Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

The effect of Auger heating on intraband carrier relaxation in semiconductor quantum rods

Abstract

The rate at which excited charge carriers relax to their equilibrium state affects many aspects of the performance of nanoscale devices, including switching speed, carrier mobility and luminescence efficiency. A better understanding of the processes that govern carrier relaxation therefore has important technological implications. A significant increase in carrier–carrier interactions caused by strong spatial confinement of electronic excitations in semiconductor nanostructures leads to a considerable enhancement of Auger effects, which can further result in unusual, Auger-process-controlled recombination and energy relaxation regimes. Here, we report the first experimental observation of efficient Auger heating in CdSe quantum rods at high pump intensities, leading to a strong reduction of carrier cooling rates. In this regime, the carrier temperature is determined by the balance between energy outflow through phonon emission and energy inflow because of Auger heating. This equilibrium results in peculiar carrier cooling dynamics that closely correlate with recombination dynamics, an effect never seen before in bulk or nanoscale semiconductors.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Schematic representation of two different types of Auger effects in semiconductor nanocrystals.
Figure 2: Time-resolved uPL spectra of QR samples and carrier temperature dynamics derived from them.
Figure 3: Carrier cooling in the regime controlled by the competition between Auger heating and phonon emission.
Figure 4: Carrier overheating, ΔTe, at Δt=2 ps as a function of the average number of e–h pairs per QR.

Similar content being viewed by others

References

  1. Alivisatos, A. P. Semiconductor clusters, nanocrystals, and quantum dots. Science 271, 933–937 (1996).

    Article  ADS  Google Scholar 

  2. Efros, Al. L., Kharchenko, V. A. & Rosen, M. Breaking the phonon bottleneck in nanometer quantum dots: Role of Auger-like processes. Solid State Commun. 93, 281–284 (1995).

    Article  ADS  Google Scholar 

  3. Klimov, V. I. & McBranch, D. W. Femtosecond 1P-to-1S electron relaxation in strongly confined semiconductor nanocrystals. Phys. Rev. Lett. 80, 4028–4031 (1998).

    Article  ADS  Google Scholar 

  4. Guyot-Sionnest, P., Shim, M., Matranga, C. & Hines, M. Intraband relaxation in CdSe quantum dots. Phys. Rev. B 60, R2181–R2184 (1999).

    Article  ADS  Google Scholar 

  5. Mohamed, M. B., Burda, C. & El-Sayed, M. A. Shape dependent ultrafast relaxation dynamics of CdSe nanocrystals: Nanorods vs nanodots. Nano Lett. 1, 589–593 (2001).

    Article  ADS  Google Scholar 

  6. Chepic, D. I. et al. Auger ionization of semiconductor quantum drops in a glass matrix. J. Lumin. 47, 113–127 (1990).

    Article  Google Scholar 

  7. Klimov, V. I., Mikhailovsky, A. A., McBranch, D. W., Leatherdale, C. A. & Bawendi, M. G. Quantization of multiparticle Auger rates in semiconductor quantum dots. Science 287, 1011–1013 (2000).

    Article  ADS  Google Scholar 

  8. Htoon, H., Hollingsworth, J. A., Dickerson, R. & Klimov, V. I. Effect of zero-dimensional to one-dimensional transformation on Auger recombination in semiconductor quantum rods. Phys. Rev. Lett. 91, 227401 (2003).

    Article  ADS  Google Scholar 

  9. Wang, L.-W., Califano, M., Zunger, A. & Franceschetti, A. Pseudopotential theory of Auger processes in CdSe quantum dots. Phys. Rev. Lett. 91, 056404 (2003).

    Article  ADS  Google Scholar 

  10. Downer, M. C. & Shank, C. V. Ultrafast heating of silicon on sapphire by femtosecond optical pulses. Phys. Rev. Lett. 56, 761–764 (1986).

    Article  ADS  Google Scholar 

  11. Borri, P., Ceccherini, S., Gurioli, M. & Bogani, F. Auger heating of carriers in GaAs/AlAs heterostructures. Solid State Commun. 103, 77–81 (1997).

    Article  ADS  Google Scholar 

  12. Klimov, V., Haring Bolivar, P. & Kurz, H. Hot-phonon effects in femtosecond luminescence spectra of electron-hole plasmas in CdS. Phys. Rev. B 52, 4728–4731 (1995).

    Article  ADS  Google Scholar 

  13. Murray, C. B., Norris, D. J. & Bawendi, M. G. Synthesis and characterization of nearly monodisperse CdE (E=S,Se,Te) semiconductor nanocrystallites. J. Am. Chem. Soc. 115, 8706–8715 (1993).

    Article  Google Scholar 

  14. Manna, L., Scher, E. C. & Alivisatos, A. P. Synthesis of soluble and processable rod-, arrow-, teardrop-, and tetrapod-shaped CdSe nanocrystals. J. Am. Chem. Soc. 122, 12700–12706 (2000).

    Article  Google Scholar 

  15. Peng, Z. A. & Peng, X. Mechanisms of the shape evolution of CdSe nanocrystals. J. Am. Chem. Soc. 123, 1389–1395 (2001).

    Article  Google Scholar 

  16. Shah, J. Ultrafast luminescence spectroscopy using sum frequency generation. IEEE J. Quantum Electron. 24, 276–288 (1988).

    Article  ADS  Google Scholar 

  17. Achermann, M., Hollingsworth, J. A. & Klimov, V. I. Multiexcitons confined within a subexcitonic volume: Spectroscopic and dynamical signatures of neutral and charged biexcitons in ultrasmall semiconductor nanocrystals. Phys. Rev. B 68, 245302 (2003).

    Article  ADS  Google Scholar 

  18. Xu, S., Mikhailovsky, A. A., Hollingsworth, J. A. & Klimov, V. I. Hole intraband relaxation in strongly confined quantum dots: Revisiting the 'phonon bottleneck' problem. Phys. Rev. B 65, 045319 (2002).

    Article  ADS  Google Scholar 

  19. Pötz, W. & Kocevar, P. Electronic power transfer in pulsed laser excitation of polar semiconductors. Phys. Rev. B 28, 7040–7047 (1983).

    Article  ADS  Google Scholar 

  20. Kocevar, P. Hot phonon dynamics. Physica B 134, 155–163 (1985).

    Article  Google Scholar 

Download references

Acknowledgements

The authors thank Dr. H. Htoon for useful discussions. This work was supported by Los Alamos LDRD Funds and the Chemical Sciences, Biosciences, and Geosciences Division of the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Victor I. Klimov.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Achermann, M., Bartko, A., Hollingsworth, J. et al. The effect of Auger heating on intraband carrier relaxation in semiconductor quantum rods. Nature Phys 2, 557–561 (2006). https://doi.org/10.1038/nphys363

Download citation

  • Received:

  • Revised:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nphys363

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing