Browse
Submit Data
Databases
API
Help

Dataset Information

0 Views

0 Connections

0 Citations

0 Reanalyses

0 Downloads

Omics score: 0

Influence of the asymmetric excited state decay on coherent population trapping.

ABSTRACT: Electromagnetically induced transparency (EIT) is an optical phenomenon which allows a drastic modification of the optical properties of an atomic system by applying a control field. It has been largely studied in the last decades and nowadays we can find a huge number of experimental and theoretical related studies. Recently a similar phenomenon was also shown in quantum dot molecules (QDM), where the control field is replaced by the tunneling rate between quantum dots. Our results show that in the EIT regime, the optical properties of QDM and the atomic system are identical. However, here we show that in the strong probe field regime, i.e., "coherent population trapping" (CPT) regime, it appears a strong discrepancy on the optical properties of both systems. We show that the origin of such difference relies on the different decay rates of the excited state of the two systems, implying in a strong difference on their higher order nonlinear susceptibilities. Finally, we investigate the optical response of atom/QDM strongly coupled to a cavity mode. In particular, the QDM-cavity system has the advantage of allowing a better narrowing of the width of the dark state resonance in the CPT regime when compared with atom-cavity system.

SUBMITTER: Borges HS

PROVIDER: S-EPMC5541112 | biostudies-other | 2017 Aug

REPOSITORIES: biostudies-other

ACCESS DATA

Json Xml

Similar Datasets

Coherent population trapping by dark state formation in a carbon nanotube quantum dot.

Project description:Illumination of atoms by resonant lasers can pump electrons into a coherent superposition of hyperfine levels which can no longer absorb the light. Such superposition is known as a dark state, because fluorescent light emission is then suppressed. Here we report an all-electric analogue of this destructive interference effect in a carbon nanotube quantum dot. The dark states are a coherent superposition of valley (angular momentum) states which are decoupled from either the drain or the source leads. Their emergence is visible in asymmetric current-voltage characteristics, with missing current steps and current suppression which depend on the polarity of the applied source-drain bias. Our results demonstrate coherent-population trapping by all-electric means in an artificial atom.

| S-EPMC6343009 | biostudies-literature

Excited-State Decay Paths in Tetraphenylethene Derivatives.

Project description:The photophysical properties of tetraphenylethene (TPE) compounds may differ widely depending on the substitution pattern, for example, with regard to the fluorescence quantum yield ϕf and the propensity to exhibit aggregation-induced emission (AIE). We report combined electronic structure calculations and nonadiabatic dynamics simulations to study the excited-state decay mechanisms of two TPE derivatives with four methyl substituents, either in the meta position (TPE-4mM, ϕf = 0.1%) or in the ortho position (TPE-4oM, ϕf = 64.3%). In both cases, two excited-state decay pathways may be relevant, namely, photoisomerization around the central ethylenic double bond and photocyclization involving two adjacent phenyl rings. In TPE-4mM, the barrierless S1 cyclization is favored; it is responsible for the ultralow fluorescence quantum yield observed experimentally. In TPE-4oM, both the S1 photocyclization and photoisomerization paths are blocked by non-negligible barriers, and fluorescence is thus feasible. Nonadiabatic dynamics simulations with more than 1000 surface hopping trajectories show ultrafast cyclization upon photoexcitation of TPE-4mM, whereas TPE-4oM remains unreactive during the 1 ps simulations. We discuss the chances for spectroscopic detection of the postulated cyclic photoproduct of TPE-4mM and the relevance of our findings for the AIE process.

| S-EPMC5385518 | biostudies-literature

New Insights into the State Trapping of UV-Excited Thymine.

Project description:After UV excitation, gas phase thymine returns to a ground state in 5 to 7 ps, showing multiple time constants. There is no consensus on the assignment of these processes, with a dispute between models claiming that thymine is trapped either in the first (S?) or in the second (S?) excited states. In the present study, a nonadiabatic dynamics simulation of thymine is performed on the basis of ADC(2) surfaces, to understand the role of dynamic electron correlation on the deactivation pathways. The results show that trapping in S? is strongly reduced in comparison to previous simulations considering only non-dynamic electron correlation on CASSCF surfaces. The reason for the difference is traced back to the energetic cost for formation of a CO ? bond in S?.

| S-EPMC6273395 | biostudies-literature

Tracking excited state decay mechanisms of pyrimidine nucleosides in real time.

