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Longer than 1 nano-second !!! Long-Lived Dilute Photocarriers in Individualy-suspended Single-Walled Carbon Nanotubes Y. Hashimoto, A. Srivastava, J. Shaver, G. N. Ostojic, S. Zaric, V. C. Moore, R. H. Hauge, R. E. Smalley, and J. Kono Rice University Out line •Introduction & Purpose •Sample and Experimental setup •Results and discussion •Photo-induced carrier dynamics •Polarization memory •Summary Supported by TATP and Welch Foundation Introduction to Single-Walled Carbon Nanotube Diameter: 1 nano-meter Length: < 1 inch ultimate quantum wire Each peak corresponds to particular (n,m) Single Walled Carbon Nanotubes photo-induced carrier life time < 1 ps Bundled SWNT 5 - 50 ps Isolated SWNT ~ ns Isolated SWNT ~ 20 ns Theoretical Hertel and Moos, Phys. Rev. Lett. 84, 5002 (2000) Chen et al., Appl. Phys. Lett. 81, 975 (2002) Han et al., Appl. Phys. Lett. 82, 1458 (2003) Lauret et al., Phys. Rev. Lett. 90, 057404 (2003) Korovyanko et al. Phys. Rev. Lett. 92, 017403 (2004) G. N. Ostojic et al., Phys. Rev. Lett. 92, 117402 (2004) Y.-Z. Ma et al., J. Chem. Phys. 120, 3368 (2004) A. Hagen et al., Appl. Phys. A 78, 1137 (2004) F. Wang et al., Phys. Rev. Lett. 92, 177401 (2004) This work C. D. Spataru et al., cond-mat/0301220 v1 (2003) The relaxation dynamics of the photo-excited carriers in SWNTs radiative Non-radiative 1 1 rad ~ ps 1 non rad ~ ns non rad rad nonrad What kind of the Non-radiative relaxation is taken place ? ~640 e-h pairs rs 1.5nm rex 2.5nm ~1mJ/cm2 in In the previous study with a high-peak power OPA laser PRL. 92, 077402 (2004) 1 mm SWNT < 20 ps Exciton-exciton interaction ? Purpose Photo-induced carrier relaxation dynamics in the low excitation limit 1 e-h pair per 1 mm SWNT Single Walled Carbon Nanotube Sample Absorption spectrum -1 Absorption [cm ] SDS miscelled SWNT SWNT 2.2 2.0 1.8 1.6 1.4 1.2 1.2 1.4 1.6 Photon energy [eV] 1.8 Absorption shows sharp peaks SDS micelle Science VOL 297 593 (2002) SWNT is well isolated Experimental setup -1 Absorption [cm ] Pulse picker 80 MHz – 800 kHz Laser wavelength: 1.550 eV (E2H2) Ti:s laser 80MHz 2.4 2.0 1.6 1.2 1.4 1.5 1.6 1.7 1.8 Photon Energy [eV] Si detector Delay stage (2 ns) l/2 Excitation fluence: 100 nJ/cm2 Pump : Probe = 10 : 1 SWNT Aperture Lock in Photo-induced carrier dynamics in SWNT in low excitation limit Room temperature T/T 10 10 10 10 -3 Repetition rate: 8 MHz -4 Polarization of the pump and probe: -5 -6 0 400 Time delay [ps] 800 Previous report in high excitation ~ 20 ps Photo-induced carrier dynamics shows very long decay !!! Pump and probe signal persist even at 1 nano-second Decay dynamics 1.0x10 -3 1: < 1 ps T/T 0.8 0.6 2: ~ 1 ns 0.4 0.2 0.0 0 500 Time delay [ps] 1000 Decay dynamics E2H2 E1H1 intraband transition E 5x10 -3 4 T/T 3 2 1 < 1 ps E2 0 -1 E1 ~ ns DOS E1H1 carrier recombination H1 1.0x10 -3 0.8 T/T H2 0 1 Time delay [ps] 0.6 0.4 0.2 0.0 0 500 1000 Time delay [ps] Polarization memory Polarization of the pump and probe pulses 1.0 10 Tll T P TllTll TT 0.8 P 0.6 -4 P T/T 10 Parallel Perpendicular -3 0.4 10 Tll T -5 0.2 0 400 800 Time delay [ps] 0.0 0 200 400 600 800 1000 Time delay [ps] Polarization memory persist even at 1 ns !!! In bundled SWNT, the polarization decay time ~ 10 ps O. J. Korovyanko et al., Phys. Rev. Lett. 92 017403 (2004) Summary T/T 10 10 10 10 -3 -4 -5 -6 0 400 Time delay [ps] 800 •The transient absorption of the isolated SWNTs in low excitation regime shows very fast (< 1 ps) E2H2 E1H1 intraband transition and very long (~ 1ns) E1H1 carrier recombination 1.0 0.6 P •The polarization memory in isolated SWNTs shows no decay even at 1 ns. 0.8 0.4 0.2 0.0 0 200 400 600 800 Time delay [ps] 1000 Future work Two color pump-probe in the isolated SWNT in the low excitation limit Excited SWNT (12,1)L : 797 nm (11,3)L : 792 nm (10,5)l : 786 nm (9,7)l : 790 nm Raman spectrum G mode ~200meV Intensity Caused by the graphite structure Depend on the chirality RBM mode ~30meV Depend on the diameter of the CNT 0 500 1000 1500 -1 Raman shift [cm ] How to estimate the carrier concentration Density of the SWNT: 9.7 x 1011mm/cm2 (in the 1mm path length cuvette) Density of the SWNT in solution: ~20 x 10-6g/cm3 Mass density of SWNT (11. 