Sub-millielectronvolt Line Widths in Polarized Low-Temperature Photoluminescence of 2D PbS Nanoplatelets

Overview

Journal Nano Lett

Publisher American Chemical Society

Specialty Biotechnology

Date 2024 Nov 22

PMID 39576056

Authors

Pengji Li

Leon Biesterfeld

Lars F Klepzig

Jingzhong Yang

Huu Thoai Ngo

Ahmed Addad

Tom N Rakow

Ruolin Guan

Eddy P Rugeramigabo

Ivan Zaluzhnyy

Frank Schreiber

Louis Biadala

Jannika Lauth

Michael Zopf

Affiliations

Soon will be listed here.

Abstract

Colloidal semiconductor nanocrystals are promising materials for classical and quantum light sources due to their efficient photoluminescence (PL) and versatile chemistry. While visible emitters are well-established, excellent (near-infrared) sources are still being pursued. We present the first comprehensive analysis of low-temperature PL from two-dimensional (2D) PbS nanoplatelets (NPLs). Ultrathin 2D PbS NPLs exhibit high crystallinity confirmed by scanning transmission electron microscopy, revealing Moiré patterns in overlapping NPLs. At 4 K, unique PL features are observed in single PbS NPLs, including narrow zero-phonon lines with line widths down to 0.6 meV and a linear degree of polarization up to 90%. Time-resolved measurements identify trions as the dominant emission source with a 2.3 ns decay time. Sub-meV spectral diffusion and no inherent blinking over minutes are observed, as well as discrete spectral jumps without memory effects. These findings advance the understanding and underscore the potential of colloidal PbS NPLs for optical and quantum technologies.

References

Hu F, Zhang H, Sun C, Yin C, Lv B, Zhang C . Superior Optical Properties of Perovskite Nanocrystals as Single Photon Emitters. ACS Nano. 2015; 9(12):12410-6. DOI: 10.1021/acsnano.5b05769. View

Girard A, Saviot L, Pedetti S, Tessier M, Margueritat J, Gehan H . The mass load effect on the resonant acoustic frequencies of colloidal semiconductor nanoplatelets. Nanoscale. 2016; 8(27):13251-6. DOI: 10.1039/c5nr07383a. View

Kagan C, Bassett L, Murray C, Thompson S . Colloidal Quantum Dots as Platforms for Quantum Information Science. Chem Rev. 2020; 121(5):3186-3233. DOI: 10.1021/acs.chemrev.0c00831. View

Park Y, Guo S, Makarov N, Klimov V . Room Temperature Single-Photon Emission from Individual Perovskite Quantum Dots. ACS Nano. 2015; 9(10):10386-93. DOI: 10.1021/acsnano.5b04584. View

Moreels I, Justo Y, De Geyter B, Haustraete K, Martins J, Hens Z . Size-tunable, bright, and stable PbS quantum dots: a surface chemistry study. ACS Nano. 2011; 5(3):2004-12. DOI: 10.1021/nn103050w. View

Klepzig L, Biesterfeld L, Romain M, Niebur A, Schlosser A, Hubner J . Colloidal 2D PbSe nanoplatelets with efficient emission reaching the telecom O-, E- and S-band. Nanoscale Adv. 2022; 4(2):590-599. PMC: 9418099. DOI: 10.1039/d1na00704a. View

Ithurria S, Tessier M, Mahler B, Lobo R, Dubertret B, Efros A . Colloidal nanoplatelets with two-dimensional electronic structure. Nat Mater. 2011; 10(12):936-41. DOI: 10.1038/nmat3145. View

Bielewicz T, Dogan S, Klinke C . Tailoring the height of ultrathin PbS nanosheets and their application as field-effect transistors. Small. 2014; 11(7):826-33. DOI: 10.1002/smll.201402144. View

Canneson D, Shornikova E, Yakovlev D, Rogge T, Mitioglu A, Ballottin M . Negatively Charged and Dark Excitons in CsPbBr Perovskite Nanocrystals Revealed by High Magnetic Fields. Nano Lett. 2017; 17(10):6177-6183. DOI: 10.1021/acs.nanolett.7b02827. View

10.

Hinterding S, Salzmann B, Vonk S, Vanmaekelbergh D, Weckhuysen B, Hutter E . Single Trap States in Single CdSe Nanoplatelets. ACS Nano. 2021; 15(4):7216-7225. PMC: 8155320. DOI: 10.1021/acsnano.1c00481. View

11.

Pietryga J, Schaller R, Werder D, Stewart M, Klimov V, Hollingsworth J . Pushing the band gap envelope: mid-infrared emitting colloidal PbSe quantum dots. J Am Chem Soc. 2004; 126(38):11752-3. DOI: 10.1021/ja047659f. View

12.

Xie R, Peng X . Synthetic scheme for high-quality InAs nanocrystals based on self-focusing and one-pot synthesis of InAs-based core-shell nanocrystals. Angew Chem Int Ed Engl. 2008; 47(40):7677-80. DOI: 10.1002/anie.200802867. View

13.

Protesescu L, Yakunin S, Bodnarchuk M, Krieg F, Caputo R, Hendon C . Nanocrystals of Cesium Lead Halide Perovskites (CsPbX₃, X = Cl, Br, and I): Novel Optoelectronic Materials Showing Bright Emission with Wide Color Gamut. Nano Lett. 2015; 15(6):3692-6. PMC: 4462997. DOI: 10.1021/nl5048779. View

14.

Izquierdo E, Robin A, Keuleyan S, Lequeux N, Lhuillier E, Ithurria S . Strongly Confined HgTe 2D Nanoplatelets as Narrow Near-Infrared Emitters. J Am Chem Soc. 2016; 138(33):10496-501. DOI: 10.1021/jacs.6b04429. View

15.

Fernee M, Plakhotnik T, Louyer Y, Littleton B, Potzner C, Tamarat P . Spontaneous Spectral Diffusion in CdSe Quantum Dots. J Phys Chem Lett. 2015; 3(12):1716-20. DOI: 10.1021/jz300456h. View

16.

Morad V, Stelmakh A, Svyrydenko M, Feld L, Boehme S, Aebli M . Designer phospholipid capping ligands for soft metal halide nanocrystals. Nature. 2023; 626(7999):542-548. PMC: 10866715. DOI: 10.1038/s41586-023-06932-6. View

17.

Califano M, Franceschetti A, Zunger A . Temperature dependence of excitonic radiative decay in CdSe quantum dots: the role of surface hole traps. Nano Lett. 2005; 5(12):2360-4. DOI: 10.1021/nl051027p. View

18.

Schmidt , Lischka , Zulehner . Excitation-power dependence of the near-band-edge photoluminescence of semiconductors. Phys Rev B Condens Matter. 1992; 45(16):8989-8994. DOI: 10.1103/physrevb.45.8989. View

19.

Diroll B, Guzelturk B, Po H, Dabard C, Fu N, Makke L . 2D II-VI Semiconductor Nanoplatelets: From Material Synthesis to Optoelectronic Integration. Chem Rev. 2023; 123(7):3543-3624. DOI: 10.1021/acs.chemrev.2c00436. View

20.

Hu Z, Kim Y, Krishnamurthy S, Avdeev I, Nestoklon M, Singh A . Intrinsic Exciton Photophysics of PbS Quantum Dots Revealed by Low-Temperature Single Nanocrystal Spectroscopy. Nano Lett. 2019; 19(12):8519-8525. DOI: 10.1021/acs.nanolett.9b02937. View