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Klaas-Jan Tielrooij

Publications and source records attributed to Klaas-Jan Tielrooij.

At least 19 recordsLinked to original sources

Graphene-enabled coherent (sub-)terahertz wave detection and thickness determination

Phase-sensitive terahertz (THz) detection enables applications ranging from astronomy to non-destructive testing. However, current THz detectors lack phase sensitivity, unless they are combined with external interferometers, or through photomixing. This implies a large footprint and sensitive dependence on alignment. Here, we demonstrate a graphene-enabled, on-chip, integrated (sub-)THz detector-interferometer with optical cavity and antenna, exhibiting high sensitivity to the phase of incident THz light. We exploit this by determining the thickness of thin films placed in front of the detector-interferometer, obtaining a deep sub-wavelength thickness accuracy of a few micrometer, while we predict that an improved accuracy is within reach. This is relevant for a range of industrial application domains, including automotive, construction, and health. We furthermore achieve a record-high external responsivity - considering bias-free graphene-based (sub-)THz detectors - of 172 mA/W and a noise-equivalent power of 26 pW$~\rm{Hz}^{-1/2}$. This performance is due to enhanced absorption at the resonant cavity mode around 89 GHz, in agreement with multi-physics simulations. These results pave the way to exploiting coherent wave detection in the (sub-)THz regime with utility in spectroscopy, next-generation wireless communication, and beyond.

physics.optics↗

Direct spatiotemporal imaging of carriers reveals a long-lived bulk photovoltaic mechanism

The bulk photovoltaic effect (BPVE), a manifestation of broken centrosymmetry, has attracted interest as a probe of the symmetry and quantum geometry of materials, and for use in photovoltaic and optoelectronic devices. However, so far the effect has not been captured directly in space and time. Here, we use contactless pump-probe microscopy to visualize the spatiotemporal evolution of photoexcited carriers in single-crystal, mono-domain $BiFeO_{3}$, a prototypical ferroelectric material. We observe asymmetric carrier transport along the polar axis, which confirms the intrinsic bulk- and symmetry-driven nature of the BPVE. Remarkably, this asymmetric transport persists for several nanoseconds after photoexcitation, which cannot be explained by conventional short-lived shift or phonon ballistic current BPVE mechanisms. Our Monte Carlo simulations show that asymmetric momentum scattering by defects, such as oxygen vacancies, leads to long-lived asymmetric carrier transport, as observed experimentally. Beyond fundamental insights, this paves the way towards controlling symmetry- and defect-driven photoresponses.

cond-mat.mtrl-sci↗

C-band 160 Gbs-1 Zero-bias Graphene Photodetectors: Breaking the Responsivity-Bandwidth Trade-off by Heterostructure Engineering

Graphene photodetectors offer ultrafast response and broadband operation, but their responsivity is typically limited by rapid hot-carrier cooling, leading to a trade-off between sensitivity and speed. Here, we demonstrate that modifying the dielectric environment provides an effective route to control hot-carrier cooling and enhance device performance. By employing a WSe2 encapsulation architecture, we suppress out-of-plane energy dissipation, leading to an increased cooling length (~2.68 um) and a reduced heat-exchange coefficient. As a result, we obtain zero-bias graphene photodetectors with responsivities up to ~0.12 A/W (potentially ~0.4 A/W) while maintaining ultrafast operation beyond the setup-limited 110 GHz bandwidth. The devices enable direct detection at data rates of 120 Gb s-1 (NRZ) and 160 Gb s-1 (PAM-4), with performance achieved using minimal digital signal processing. These results establish dielectric engineering as a key design axis for controlling hot-carrier dynamics, enabling energy-efficient, high-speed optical receivers for next-generation interconnects and AI-driven data systems.

physics.optics↗

Graphene-based Photodetector with Engineered Hot Carrier Cooling Dynamics

Graphene has emerged as a promising material for integration into silicon photonics, owing to its ultrafast and broadband photoresponse without the need for an external bias voltage. This photoresponse relies on the photo-thermoelectric effect created by hot carriers. A key factor underlying the performance of graphene photodetectors is the cooling dynamics of these hot carriers. In this work, we engineer these dynamics in a WSe2-graphene-WSe2 waveguide-integrated photodetector. In particular, by introducing proximity screening by a nearby graphite layer to this structure, we prolong the hot-carrier cooling time, leading to an enhanced photoresponse. We characterize the cooling dynamics under continuous-wave laser excitation by employing a photomixing technique, revealing an increase in the cooling time by up to a factor of four. Direct photoresponse measurements show that the internal photoresponsivity improves by approximately 50%. Together, these results demonstrate the potential of proximity screening to enhance the performance of graphene-based photodetectors on an integrated photonics platform.

