 z x Δ -1/2 z GaAs QW x

Coherent Zeeman Resonance in the Λ-System B ΔT (Arb. Units) T=10K B=0.3T Absorption Probe pump Pump 1.528 1.532 1.536 Energy (ev) -5 0 5 Pump-Probe Detuning (GHz) The width of the coherent Zeeman resonance corresponds to a spin decoherence time of 1 ns. Opt. Lett. 32, 569 (2007). Amplitude (Arb. Units) Trion HH 1.531 1.532 1.533 1.534 1.535 Pump Energy (ev) 0.5 0.4 0.3 0.2 0.1 0.0 Absorption (αl)

Effects of Electron Injection ΔT (Arb. Units) -10-5 0 5 10 Pump-Probe Detuning (GHz) 0.5 W/cm 2 1 W/cm 2 5 W/cm 2 NL P γ 1 2 The coherent response is quenched by the increased dipole decoherence induced by the carrier injection. Coherent Zeeman resonance amplitudes are suppressed with increased electron injection. The linewidth does not appreciably broaden.

Effects of Carrier-Carrier Interactions Absorption (Arb. Units) HH LH 1.530 1.532 1.534 1.536 1.538 1.540 Energy (ev) Red curve: absorption spectrum obtained at an injection level of 0.25 mw/cm 2 Trion resonance present without injection due to residual doping. Trion absorption peak enhanced by the injection of electrons. Absorption resonance broadens dramatically due to efficient carrier-carrier carrier scattering. What is next?

Trions in II-VI Semiconductors CdTe/CdZnTe quantum well Modulation doping: 2x10 10 /cm 2 Kheng et al., PRL 71, 1752 (1993). II-VI semiconductors feature greater binding energy. Pronounced and robust trion resonance in both absorption and emission spectra (the Y-resonance).

Spin Precession from Trions in CdTe QW Spin decoherence time ~ 1 ns ΔT/T Modulation doping: 2x10 10 /cm 2 0 500 1000 1500 2000 Delay time (ps)

EIT from Trions in CdTe Quantum wells ΔT (Arb. Units) T=10 K B=0.4 T Probe Pump B 771.88 771.90 771.92 771.94 771.96 Probe Wavelength (nm) The pump is at the trion resonance (λ ~ 771.92 nm). Pronounced coherent Zeeman resonance arising from destructive interference induced by the electron spin coherence.

Future Work Optimize the EIT process using trions and electron spin coherences. Coherent spin flipping via adiabatic passage. Incorporate EIT via trions in a waveguide geometry. Spin-phonon correlations. Generation of entangled photons.

Summary Main Theme: EIT can be realized in semiconductors. Demonstrated EIT with exciton spin coherence and biexciton coherence. EIT can also be realized with robust electron spin coherence, opening possibilities for applications. Manybody interactions between optical excitations modifies fundamentally coherent optical processes in semiconductors.

Acknowledgement University of Oregon: Mark Phillips (now at Sandia National Labs) Phedon Palinginis (now at UC Berkeley) Susanta Sarkar Yumin Shen Collaborations: Connie Chang-Hasnain Rolf Binder UC Berkeley University of Arizona Supported by DARPA, NSF, and ARO