4.8 Article

In Situ SERS Monitoring of Photochemistry within a Nanojunction Reactor

期刊

NANO LETTERS
卷 13, 期 12, 页码 5985-5990

出版社

AMER CHEMICAL SOC
DOI: 10.1021/nl403164c

关键词

Cucurbiturils; gold nanoparticles; diaminostilbene; photoreaction; SERS

资金

  1. UK EPSRC [EP/F059396/1, EP/G060649/1 EP/F035535/1]
  2. ERC [240629]
  3. ERC LINASS [320503]
  4. [EP/H007024/1]
  5. EPSRC [EP/G060649/1, EP/F059396/1, EP/H007024/1, EP/F035535/1, EP/K028510/1] Funding Source: UKRI
  6. Engineering and Physical Sciences Research Council [EP/K028510/1, EP/G060649/1, EP/F035535/1, EP/F059396/1, EP/H007024/1] Funding Source: researchfish

向作者/读者索取更多资源

We demonstrate a powerful SERS-nanoreactor concept composed of self-assembled gold nanoparticles (AuNP) linked by the sub-nm macrocycle cucurbit[n]uril (CB[n]). The CB[n] functions simultaneously as a nanoscale reaction vessel, sequestering and templating a photoreaction within, and also as a powerful SERS-transducer through the large field enhancements generated within the nanojunctions that CB[n]s define. Through the enhanced Raman fingerprint, the real-time SERS-monitoring of a prototypical stilbene photoreaction is demonstrated. By choosing the appropriate CB[n] nanoreactor, selective photoisomerism or photodimerization is monitored in situ from within the AuNP-CB[n] nanogap.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Nanoscience & Nanotechnology

Accurate Transfer of Individual Nanoparticles onto Single Photonic Nanostructures

Javier Redolat, Maria Camarena-Perez, Amadeu Griol, Miroslavna Kovylina, Angelos Xomalis, Jeremy J. Baumberg, Alejandro Martinez, Elena Pinilla-Cienfuegos

Summary: Controlled integration of metallic nanoparticles onto photonic nanostructures enables the realization of complex devices for extreme light confinement and enhanced light-matter interaction. A methodology for precise transfer and positioning of individual nanoparticles onto different photonic nanostructures is presented, using soft lithography printing. Raman spectroscopy confirms enhanced light-matter interactions in the resulting nanophotonic devices.

ACS APPLIED MATERIALS & INTERFACES (2023)

Article Optics

Multimodal image and spectral feature learning for efficient analysis of water-suspended particles

Tomoko Takahashi, Zonghua Liu, Thangavel Thevar, Nicholas Burns, Dhugal Lindsay, John Watson, Sumeet Mahajan, Sato Yukioka, Shuhei Tanaka, Yukiko Nagai, Balair Thornton

Summary: Researchers have developed a method that combines morphological and chemical information to accurately identify different particle types using optical measurement techniques that don't require sample preparation. By using a combined holographic imaging and Raman spectroscopy setup, they collected data from six different types of marine particles suspended in a large volume of seawater. Unsupervised feature learning was performed on the images and spectral data, and the learned features were combined to achieve better clustering results compared to using only image or spectral features. This method can be used for long-term monitoring of ocean particles without the need for sample collection, and it can be applied to different types of sensor measurements without significant modifications.

OPTICS EXPRESS (2023)

Article Chemistry, Multidisciplinary

Tris(4-azidophenyl)methanol - a novel and multifunctional thiol protecting group

Xujun Qiu, Julian Brueckel, Christoph Zippel, Martin Nieger, Frank Biedermann, Stefan Braese

Summary: In this article, a multifunctionalisable aryl azide, tris(4-azidophenyl)methanol, is reported. It can be used as a protecting group for thiols in peptoid synthesis and can be cleaved under mild reaction conditions via a Staudinger reduction. Additionally, the easily accessible aryl azide can be functionalised through copper-catalysed cycloaddition reactions, offering more possibilities for materials chemistry applications.

RSC ADVANCES (2023)

Article Chemistry, Multidisciplinary

Single-Molecule Sizing through Nanocavity Confinement

Raphael P. B. Jacquat, Georg Krainer, Quentin A. E. Peter, Ali Nawaz Babar, Oliver Vanderpoorten, Catherine K. Xu, Timothy J. Welsh, Clemens F. Kaminski, Ulrich F. Keyser, Jeremy J. Baumberg, Tuomas P. J. Knowles

Summary: This paper presents an approach called nanocavity diffusional sizing (NDS) that relies on nanocavity confinement to measure the size of nanoscale particles and single biomolecules in solution. It uses particle residence times within nanofluidic cavities to determine their hydrodynamic radii. Experimental results show that the residence times scale linearly with the sizes of nanoscale colloids, protein aggregates, and single DNA oligonucleotides. NDS offers a new optofluidic approach for rapid and quantitative sizing of nanoscale particles with potential applications in nanobiotechnology, biophysics, and clinical diagnostics.

