Abstract
Designing colloidal assemblies with molecule-like architectures comprising more than two electronically coupled quantum dots has often required technologically complex, expensive, and top-down nanofabrication. Here we demonstrate a one-pot chemical synthesis of dimeric, trimeric, and tetrameric assemblies of coupled molecule-like quantum dots (CMQDs), using ZnSe@ZnS quantum dots as model. We show that the “valence” of these “artificial atoms” can be readily tuned by the amount of a suitable ligand in the reaction mixture, and that high-temperature fusion yields highly ordered oriented attachment and strong electron coupling between bound QDs. The shapes of the fused assemblies echo the canonical sp-, sp²-, and sp³-hybridization motifs and can be interpreted as appropriately shaped confining potential wells for electrons and holes. This work establishes an experimentally accessible entry point to related “artificial molecules” with controllable chemical composition, geometry, and electronic structure. The enhanced or emergent properties of such nanomaterials are anticipated to advance applications in optoelectronics, sensing, and quantum photonic technologies.
Similar content being viewed by others
Data availability
The data that support the findings of this study are available from the corresponding authors upon request. Source data are provided with this paper.
References
Mao, Y. et al. Orbital hybridization in graphene-based artificial atoms. Nature 639, 73–78 (2025).
Kagan, C. R., Lifshitz, E., Sargent, E. H. & Talapin, D. V. Building devices from colloidal quantum dots. Science 353, 6302 (2016).
Kouwenhoven, L. Coupled quantum dots as artificial molecules. Science 268, 1440–1441 (1995).
Alivisatos, A. P. Semiconductor clusters, nanocrystals, and quantum dots. Science 271, 933–937 (1996).
Huang, H. M., Alkhazragi, O., Liang, D. & Grillot, F. Future roles of solid-state quantum dot light sources. Appl. Phys. Lett. 126, 080501 (2025).
Yuan, Z. L. et al. Electrically driven single-photon source. Science 295, 102–105 (2002).
Salter, C. L. et al. An entangled-light-emitting diode. Nature 465, 594–597 (2010).
Zhu, C. et al. Supramolecular assembly of halide perovskite building blocks. J. Am. Chem. Soc. 144, 12450–12458 (2022).
Tang, Z. Y., Kotov, N. A. & Giersig, M. Spontaneous organization of single CdTe nanoparticles into luminescent nanowires. Science 297, 237–240 (2002).
Schliehe, C. et al. Ultrathin PbS sheets by two-dimensional oriented attachment. Science 329, 550–553 (2010).
Rainò, G. et al. Superfluorescence from lead halide perovskite quantum dot superlattices. Nature 563, 671 (2018).
Yi, C. L. et al. Self-limiting directional nanoparticle bonding governed by reaction stoichiometry. Science 369, 1369 (2020).
Fang, H. et al. Dynamic and asymmetric colloidal molecules. Nat. Commun. 16, 2819 (2025).
Han, M. Y., Gao, X. H., Su, J. Z. & Nie, S. Quantum-dot-tagged microbeads for multiplexed optical coding of biomolecules. Nat. Biotechnol. 19, 631–635 (2001).
Teitelboim, A., Meir, N., Kazes, M. & Oron, D. Colloidal double quantum dots. Acc. Chem. Res. 49, 902–910 (2016).
Banin, U., Cao, Y. W., Katz, D. & Millo, O. Identification of atomic-like electronic states in indium arsenide nanocrystal quantum dots. Nature 400, 542–544 (1999).
Mirkin, C. A., Letsinger, R. L., Mucic, R. C. & Storhoff, J. J. A DNA-based method for rationally assembling nanoparticles into macroscopic materials. Nature 382, 607–609 (1996).
Alivisatos, A. P. et al. Organization of ‘nanocrystal molecules’ using DNA. Nature 382, 609–611 (1996).
Tan, S. J., Campolongo, M. J., Luo, D. & Cheng, W. Building plasmonic nanostructures with DNA. Nat. Nanotechnol. 6, 268–276 (2011).
Schedelbeck, G., Wegscheider, W., Bichler, M. & Abstreiter, G. Coupled quantum dots fabricated by cleaved edge overgrowth: from artificial atoms to molecules. Science 278, 1792–1795 (1997).
