scholarly journals Confinement Effect of Micro- and Mesoporous Materials on the Spectroscopy and Dynamics of a Stilbene Derivative Dye

2019 ◽  
Vol 20 (6) ◽  
pp. 1316
Author(s):  
Maria di Nunzio ◽  
Ganchimeg Perenlei ◽  
Abderrazzak Douhal
Keyword(s):  
Chemical Properties ◽  
Emission Spectra ◽  
Guest Molecules ◽  
Time Resolved ◽  
Preferential Formation ◽  
J Aggregates ◽  
Confined Media ◽  
A Charge ◽  
Electron Transfer Processes ◽  
Hybrid Complexes

Micro- and mesoporous silica-based materials are a class of porous supports that can encapsulate different guest molecules. The formation of these hybrid complexes can be associated with significant alteration of the physico-chemical properties of the guests. Here, we report on a photodynamical study of a push–pull molecule, trans-4-(dicyanomethylene)-2-methyl-6-(4-dimethylaminostyryl)-4H-pyran (DCM), entrapped within faujasite-type zeolites (HY, NaX, and NaY) and MCM-41 in dichloromethane suspensions. The complex formation gives rise to caged monomers and H- and J-aggregates. Steady-state experiments show that the nanoconfinement provokes net blue shifts of both the absorption and emission spectra, which arise from preferential formation of H-aggregates concomitant with a distortion and/or protonation of the DCM structure. The photodynamics of the hybrid complexes are investigated by nano- to picosecond time-resolved emission experiments. The obtained fluorescence lifetimes are 65–99 ps and 350–400 ps for H- and J-aggregates, respectively, while those of monomers are 2.46–3.87 ns. Evidences for the presence of a charge-transfer (CT) process in trapped DCM molecules (monomers and/or aggregates) are observed. The obtained results are of interest in the interpretation of electron-transfer processes, twisting motions of analogues push–pull systems in confined media and understanding photocatalytic mechanisms using this type of host materials.

scholarly journals Laurdan and Di-4-ANEPPDHQ probe different properties of the membrane

2016 ◽  
Author(s):  
Mariana Amaro ◽  
Francesco Reina ◽  
Martin Hof ◽  
Christian Eggeling ◽  
Erdinc Sezgin
Keyword(s):  
Cell Biology ◽  
Lipid Membrane ◽  
Chemical Properties ◽  
Emission Spectra ◽  
Spectral Shift ◽  
Membrane Lipid ◽  
Time Resolved ◽  
Lipid Packing ◽  
Physico Chemical ◽  
Polarity Sensitive

AbstractLipid packing is a crucial feature of cellular membranes. Quantitative analysis of membrane lipid packing can be achieved using polarity sensitive probes whose emission spectrum depends on the lipid packing. However, detailed insight into the exact mechanism that causes the spectral shift is essential to interpret the data correctly. Here, we analysed frequently used polarity sensitive probes, Laurdan and di-4-ANEPPDHQ, to test whether the underlying physical mechanisms of their spectral shift is the same, thus whether they report on the same physico-chemical properties of the cell membrane. Their steady-state spectra as well as time-resolved emission spectra in solvents and model membranes showed that they probe different properties of the lipid membrane. Our findings are important for the application of these dyes in cell biology.

scholarly journals Probing the interplay between lattice dynamics and short-range magnetic correlations in CuGeO3 with femtosecond RIXS

2021 ◽  
Vol 6 (1) ◽  
Author(s):  
E. Paris ◽  
C. W. Nicholson ◽  
S. Johnston ◽  
Y. Tseng ◽  
M. Rumo ◽  
...  
Keyword(s):  
Short Range ◽  
Degrees Of Freedom ◽  
Time Resolved ◽  
Model Calculations ◽  
Spin Correlations ◽  
Singlet Exciton ◽  
Magnetic Correlations ◽  
Local Lattice ◽  
Frustrated Systems ◽  
A Charge

AbstractInvestigations of magnetically ordered phases on the femtosecond timescale have provided significant insights into the influence of charge and lattice degrees of freedom on the magnetic sub-system. However, short-range magnetic correlations occurring in the absence of long-range order, for example in spin-frustrated systems, are inaccessible to many ultrafast techniques. Here, we show how time-resolved resonant inelastic X-ray scattering (trRIXS) is capable of probing such short-ranged magnetic dynamics in a charge-transfer insulator through the detection of a Zhang–Rice singlet exciton. Utilizing trRIXS measurements at the O K-edge, and in combination with model calculations, we probe the short-range spin correlations in the frustrated spin chain material CuGeO3 following photo-excitation, revealing a strong coupling between the local lattice and spin sub-systems.

