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The use of nanoscale lasers in new space technologies can enable a variety of applications. Metal lead halide perovskites have emerged and been verified to possess many unique properties for optoelectronic applications, which are key elements for the space mission system. However, the basic knowledge of radiation damage of perovskite materials and the in-depth experimental irradiation testing on their lasing properties are still lacking. Here, the performance of a CsPbBr3 nanoplate (NP) laser is measured to be maintained after exposure to 150 keV proton beam with fluence up to 1 × 1015 p/cm2, an extremely high level of collision that destroys CdS NPs with similar shapes and emission wavelengths. Lasing characteristics and carrier dynamics of the CsPbBr3 and CdS NPs have been studied and compared in detail before and after proton irradiation with different beam fluences. Concurrently, simulation results manifest that negligible atomic displacement damage is caused by proton bombardment in CsPbBr3, ensuring its high resistance to proton irradiation. The findings of the high radiation resistance of the CsPbBr3 NP lasers and the insights into the underlying mechanism are conceivably important, which might make recommendations for the development of perovskite coherent light sources for new space applications. [ABSTRACT FROM AUTHOR]

Understanding ultrafast electronic dynamics of the interlayer excitonic states in atomically thin transition metal dichalcogenides is of importance in engineering valleytronics and developing excitonic integrated circuits. In this work, we experimentally explored the ultrafast dynamics of indirect interlayer excitonic states in monolayer type II WSe 2 /ReS 2 heterojunctions using time-resolved photoemission electron microscopy, which reveals its anisotropic behavior. The ultrafast cooling and decay of excited-state electrons exhibit significant linear dichroism. The ab initio theoretical calculations provide unambiguous evidence that this linear dichroism result is primarily associated with the anisotropic nonradiative recombination of indirect interlayer excitonic states. Measuring time-resolved photoemission energy spectra, we have further revealed the ultrafast evolution of excited-state electrons in anisotropic indirect interlayer excitonic states. The findings have important implications for controlling the interlayer moiré excitonic effects and designing anisotropic optoelectronic devices.

Two-dimensional (2D) material bubbles, as a straightforward method to induce strain, represent a potentially powerful platform for the modulation of different properties of 2D materials and the exploration of their strain-related applications. Here, we prepare ReS 2 /graphene heterojunction bubbles (ReS 2 /gr heterobubbles) and investigate their strain and interference synergistically modulated optical and electrical properties. We perform Raman and photoluminescence (PL) spectra to verify the continuously varying strain and the microcavity induced optical interference in ReS 2 /gr heterobubbles. Kelvin probe force microscopy (KPFM) is carried out to explore the photogenerated carrier transfer behavior in both strained ReS 2 /gr heterobubbles and ReS 2 /gr interfaces, as well as the oscillation of surface potential caused by optical interference under illumination conditions. Moreover, the switching of in-plane crystal orientation and the modulation of optical anisotropy of ReS 2 /gr heterobubbles are observed by azimuth-dependent reflectance difference microscopy (ADRDM), which can be attributed to the action of both strain effect and interference. Our study proves that the optical and electrical properties can be effectively modulated by the synergistical effect of strain and interference in a 2D material bubble.

The electron-phonon (e-ph) interaction in lead halide perovskites (LHPs) plays a role in a variety of physical phenomena. Unveiling how the local lattice distortion responds to charge carriers is a critical step toward understanding the e-ph interaction in LHPs. Herein, we advance a fundamental understanding of the e-ph interaction in LHPs from the perspective of stereochemical activity of 6s 2 lone-pair electrons on the Pb 2+ cation. We demonstrate a model system based on three LHPs with distinctive lone-pair activities for studying the structure-property relationships. By tuning the A-cation chemistry, we synthesized single-crystal CsPbBr 3 , (MA 0.13 EA 0.87 )PbBr 3 (MA + = methylammonium; EA + = ethylammonium), and (MHy)PbBr 3 (MHy + = methylhydrazinium), which exhibit stereo-inactive, dynamic stereo-active, and static stereo-active lone pairs, respectively. This gives rise to distinctive local lattice distortions and low-frequency vibrational modes. We find that the e-ph interaction leads to a blue shift of the band gap as temperature increases in the structure with the dynamic stereo-active lone pair but to a red shift in the structure with the static stereo-active lone pair. Furthermore, analyses of the temperature-dependent low-energy photoluminescence tails reveal that the strength of the e-ph interaction increases with increasing lone-pair activity, leading to a transition from a large polaron to a small polaron, which has significant influence on the emission spectra and charge carrier dynamics. Our results highlight the role of the lone-pair activity in controlling the band gap, phonon, and polaronic effect in LHPs and provide guidelines for optimizing the optoelectronic properties, especially for tin-based and germanium-based halide perovskites, where stereo-active lone pairs are more prominent than their lead counterparts.

