Anti-Blooming Clocking for Time-Delay Integration CCDs.

This paper presents an investigation of the responsivity of a time-delay integration (TDI) charge-coupled device that employs anti-blooming clocking and uses a varying number of TDI stages. The influence of charge blooming caused by unused TDI stages in a TDI deployed selection scheme is shown experimentally, and an anti-blooming clocking mechanism is analyzed. The impact of blooming on sensor characteristics, such as the responsivity, the conversion gain, and the signal-to-noise ratio, is investigated. A comparison of the measurements with and without this anti-blooming clocking mechanism is presented and discussed in detail.

Analytical Evaluation of Signal-to-Noise Ratios for Avalanche- and Single-Photon Avalanche Diodes.

Performance of systems for optical detection depends on the choice of the right detector for the right application. Designers of optical systems for ranging applications can choose from a variety of highly sensitive photodetectors, of which the two most prominent ones are linear mode avalanche photodiodes (LM-APDs or APDs) and Geiger-mode APDs or single-photon avalanche diodes (SPADs). Both achieve high responsivity and fast optical response, while maintaining low noise characteristics, which is crucial in low-light applications such as fluorescence lifetime measurements or high intensity measurements, for example, Light Detection and Ranging (LiDAR), in outdoor scenarios. The signal-to-noise ratio (SNR) of detectors is used as an analytical, scenario-dependent tool to simplify detector choice for optical system designers depending on technologically achievable photodiode parameters. In this article, analytical methods are used to obtain a universal SNR comparison of APDs and SPADs for the first time. Different signal and ambient light power levels are evaluated. The low noise characteristic of a typical SPAD leads to high SNR in scenarios with overall low signal power, but high background illumination can saturate the detector. LM-APDs achieve higher SNR in systems with higher signal and noise power but compromise signals with low power because of the noise characteristic of the diode and its readout electronics. Besides pure differentiation of signal levels without time information, ranging performance in LiDAR with time-dependent signals is discussed for a reference distance of 100 m. This evaluation should support LiDAR system designers in choosing a matching photodiode and allows for further discussion regarding future technological development and multi pixel detector designs in a common framework.

Microscopic Insight into Electron-Induced Dissociation of Aromatic Molecules on Ice.

We use scanning tunneling microscopy, photoelectron spectroscopy, and ab initio calculations to investigate the electron-induced dissociation of halogenated benzene molecules adsorbed on ice. Dissociation of halobenzene is triggered by delocalized excess electrons attaching to the π^{*} orbitals of the halobenzenes from where they are transferred to σ^{*} orbitals. The latter orbitals provide a dissociative potential surface. Adsorption on ice sufficiently lowers the energy barrier for the transfer between the orbitals to facilitate dissociation of bromo- and chloro- but not of flourobenzene at cryogenic temperatures. Our results shed light on the influence of environmentally important ice particles on the reactivity of halogenated aromatic molecules.

Nonequilibrium electron and lattice dynamics of strongly correlated Bi2Sr2CaCu2O8+δ single crystals.

The interplay between the electronic and lattice degrees of freedom in nonequilibrium states of strongly correlated systems has been debated for decades. Although progress has been made in establishing a hierarchy of electronic interactions with the use of time-resolved techniques, the role of the phonons often remains in dispute, a situation highlighting the need for tools that directly probe the lattice. We present the first combined megaelectron volt ultrafast electron diffraction and time- and angle-resolved photoemission spectroscopy study of optimally doped Bi2Sr2CaCu2O8+δ. Quantitative analysis of the lattice and electron subsystems' dynamics provides a unified picture of nonequilibrium electron-phonon interactions in the cuprates beyond the N-temperature model. The work provides new insights on the specific phonon branches involved in the nonequilibrium heat dissipation from the high-energy Cu-O bond stretching "hot" phonons to the lowest-energy acoustic phonons with correlated atomic motion along the <110> crystal directions and their characteristic time scales. It reveals a highly nonthermal phonon population during the first several picoseconds after the photoexcitation. The approach, taking advantage of the distinct nature of electrons and photons as probes, is applicable for studying energy relaxation in other strongly correlated electron systems.

The energy barrier in singlet fission can be overcome through coherent coupling and entropic gain.

One strategy to improve solar-cell efficiency is to generate two excited electrons from just one photon through singlet fission, which is the conversion of a singlet (S(1)) into two triplet (T(1)) excitons. For efficient singlet fission it is believed that the cumulative energy of the triplet states should be no more than that of S(1). However, molecular analogues that satisfy this energetic requirement do not show appreciable singlet fission, whereas crystalline tetracene displays endothermic singlet fission with near-unity quantum yield. Here we probe singlet fission in tetracene by directly following the intermediate multiexciton (ME) state. The ME state is isoenergetic with 2 × T(1), but fission is not activated thermally. Rather, an S(1) â‡” ME superposition formed through a quantum-coherent process allows access to the higher-energy ME. We attribute entropic gain in crystalline tetracene as the driving force for the subsequent decay of S(1) â‡” ME into 2 × T(1), which leads to a high singlet-fission yield.

Observing the multiexciton state in singlet fission and ensuing ultrafast multielectron transfer.

Multiple exciton generation (MEG) refers to the creation of two or more electron-hole pairs from the absorption of one photon. Although MEG holds great promise, it has proven challenging to implement, and questions remain about the underlying photo-physical dynamics in nanocrystalline as well as molecular media. Using the model system of pentacene/fullerene bilayers and femtosecond nonlinear spectroscopies, we directly observed the multiexciton (ME) state ensuing from singlet fission (a molecular manifestation of MEG) in pentacene. The data suggest that the state exists in coherent superposition with the singlet populated by optical excitation. We also found that multiple electron transfer from the ME state to the fullerene occurs on a subpicosecond time scale, which is one order of magnitude faster than that from the triplet exciton state.

Communication: Momentum-resolved quantum interference in optically excited surface states.

Surface states play essential roles in condensed matter physics, e.g., as model two-dimensional (2D) electron gases and as the basis for topological insulators. Here, we demonstrate quantum interference in the optical excitation of 2D surface states using the model system of C(60)/Au(111). These surface states are transiently populated and probed in a femtosecond time- and angle-resolved two-photon photoemission experiment. We observe quantum interference within the excited populations of these surface states as a function of parallel momentum vector. Such quantum interference in momentum space may allow one to control 2D transport properties by optical fields.