Pournima Narayanan

All Publications

• Triplet Fusion Upconversion Nanocapsule Synthesis. Journal of visualized experiments : JoVE Schloemer, T. H., Sanders, S. N., Zhou, Q., Narayanan, P., Hu, M., Gangishetty, M. K., Anderson, D., Seitz, M., Gallegos, A. O., Stokes, R. C., Congreve, D. N. 2022

  Abstract

  Triplet fusion upconversion (UC) allows for the generation of one high energy photon from two low energy input photons. This well-studied process has significant implications for producing high energy light beyond a material's surface. However, the deployment of UC materials has been stymied due to poor material solubility, high concentration requirements, and oxygen sensitivity, ultimately resulting in reduced light output. Toward this end, nanoencapsulation has been a popular motif to circumvent these challenges, but durability has remained elusive in organic solvents. Recently, a nanoencapsulation technique was engineered to tackle each of these challenges, whereupon an oleic acid nanodroplet containing upconversion materials was encapsulated with a silica shell. Ultimately, these nanocapsules (NCs) were durable enough to enable triplet fusion upconversion-facilitated volumetric three-dimensional (3D) printing. By encapsulating upconversion materials with silica and dispersing them in a 3D printing resin, photopatterning beyond the surface of the printing vat was made possible. Here, video protocols for the synthesis of upconversion NCs are presented for both small-scale and large-scale batches. The outlined protocols serve as a starting point for adapting this encapsulation scheme to multiple upconversion schemes for use in volumetric 3D printing applications.

  View details for DOI 10.3791/64374

  View details for PubMedID 36155426

• Luminescence Enhancement Due to Symmetry Breaking in Doped Halide Perovskite Nanocrystals. Journal of the American Chemical Society Ahmed, G. H., Liu, Y., Bravic, I., Ng, X., Heckelmann, I., Narayanan, P., Fernandez, M. S., Monserrat, B., Congreve, D. N., Feldmann, S. 2022

  Abstract

  Metal-halide perovskite nanocrystals have demonstrated excellent optoelectronic properties for light-emitting applications. Isovalent doping with various metals (M2+) can be used to tailor and enhance their light emission. Although crucial to maximize performance, an understanding of the universal working mechanism for such doping is still missing. Here, we directly compare the optical properties of nanocrystals containing the most commonly employed dopants, fabricated under identical synthesis conditions. We show for the first time unambiguously, and supported by first-principles calculations and molecular orbital theory, that element-unspecific symmetry-breaking rather than element-specific electronic effects dominate these properties under device-relevant conditions. The impact of most dopants on the perovskite electronic structure is predominantly based on local lattice periodicity breaking and resulting charge carrier localization, leading to enhanced radiative recombination, while dopant-specific hybridization effects play a secondary role. Our results suggest specific guidelines for selecting a dopant to maximize the performance of perovskite emitters in the desired optoelectronic devices.

  View details for DOI 10.1021/jacs.2c07111

  View details for PubMedID 35977424