Periodic Reporting for period 2 - 2D-Liquid (2D material interactions with liquids probed with nanoscopy tools)
Periodo di rendicontazione: 2023-04-01 al 2024-09-30
This project explores the reactivity mechanisms of 2D materials with aqueous electrolytes under ambient conditions, focusing on solid-liquid interactions and their implications for nanoscale ion transport. The challenge lies in understanding how pristine and defective surfaces of 2D materials influence interactions with liquids, which is crucial for practical applications. The project bridges the gap between Nanofluidics and advanced optical methods. Understanding the interactions between 2D materials and liquids is vital for developing advanced technologies in nanofluidics, biosensing, energy harvesting, molecular separation, and other nanoscale applications. Enhanced knowledge of 2D material reactivity can lead to better industrial applications in electronics, water purification, transportation, pollution control, and health, ultimately improving quality of life and driving technological innovation. Utilize a myriad of nanoscopy techniques to study interactions between 2D materials and liquids, leveraging either engineered defects or naturally occurring ones.
The main aim of the project was to focus on the characterization of Defects in 2D Materials: Explore defects in hexagonal boron nitride (h-BN) and transition metal dichalcogenides (TMDs). Through the project, we introduced various defects into native hBN using different methods. We employed focused ion beam irradiation to create defects and also used neutron irradiation, among other techniques, to control defect density and study their effects. In addition, we explored the interaction of the surface with various types of solvents and compared their behaviour under strong confinement. We used existing nanofluidic platforms and innovated new ones, such as mechano-ionic switches. Characterization and observations were often supplemented with in-operando microscopy. For the project, we developed or adapted several forefront nanoscopy methods, such as single-molecule localization microscopy (SMLM), single-particle tracking (SPT), PAINT, and scanning ion conductance microscopy (SICM), to study the dynamics of interfacial charges.
The project aims to establish super-resolution microscopy as a routine technique for characterizing solid-liquid interactions across different environments. Success will depend on scaling up methodologies and simplifying imaging and analysis processes, potentially transforming industrial applications and advancing the field of nanofluidics and 2D material technologies.
The main aim of the project was to focus on the characterization of Defects in 2D Materials: Explore defects in hexagonal boron nitride (h-BN) and transition metal dichalcogenides (TMDs). Through the project, we introduced various defects into native hBN using different methods. We employed focused ion beam irradiation to create defects and also used neutron irradiation, among other techniques, to control defect density and study their effects. In addition, we explored the interaction of the surface with various types of solvents and compared their behaviour under strong confinement. We used existing nanofluidic platforms and innovated new ones, such as mechano-ionic switches. Characterization and observations were often supplemented with in-operando microscopy. For the project, we developed or adapted several forefront nanoscopy methods, such as single-molecule localization microscopy (SMLM), single-particle tracking (SPT), PAINT, and scanning ion conductance microscopy (SICM), to study the dynamics of interfacial charges.
The project aims to establish super-resolution microscopy as a routine technique for characterizing solid-liquid interactions across different environments. Success will depend on scaling up methodologies and simplifying imaging and analysis processes, potentially transforming industrial applications and advancing the field of nanofluidics and 2D material technologies.
During the project period, we achieved several significant milestones that greatly impacted our research. Firstly, we successfully established five fully functional experimental setups, either constructed by our team members, including PhD students, postdocs, and the principal investigator, or acquired from Bruker/JPK. Secondly, we assembled a talented team through the hiring process. The project's aim was to develop new tools to reveal the interfacial dynamics of water, ions, and molecules in nanofluidics platforms. We identified a significant knowledge gap due to the lack of appropriate tools to study these dynamics. To address this, we constructed dedicated experimental setups that combine nanoscale conductance measurements and electrochemistry with optical imaging at the nanoscale. These setups include super-resolution localization microscopy, which enhances spatial, spectral, and temporal resolution, as well as setups that allow us to infer the orientation of molecules (3D polarization setup) and perform wide-field lifetime measurements.
To improve the temporal resolution of single-molecule imaging and tracking, we explored the use of SPAD arrays for fluorescence microscopy, focusing on challenging single-molecule imaging. SPAD cameras enable high-speed imaging of fast-moving emitters, which we applied to single proteins on lipid membranes and 2D crystals of hexagonal boron nitride. Single-molecule imaging was achievable in both cases, with photon arrival sub-information at 10-100 µs resolution, enriching trajectory analysis possibilities. Additionally, we investigated the time-resolved capabilities of SPAD cameras for lifetime measurements of fluorescent emitters on a wide-field basis. This resulted in a new high-throughput method, normally achieved by scanning one molecule at a time on a confocal microscope. Our method could enhance techniques like STORM and PAINT used in single-molecule localization microscopy by adding lifetime information, potentially leading to improved imaging of multiple targets simultaneously and better detection of environmental changes at the super-resolution level.
