Wavelength dependence of optical nonlinearity of terpyridine-based Zn(II)-coordinated rigid linear polymers

He, Tingchao; Rajwar, Deepa; Ma, Lin; Wang, Yue; Lim, Zheng Bang; Grimsdale, Andrew C.; Sun, Handong

doi:10.1063/1.4767390

Cited by 18 publications

(26 citation statements)

References 25 publications

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“…The comparison between the normalized one-photon-excited PL spectra and MEPL spectra of the NCs are displayed in Supplementary Figure 10. As illustrated in Supplementary Figure 10, the slight redshift of the MEPL spectra with respect to one-photon counterpart has been well reported in traditional semiconductor NCs42 and can be ascribed to the reabsorption effect and size inhomogeneity4344. Further excitation fluence-dependent MEPL measurements at wavelengths ranging from 675 to 2,300 nm were also performed.…”

Section: Resultsmentioning

confidence: 59%

Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals

Chen

Bhaumik²,

Veldhuis³

et al. 2017

Nat Commun

190

280

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Multiphoton absorption processes enable many technologically important applications, such as in vivo imaging, photodynamic therapy and optical limiting, and so on. Specifically, higher-order nonlinear absorption such as five-photon absorption offers significant advantages of greater spatial confinement, increased penetration depth, reduced autofluorescence, enhanced sensitivity and improved resolution over lower orders in bioimaging. Organic chromophores and conventional semiconductor nanocrystals are leaders in two-/three-photon absorption applications, but face considerable challenges from their small five-photon action cross-sections. Herein, we reveal that the family of halide perovskite colloidal nanocrystals transcend these constraints with highly efficient five-photon-excited upconversion fluorescence—unprecedented for semiconductor nanocrystals. Amazingly, their multidimensional type I (both conduction and valence band edges of core lie within bandgap of shell) core–shell (three-dimensional methylammonium lead bromide/two-dimensional octylammonium lead bromide) perovskite nanocrystals exhibit five-photon action cross-sections that are at least 9 orders larger than state-of-the-art specially designed organic molecules. Importantly, this family of halide perovskite nanocrystals may enable fresh approaches for next-generation multiphoton imaging applications.

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Section: Resultsmentioning

confidence: 59%

Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals

Chen

Bhaumik²,

Veldhuis³

et al. 2017

Nat Commun

190

280

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“…Figure 5a-d shows the upconversion luminescence spectra of an isolated ZJU-28⊃MAPbBr 3 crystal with excitation ranged from 960 to 2100 nm. [21,22] In order to determine the MPACs of the single ZJU-28⊃MAPbBr 3 crystal, the multiphoton excited fluorescence reference method was used (see Supporting Information). The slope (that is, the order of MPE process) of 2.03 is very close to 2, indicating that the twophoton excitation (2PE) luminescence process occurs.…”

Section: Multiphoton Excitationmentioning

confidence: 99%

“…Both ZJU-28⊃MAPbBr 3 with average QD size of ≈9.5 and ≈11 nm show the slight redshift of the MEPL spectra with respect to single-photon counterpart, which can be ascribed to the reabsorption effect and size inhomogeneity. [21,22] In order to determine the MPACs of the single ZJU-28⊃MAPbBr 3 crystal, the multiphoton excited fluorescence reference method was used (see Supporting Information). [6,7,[23][24][25] We choose the MAPbBr 3 (up to five-photon) of MAPbBr 3 NCs have been investigated.…”

Section: Multiphoton Excitationmentioning

confidence: 99%

Confinement of Perovskite‐QDs within a Single MOF Crystal for Significantly Enhanced Multiphoton Excited Luminescence