0): 2.06 x 10-18 g/mm Excitation intensity: Absorption: 6.2 x 1015 photon/cm2 Excitation intensity: 1 mJ/cm2 Photon energy: 1 eV 10% (per 1 mm) 6.2 1015 photon/ cm2 10% 2 6 . 4 10 photon/ mm 11 2 9.7 10 mm / cm Longer than 1 nano-second !!! Long-Lived Dilute Photocarriers in Individualy-suspended Single-Walled Carbon Nanotubes Y. Hashimoto, A. Srivastava, J. Shaver, G. N. Ostojic, S. Zaric, V. C. Moore, R. H. Hauge, R. E. Smalley, and J. Kono Rice University Out line •Introduction & Purpose •Sample and Experimental setup •Results and discussion •Photo-induced carrier dynamics •Polarization memory •Summary Supported by TATP and Welch Foundation Introduction to Single-Walled Carbon Nanotube Diameter: 1 nano-meter Length: < 1 inch ultimate quantum wire Single Walled Carbon Nanotubes photo-induced carrier life time < 1 ps Bundled SWNT 5 - 50 ps Isolated SWNT ~ ns Isolated SWNT ~ 20 ns Theoretical Hertel and Moos, Phys. Rev. Lett. 84, 5002 (2000) Chen et al., Appl. Phys. Lett. 81, 975 (2002) Han et al., Appl. Phys. Lett. 82, 1458 (2003) Lauret et al., Phys. Rev. Lett. 90, 057404 (2003) Korovyanko et al. Phys. Rev. Lett. 92, 017403 (2004) G. N. Ostojic et al., Phys. Rev. Lett. 92, 117402 (2004) Y.-Z. Ma et al., J. Chem. Phys. 120, 3368 (2004) A. Hagen et al., Appl. Phys. A 78, 1137 (2004) F. Wang et al., Phys. Rev. Lett. 92, 177401 (2004) This work C. D. Spataru et al., cond-mat/0301220 v1 (2003) The relaxation dynamics of the photo-excited carriers in SWNTs radiative Non-radiative 1 1 rad ~ ps 1 non rad ~ ns non rad rad nonrad What kind of the Non-radiative relaxation is taken place ? ~640 e-h pairs rs 1.5nm rex 2.5nm ~1mJ/cm2 in In the previous study with a high-peak power OPA laser PRL. 92, 077402 (2004) 1 mm SWNT < 20 ps Exciton-exciton interaction ? Purpose Photo-induced carrier relaxation dynamics in the low excitation limit 1 e-h pair per 1 mm SWNT Single Walled Carbon Nanotube Sample Absorption spectrum -1 Absorption [cm ] SDS miscelled SWNT SWNT 2.2 2.0 1.8 1.6 1.4 1.2 1.2 1.4 1.6 Photon energy [eV] 1.8 Absorption shows sharp peaks SDS micelle Science VOL 297 593 (2002) SWNT is well isolated Experimental setup -1 Absorption [cm ] Pulse picker 80 MHz – 800 kHz Laser wavelength: 1.550 eV (E2H2) Ti:s laser 80MHz 2.4 2.0 1.6 1.2 1.4 1.5 1.6 1.7 1.8 Photon Energy [eV] Si detector Delay stage (2 ns) l/2 Excitation fluence: 100 nJ/cm2 Pump : Probe = 10 : 1 SWNT Aperture Lock in Photo-induced carrier dynamics in SWNT in low excitation limit Room temperature T/T 10 10 10 10 -3 Repetition rate: 8 MHz -4 Polarization of the pump and probe: -5 -6 0 400 Time delay [ps] 800 Previous report in high excitation ~ 20 ps Photo-induced carrier dynamics shows very long decay !!! Pump and probe signal persist even at 1 nano-second Decay dynamics 1.0x10 -3 1: < 1 ps T/T 0.8 0.6 2: ~ 1 ns 0.4 0.2 0.0 0 500 Time delay [ps] 1000 Decay dynamics E2H2 E1H1 intraband transition E 5x10 -3 4 T/T 3 2 1 < 1 ps E2 0 -1 E1 ~ ns DOS E1H1 carrier recombination H1 1.0x10 -3 0.8 T/T H2 0 1 Time delay [ps] 0.6 0.4 0.2 0.0 0 500 1000 Time delay [ps] Polarization memory Polarization of the pump and probe pulses 1.0 10 Tll T P TllTll TT 0.8 P 0.6 -4 P T/T 10 Parallel Perpendicular -3 0.4 10 Tll T -5 0.2 0 400 800 Time delay [ps] 0.0 0 200 400 600 800 1000 Time delay [ps] Polarization memory persist even at 1 ns !!! In bundled SWNT, the polarization decay time ~ 10 ps O. J. Korovyanko et al., Phys. Rev. Lett. 92 017403 (2004) Summary T/T 10 10 10 10 -3 -4 -5 -6 0 400 Time delay [ps] 800 •The transient absorption of the isolated SWNTs in low excitation regime shows very fast (< 1 ps) E2H2 E1H1 intraband transition and very long (~ 1ns) E1H1 carrier recombination 1.0 0.6 P •The polarization memory in isolated SWNTs shows no decay even at 1 ns. 0.8 0.4 0.2 0.0 0 200 400 600 800 Time delay [ps] 1000 Future work Two color pump-probe in the isolated SWNT in the low excitation limit