Ultrafast multiexciton Auger recombination of CdSeS

Qin Chao-Chao; Cui Ming-Huan; Song Di-Di; He Wei

doi:10.7498/aps.68.20190291

Abstract

Multiexciton generation is a process where multiple excitons are generated by absorbing single photons. Efficient multiexciton generation in quantum dots may be a revolutionary discovery, because it provides a new method to improve the solar-to-electric power conversion efficiency in quantum dots-based solar cells and to design novel quantum dots-based multielectron or hole photocatalysts. However, the mechanism of ultrafast multiexciton generation and recombination remain unclear. In this paper, alloy-structured quantum dots, CdSeS, are prepared by the hot injection method. The generation and recombination mechanism of charge carriers in quantum dots samples are discussed in detail. The bivalent band structure of alloy-structured quantum dots is determined by ultraviolet-visible absorption spectra. It is found that the 1S_3/2(h)-1S(e) (or 1S), 2S_3/2(h)-1S(e) (or 2S) and 1P_3/2(h)-1P(e) (or 1P) exciton absorption bands of these quantum dots are at 510 nm, 468 nm and 430 nm, respectively. Femtosecond transient absorption spectroscopy and nanosecond time-resolved photoluminescence spectroscopy are used to investigate the ultrafast exciton generation and recombination dynamics in the alloy-structured quantum dots. By fitting the transient kinetics of 1S exciton bleach, an average biexciton decay time is obtained to be about 80 ps, which is almost twice the decay time of traditional quantum dots (less than 50 ps). Combined with the recently developed ultrafast interface charge separation technology that can extract multiple excitons before their annihilation, it will have a promising application prospect. Moreover, there is a hole relaxation on a the time scale of 5-6 ps via a phonon coupling pathway to lower-energy hole states in addition to the above-described ultrafast exciton-exciton annihilation process in 2S and 1P excitons. Furthermore, by nanosecond time-resolved photoluminescence spectroscopy, it can be concluded that the charge separated state is long-lived (200 ns). Our findings provide a valuable insight into the understanding of ultrafast multiexciton generation and recombination in quantum dots. These results are helpful to understand the intrinsic photo-physics of multiexciton generation in quantum dots, to implement the photovoltaic and optoelectronic applications, and to ascertain the exciton relaxation dynamics of quantum dots.

Keywords:

Authors and contacts

College of Physics and Materials Science, Henan Normal University, Xinxiang 453007, China

Corresponding author: Qin Chao-Chao, qinch@hotmail.com

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. U1404112, 11804084), the Advanced Technology Research Program of Henan Province, China (Grant Nos. 182102210369), and the Foundation for Key Program of Education Department of Henan Province, China (Grant No. 19A140011).

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References

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[2]	Werner J H, Kolodinski S, Queisser H J 1994 Phys. Rev. Lett. 72 3851 Google Scholar
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图 1 样品的稳态吸收光谱(实线)和稳态荧光光谱(虚线), 其中插图部分为样品的能带跃迁示意图

Figure 1. Steady-state absorption (solid-line) and fluorescence (dash-line) spectrum of QDs sample. Inset: energy level diagram illustrating the relevant energy of electron/hole states and allowed optical transitions (diagram not drawn to scale).

DownLoad: Full-Size Img PowerPoint

图 2 365 nm不同光强激发下的飞秒时间分辨瞬态吸收光谱　(a) 激发脉冲能量为8 nJ的瞬态吸收光谱彩图; (b) 激发脉冲能量为50 nJ的瞬态吸收光谱彩图; (c) 激发脉冲能量为8 nJ的演变相关差分光谱; (d) 激发脉冲能量为50 nJ的演变相关差分光谱

Figure 2. Femtosecond time-resolved transient absorption (TA) spectra at 365 nm excitation with different intensities: (a) TA color map with excitation pulse energy of 8 nJ; (b) TA color map with excitation pulse energy of 50 nJ; (c) evolution-associated difference spectrum (EADS) with excitation pulse energy of 8 nJ; (d) EADS with excitation pulse energy of 50 nJ.

DownLoad: Full-Size Img PowerPoint

图 3 365 nm不同光强激发下的飞秒时间分辨瞬态吸收光谱　(a) 激发脉冲能量为100 nJ的瞬态吸收光谱彩图; (b)激发脉冲能量为500 nJ的瞬态吸收光谱彩图; (c) 激发脉冲能量为100 nJ的演变相关差分光谱; (d)激发脉冲能量为500 nJ的演变相关差分光谱

Figure 3. Femtosecond time-resolved transient absorption (TA) spectra at 365 nm excitation with different intensities: (a) TA color map with excitation pulse energy of 100 nJ; (b) TA color map with excitation pulse energy of 500 nJ; (c) EADS with excitation pulse energy of 100 nJ; (d) EADS with excitation pulse energy of 500 nJ.