scholarly journals A time-domain phase diagram of metastable states in a charge ordered quantum material

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Jan Ravnik ◽  
Michele Diego ◽  
Yaroslav Gerasimenko ◽  
Yevhenii Vaskivskyi ◽  
Igor Vaskivskyi ◽  
...  
Keyword(s):  
Phase Diagram ◽  
Time Domain ◽  
Metastable States ◽  
Scanning Tunneling ◽  
Photon Density ◽  
Tunneling Microscopy ◽  
Equilibrium Conditions ◽  
Time Resolved ◽  
A Charge ◽  
Non Equilibrium

AbstractMetastable self-organized electronic states in quantum materials are of fundamental importance, displaying emergent dynamical properties that may be used in new generations of sensors and memory devices. Such states are typically formed through phase transitions under non-equilibrium conditions and the final state is reached through processes that span a large range of timescales. Conventionally, phase diagrams of materials are thought of as static, without temporal evolution. However, many functional properties of materials arise as a result of complex temporal changes in the material occurring on different timescales. Hitherto, such properties were not considered within the context of a temporally-evolving phase diagram, even though, under non-equilibrium conditions, different phases typically evolve on different timescales. Here, by using time-resolved optical techniques and femtosecond-pulse-excited scanning tunneling microscopy (STM), we track the evolution of the metastable states in a material that has been of wide recent interest, the quasi-two-dimensional dichalcogenide 1T-TaS2. We map out its temporal phase diagram using the photon density and temperature as control parameters on timescales ranging from 10−12 to 103 s. The introduction of a time-domain axis in the phase diagram enables us to follow the evolution of metastable emergent states created by different phase transition mechanisms on different timescales, thus enabling comparison with theoretical predictions of the phase diagram, and opening the way to understanding of the complex ordering processes in metastable materials.

scholarly journals Metal-Organic Framework-Based Stimuli-Responsive Polymers

2021 ◽  
Vol 5 (4) ◽  
pp. 101
Author(s):  
Menglian Wei ◽  
Yu Wan ◽  
Xueji Zhang
Keyword(s):  
Metal Organic Framework ◽  
Chemical Properties ◽  
Stimuli Responsive ◽  
Guest Molecules ◽  
Stimuli Responsive Polymers ◽  
Responsive Polymers ◽  
Reversible Phase Transition ◽  
Metal Organic ◽  
External Stimuli ◽  
Organic Framework

Metal-organic framework (MOF) based stimuli-responsive polymers (coordination polymers) exhibit reversible phase-transition behavior and demonstrate attractive properties that are capable of altering physical and/or chemical properties upon exposure to external stimuli, including pH, temperature, ions, etc., in a dynamic fashion. Thus, their conformational change can be imitated by the adsorption/desorption of target analytes (guest molecules), temperature or pressure changes, and electromagnetic field manipulation. MOF-based stimuli responsive polymers have received great attention due to their advanced optical properties and variety of applications. Herein, we summarized some recent progress on MOF-based stimuli-responsive polymers (SRPs) classified by physical and chemical responsiveness, including temperature, pressure, electricity, pH, metal ions, gases, alcohol and multi-targets.

scholarly journals Synthesis and Photobehavior of a NewDehydrobenzoannulene-Based HOF with Fluorine Atoms: From Solution to Single Crystals Observation

2021 ◽  
Vol 22 (9) ◽  
pp. 4803
Author(s):  
Eduardo Gomez ◽  
Ichiro Hisaki ◽  
Abderrazzak Douhal
Keyword(s):  
Charge Transfer ◽  
Single Crystals ◽  
Parent Compound ◽  
Time Resolved ◽  
Strong Basis ◽  
Triplet Structure ◽  
Carboxylic Groups ◽  
Potential Applications ◽  
A Charge ◽  
Further Development