Project description:DNA owes its remarkable photostability to its building blocks-the nucleosides-that efficiently dissipate the energy acquired upon ultraviolet light absorption. The mechanism occurring on a sub-picosecond time scale has been a matter of intense debate. Here we combine sub-30-fs transient absorption spectroscopy experiments with broad spectral coverage and state-of-the-art mixed quantum-classical dynamics with spectral signal simulations to resolve the early steps of the deactivation mechanisms of uridine (Urd) and 5-methyluridine (5mUrd) in aqueous solution. We track the wave packet motion from the Franck-Condon region to the conical intersections (CIs) with the ground state and observe spectral signatures of excited-state vibrational modes. 5mUrd exhibits an order of magnitude longer lifetime with respect to Urd due to the solvent reorganization needed to facilitate bulky methyl group motions leading to the CI. This activates potentially lesion-inducing dynamics such as ring opening. Involvement of the 1nπ* state is found to be negligible.

| S-EPMC8671501 | biostudies-literature

Coherent structural trapping through wave packet dispersion during photoinduced spin state switching.

Project description:The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3]2+ compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265?fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.

| S-EPMC5458100 | biostudies-literature

Hydrogen bonding controls excited-state decay of the photoactive yellow protein chromophore.

Project description:We have performed excited-state dynamics simulations of a Photoactive Yellow Protein chromophore analogue in water. The results of the simulations demonstrate that in water the chromophore predominantly undergoes single-bond photoisomerization, rather than double-bond photoisomerization. Despite opposite charge distributions in the chromophore, excited-state decay takes place very efficiently from both single- and double-bond twisted minima in water. Radiationless decay is facilitated by ultrafast solvent reorganization, which stabilizes both minima by specific hydrogen bond interactions. Changing the solvent to the slightly more viscous D(2)O leads to an increase of the excited-state lifetime. Together with previous simulations, the present results provide a complete picture of the effect of the protein on the photoisomerization of the chromophore in PYP: the positive guanidinium group of Arg52 favors double-bond isomerization over single-bond isomerization by lowering the barrier for double-bond isomerization, while the hydrogen bonds with Tyr42 and Glu46 enhance deactivation from the double-bond twisted minimum.

| S-EPMC2749550 | biostudies-literature

Unified Description of Ultrafast Excited State Decay Processes in Epigenetic Deoxycytidine Derivatives.

Project description:Epigenetic DNA modifications play a fundamental role in modulating gene expression and regulating cellular and developmental biological processes, thereby forming a second layer of information in DNA. The epigenetic 2'-deoxycytidine modification 5-methyl-2'-deoxycytidine, together with its enzymatic oxidation products (5-hydroxymethyl-2'-deoxycytidine, 5-formyl-2'-deoxycytidine, and 5-carboxyl-2'-deoxycytidine), are closely related to deactivation and reactivation of DNA transcription. Here, we combine sub-30-fs transient absorption spectroscopy with high-level correlated multiconfigurational CASPT2/MM computational methods, explicitly including the solvent, to obtain a unified picture of the photophysics of deoxycytidine-derived epigenetic DNA nucleosides. We assign all the observed time constants and identify the excited state relaxation pathways, including the competition of intersystem crossing and internal conversion for 5-formyl-2'-deoxycytidine and ballistic decay to the ground state for 5-carboxy-2'-deoxycytidine. Our work contributes to shed light on the role of epigenetic derivatives in DNA photodamage as well as on their possible therapeutic use.

| S-EPMC8607503 | biostudies-literature

All-optical coherent population trapping with defect spin ensembles in silicon carbide.

