Abstract

We propose an experimentally viable attosecond transient absorption spectroscopy scheme to resolve controversies regarding multiexciton (ME) generation in nanoscale systems. Absence of oscillations indicates that light excites single excitons, and MEs are created by incoherent impact ionization. An oscillation indicates the coherent mechanism, involving excitation of superpositions of single and MEs. The oscillation decay, ranging from 5 fs at ambient temperature to 20 fs at 100 K, gives the elastic exciton-phonon scattering time. The signal is best observed with multiple-cycle pump pulses.

© 2014 Optical Society of America

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2013 (6)

K. T. Kim, C. Zhang, A. D. Shiner, S. E. Kirkwood, E. Frumker, G. Gariepy, A. Naumov, D. M. Villeneuve, and P. B. Corkum, “Manipulation of quantum paths for spacetime characterization of attosecond pulses,” Nat. Phys. 9, 159–163 (2013).
[Crossref]

J. Prell, L. Borja, D. Neumark, and S. Leone, “Simulation of attosecond-resolved imaging of the plasmon electric field in metallic nanoparticles,” Ann. Phys. 525, 151–161 (2013).
[Crossref]

M. Schultze, E. Bothschafter, A. Sommer, S. Holzner, W. Schweinberger, M. Fiess, M. Hofstetter, R. Kienberger, V. Apalkov, V. Yakovlev, M. Stockman, and F. Krausz, “Controlling dielectrics with the electric field of light,” Nature 493, 75–78 (2013).
[Crossref]

A. Schiffrin, T. Paasch-Colberg, N. Karpowicz, V. Apalkov, D. Gerster, S. Mühlbrandt, M. Korbman, J. Reichert, M. Schultze, S. Holzner, J. V. Barth, R. Kienberger, R. Ernstorfer, V. S. Yakovlev, M. I. Stockman, and F. Krausz, “Optical-field-induced current in dielectrics,” Nature 493, 70–74 (2013).
[Crossref]

A. Wirth, R. Santra, and E. Goulielmakis, “Real time tracing of valence-shell electronic coherences with attosecond transient absorption spectroscopy,” Chem. Phys. 414, 149–159 (2013).
[Crossref]

C. Ott, A. Kaldun, P. Raith, K. Meyer, M. Laux, J. Evers, C. Keitel, C. Greene, and T. Pfeifer, “Lorentz meets fano in spectral line shapes: A universal phase and its laser control,” Science 340, 716–720 (2013).
[Crossref] [PubMed]

2012 (5)

S. Chen, M. J. Bell, A. R. Beck, H. Mashiko, M. Wu, A. N. Pfeiffer, M. B. Gaarde, D. M. Neumark, S. R. Leone, and K. J. Schafer, “Light-induced states in attosecond transient absorption spectra of laser-dressed helium,” Phys. Rev. A. 86, 063408 (2012).
[Crossref]

G. Herink, D. Solli, M. Gulde, and C. Ropers, “Field-driven photoemission from nanostructures quenches the quiver motion,” Nature 483, 190–193 (2012).
[Crossref] [PubMed]

S. Chew, F. Süßmann, C. Späth, A. Wirth, J. Schmidt, S. Zherebtsov, A. Guggenmos, A. Oelsner, N. Weber, J. Kapaldo, A. Gliserin, M. Stockman, M. Kling, and U. Kleineberg, “Time-of-flight-photoelectron emission microscopy on plasmonic structures using attosecond extreme ultraviolet pulses,” Appl. Phys. Lett. 100, 051904 (2012).
[Crossref]

X. Zhou, P. Ranitovic, C. W. Hogle, J. H. D. Eland, H. C. Kapteyn, and M. M. Murnane, “Probing and controlling non-bornoppenheimer dynamics in highly excited molecular ions,” Nat. Phys. 8, 232–237 (2012).
[Crossref]

A. Borisov, P. Echenique, and A. Kazansky, “Attostreaking with metallic nano-objects,” New J. Phys. 14, 023036 (2012).
[Crossref]

2011 (7)

E. Skopalová, D. Lei, T. Witting, C. Arrell, F. Frank, Y. Sonnefraud, S. Maier, J. Tisch, and J. Marangos, “Numerical simulation of attosecond nanoplasmonic streaking,” New J. Phys. 12, 083003 (2011).
[Crossref]

