二维材料弹道输运与载流子扩散测量（非电学）顶刊

We report spatiotemporal observations of room-temperature quasi-ballistic electron transport in graphene, which is achieved by utilizing a four-layer van der Waals heterostructure to generate free charge carriers. The heterostructure is formed by sandwiching a MoS2 and MoSe2 heterobilayer between two graphene monolayers. Transient absorption measurements reveal that the electrons and holes separated by the type-II interface between MoS2 and MoSe2 can transfer to the two graphene layers, respectively. Transient absorption microscopy measurements, with high spatial and temporal resolution, reveal that while the holes in one graphene layer undergo a classical diffusion process with a large diffusion coefficient of 65 cm2 s-1 and a charge mobility of 5000 cm2 V-1 s-1, the electrons in the other graphene layer exhibit a quasi-ballistic transport feature, with a ballistic transport time of 20 ps and a speed of 22 km s-1, respectively. The different in-plane transport properties confirm that electrons and holes move independently of each other as charge carriers. The optical generation of ballistic charge carriers suggests potential applications for such van der Waals heterostructures as optoelectronic materials.

ConspectusUnderstanding charge transfer (CT) between two chemical entities and the subsequent change in their charge densities is essential not only for molecular species but also for various low-dimensional materials. Because of their extremely high fraction of surface atoms, two-dimensional (2-D) materials are most susceptible to charge exchange and exhibit drastically different physicochemical properties depending on their charge density. In this regard, spontaneous and uncontrollable ionization of graphene in the ambient air has caused much confusion and technical difficulty in achieving experimental reproducibility since its first report in 2004. Moreover, the same ambient hole doping was soon observed in 2-D semiconductors, which implied that a common mechanism should be operative and apply to other low-dimensional materials universally. Notably, a similar CT reaction has long been known for carbon nanotubes but is still controversial in its mechanism.In this Account, we review our breakthroughs in unraveling the chemical origin and mechanistic requirements of the hidden CT reactions using 2-D crystals. As a first step, we have developed in situ optical methods to quantify charge density using Raman and photoluminescence (PL) spectroscopy and imaging. To overcome the multimodal sensitivity of Raman frequencies, we established a novel analytical method based on theory and experiments with excellent resolution for the charge density (∼1 × 1012 cm-2) and lattice strain (∼0.02%) of graphene. For 2-D transition-metal dichalcogenides, PL spectroscopy and imaging provided a high precision and sensitivity that enabled rapid kinetic measurements in a spatially resolved manner.Using gas- and temperature-controlled in situ measurements, we revealed that the electrical holes are injected by the oxygen reduction reaction (ORR) O2 + 4H+ + 4e- ⇄ 2H2O, which was independently verified by the pH dependence in HCl solutions. In addition to oxygen and water vapor, the overall CT reaction requires hydrophilic dielectric substrates, which assist the hydration of the sample-substrate interface. We also found that the CT reaction is substantially enhanced when samples are thermally annealed. The amplification is due to the interfacial hydrophilicity increased by the thermal hydroxylation of substrates, which indicates that the CT reaction is localized at the interface and boosted by interfacial water.The interface-localized CT allowed us to study and control molecular diffusion through the 2-D van der Waals space between samples and substrates. Wide-field PL imaging showed how fast oxygen molecules diffuse through the interfacial space, subsequently inducing the CT reaction. By increasing the 2-D gap spacing, the diffusion kinetics could be accelerated. The rate of CT could also be enhanced by introducing defects on the basal plane of 2-D crystals, which demonstrates the decisive role of defects as CT centers.Because of their unique geometry, low-dimensional materials are highly susceptible to external perturbation including charge exchange. Because the vulnerability can be exploited to modify material properties, the complete mechanism of the fundamental charge exchange summarized in this Account will be essential to exploring material and device properties of other low-dimensional materials.

