Abstract
Coherently driven semiconductor quantum dots are one of the most promising platforms for non-classical light sources and quantum logic gates which form the foundation of photonic quantum technologies. However, to date, coherent manipulation of single charge carriers in quantum dots is limited mainly to their lowest orbital states. Ultrafast coherent control of high-orbital states is obstructed by the demand for tunable terahertz pulses. To break this constraint, we demonstrate an all-optical method to control high-orbital states of a hole via a stimulated Auger process. The coherent nature of the Auger process is proved by Rabi oscillation and Ramsey interference. Harnessing this coherence further enables the investigation of the single-hole relaxation mechanism. A hole relaxation time of 161 ps is observed and attributed to the phonon bottleneck effect. Our work opens new possibilities for understanding the fundamental properties of high-orbital states in quantum emitters and for developing new types of orbital-based quantum photonic devices.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Data availability
The raw data that support the findings of this study are available at https://doi.org/10.5281/zenodo.7947362 and from the corresponding author upon reasonable request.
Code availability
The codes that have been used for this study are available from the corresponding author upon reasonable request.
References
Zrenner, A. et al. Coherent properties of a two-level system based on a quantum-dot photodiode. Nature 418, 612–614 (2002).
Press, D., Ladd, T. D., Zhang, B. & Yamamoto, Y. Complete quantum control of a single quantum dot spin using ultrafast optical pulses. Nature 456, 218–221 (2008).
Fleischhauer, M., Imamoglu, A. & Marangos, J. P. Electromagnetically induced transparency: optics in coherent media. Rev. Mod. Phys. 77, 633–673 (2005).
Faraon, A. et al. Coherent generation of non-classical light on a chip via photon-induced tunnelling and blockade. Nat. Phys. 4, 859–863 (2008).
Michler, P. et al. A quantum dot single-photon turnstile device. Science 290, 2282–2285 (2000).
Ding, X. et al. On-demand single photons with high extraction efficiency and near-unity indistinguishability from a resonantly driven quantum dot in a micropillar. Phys. Rev. Lett. 116, 020401 (2016).
Tomm, N. et al. A bright and fast source of coherent single photons. Nat. Nanotechnol. 16, 399–403 (2021).
Liu, F. et al. High Purcell factor generation of indistinguishable on-chip single photons. Nat. Nanotechnol. 13, 835–840 (2018).
Huber, D. et al. Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots. Nat. Commun. 8, 15506 (2017).
Liu, J. et al. A solid-state source of strongly entangled photon pairs with high brightness and indistinguishability. Nat. Nanotechnol. 14, 586–593 (2019).
Sun, S., Kim, H., Luo, Z., Solomon, G. S. & Waks, E. A single-photon switch and transistor enabled by a solid-state quantum memory. Science 361, 57–60 (2018).
Jeannic, H. L. et al. Dynamical photon–photon interaction mediated by a quantum emitter. Nat. Phys. 18, 1191–1195 (2022).
Li, X. et al. An all-optical quantum gate in a semiconductor quantum dot. Science 301, 809–811 (2003).
Pelucchi, E. et al. The potential and global outlook of integrated photonics for quantum technologies. Nat. Rev. Phys. 4, 194–208 (2021).
Bayer, M. et al. Fine structure of neutral and charged excitons in self-assembled In(Ga)As/(Al)GaAs quantum dots. Phys. Rev. B 65, 195315 (2002).
Zibik, E. A. et al. Long lifetimes of quantum-dot intersublevel transitions in the terahertz range. Nat. Mater. 8, 803–807 (2009).
Löbl, M. C. et al. Radiative Auger process in the single-photon limit. Nat. Nanotechnol. 15, 558–562 (2020).
Qian, C. et al. Enhanced strong interaction between nanocavities and p-shell excitons beyond the dipole approximation. Phys. Rev. Lett. 122, 087401 (2019).
Volz, T. et al. Ultrafast all-optical switching by single photons. Nat. Photonics 6, 605–609 (2012).
Kimble, H. J. The quantum internet. Nature 453, 1023–1030 (2008).
Litvinenko, K. et al. Coherent creation and destruction of orbital wavepackets in Si:P with electrical and optical read-out. Nat. Commun. 6, 6549 (2015).
Qin, Q., Williams, B. S., Kumar, S., Reno, J. L. & Hu, Q. Tuning a terahertz wire laser. Nat. Photonics 3, 732–737 (2009).
Täschler, P. et al. Femtosecond pulses from a mid-infrared quantum cascade laser. Nat. Photonics 15, 919–924 (2021).
Åberg, T. & Utriainen, J. Evidence for a ‘radiative Auger effect’ in X-ray photon emission. Phys. Rev. Lett. 22, 1346–1348 (1969).
