Efficient carrier multiplication in CsPbI3 perovskite nanocrystals

被引:107
作者
de Weerd, Chris [1 ]
Gomez, Leyre [1 ]
Capretti, Antonio [1 ]
Lebrun, Delphine M. [2 ]
Matsubara, Eiichi [3 ,4 ]
Lin, Junhao [5 ]
Ashida, Masaaki [4 ]
Spoor, Frank C. M. [6 ]
Siebbeles, Laurens D. A. [6 ]
Houtepen, Arjan J. [6 ]
Suenaga, Kazutomo [7 ]
Fujiwara, Yasufumi [2 ]
Gregorkiewicz, Tom [1 ,2 ]
机构
[1] Univ Amsterdam, Inst Phys, Sci Pk 904, NL-1098 XH Amsterdam, Netherlands
[2] Osaka Univ, Grad Sch Engn, Div Mat & Mfg Sci, 2-1 Yamadaoka, Suita, Osaka 5650871, Japan
[3] Osaka Dent Univ, Dept Phys, 8-1 Kuzuha Hanazono, Hirakata, Osaka 5731121, Japan
[4] Osaka Univ, Grad Sch Engn Sci, 1-3 Machikaneyama, Toyonaka, Osaka 5608531, Japan
[5] Southern Univ Sci & Technol, Dept Phys, Shenzhen 518055, Peoples R China
[6] Delft Univ Technol, Fac Appl Sci, Bldg 58,van der Maasweg 9, NL-2629 HZ Delft, Netherlands
[7] Natl Inst Adv Ind Sci & Technol, AIST Cent 5, Tsukuba, Ibaraki 3058565, Japan
基金
奥地利科学基金会;
关键词
MULTIPLE EXCITON GENERATION; CONVERSION EFFICIENCY; DYNAMICAL PROPERTIES; QUANTUM EFFICIENCY; IMPACT IONIZATION; SILICON; LIGHT; PBSE; ABSORPTION; COST;
D O I
10.1038/s41467-018-06721-0
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The all-inorganic perovskite nanocrystals are currently in the research spotlight owing to their physical stability and superior optical properties-these features make them interesting for optoelectronic and photovoltaic applications. Here, we report on the observation of highly efficient carrier multiplication in colloidal CsPbl(3) nanocrystals prepared by a hot-injection method. The carrier multiplication process counteracts thermalization of hot carriers and as such provides the potential to increase the conversion efficiency of solar cells. We demonstrate that carrier multiplication commences at the threshold excitation energy near the energy conservation limit of twice the band gap, and has step-like characteristics with an extremely high quantum yield of up to 98%. Using ultrahigh temporal resolution, we show that carrier multiplication induces a longer build-up of the free carrier concentration, thus providing important insights into the physical mechanism responsible for this phenomenon. The evidence is obtained using three independent experimental approaches, and is conclusive.
引用
收藏
页数:9
相关论文
共 62 条
[1]   Multiexcitons confined within a subexcitonic volume: Spectroscopic and dynamical signatures of neutral and charged biexcitons in ultrasmall semiconductor nanocrystals [J].
Achermann, M ;
Hollingsworth, JA ;
Klimov, VI .
PHYSICAL REVIEW B, 2003, 68 (24)
[2]   Highly efficient carrier multiplication in PbS nanosheets [J].
Aerts, Michiel ;
Bielewicz, Thomas ;
Klinke, Christian ;
Grozema, Ferdinand C. ;
Houtepen, Arjan J. ;
Schins, Juleon M. ;
Siebbeles, Laurens D. A. .
NATURE COMMUNICATIONS, 2014, 5
[3]   Multiple exciton generation and ultrafast exciton dynamics in HgTe colloidal quantum dots [J].
Al-Otaify, Ali ;
Kershaw, Stephen V. ;
Gupta, Shuchi ;
Rogach, Andrey L. ;
Allan, Guy ;
Delerue, Christophe ;
Binks, David. J. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2013, 15 (39) :16864-16873
[4]   Semiconductor clusters, nanocrystals, and quantum dots [J].
Alivisatos, AP .
SCIENCE, 1996, 271 (5251) :933-937
[5]   Multiple exciton generation in colloidal silicon nanocrystals [J].
Beard, Matthew C. ;
Knutsen, Kelly P. ;
Yu, Pingrong ;
Luther, Joseph M. ;
Song, Qing ;
Metzger, Wyatt K. ;
Ellingson, Randy J. ;
Nozik, Arthur J. .
NANO LETTERS, 2007, 7 (08) :2506-2512
[6]   Third Generation Photovoltaics based on Multiple Exciton Generation in Quantum Confined Semiconductors [J].
Beard, Matthew C. ;
Luther, Joseph M. ;
Semonin, Octavi E. ;
Nozik, Arthur J. .
ACCOUNTS OF CHEMICAL RESEARCH, 2013, 46 (06) :1252-1260
[7]   Comparing Multiple Exciton Generation in Quantum Dots To Impact Ionization in Bulk Semiconductors: Implications for Enhancement of Solar Energy Conversion [J].
Beard, Matthew C. ;
Midgett, Aaron G. ;
Hanna, Mark C. ;
Luther, Joseph M. ;
Hughes, Barbara K. ;
Nozik, Arthur J. .
NANO LETTERS, 2010, 10 (08) :3019-3027
[8]   Variations in the Quantum Efficiency of Multiple Exciton Generation for a Series of Chemically Treated PbSe Nanocrystal Films [J].
Beard, Matthew C. ;
Midgett, Aaron G. ;
Law, Matt ;
Semonin, Octavi E. ;
Ellingson, Randy J. ;
Nozik, Arthur J. .
NANO LETTERS, 2009, 9 (02) :836-845
[9]   Bright triplet excitons in caesium lead halide perovskites [J].
Becker, Michael A. ;
Vaxenburg, Roman ;
Nedelcu, Georgian ;
Sercel, Peter C. ;
Shabaev, Andrew ;
Mehl, Michael J. ;
Michopoulos, John G. ;
Lambrakos, Samuel G. ;
Bernstein, Noam ;
Lyons, John L. ;
Stoferle, Thilo ;
Mahrt, Rainer F. ;
Kovalenko, Maksym V. ;
Norris, David J. ;
Raino, Gabriele ;
Efros, Alexander L. .
NATURE, 2018, 553 (7687) :189-+
[10]   Multiple exciton generation in nanocrystal quantum dots - controversy, current status and future prospects [J].
Binks, David J. .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2011, 13 (28) :12693-12704