Interlayer carrier transfer at heterointerfaces plays a critical role in light to electricity conversion using organic and nanostructured materials. However, how interlayer carrier extraction at these interfaces is poorly understood, especially in organic-inorganic heterogeneous systems. Here, we provide a direct strategy for manipulating the interlayer carrier diffusion process, transfer rate and extraction efficiency in tetracene/MoS 2 type-II band alignment heterostructure by constructing the 2D–3D organic-inorganic (O-I) system. As a result, the prolonged diffusion length (12.32 nm), enhanced electron transfer rate (9.53 × 10 9  s −1 ) and improved carrier extraction efficiency (60.9%) are obtained in the 2D O-I structure which may be due to the more sufficient charge transfer (CT) state generation. In addition, we have demonstrated that the interlayer carrier transfer behavior complied with the diffusion mechanism based on the one-dimensional diffusion model. The diffusion coefficients have varied from 0.0027 to 0.0036 cm 2  s −1 as the organic layer changes from 3D to 2D structures. Apart from the relationship between the carrier injection and diffusion process, temperature-dependent time-resolved spectra measurement is used to reveal the trap-related recombination that may limit the interlayer carrier extraction. The controllable interlayer carrier transfer behavior enables O-I heterojunction to be optimized for optoelectronic applications.

… Two-dimensional (2D) atomic materials such as graphene and transition metal … in semiconductor materials with higher energies compared with the Fermi energy are called hot …

This review briefly covers several typical topics of ultrafast carrier dynamics in two-dimensional transition metal dichalcogenides (TMDs) such as many-body effects, ultrafast nonradiative recombination, intervalley transfer of carriers, high-energy C exciton cooling, and carrier dynamics in TMD-based heterostructures.

… thin PtSe 2 , a new rising two-dimensional material in electronics and optoelectronics. We … the carrier diffusion dynamics. Interestingly, the observed spatial width of the optical response …

A contact-free optical technique is developed to enable a spatially resolved measurement of minority carrier diffusion length and the associated mobility-lifetime (μτ) product in bulk semiconductor materials. A scanning electron microscope is used in combination with an internal optical microscope and imaging charge-coupled device (CCD) to image the bulk luminescence from minority carrier recombination associated with one-dimensional excess carrier generation. Using a Green's function to model steady-state minority carrier diffusion in a three-dimensional half space, non-linear least squares analysis is then applied to extract values of carrier diffusion length and surface recombination velocity. The approach enables measurement of spatial variations in the μτ product with a high degree of spatial resolution.

… So far, studies on two-dimensional materials have mainly focused on crystalline materials. … black phosphorus, as the first two-dimensional amorphous material. Spatially and temporally …

In layered two-dimensional (2D) perovskites, the inorganic perovskite layers sandwiched between cation spacers create quantum well (QW) structures, showing large exciton binding energies that hinder the efficient dissociation of excitons into free carriers. This leads to poor carrier transport properties and low-performance light-conversion-based devices, and the direct understanding of the underlying physics, particularly concerning surface states, remains extremely difficult, if not impossible, due to the challenges in real-time accessibility. Here, we utilized four-dimensional scanning ultrafast electron microscopy (4D-SUEM), a highly sensitive technique for mapping surface carrier diffusion that diverges from those in the bulk and substantially affects material properties. We directly visualize photo-generated carrier transport over both spatial and temporal dimensions on the top surface of 2D perovskites with varying inorganic perovskite layer thicknesses (n = 1, 2, and 3). The results reveal the photo-induced surface carrier diffusion rates of ~30 cm2·s-1 for n = 1, ~180 cm2·s-1 for n = 2, and ~470 cm2·s-1 for n = 3, which are over 20 times larger than bulk. This is because charge carrier transmission channels have much wider distributions on the top surface compared to the bulk, as supported by the Density Functional Theory (DFT) calculations. Finally, our findings represent the demonstration to directly correlate the discrepancies between surface and bulk carrier diffusion behaviors, their relationship with exciton binding energy, and the number of layers in 2D perovskites, providing valuable insights into enhancing the performance of 2D perovskite-based optoelectronic devices through interface engineering. Using 4D-SUEM, we revealed photo-induced surface carrier diffusion in 2D perovskites, with rates far exceeding bulk values, driven by broader carrier transmission channels, highlighting the crucial role of surface dynamics.