NANO LETTERS (2023)

Article Chemistry, Physical

Mapping Atomic-Scale Metal-Molecule Interactions: Salient Feature Extraction through Autoencoding of Vibrational Spectroscopy Data

Alex Poppe, Jack Griffiths, Shu Hu, Jeremy J. Baumberg, Margarita Osadchy, Stuart Gibson, Bart de Nijs

Summary: Atomic-scale features play crucial roles in metal-molecule interactions and have significant implications in various applications. However, studying these interactions is challenging due to the small size and transient nature of atomic-scale structures. In this study, we combine single-molecule surface-enhanced Raman spectroscopy with machine learning to extract spectra of perturbed molecules and investigate the formation dynamics of adatoms on metal surfaces. This approach provides unique insights into atomic-scale processes and helps us understand how metallic protrusions form and interact with nearby molecules. Our technique opens new possibilities for controlling metal-molecule interactions at an atomic level and contributes to rational heterogeneous catalyst design.

JOURNAL OF PHYSICAL CHEMISTRY LETTERS (2023)

Article Chemistry, Multidisciplinary

Responsive Nucleic Acid-Based Organosilica Nanoparticles

Pierre Picchetti, Stefano Volpi, Marianna Rossetti, Michael D. Dore, Tuan Trinh, Frank Biedermann, Martina Neri, Alessandro Bertucci, Alessandro Porchetta, Roberto Corradini, Hanadi Sleiman, Luisa De Cola

Summary: The development of smart nanoparticles with responsive features has expanded the applications of NP-based drugs, vaccines, and diagnostic tools. By combining nucleic acid interactions and sol-gel chemistry, researchers have successfully incorporated synthetic nucleic acids into organosilica nanoparticles, enabling them to respond to various biological, physical, and chemical inputs.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2023)

Article Chemistry, Multidisciplinary

Amplified Plasmonic Forces from DNA Origami-Scaffolded Single Dyes in Nanogaps

Sara Rocchetti, Alexander Ohmann, Rohit Chikkaraddy, Gyeongwon Kang, Ulrich F. Keyser, Jeremy J. Baumberg

Summary: Developing highly enhanced plasmonic nanocavities allows direct observation of light-matter interactions at the nanoscale. With DNA origami, precise nanopositioning of single-quantum emitters in ultranarrow plasmonic gaps enables detailed study of their modified light emission. By developing nanoparticle-on-mirror constructs with DNA nanostructures as reliable and customizable spacers for nanoparticle binding, it is revealed that the traditional understanding of Purcell-enhanced molecular dye emission is misleading, and the enhanced dipolar dye polarizability greatly amplifies optical forces acting on the facet Au atoms, causing their rapid destabilization. Different dyes exhibit emission spectra dominated by inelastic (Raman) scattering rather than fluorescence, challenging the conventional theories in the field of quantum optics using plasmonics.

NANO LETTERS (2023)

Article Optics

Single-molecule mid-infrared spectroscopy and detection through vibrationally assisted luminescence

Rohit Chikkaraddy, Rakesh Arul, Lukas A. Jakob, Jeremy J. Baumberg

Summary: This study proposes a method for detecting molecular vibrations in the mid-infrared range at room temperature. By assembling molecules into a plasmonic nanocavity resonant at both mid-infrared and visible wavelengths, and optically pumping them below the electronic absorption band, successful conversion of mid-infrared light and observation of enhanced visible luminescence were achieved.