Distribution of the transition dipole moments (TDMs) of light emitters can intrinsically affect the light out-coupling efficiency of planar light-emitting diodes (LEDs). Lacking the control of TDM distribution has limited the efficiency of nanocrystal-based LEDs to 20%. Here, we present a method that deposits uniform nanocrystal films with unity in-plane TDM distribution. Combining an inkjet printing technique and colloidal nanocrystal self-assembly, we achieved direct printing and in situ assembly of colloidal CdSe/CdS nanoplatelets to all orient "face-down" on various substrates. With motorized translation stages, pattern printing is realized, which demonstrates the potential for integration in industrial-scale fabrication. The method is applied to achieve uniform nanoplatelet films with unity in-plane TDM distribution on zinc-oxide films, a commonly used electron-transport layer. Thus, our work paves the way to break the light out-coupling efficiency limitation of 20% in state-of-the-art nanocrystal-based LEDs, which exclusively possess an isotropic TDM distribution.

A comprehensive understanding of the ultrafast electron dynamics in two-dimensional transition metal dichalcogenides (TMDs) is necessary for their applications in optoelectronic devices. In this work, we contribute a study of ultrafast electron cooling and decay dynamics in the supported and suspended monolayer WS 2 by time- and energy-resolved photoemission electron microscopy (PEEM). Electron cooling in the Q valley of the conduction band is clearly resolved in energy and time, on a time scale of 0.3 ps. Electron decay is mainly via a defect trapping process on a time scale of several picoseconds. We observed that the trap states can be produced and increased by laser illumination under an ultrahigh vacuum, and the higher local optical-field intensity led to the faster increase of trap states. The enhanced defect trapping could significantly modify the carrier dynamics and should be paid attention to in photoemission experiments for two-dimensional materials.

Using liquid-liquid interfacial assembly, we control the deposition of CdSe nanoplatelets into face-down or edge-up configurations. Controlled assembly, combined with back focal plane imaging, enabled unambiguous determination of the transition dipole orientation. The transition dipole moment of the emissive band-edge exciton in CdSe nanoplatelets was found to be isotropically oriented within the plane of the nanoplatelet with no measurable out-of-plane component and no preference for the long- or short-axis of the nanoplatelet. Importantly, CdSe nanoplatelet films in the face-down configuration exhibited unity dipole orientation within the plane of the film, which could improve the external efficiency of nanoplatelet LEDs, lasers, photodetectors, and photovoltaic cells beyond that which is possible with isotropic emitters. We also show that the two self-assembled configurations have different Förster energy transfer rates, as a result of different dipole orientation and internanoplatelet distance.

The assembly of quantum dots is an essential step toward many of their potential applications. To form conductive solids from colloidal quantum dots, ligand exchange is required. Here we study the influence of ligand replacement on the photoconductivity of PbSe quantum-dot solids, using the time-resolved microwave conductivity technique. Bifunctional replacing ligands with amine, thiol, or carboxylic acid anchor groups of various lengths are used to assemble quantum solids via a layer-by-layer dip-coating method. We find that when the ligand lengths are the same, the charge carrier mobility is higher in quantum-dot solids with amine ligands, while in quantum-dot solids with thiol ligands the charge carrier lifetime is longer. If the anchor group is the same, the charge carrier mobility is ligand length dependent. The results show that the diffusion length of charge carriers can reach several hundred nanometers.

We report on a photodetector in which colloidal quantum dots directly bridge nanometer-spaced electrodes. Unlike in conventional quantum-dot thin film photodetectors, charge mobility no longer plays a role in our quantum-dot junctions as charge extraction requires only two individual tunnel events. We find an efficient photoconductive gain mechanism with external quantum efficiencies of 38 electrons-per-photon in combination with response times faster than 300 ns. This compact device-architecture may open up new routes for improved photodetector performance in which efficiency and bandwidth do not go at the cost of one another.

