Unity quantum yield of photogenerated charges and band-like transport in quantum-dot solids
Source abstract
Abstract
Solid films of colloidal quantum dots show promise in the manufacture of photodetectors and solar cells. These devices require high yields of photogenerated charges and high carrier mobilities, which are difficult to achieve in quantum-dot films owing to a strong electron-hole interaction and quantum confinement. Here, we show that the quantum yield of photogenerated charges in strongly coupled PbSe quantum-dot films is unity over a large temperature range. At high photoexcitation density, a transition takes place from hopping between localized states to band-like transport. These strongly coupled quantum-dot films have electrical properties that approach those of crystalline bulk semiconductors, while retaining the size tunability and cheap processing properties of colloidal quantum dots.
Source: europepmc · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films · Advanced Photocatalysis Techniques
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (49)
Show source-provided references
1. Talapin, D. V. & Murray, C. B. PbSe nanocrystal solids for n- and p-channel thin film field-effect transistors. Science 310, 86–89 (2005).10.1126/science.1116703 ↗
2. Hansen, J. A. et al. Quantum-dot/aptamer-based ultrasensitive multi-analyte electrochemical biosensor. J. Am. Chem. Soc. 128, 2228–2229 (2006).10.1021/ja060005h ↗
3. Konstantatos, G. et al. Ultrasensitive solution-cast quantum dot photodetectors. Nature 442, 180–183 (2006).10.1038/nature04855 ↗
4. Coe, S., Woo, W. K., Bawendi, M. & Bulovic, V. Electroluminescence from single monolayers of nanocrystals in molecular organic devices. Nature 420, 800–803 (2002).10.1038/nature01217 ↗
5. Klimov, V. I. et al. Optical gain and stimulated emission in nanocrystal quantum dots. Science 290, 314–317 (2000).10.1126/science.290.5490.314 ↗
6. Leschkies, K. S., Beatty, T. J., Kang, M. S., Norris, D. J. & Aydil, E. S. Solar cells based on junctions between colloidal PbSe nanocrystals and thin ZnO films. ACS Nano 3, 3638–3648 (2009).10.1021/nn901139d ↗
7. Choi, J. J. et al. PbSe nanocrystal excitonic solar cells. Nano Lett. 9, 3749–3755 (2009).10.1021/nl901930g ↗
8. Gur, I., Fromer, N. A., Geier, M. L. & Alivisatos, A. P. Air-stable all-inorganic nanocrystal solar cells processed from solution. Science 310, 462–465 (2005).10.1126/science.1117908 ↗
9. Luther, J. M. et al. Schottky solar cells based on colloidal nanocrystal films. Nano Lett. 8, 3488–3492 (2008).10.1021/nl802476m ↗
10. Ma, W., Luther, J. M., Zheng, H. M., Wu, Y. & Alivisatos, A. P. Photovoltaic devices employing ternary PbSxSe1–x nanocrystals. Nano Lett. 9, 1699–1703 (2009).10.1021/nl900388a ↗
11. Pattantyus-Abraham, A. G. et al. Depleted-heterojunction colloidal quantum dot solar cells. ACS Nano 4, 3374–3380 (2010).10.1021/nn100335g ↗
12. Ginger, D. S. & Greenham, N. C. Charge injection and transport in films of CdSe nanocrystals. J. Appl. Phys. 87, 1361–1368 (2000).10.1063/1.372021 ↗
13. Yu, D., Wang, C. J. & Guyot-Sionnest, P. n-Type conducting CdSe nanocrystal solids. Science 300, 1277–1280 (2003).10.1126/science.1084424 ↗
