Electron transfer processes at molecule-semiconductor interfaces involve a complex mixture of thermionic, tunneling and hopping events. Traditionally these processes have been modeled in a piece-meal fashion, relying on phenomenological treatments such as Simmons and Richardson equations that are not vetted in atomistic systems and do not flow seamlessly into each other. We present a unified modeling approach, based on the Non-equilibrium Greens function (NEGF) formalism that allows us to integrate diverse transport regimes and establish a comprehensive quantitative theory. By comparing our simulations with experiments on a metal-molecule-semiconductor junction (varying molecular lengths ~1-3nm), we identify the role of molecular monolayers in tuning the semiconductor band-bending, and thereby overall device conductivity. We find that the principal role of molecules is to act as a voltage divider, altering the Schottky barriers, thereby modulating current levels, voltage-asymmetries and crossover from Schottky to tunneling transport. While this provides an appealingly simple explanation for our observed experimental trends, the calculated shifts in crossover voltages are insufficient to explain the experiments quantitatively. Quantitative correspondence with experiments requires invocation of an additional voltage divider arising from molecular dipoles that further tunes semiconductor band-bending. The extracted dipole moments are rationalized using ab-initio calculations for each molecule, along-with a dilution of packing fraction for the shortest molecular lengths. The methodology described herein can be used to better understand and predict transport characteristics of such junctions.
Recent development in fabrication of hybrid nanostructures allows for creation of quantum interferometers that combine semiconductor and superconductor materials. We show that in those nanostructures the joint phenomena of Aharonov-Bohm effect and Andreev reflections can be used to determine the length on which the electron is retro-reflected as a hole. We propose to exploit this feature for probing of the quasiparticle coherence length in semiconductor-superconductor hybrids by a magnetoconductance measurement.
While the study of space charge potentials has a long history, present models are largely based on the notion of steady state equilibrium, ill-suited to describe wide bandgap semiconductors with moderate to low concentrations of defects. Here we build on color centers in diamond both to locally inject carriers into the crystal and probe their evolution as they propagate in the presence of external and internal potentials. We witness the formation of metastable charge patterns whose shape - and concomitant field - can be engineered through the timing of carrier injection and applied voltages. W…
Interface phonon modes that are generated by several atomic layers at the heterointerface play a major role in the interface thermal conductance for nanoscale high-power devices such as nitride-based high-electron-mobility transistors and light emitting diodes. Here we measure the local phonon spectra across AlN/Si and AlN/Al interfaces using atomically resolved vibrational electron energy-loss spectroscopy in a scanning transmission electron microscope. At the AlN/Si interface, we observe various localized phonon modes, of which the extended and interfacial modes act as bridges to connect the…
Understanding the formation of metal-molecule contact at the microscopic level is the key towards controlling and manipulating atomic scale devices. Employing two isomers of bipyridine, $4, 4^\prime$ bipyridine and $2, 2^\prime$ bipyridine between gold electrodes, here, we investigate the formation of metal-molecule bond by studying charge transport through single molecular junctions using a mechanically controlled break junction technique at room temperature. While both molecules form molecular junctions during the breaking process, closing traces show the formation of molecular junctions una…
Probing exciton interaction with a spatially defined charge accumulation layer in the organic semiconductor Diindenoperylene
利用有机薄膜晶体管（OTFT）的光致发光（PL）和载流子输运测量，研究了激子和载流子之间的微观相互作用。为此目的，原型有机半导体二茚并萘嵌苯（DIP）被用作活性物质。OTFT累积层提供了空间限定的电荷和光生激子的相互作用区，导致PL强度降低高达4.5%。这种效应与累积的空穴载流子密度相关，并为非辐射激子-空穴过程的横截面提供了约1.3E-10 cm 3/s的较低估计。这是合理的，这些过程优先介导的陷阱空穴。
Room-temperature tuning and probing of Fermi polarons in atomically thin semiconductors on a plasmonic metasurface
Nanyang Technological University（南洋理工大学）；Universidad Autónoma de Madrid（马德里自治大学）；Condensed Matter Physics Center (IFIMAC), Universidad Autónoma de Madrid（马德里自治大学凝聚态物理中心（IFIMAC））；Jilin University（吉林大学）；Zhejiang University（浙江大学）
Interfaces of dye molecules and two-dimensional transition metal dichalcogenides (TMDCs) combine strong molecular dipole excitations with high carrier mobilities in semiconductors. Förster type energy transfer is one key mechanism for the coupling between both constituents. We report microscopic calculations of a spectrally resolved Förster induced transition rate from dye molecules to a TMDC layer. Our approach is based on microscopic Bloch equations which are solved self-consistently together with Maxwells equations. This approach allows to incorporate the dielectric environment of a TMDC se…
