In this work, different from the commonly explored strategy of incorporating a smaller cation, MA + and Cs into FAPbI 3 lattice to improve efficiency stability, it is revealed that introduction phenylethylammonium iodide (PEAI) perovksite form mixed cation FA x PEA 1–x PbI can effectively enhance both phase ambient stability as well resulting performance derived devices. From our experimental theoretical calculation results, proposed larger capable assembling on surface grain boundaries...

Magic-sized nanoclusters have been implicated as mechanistically relevant intermediates in the synthesis of group III-V quantum dots. Herein we report single-crystal X-ray diffraction structure a carboxylate-ligated indium phosphide magic-sized nanocluster at 0.83 Å resolution. The this cluster, In37P20(O2CR)51, deviates from that known crystal phases and possesses non-stoichiometric, charged core composed series fused 6-membered rings. cluster is completely passivated by bidentate...

The Chronus Quantum (ChronusQ) software package is an open source (under the GNU General Public License v2) infrastructure which targets solution of challenging problems that arise in ab initio electronic structure theory. Special emphasis placed on consistent treatment time dependence and spin wave function, as well inclusion relativistic effects said treatments. In addition, ChronusQ provides support for uniform finite magnetic fields external perturbations through use gauge-including...

ABSTRACT Light‐driven molecular rotary motors are nanometric machines able to convert light into unidirectional motions. Several types of have been developed better respond stimuli, opening new avenues for developing smart materials ranging from nanomedicine robotics. They great importance in the scientific research across various disciplines, but a detailed comprehension underlying ultrafast photophysics immediately after photo‐excitation, that is, Franck–Condon region characterization, is...

Magic-sized clusters (MSCs) can provide valuable insight into the atomically precise progression of semiconductor nanocrystal transformations. We report conversion an InP MSC to a Cd3P2 through cation exchange mechanism and attempt shed light on evolution physical electronic structure during transformation. Utilizing combination spectroscopic (NMR/UV–vis) structural characterization (ICP-OES/MS/PXRD/XPS/PDF) tools, we demonstrate retention original crystal lattice as Z-type ligand initially...

We study the absorption and emission electronic spectra in an aqueous solution of N-methyl-6-oxyquinolinium betaine (MQ), interesting dye characterized by a large change polarity H-bond ability between ground (S0) excited (S1) states. To that end we compare alternative approaches based either on explicit solvent models density functional theory (DFT)/molecular-mechanics (MM) calculations or DFT clusters embedded polarizable continuum (PCM). In first approach (ClMD), spectrum is computed...

Real-time TDDFT electronic dynamics for studying the charge separation mechanisms in donor/acceptor block copolymers.

The formation of polaron pairs is one the important photophysical processes that take place after excitation in semiconducting organic polymers. First-principles Ehrenfest excited-state dynamics a unique tool to investigate ultrafast photoinduced charge carrier and related nonequilibrium involving correlated electron-nuclear dynamics. In this work their dynamical evolution an oligomer seven thiophene units investigated with combined approach first-principles exciton-nuclear wavelet analysis....

We simulated an excited state proton transfer in green fluorescent protein by ab initio dynamics, and examined the reaction mechanism both time frequency domain through a multi resolution wavelet analysis. This original approach allowed us, for first time, to directly compare trends of photoactivated vibrations femtosecond stimulated Raman spectroscopy results, give unequivocal interpretation role played low modes promoting reaction. could attribute main driving force important photoinduced...

We create defects for quantum technologies by using high temperatures and pressures to convert molecularly doped carbon diamond.

Photoinduced charge transfer (CT) excited states and their relaxation mechanisms can be highly interdependent on the environment effects consequent changes in electronic density. Providing a molecular interpretation of ultrafast (subpicosecond) interplay between initial photoexcited such dense manifolds condensed phase is crucial for improving understanding phenomena. Real-time time-dependent density functional theory here method choice to observe density, explicitly propagated an time...

Modern, nonlinear, time-resolved spectroscopic techniques have opened new doors for investigating the intriguing but complex world of photoinduced ultrafast out-of-equilibrium phenomena and charge dynamics. The interaction between light matter introduces an additional dimension, where interplay electronic vibrational dynamics needs most advanced theoretical–computational protocols to be fully understood on molecular scale. In this study, we showcase capabilities ab initio simulation...

