Conditions for excited-state Raman and absorption processes during optical pumping

1981 ◽  
Vol 59 (18) ◽  
pp. 2792-2802 ◽  
Author(s):  
B. Halperin ◽  
J. A. Koningstein
Keyword(s):  
Excited State ◽  
Excited States ◽  
Optical Pumping ◽  
Excited Level ◽  
Tunable Laser ◽  
Laser Wavelength ◽  
Photon Flux ◽  
Optical Pump ◽  
Linear Behaviour ◽  
Transmission Studies

A theoretical analysis is presented for conditions of optical pumping of an electronic excited state and the subsequent induction of Raman scattering thereof, using the radiation of a tunable laser with a specific λ for pumping and Raman probing.The analysis shows that the number of excited states created by the optical pump can be estimated as a function of the photon flux from the (non-linear) behaviour of the transmission of the sample at the selected laser wavelength. It is shown that such transmission studies are a prerequisite before attempts are made to record any excited level Raman spectrum.

Time-resolved pulsed-laser Raman studies at the nanosecond level of an aqueous solution of UO2(NO3)2

1982 ◽  
Vol 60 (17) ◽  
pp. 2207-2215 ◽  
Author(s):  
M. Asano ◽  
J. A. Koningstein
Keyword(s):  
Aqueous Solution ◽  
Excited States ◽  
Scattered Light ◽  
Excited Level ◽  
Pulsed Laser ◽  
Population Characteristics ◽  
Optical Pump ◽  
Time Resolved ◽  
Electronic Excited States ◽  
Laser Raman

The pulsed-laser Raman spectrum of aqueous solution of UO2(NO3)2•6H2O is reported. Raman shifts were observed which could be assigned to the v1 mode of the UO2 unit in species (UO2)3(OH),+, (UO2)2(OH)52+, and UO22+. Vibrational ground and excited level transitions were induced, where part of the laser radiation at 22350 cm−1 was used as an optical pump while the remaining part served as Raman probe. The lifetimes of the excited states were 7 μs and 1.5 μs for the trinuclear and dinuclear species, respectively. An analysis of the population characteristics of the ground and electronic excited states of the trinuclear species was performed and compared with the time evolution of the scattered light due to vibrational Raman processes in the ground and electronic excited states

Excited-State Dynamics in the RNA Nucleotide Uridine 5’-Monophosphate Investigated by Femtosecond Broadband Transient Absorption Spectroscopy

2019 ◽  
Author(s):  
Matthew M. Brister ◽  
Carlos Crespo-Hernández
Keyword(s):  
Excited State ◽  
Excited States ◽  
Ground State ◽  
Transient Absorption ◽  
Electronic Energy ◽  
Transient Absorption Spectroscopy ◽  
Electronic Relaxation ◽  
Vibrationally Excited ◽  
Excited State Dynamics ◽  
Π State

<p></p><p> Damage to RNA from ultraviolet radiation induce chemical modifications to the nucleobases. Unraveling the excited states involved in these reactions is essential, but investigations aimed at understanding the electronic-energy relaxation pathways of the RNA nucleotide uridine 5’-monophosphate (UMP) have not received enough attention. In this Letter, the excited-state dynamics of UMP is investigated in aqueous solution. Excitation at 267 nm results in a trifurcation event that leads to the simultaneous population of the vibrationally-excited ground state, a longlived <sup>1</sup>n<sub>O</sub>π* state, and a receiver triplet state within 200 fs. The receiver state internally convert to the long-lived <sup>3</sup>ππ* state in an ultrafast time scale. The results elucidate the electronic relaxation pathways and clarify earlier transient absorption experiments performed for uracil derivatives in solution. This mechanistic information is important because long-lived nπ* and ππ* excited states of both singlet and triplet multiplicities are thought to lead to the formation of harmful photoproducts.</p><p></p>

