arXiv subjects

Niek F. van Hulst

Publications and source records attributed to Niek F. van Hulst.

15 recordsLinked to original sources

arXiv2024

Ultra-broadband Optical Diffraction Tomography

Optical diffraction tomography (ODT) is a powerful non-invasive 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, a crucial information that is difficult to assess with existing methodologies. We present broadband, spectrally resolved ODT images of HeLa cells, obtained via pulse-shaping based Fourier transform spectroscopy. The spectral observations enabled by ultrabroadband ODT, combined with material-dependent refractive index responses, allow for precise three-dimensional identification of the nanoparticles within cellular structures. Our work represents a crucial step towards time and spectrally-resolved tomography of complex 3D structures with implications for life and materials science applications.

physics.optics↗

arXiv2022

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. This corresponds to an effective pump-probe time delay of 13 ns, determined by the repetition rate of our laser system (76 MHz). This pre-time-zero technique enables probing the diffusion of long-lived excitations created by previous pump pulses with nanometer accuracy, and is particularly powerful for following in-plane heat diffusion in thin films. In contrast to existing techniques for quantifying thermal transport it does not require any material input parameters or strong heating. We demonstrate the direct determination of the thermal diffusivities of the layered materials MoSe$_2$ (0.18 cm$^2$/s), WSe$_2$ (0.20 cm$^2$/s), MoS$_2$ (0.35 cm$^2$/s), and WS$_2$ (0.59 cm$^2$/s). This technique paves the way for observing novel nanoscale thermal transport phenomena and tracking diffusion of a broad range of species.

cond-mat.mes-hall↗

arXiv2021

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. We then demonstrate the capability of UHT microscopy to holographically localize in 3D single particles over large volumes of view. Ultimately, we combine the two concepts to simultaneously track several tens of freely diffusing gold nanoparticles, within a 110x110x110 $μ$m volume of view at an integration time of 10 ms per frame, while simultaneously recording their phototransient signals. The combined experimental concepts outlined and validated in this work lay the foundation for background-free 3D single-particle tracking applications or spectroscopy in scattering environments and are immediately applicable to systems as diverse as live cells and tissues or supported heterogeneous catalysts.

physics.optics↗

arXiv2021

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 sub-wavelength assembly of many individual nano-building-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. Here, we address this shortcoming and measure the quantitative scattering phase of different nanomaterials such as gold nanorods and spheres as well as dielectric nanoparticles. Beyond reporting spectrally resolved responses, with phase-changes close to pi when passing the particles' plasmon resonance, we devise a simple method for distinguishing different plasmonic and dielectric particles purely based on their phase behavior. Finally, we integrate this novel approach in a single-shot two-color scheme, capable of directly identifying different types of nanoparticles on one sample, from a single widefield image.

physics.optics↗

arXiv2020

Observation of giant and tuneable thermal diffusivity of Dirac fluid at room temperature

Conducting materials typically exhibit either diffusive or ballistic charge transport. However, when electron-electron interactions dominate, a hydrodynamic regime with viscous charge flow emerges (1-13). More stringent conditions eventually yield a quantum-critical Dirac-fluid regime, where electronic heat can flow more efficiently than charge (14-22). Here we observe heat transport in graphene in the diffusive and hydrodynamic regimes, and report a controllable transition to the Dirac-fluid regime at room temperature, using carrier temperature and carrier density as control knobs. We introduce the technique of spatiotemporal thermoelectric microscopy with femtosecond temporal and nanometre spatial resolution, which allows for tracking electronic heat spreading. In the diffusive regime, we find a thermal diffusivity of $\sim$2,000 cm$^2$/s, consistent with charge transport. Remarkably, during the hydrodynamic time window before momentum relaxation, we observe heat spreading corresponding to a giant diffusivity up to 70,000 cm$^2$/Vs, indicative of a Dirac fluid. These results are promising for applications such as nanoscale thermal management.