… two-dimensional (2D) CuInSe 2 nanosheets and the studies of ultrafast carrier dynamics and transport in this 2D material. … transient optical reflectivity, obtained from femtosecond optical …

The diffusion length of photogenerated carriers is a crucial parameter in semiconductors for optoelectronic applications. However, it is a challenging task to determine the diffusion length in layered nanoplatelets due to their anisotropic diffusion of photogenerated carriers and nanometer-thin thickness. Here, we demonstrate a novel method to determine the in-plane diffusion length of photogenerated carriers in layered nanoplatelets using local time-resolved photoluminescence. An in-plane carrier diffusion length of 1.82 µm is obtained for an exfoliated (BA)2PbI4 (BA=CH3(CH2)3NH3) perovskite nanoplatelet. This method is particularly useful for weak luminescent materials and the materials that are easily damaged by long-term laser beam because of the high detection sensitivity. This technique is extendable to other layered materials and therefore plays a valuable role in the development and optimization of 2D and 3D semiconductor materials and devices for photovoltaic and photonic applications.

… , thermal, and optical properties have drawn considerable … exploration of these two-dimensional materials and their novel … photocarrier dynamics in two-dimensional materials and laid …

We use two-dimensional numerical simulations to analyze high spatial resolution time-resolved spectroscopy data. This analysis is applied to two-photon excitation time-resolved photoluminescence (2PE-TRPL) but is broadly applicable to all microscopic time-resolved techniques. By solving time-dependent drift-diffusion equations, we gain insight into carrier dynamics and transport characteristics. Accurate understanding of measurement results establishes the limits and potential of the measurement and enhances its value as a characterization method. Diffusion of carriers outside of the collection volume can have a significant impact on the measured decay but can also provide an estimate of carrier mobility as well as lifetime. In addition to material parameters, the experimental conditions, such as spot size and injection level, can impact the measurement results. Although small spot size provides better resolution, it also increases the impact of diffusion on the decay; if the spot size is much smaller than the diffusion length, it impacts the entire decay. By reproducing experimental 2PE-TRPL decays, the simulations determine the bulk carrier lifetime from the data. The analysis is applied to single-crystal and heteroepitaxial CdTe, material important for solar cells, but it is also applicable to other semiconductors where carrier diffusion from the excitation volume could affect experimental measurements.

2D materials, characterized by atomically thin structures and extraordinary electronic properties, offer fertile ground for exploring quantum phenomena governed by reduced dimensionality, quantum confinement, and strong many‐body interactions. Understanding these quantum effects‐such as quantum tunneling, plasmonic excitations, and exciton dynamics is crucial for enabling future quantum technologies. Optical spectroscopy, due to its non‐invasive nature, ultrahigh spatial, and temporal resolution, and exceptional sensitivity to electronic, vibrational, and structural states, has emerged as an indispensable approach for investigating these phenomena. Despite extensive theoretical predictions, a systematic experimental review explicitly connecting quantum properties in 2D materials to advanced optical spectroscopic techniques remains lacking. This review addresses this gap by describing the experimental manifestations of quantum properties and their characterization using cutting‐edge optical tools, including near‐field scanning optical microscopy (NSOM), pump–probe spectroscopy, advanced Raman‐based methods (such as coherent anti‐Stokes Raman scattering (CARS) and time‐resolved Raman (TRR)), and optical frequency comb spectroscopy. Emphasis is placed on the distinct capabilities of each technique for elucidating ultrafast carrier dynamics, phonon coherence, interlayer tunneling, and exciton relaxation processes. By linking individual quantum phenomenon to appropriate spectroscopic approaches, this review shines a light on optical spectroscopy in advancing both fundamental understanding and technological development of next‐generation quantum materials.

Ever since Ernest Rutherford scattered α-particles from gold foils, collision experiments have revealed insights into atoms, nuclei and elementary particles. In solids, many-body correlations lead to characteristic resonances—called quasiparticles—such as excitons, dropletons, polarons and Cooper pairs. The structure and dynamics of quasiparticles are important because they define macroscopic phenomena such as Mott insulating states, spontaneous spin- and charge-order, and high-temperature superconductivity. However, the extremely short lifetimes of these entities make practical implementations of a suitable collider challenging. Here we exploit lightwave-driven charge transport, the foundation of attosecond science, to explore ultrafast quasiparticle collisions directly in the time domain: a femtosecond optical pulse creates excitonic electron–hole pairs in the layered dichalcogenide tungsten diselenide while a strong terahertz field accelerates and collides the electrons with the holes. The underlying dynamics of the wave packets, including collision, pair annihilation, quantum interference and dephasing, are detected as light emission in high-order spectral sidebands of the optical excitation. A full quantum theory explains our observations microscopically. This approach enables collision experiments with various complex quasiparticles and suggests a promising new way of generating sub-femtosecond pulses.