cond-mat.mes-hall↗

Suppressing Plasmonic Heating in Aqueous Environments with Hexagonal Boron Nitride

Optical heating of plasmonic nanostructures is a critical challenge in nanoscale systems. Although plasmonic effects enable enhanced optical functionalities, the associated temperature rise can degrade performance in heat-sensitive applications such as biosensing, nanophotonics, and microelectronics. Conventional cooling strategies fail at these scales due to limited heat transport and high interfacial thermal resistance, motivating the integration of advanced materials for thermal management. Here, we investigate hexagonal boron nitride (hBN) thin flakes as heat spreaders to mitigate plasmonic heating of gold nanospheres immobilized on hBN deposited on glass and surrounded by water. Using finite-element simulations, we quantify the influence of hBN thickness, in-plane thermal conductivity, and interfacial thermal conductance on cooling efficiency. Complementary experiments employ cross-grating wavefront microscopy (CGM) for nanothermometry to map the temperature around optically heated gold nanoparticles and quantify the cooling effect of hBN. We extend the application of CGM for rapid, non-invasive, and all-optical characterization of non-absorbing 2D materials. Our results reveal a strong thickness dependence, where heat dissipation in thin flakes is limited by the heat capacity of hBN and in thick flakes by interfacial thermal conductance. Including hBN, we obtain a reduction in temperature rise by up to 60% compared to glass. In addition, the presence of two main heat dissipation pathways emerges: a direct one from the nanoparticle to the hBN and an indirect one from the particle via water to the hBN. This combined simulation-experiment framework offers a versatile approach to improve thermal management in plasmonic systems and beyond, establishing design guidelines for integrating 2D materials into thermally sensitive platforms such as biosensors and integrated circuits.

physics.optics↗

Electrical tunability of terahertz nonlinearity in graphene

Graphene is conceivably the most nonlinear optoelectronic material. Its nonlinear optical coefficients in the terahertz (THz) frequency range surpass those of other materials by many orders of magnitude. This, in particular, allows one to use graphene for extremely efficient up-conversion of sub-THz electronic input signals into the THz frequency range at room temperature and under ambient conditions, thus paving the way for practical graphene-based ultrahigh-frequency electronic technology. Here, we show that the THz nonlinearity of graphene can be efficiently controlled using electrical gating, with gating voltages as low as a few volts. For example, optimal electrical gating enhances the power conversion efficiency in THz third-harmonic generation in graphene by about two orders of magnitude. This essentially converts graphene from an almost perfectly linear, inert electronic material to a material with the highest possible THz nonlinearity. We demonstrate gating control of THz nonlinearity of graphene for both ultrashort single-cycle and quasi-monochromatic multi-cycle input signals. Our experimental results are in quantitative agreement with a physical model of graphene nonlinearity, describing the time-dependent thermodynamic balance maintained within the electronic population of graphene during interaction with ultrafast electric fields. Our results can serve as a basis for straightforward and accurate design of devices and applications for efficient electronic signal processing in graphene at ultra-high frequencies.

cond-mat.mes-hall↗

Dielectric control of ultrafast carrier dynamics and transport in graphene

Understanding the ultrafast dynamics of photoexcited charges in graphene is essential, as the microscopic mechanisms underlying these dynamics determine many of graphene's optical, optothermal, and optoelectronic properties. These are crucial properties for many functionalities and devices enabled by graphene, such as high-speed photodectors. Therefore, beyond scientific understanding, it is highly desirable to control ultrafast carrier dynamics for practical applications. Here, we establish this control by engineering the dielectric environment of graphene, thereby regulating both heating and cooling dynamics without altering the Fermi energy, optical power, or ambient temperature. By combining optical pump-terahertz probe experiments with theoretical calculations, we show that dielectric screening suppresses carrier-carrier interactions and slows the dynamics. In particular, reduced carrier-carrier scattering delays the formation of a quasi-equilibrium hot electron distribution, thus slowing carrier heating. It also slows carrier cooling because re-thermalization after optical-phonon emission depends on the same interactions. The enhanced screening further reduces the energy of electron-hole puddles, thereby increasing charge mobility and the Seebeck coefficient. This ability to externally control internal graphene dynamics and transport properties enables the optimization of device performance, such as the sensitivity of photodetectors for data communication and wireless communication applications.

cond-mat.mes-hall↗

Photonics in Flatland: Challenges and Opportunities for Nanophotonics with 2D Semiconductors