Cui, J. et al. Colloidal quantum dot molecules manifesting quantum coupling at room temperature. Nat. Commun. 10, 5401 (2019).
Lienhart, M. et al. Resonant and antiresonant exciton-phonon coupling in quantum dot molecules. Phys. Rev. B 112, 235305 (2025).
Stinaff, E. A. et al. Optical signatures of coupled quantum dots. Science 311, 636–639 (2006).
Bayer, M. et al. Coupling and entangling of quantum states in quantum dot molecules. Science 291, 451–453 (2001).
Ji, B. T. et al. Strain-controlled shell morphology on quantum rods. Nat. Commun. 10, 2 (2019).
Jing, L. H. et al. Aqueous based semiconductor nanocrystals. Chem. Rev. 116, 10623–10730 (2016).
Lee, J., Yang, J., Kwon, S. G. & Hyeon, T. Nonclassical nucleation and growth of inorganic nanoparticles. Nat. Rev. Mater. 1, 16034 (2016).
Mourdikoudis, S. et al. Oleic acid/oleylamine ligand pair: a versatile combination in the synthesis of colloidal nanoparticles. Nanoscale Horiz. 7, 941–1015 (2022).
Cui, J. et al. Neck barrier engineering in quantum dot dimer molecules via intraparticle ripening. J. Am. Chem. Soc. 143, 19816–19823 (2021).
Murray, C. B., Norris, D. J. & Bawendi, M. G. Synthesis and characterization of nearly monodisperse CdE (E = sulfur, selenium, tellurium) semiconductor nanocrystallites. J. Am. Chem. Soc. 115, 8706–8715 (1993).
Battaglia, D., Blackman, B. & Peng, X. Coupled and decoupled dual quantum systems in one semiconductor nanocrystal. J. Am. Chem. Soc. 127, 10889–10897 (2005).
Chen, O. et al. Compact high-quality CdSe-CdS core-shell nanocrystals with narrow emission linewidths and suppressed blinking. Nat. Mater. 12, 445–451 (2013).
Fan, F. et al. Continuous-wave lasing in colloidal quantum dot solids enabled by facet-selective epitaxy. Nature 544, 75 (2017).
Oh, N. et al. Double-heterojunction nanorod light-responsive LEDs for display applications. Science 355, 616–619 (2017).
Cui, J. et al. Semiconductor bow-tie nanoantenna from coupled colloidal quantum dot molecules. Angew. Chem. Int. Ed. 60, 14467–14472 (2021).
Penn, R. L. & Banfield, J. F. Imperfect oriented attachment: dislocation generation in defect-free nanocrystals. Science 281, 969–971 (1998).
Ondry, J. C., Hauwiller, M. R. & Alivisatos, A. P. Dynamics and removal pathway of edge dislocations in imperfectly attached PbTe nanocrystal pairs: toward design rules for oriented attachment. ACS Nano 12, 3178–3189 (2018).
Koley, S., Cui, J., Panfil, Y. E. & Banin, U. Coupled colloidal quantum dot molecules. Acc. Chem. Res. 54, 1178–1188 (2021).
Ashoori, R. C. Electrons in artificial atoms. Nature 379, 413–419 (1996).
Ouyang, M. & Awschalom, D. D. Coherent spin transfer between molecularly bridged quantum dots. Science 301, 1074–1078 (2003).
Petta, J. R. et al. Coherent manipulation of coupled electron spins in semiconductor quantum dots. Science 309, 2180–2184 (2005).
Coropceanu, I. et al. Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals. Science 375, 1422–1426 (2022).
Ossia, Y. et al. Electric-field-induced colour switching in colloidal quantum dot molecules at room temperature. Nat. Mater. 22, 1210–1217 (2023).
Galland, C. et al. Two types of luminescence blinking revealed by spectroelectrochemistry of single quantum dots. Nature 479, 203 (2011).
Yang, C. et al. Mechanisms and suppression of quantum dot blinking. Laser Photonics Rev. 19, 9 (2025).
Nair, G., Zhao, J. & Bawendi, M. G. Biexciton quantum yield of single semiconductor nanocrystals from photon statistics. Nano Lett. 11, 1136–1140 (2011).
Frenkel, N. et al. Two biexciton types coexisting in coupled quantum dot molecules. ACS Nano 17, 14990–15000 (2023).
