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Engineering Efficient Photon Upconversion in Semiconductor Heterostructures

DOI:10.1021/acsnano.8b07062 期刊:ACS Nano 出版年份:2018 更新时间:2025-09-23 15:19:57
摘要: Photon upconversion is a photophysical process in which two low-energy photons are converted into one high-energy photon. Photon upconversion has broad appeal for a range of applications from biomedical imaging and targeted drug-release to solar energy harvesting. Current upconversion nanosystems, including lanthanide-doped nanocrystals and triplet-triplet annihilation (TTA) molecules, have achieved upconversion quantum yields of order 10-30%. However, the performance of these materials is hampered by inherently narrow absorption cross-sections and fixed energy levels originating in atomic, ionic, or molecular states. Semiconductors, on the other hand, have inherently wide absorption cross-sections. Moreover, recent advances enable the synthesis of colloidal semiconductor nanoparticles with complex heterostructures that can control band alignments and tune optical properties. We synthesize and characterize a three-component heterostructure that successfully upconverts photons under continuous-wave (CW) illumination and solar-relevant photon fluxes. The heterostructure is composed of two cadmium selenide (CdSe) quantum dots (QDs), an absorber and emitter, spatially separated by a cadmium sulfide (CdS) nanorod (NR). We demonstrate that the principles of semiconductor heterostructure engineering can be applied to engineer improved upconversion efficiency. We first eliminate electron trap-states near the surface of the absorbing QD and then tailor the bandgap of the NR such that charge carriers are funneled to the emitting QD. When combined, these two changes result in a 100-fold improvement in photon upconversion performance.
作者: Christopher C. Milleville,Eric Y. Chen,Kyle R. Lennon,Jill M. Cleveland,Abinash Kumar,Jing Zhang,James A. Bork,Ansel Tessier,James M. LeBeau,D. Bruce Chase,Joshua M. O. Zide,Matthew F. Doty
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To develop and realize nanoscale heterostructures that upconvert photons efficiently for applications in biomedical imaging, targeted drug delivery, and solar energy harvesting.

The study demonstrates that colloidal semiconductor heterostructures can implement photon upconversion under CW illumination and photon fluxes equivalent to the unconcentrated solar spectrum. The systematic employment of semiconductor heterostructure engineering methods achieves a 100-fold improvement in the upconversion performance of these heterostructures. Future improvements can be expected with the passivation of surface defects by wide bandgap shells.

The performance of the upconversion heterostructures is limited by surface defects and thermally-driven diffusion of carriers from the emitter to the absorber QD. Improvements by a factor of as much as 100 can be expected when surface defects are passivated by wide bandgap shells.

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