… 2D materials support unique excitations of quasi-particles that consist of a material excitation … It can further be seen in figure 2(b),(c),(e), and (f), that the majority of the spectral region …

Polaritons, which are quasiparticles composed of a photon coupled to an electric or magnetic dipole, are a major focus in nanophotonic research of van der Waals (vdW) crystals and their derived 2D materials. For the variety of existing vdW materials, polaritons can be active in a broad range of the electromagnetic spectrum (meVs to eVs) and exhibit momenta much higher than the corresponding free‐space radiation. Hence, the use of high momentum broadband sources or probes is imperative to excite those quasiparticles and measure the frequency‐momentum dispersion relations, which provide insights into polariton dynamics. Synchrotron infrared nanospectroscopy (SINS) is a technique that combines the nanoscale spatial resolution of scattering‐type scanning near‐field optical microscopy with ultrabroadband synchrotron infrared radiation, making it highly suitable to probe and characterize a variety of vdW polaritons. Here, the advances enabled by SINS on the study of key photonic attributes of far‐ and mid‐infrared plasmon‐ and phonon‐polaritons in vdW and 2D crystals are reviewed. In that context the SINS technique is comprehensively described and it is demonstrated how fundamental polaritonic properties are retrieved for a range of atomically thin systems including hBN, MoS2, graphene and 2D heterostructures.

Terahertz two-dimensional coherent spectroscopy (THz-2DCS) is transforming our ability to probe, visualize, and control quantum materials far from equilibrium. This emerging technique brings multi-dimensional resolution to the ultrafast dynamics of nonequilibrium phases of matter, enabling new capabilities demanding precise coherent control and measurement of many-body dynamics and multi-order correlations. By mapping complex excitations across time and frequency dimensions, THz-2DCS delivers coherence tomography of driven quantum matter, thus revealing hidden excitation pathways, measuring higher order nonlinear response functions, disentangling various quantum pathways, capturing collective modes on ultrafast timescales and at terahertz frequencies. These experimental features frequently remain obscured in traditional single particle measurements, ultrafast spectroscopy techniques, and equilibrium-based probes. This Review traces the early development of THz-2DCS and showcases significant recent progress in leveraging this technique to probe and manipulate quantum material properties, including nonequilibrium superconductivity, nonlinear magnonics, dynamical topological phases, and the detection of novel excitations and exotic collective modes with potential technological impact. Looking forward, we identify critical opportunities in advancing THz-2DCS instrumentation and experimental strategies that are shaping future applications in THz optoelectronics, quantum information processing, and sensing.

… Therefore, our results provide a deeper understanding of the interfacial carrier dynamics of 2D-MoS 2 materials and the effects of defects on charge carrier lifetime in the SCL. …

Studies of the ultrafast carrier dynamics of transition metal dichalcogenides have employed spatially averaged measurements, which obfuscate the rich variety of dynamics that originate from the structural heterogeneity of these materials. Here, we employ femtosecond time-resolved photoemission electron microscopy (TR-PEEM) with sub-80 nm spatial resolution to image the ultrafast subpicosecond to picosecond carrier dynamics of monolayer tungsten diselenide (WSe2). The dynamics observed following 2.41 eV pump and 3.61 eV probe occurs on two distinct time scales. The 0.1 ps process is assigned to electron cooling via intervalley scattering, whereas the picosecond dynamics is attributed to exciton-exciton annihilation. The 70 fs decay dynamics observed at negative time delay reflects electronic relaxation from the Γ point. Analysis of the TR-PEEM data furnishes the spatial distributions of the various time constants within a single WSe2 flake. The spatial heterogeneity of the lifetime maps is consistent with increased disorder along the edges of the flake and the presence of nanoscale charge puddles in the interior. Our results indicate the need to go beyond spatially averaged time-resolved measurements to understand the influence of structural heterogeneities on the elementary carrier dynamics of two-dimensional materials.