DownLoad: Full-Size Img PowerPoint

图 4 不同激发能量的瞬态吸收光谱数据在各个激子峰处的漂白动力学曲线　(a) 1P激子漂白峰(430 nm); (b) 2S激子漂白峰(468 nm); (c) 1S激子漂白峰(510 nm). 所有动力学曲线已经归一化至最大振幅

Figure 4. The kinetics of TA with different excitation intensities at exciton peaks: (a) 1P exciton bleach recovery (at 430 nm); (b) 2S exciton bleach recovery (at 468 nm); (c) 1S exciton bleach recovery (at 430 nm). All kinetic traces have been normalized to the same maximum amplitude.

DownLoad: Full-Size Img PowerPoint

图 5 时间分辨荧光光谱图

Figure 5. Time-resolved photoluminescence color map.

DownLoad: Full-Size Img PowerPoint

表 1 样品的瞬态吸收数据在510 nm(1S激子)处动力学曲线的拟合参数

Table 1. Best-fit parameters of the kinetic curve of the transient absorption data of the QDs at 510 nm (1S exciton).

激发脉冲能量	寿命值
激发脉冲能量	τ_et/ps (权重/%)	τ₁/ps (权重/%)	τ₂/ns (权重/%)
8 nJ	0.391 (100)	–	$\gg$10 (100)
50 nJ	0.431 (100)	82.6 (52.5)	$ \gg$10 (47.5)
100 nJ	0.374 (100)	82.5 (55.6)	$ \gg$10 (44.4)
500 nJ	0.381 (100)	80.9 (54)	$ \gg$10 (46)

DownLoad: CSV

表 2 样品的瞬态吸收数据在468 nm(2S激子)处动力学曲线的拟合参数

Table 2. Best-fit parameters of the kinetic curve of the transient absorption data of the QDs at 468 nm (2S exciton).

激发脉冲能量	寿命值
激发脉冲能量	τ_et/ps (权重/%)	τ₁/ps (权重/%)	τ₂/ps (权重/%)	τ₃/ns (权重/%)
8 nJ	0.353 (100)	–	–	$ \gg$10 (100)
50 nJ	0.429 (100)	6.0 (67.7)	59.1 (8.5)	$ \gg$10 (23.8)
100 nJ	0.362 (100)	5.5 (32.7)	59.8 (43.5)	$ \gg$10 (25)
500 nJ	0.340 (100)	5.1 (50.1)	53.7 (41.3)	$ \gg$10 (8.3)

DownLoad: CSV

表 3 样品的瞬态吸收数据在430 nm(1P激子)处动力学曲线的拟合参数

Table 3. Best-fit parameters of the kinetic curve of the transient absorption data of the QDs at 430 nm (1P exciton).

激发脉冲能量	寿命值
激发脉冲能量	τ_et/ps (权重/%)	τ₁/ps (权重/%)	τ₂/ps (权重/%)	τ₃/ns (权重/%)
8 nJ	0.188 (100)	–	–	$ \gg$10 (100)
50 nJ	0.269 (100)	8.2 (27.1)	57.0 (22.9)	$ \gg$10 (50)
100 nJ	0.213 (100)	6.8 (27.2)	52.8 (47.7)	$ \gg$10 (21.9)
500 nJ	0.207 (100)	6.3 (49.5)	51.4 (33.3)	$ \gg$10 (17.1)

