Ultrabroadband Optical Diffraction Tomography.

Optical diffraction tomography (ODT) is a powerful noninvasive 3D imaging technique, but its combination with broadband light sources is difficult. In this study, we introduce ultrabroadband ODT, covering over 150 nm of visible spectral bandwidth with a lateral spatial resolution of 150 nm. Our work addresses a critical experimental gap by enabling the measurement of broadband refractive index changes in 3D samples, crucial information that is difficult to assess with existing methodologies.

Photoelectrochemical Two-Dimensional Electronic Spectroscopy (PEC2DES) of Photosystem I: Charge Separation Dynamics Hidden in a Multichromophoric Landscape.

We present a nonlinear spectroelectrochemical technique to investigate photosynthetic protein complexes. The PEC2DES setup combines photoelectrochemical detection (PEC) that selectively probes the protein photogenerated charges output with two-dimensional electronic spectroscopy (2DES) excitation that spreads the nonlinear optical response of the system in an excitation-detection map. PEC allows us to distinguish the contribution of charge separation (CS) from other de-excitation pathways, whereas 2DES allows us to disentangle congested spectral bands and evaluate the exciton dynamics (decays and coherences) of the photosystem complex.

Fisher information for smart sampling in time-domain spectroscopy.

Time-domain spectroscopy encompasses a wide range of techniques, such as Fourier-transform infrared, pump-probe, Fourier-transform Raman, and two-dimensional electronic spectroscopies. These methods enable various applications, such as molecule characterization, excited state dynamics studies, or spectral classification. Typically, these techniques rarely use sampling schemes that exploit the prior knowledge scientists typically have before the actual experiment.

Structured Excitation Energy Transfer: Tracking Exciton Diffusion below Sunlight Intensity.

With the increasing demand for new materials for light-harvesting applications, spatiotemporal microscopy techniques are receiving increasing attention as they allow direct observation of the nanoscale diffusion of excitons. However, the use of pulsed and tightly focused laser beams generates light intensities far above those expected under sunlight illumination, leading to photodamage and nonlinear effects that seriously limit the accuracy and applicability of these techniques, especially in biological or atomically thin materials. In this work, we present a novel spatiotemporal microscopy technique that exploits structured excitation in order to dramatically decrease the excitation intensity, up to 10,000-fold when compared with previously reported spatiotemporal photoluminescence microscopy experiments.

Nonlinear Optical Spectroscopy of Molecular Assemblies: What Is Gained and Lost in Action Detection?

This study elucidates the information content that is extracted from action-2D electronic spectroscopy (A-2DES) when the output intensity is not proportional to the number of excitations generated. Such a scenario can be realized in both fluorescence and photocurrent detection because of interaction like exciton-exciton annihilation or effects in the signal generation or detection. By means of an intuitive probabilistic model supported by nonlinear response theory, the study concludes that in molecular assemblies the ground-state bleaching contribution can dominate the nonlinear signal and partially or completely hide the stimulated emission.

A pre-time-zero spatiotemporal microscopy technique for the ultrasensitive determination of the thermal diffusivity of thin films.

Diffusion is one of the most ubiquitous transport phenomena in nature. Experimentally, it can be tracked by following point spreading in space and time. Here, we introduce a spatiotemporal pump-probe microscopy technique that exploits the residual spatial temperature profile obtained through the transient reflectivity when probe pulses arrive before pump pulses.

What is special about Y6; the working mechanism of neat Y6 organic solar cells.

Non-fullerene acceptors (NFAs) have delivered advancement in bulk heterojunction organic solar cell efficiencies, with a significant milestone of 20% now in sight. However, these materials challenge the accepted wisdom of how organic solar cells work. In this work we present a neat Y6 device with an efficiency above 4.

Spatiotemporal Mapping Uncouples Exciton Diffusion from Singlet-Singlet Annihilation in the Electron Acceptor Y6.

