arXiv subjects

Niek van Hulst

Publications and source records attributed to Niek van Hulst.

3 recordsLinked to original sources

arXiv2026

Operando multidimensional spectroscopy reveals A-site-dependent carrier cooling in perovskite solar cells

Understanding how photogenerated carriers dissipate excess energy in operating perovskite solar cells is essential for connecting ultrafast photophysics with photovoltaic function and provides design principles for engineering next-generation cell architectures. Here we use photocurrent-detected two-dimensional electronic spectroscopy (PC-2DES) to resolve energy-dependent carrier relaxation in fully encapsulated, functioning metal halide perovskite solar cells. By comparing devices with identical architecture but different absorber compositions - MAPbI3, mixed FAMA, and FAPbI3 - we directly follow the redistribution of photoexcited carriers from initially populated high-energy states toward lower-energy band-edge states. The multidimensional photocurrent response reveals a cascade-like intraband cooling process whose rate depends strongly on absorber composition, with the slowest relaxation in MA-based devices, intermediate behaviour in mixed-cation devices, and fastest relaxation in FA-based devices. A reduced kinetic model incorporating phonon-mediated intraband scattering, supplemented by a phenomenological many-body contribution, captures the main energy-dependent trends. These results establish action-detected multidimensional spectroscopy as a device-level probe of ultrafast energy dissipation and show that subtle changes in perovskite composition can substantially reshape the carrier relaxation pathways that precede charge extraction.

physics.chem-ph↗

arXiv2021

Hot-Carrier Cooling in High-Quality Graphene is Intrinsically Limited by Optical Phonons

Many promising optoelectronic devices, such as broadband photodetectors, nonlinear frequency converters, and building blocks for data communication systems, exploit photoexcited charge carriers in graphene. For these systems, it is essential to understand, and eventually control, the cooling dynamics of the photoinduced hot-carrier distribution. There is, however, still an active debate on the different mechanisms that contribute to hot-carrier cooling. In particular, the intrinsic cooling mechanism that ultimately limits the cooling dynamics remains an open question. Here, we address this question by studying two technologically relevant systems, consisting of high-quality graphene with a mobility >10,000 cm$^2$V$^{-1}$s$^{-1}$ and environments that do not efficiently take up electronic heat from graphene: WSe$_2$-encapsulated graphene and suspended graphene. We study the cooling dynamics of these two high-quality graphene systems using ultrafast pump-probe spectroscopy at room temperature. Cooling via disorder-assisted acoustic phonon scattering and out-of-plane heat transfer to the environment is relatively inefficient in these systems, predicting a cooling time of tens of picoseconds. However, we observe much faster cooling, on a timescale of a few picoseconds. We attribute this to an intrinsic cooling mechanism, where carriers in the hot-carrier distribution with enough kinetic energy emit optical phonons. During phonon emission, the electronic system continuously re-thermalizes, re-creating carriers with enough energy to emit optical phonons. We develop an analytical model that explains the observed dynamics, where cooling is eventually limited by optical-to-acoustic phonon coupling. These fundamental insights into the intrinsic cooling mechanism of hot carriers in graphene will play a key role in guiding the development of graphene-based optoelectronic devices.

cond-mat.mes-hall↗

arXiv2019

Statistical analysis of many single-molecule encounters reveals plasmonic resonance dependent nanoantenna-molecule interactions

The nanoscale interaction between single emitters and plasmonic structures is traditionally studied by relying on near-perfect, deterministic, nanoscale-control. This approach is ultra-low throughput thus rendering systematic studies difficult to impossible. Here, we show that super resolution microscopy in combination with data-driven statistical analysis allows studying near-field interactions of single molecules with resonant nanoantennas. We systematically tune the antennas' spectral resonances and show that emitters can be separated according to their coupling strength with said structures which ultimately allows the reconstruction of 2D interaction maps around individual nanoantennas.

physics.chem-ph↗