… the surface dynamics and is detected in real time. In several unique applications, we spatially and temporally visualize the SE energy gain and loss, the charge carrier dynamics on the …

… To confirm that the morphology, grains, and surface defects are key components for controlling the carrier dynamics on materials surfaces, we conducted time-resolved imaging on a …

We highlight the recent progress in ultrafast dynamic microscopy that combines ultrafast optical spectroscopy with microscopy approaches, focusing on the application transient absorption microscopy (TAM) to directly image energy and charge transport in solar energy harvesting and conversion systems. We discuss the principles, instrumentation, and resolutions of TAM. The simultaneous spatial, temporal, and excited-state-specific resolutions of TAM unraveled exciton and charge transport mechanisms that were previously obscured in conventional ultrafast spectroscopy measurements for systems such as organic solar cells, hybrid perovskite thin films, and molecular aggregates. We also discuss future directions to improve resolutions and to develop other ultrafast imaging contrasts beyond transient absorption.

… has driven the recent development of ultrafast microscopy, … The ability to achieve such high temporal and spatial … , and 2D materials, where surface carrier dynamics differ significantly …

Transport phenomena like diffusion, convection, and drift play key roles in the sciences and engineering disciplines. They belong to the most omnipresent and important phenomena in nature that describe the motion of entities such as mass, charge or heat. Understanding and controlling these transport phenomena is crucial for a host of industrial technologies and applications, from cooling nuclear reactors to nanoscale heat‐management in the semiconductor industry. For decades, macroscopic transport techniques have been used to access important parameters such as charge mobilities or thermal conductivities. While being powerful, they often require physical contacts, which can lead to unwanted effects. Over the past years, an exciting solution has emerged: a technique called spatiotemporal microscopy (SPTM) that accesses crucial transport phenomena in a contactless, all‐optical, fashion. This technique offers powerful advantages in terms of accessible timescales, down to femtoseconds, and length scales, down to nanometres, and, further, selectively observes different species of interest. This tutorial review discusses common experimental configurations of SPTM and explains how they can be implemented by those entering the field. This review highlights the broad applicability of SPTM by presenting several exciting examples of transport phenomena that were unravelled thanks to this technique.

By combining advanced ultrashort-pulse laser technology with scanning tunneling microscopy, scientists demonstrate that they can directly image transient carrier dynamics in nanostructures in real space.

Conventional electron microscopy during the last three decades has experienced tremendous developments, especially in equipment design and engineering, to become one of the most widely recognized and powerful tools for key research areas in materials science and nanotechnology. In this article, we discuss scanning ultrafast electron microscopy (S-UEM) as a new methodology for four-dimensional electron imaging of material surfaces. We also illustrate a few unique applications . By monitoring secondary electrons emitted from surfaces of photoactive materials, photo- and electron-impact-induced electrons and holes near surfaces, interfaces, and heterojunctions can be imaged with adequate spatial and temporal resolution. Charge separation, transport, and anisotropic motions as well as their dependence on carrier energies can be resolved. S-UEM is poised to directly image and visualize relevant interfacial dynamics in real space and time for emerging optoelectronic devices and help push their performance.

We review recent advances in the characterization of electronic forms of energy transport in emerging semiconductors. The approaches described all temporally and spatially resolve the evolution of initially localized populations of photogenerated excitons or charge carriers. We first provide a comprehensive background for describing the physical origin and nature of electronic energy transport both microscopically and from the perspective of the observer. We introduce the new family of far-field, time-resolved optical microscopies developed to directly resolve not only the extent of this transport but also its potentially temporally and spatially dependent rate. We review a representation of examples from the recent literature, including investigation of energy flow in colloidal quantum dot solids, organic semiconductors, organic-inorganic metal halide perovskites, and 2D transition metal dichalcogenides. These examples illustrate how traditional parameters like diffusivity are applicable only within limited spatiotemporal ranges and how the techniques at the core of this review, especially when taken together, are revealing a more complete picture of the spatiotemporal evolution of energy transport in complex semiconductors, even as a function of their structural heterogeneities. Expected final online publication date for the Annual Review of Physical Chemistry, Volume 71 is April 20, 2020. Please see http://www.annualreviews.org/page/journal/pubdates for revised estimates.