Understanding the spatial dynamics of nanoscale exciton transport beyond the temporal decay is essential for further improvements of nanostructured optoelectronic devices, such as solar cells. The diffusion coefficient () of the nonfullerene electron acceptor Y6 has so far only been determined indirectly, from singlet-singlet annihilation (SSA) experiments. Here, we present the full picture of the exciton dynamics, adding the spatial domain to the temporal one, by spatiotemporally resolved photoluminescence microscopy.

Simultaneous Sizing and Refractive Index Analysis of Heterogeneous Nanoparticle Suspensions.

Rapid and reliable characterization of heterogeneous nanoparticle suspensions is a key technology across the nanosciences. Although approaches exist for homogeneous samples, they are often unsuitable for polydisperse suspensions, as particles of different sizes and compositions can lead to indistinguishable signals at the detector. Here, we introduce holographic nanoparticle tracking analysis, holoNTA, as a straightforward methodology that decouples size and material refractive index contributions.

Direct Modular Printing of Plasmonic Chemosensors.

Here, we present and implement a new approach for producing modular inkjet-printable surface-enhanced Raman scattering (SERS) chemosensors. These sensors, combined with a rapid large field-of-view imaging system allow for fast imaging of the chemical characteristics of a sample. The performance of these materials is illustrated by printing a pH sensor on paper and interrogating aqueous solutions at different pH values.

Widefield SERS for High-Throughput Nanoparticle Screening.

Surface-enhanced Raman scattering (SERS) imaging is a powerful technology with unprecedent potential for ultrasensitive chemical analysis. Point-by-point scanning and often excessively long spectral acquisition-times hamper the broad exploitation of the full analytical potential of SERS. Here, we introduce large-scale SERS particle screening (LSSPS), a multiplexed widefield screening approach to particle characterization, which is 500-1000 times faster than typical confocal Raman implementations.

Widefield phototransient imaging for visualizing 3D motion of resonant particles in scattering environments.

Identifying, visualising and ultimately tracking dynamically moving non-fluorescent nanoparticles in the presence of non-specific scattering is a long-standing challenge across the nano- and life-sciences. In this work we demonstrate that our recently developed ultrafast holographic transient (UHT) microscope is ideally suited for meeting this challenge. We show that UHT microscopy allows reliably distinguishing off-resonant, dielectric, from resonant, metallic, nanoparticles, based on the phototransient signal: a pre-requisite for single-particle tracking in scattering environments.

Unraveling Heat Transport and Dissipation in Suspended MoSe from Bulk to Monolayer.

Understanding heat flow in layered transition metal dichalcogenide (TMD) crystals is crucial for applications exploiting these materials. Despite significant efforts, several basic thermal transport properties of TMDs are currently not well understood, in particular how transport is affected by material thickness and the material's environment. This combined experimental-theoretical study establishes a unifying physical picture of the intrinsic lattice thermal conductivity of the representative TMD MoSe .

Observation of giant and tunable thermal diffusivity of a Dirac fluid at room temperature.

Conducting materials typically exhibit either diffusive or ballistic charge transport. When electron-electron interactions dominate, a hydrodynamic regime with viscous charge flow emerges. More stringent conditions eventually yield a quantum-critical Dirac-fluid regime, where electronic heat can flow more efficiently than charge.

One-Shot Phase Image Distinction of Plasmonic and Dielectric Nanoparticles.

Nanoscale phase control is one of the most powerful approaches to specifically tailor electrical fields in modern nanophotonics. Especially the precise subwavelength assembly of many individual nanobuilding blocks has given rise to exciting new materials as diverse as metamaterials, for miniaturizing optics, or 3D assembled plasmonic structures for biosensing applications. Despite its fundamental importance, the phase response of individual nanostructures is experimentally extremely challenging to visualize.

Photocurrent-Detected 2D Electronic Spectroscopy Reveals Ultrafast Hole Transfer in Operating PM6/Y6 Organic Solar Cells.

