journal article·2023-02-14Open access

Measuring the Ultrafast Spectral Diffusion and Vibronic Coupling Dynamics in CdSe Colloidal Quantum Wells using Two-Dimensional Electronic Spectroscopy

Hoang Long Nguyen, Thanh Nhut Do, Emek G. Durmusoglu, Merve Izmir, Ritabrata Sarkar, Sougata Pal, Oleg V. Prezhdo, Hilmi Volkan Demir, Howe-Siang Tan

ACS Nano· Volume 17· Issue 3

Abstract

We measure the ultrafast spectral diffusion, vibronic dynamics, and energy relaxation of a CdSe colloidal quantum wells (CQWs) system at room temperature using two-dimensional electronic spectroscopy (2DES). The energy relaxation of light-hole (LH) excitons and hot carriers to heavy-hole (HH) excitons is resolved with a time scale of ∼210 fs. We observe the equilibration dynamics between the spectroscopically accessible HH excitonic state and a dark state with a time scale of ∼160 fs. We use the center line slope analysis to quantify the spectral diffusion dynamics in HH excitons, which contains an apparent sub-200 fs decay together with oscillatory features resolved at 4 and 25 meV. These observations can be explained by the coupling to various lattice phonon modes. We further perform quantum calculations that can replicate and explain the observed dynamics. The 4 meV mode is observed to be in the near-critically damped regime and may be mediating the transition between the bright and dark HH excitons. These findings show that 2DES can provide a comprehensive and detailed characterization of the ultrafast spectral properties in CQWs and similar nanomaterials.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Spectroscopy and Quantum Chemical Studies · Quantum Dots Synthesis And Properties · Electrochemical Analysis and Applications

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

Affiliations

School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 21 Nanyang Link, Singapore637371, Singapore

University of Groningen, Zernike Institute for Advanced Materials, Nijenborgh 4, 9747 AGGroningen, The Netherlands

LUMINOUS! Centre of Excellence for Semiconductor Lighting and Displays, The Photonics Institute, School of Electrical and Electronic Engineering, Nanyang Technological University, Singapore639798, Singapore

Division of Physics and Applied Physics, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore637371, Singapore

School of Materials Science and Engineering, Nanyang Technological University, Singapore639798, Singapore

Department of Chemistry, University of Gour Banga, Malda732103, India

Bremen Center for Computational Materials Science, University of Bremen, Bremen28359, Germany

Department of Chemistry, University of Southern California, Los Angeles, California90089, United States

Department of Electrical and Electronics Engineering, Department of Physics, UNAM─Institute of Materials Science and Nanotechnology, Bilkent University, Ankara06800, Turkey

Funding

Division of Chemistry · Agency for Science, Technology and Research · Ministry of Education - Singapore · T?rkiye Bilimler Akademisi

References (77)