Because of the strong Coulomb interaction and quantum confinement effect, 2-dimensional transition metal dichalcogenides possess a stable excitonic population. To realize excitonic device applications, such as excitonic circuits, switches, and transistors, it is of paramount importance for understanding the optical properties of transition metal dichalcogenides. Furthermore, the strong quantum confinement in 2-dimensional space introduces exotic properties, such as enhanced phonon bottlenecking effect, many-body interaction of excitons, and ultrafast nonequilibrium exciton–exciton annihilation. Exciton diffusion is the primary energy dissipation process and a working horse in excitonic devices. In this work, we investigated time-resolved exciton propagation in monolayer semiconductors of WSe 2 , MoWSe 2 , and MoSe 2 , with a home-built femtosecond pump-probe microscope. We observed ultrafast exciton expansion behavior with an equivalent diffusivity of up to 502 cm 2 s −1 at the initial delay time, followed by a slow linear diffusive regime (20.9 cm 2 s −1 ) in the monolayer WSe 2 . The fast expansion behavior is attributed to energetic carrier-dominated superdiffusive behavior. We found that in the monolayers MoWSe 2 and MoSe 2 , the energetic carrier-induced exciton expansion is much more effective, with diffusivity up to 668 and 2295 cm 2 s −1 , respectively. However, the “cold” exciton transport is trap limited in MoWSe 2 and MoSe 2 , leading to negative diffusion behavior at later time. Our findings are helpful to better understand the ultrafast nonlinear diffusive behavior in strongly quantum-confined systems. It may be harnessed to break the limit of conventional slow diffusion of excitons for advancing more efficient and ultrafast optoelectronic devices.

… Pump–probe microscopy combines the spatial resolution of far-field optical microscopy with … It has also enabled direct imaging of transport phenomena such as free carrier diffusion, …

… By applying the microscopy technique, fundamental carrier dynamics in semiconductors … photoexcited carrier dynamics, 27 as well as the direct detection of photoexcited carrier diffusion…

In recent years, optical pump-probe microscopy (PPM) has become a vital technique for spatiotemporally imaging electronic excitations and charge-carrier transport in metals and semiconductors. However, existing methods are limited by mechanical delay lines with a probe time window up to several nanoseconds (ns) or monochromatic pump and probe sources with restricted spectral coverage and temporal resolution, hindering their amenability in studying relatively slow processes. To bridge these gaps, we introduce a dual-hyperspectral PPM setup with a time window spanning from nanoseconds to milliseconds and single-nanosecond resolution. Our method features a wide-field probe tunable from 370 to 1000 nm and a pump spanning from 330 nm to 16 μm. We apply this PPM technique to study various two-dimensional metal-halide perovskites (2D-MHPs) as representative semiconductors by imaging their transient responses near the exciton resonances under both above-band gap electronic pump excitation and below-band gap vibrational pump excitation. The resulting spatially and temporally resolved images reveal insights into heat dissipation, film uniformity, distribution of impurity phases, and film-substrate interfaces. In addition, the single-nanosecond temporal resolution enables the imaging of in-plane strain wave propagation in 2D-MHP single crystals. Our method, which offers extensive spectral tunability and significantly improved time resolution, opens new possibilities for the imaging of charge carriers, heat, and transient phase transformation processes, particularly in materials with spatially varying composition, strain, crystalline structure, and interfaces.

Understanding carrier and exciton transport with a high spatiotemporal resolution is essential for the advancement of next-generation electronic and optoelectronic devices. However, traditional time-resolved spectroscopic techniques are constrained in their ability to resolve spatially dependent ultrafast dynamics. In recent years, transient absorption microscopy (TAM) has emerged by integrating time-resolved spectroscopy with optical microscopy, enabling the simultaneous capture of spatial and temporal evolution of photoinduced carrier transport processes. Nevertheless, the point-scanning nature of conventional TAM leads to long acquisition times and imposes stringent requirements on laser stability and sample robustness, which significantly limit its application. Wide-field transient absorption microscopy (WTAM) effectively addresses these limitations by combining femtosecond temporal resolution with subdiffraction spatial imaging across a broad field of view, thereby enabling direct and rapid visualization of carrier and exciton diffusion and transport dynamics. In this review, we present the fundamental principles and instrumentation of WTAM, and summarize its unique advantages in mapping spatiotemporal dynamics. We further highlight recent advances in applying WTAM to investigate both equilibrium and nonequilibrium transport processes in various materials including perovskites, organic semiconductors, and two-dimensional materials. Finally, we discuss current challenges and propose future opportunities for expanding WTAM's role in characterizing advanced materials and guiding the design of high-performance optoelectronic devices.