et al. 2018

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and then generate a high-energy photon through radiation transitions from the excited state. Compared with single photon excited luminescence, MPE luminescence has the advantages of stronger spatial confinement, longer penetration depth, smaller biological damage, and less Rayleigh scattering, so the high-order MPE luminescence materials have great potential applications in bioimaging, 3D optical data storage, sensing, and so on, but basically have not been fulfilled yet, [1][2][3][4][5] mainly because of the big challenge and difficulty to realize high-order MPE luminescence. Even for those materials exhibiting such MPE luminescence, the five-photon excited luminescence phenomena can be only observed in the dispersed solutions of either organic chromophore molecules or core-shell halide perovskite semiconductor nanocrystals (MAPbBr 3 /(OA) 2 PbBr 4 ) in order to diminish the aggregation-caused quenching (ACQ) while still with quite low multiphoton action cross-sections (MPACs), or have poor stability without any encapsulation approaches (The MPAC (ησ n ) is the product of photoluminescence quantum yield (PLQY, η) and multiphoton absorption cross-section (σ n ), the parameter to evaluate the multiphoton excited luminescence brightness). [6,7] The deficiency of bulky high-order MPE luminescence solid single crystals with low excitation threshold have further limited the exploration and implementation of such MPE materials into miniaturization and device, and thus their practical applications.Some porous materials such as mesoporous silica and porous alumina have been utilized to confine dye molecules and perovskite nanoparticles and thus to diminish the ACQ and to develop the solid-state luminescence. [4,[8][9][10][11] The emergence of a new type of porous materials, metal-organic frameworks (MOFs), has provided the significant promise to provide much better confinement for the potentially luminescent dye molecules and perovskite nanoparticles because of their more tunable pores/cages and specific sites to introduce strong recognitions. Indeed, we have recently realized a three-photon excited emissive material ZJU-68⊃DMASM through an exact match of a dye molecule with the pores of the metal-organic framework although high-order MPE luminescence solid single The development of the photostable higher-order multiphoton-excited (MPE) upconversion single microcrystalline material is fundamentally and technologically important, but very challenging. Here, up to five-photon excited luminescence in a host-guest metal-organic framework (MOF) and perovskite quantum dot (QD) hybrid single crystal ZJU-28⊃MAPbBr 3 is shown via an in situ growth approach. Such a MOF strategy not only results in a high QD loading concentration, but also significantly diminishes the aggregationcaused quenching (ACQ) effect, provides effective surface passivation, and greatly reduces the contact of the QDs with the external bad atmosphere due to the confinement effect and protection of the framework. These advantages make the resulting ZJU-28⊃MAPb...

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“…Ru 2+ dendrimers and 2, 2′:6′,2′′-terpyridine (tpy) derivatives and their metal complexes have previously been found to show NLO properties. [ 41,71,73,[89][90][91] The NLO properties of tpy can be attributed to the three pyridine rings, which prefer a planar geometry to achieve maximum conjugation, which is helpful for the π-electron delocalization. Selection of metal ions is also very important for achieving metal coordination networks for their application as NLO materials.…”

Section: Nonlinear Optical Properties Of Terpyridine Ligands and Theimentioning

confidence: 99%

“…This motivated us to study the TPA properties of their self-assembled networks, and the 1D selfassembled polymers have also shown large TPA, which was solvent dependent. [ 89 ] It has been shown that alkylcarbazole as the donor and bis(styryl)benzene as a conjugation bridge in terpyridine-based compounds, which are the basis for the development of our 1D, 2D, and 3D supramolecular networks and 2D metallocycles, enhance TPA cross sections in both organic solvent and aqueous media. [ 71 ] Based on their large TPA cross section, these molecules have been tested for optical limiting materials.…”

Section: Nonlinear Optical Properties Of Terpyridine Ligands and Theimentioning

confidence: 99%

Self‐Assembly of Conjugated Units Using Metal‐Terpyridine Coordination

Gao

Rajwar

Grimsdale

2014

Macromol. Rapid Commun.

Self Cite

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Due to their inherently dynamic natures and fascinating photoluminescent/photoelectronic properties, coordination compounds of metal ions and conjugated terpyridine ligands have attracted considerable attention as functional materials for a variety of potential applications. In this feature article, a summary of recent work toward the development of one- (1D), two- (2D), and three-dimensional (3D) supramolecular polymers, networks, and metallomacrocycles based on zinc metal ion coordination of conjugated units bearing terpyridine ligands is presented, and it is shown how it fits within the overall framework of work in this field. Here, a sequential study from terpyridines as basic building blocks to their zinc-coordinated supramolecular 1D polymers, 2D macrocycles, and 2D and 3D networks is developed. These networks are compared with respect to their thermal stabilities, molecular organization, and linear and nonlinear optical properties. This work opens new prospects for the development of supramolecular chemistry of terpyridines and other transition metal ions, and also their application in future optoelectronic devices.

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Wavelength dependence of optical nonlinearity of terpyridine-based Zn(II)-coordinated rigid linear polymers

Cited by 18 publications

References 25 publications

Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals

Giant five-photon absorption from multidimensional core-shell halide perovskite colloidal nanocrystals

Confinement of Perovskite‐QDs within a Single MOF Crystal for Significantly Enhanced Multiphoton Excited Luminescence

Self‐Assembly of Conjugated Units Using Metal‐Terpyridine Coordination

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