The performance of nonfullerene-acceptor-(NFA)-based organic solar cells is rapidly approaching the efficiency of inorganic cells. The chemical versatility of NFAs extends the light-harvesting range to the infrared, while preserving a considerably high open-circuit-voltage, crucial to achieve power-conversion efficiencies >17%. Such low voltage losses in the charge separation process have been attributed to a low-driving-force and efficient exciton dissociation.

Fast Photo-Chrono-Amperometry of Photosynthetic Complexes for Biosensors and Electron Transport Studies.

Photosynthetic reactions in plants, algae, and cyanobacteria are driven by photosystem I and photosystem II complexes, which specifically reduce or oxidize partner redox biomolecules. Photosynthetic complexes can also bind synthetic organic molecules, which inhibit their photoactivity and can be used both to study the electron transport chain and as herbicides and algicides. Thus, their development, characterization, and sensing bears fundamental and applied interest.

Ultrafast Transient Holographic Microscopy.

Nanotechnology is increasingly being applied in many emerging technologies, ranging from metamaterials to next-generation nanodrugs. A key ingredient for its success is the ability to specifically tailor ultrafast nanoscale light-matter interactions over very large areas. Unfortunately, dynamic imaging by ultrafast nanoscopy so far remains limited to very small 2D areas.

Precise Nanosizing with High Dynamic Range Holography.

Optical sensing is one of the key enablers of modern diagnostics. Especially label-free imaging modalities hold great promise as they eliminate labeling procedures prior to analysis. However, scattering signals of nanometric particles scale with their volume square.

3D tracking of extracellular vesicles by holographic fluorescence imaging.

Fluorescence microscopy is the method of choice in biology for its molecular specificity and super-resolution capabilities. However, it is limited to a narrow range around one observation plane. Here, we report an imaging approach that recovers the full electric field of fluorescent light with single-molecule sensitivity.

Surface-enhanced Raman scattering holography.

Nanometric probes based on surface-enhanced Raman scattering (SERS) are promising candidates for all-optical environmental, biological and technological sensing applications with intrinsic quantitative molecular specificity. However, the effectiveness of SERS probes depends on a delicate trade-off between particle size, stability and brightness that has so far hindered their wide application in SERS imaging methodologies. In this Article, we introduce holographic Raman microscopy, which allows single-shot three-dimensional single-particle localization.

Cold and Hot Spots: From Inhibition to Enhancement by Nanoscale Phase Tuning of Optical Nanoantennas.

Optical nanoantennas are well-known for the confinement of light into nanoscale hot spots, suitable for emission enhancement and sensing applications. Here, we show how control of the antenna dimensions allows tuning the local optical phase, hence turning a hot spot into a cold spot. We manipulate the local intensity exploiting the interference between driving and scattered field.

Control of Vibronic Transition Rates by Resonant Single-Molecule-Nanoantenna Coupling.

Plasmonic nanostructures dramatically alter the radiative and nonradiative properties of single molecules in their vicinity. This coupling-induced change in decay channels selectively enhances specific vibronic transitions, which can enable plasmonic control of molecular reactivity. Here, we report coupling-dependent spectral emission shaping of single Rhodamine 800 molecules in the vicinity of plasmonic gold nanorods.

Room-Temperature Excitation-Emission Spectra of Single LH2 Complexes Show Remarkably Little Variation.

Excitation spectroscopy gives direct insight into the excited state manifold, energy transfer, transient intermediates, vibrations, and so on. Unfortunately, excitation spectroscopy of single molecules under ambient conditions has remained challenging. Here we present excitation spectra alongside emission spectra of the same individual light-harvesting complex LH2 of the purple bacteria .

Nanoscale Imaging and Control of Hexagonal Boron Nitride Single Photon Emitters by a Resonant Nanoantenna.

Defect centers in two-dimensional hexagonal boron nitride (hBN) are drawing attention as single-photon emitters with high photostability at room temperature. With their ultrahigh photon-stability, hBN single-photon emitters are promising for new applications in quantum technologies and for 2D-material based optoelectronics. Here, we control the emission rate of hBN-defects by coupling to resonant plasmonic nanocavities.