Nash, K. J., Skolnick, M. S., Saker, M. K. & Bass, S. J. Many body shakeup in quantum well luminescence spectra. Phys. Rev. Lett. 70, 3115–3118 (1993).
Paskov, P. et al. Auger processes in InAs self-assembled quantum dots. Physica E Low Dimens. Syst. Nanostruct. 6, 440–443 (2000).
Antolinez, F. V., Rabouw, F. T., Rossinelli, A. A., Cui, J. & Norris, D. J. Observation of electron shakeup in CdSe/CdS core/shell nanoplatelets. Nano Lett. 19, 8495–8502 (2019).
Spinnler, C. et al. Optically driving the radiative Auger transition. Nat. Commun. 12, 6575 (2021).
Cygorek, M., Korkusinski, M. & Hawrylak, P. Atomistic theory of electronic and optical properties of InAsP/InP nanowire quantum dots. Phys. Rev. B 101, 075307 (2020).
Zieliński, M., Korkusiński, M. & Hawrylak, P. Atomistic tight-binding theory of multiexciton complexes in a self-assembled InAs quantum dot. Phys. Rev. B 81, 085301 (2010).
Holtkemper, M., Reiter, D. E. & Kuhn, T. Influence of the quantum dot geometry on p-shell transitions in differently charged quantum dots. Phys. Rev. B 97, 075308 (2018).
Reindl, M. et al. Highly indistinguishable single photons from incoherently excited quantum dots. Phys. Rev. B 100, 155420 (2019).
Gawarecki, K. et al. Structural symmetry-breaking to explain radiative Auger transitions in self-assembled quantum dots. Preprint at arXiv https://doi.org/10.48550/arXiv.2208.12069 (2022).
Iles-Smith, J., McCutcheon, D. P. S., Nazir, A. & Mørk, J. Phonon scattering inhibits simultaneous near-unity efficiency and indistinguishability in semiconductor single-photon sources. Nat. Photonics 11, 521–526 (2017).
Roy, C. & Hughes, S. Influence of electron–acoustic-phonon scattering on intensity power broadening in a coherently driven quantum-dot-cavity system. Phys. Rev. X 1, 021009 (2011).
Reigue, A. et al. Probing electron–phonon interaction through two-photon interference in resonantly driven semiconductor quantum dots. Phys. Rev. Lett. 118, 233602 (2017).
De Greve, K. et al. Ultrafast coherent control and suppressed nuclear feedback of a single quantum dot hole qubit. Nat. Phys. 7, 872–878 (2011).
Greilich, A., Carter, S. G., Kim, D., Bracker, A. S. & Gammon, D. Optical control of one and two hole spins in interacting quantum dots. Nat. Photonics 5, 702–708 (2011).
Godden, T. M. et al. Coherent optical control of the spin of a single hole in an InAs/GaAs quantum dot. Phys. Rev. Lett. 108, 017402 (2012).
Greve, K. D., Press, D., McMahon, P. L. & Yamamoto, Y. Ultrafast optical control of individual quantum dot spin qubits. Rep. Prog. Phys. 76, 092501 (2013).
Ramsay, A. J. et al. Damping of exciton rabi rotations by acoustic phonons in optically excited InGaAs/GaAs quantum dots. Phys. Rev. Lett. 104, 017402 (2010).
Tredicucci, A. Long life in zero dimensions. Nat. Mater. 8, 775–776 (2009).
Jin, C. Y. et al. Vertical-geometry all-optical switches based on InAs/GaAs quantum dots in a cavity. Appl. Phys. Lett. 95, 021109 (2009).
Vurgaftman, I. & Singh, J. Effect of spectral broadening and electron hole scattering on carrier relaxation in GaAs quantum dots. Appl. Phys. Lett. 64, 232–234 (1994).
Cogan, D., Su, Z.-E., Kenneth, O. & Gershoni, D. Deterministic generation of indistinguishable photons in a cluster state. Nat. Photonics 17, 324–329 (2023).
Efros, A. L., Kharchenko, V. & Rosen, M. Breaking the phonon bottleneck in nanometer quantum dots: role of Auger-like processes. Solid State Commun. 93, 281–284 (1995).
Hopfmann, C. et al. Heralded preparation of spin qubits in droplet-etched GaAs quantum dots using quasiresonant excitation. Phys. Rev. B 104, 075301 (2021).
Benisty, H., Sotomayor-Torrès, C. M. & Weisbuch, C. Intrinsic mechanism for the poor luminescence properties of quantum-box systems. Phys. Rev. B 44, 10945–10948 (1991).
Urayama, J., Norris, T. B., Singh, J. & Bhattacharya, P. Observation of phonon bottleneck in quantum dot electronic relaxation. Phys. Rev. Lett. 86, 4930–4933 (2001).
Madsen, K. H. et al. Measuring the effective phonon density of states of a quantum dot in cavity quantum electrodynamics. Phys. Rev. B 88, 045316 (2013).