Two-dimensional (2D) semiconductors are emerging as a versatile platform for nanophotonics, offering unprecedented tunability in optical properties through exciton resonance engineering, van der Waals heterostructuring, and external field control. These materials enable active optical modulation, single-photon emission, quantum photonics, and valleytronic functionalities, paving the way for next-generation optoelectronic and quantum photonic devices. However, key challenges remain in achieving large-area integration, maintaining excitonic coherence, and optimizing amplitude-phase modulation for efficient light manipulation. Advances in fabrication, strain engineering, and computational modelling will be crucial to overcoming these limitations. This perspective highlights recent progress in 2D semiconductor-based nanophotonics, emphasizing opportunities for scalable integration into photonics.

physics.optics↗

High-Speed Graphene-based Sub-Terahertz Receivers enabling Wireless Communications for 6G and Beyond

In recent years, the telecommunications field has experienced an unparalleled proliferation of wireless data traffic. Innovative solutions are imperative to circumvent the inherent limitations of the current technology, in particular in terms of capacity. Carrier frequencies in the sub-terahertz (sub-THz) range (~0.2-0.3 THz) can deliver increased capacity and low attenuation for short-range wireless applications. Here, we demonstrate a direct, passive and compact sub-THz receiver based on graphene, which outperforms state-of-the-art sub-THz receivers. These graphene-based receivers offer a cost-effective, CMOS-compatible, small-footprint solution that can fulfill the size, weight, and power consumption (SWaP) requirements of 6G technologies. We exploit a sub-THz cavity, comprising an antenna and a back mirror, placed in the vicinity of the graphene channel to overcome the low inherent absorption in graphene and the mismatch between the areas of the photoactive region and the incident radiation, which becomes extreme in the sub-THz range. The graphene receivers achieve a multigigabit per second data rate with a maximum distance of ~3 m from the transmitter, a setup-limited 3 dB bandwidth of 40 GHz, and a high responsivity of 0.16 A/W, enabling applications such as chip-to-chip communication and close proximity device-to-device communication.

physics.optics↗

Electron cooling in graphene enhanced by plasmon-hydron resonance

Evidence is accumulating for the crucial role of a solid's free electrons in the dynamics of solid-liquid interfaces. Liquids induce electronic polarization and drive electric currents as they flow; electronic excitations, in turn, participate in hydrodynamic friction. Yet, the underlying solid-liquid interactions have been lacking a direct experimental probe. Here, we study the energy transfer across liquid-graphene interfaces using ultrafast spectroscopy. The graphene electrons are heated up quasi-instantaneously by a visible excitation pulse, and the time evolution of the electronic temperature is then monitored with a terahertz pulse. We observe that water accelerates the cooling of the graphene electrons, whereas other polar liquids leave the cooling dynamics largely unaffected. A quantum theory of solid-liquid heat transfer accounts for the water-specific cooling enhancement through a resonance between the graphene surface plasmon mode and the so-called hydrons -- water charge fluctuations --, particularly the water libration modes, that allows for efficient energy transfer. Our results provide direct experimental evidence of a solid-liquid interaction mediated by collective modes and support the theoretically proposed mechanism for quantum friction. They further reveal a particularly large thermal boundary conductance for the water-graphene interface and suggest strategies for enhancing the thermal conductivity in graphene-based nanostructures.

cond-mat.mes-hall↗

Ultrafast Umklapp-assisted electron-phonon cooling in magic-angle twisted bilayer graphene

Carrier relaxation measurements in moiré materials offer a unique probe of the microscopic interactions, in particular the ones that are not easily measured by transport. Umklapp scattering between phonons is a ubiquitous momentum-nonconserving process that governs the thermal conductivity of semiconductors and insulators. In contrast, Umklapp scattering between electrons and phonons has not been demonstrated experimentally. Here, we study the cooling of hot electrons in moiré graphene using time- and frequency-resolved photovoltage measurements as a direct probe of its complex energy pathways including electron-phonon coupling. We report on a dramatic speedup in hot carrier cooling of twisted bilayer graphene near the magic angle: the cooling time is a few picoseconds from room temperature down to 5 K, whereas in pristine graphene coupling to acoustic phonons takes nanoseconds. Our analysis indicates that this ultrafast cooling is a combined effect of the formation of a superlattice with low-energy moiré phonons, spatially compressed electronic Wannier orbitals, and a reduced superlattice Brillouin zone, enabling Umklapp scattering that overcomes electron-phonon momentum mismatch. These results demonstrate a way to engineer electron-phonon coupling in twistronic systems, an approach that could contribute to the fundamental understanding of their transport properties and enable applications in thermal management and ultrafast photodetection.