… densities, we observe that the built-in field suppresses electron transport towards and … a recently developed femtosecond-resolved near-field scanning optical microscope NSOM.The …

… We measure S as we scan the probe spot along the x ^ direction with y = 1 μm [white … To monitor that transport, we measure Δ N as we scan the probe spot along y ^ with x = 1 μm [white …

Passive scattering-type, scanning near-field optical microscopy (s-SNOM) has been employed to study localized, long-wavelength infrared (LWIR) surface waves without external illumination. Here, we develop a cryogenic passive s-SNOM instrument in a vacuum chamber with 4 K liquid-helium cooling. Notably, the extremely low-temperature environment inside the chamber enables the realization of passive near-field detection with low background thermal noise. The technique mainly utilizes a highly sensitive LWIR confocal optical system and a tuning fork-based atomic force microscope, and the near-field detection was performed at a wavelength of 10.2 ± 0.9 µm. In this paper, we discuss the cryogenic s-SNOM implementation in detail and report the investigation of thermally excited surface electromagnetic fields on a self-heated NiCr wire deposited on SiO2 at a temperature of 5 K. The origin of the surface electromagnetic fields was established to be the thermally excited fluctuating charges of the conduction electrons. The cryogenic s-SNOM method presented herein shows significant promise for application in a variety of spheres, including hot-carrier dissipation in ballistic conductors.

… Steininger et al. calculated that the transition from ballistic to diffusive carrier transport behaviour in semiconductors should occur at ≈1 ps and several hundred nanometres (Steininger …

… on the ballistic and diffusive real-space transfer of photogenerated carriers or their trapping … In this report, we combine low-temperature near-field scanning optical microscopy and time-…

… carrier transport in a GaAs quantum wire structure are directly mapped by low-temperature near-field scanning optical … ballistic electron emission microscopy,1,2 which was derived from …

… on carrier transport and trapping into the quantum wire is analyzed in steady state and time-resolved near-field … ning or transmission electron microscopy, scanning tunneling, ballistic …

… insight into the ballistic and diffusive propagation of photogenerated carriers [1617], or the … The decay of the reflectivity signal reflects the carrier transport along the QWR. The solid line …

… in transient spectroscopy … diffusion length in 2D perovskites, we further performed electric-field-dependent SPCM complemented by field-dependent time-resolved photoluminescence …

Atomically thin two-dimensional transition metal dichalcogenides (TMDs) have shown great potential for optoelectronic applications, including photodetectors, phototransistors, and spintronic devices. However, the applications of TMD-based optoelectronic devices are severely restricted by their weak light absorption and short exciton lifetime due to their atomically thin nature and strong excitonic effect. To simultaneously enhance the light absorption and photocarrier lifetime of monolayer semiconductors, here, we report 3D/2D perovskite/TMD type II heterostructures by coupling solution processed highly smooth and ligand free CsPbBr3 film with MoS2 and WS2 monolayers. By time-resolved spectroscopy, we show interfacial hole transfer from MoS2 (WS2) to the perovskite layer occurs in an ultrafast time scale (100 and 350 fs) and interfacial electron transfer from ultrathin CsPbBr3 to MoS2 (WS2) in ∼3 (9) ps, forming a long-lived charge separation with a lifetime of >20 ns. With increasing CsPbBr3 thickness, the electron transfer rate from CsPbBr3 to TMD is slower, but the efficiency remains to be near-unity due to coupled long-range diffusion and ultrafast interfacial electron transfer. This study indicates that coupling solution processed lead halide perovskites with strong light absorption and long carrier diffusion length to monolayer semiconductors to form a type II heterostructure is a promising strategy to simultaneously enhance the light harvesting capability and photocarrier lifetime of monolayer semiconductors.

Transition metal dichalcogenides are expected to be used in transparent, flexible, and highly efficient light-emitting devices. Exciton diffusion is a key factor in device applications. In this study, we measured the photoluminescence (PL) decay of excitons in a ${\mathrm{MoS}}_{2}$ monolayer synthesized by chemical vapor deposition on a sapphire substrate. The PL decay of A and B excitons in the femtosecond regime was observed. The PL decay curves were analyzed based on a model of exciton trapping at the deactivation center via diffusion, and the diffusion time until trapping was obtained. The diffusion coefficient and the corresponding exciton mobility were also determined. This study demonstrates the two-dimensional exciton diffusion in the femtosecond regime in the ${\mathrm{MoS}}_{2}$ monolayer.