The Malleable Excited States of Benzothiadiazole Dyes and Investigation of their Potential for Photochemical Control

2019 ◽  
Author(s):  
Caroline C. Warner ◽  
andrea thooft ◽  
Bryan J. Lampkin ◽  
selin demirci ◽  
Brett VanVeller
Keyword(s):  
Excited State ◽  
Excited States ◽  
Polar Solvent ◽  
Nonpolar Solvent ◽  
Photochemical Degradation ◽  
Solvent Lead ◽  
Environmentally Sensitive

<p>A strategy to control the efficiency of a photocleavage reaction based on changing the nature of the excited state is presented. A novel class of photoactive compounds has been synthesized by combining the classical o-nitrobenzyl scaffold with an environmentally sensitive dye, 4-amino-nitrobenzothiazole. Irradiation in a polar solvent lead to an excited state that is inoperative for photochemistry whereas excitation in a nonpolar solvent lead to an excited state that is photochemically active. A photochemical degradation appears to be the preferred process in contrast to the intended photocleavage process.</p>

Excited State Tracking During the Relaxation of Coordination Compounds

2018 ◽  
Author(s):  
Juan Sanz García ◽  
Martial Boggio-Pasqua ◽  
Ilaria Ciofini ◽  
Marco Campetella
Keyword(s):  
Excited State ◽  
Excited States ◽  
Potential Energy Surfaces ◽  
Photochemical Reactions ◽  
Complex Nature ◽  
Electronic Excited States ◽  
Ruthenium Nitrosyl ◽  
State Tracking ◽  
Energy Surfaces ◽  
Electronic Wavefunction

<div>The ability to locate minima on electronic excited states (ESs) potential energy surfaces (PESs) both in the case of bright and dark states is crucial for a full understanding of photochemical reactions. This task has become a standard practice for small- to medium-sized organic chromophores thanks to the constant developments in the field of computational photochemistry. However, this remains a very challenging effort when it comes to the optimization of ESs of transition metal complexes (TMCs), not only due to the presence of several electronic excited states close in energy, but also due to the complex nature of the excited states involved. In this article, we present a simple yet powerful method to follow an excited state of interest during a structural optimization in the case of TMC, based on the use of a compact hole-particle representation of the electronic transition, namely the natural transition orbitals (NTOs). State tracking using NTOs is unambiguously accomplished by computing the mono-electronic wavefunction overlap between consecutive steps of the optimization. Here, we demonstrate that this simple but robust procedure works not only in the case of the cytosine but also in the case of the ES optimization of a ruthenium-nitrosyl complex which is very problematic with standard approaches.</div>

scholarly journals Ground- and excited-state characteristics in photovoltaic polymer N2200

RSC Advances ◽  
2021 ◽  
Author(s):  
Guanzhao Wen ◽  
Xianshao Zou ◽  
Rong Hu ◽  
Jun Peng ◽  
Zhifeng Chen ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Excited State ◽  
Steady State ◽  
Excited States ◽  
Density Functional ◽  
Density Functional Theory Calculations ◽  
Time Dependent ◽  
Functional Theory ◽  
Time Resolved ◽  
Dependent Density

Ground- and excited-states properties of N2200 have been studied by steady-state and time-resolved spectroscopies as well as time-dependent density functional theory calculations.

scholarly journals Theoretical Electronic and Rovibrational Studies for Anions of Interest to the DIBs

2013 ◽  
Vol 9 (S297) ◽  
pp. 344-348 ◽  
Author(s):  
R. C. Fortenberry
Keyword(s):  
Excited State ◽  
Excited States ◽  
State Of The Art ◽  
Spectroscopic Constants ◽  
Coupled Cluster ◽  
Electronic Excitations ◽  
Electronically Excited States ◽  
Coupled Cluster Theory ◽  
Electronically Excited ◽  
Enolate Anion

