Surface-Sensitive Photon Avalanche Behavior Revealed by Single-Avalanching-Nanoparticle Imaging

Year: 2021

Type: article

Abstract: Avalanching nanoparticles (ANPs) are a new class of lanthanide-based upconverting material demonstrating steep optical nonlinearities with the potential to advance applications ranging from subwavelength bioimaging to neuromorphic computing, nanothermometry, and pressure transduction. Here, we use single-nanocrystal imaging to uncover design-dependent heterogeneity in ANP threshold intensity ( I th ). Quantitative comparisons between distributions of I th and ANP shell properties reveal correlations between mean I th values, histogram widths, and nanocrystal shell thickness. Evaluating avalanching behaviors using an established model of shell-dependent surface energy transfer shows that variations in shell thickness–and the resultant energy transfer through the shell to the surface and environment–are likely the primary contributor to ANP-to-ANP I th heterogeneity. Further, nanocrystals with an ∼6 nm average shell thickness show I th heterogeneity beyond the extent expected from statistical measurements of shell size and variability using transmission electron microscopy (TEM). These results provide a principal guide for the design and application of ANPs to environmental sensing.

Source: The Journal of Physical Chemistry C

DOI: 10.1021/acs.jpcc.1c07721

Authors: Kevin W. C. Kwock, Changhwan Lee, Ayelet Teitelboim, Yawei Liu, Kaiyuan Yao, Sardar B. Alam, Bruce E. Cohen, Emory M. Chan, P. James Schuck

Institutions: Columbia University, Lawrence Berkeley National Laboratory, Molecular Foundry, Chinese Academy of Sciences, Changchun Institute of Applied Chemistry, State Key Laboratory of Rare Earth Resources Utilization

Language: English

Topic: Luminescence Properties of Advanced Materials

Subfield: Materials Chemistry

Field: Materials Science

Domain: Physical Sciences

Open Access status: green

Funders: U.S. Department of Energy, National Research Foundation, Korea Research Institute of Chemical Technology, National Research Foundation of Korea, Ministry of Science and ICT, South Korea, Office of Science, National Nuclear Security Administration, Basic Energy Sciences

OpenAlex ID: W3208679783