Hydrogen-bonded organic frameworks (HOFs) are the focus of intense scientific research due their potential applications in science and technology. Here, we report on the synthesis, characterization, and photobehavior of a new HOF (T12F-1(124TCB)) based on a dehydrobenzoannulene derivative containing fluorine atoms (T12F-COOH). This HOF exhibits a 2D porous sheet, which is hexagonally networked via H-bonds between the carboxylic groups, and has an interlayers distance (4.3 Å) that is longer than that of a typical π–π interaction. The presence of the fluorine atoms in the DBA molecular units largely increases the emission quantum yield in DMF (0.33, T12F-COOH) when compared to the parent compound (0.02, T12-COOH). The time-resolved dynamics of T12F-COOH in DMF is governed by the emission from a locally excited state (S1, ~ 0.4 ns), a charge-transfer state (S1(CT), ~ 2 ns), and a room temperature emissive triplet state (T1, ~ 20 ns), in addition to a non-emissive triplet structure with a charge-transfer character (T1(CT), τ = 0.75 µs). We also report on the results using T12F-ester. Interestingly, FLIM experiments on single crystals unravel that the emission lifetimes of the crystalline HOF are almost twice those of the amorphous ones or the solid T12F-ester sample. This shows the relevance of the H-bonds in the photodynamics of the HOF and provides a strong basis for further development and study of HOFs based on DBAs for potential applications in photonics.

scholarly journals The role of spin in the degradation of organic photovoltaics

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Ivan Ramirez ◽  
Alberto Privitera ◽  
Safakath Karuthedath ◽  
Anna Jungbluth ◽  
Johannes Benduhn ◽  
...  
Keyword(s):  
Transient Absorption ◽  
Bulk Heterojunction ◽  
Critical Factor ◽  
Model Systems ◽  
Transient Absorption Spectroscopy ◽  
Triplet States ◽  
Paramagnetic Resonance ◽  
Time Resolved ◽  
A Charge

AbstractStability is now a critical factor in the commercialization of organic photovoltaic (OPV) devices. Both extrinsic stability to oxygen and water and intrinsic stability to light and heat in inert conditions must be achieved. Triplet states are known to be problematic in both cases, leading to singlet oxygen production or fullerene dimerization. The latter is thought to proceed from unquenched singlet excitons that have undergone intersystem crossing (ISC). Instead, we show that in bulk heterojunction (BHJ) solar cells the photo-degradation of C60 via photo-oligomerization occurs primarily via back-hole transfer (BHT) from a charge-transfer state to a C60 excited triplet state. We demonstrate this to be the principal pathway from a combination of steady-state optoelectronic measurements, time-resolved electron paramagnetic resonance, and temperature-dependent transient absorption spectroscopy on model systems. BHT is a much more serious concern than ISC because it cannot be mitigated by improved exciton quenching, obtained for example by a finer BHJ morphology. As BHT is not specific to fullerenes, our results suggest that the role of electron and hole back transfer in the degradation of BHJs should also be carefully considered when designing stable OPV devices.

Optical, electrochemical and third-order nonlinear optical studies of triphenylamine substituted zinc phthalocyanine

2016 ◽  
Vol 20 (08n11) ◽  
pp. 1173-1181 ◽  
Author(s):  
Narra Vamsi Krishna ◽  
Puliparambil Thilakan Anusha ◽  
S. Venugopal Rao ◽  
L. Giribabu
Keyword(s):  
Nonlinear Optical ◽  
Emission Spectra ◽  
Optical Emission ◽  
Soret Band ◽  
Laser Pulses ◽  
Zinc Phthalocyanine ◽  
Third Order ◽  
Time Resolved ◽  
Nlo Properties ◽  
Scan Data

Zinc phthalocyanine possessing triphenylamine at its peripheral position has been synthesized and its optical, emission, electrochemical and third-order nonlinear optical (NLO) properties were investigated. Soret band was broadened due to the presence of triphenylamine moiety. Electrochemical properties indicated that both oxidation and reduction processes were ring centered. Emission spectra were recorded in different solvents and the fluorescence yields obtained were in the range of 0.02–0.17 while the time-resolved fluorescence data revealed radiative lifetimes of typically few ns. Third-order NLO properties of this molecule have been examined using the Z-scan technique with picosecond (ps) and femtoseocnd (fs) pulses. Closed and open aperture Z-scan data were recorded with 2 ps/1 50 fs laser pulses at a wavelength of 800 nm and NLO coefficients were extracted from both the data. Our data clearly suggests the potential of this molecule for photonics applications.