2D lead halide perovskites (2DPs) offer chemical compatibility with 3D perovskites and enhanced stability, which are attractive for applications in photovoltaic and light‐emitting devices. However, such lowered structural dimensionality causes increased excitonic effects and highly anisotropic charge‐carrier transport. Determining the diffusivity of excitations, in particular for out‐of‐plane or inter‐layer transport, is therefore crucial, yet challenging to achieve. Here, an effective method is demonstrated for monitoring inter‐layer diffusion of photoexcitations in (PEA)2PbI4 thin films by tracking time‐dependent changes in photoluminescence spectra induced by photon reabsorption effects. Selective photoexcitation from either substrate‐ or air‐side of the films reveals differences in diffusion dynamics encountered through the film profile. Time‐dependent diffusion coefficients are extracted from spectral dynamics through a 1D diffusion model coupled with an interference correction for refractive index variations arising from the strong excitonic resonance of 2DPs. Such analysis, together with structural probes, shows that minute misalignment of 2DPs planes occurs at distances far from the substrate, where efficient in‐plane transport consequently overshadows the less efficient out‐of‐plane transport in the direction perpendicular to the substrate. Through detailed analysis, a low out‐of‐plane excitation diffusion coefficient of (0.26 ± 0.03) ×10−4 cm2 s−1 is determined, consistent with a diffusion anisotropy of ≈4 orders of magnitude.

… A home-built transient photoluminescence microscopy (TPLM) was used to measure … in both xy directions to obtain a one- or two-dimensional time-resolved photoluminescence. …

Two-dimensional hybrid organic-inorganic perovskites with strongly bound excitons and tunable structures are desirable for optoelectronic applications. Exciton transport and annihilation are two key processes in determining device efficiencies; however, a thorough understanding of these processes is hindered by that annihilation rates are often convoluted with exciton diffusion constants. Here we employ transient absorption microscopy to disentangle quantum-well-thickness-dependent exciton diffusion and annihilation in two-dimensional perovskites, unraveling the key role of electron-hole interactions and dielectric screening. The exciton diffusion constant is found to increase with quantum-well thickness, ranging from 0.06 ± 0.03 to 0.34 ± 0.03 cm2 s−1, which leads to long-range exciton diffusion over hundreds of nanometers. The exciton annihilation rates are more than one order of magnitude lower than those found in the monolayers of transition metal dichalcogenides. The combination of long-range exciton transport and slow annihilation highlights the unique attributes of two-dimensional perovskites as an exciting class of optoelectronic materials. Two-dimensional hybrid perovskites are promising excitonic materials; however, there currently lacks understanding on exciton diffusion and annihilation. Here Deng et al. employ transient absorption microscopy to disentangle quantum-well-thickness-dependent exciton transport and annihilation in these materials.

This is the publisher's version, also available electronically from http://journals.aps.org/prb/abstract/10.1103/PhysRevB.86.205417.

Devices operating with excitons have promising prospect for overcoming the dilemma of response time and integration in current generation of electron or/and photon based elements and devices. Although the intrinsic properties including edges, grain boundaries and defects of atomically thin semiconductors have been demonstrated as a powerful tool to adjust bandgap and exciton energy, investigating the intrinsic modulation of spatio-temporal dynamics still remains challenging on account of the short exciton diffusion length. Here, we achieve the attractive remote lightening that the emission region could be far away (up to 14.6 μm) from excitation centre, by utilizing the femtosecond laser with ultrahigh peak power as excitation source and the edge region with high photoluminescence efficiency as a bright emitter. Furthermore, the ultrafast transition between exciton and trion is demonstrated, which provides an insight into the intrinsic modulation on populations of exciton and trion states. The complete cascaded physical scenario of exciton spatio-temporal dynamics is eventually established. This work can refresh our perspective on the spatial nonuniformities of CVD grown atomically thin semiconductors and provide important implications for developing durable and stable excitonic devices in future.