cond-mat.mes-hall↗

arXiv2020

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. This unfavorable scaling makes it extremely difficult to quantitatively characterize intrinsically heterogeneous clinical samples, such as extracellular vesicles, as their signal variation easily exceeds the dynamic range of currently available cameras. Here, we introduce off-axis k-space holography that circumvents this limitation. By imaging the back-focal-plane of our microscope we project the scattering signal of all particles onto all camera pixels thus dramatically boosting the achievable dynamic range to up-to 110 dB. We validate our platform by detecting, and quantitatively sizing, metallic and dielectric particles over a 200x200 $μ$m field-of-view and demonstrate that independently performed signal calibrations allow correctly sizing particles made from different materials. Finally, we present quantitative size-distributions of extracellular vesicle samples.

physics.optics↗

arXiv2018

Tracking ultrafast hot-electron diffusion in space and time by ultrafast thermo-modulation microscopy

The ultrafast response of metals to light is governed by intriguing non-equilibrium dynamics involving the interplay of excited electrons and phonons. The coupling between them gives rise to nonlinear diffusion behavior on ultrashort timescales. Here, we use scanning ultrafast thermo-modulation microscopy to image the spatio-temporal hot-electron diffusion in a thin gold film. By tracking local transient reflectivity with 20 nm and 0.25 ps resolution, we reveal two distinct diffusion regimes, consisting of an initial rapid diffusion during the first few picoseconds after optical excitation, followed by about 100-fold slower diffusion at longer times. We simulate the thermo-optical response of the gold film with a comprehensive three-dimensional model, and identify the two regimes as hot-electron and phonon-limited thermal diffusion, respectively.

physics.optics↗

arXiv2018

On the theory of excitonic delocalization for robust vibronic dynamics in LH2

Nonlinear spectroscopy has revealed long-lasting oscillations in the optical response of a variety of photosynthetic complexes. Different theoretical models which involve the coherent coupling of electronic (excitonic) or electronic-vibrational (vibronic) degrees of freedom have been put forward to explain these observations. The ensuing debate concerning the relevance of either one or the other mechanism may have obscured their potential synergy. To illustrate this synergy, we quantify how the excitonic delocalization in the LH2 unit of Rhodopseudomonas Acidophila purple bacterium, leads to correlations of excitonic energy fluctuations, relevant coherent vibronic coupling and, importantly, a decrease in the excitonic dephasing rates. Combining these effects, we identify a feasible origin for the long-lasting oscillations observed in fluorescent traces from time-delayed two-pulse single molecule experiments performed on this photosynthetic complex.

q-bio.BM↗

arXiv2017

Room-temperature ultrafast non-linear spectroscopy of a single molecule

Single molecule spectroscopy aims at unveiling often hidden but potentially very important contributions of single entities to a system's ensemble response. Albeit contributing tremendously to our ever growing understanding of molecular processes the fundamental question of temporal evolution, or change, has thus far been inaccessible, resulting in a static picture of a dynamic world. Here, we finally resolve this dilemma by performing the first ultrafast time-resolved transient spectroscopy on a single molecule. By tracing the femtosecond evolution of excited electronic state spectra of single molecules over hundreds of nanometres of bandwidth at room temperature we reveal their non-linear ultrafast response in an effective 3-pulse scheme with fluorescence detection. A first excitation pulse is followed by a phase-locked de-excitation pulse-pair, providing spectral encoding with 25 fs temporal resolution. This experimental realisation of true single molecule transient spectroscopy demonstrates that two-dimensional electronic spectroscopy of single molecules is experimentally in reach.

physics.chem-ph↗

arXiv2015

Generation of photovoltage in graphene on a femtosecond time scale through efficient carrier heating

Graphene is a promising material for ultrafast and broadband photodetection. Earlier studies addressed the general operation of graphene-based photo-thermoelectric devices, and the switching speed, which is limited by the charge carrier cooling time, on the order of picoseconds. However, the generation of the photovoltage could occur at a much faster time scale, as it is associated with the carrier heating time. Here, we measure the photovoltage generation time and find it to be faster than 50 femtoseconds. As a proof-of-principle application of this ultrafast photodetector, we use graphene to directly measure, electrically, the pulse duration of a sub-50 femtosecond laser pulse. The observation that carrier heating is ultrafast suggests that energy from absorbed photons can be efficiently transferred to carrier heat. To study this, we examine the spectral response and find a constant spectral responsivity between 500 and 1500 nm. This is consistent with efficient electron heating. These results are promising for ultrafast femtosecond and broadband photodetector applications.

