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We investigate hot carrier propagation across graphene using an electrical nonlocal injection/detection method. The device consists of a monolayer graphene flake contacted by multiple metal leads. Using two remote leads for electrical heating, we generate a carrier temperature gradient that results in a measurable thermoelectric voltage VNL across the remaining (detector) leads. Due to the nonlocal character of the measurement, VNL is exclusively due to the Seebeck effect. Remarkably, a departure from the ordinary relationship between Joule power P and VNL, VNL ~ P, becomes readily apparent at low temperatures, representing a fingerprint of hot-carrier dominated thermoelectricity. By studying VNL as a function of bias, we directly determine the carrier temperature and the characteristic cooling length for hot-carrier propagation, which are key parameters for a variety of new applications that rely on hot-carrier transport.
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The broadband and ultrafast photoresponse of graphene has been extensively studied in recent years, although the photoexcited carrier dynamics is still far from being completely understood. Different experimental approaches imply either one of two fundamentally different scattering mechanisms for hot electrons. One is high-energy optical phonons, while the other is disorder-driven supercollisions with acoustic phonons. However, the concurrent relaxation via both optical and acoustic phonons has not been considered so far, hindering the interpretation of different experiments within a unified framework. Here we expand the optical phonon-mediated cooling model, to include electron scattering with the acoustic phonons. By assuming the enhancement of electron-acoustic phonon supercollisions from the localized defect at the photothermoelectric current-generating interface, we provide a broader perspective to the ultrafast photoresponse of graphene, highlighting the previously overlooked effect of the interface for cooling dynamics. We show that the transient photothermoelectric response, which has been attributed exclusively to supercollisions, can be successfully explained without rejecting the established optical phonon relaxation pathway, demonstrating that the two cooling mechanisms are not mutually exclusive but complement each other.
The diffusion of electron-hole pairs, which are excited in an intrinsic graphene by the ultrashort focused laser pulse in mid-IR or visible spectral region, is described for the cases of peak-like or spread over the passive region distributions of carriers. The spatio-temporal transient optical response on a high-frequency probe beam appears to be strongly dependent on the regime of diffusion and can be used for verification of the elasic relaxation mechanism. Sign flip of the differential transmission coefficient takes place due to interplay of the carrier-induced contribution and weak dynamic conductivity of undoped graphene.
In conventional light harvesting devices, the absorption of a single photon only excites one electron, which sets the standard limit of power-conversion efficiency, such as the Shockley-Queisser limit. In principle, generating and harnessing multiple carriers per absorbed photon can improve the efficiency and possibly overcome this limit. Here, we report the observation of multiple hot carrier collection in graphene-boron-nitride Moire superlattice structures. A record-high zero-bias photoresponsivity of 0.3 ampere per watt, equivalently, an external quantum efficiency exceeding 50 percent, is achieved utilizing graphene photo-Nernst effect, which demonstrates a collection of at least 5 carriers per absorbed photon. We reveal that this effect arises from the enhanced Nernst coefficient through Lifshtiz transition at low energy Van Hove singularities, which is an emergent phenomenon due to the formation of Moire minibands. Our observation points to a new means for extremely efficient and flexible optoelectronics based on van der Waals heterostructures.
We present a numerical study on the intraband optical conductivity of hot carriers at quasi-equilibria in photoexcited graphene based on the semiclassical Boltzmann transport equations (BTE) with the aim of understanding the effects of intrinsic optical phonon and extrinsic coulomb scattering caused by charged impurities at the graphene--substrate interface. Instead of using full-BTE solutions, we employ iterative solutions of the BTE and the comprehensive model for the temporal evolutions of hot-carrier temperature and hot-optical-phonon occupations to reduce computational costs. Undoped graphene exhibits large positive photoconductivity owing to the increase in thermally excited carriers and the reduction in charged impurity scattering. The frequency dependencies of the photoconductivity in undoped graphene having high concentrations of charged impurities significantly deviate from those observed in the simple Drude model, which can be attributed to temporally varying charged impurity scattering during terahertz (THz) probing in the hot-carrier cooling process. Heavily doped graphene exhibits small negative photoconductivity similar to that of the Drude model. In this case, charged impurity scattering is substantially suppressed by the carrier-screening effect, and the temperature dependencies of the Drude weight and optical phonon scattering governs the negative photoconductivity. In lightly doped graphene, the appearance of negative and positive photoconductivity depends on the frequency and the crossover from negative photoconductivity to positive emerges from increasing the charged impurity concentration. This indicates the change of the dominant scattering mechanism from optical phonons to charged impurities. Our approach provides a quantitative understanding of non-Drude behaviors and the temporal evolution of photoconductivity in graphene.
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.
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