Full Control of Plasmonic Nanocavities Using Gold Decahedra‐on‐Mirror Constructs with Monodisperse Facets

Hu, Shu; Elliott, Eoin; Sánchez‐Iglesias, Ana; Huang, Junyang; Guo, Chenyang; Hou, Yidong; Kamp, Marlous; Goerlitzer, Eric S. A.; Bedingfield, Kalun; Nijs, Bart de; Peng, Jialong; Demetriadou, Angela; Liz‐Marzán, Luis M.; Baumberg, Jeremy J.

doi:10.1002/advs.202207178

Cited by 12 publications

(12 citation statements)

References 48 publications

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“…The Ag NCs are coated with a protective shell of approximately 3 nm poly(vinylpyrrolidone) (PVP) (Figure e). The ultra-flatness of the Au film and the uniformity of the plasmonic particles are critical because the optical properties of this plasmonic cavity are highly dependent on nanometer- or even angstrom-scale variations of the substrate, particle size, and gap spacing. , The PEs layer, composed of poly(allylamine hydrochloride) (PAH) and polystyrene sulfonate, was assembled layer by layer (Figure S1), acting as an accurate dielectric spacer which separates the Ag NCs from the Au film while situating the probe molecules within the SPR hotspot. The classic photosensitizer, rose bengal (RB), was chosen as the research molecule because it contains both singlet state fluorescence and triplet state phosphorescence (Figures c and S2).…”

Section: Resultsmentioning

confidence: 99%

Tailoring Fluorescence–Phosphorescence Emission with a Single Nanocavity

Peng,

Wang,

et al. 2023

J. Am. Chem. Soc.

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Realizing the dual emission of fluorescence−phosphorescence in a single system is an extremely important topic in the fields of biological imaging, sensing, and information encryption. However, the phosphorescence process is usually in an inherently "dark state" at room temperature due to the involvement of spin-forbidden transition and the rapid non-radiative decay rate of the triplet state. In this work, we achieved luminescent harvesting of the dark phosphorescence processes by coupling singlet-triplet molecular emitters with a rationally designed plasmonic cavity. The achieved Purcell enhancement effect of over 1000-fold allows for overcoming the triplet forbidden transitions, enabling radiation enhancement with selectable emission wavelengths. Spectral results and theoretical simulations indicate that the fluorescence−phosphorescence peak position can be intelligently tailored in a broad range of wavelengths, from visible to near-infrared. Our study sheds new light on plasmonic tailoring of molecular emission behavior, which is crucial for advancing research on plasmon-tailored fluorescence−phosphorescence spectroscopy in optoelectronics and biomedicine.

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Section: Resultsmentioning

confidence: 99%

Tailoring Fluorescence–Phosphorescence Emission with a Single Nanocavity

Peng,

Wang,

et al. 2023

J. Am. Chem. Soc.

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“…A smoother PMMA interface may be obtained from employing a different solvent used for similar coatings. 65,66 The coating with a PMMA film did not disturb the positions of the individual NP in the arrays, as evidenced by the persistence of SLRs with similar quality compared to reference measurements using only indexmatching oils. 62,64 The large area covered by the AuNP array allows us to measure the samples in a commercial CD spectrometer (Jasco J-815a) under normal illumination with a simple, custom-built sample holder (Figure S3).…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…All substrate films were covered with immersion oil and a cover slide (Figures S2 and S3) to match the refractive index (RI), and thus, we effectively excite SLRs. − The homogeneous RI environment also prevents scattering, so that the surface roughness of the PMMA film does not compromise the optical properties. A smoother PMMA interface may be obtained from employing a different solvent used for similar coatings. , The coating with a PMMA film did not disturb the positions of the individual NP in the arrays, as evidenced by the persistence of SLRs with similar quality compared to reference measurements using only index-matching oils. , …”

Section: Results and Discussionmentioning

confidence: 99%

Molecular-Induced Chirality Transfer to Plasmonic Lattice Modes

et al. 2023

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Molecular chirality plays fundamental roles in biology. The chiral response of a molecule occurs at a specific spectral position, determined by its molecular structure. This fingerprint can be transferred to other spectral regions via the interaction with localized surface plasmon resonances of gold nanoparticles. Here, we demonstrate that molecular chirality transfer occurs also for plasmonic lattice modes, providing a very effective and tunable means to control chirality. We use colloidal self-assembly to fabricate non-close packed, periodic arrays of achiral gold nanoparticles, which are embedded in a polymer film containing chiral molecules. In the presence of the chiral molecules, the surface lattice resonances (SLRs) become optically active, i.e., showing handedness-dependent excitation. Numerical simulations with varying lattice parameters show circular dichroism peaks shifting along with the spectral positions of the lattice modes, corroborating the chirality transfer to these collective modes. A semi-analytical model based on the coupling of singlemolecular and plasmonic resonances rationalizes this chirality transfer.

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“…To tackle the challenges associated with controlling particle crystal facets and to deepen our understanding of light coupling, Professor Jeremy J. Baumberg's research group developed a nano-cavity based on Au nanodecahedra. 67 Utilizing an automated particle tracking system, they investigated over 20 000 individual nano-cavities, systematically comparing the scattering spectra and SERS enhancement capabilities of NPoM nanocavities and nanodecahedron-on-mirror (NDoM) nanocavities.…”

Section: Applications In Dark-field Scattering Spectroscopy and Plasm...mentioning

confidence: 99%