cond-mat.mes-hall↗

arXiv2014

Non-Reciprocal Optical Antennas

Plasmonics aims to interface photonics and electronics. Finding optical, near-field analogues of much used electro-technical components is crucial to the success of such a platform. Here we present the plasmonic analogue of a non-reciprocal antenna. For non-reciprocality in a plasmonic context, the optical excitation and emission resonances of the antenna need to be an orthogonal set. We show that nonlinear excitation of metal nanoantennas creates a sufficient shift between excitation and emission wavelengths that they can be interpreted as decoupled, allowing for independent tuning of excitation and emission properties along different spatial dimensions. This leads, for given excitation wavelength and polarization, to independent optimization of emission intensity, frequency spectrum, polarization and angular spectrum. Non-reciprocal optical antennas of both gold and aluminum are characterized and shown to be useful as e.g. nonlinear signal transducers or nanoscale sources of widely tunable light.

physics.optics↗

arXiv2013

Second harmonic nano-particles for femtosecond coherent control on the nanoscale

We provide a complete toolkit for coherent control experiments on the nano-scale. By exploiting the second harmonic emission from single (150 nm) nonlinear nano-particles, we show that ultrafast femtosecond laser pulses can be compressed and controlled in time with unprecedented spatial accuracy. The method is tested on various nano-particles of different sizes, shapes and materials, both dielectric BaTiO3, Fe(IO3)3) and metallic (Au) thus demonstrating its robustness and versatility.

physics.optics↗

arXiv2012

Plasmonic Antennas as Design Elements for Coherent Ultrafast Nanophotonics

Coherent broadband excitation of plasmons brings ultrafast photonics to the nanoscale. However, to fully leverage this potential for ultrafast nanophotonic applications, the capacity to engineer and control the ultrafast response of a plasmonic system at will is crucial. Here, we develop a framework for systematic control and measurement of ultrafast dynamics of near-field hotspots. We show deterministic design of the coherent response of plasmonic antennas at femtosecond timescales. Exploiting the emerging properties of coupled antenna configurations, we use the calibrated antennas to engineer two sought-after applications of ultrafast plasmonics: a subwavelength resolution phase shaper, and an ultrafast hotspot switch. Moreover, we demonstrate that mixing localized resonances of lossy plasmonic particles is the mechanism behind nanoscale coherent control. This simple, reproducible and scalable approach promises to transform ultrafast plasmonics into a straightforward tool for use in fields as diverse as room temperature quantum optics, nanoscale solid state physics and quantum biology.

physics.optics↗

arXiv2010

Femtosecond Coherence and Quantum Control of Single Molecules at Room Temperature

Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing interest in the possibility of organic quantum computing. Since biological systems are intrinsically heterogeneous, clear relations between structural and quantum-mechanical properties can only be obtained by investigating individual assemblies. However, single-molecule techniques to access ultrafast coherences at physiological conditions were not available so far. Here we show by employing femtosecond pulse-shaping techniques that quantum coherences in single organic molecules can be created, probed, and manipulated at ambient conditions even in highly disordered solid environments. We find broadly distributed coherence decay times for different individual molecules giving direct insight into the structural heterogeneity of the local surroundings. Most importantly, we induce Rabi-oscillations and control the coherent superposition state in a single molecule, thus performing a basic femtosecond single-qubit operation at room temperature.

quant-ph↗

arXiv2009

Nanorod optical antennas for dipolar transitions

Optical antennas link objects to light. Here, we analyze metal nanorod antennas as cavities with variable reflection coefficients to derive the interaction of dipolar transitions with radiation through the antenna modes. The presented analytical model accurately describes the complete emission process, and is summarized in a phase-matching equation. We show how antenna modes evolve as they become increasingly more bound, i.e. plasmonic. The results illustrate why efficient antennas should not be too plasmonic, and how subradiant even modes can evolve into weakly-interacting dark modes. Our description is valid for the interaction of nanorods with light in general, and is thus widely applicable.

physics.optics↗