scholarly journals Photoinduced electron transfer processes of single-wall carbon nanotube (SWCNT)–based hybrids

Nanophotonics ◽  
2020 ◽  
Vol 9 (16) ◽  
pp. 4689-4701
Author(s):  
Lili Du ◽  
Wenjuan Xiong ◽  
Wai Kin Chan ◽  
David Lee Phillips
Keyword(s):  
Electron Transfer ◽  
Transient Absorption ◽  
Electronic Materials ◽  
Photophysical Properties ◽  
Functional Materials ◽  
Single Wall Carbon Nanotubes ◽  
Spectroscopic Techniques ◽  
Time Resolved ◽  
Single Wall Carbon ◽  
Electron Transfer Processes

AbstractIn this review, noncovalent functionalization of single-wall carbon nanotubes (SWCNTs) is briefly reviewed. The functional materials summarized here include metalloporphyrin derivatives, biomolecules and conjugated polymers. Notably, time-resolved spectroscopic techniques such as time-resolved fluorescence and transient absorption were employed to directly investigate the electron transfer and recombination processes between the functionalities and the SWCNTs. In addition, Raman spectroscopy is also useful to identify the interaction and the electron transfer direction between both the functionalities and the SWCNTs. An improved understanding of the mechanisms of these SWCNT-based nanohybrids in terms of their structural and photophysical properties can provide more insights into the design of new electronic materials.

scholarly journals Ultrafast manipulation of mirror domain walls in a charge density wave

2018 ◽  
Vol 4 (10) ◽  
pp. eaau5501 ◽  
Author(s):  
Alfred Zong ◽  
Xiaozhe Shen ◽  
Anshul Kogar ◽  
Linda Ye ◽  
Carolyn Marks ◽  
...  
Keyword(s):  
Charge Density ◽  
Charge Density Wave ◽  
Room Temperature ◽  
Domain Walls ◽  
Density Wave ◽  
Charge Ordering ◽  
Time Resolved ◽  
Insulator Metal Transition ◽  
Femtosecond Light Pulse ◽  
A Charge

Domain walls (DWs) are singularities in an ordered medium that often host exotic phenomena such as charge ordering, insulator-metal transition, or superconductivity. The ability to locally write and erase DWs is highly desirable, as it allows one to design material functionality by patterning DWs in specific configurations. We demonstrate such capability at room temperature in a charge density wave (CDW), a macroscopic condensate of electrons and phonons, in ultrathin 1T-TaS2. A single femtosecond light pulse is shown to locally inject or remove mirror DWs in the CDW condensate, with probabilities tunable by pulse energy and temperature. Using time-resolved electron diffraction, we are able to simultaneously track anti-synchronized CDW amplitude oscillations from both the lattice and the condensate, where photoinjected DWs lead to a red-shifted frequency. Our demonstration of reversible DW manipulation may pave new ways for engineering correlated material systems with light.

scholarly journals Spectral properties and photophysics of arylacetylenes in thin films

2014 ◽  
Vol 2 (1) ◽  
Author(s):  
Rebecca Flamini ◽  
Benedetta Carlotti ◽  
Anna Spalletti ◽  
Assunta Marrocchi
Keyword(s):  
Thin Films ◽  
Energy Transfer ◽  
Singlet State ◽  
Excited Singlet ◽  
Acetylene Derivative ◽  
Time Resolved ◽  
Homogeneous Surface ◽  
Blend Films ◽  
J Aggregates ◽  
Emitting Species

AbstractWe report the photobehaviour of a series of eight structurally related arylacetylene derivatives, in solution as well as in pristine and PC61BM blended thin-_lms. The formation of both H- and J-aggregates in the solid state have been demonstrated, and, interestingly, an energy transfer from H-aggregates or/and from residual "unstacked" molecules to J-aggregates has been found, the latter being the only emitting species. The fuorescence quenching by PC61BM at di_erent loadings has been studied in blend films, and it has been found particularly effcient in the case of a symmetrical peripheral substitution of the acetylene derivative core. Preliminary time-resolved measurements in emission (ns resolution) and in absorption (fs resolution) con_rmed the H⟶J energy transfer and underlined the presence of delayed fuorescence from Jaggregates, formed by energy transfer from the long-lived first excited singlet state of H-aggregates. In all cases, a homogeneous surface morphology of thin films.

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