Reiter, D. E., Kuhn, T. & Axt, V. M. Distinctive characteristics of carrier–phonon interactions in optically driven semiconductor quantum dots. Adv. Phys. X 4, 1655478 (2019).
Pan, D., Towe, E., Kennerly, S. & Kong, M.-Y. Tuning of conduction intersublevel absorption wavelengths in (In, Ga)As/GaAs quantum-dot nanostructures. Appl. Phys. Lett. 76, 3537–3539 (2000).
Zibik, E. A. et al. Effects of alloy intermixing on the lateral confinement potential in InAs/GaAs self-assembled quantum dots probed by intersublevel absorption spectroscopy. Appl. Phys. Lett. 90, 163107 (2007).
Monroe, C., Meekhof, D. M., King, B. E., Itano, W. M. & Wineland, D. J. Demonstration of a fundamental quantum logic gate. Phys. Rev. Lett. 75, 4714–4717 (1995).
Kaldewey, T. et al. Far-field nanoscopy on a semiconductor quantum dot via a rapid-adiabatic-passage-based switch. Nat. Photonics 12, 68–72 (2018).
Kianinia, M. et al. All-optical control and super-resolution imaging of quantum emitters in layered materials. Nat. Commun. 9, 874 (2018).
Chen, P. et al. Approaching the intrinsic exciton physics limit in two-dimensional semiconductor diodes. Nature 599, 404–410 (2021).
Chow, C. M. E. et al. Monolayer semiconductor auger detector. Nano Lett. 20, 5538–5543 (2020).
Babin, H. G. et al. Charge tunable GaAs quantum dots in a photonic n-i-p diode. Nanomaterials 11, 2703 (2021).
Zhai, L. et al. Low-noise GaAs quantum dots for quantum photonics. Nat. Commun. 11, 4745 (2020).
Babin, H.-G. et al. Full wafer property control of local droplet etched GaAs quantum dots. J. Cryst. Growth 591, 126713 (2022).
Kuhlmann, A. V. et al. A dark-field microscope for background-free detection of resonance fluorescence from single semiconductor quantum dots operating in a set-and-forget mode. Rev. Sci. Instrum. 84, 073905 (2013).
Yan, J. et al. Double-pulse generation of indistinguishable single photons with optically controlled polarization. Nano Lett. 22, 1483–1490 (2022).
Acknowledgements
We thank N. Viteritti for electrical contact preparation of the sample and D. E. Reiter for fruitful discussions. F.L., D.-W.W. and W.C. acknowledge support from the National Natural Science Foundation of China (U21A6006, 62075194, 61975177, U20A20164, 11934011, 62122067) and Fundamental Research Funds for the Central Universities (2021QNA5006). H.-G.B., A.D.W. and A.L. acknowledge support from the BMBF-QR.X Project 16KISQ009 and the DFH/UFA, Project CDFA-05-06.
Author information
Authors and Affiliations
Contributions
F.L. and J.-Y.Y. conceived the project. H.-G.B., A.D.W. and A.L. grew the wafer and fabricated the sample. Y.-T.W., H.D. and W.C. performed optical and electronic transport simulations for the sample. J.-Y.Y., C.C., X.-D.Z. and Y.M. carried out the experiments. J.-Y.Y., M.C. and F.L. analysed the data. J.-Y.Y. and D.-W.W. performed the quantum dynamics simulation. X.H., W.F., X.L., D.-W.W., C.-Y.J. and F.L. provided supervision and expertise. J.-Y.Y. and F.L. wrote the manuscript with comments and inputs from all the authors.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Nanotechnology thanks the anonymous reviewers for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Extended data
Extended Data Fig. 1 Schematic of the experimental set-up.
A single QD device is kept in a cryostat at 3.6 K and is excited under pulsed resonant excitation. A Ti-sapphire laser is used to generate 140 femtosecond optical pulses with an 80 MHz repetition rate. The femtosecond pulses are then sent into two folded pulse shapers63 to pick out two picosecond pulses with time delay controlled by delayline 1. Each pulse is divided into two arms and another controlled delay is introduced by delayline 2 and 3. Finally, the four pulses are recombined and focused on the sample by an NA=0.81 objective lens. A pair of polarizers working at a cross-polarization configuration is used to filter out the resonant excitation laser62. The experimental data shown in the main text are acquired with the pulse sequences shown in the lower right corner.
Supplementary information
Supplementary Information
Supplementary sections I–VIII and Figs. 1–14.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Yan, JY., Chen, C., Zhang, XD. et al. Coherent control of a high-orbital hole in a semiconductor quantum dot. Nat. Nanotechnol. 18, 1139–1146 (2023). https://doi.org/10.1038/s41565-023-01442-y
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41565-023-01442-y