Conventional SMLM only contains information about the position of the emitter, but features such as its wavelength, polarization, and lifetime are also essential for a complete depiction of the profile. The process of stimulated emission is a consequence of the uneven distribution of charge within a molecule. As a result, the polarization of the emitted fluorescent photon depends on the molecule's orientation. Within this project, we constructed a 3D polarization SMLM imaging platform that allows us to investigate the three-dimensional orientations of these molecules.
1. Nathan Ronceray, et.al Nature Materials 22, no. 10 (2023): 1236-1242.
The paper has been disseminated at the following conferences by Nathan Ronceray (NR) and Aleksandra Radenovic (AR): SMLMS 2023, Vienna (NR); SMLMS 2022, Paris (NR); Heraeus-Seminar on "Defects in Two-dimensional Materials, Bad Honnef (AR); Cambridge 2D TMD 2023, Cambridge (AR); BoronNitrideWorkshop 2023, Montpellier (AR, NR);
2. 2. Emmerich, Theo et al. Nature Electronics (2024): 1-8.
The paper has been disseminated at the following conferences by AR, NR, and Theo Emmerich (TE) Nanofluidics conference, Lenzerheide (AR, NR); Nanofluidics 23 in physics and biology, Lyon (AR); Dubrovnik - Solid State to BioPhysics X, Cavtat, Dubrovnik (AR, NR, TE).
To improve the temporal resolution of single-molecule imaging and tracking, we explored the use of SPAD arrays for fluorescence microscopy, focusing on challenging single-molecule imaging. SPAD cameras enable high-speed imaging of fast-moving emitters, which we applied to single proteins on lipid membranes and 2D crystals of hexagonal boron nitride. Single-molecule imaging was achievable in both cases, with photon arrival sub-information at 10-100 µs resolution, enriching trajectory analysis possibilities. Additionally, we investigated the time-resolved capabilities of SPAD cameras for lifetime measurements of fluorescent emitters on a wide-field basis. This resulted in a new high-throughput method, normally achieved by scanning one molecule at a time on a confocal microscope. Our method could enhance techniques like STORM and PAINT used in single-molecule localization microscopy by adding lifetime information, potentially leading to improved imaging of multiple targets simultaneously and better detection of environmental changes at the super-resolution level.
Conventional SMLM only contains information about the position of the emitter, but features such as its wavelength, polarization, and lifetime are also essential for a complete depiction of the profile. The process of stimulated emission is a consequence of the uneven distribution of charge within a molecule. As a result, the polarization of the emitted fluorescent photon depends on the molecule's orientation. Within this project, we constructed a 3D polarization SMLM imaging platform that allows us to investigate the three-dimensional orientations of these molecules.
1. Nathan Ronceray, et.al Nature Materials 22, no. 10 (2023): 1236-1242.
The paper has been disseminated at the following conferences by Nathan Ronceray (NR) and Aleksandra Radenovic (AR): SMLMS 2023, Vienna (NR); SMLMS 2022, Paris (NR); Heraeus-Seminar on "Defects in Two-dimensional Materials, Bad Honnef (AR); Cambridge 2D TMD 2023, Cambridge (AR); BoronNitrideWorkshop 2023, Montpellier (AR, NR);
2. 2. Emmerich, Theo et al. Nature Electronics (2024): 1-8.
The paper has been disseminated at the following conferences by AR, NR, and Theo Emmerich (TE) Nanofluidics conference, Lenzerheide (AR, NR); Nanofluidics 23 in physics and biology, Lyon (AR); Dubrovnik - Solid State to BioPhysics X, Cavtat, Dubrovnik (AR, NR, TE).
We achieved two major milestones as planned. First, we successfully monitored the dynamics of emitters confined to nanoslits using the single-particle tracking (SPT) approach. These results confirm that the dipolar environment can influence emitter properties. The angstrom-scale nanoslit geometry provides strong confinement, enclosing fewer than 100 molecules in the case of acetonitrile. Beyond passive diffusion and dielectric sensing of confined liquids, tracking emitter dynamics in confinement allows for direct imaging of nanoscale flow and the study of its interaction with defects. The second is unexpected discovery of mechano-ionic nanofluidics with a memristive signature was significant. Similar phenomena were observed later in the gating of porins. The project's major contribution is the insight that operando microscopy can reveal intricate mechanisms behind observed behaviours..
Solid-state neuromorphic chips have already shown they can reduce the power consumption of specific tasks tenfold. Our approach, utilizing ion transport in water through artificial ion channels, offers a biomimetic route to overcoming these
Solid-state neuromorphic chips have already shown they can reduce the power consumption of specific tasks tenfold. Our approach, utilizing ion transport in water through artificial ion channels, offers a biomimetic route to overcoming these