cond-mat.mes-hall↗

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↗

Milliwatt terahertz harmonic generation from topological insulator metamaterials

Achieving efficient, high-power harmonic generation in the terahertz spectral domain has technological applications, for example in sixth generation (6G) communication networks. Massless Dirac fermions possess extremely large terahertz nonlinear susceptibilities and harmonic conversion efficiencies. However, the observed maximum generated harmonic power is limited, because of saturation effects at increasing incident powers, as shown recently for graphene. Here, we demonstrate room-temperature terahertz harmonic generation in a Bi$_2$Se$_3$ topological insulator and topological-insulator-grating metamaterial structures with surface-selective terahertz field enhancement. We obtain a third-harmonic power approaching the milliwatt range for an incident power of 75 mW - an improvement by two orders of magnitude compared to a benchmarked graphene sample. We establish a framework in which this exceptional performance is the result of thermodynamic harmonic generation by the massless topological surface states, benefiting from ultrafast dissipation of electronic heat via surface-bulk Coulomb interactions. These results are an important step towards on-chip terahertz (opto)electronic applications.

physics.optics↗

Ultrafast electronic heat dissipation through surface-to-bulk Coulomb coupling in quantum materials

The timescale of electronic cooling is an important parameter controlling the performance of devices based on quantum materials for optoelectronic, thermoelectric and thermal management applications. In most conventional materials, cooling proceeds via the emission of phonons, a relatively slow process that can bottleneck the carrier relaxation dynamics, thus degrading the device performance. Here we present the theory of near-field radiative heat transfer, that occurs when a two-dimensional electron system is coupled via the non-retarded Coulomb interaction to a three-dimensional bulk that can behave as a very efficient electronic heat sink. We apply our theory to study the cooling dynamics of surface states of three dimensional topological insulators, and of graphene in proximity to small-gap bulk materials. The ``Coulomb cooling'' we introduce is alternative to the conventional phonon-mediated cooling, can be very efficient and dominate the cooling dynamics under certain circumstances. We show that this cooling mechanism can lead to a sub-picosecond time scale, significantly faster than the cooling dynamics normally observed in Dirac materials.

cond-mat.mes-hall↗

Electrically tuneable nonequilibrium optical response of graphene

The ability to tune the optical response of a material via electrostatic gating is crucial for optoelectronic applications, such as electro-optic modulators, saturable absorbers, optical limiters, photodetectors and transparent electrodes. The band structure of single layer graphene (SLG), with zero-gap, linearly dispersive conduction and valence bands, enables an easy control of the Fermi energy E$_F$ and of the threshold for interband optical absorption. Here, we report the tunability of the SLG non-equilibrium optical response in the near-infrared (1000-1700nm/0.729-1.240eV), exploring a range of E$_F$ from -650 to 250 meV by ionic liquid gating. As E$_F$ increases from the Dirac point to the threshold for Pauli blocking of interband absorption, we observe a slow-down of the photobleaching relaxation dynamics, which we attribute to the quenching of optical phonon emission from photoexcited charge carriers. For E$_F$ exceeding the Pauli blocking threshold, photobleaching eventually turns into photoinduced absorption, due to hot electrons' excitation increasing SLG absorption. The ability to control both recovery time and sign of nonequilibrium optical response by electrostatic gating makes SLG ideal for tunable saturable absorbers with controlled dynamics.

cond-mat.mtrl-sci↗

Hot carriers in graphene -- fundamentals and applications

Hot charge carriers in graphene exhibit fascinating physical phenomena, whose understanding has improved greatly over the past decade. They have distinctly different physical properties compared to, for example, hot carriers in conventional metals. This is predominantly the result of graphene's linear energy-momentum dispersion, its phonon properties, its all-interface character, and the tunability of its carrier density down to very small values, and from electron- to hole-doping. Since a few years, we have witnessed an increasing interest in technological applications enabled by hot carriers in graphene. Of particular interest are optical and optoelectronic applications, where hot carriers are used to detect (photodetection), convert (nonlinear photonics), or emit (luminescence) light. Graphene-enabled systems in these application areas could find widespread use and have a disruptive impact, for example in the field of data communication, high-frequency electronics, and industrial quality control. The aim of this review is to provide an overview of the most relevant physics and working principles that are relevant for applications exploiting hot carriers in graphene.

cond-mat.mes-hall↗

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↗

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↗