534
M. Vacha and S. Hirata
30.4 Conclusion
In conclusion, we studied collective photoresponse of molecular complexes and
related inorganic and hybrid materials on nanometer scales using single-molecule
detection and spectroscopy. The single-molecule and single-particle approach have
demonstrated its unique abilities and advantages in uncovering mechanisms that
lead to decrease of emission quantum efficiency of photoluminescence and electroluminescence due to emission blinking in perovskite nanocrystals and quantum
dots, in revealing excitonic and electrical interactions in aggregates of nanocrystals,
in demonstrating light polarization selectivity of plasmon enhancement in energy
transfer processes and in nanoscale characterization of exciton diffusion in molecular solids. We hope that the current work will stimulate further research using the
high potential of this optical nanoscale characterization technique.
Acknowledgements The present work was supported by JSPS KAKENHI Grant Numbers
JP26107014, JP26107004, JP15H01082, JP15H01099, JP17H05254, 17H05243, Grant-in-Aid for
Scientific Research on Innovative Areas “Photosynergetics” and by the Grant-in-Aid Number
19H02684.
References
1. Vacha M, Habuchi S (2010) Conformation and physics of polymer chains: a single-molecule
perspective. NPG Asia Mater 2:134–142
2. Vacha M, Sharma DK, Hirata S (2018) Single-molecule studies beyond optical imaging: multiparameter single-molecule spectroscopy. J Photochem Photobiol C Photochem Rev 34:121–
136
3. Sharma DK, Hirata S, Vacha M (2019) Single-particle electroluminescence of CsPbBr 3
perovskite nanocrystals reveals particle-selective recombination and blinking as key efficiency
factors. Nat Commun 10:4499
4. Sharma DK, Hirata S, Biju V, Vacha M (2019) Stark effect and environment induced modulation
of emission in single halide perovskite nanocrystals. ACS Nano 13:624–632
5. Narushima K, Kiyota Y, Mori T, Hirata S, Vacha M (2019) Suppressed triplet exciton diffusion due to small orbital overlap as a key design factor for ultralong-lived room temperature
phosphorescence in molecular crystals. Adv Mater 31:1807268
6. Kameyama T, Kishi M, Miyamae C, Sharma DK, Hirata S, Yamamoto T, Uematsu T, Vacha
M, Kuwabata S, Torimoto T (2018) Wavelength-tunable band-edge photoluminescence of
non-stoichiometric Ag-In-S nanoparticles via Ga 3+ doping. ACS Appl Mater Interf 10:42844–
42855
7. Hatazaki S, Sharma DK, Hirata S, Nose K, Iyoda T, Kölsch A, Lokstein H, Vacha M (2018)
Identification of short- and long-wavelength emitting chlorophylls in cyanobacterial photosystem I by plasmon-enhanced single-particle spectroscopy at room temperature. J Phys Chem
Lett 9:6669–6675
8. Uematsu T, Wajima K, Sharma DK, Hirata S, Yamamoto T, Kameyama T, Vacha M, Torimoto
T, Kuwabata S (2018) Narrow band-edge photoluminescence from AgInS 2 semiconductor
nanoparticles by the formation of amorphous III-VI semiconductor shells. NPG Asia Mater
10:713–726
M. Vacha and S. Hirata
30.4 Conclusion
In conclusion, we studied collective photoresponse of molecular complexes and
related inorganic and hybrid materials on nanometer scales using single-molecule
detection and spectroscopy. The single-molecule and single-particle approach have
demonstrated its unique abilities and advantages in uncovering mechanisms that
lead to decrease of emission quantum efficiency of photoluminescence and electroluminescence due to emission blinking in perovskite nanocrystals and quantum
dots, in revealing excitonic and electrical interactions in aggregates of nanocrystals,
in demonstrating light polarization selectivity of plasmon enhancement in energy
transfer processes and in nanoscale characterization of exciton diffusion in molecular solids. We hope that the current work will stimulate further research using the
high potential of this optical nanoscale characterization technique.
Acknowledgements The present work was supported by JSPS KAKENHI Grant Numbers
JP26107014, JP26107004, JP15H01082, JP15H01099, JP17H05254, 17H05243, Grant-in-Aid for
Scientific Research on Innovative Areas “Photosynergetics” and by the Grant-in-Aid Number
19H02684.
References
1. Vacha M, Habuchi S (2010) Conformation and physics of polymer chains: a single-molecule
perspective. NPG Asia Mater 2:134–142
2. Vacha M, Sharma DK, Hirata S (2018) Single-molecule studies beyond optical imaging: multiparameter single-molecule spectroscopy. J Photochem Photobiol C Photochem Rev 34:121–
136
3. Sharma DK, Hirata S, Vacha M (2019) Single-particle electroluminescence of CsPbBr 3
perovskite nanocrystals reveals particle-selective recombination and blinking as key efficiency
factors. Nat Commun 10:4499
4. Sharma DK, Hirata S, Biju V, Vacha M (2019) Stark effect and environment induced modulation
of emission in single halide perovskite nanocrystals. ACS Nano 13:624–632
5. Narushima K, Kiyota Y, Mori T, Hirata S, Vacha M (2019) Suppressed triplet exciton diffusion due to small orbital overlap as a key design factor for ultralong-lived room temperature
phosphorescence in molecular crystals. Adv Mater 31:1807268
6. Kameyama T, Kishi M, Miyamae C, Sharma DK, Hirata S, Yamamoto T, Uematsu T, Vacha
M, Kuwabata S, Torimoto T (2018) Wavelength-tunable band-edge photoluminescence of
non-stoichiometric Ag-In-S nanoparticles via Ga 3+ doping. ACS Appl Mater Interf 10:42844–
42855
7. Hatazaki S, Sharma DK, Hirata S, Nose K, Iyoda T, Kölsch A, Lokstein H, Vacha M (2018)
Identification of short- and long-wavelength emitting chlorophylls in cyanobacterial photosystem I by plasmon-enhanced single-particle spectroscopy at room temperature. J Phys Chem
Lett 9:6669–6675
8. Uematsu T, Wajima K, Sharma DK, Hirata S, Yamamoto T, Kameyama T, Vacha M, Torimoto
T, Kuwabata S (2018) Narrow band-edge photoluminescence from AgInS 2 semiconductor
nanoparticles by the formation of amorphous III-VI semiconductor shells. NPG Asia Mater
10:713–726