Gate patterning on semiconductors is routinely used to electrostatically restrict electron movement into reduced dimensions. At cryogenic temperatures, where most studies are carried out, differential thermal contraction between the patterned gate and the semiconductor often lead to an appreciable strain modulation. The impact of such modulated strain to the conductive channel buried in a semiconductor has long been recognized, but measuring its magnitude and variation is rather challenging. Here we present a way to measure that modulation in a gate-defined GaAs-based one-dimensional channel b…
Similarities and differences in the construction of dispersion laws for charge carriers in semiconductor crystals and adiabatic potentials in molecules
Top-down fabricated nanoantenna architectures of both metallic and dielectric materials demonstrated powerful functionalities for Raman and fluorescence enhancement with relevance to single molecule sensing, while inducing directionality of chromophore emission with implications for single photon sources. Herein, we synthesize the smallest bowtie nanoantenna by selective tip-to-tip fusion of two tetrahedral colloidal quantum dots (CQDs) forming a dimer. While the tetrahedral monomers emit non-polarized light, the bowtie architecture manifests nanoantenna functionality of enhanced emission pola…
Electron-phonon scatterings in solid-state systems are pivotal processes in determining many key physical quantities such as charge carrier mobilities and thermal conductivities. Here, we report on the direct probing of phonon mode specific electron-phonon scatterings in layered semiconducting transition metal dichalcogenides WSe2, MoSe2, WS2, and MoS2 through inelastic electron tunneling spectroscopy measurements, quantum transport simulations, and density functional calculation. We experimentally and theoretically characterize momentum-conserving single- and two-phonon electron-phonon scatte…
Multi-electron semiconductor quantum dots have found wide application in qubits, where they enable readout and enhance polarizability. However, coherent control in such dots has typically been restricted to only the lowest two levels, and such control in the strongly interacting regime has not been realized. Here we report quantum control of eight different resonances in a silicon-based quantum dot. We use qubit readout to perform spectroscopy, revealing a dense set of energy levels with characteristic spacing far smaller than the single-particle energy. By comparing with full configuration in…
By employing single charge injections with an atomic force microscope, we investigated redox reactions of a molecule on a multilayer insulating film. First, we charged the molecule positively by attaching a single hole. Then we neutralized it by attaching an electron and observed three channels for the neutralization. We rationalize that the three channels correspond to transitions to the neutral ground state, to the lowest energy triplet excited states and to the lowest energy singlet excited states. By single-electron tunneling spectroscopy we measured the energy differences between the tran…
We investigate the temperature dependence of photon coherence properties through two photon interference (TPI) measurements from a single QD under resonant excitation. We show that the loss of indistinguishability is only related to the electron-phonon coupling without being affected by spectral diffusion. Through these measurements, and a complementary microscopic theory, we identify two independent separate decoherence processes each associated to phonons. Below 10K, we find that the relaxation of the vibrational lattice is the dominant contribution to the loss of TPI visibility. This proces…
The geometry-dependent energy transfer rate from an electrically pumped inorganic semiconductor quantum well into an organic molecular layer is studied theoretically. We focus on Förster-type nonradiative excitation transfer between the organic and inorganic layer and include quasi-momentum conservation and intermolecular coupling between the molecules in the organic film. (Transition) partial charges calculated from density-functional theory are used to calculate the coupling elements. The partial charges describe the spatial charge distribution and go beyond the common dipole-dipole interact…
Probing up-conversion electroluminescence of decoupled porphyrin molecules in a plasmonic nanocavity
Max-Planck-Institut für Festkörperforschung（马克斯·普朗克固体研究所）；Institut de Physique, École Polytechnique Fédéral Lausanne（洛桑联邦理工学院物理研究所）；Gleb Wataghin Institute of Physics - University of Campinas - UNICAMP（坎皮纳斯大学格莱布·瓦塔金物理研究所）；Nanjing University（南京大学）
Understanding the movement of charge within organic semiconducting films is crucial for applications in photo-voltaics and flexible electronics. We study the sensitivity of the electrical conductance of a silicon nanowire to changes of charge states within an organic semiconductor physisorbed on the surface of the nanowire. Elastic scattering caused by motion of charge carriers near the nanowire modifies the mean-free path for backscattering of electrons propagating within it, which we have mathematically expressed in terms of the causal Green's functions. The scattering potential has been com…
We optimized the performance of quantum confined Stark effect QCSE based voltage nanosensors. A high throughput approach for single particle QCSE characterization was developed and utilized to screen a library of such nanosensors. Type II ZnSe CdS seeded nanorods were found to have the best performance among the different nanosensors evaluated in this work. The degree of correlation between intensity changes and spectral changes of the excitons emission under applied field was characterized. An upper limit for the temporal response of individual ZnSe CdS nanorods to voltage modulation was char…