NATURE PHOTONICS (2023)

Article Chemistry, Multidisciplinary

Kinetics of Light-Responsive CNT / PNIPAM Hydrogel Microactuators

Aoife Gregg, Michael De Volder, Jeremy J. Baumberg

Summary: Light-responsive microactuators composed of carbon nanotube and hydrogel composites exhibit efficient radiative heating capture and fast response time. The kinetics of these microactuators are limited by polymer diffusion. Additionally, these actuators have potential applications as microswimmers.
Article Chemistry, Multidisciplinary

SERS Sensing of Dopamine with Fe(III)-Sensitized Nanogaps in Recleanable AuNP Monolayer Films

Marika Niihori, Tamas Foeldes, Charlie A. Readman, Rakesh Arul, David-Benjamin Grys, Bart de Nijs, Edina Rosta, Jeremy J. Baumberg

Summary: This study demonstrates the sensing of neurotransmitters at nm concentrations using self-assembled monolayers of plasmonic Au nanoparticles. By integrating Fe(III) sensitizers into nanogaps, enhanced surface-enhanced Raman spectroscopy is achieved for dopamine sensing. The transparent glass substrates allow for repeated sensing in different analytes.
Article Chemistry, Multidisciplinary

Controlling Atomic-Scale Restructuring and Cleaning of Gold Nanogap Multilayers for Surface-Enhanced Raman Scattering Sensing

David-Benjamin Grys, Marika Niihori, Rakesh Arul, Sarah May Sibug-Torres, Elle W. Wyatt, Bart de Nijs, Jeremy J. Baumberg

Summary: We demonstrate reliable creation of multiple layers of Au nanoparticles in random close-packed arrays with sub-nm gaps as a sensitive surface-enhanced Raman scattering substrate. The nanogaps can be precisely controlled below 1 nm by removing and replacing the original molecules with scaffolding ligands using oxygen plasma etching. The resulting high-performance fluidic sensing cells allow cyclic cleaning and reusing of the films for various analytes.

ACS SENSORS (2023)

Article Optics

Multi-wavelength lock-in spectroscopy for extracting perturbed spectral responses: molecular signatures in nanocavities

Angelos Xomalis, Jeremy J. Baumberg

Summary: In this article, a multichannel lock-in vibrational spectroscopy method is reported, which utilizes acousto-optic modulators to convert nanosecond periodic temporal perturbations into spatially distinct spectra. By projecting the perturbed and reference spectra onto different locations of the spectrometer image, they can be simultaneously resolved. This multichannel time-resolved technique is applied to detect molecular frequency upconversion in plasmonic nanocavities through perturbed Raman scattering at different wavelengths. The phase-sensitive detection scheme can be applied to any spectroscopy within the visible and near-infrared wavelength ranges.

OPTICS EXPRESS (2023)

Article Nanoscience & Nanotechnology

Plasmonic Sensing Assay for Long-Term Monitoring (PSALM) of Neurotransmitters in Urine

Wei-Hsin Chen, Wenting Wang, Qianqi Lin, David-Benjamin Grys, Marika Niihori, Junyang Huang, Shu Hu, Bart de Nijs, Oren A. Scherman, Jeremy J. Baumberg

Summary: A liquid-based surface-enhanced Raman spectroscopy assay, called PSALM, has been developed for the selective detection of neurotransmitters (NTs) in urine with a detection limit below the physiological range. This assay involves quick and simple mix-and-measure protocols with nanoparticles (NPs), where Fe-III bridges NTs and gold NPs in sensing hotspots. The optimized PSALM allows long-term monitoring of NT variation in urine, enabling the development of NTs as predictive or correlative biomarkers for clinical diagnosis.

ACS NANOSCIENCE AU (2023)

Article Biochemistry & Molecular Biology

Binding affinity-based intracellular drug detection enabled by a unimolecular cucurbit[7]uril-dye conjugate

Yanxi Liu, Changming Hu, Julian A. Serna, Frank Biedermann, Pavel A. Levkin

Summary: Label-free fluorescence-based chemosensing offers simplicity and high sensitivity for intracellular monitoring of molecules. However, conventional indicator displacement assays (IDAs) have limitations. In this study, a covalently coupled CB7-NBD conjugate was used to overcome these limitations and demonstrated to respond to various target analytes in complex live cell systems.

RSC CHEMICAL BIOLOGY (2023)

Article Chemistry, Multidisciplinary

The temperature-dependence of host-guest binding thermodynamics: experimental and simulation studies

Laura M. Grimm, Jeffry Setiadi, Boryslav Tkachenko, Peter R. Schreiner, Michael K. Gilson, Frank Biedermann

Summary: The thermodynamic parameters of host-guest binding can be used to describe, understand, and predict molecular recognition events in aqueous systems. This study focuses on the contributions of water to binding by studying binding thermodynamics for a series of host-guest systems. It is found that the enthalpic driving forces for binding increase at higher temperatures, and heat capacity changes appear to be a general feature of host-guest complex formation in water.

CHEMICAL SCIENCE (2023)

暂无数据