In conventional light-harvesting devices, the absorption of a single photon only excites one electron, which sets the standard limit of power-conversion efficiency, such as the Shockley-Queisser limit. In principle, generating and harnessing multiple carriers per absorbed photon can improve efficiency and possibly overcome this limit. We report the observation of multiple hot-carrier collection in graphene/boron-nitride Moiré superlattice structures. A record-high zero-bias photoresponsivity of 0.3 A/W (equivalently, an external quantum efficiency exceeding 50%) is achieved using graphene's photo-Nernst effect, which demonstrates a collection of at least five carriers per absorbed photon. We reveal that this effect arises from the enhanced Nernst coefficient through Lifshtiz transition at low-energy Van Hove singularities, which is an emergent phenomenon due to the formation of Moiré minibands. Our observation points to a new means for extremely efficient and flexible optoelectronics based on van der Waals heterostructures.
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http://dx.doi.org/10.1126/sciadv.1600002 | DOI Listing |
Adv Mater
December 2024
Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, Kowloon, China.
Hot-carrier relaxation above the bandgap results in significant energy losses, making the extraction of hot carriers a critical challenge for efficient hot-carrier photocurrent generation in devices. In this study, we observe long-lived hot carriers in the metal-halide perovskite multiple quantum wells, (BA)(MA)PbI (n = 3), and demonstrate effective hot-hole photocurrent generation using 2D MoS₂ as an extraction layer. A high external quantum efficiency of short-circuit hot-carrier photocurrent of up to 35.
View Article and Find Full Text PDFJ Chem Phys
August 2024
Department of Chemistry, Indian Institute of Technology Bombay, Powai, Mumbai 400076, India.
Single particle level microscopy of immobilized FAPbBr3 nanocrystals (NCs) has elucidated the involvement of different processes in their photoluminescence (PL) intermittency. Four different blinking patterns are observed in the data from more than 100 NCs. The dependence of PL decays on PL intensities brought out in fluorescence lifetime intensity distribution (FLID) plots is rationalized by the interplay of exciton- and trion-mediated recombinations along with hot carrier (HC) trapping.
View Article and Find Full Text PDFACS Nano
July 2024
Department of Physics and William Mong Institute of Nano Science and Technology, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong S.A.R., P. R. China.
Rapid hot-carrier/exciton cooling constitutes a major loss channel for photovoltaic efficiency. How to decelerate the hot-carrier/exciton relaxation remains a crux for achieving high-performance photovoltaic devices. Here, we demonstrate slow hot-exciton cooling that can be extended to hundreds of picoseconds in colloidal HgTe quantum dots (QDs).
View Article and Find Full Text PDFNano Lett
March 2024
Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea.
Hot electrons are crucial for unraveling the intrinsic relationship between chemical reactions and charge transfer in heterogeneous catalysis. Significant research focused on real-time detection of reaction-driven hot electron flow (chemicurrent) to elucidate the energy conversion mechanisms, but it remains elusive because carrier generation contributes to only part of the entire process. Here, a theoretical model for quantifying the chemicurrent yield is presented by clarifying the contributions of hot carrier losses from the internal emission and multiple reflections.
View Article and Find Full Text PDFPhys Rev Lett
October 2023
State Key Laboratory of Superlattices and Microstructures, Institute of Semiconductors, Chinese Academy of Science, Beijing 100083, China.
With the rapid development of ultrafast experimental techniques for the research of carrier dynamics in solid-state systems, a microscopic understanding of the related phenomena, particularly a first-principle calculation, is highly desirable. Nonadiabatic molecular dynamics (NAMD) offers a real-time direct simulation of the carrier transfer or carrier thermalization. However, when applied to a periodic supercell, there is no cross-k-point transitions during the NAMD simulation.
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