journal article·2021-09-28Open access

Enhanced Emission from Bright Excitons in Asymmetrically Strained Colloidal CdSe/CdxZn1–xSe Quantum Dots

Igor Fedin, Mateusz Goryca, Dan Liu, Sergei Tretiak, Victor I. Klimov, Scott A. Crooker

ACS Nano· Volume 15· Issue 9

Abstract

Colloidal CdSe quantum dots (QDs) designed with a high degree of asymmetric internal strain have recently been shown to host a number of desirable optical properties including subthermal room-temperature line widths, suppressed spectral diffusion, and high photoluminescence (PL) quantum yields. It remains an open question, however, whether they are well-suited for applications requiring emission of identical single photons. Here we measure the low-temperature PL dynamics and the polarization-resolved fluorescence line narrowing spectra from ensembles of these strained QDs. Our spectroscopy reveals the radiative recombination rates of bright and dark excitons, the relaxation rate between the two, and the energy spectra of the quantized acoustic phonons in the QDs that can contribute to relaxation processes. In comparison to conventional colloidal CdSe/ZnS core/shell QDs, we find that in asymmetrically strained CdSe QDs over six times more light is emitted directly by the bright exciton. These results are therefore encouraging for the prospects of chemically synthesized colloidal QDs as emitters of single indistinguishable photons.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Quantum Dots Synthesis And Properties · Chalcogenide Semiconductor Thin Films · Gold and Silver Nanoparticles Synthesis and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Chemistry Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

Department of Chemistry and Biochemistry, University of Alabama, Tuscaloosa, Alabama 35487, United States

National High Magnetic Field Lab, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

Theory Division, Los Alamos National Laboratory, Los Alamos, New Mexico 87545, United States

Funding

Laboratory Directed Research and Development · National Science Foundation

References (62)

Show source-provided references
1. 10.1038/nnano.2017.21810.1038/nnano.2017.218 ↗
2. 10.1038/nphoton.2016.18610.1038/nphoton.2016.186 ↗
3. 10.1103/PhysRevLett.116.02040110.1103/PhysRevLett.116.020401 ↗
4. 10.1038/nphoton.2016.2310.1038/nphoton.2016.23 ↗
5. 10.1038/nphoton.2013.37710.1038/nphoton.2013.377 ↗
6. 10.1103/PhysRevLett.118.25360210.1103/PhysRevLett.118.253602 ↗
7. 10.1038/3502310010.1038/35023100 ↗
8. 10.1021/acsnano.5b0458410.1021/acsnano.5b04584 ↗
9. 10.1038/s41467-017-01379-610.1038/s41467-017-01379-6 ↗
10. 10.1126/science.aau739210.1126/science.aau7392 ↗
11. 10.1038/s41598-019-52377-110.1038/s41598-019-52377-1 ↗
12. 10.1126/sciadv.abb182110.1126/sciadv.abb1821 ↗
13. 10.1021/acsphotonics.9b0148110.1021/acsphotonics.9b01481 ↗
14. 10.1103/PhysRevLett.78.111010.1103/PhysRevLett.78.1110 ↗
15. 10.1063/1.199356710.1063/1.1993567 ↗
16. 10.1038/nature1056910.1038/nature10569 ↗
17. 10.1021/acsnano.7b0905210.1021/acsnano.7b09052 ↗
18. 10.1126/science.278.5346.211410.1126/science.278.5346.2114 ↗
19. 10.1103/PhysRevLett.77.387310.1103/PhysRevLett.77.3873 ↗
20. 10.1038/nmat222210.1038/nmat2222 ↗
21. 10.1021/ja711379k10.1021/ja711379k ↗
22. 10.1038/s41563-018-0254-710.1038/s41563-018-0254-7 ↗
23. 10.1038/nmat501110.1038/nmat5011 ↗
24. 10.1103/PhysRevLett.71.357710.1103/PhysRevLett.71.3577 ↗
25. 10.1016/0022-2313(96)00050-610.1016/0022-2313(96)00050-6 ↗
26. 10.1103/PhysRevB.77.23532110.1103/PhysRevB.77.235321 ↗
27. 10.1063/1.335087110.1063/1.3350871 ↗
28. 10.1103/PhysRevLett.108.08740110.1103/PhysRevLett.108.087401 ↗
29. 10.1021/acs.jpclett.9b0247410.1021/acs.jpclett.9b02474 ↗
30. 10.1038/nnano.2017.2210.1038/nnano.2017.22 ↗
31. 10.1021/acs.jpcc.8b1109910.1021/acs.jpcc.8b11099 ↗
32. 10.1126/science.aax348910.1126/science.aax3489 ↗
33. 10.1103/PhysRevLett.75.372810.1103/PhysRevLett.75.3728 ↗
34. 10.1063/1.157092310.1063/1.1570923 ↗
35. 10.1103/PhysRevLett.90.25740410.1103/PhysRevLett.90.257404 ↗
36. 10.1021/jp051738b10.1021/jp051738b ↗
37. 10.1103/PhysRevLett.102.17740210.1103/PhysRevLett.102.177402 ↗
38. 10.1103/PhysRevLett.103.03740410.1103/PhysRevLett.103.037404 ↗
39. 10.1021/jz302142d10.1021/jz302142d ↗
40. 10.1021/acs.nanolett.6b0266710.1021/acs.nanolett.6b02667 ↗
41. 10.1103/PhysRevB.54.484310.1103/PhysRevB.54.4843 ↗
42. 10.1103/PhysRevB.53.133610.1103/PhysRevB.53.1336 ↗
43. 10.1134/1.132403610.1134/1.1324036 ↗
44. 10.1103/PhysRevLett.94.01680310.1103/PhysRevLett.94.016803 ↗
45. 10.1021/nl071307010.1021/nl0713070 ↗
46. 10.1021/jp503823810.1021/jp5038238 ↗
47. 10.1021/acsphotonics.8b0061510.1021/acsphotonics.8b00615 ↗
48. 10.1038/ncomms128110.1038/ncomms1281 ↗
49. 10.1103/PhysRevB.74.08532010.1103/PhysRevB.74.085320 ↗
50. 10.1103/PhysRevB.53.1634710.1103/PhysRevB.53.16347 ↗
51. 10.1103/PhysRevB.54.150610.1103/PhysRevB.54.1506 ↗
52. 10.1112/plms/s1-13.1.18910.1112/plms/s1-13.1.189 ↗
53. 10.1134/1.113099710.1134/1.1130997 ↗
54. 10.1016/0022-3093(96)00164-010.1016/0022-3093(96)00164-0 ↗
55. 10.1103/PhysRevB.58.207710.1103/PhysRevB.58.2077 ↗
56. 10.1063/1.236319010.1063/1.2363190 ↗
57. 10.1103/PhysRevLett.100.05740310.1103/PhysRevLett.100.057403 ↗
58. 10.1021/acs.jpclett.6b0165910.1021/acs.jpclett.6b01659 ↗
59. 10.1103/PhysRevB.73.24131310.1103/PhysRevB.73.241313 ↗
60. 10.1103/PhysRevLett.107.17740310.1103/PhysRevLett.107.177403 ↗
61. 10.1103/PhysRevB.93.15542710.1103/PhysRevB.93.155427 ↗
62. 10.1021/nn501026t10.1021/nn501026t ↗