14. Lee, J-S., Kovalenko, M. V., Huang, J., Chung, D. S. & Talapin, D. V. Band-like transport, high electron mobility and high photoconductivity in all-inorganic nanocrystal arrays. Nature Nanotech. 6, 348–352 (2011).10.1038/nnano.2011.46 ↗
15. Tang, J. A. & Sargent, E. H. Infrared colloidal quantum dots for photovoltaics: fundamentals and recent progress. Adv. Mater. 23, 12–29 (2011).10.1002/adma.201001491 ↗
16. Jarosz, M. V., Porter, V. J., Fisher, B. R., Kastner, M. A. & Bawendi, M. G. Photoconductivity studies of treated CdSe quantum dot films exhibiting increased exciton ionization efficiency. Phys. Rev. B 70, 195327 (2004).10.1103/PhysRevB.70.195327 ↗
17. Loef, R., Houtepen, A. J., Talgorn, E., Schoonman, J. & Goossens, A. Study of electronic defects in CdSe quantum dots and their involvement in quantum dot solar cells. Nano Lett. 9, 856–859 (2009).10.1021/nl803738q ↗
18. Sambur, J. B., Novet, T. & Parkinson, B. A. Multiple exciton collection in a sensitized photovoltaic system. Science 330, 63–66 (2010).10.1126/science.1191462 ↗
19. Trinh, M. T. et al. In spite of recent doubts carrier multiplication does occur in PbSe nanocrystals. Nano Lett. 8, 1713–1718 (2008).10.1021/nl0807225 ↗
20. Trinh, M. T. et al. Anomalous independence of multiple exciton generation on different group IV–VI quantum dot architectures. Nano Lett. 11, 1623–1629 (2011).10.1021/nl200014g ↗
21. Luther, J. M. et al. Structural, optical and electrical properties of self-assembled films of PbSe nanocrystals treated with 1,2-ethanedithiol. ACS Nano 2, 271–280 (2008).10.1021/nn7003348 ↗
22. Wolcott, A. et al. Anomalously large polarization effect responsible for excitonic red shifts in PbSe quantum dot solids. J. Phys. Chem. Lett. 2, 795–800 (2011).10.1021/jz200080d ↗
23. Dollefeld, H., Weller, H. & Eychmuller, A. Particle–particle interactions in semiconductor nanocrystal assemblies. Nano Lett. 1, 267–269 (2001).10.1021/nl015524r ↗
24. Artemyev, M. V., Woggon, U., Jaschinski, H., Gurinovich, L. I. & Gaponenko, S. V. Spectroscopic study of electronic states in an ensemble of close-packed CdSe nanocrystals. J. Phys. Chem. B 104, 11617–11621 (2000).10.1021/jp002085w ↗
25. Moreels, L. et al. Composition and size-dependent extinction coefficient of colloidal PbSe quantum dots. Chem. Mater. 19, 6101–6106 (2007).10.1021/cm071410q ↗
26. Talgorn, E. et al. Highly photoconductive CdSe quantum-dot films: influence of capping molecules and film preparation procedure. J. Phys. Chem. C 114, 3441–3447 (2010).10.1021/jp9109546 ↗
27. Talgorn, E. et al. Supercrystals of CdSe quantum dots with high charge mobility and efficient electron transfer to TiO2 . ACS Nano 4, 1723–1731 (2010).10.1021/nn901709a ↗
28. Trinh, M. T., Houtepen, A. J., Schins, J. M., Piris, J. & Siebbeles, L. D. A. Nature of the second optical transition in PbSe nanocrystals. Nano Lett. 8, 2112–2117 (2008).10.1021/nl8010963 ↗
29. Dakovski, G. L., Lan, S., Xia, C. & Shan, J. Terahertz electric polarizability of excitons in PbSe and CdSe quantum dots. J. Phys. Chem. C 111, 5904–5908 (2007).10.1021/jp069026o ↗
30. Murphy, J. E., Beard, M. C. & Nozik, A. J. Time-resolved photoconductivity of PbSe nanocrystal arrays. J. Phys. Chem. B 110, 25455–25461 (2006).10.1021/jp0646123 ↗
31. Schins, J. M. Thin-sample limit for time-resolved terahertz spectroscopy. Appl. Phys. Lett. 97, 1772110–1772112 (2010).10.1063/1.3505340 ↗