F. Süßmann and M. F. Kling, “Attosecond nanoplasmonic streaking of localized fields near metal nanospheres,” Phys. Rev. B 84, 121406 (2011).
[Crossref]

P. Kambhampati, “Unraveling the structure and dynamics of excitons in semiconductor quantum dots,” Acc. Chem. Res. 44, 1–13 (2011).
[Crossref]

S. Zherebtsov, T. Fennel, J. Plenge, E. Antonsson, I. Znakovskaya, A. Wirth, O. Herrwerth, F. Süßmann, C. Peltz, I. Ahmad, S. a. Trushin, V. Pervak, S. Karsch, M. J. J. Vrakking, B. Langer, C. Graf, M. I. Stockman, F. Krausz, E. Rühl, and M. F. Kling, “Controlled near-field enhanced electron acceleration from dielectric nanospheres with intense few-cycle laser fields,” Nat. Phys. 7, 656–662 (2011).
[Crossref]

M. Krüger, M. Schenk, and P. Hommelhoff, “Attosecond control of electrons emitted from a nanoscale metal tip,” Nature 475, 78–81 (2011).
[Crossref] [PubMed]

M. Durach, A. Rusina, M. F. Kling, and M. I. Stockman, “Predicted ultrafast dynamic metallization of dielectric nanofilms by strong single-cycle optical fields,” Phys. Rev. Lett. 107, 086602 (2011).
[Crossref] [PubMed]

M. Holler, F. Schapper, L. Gallmann, and U. Keller, “Attosecond electron wave-packet interference observed by transient absorption,” Phys. Rev. Lett. 106, 123601 (2011).
[Crossref] [PubMed]

2010 (8)

E. Goulielmakis, Z. Loh, A. Wirth, R. Santra, N. Rohringer, V. S. Yakovlev, S. Zherebtsov, T. Pfeifer, A. M. Azzeer, M. F. Kling, S. R. Leone, and F. Krausz, “Real-time observation of valence electron motion,” Nature 466, 739–743 (2010).
[Crossref] [PubMed]

F. Reiter, U. Graf, E. E. Serebryannikov, W. Schweinberger, M. Fiess, M. Schultze, A. M. Azzeer, R. Kienberger, F. Krausz, A. M. Zheltikov, and E. Goulielmakis, “Route to attosecond nonlinear spectroscopy,” Phys. Rev. Lett. 105, 243902 (2010).
[Crossref]

H. Wang, M. Chini, S. Chen, C.-H. Zhang, F. He, Y. Cheng, Y. Wu, U. Thumm, and Z. Chang, “Attosecond time-resolved autoionization of argon,” Phys. Rev. Lett. 105, 143002 (2010).
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2005 (3)

R. D. Schaller, V. M. Agranovich, and V. I. Klimov, “High-efficiency carrier multiplication through direct photogeneration of multi-excitons via virtual single-exciton states,” Nat. Phys. 1, 189–194 (2005).
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Figures (4)

Fig. 1
Fig. 1 Experimental method. A femtosecond or attosecond UV/VUV pump pulse creates a superposition of SE and ME states. Phonon-induced dephasing and relaxation are probed using attosecond transient absorption via promotion of a core electron into the valence band using an EUV probe pulse.
Fig. 2
Fig. 2 Absorption of the probe pulse centered at the frequency of the transition from a core electron to the ME hole as a function of the pump-probe delay.
Fig. 3
Fig. 3 (a) Population of the SE electron and hole states forming the wave-packet excited in the Pb68Se68 QD by the femtosecond pump. (b) Coherence oscillations in the attosecond probe absorption signal at T=347 K (bold green), 128 K (dashed purple), and 0 K (solid blue).
Fig. 4
Fig. 4 Transient absorption spectrum of a PbSe QD. The pulse is centered at 47 eV, the absorption peak at 46.6 eV is from the SE states, and the absorption peak at 47.4 eV is from the MEs.

Tables (1)

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Table 1 Dephasing times for a superposition of many states vs. a superposition of two states.

Equations (2)

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σ ( ω , t ) = 4 π c I , I ρ I , I ( t ) F I | Z | F F | Z | I E F i 2 Γ E I ω .
[ ρ ME , ME ρ ME , SE n e i Δ E t e t 2 τ 2 ρ SE n , ME e i Δ E t e t 2 τ 2 ρ SE n , SE n ] .

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