Show source-provided references
1. 10.1002/inf2.1210610.1002/inf2.12106 ↗
2. 10.1021/acsnano.5b0250910.1021/acsnano.5b02509 ↗
3. 10.1021/acs.jpcc.0c0941610.1021/acs.jpcc.0c09416 ↗
4. 10.1021/ja807724e10.1021/ja807724e ↗
5. 10.1038/nmat314510.1038/nmat3145 ↗
6. Davies J. H. · 1998
7. 10.1103/PhysRevB.102.19540510.1103/PhysRevB.102.195405 ↗
8. 10.1021/acs.jpcc.5b0927510.1021/acs.jpcc.5b09275 ↗
9. 10.1021/acs.jpcc.9b0463910.1021/acs.jpcc.9b04639 ↗
10. 10.1021/acs.jpcc.8b0773310.1021/acs.jpcc.8b07733 ↗
11. 10.1038/ncomms708610.1038/ncomms7086 ↗
12. 10.1103/PhysRevB.54.484310.1103/PhysRevB.54.4843 ↗
13. 10.1039/C7NR07206F10.1039/C7NR07206F ↗
14. 10.1021/nl403311n10.1021/nl403311n ↗
15. 10.1021/nl503406a10.1021/nl503406a ↗
16. 10.1021/acsnano.5b0192710.1021/acsnano.5b01927 ↗
17. 10.1021/acsnano.9b0496710.1021/acsnano.9b04967 ↗
18. 10.1021/acs.chemmater.9b0013610.1021/acs.chemmater.9b00136 ↗
19. 10.1021/acs.jpcc.7b1262910.1021/acs.jpcc.7b12629 ↗
20. 10.1021/acs.jpclett.5b0027910.1021/acs.jpclett.5b00279 ↗
21. 10.1038/ncomms743410.1038/ncomms7434 ↗
22. 10.1039/C7CC04503D10.1039/C7CC04503D ↗
23. 10.1021/nl403746p10.1021/nl403746p ↗
24. 10.1021/nl401538n10.1021/nl401538n ↗
25. 10.1002/adfm.20130171110.1002/adfm.201301711 ↗
26. 10.1021/acs.nanolett.5b0123310.1021/acs.nanolett.5b01233 ↗
27. 10.1021/nn502229610.1021/nn5022296 ↗
28. Hamm P. · 201110.1017/CBO9780511675935 ↗
29. 10.1103/PhysRevB.74.23532810.1103/PhysRevB.74.235328 ↗
30. 10.1146/annurev.physchem.58.032806.10453710.1146/annurev.physchem.58.032806.104537 ↗
31. 10.1103/PhysRevLett.102.12740410.1103/PhysRevLett.102.127404 ↗
32. 10.1021/jp205867310.1021/jp2058673 ↗
33. 10.1016/j.chemphys.2016.08.02710.1016/j.chemphys.2016.08.027 ↗
34. 10.1557/adv.2019.3810.1557/adv.2019.38 ↗
35. 10.1073/pnas.191679211710.1073/pnas.1916792117 ↗
36. 10.1063/1.486583210.1063/1.4865832 ↗
37. 10.1021/acs.nanolett.8b0047010.1021/acs.nanolett.8b00470 ↗
38. 10.1021/acs.nanolett.7b0139410.1021/acs.nanolett.7b01394 ↗
39. 10.1021/acsnano.6b0421010.1021/acsnano.6b04210 ↗
40. 10.1039/C6CP08689F10.1039/C6CP08689F ↗
41. 10.1021/acs.jpcb.9b0542110.1021/acs.jpcb.9b05421 ↗
42. 10.1063/1.496257710.1063/1.4962577 ↗
43. 10.1021/acs.jpclett.2c0019410.1021/acs.jpclett.2c00194 ↗
44. 10.1016/j.trechm.2021.05.00810.1016/j.trechm.2021.05.008 ↗
45. 10.1021/acs.jpcb.0c1063410.1021/acs.jpcb.0c10634 ↗
46. 10.1021/ar900107510.1021/ar9001075 ↗
47. Mukamel S. · 1995
48. 10.1021/acs.jpclett.0c0324310.1021/acs.jpclett.0c03243 ↗
49. 10.1063/1.277226910.1063/1.2772269 ↗
50. 10.1021/acs.jpca.5b0890910.1021/acs.jpca.5b08909 ↗
51. 10.1016/j.cocis.2007.07.01210.1016/j.cocis.2007.07.012 ↗
52. 10.1073/pnas.070616410410.1073/pnas.0706164104 ↗
53. 10.1021/acs.nanolett.6b0005310.1021/acs.nanolett.6b00053 ↗
54. 10.1021/acs.jpcc.1c0378410.1021/acs.jpcc.1c03784 ↗
55. 10.1063/1.223227110.1063/1.2232271 ↗
56. 10.1103/PhysRevB.91.12130210.1103/PhysRevB.91.121302 ↗
57. 10.1021/acs.jpclett.5b0014310.1021/acs.jpclett.5b00143 ↗
58. 10.1021/nl302986y10.1021/nl302986y ↗
59. 10.1021/nl504706w10.1021/nl504706w ↗
60. 10.1146/annurev.physchem.040808.09025910.1146/annurev.physchem.040808.090259 ↗
61. 10.1002/asia.20190099410.1002/asia.201900994 ↗
62. 10.1063/5.005552810.1063/5.0055528 ↗
63. 10.1063/1.473784310.1063/1.4737843 ↗
64. 10.1021/acs.nanolett.6b0536810.1021/acs.nanolett.6b05368 ↗
65. 10.1103/PhysRevB.63.08510810.1103/PhysRevB.63.085108 ↗
66. 10.1103/PhysRevB.51.1294710.1103/PhysRevB.51.12947 ↗
67. 10.1103/PhysRevLett.70.101410.1103/PhysRevLett.70.1014 ↗
68. 10.1021/nn201475d10.1021/nn201475d ↗
69. 10.1021/jp803386g10.1021/jp803386g ↗
70. 10.1103/PhysRevB.96.18430610.1103/PhysRevB.96.184306 ↗
71. 10.1021/acs.jpcc.0c1052910.1021/acs.jpcc.0c10529 ↗
72. 10.1021/nn301485510.1021/nn3014855 ↗
73. 10.1103/PhysRevLett.102.17740210.1103/PhysRevLett.102.177402 ↗
74. 10.1063/1.11660910.1063/1.116609 ↗
75. 10.1007/s00340-004-1650-z10.1007/s00340-004-1650-z ↗
76. 10.1364/JOSAB.27.00061910.1364/JOSAB.27.000619 ↗
77. 10.1016/j.cplett.2012.08.03710.1016/j.cplett.2012.08.037 ↗