Project description:Divacancy defects in silicon carbide have long-lived electronic spin states and sharp optical transitions. Because of the various polytypes of SiC, hundreds of unique divacancies exist, many with spin properties comparable to the nitrogen-vacancy center in diamond. If ensembles of such spins can be all-optically manipulated, they make compelling candidate systems for quantum-enhanced memory, communication, and sensing applications. We report here direct all-optical addressing of basal plane-oriented divacancy spins in 4H-SiC. By means of magneto-spectroscopy, we fully identify the spin triplet structure of both the ground and the excited state, and use this for tuning of transition dipole moments between particular spin levels. We also identify a role for relaxation via intersystem crossing. Building on these results, we demonstrate coherent population trapping -a key effect for quantum state transfer between spins and photons- for divacancy sub-ensembles along particular crystal axes. These results, combined with the flexibility of SiC polytypes and device processing, put SiC at the forefront of quantum information science in the solid state.

| S-EPMC4456942 | biostudies-literature

Acoustically induced coherent spin trapping

Project description:Description Simultaneous strain-driven transitions in ground and excited state of spin qubits lead to the coherent trapping of the spin state. Spin centers are promising qubits for quantum technologies. Here, we show that the acoustic manipulation of spin qubits in their electronic excited state provides an approach for coherent spin control inaccessible so far. We demonstrate a giant interaction between the strain field of a surface acoustic wave (SAW) and the excited-state spin of silicon vacancies in silicon carbide, which is about two orders of magnitude stronger than in the ground state. The simultaneous spin driving in the ground and excited states with the same SAW leads to the trapping of the spin along a direction given by the frequency detuning from the corresponding spin resonances. The coherence of the spin-trapped states becomes only limited by relaxation processes intrinsic to the ground state. The coherent acoustic manipulation of spins in the ground and excited state provides new opportunities for efficient on-chip quantum information protocols and coherent sensing.

| S-EPMC8555898 | biostudies-literature

Excited-State Proton-Transfer-Induced Trapping Enhances the Fluorescence Emission of a Locked GFP Chromophore.

Project description:The chemical locking of the central single bond in core chromophores of green fluorescent proteins (GFPs) influences their excited-state behavior in a distinct manner. Experimentally, it significantly enhances the fluorescence quantum yield of GFP chromophores with an ortho-hydroxyl group, while it has almost no effect on the photophysics of GFP chromophores with a para-hydroxyl group. To unravel the underlying physical reasons for this different behavior, we report static electronic structure calculations and nonadiabatic dynamics simulations on excited-state intramolecular proton transfer, cis-trans isomerization, and excited-state deactivation in a locked ortho-substituted GFP model chromophore (o-LHBI). On the basis of our previous and present results, we find that the S1 keto species is responsible for the fluorescence emission of the unlocked o-HBI and the locked o-LHBI species. Chemical locking does not change the parts of the S1 and S0 potential energy surfaces relevant to enol-keto tautomerization; hence, in both chromophores, there is an ultrafast excited-state intramolecular proton transfer that takes only 35 fs on average. However, the locking effectively hinders the S1 keto species from approaching the keto S1/S0 conical intersections so that most of trajectories are trapped in the S1 keto region for the entire 2 ps simulation time. Therefore, the fluorescence quantum yield of o-LHBI is enhanced compared with that of unlocked o-HBI, in which the S1 excited-state decay is efficient and ultrafast. In the case of the para-substituted GFP model chromophores p-HBI and p-LHBI, chemical locking hardly affects their efficient excited-state deactivation via cis-trans isomerization; thus, the fluorescence quantum yields in these chromophores remain very low. The insights gained from the present work may help to guide the design of new GFP chromophores with improved fluorescence emission and brightness.

| S-EPMC4750082 | biostudies-literature

OmicsDI is part of the ELIXIR infrastructure

OmicsDI is an Elixir interoperability service. Learn more ›

Tweets

OmicsDI Databases

PRIDE
PeptideAtlas
MassIVE
JPOST Repository
Physiome Model Repository

EGA
EVA
ENA
LINCS
PAXDB
Cell Collective

MetaboLights
Metabolomics Workbench
MetabolomeExpress
GNPS
BioModels
FAIRDOMHub

ArrayExpress
dbGaP
ExpressionAtlas
GEO
NODE

Information

Databases
Help
API
Contact us
Code on GitHub
Terms of use
Submit Data