Park, Y. S., Bae, W. K., Pietryga, J. M. & Klimov, V. I. Auger recombination of biexcitons and negative and positive trions in individual quantum dots. ACS Nano 8, 7288–7296 (2014).
Makarov, N. S. et al. Spectral and dynamical properties of single excitons, biexcitons, and trions in cesium-lead-halide perovskite quantum dots. Nano Lett. 16, 2349–2362 (2016).
Lin, X. et al. Blue lasers using low-toxicity colloidal quantum dots. Nat. Nanotechnol. 20, 229–236 (2025).
Martins, J. R. et al. Statistical analysis of photoluminescence decay kinetics in quantum dot ensembles: effects of inorganic shell composition and environment. J. Phys. Chem. C. 126, 20480–20490 (2022).
Chen, Q. S. et al. All-inorganic perovskite nanocrystal scintillators. Nature 561, 88–93 (2018).
Sun, M. Z. et al. Site-selective photoinduced cleavage and profiling of DNA by chiral semiconductor nanoparticles. Nat. Chem. 10, 821–830 (2018).
Hou, X., Qin, H. & Peng, X. Enhancing dielectric screening for auger suppression in CdSe/CdS quantum dots by epitaxial growth of ZnS shell. Nano Lett. 21, 3871–3878 (2021).
Bertoni, G. et al. Direct determination of polarity, faceting, and core location in colloidal core/shell wurtzite semiconductor nanocrystals. ACS Nano 6, 6453–6461 (2012).
Cho, K.-S., Talapin, D. V., Gaschler, W. & Murray, C. B. Designing PbSe nanowires and nanorings through oriented attachment of nanoparticles. J. Am. Chem. Soc. 127, 7140–7147 (2005).
Deutsch, Z., Neeman, L. & Oron, D. Luminescence upconversion in colloidal double quantum dots. Nat. Nanotechnol. 8, 649 (2013).
Wang, T. et al. Self-assembled colloidal superparticles from nanorods. Science 338, 358–363 (2012).
Yang, X. L. et al. Temperature- and Mn2+ concentration-dependent emission properties of Mn2+-doped ZnSe nanocrystals. J. Am. Chem. Soc. 141, 2288–2298 (2019).
Yeom, J. et al. Chiral templating of self-assembling nanostructures by circularly polarized light. Nat. Mater. 14, 66 (2014).
Lv, B. et al. Photon antibunching in a cluster of giant CdSe/CdS nanocrystals. Nat. Commun. 9, 1536 (2018).
Acknowledgements
This work was supported by the National Natural Science Foundation of China (No. 82130059, 22104105, 62127817, U23A20380, 62575162, 22574118), Jiangsu Provincial Department of Science and Technology leading technology basic research major project (No. BK20232041), Science and Technology Project of Jiangsu Province (No. BZ2025036), and the Leading Talents of Innovation and Entrepreneurship of Gusu (No. ZXL2022515), Shanxi Province Science and Technology Innovation Talent Team (No. 202204051001014). We are grateful to Oleksandr Ivasenko for assistance with language and grammar in the manuscript.
Author information
Authors and Affiliations
Contributions
J.B.C. and M.Y.G. contributed to the conception and design of the work. G.F.Z., J.B.C. and M.Y.G. supervised the project and led the collaboration efforts. J.D.F., C.H.Y. and H.R.J. performed the quantum dots synthesis and spectral measurements. J.C.M. contributed to the design and implementation of the X-ray imaging experiments. Z.Y., L.T.X., G.F.Z. carried out the single-particle photoluminescence spectroscopy test. J.L.X. and H.C. contributed to data curation. Q.L.M., M.C., J.L. and X.Y.W. contributed to the additional experiments. X.Y.W. and J.L. contributed validation. J.D.F., J.C.M. and J.B.C. contributed writing and original draft preparation. Y.G.P. contributed the theoretical calculation of the wave functions and energy levels of the molecules. G.F.Z., J.B.C., and M.Y.G. contributed review and editing. All authors discussed the results and commented on the manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Communications thanks the anonymous reviewers for their contribution to the peer review of this work. A peer review file is available.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Source data
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.
About this article
Cite this article
Fan, J., Ying, Z., Ma, J. et al. Template-free synthesis of colloidal quantum dot assemblies with molecule-like architectures. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70555-4
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41467-026-70555-4