Using femtosecond transient absorption spectroscopy, we demonstrate that lead chalcogenide nanocrystals show considerable photoinduced absorption (PA) in a broad wavelength range just below the band gap. The time-dependent decay of the PA signal correlates with the recovery of the band gap absorption, indicating that the same carriers are involved. On this basis, we assign this PA signal to intraband absorption, that is, the excitation of photogenerated carriers from the bottom of the conduction band or the top of the valence band to higher energy levels in the conduction and valence band continuum. We confirm our experiments with tight-binding calculations. This broadband response in the commercially interesting near- to mid-infrared range is very relevant for ultra-high-speed all-optical signal processing. We benchmark the performance with bulk Si and Si nanocrystals.

We report the direct and unambiguous determination of electron transfer rates and efficiencies from PbSe quantum dots (QDs) to mesoporous SnO2 films. We monitor the time-dependent electron density within the oxide with picosecond time resolution using Terahertz spectroscopy, following optical excitation of the QDs using a femtosecond laser pulse. QD-oxide electron transfer occurs with efficiencies of ∼2% in our samples under 800 nm pumping with a marked dependence on QD size, ranging from ∼100 ps injection times for the smallest, ∼2 nm diameter QDs, to ∼1 ns time scale for ∼7 nm QDs. The size-dependent electron transfer rates are modeled within the framework of Marcus theory and the implications of the results for device design are discussed.

PbSe quantum-dot solids are of great interest for low cost and efficient photodetectors and solar cells. We have prepared PbSe quantum-dot solids with high charge carrier mobilities using layer-by-layer dip-coating with 1,2-ethanediamine as substitute capping ligands. Here we present a time and energy resolved transient absorption spectroscopy study on the kinetics of photogenerated charge carriers, focusing on 0-5 ps after photoexcitation. We compare the observed carrier kinetics to those for quantum dots in dispersion and show that the intraband carrier cooling is significantly faster in quantum-dot solids. In addition we find that carriers diffuse from higher to lower energy sites in the quantum-dot solid within several picoseconds.

We show that in films of strongly coupled PbSe quantum dots multiple electron-hole pairs can be efficiently produced by absorption of a single photon (carrier multiplication). Moreover, in these films carrier multiplication leads to the generation of free, highly mobile charge carriers rather than excitons. Using the time-resolved microwave conductivity technique, we observed the production of more than three electron-hole pairs upon absorption of a single highly energetic photon (5.7E(g)). Free charge carriers produced via carrier multiplication are readily available for use in optoelectronic devices even without employing any complex donor/acceptor architecture or electric fields.

We study the rotational wave packet created by nonadiabatic rotational excitation of molecules with strong femtosecond laser pulses. The applicable condition of the Delta-Kick method is obtained by comparing the laser intensity and pulse duration dependences of the wave packet calculated with different methods. The wave packet evolution is traced analytically with the Delta-Kick method. The calculations demonstrate that the rotational populations can be controlled for the rotational wave packet created by two femtosecond laser pulses. The evolution of the rotational wave packet with controlled populations produces interference patterns with exotic spatial symmetries. These calculations are validated by comparing the theoretical calculations with our experimental measurements for the rotational wave packet created by thermal ensemble CO(2) and two strong femtosecond laser pulses. Potential applications in molecular science are also discussed for the rotational wave packet with controlled populations and spatial symmetries.

An apparatus was constructed to experimentally quantify the field-free alignment of diatomic molecules irradiated by strong femtosecond laser pulses. In this apparatus, both homodyne and pure heterodyne detections were realized. The alignment signal is proportional to [ - 1/3](2) for homodyne detection and ( - 1/3) for pure heterodyne detection, where theta is the polar angle between the molecular axis and the laser polarization direction. Fourier transform spectra of the homodyne signal and the pure heterodyne signal were also studied. By comparing the alignment signal and its Fourier transform spectrum with the numerical calculation of the time-dependent Schrödinger equation, we demonstrated that the pure heterodyne signal directly reproduced the alignment parameter , and its Fourier transform spectrum provided information regarding the populations of different J states in the rotational wavepacket.