DownLoad: CSV

[1]	Shockley W, Queisser H J 1961 J. Appl. Phys. 32 510 Google Scholar
[2]	Werner J H, Kolodinski S, Queisser H J 1994 Phys. Rev. Lett. 72 3851 Google Scholar
[3]	Beard M C, Luther J M, Nozik A J 2014 Nat. Nanotechnol. 9 951 Google Scholar
[4]	ten Cate S, Sandeep C S S, Liu Y, Law M, Kinge S, Houtepen A J, Schins J M, Siebbeles L D A 2015 Acc. Chem. Res. 48 174 Google Scholar
[5]	Tahara H, Sakamoto M, Teranishi T, Kanemitsu Y 2017 Phys. Rev. Lett. 119 247401 Google Scholar
[6]	Tahara H, Sakamoto M, Teranishi T, Kanemitsu Y 2018 Nat. Commun. 9 3179 Google Scholar
[7]	Damtie F A, Karki K J, Pullerits T, Wacker A 2016 J. Chem. Phys. 145 064703 Google Scholar
[8]	Park Y S, Guo S J, Makarov N S, Klimov V I 2015 ACS Nano 9 10386 Google Scholar
[9]	Hu F R, Yin C Y, Zhang H C, Sun C, Yu W W, Zhang C F, Wang X Y, Zhang Y, Xiao M 2016 Nano Lett. 16 6425 Google Scholar
[10]	Hu F R, Zhang H C, Sun C, Yin C Y, Lü B H, Zhang C F, Yu W W, Wang X Y, Zhang Y, Xiao M 2015 ACS Nano 9 12410 Google Scholar
[11]	Zhao G, Cai Q B, Liu X T, Li P W, Zhang Y Q, Shao G S, Liang C 2019 IEEE J. Photovolt. 9 194 Google Scholar
[12]	Chen Z H, Zhang Z L, Yang J F, Chen W J, Teh Z L, Wang D, Yuan L, Zhang J B, Stride J A, Conibeer G J, Patterson R J, Huang S J 2018 J. Mater. Chem. C 6 9861 Google Scholar
[13]	Lin Q L, Yun H J, Liu W Y, Song H J, Makarov N S, Isaienko O, Nakotte T, Chen G, Luo H M, Klimov V I, Pietryga J M 2017 J. Am. Chem. Soc. 139 6644 Google Scholar
[14]	Zhang Z L, Chen Z H, Yuan L, Chen W J, Yang J F, Wang B, Wen X M, Zhang J B, Hu L, Stride J A, Conibeer G J, Patterson R J, Huang S J 2017 Adv. Mater. 29 1703214 Google Scholar
[15]	Li Q Y, Xu Z H, McBride J R, Lian T Q 2017 ACS Nano 11 2545 Google Scholar
[16]	Debnath T, Maity P, Maiti S, Ghosh H N 2014 J. Phys. Chem. Lett. 5 2836 Google Scholar
[17]	Spencer A P, Peters W K, Neale N R, Jonas D M 2019 J. Phys. Chem. C 123 848 Google Scholar
[18]	Al-Ghamdi M S, Sayari A, Sfaxi L 2016 J. Alloys Compd. 685 202 Google Scholar
[19]	Kwak G Y, Kim T G, Hong S, Kim A, Ha M H, Kim K J 2018 Sol. Energy 164 89 Google Scholar
[20]	Zhang P F, Feng Y, Wen X M, Cao W K, Anthony R, Kortshagen U, Conibeer G, Huang S J 2016 Sol. Energ. Mat. Sol. C 145 391 Google Scholar
[21]	Kryjevski A, Mihaylov D, Kilina S, Kilin D 2017 J. Chem. Phys. 147 154106 Google Scholar
[22]	Amori A R, Hou Z T, Krauss T D 2018 Annu. Rev. Phys. Chem. 69 81 Google Scholar
[23]	Schaller R D, Sykora M, Pietryga J M, Klimov V I 2006 Nano Lett. 6 424 Google Scholar
[24]	Ghimire S, Biju V 2018 J. Photoch. Photobio. C 34 137 Google Scholar
[25]	Zhu H, Lian T 2012 J. Am. Chem. Soc. 134 11289 Google Scholar
[26]	Shi X F, Xia X Y, Cui G W, Deng N, Zhao Y Q, Zhuo L H, Tang B 2015 Appl. Catal. B. Environ. 163 123 Google Scholar
[27]	Schaller R D, Agranovich V M, Klimov V I 2005 Nat. Phys. 1 189
[28]	Gordi M, Moravvej-Farshi M K, Ramezani H 2018 Chemphyschem 19 2782 Google Scholar
[29]	Jier H, Zhuangqun H, Ye Y, Haiming Z, Tianquan L 2010 J. Am. Chem. Soc. 132 4858 Google Scholar
[30]	Pijpers J J H, Milder M T W, Delerue C, Bonn M 2010 J. Phys. Chem. C 114 6318 Google Scholar
[31]	Yang Y, Lian T Q 2014 Coordin. Chem. Rev. 263 229
[32]	Ghosh H N, Singhal P, Maity P, Jha S K 2017 Chemistry 23 10590 Google Scholar
[33]	Kroupa D M, Pach G F, Voros M, Giberti F, Chernomordik B D, Crisp R W, Nozik A J, Johnson J C, Singh R, Klimov V I, Galli G, Beard M C 2018 ACS Nano 12 10084 Google Scholar
[34]	Harris R D, Homan S B, Kodaimati M, He C, Nepomnyashchii A B, Swenson N K, Lian S C, Calzada R, Weiss E A 2016 Chem. Rev. 116 12865 Google Scholar
[35]	Klimov V I 2007 Annu. Rev. Phys. Chem. 58 635 Google Scholar
[36]	韩元春, 包特木耳巴根 2015 物理学报 64 113021 Han Y C, Bao T 2015 Acta Phys. Sin. 64 113021
[37]	Liu C, Peterson J J, Krauss T D 2014 J. Phys. Chem. Lett. 5 3032 Google Scholar

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