journal article·2020-04-28Open access

Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy

Burak Guzelturk, James K. Utterback, Igor Coropceanu, Vladislav Kamysbayev, Eric M. Janke, Marc Zajac, Nuri Yazdani, Benjamin L. Cotts, Suji Park, Aditya Sood, Ming-Fu Lin, Alexander H. Reid, Michael E. Kozina, Xiaozhe Shen, Stephen P. Weathersby, Vanessa Wood, Alberto Salleo, Xijie Wang, Dmitri V. Talapin, Naomi S. Ginsberg, Aaron M. Lindenberg

ACS Nano· Volume 14· Issue 4

Abstract

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. Here, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron–phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron–phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.
Source: openalex_inverted_index · Quality: baseline

Research context

OpenAlex topics: Gold and Silver Nanoparticles Synthesis and Applications · nanoparticles nucleation surface interactions · Quantum Dots Synthesis And Properties

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

Affiliations

Department of Materials Science and Engineering, Stanford University, Stanford, California 94305, United States

Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, California 94025 United States

Department of Chemistry, University of California, Berkeley, California 94720, United States

Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, United States

Department of Information Technology and Electrical Engineering, ETH Zurich, 8092 Zurich, Switzerland

SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Department of Physics, University of California, Berkeley, California 94720, United States

Molecular Biophysics and Integrated Bioimaging Division and Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Kavli Energy NanoSciences Institute, Berkeley, California 94720, United States

The PULSE Institute for Ultrafast Energy Science, SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Department of Photon Science, Stanford University and SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States

Funding

Schweizerischer Nationalfonds zur F?rderung der Wissenschaftlichen Forschung · Basic Energy Sciences · Alfred P. Sloan Foundation · Camille and Henry Dreyfus Foundation · David and Lucile Packard Foundation · Division of Materials Research

References (77)