The detailed interpretation of time-resolved spectroscopic signals in terms the molecular rearrangement during a photoreaction or photophysical event is one most important challenges both experimental and theoretical chemistry. Here we simulate fluorescence spectrum dye aqueous solution, N-methyl-6-oxyquinolinium betaine, analyze it far IR THz frequency contributions, providing direct connection to specific motions. To obtain this result, build up an innovative general approach based on...

Colored nitrogen-vacancy (NV) centers in nanosize diamonds ($d\ensuremath{\sim}5$ nm) are promising probe materials because their optical transitions sensitive to mechanical, vibrational, and spin changes the surroundings. Here, a linear response time-dependent density functional theory approach is used describe several NV-doped diamond quantum dots (QDs) order investigate size effects on absorption spectra. By computing full spectrum up band-to-band transitions, we analyze both localized...

Pump probe spectroscopy techniques have enabled the direct observation of a variety transient molecular species in both ground and excited electronic states. Time-resolved vibrational is becoming an indispensable tool for investigating photoinduced nuclear dynamics chemical systems all kinds. On other hand, complete picture encoded these spectra cannot be achieved without full temporal description structural relaxation, including explicit time-dependence coordinates that are substantially...

Tractable methods for studying the molecular dynamics of chemical processes driven by electronic nonadiabaticity are highly sought after to provide insight into, example, photochemical reaction mechanisms, collisions, and thermalized band structures. Starting from time-dependent Schrödinger equation a many-body system, direct ab initio trajectory surface-hopping (TSH) method relying on an analytical treatment nonadiabatic couplings between states is developed in this work. An approach that...

This study uses polarization-selective two-dimensional electronic–vibrational (2D EV) spectroscopy to map intramolecular charge transfer in the well-known solar cell dye, [Ru(dcbpy)2(NCS)2]4– (N34–), dissolved water. A static snapshot of vibronic couplings present aqueous N34– is reported. At least three different initially excited singlet metal-to-ligand charge-transfer (MLCT) states are observed be coupled vibrational modes probed lowest energy triplet MLCT state, emphasizing role coupling...

The Green Fluorescent Protein (GFP) is a widely studied chemical system both for its large amount of applications and the complexity excited state proton transfer responsible change in protonation chromophore. A detailed investigation on structure chromophore environment influence form (either neutral or anionic) it crucial importance to understand how these factors could potentially protein function. In this study, we perform computational based analysis ab-initio molecular dynamics...

Vibrational analysis in solution and the theoretical determination of infrared Raman spectra are key importance many fields chemical interest. band dynamics molecules their sensitivity to environment can also be captured by these spectroscopies time dependent version. However, it is often difficult provide an interpretation experimental data at molecular scale, such as mechanisms or processes hidden behind them. In this work, we present a theoretical-computational protocol based on ab initio...

In the search for new therapeutic strategies to contrast SARS-CoV-2, we here studied interaction of polydatin (PD) and resveratrol (RESV)-two natural stilbene polyphenols with manifold, well known biological activities-with Spike, viral protein essential virus entry into host cells, ACE2, angiotensin-converting enzyme present on surface multiple cell types (including respiratory epithelial cells) which is main receptor Spike binding. Molecular Docking simulations evidenced that both...

Electronic properties and absorption spectra are the grounds to investigate molecular electronic states their interactions with environment. Modeling computations required for understanding design strategies of photo-active materials sensors. However, interpretation such demands expensive dealing interplay excited conformational freedom chromophores in complex matrices (i.e., solvents, biomolecules, crystals) at finite temperature. Computational protocols combining time dependent density...

In spite of the large number experimental and theoretical studies, optical absorption trend green fluorescent protein (GFP) chromophore in several environments has not been fully understood. We calculated at same level time dependent density functional theory vertical excitation energy anionic GFP ethanol, dioxane, methanol water solutions. As result, we reproduced for first peaks with 0.015 eV as standard deviation accuracy. This systematic error allowed us to analyze confidence relative...