Excited-State Relaxation in Group IV Nanocrystals Investigated Using Optical Methods

2015 ◽  
pp. 159-190 ◽  
2020 ◽  
Vol 5 (1) ◽  
Author(s):  
Christopher J. Ciccarino ◽  
Johannes Flick ◽  
Isaac B. Harris ◽  
Matthew E. Trusheim ◽  
Dirk R. Englund ◽  
...  

Abstract Artificial atom qubits in diamond have emerged as leading candidates for a range of solid-state quantum systems, from quantum sensors to repeater nodes in memory-enhanced quantum communication. Inversion-symmetric group IV vacancy centers, comprised of Si, Ge, Sn, and Pb dopants, hold particular promise as their neutrally charged electronic configuration results in a ground-state spin triplet, enabling long spin coherence above cryogenic temperatures. However, despite the tremendous interest in these defects, a theoretical understanding of the electronic and spin structure of these centers remains elusive. In this context, we predict the ground-state and excited-state properties of the neutral group IV color centers from first principles. We capture the product Jahn–Teller effect found in the excited state manifold to second order in electron–phonon coupling, and present a nonperturbative treatment of the effect of spin–orbit coupling. Importantly, we find that spin–orbit splitting is strongly quenched due to the dominant Jahn–Teller effect, with the lowest optically-active 3Eu state weakly split into ms-resolved states. The predicted complex vibronic spectra of the neutral group IV color centers are essential for their experimental identification and have key implications for use of these systems in quantum information science.


2004 ◽  
Vol 108 (14) ◽  
pp. 2576-2582 ◽  
Author(s):  
Tissa Gunaratne ◽  
Vance O. Kennedy ◽  
Malcolm E. Kenney ◽  
Michael A. J. Rodgers

2021 ◽  
Vol 7 (22) ◽  
pp. eabf4741
Author(s):  
Jisu Ryu ◽  
Samuel D. Park ◽  
Dmitry Baranov ◽  
Iva Rreza ◽  
Jonathan S. Owen ◽  
...  

For quantum-confined nanomaterials, size dispersion causes a static broadening of spectra that has been difficult to measure and invalidates all-optical methods for determining the maximum photovoltage that an excited state can generate. Using femtosecond two-dimensional (2D) spectroscopy to separate size dispersion broadening of absorption and emission spectra allows a test of single-molecule generalized Einstein relations between such spectra for colloidal PbS quantum dots. We show that 2D spectra and these relations determine the thermodynamic standard chemical potential difference between the lowest excited and ground electronic states, which gives the maximum photovoltage. Further, we find that the static line broadening from many slightly different quantum dot structures allows single-molecule generalized Einstein relations to determine the average single-molecule linewidth from Stokes’ frequency shift between ensemble absorption and emission spectra.


2001 ◽  
Vol 105 (10) ◽  
pp. 1757-1766 ◽  
Author(s):  
Anna Paola Pelliccioli ◽  
Kevin Henbest ◽  
Gwanghoon Kwag ◽  
Terri R. Carvagno ◽  
Malcolm E. Kenney ◽  
...  

Author(s):  
Ben O. Spurlock ◽  
Milton J. Cormier

The phenomenon of bioluminescence has fascinated layman and scientist alike for many centuries. During the eighteenth and nineteenth centuries a number of observations were reported on the physiology of bioluminescence in Renilla, the common sea pansy. More recently biochemists have directed their attention to the molecular basis of luminosity in this colonial form. These studies have centered primarily on defining the chemical basis for bioluminescence and its control. It is now established that bioluminescence in Renilla arises due to the luciferase-catalyzed oxidation of luciferin. This results in the creation of a product (oxyluciferin) in an electronic excited state. The transition of oxyluciferin from its excited state to the ground state leads to light emission.


Author(s):  
J W Steeds

There is a wide range of experimental results related to dislocations in diamond, group IV, II-VI, III-V semiconducting compounds, but few of these come from isolated, well-characterized individual dislocations. We are here concerned with only those results obtained in a transmission electron microscope so that the dislocations responsible were individually imaged. The luminescence properties of the dislocations were studied by cathodoluminescence performed at low temperatures (~30K) achieved by liquid helium cooling. Both spectra and monochromatic cathodoluminescence images have been obtained, in some cases as a function of temperature.There are two aspects of this work. One is mainly of technological significance. By understanding the luminescence properties of dislocations in epitaxial structures, future non-destructive evaluation will be enhanced. The second aim is to arrive at a good detailed understanding of the basic physics associated with carrier recombination near dislocations as revealed by local luminescence properties.


Author(s):  
A. Legrouri

The industrial importance of metal catalysts supported on reducible oxides has stimulated considerable interest during the last few years. This presentation reports on the study of the physicochemical properties of metallic rhodium supported on vanadium pentoxide (Rh/V2O5). Electron optical methods, in conjunction with other techniques, were used to characterise the catalyst before its use in the hydrogenolysis of butane; a reaction for which Rh metal is known to be among the most active catalysts.V2O5 powder was prepared by thermal decomposition of high purity ammonium metavanadate in air at 400 °C for 2 hours. Previous studies of the microstructure of this compound, by HREM, SEM and gas adsorption, showed it to be non— porous with a very low surface area of 6m2/g3. The metal loading of the catalyst used was lwt%Rh on V2Q5. It was prepared by wet impregnating the support with an aqueous solution of RhCI3.3H2O.


Author(s):  
H. Seiler ◽  
U. Haas ◽  
K.H. Körtje

The physical properties of small metal particles reveal an intermediate position between atomic and bulk material. Especially Ag has shown pronounced size effects. We compared silver layers evaporated in high vacuum with cluster layers of small silver particles, evaporated in N2 at a pressure of about 102 Pa. The investigations were performed by electron optical methods (TEM, SEM, EELS) and by Photoacoustic (PA) Spectroscopy (gas-microphone detection).The observation of cluster layers with TEM and high resolution SEM show small silver particles with diameters of about 50 nm (Fig. 1 and Figure 2, respectively). The electron diffraction patterns of homogeneous Ag layers and of cluster layers are similar, whereas the low loss EELS spectra due to plasmon excitation are quite different. Fig. 3 and Figure 4 show first results of EELS spectra of a cluster layer of small silver particles on carbon foil and of a homogeneous Ag layer, respectively.


Author(s):  
E. G. Rightor

Core edge spectroscopy methods are versatile tools for investigating a wide variety of materials. They can be used to probe the electronic states of materials in bulk solids, on surfaces, or in the gas phase. This family of methods involves promoting an inner shell (core) electron to an excited state and recording either the primary excitation or secondary decay of the excited state. The techniques are complimentary and have different strengths and limitations for studying challenging aspects of materials. The need to identify components in polymers or polymer blends at high spatial resolution has driven development, application, and integration of results from several of these methods.


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