Show source-provided references
1. 10.1021/cr200061k10.1021/cr200061k ↗
2. 10.1002/lpor.20081000310.1002/lpor.200810003 ↗
3. 10.1021/jp984796o10.1021/jp984796o ↗
4. 10.1021/cr900137k10.1021/cr900137k ↗
5. 10.1146/annurev.matsci.30.1.54510.1146/annurev.matsci.30.1.545 ↗
6. 10.1038/nmat315110.1038/nmat3151 ↗
7. 10.1021/nl303940z10.1021/nl303940z ↗
8. 10.1038/ncomms1076610.1038/ncomms10766 ↗
9. 10.1039/C1CS15237H10.1039/C1CS15237H ↗
10. 10.1007/s10103-007-0470-x10.1007/s10103-007-0470-x ↗
11. 10.1038/nnano.2014.31110.1038/nnano.2014.311 ↗
12. 10.1146/annurev-physchem-042018-05263910.1146/annurev-physchem-042018-052639 ↗
13. 10.1021/cr100254710.1021/cr1002547 ↗
14. 10.1016/j.nantod.2019.05.00610.1016/j.nantod.2019.05.006 ↗
15. 10.1021/jp962923f10.1021/jp962923f ↗
16. 10.1063/1.48116710.1063/1.481167 ↗
17. 10.1103/PhysRevLett.90.17740110.1103/PhysRevLett.90.177401 ↗
18. 10.1016/j.chemphys.2005.06.04010.1016/j.chemphys.2005.06.040 ↗
19. 10.1073/pnas.122232711010.1073/pnas.1222327110 ↗
20. 10.1021/acsenergylett.7b0033310.1021/acsenergylett.7b00333 ↗
21. 10.1021/acs.nanolett.9b0050310.1021/acs.nanolett.9b00503 ↗
22. 10.1021/acsphotonics.6b0021710.1021/acsphotonics.6b00217 ↗
23. 10.1103/PhysRevB.66.22430110.1103/PhysRevB.66.224301 ↗
24. 10.1103/PhysRevB.80.19540610.1103/PhysRevB.80.195406 ↗
25. 10.1021/jp308130d10.1021/jp308130d ↗
26. 10.1021/acsnano.5b0662310.1021/acsnano.5b06623 ↗
27. 10.1021/acsami.5b1216310.1021/acsami.5b12163 ↗
28. 10.1021/jp027597k10.1021/jp027597k ↗
29. 10.1038/s41578-018-0024-910.1038/s41578-018-0024-9 ↗
30. 10.1126/science.123603410.1126/science.1236034 ↗
31. 10.1557/mrs.2018.14610.1557/mrs.2018.146 ↗
32. 10.1126/sciadv.160238810.1126/sciadv.1602388 ↗
33. 10.1021/acsnano.8b0142310.1021/acsnano.8b01423 ↗
34. 10.1021/nl502293a10.1021/nl502293a ↗
35. 10.1021/acs.nanolett.6b0035510.1021/acs.nanolett.6b00355 ↗
36. 10.1002/adma.20039008810.1002/adma.200390088 ↗
37. 10.1103/PhysRevB.48.1131710.1103/PhysRevB.48.11317 ↗
38. 10.1021/jp003815310.1021/jp0038153 ↗
39. 10.1038/nmat359610.1038/nmat3596 ↗
40. 10.1021/acsnano.5b0508510.1021/acsnano.5b05085 ↗
41. 10.1126/science.aac544310.1126/science.aac5443 ↗
42. 10.1021/acs.chemrev.7b0043010.1021/acs.chemrev.7b00430 ↗
43. 10.1038/s41929-018-0138-x10.1038/s41929-018-0138-x ↗
44. 10.1021/nn304738u10.1021/nn304738u ↗
45. 10.1021/acs.nanolett.8b0364010.1021/acs.nanolett.8b03640 ↗
46. 10.1038/nmat330310.1038/nmat3303 ↗
47. 10.1063/1.492699410.1063/1.4926994 ↗
48. 10.1016/j.ultramic.2015.10.02210.1016/j.ultramic.2015.10.022 ↗
49. 10.1021/acs.jpcc.8b0589710.1021/acs.jpcc.8b05897 ↗
50. 10.1063/1.499525810.1063/1.4995258 ↗
51. 10.1103/PhysRevB.51.1143310.1103/PhysRevB.51.11433 ↗
52. 10.1103/PhysRevB.77.07513310.1103/PhysRevB.77.075133 ↗
53. 10.1103/PhysRevB.61.1695610.1103/PhysRevB.61.16956 ↗
54. 10.1021/ja054734t10.1021/ja054734t ↗
55. 10.1021/la960445u10.1021/la960445u ↗
56. 10.1016/j.nantod.2014.02.00610.1016/j.nantod.2014.02.006 ↗
57. 10.1021/acscentsci.7b0012210.1021/acscentsci.7b00122 ↗
58. 10.1007/s11671-006-9015-710.1007/s11671-006-9015-7 ↗
59. 10.1021/acs.jpcc.8b0329910.1021/acs.jpcc.8b03299 ↗
60. 10.1103/PhysRevB.29.155810.1103/PhysRevB.29.1558 ↗
61. 10.1038/nnano.2015.16510.1038/nnano.2015.165 ↗
62. 10.1021/acs.jpcc.9b0366810.1021/acs.jpcc.9b03668 ↗
63. 10.1021/acsnano.6b0801010.1021/acsnano.6b08010 ↗
64. 10.1038/s41557-018-0003-110.1038/s41557-018-0003-1 ↗
65. 10.1126/science.aat696710.1126/science.aat6967 ↗
66. 10.1021/acsenergylett.8b0007010.1021/acsenergylett.8b00070 ↗
67. 10.1126/sciadv.170182310.1126/sciadv.1701823 ↗
68. 10.1021/jp412015710.1021/jp4120157 ↗
69. 10.1063/1.493995610.1063/1.4939956 ↗
70. 10.1038/s41563-019-0498-x10.1038/s41563-019-0498-x ↗
71. 10.1088/0026-1394/44/5/00510.1088/0026-1394/44/5/005 ↗
72. Koontz E. · 2019 · 85310.1007/978-3-319-93728-1_24 ↗
73. 10.1016/0370-1573(90)90099-N10.1016/0370-1573(90)90099-N ↗
74. 10.1103/PhysRevLett.91.04430110.1103/PhysRevLett.91.044301 ↗
75. 10.1038/nmeth.208910.1038/nmeth.2089 ↗
76. 10.1038/nmeth.201910.1038/nmeth.2019 ↗
77. 10.1021/jacs.8b0977910.1021/jacs.8b09779 ↗