AbstractThe dipole-bound excited state of the methylene nitrile anion (CH2CN−) has been suggested as a candidate carrier for a diffuse interstellar band (DIB) at 803.8 nm. Its corresponding radical has been detected in the interstellar medium (ISM), making the existence for the anion possible. This work applies state-of-the-art ab initio methods such as coupled cluster theory to reproduce accurately the electronic excitations for CH2CN− and the similar methylene enolate anion, CH2CHO−. This same approach has been employed to indicate that 19 other anions may possess electronically excited states, five of which are valence in nature. Concurrently, in order to assist in the detection of these anions in the ISM, work has also been directed towards predicting vibrational frequencies and spectroscopic constants for these anions through the use of quartic force fields (QFFs). Theoretical rovibrational work on anions has thus far included studies of CH2CN−, C3H−, and is currently ongoing for similar systems.

An acidity scale, [H+]hv, for proton quenching of excited states

1989 ◽  
Vol 67 (2) ◽  
pp. 227-238 ◽  
Author(s):  
J. A. Pincock ◽  
P. R. Redden
Keyword(s):  
Excited State ◽  
Fluorescence Quenching ◽  
Excited States ◽  
Benzyl Alcohols ◽  
Fluorescent Indicator ◽  
Quenching Of Fluorescence ◽  
Acidity Scale

An acidity scale for excited state protonation kinetics in 20% ethanol:80% aqueous sulfuric has been developed using 1-cyano-naphthalene as a fluorescent indicator. The utility of this new scale is demonstrated using the proton quenching of fluorescence of a variety of chromophores. These include 1- and 2-cyanonaphthalenes, 1- and 2-methoxynaphthalenes, benzyl alcohols, toluenes, and 2-vinylnaphthalene. Keywords: acidity scale, fluorescence quenching, excited state basicity.

On the optimality of optical pumping for a closed Λ-system with large decay rates of the intermediate excited state

2021 ◽  
Author(s):  
Dionisis Stefanatos ◽  
Emmanuel Paspalakis
Keyword(s):  
Optimal Control ◽  
Excited State ◽  
Decay Rate ◽  
Optimal Control Theory ◽  
Optical Pumping ◽  
Quantum Information Processing ◽  
Decay Rates ◽  
Population Transfer ◽  
Initial State ◽  
Weakly Coupled

Abstract We use optimal control theory to show that for a closed Λ-system where the excited intermediate level decays to the lower levels with a common large rate, the optimal scheme for population transfer between the lower levels is actually optical pumping. In order to obtain this result we exploit the large decay rate to eliminate adiabatically the weakly coupled excited state, then perform a transformation to the basis comprised of the dark and bright states, and finally apply optimal control to this transformed system. Subsequently, we confirm the optimality of the optical pumping scheme for the original closed Λ-system using numerical optimal control. We also demonstrate numerically that optical pumping remains optimal when the decay rate to the target state is larger than that to the initial state or the two rates are not very different from each other. The present work is expected to find application in various tasks of quantum information processing, where such systems are encountered

Effects of extending the π-conjugation of the acetylide ligand on the photophysics and reverse saturable absorption of Pt(ii) bipyridine bisacetylide complexes

2016 ◽  
Vol 18 (41) ◽  
pp. 28674-28687 ◽  
Author(s):  
Taotao Lu ◽  
Chengzhe Wang ◽  
Levi Lystrom ◽  
Chengkui Pei ◽  
Svetlana Kilina ◽  
...  
Keyword(s):  
Excited State ◽  
Excited States ◽  
Substituent Effect ◽  
Excited State Absorption ◽  
Saturable Absorption ◽  
Reverse Saturable Absorption ◽  
Triplet Excited State ◽  
Near Ir ◽  
Terminal Substituent ◽  
Acetylide Ligand

Extending the acetylide ligand π-conjugation diminishes the terminal substituent effect on the lowest excited states, but expands the triplet excited-state absorption to the near-IR region.

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