32. Savenije, T. J., de Haas, M. P. & Warman, J. M. The yield and mobility of charge carriers in smooth and nanoporous TiO2 films. Z. Phys. Chem. 212, 201–206 (1999).10.1524/zpch.1999.212.Part_2.201 ↗
33. Liu, Y. et al. Dependence of carrier mobility on nanocrystal size and ligand length in PbSe nanocrystal solids. Nano Lett. 10, 1960–1969 (2010).10.1021/nl101284k ↗
34. Romero, H. E. & Drndic, M. Coulomb blockade and hopping conduction in PbSe quantum dots. Phys. Rev. Lett. 95, 156801 (2005).10.1103/PhysRevLett.95.156801 ↗
35. Yu, D., Wang, C. J., Wehrenberg, B. L. & Guyot-Sionnest, P. Variable range hopping conduction in semiconductor nanocrystal solids. Phys. Rev. Lett. 92, 216802 (2004).10.1103/PhysRevLett.92.216802 ↗
36. Houtepen, A. J., Kockmann, D. & Vanmaekelbergh, D. Reappraisal of variable-range hopping in quantum-dot solids. Nano Lett. 8, 3516–3520 (2008).10.1021/nl8020347 ↗
37. Roest, A. L., Houtepen, A. J., Kelly, J. J. & Vanmaekelbergh, D. Electron-conducting quantum-dot solids with ionic charge compensation. Faraday Discuss. 125, 55–62 (2004).10.1039/b302839a ↗
38. Mentzel, T. S. et al. Charge transport in PbSe nanocrystal arrays. Phys. Rev. B 77, 075316 (2008).10.1103/PhysRevB.77.075316 ↗
39. Chandler, R. E., Houtepen, A. J., Nelson, J. & Vanmaekelbergh, D. Electron transport in quantum dot solids: Monte Carlo simulations of the effects of shell filling, Coulomb repulsions, and site disorder. Phys. Rev. B 75, 085325 (2007).10.1103/PhysRevB.75.085325 ↗
40. Braun, C. L. Electric-field assisted dissociation of charge-transfer states as a mechanism of photocarrier generation. J. Chem. Phys. 80, 4157–4161 (1984).10.1063/1.447243 ↗
41. Bruggeman, D. A. G. Calculation of various physics constants in heterogenous substances. Dielectricity constants and conductivity of mixed bodies from isotropic substances. Ann. Phys. 24, 636–664 (1935).10.1002/andp.19354160705 ↗
42. Brus, L. E. Electron–electron and electron–hole interactions in small semiconductor crystallites: the size dependence of the lowest excited electronic state. J. Chem. Phys. 80, 4403–4409 (1984).10.1063/1.447218 ↗
43. Delerue, C. & Lannoo, M. Nanostructures: Theory and Modelling (Springer-Verlag, 2004).10.1007/978-3-662-08903-3 ↗
44. Wehrenberg, B. L., Wang, C. J. & Guyot-Sionnest, P. Interband and intraband optical studies of PbSe colloidal quantum dots. J. Phys. Chem. B 106, 10634–10640 (2002).10.1021/jp021187e ↗
45. Anderson, P. W. Absence of diffusion in certain random lattices. Phys. Rev. 109, 1492–1505 (1958).10.1103/PhysRev.109.1492 ↗
46. Smith, B. B. & Nozik, A. J. Theoretical studies of electronic state localization and wormholes in silicon quantum dot arrays. Nano Lett. 1, 36–41 (2000).10.1021/nl0001858 ↗
47. Pepper, M., Pollitt, S., Adkins, C. J. & Stradling, R. A. Anderson localization in silicon inversion layers. Crit. Rev. Solid State 5, 375–384 (1975).10.1080/10408437508243498 ↗
48. Kovalenko, M. V. et al. Quasi-seeded growth of ligand-tailored PbSe nanocrystals through cation-exchange-mediated nucleation. Angew. Chem. Int. Ed. 47, 3029–3033 (2008).10.1002/anie.200705604 ↗
49. Han, Y., Mayer, D., Offenhausser, A. & Ingebrandt, S. Surface activation of thin silicon oxides by wet cleaning and silanization. Thin Solid Films 510, 175–180 (2006).10.1016/j.tsf.2005.11.048 ↗