Nanosecond Time Scale Research Articles

Exploring Ultrafast Carrier Dynamics in Photoelectrochemical Water Splitting Using Transient Absorption Spectroscopy

AbstractHydrogen fuel produced from water splitting using sunlight remains one of the cleanest and most sustainable energy sources. However, photoelectrochemical hydrogen production faces several challenges, including poor sunlight absorption, deficient charge carrier lifetime and transfer rates, and very sluggish kinetics of the water oxidation half‐reaction. To address these challenges, researchers have concentrated on enhancing the efficiency of photoelectrochemical water splitting. A critical factor in this enhancement is a deeper understanding of the fundamental processes involved in photoabsorption and the subsequent oxidation evolution reaction. The advent of ultrafast lasers has enabled the detailed tracking of charge carriers within materials after sunlight absorption, including their separation and migration to the surface for water oxidation. Ultrafast transient absorption spectroscopy is a powerful technique that allows real‐time observation of the behavior of excited states and charge carriers on femtosecond to nanosecond timescales. Recent studies utilizing ultrafast transient absorption spectroscopy are explored to investigate the dynamics of charge carriers in photoelectrochemical water splitting, providing insights into the mechanisms that lead to the design of enhanced photoanodes with improved efficiency.

Origin of charges in bulk Si:HfO2 FeFET probed by nanosecond polarization measurements

FeFET technology offers the potential for fast, energy-efficient, low-cost, and high-capacity non-volatile memory and neuromorphic devices. However, charge trapping significantly affects device operation, leading to issues like read-after-write delay and limited endurance. Therefore, a detailed understanding of charge trapping, charge origin and its role in polarization switching is crucial. In this study, we uncover the spectral energy origin of polarization charges in Si:HfO2 N-FeFET by probing electron (conduction band) and hole (valence band) currents separately during polarization-voltage (P–V) measurements. We utilize a fast (∼20 ns) and modified positive-up-negative-down (PUND) technique, where bulk, source, and drain currents of the FeFET are measured separately. The nanosecond timescale of the measurement results in measurable currents in FeFETs having dimensions of a few μm. This charge separation shows that program (PRG, VGS > 0) charge originates from the conduction band, whereas erase (ERS, VGS < 0) originates from the valence band of the Si. Moreover, the polarization curve (P–V) of a cycled device (following 5000 PRG/ERS pulses) shows measurable hysteresis even though the transfer curve of the same device shows that the memory window in the threshold voltage vanishes. Therefore, the FeFET polarization state can be read without delay after write operation by the fast PUND measurement, both for pristine and cycled FeFETs.

Timepix3: single-pixel multi-hit energy-measurement behaviour

The event-driven hybrid-pixel detector readout chip, Timepix3, has the ability to simultaneously measure the time of an event on the nanosecond timescale and the energy deposited in the sensor. However, the behaviour of the system when two events are recorded in quick succession of each other on the same pixel was not studied in detail previously. We present experimental measurements, circuit simulations, and an empirical model for the impact of a preceding event on this energy measurements, which can result in a loss as high as 70%. Accounting for this effect enables more precise compensation, particularly for phenomena like timewalk. This results in significant improvements in time resolution — in the best case, multiple tens of nanoseconds — when two events happen in rapid succession.

Warm-White Light Emission of Lead-free CsAg2I3 Single Crystal Scintillator with a One-Dimensional Electronic Structure.

Presently, the exploration of novel inorganic lead-free perovskite scintillators has emerged as a prominent topic in the field of perovskite materials. Extensive attention has been garnered by materials such as Cs3Cu2I5 due to their notable advantage in scintillation intensity, but the response time constants in the microsecond or even millisecond range severely constrain their potential applications in scintillators. In this study, large-sized (5-6 mm) CsAg2I3 single crystals with an ultrafast warm-white light emission on a nanosecond time scale are presented. Specifically, upon X-ray excitation, the single crystal demonstrates a broad-spectrum white light emission with a color temperature as high as 5129 K, attributed to its self-trapped exciton emission. The 137Cs energy spectrum reveals that CsAg2I3 possesses an ultrafast response for γ rays with a time constant of 15 ns, which is significantly faster than that of Cs3Cu2I5. Furthermore, time-resolved photoluminescence unveils a subnanosecond component with a response time of 0.9 ns. The characteristics of ultrafast warm-white light emission exhibit the significant potential of CsAg2I3 in radiation scintillation detection and its probability of playing a pivotal role in future radiation detection technology.

Accuracy and Reproducibility of Lipari-Szabo Order Parameters From Molecular Dynamics.

The Lipari-Szabo generalized order parameter probes the picosecond to nanosecond time scale motions of a protein and is useful for rationalizing a multitude of biological processes such as protein recognition and ligand binding. Although these fast motions are an important and intrinsic property of proteins, it remains unclear what simulation conditions are most suitable to reproduce methyl symmetry axis side chain order parameter data (Saxis2) from molecular dynamics simulations. In this study, we show that, while Saxis2 tends to converge within tens of nanoseconds, it is essential to run 10 to 20 replicas starting from configurations close to the experimental structure to obtain the best agreement with experimental Saxis2 values. Additionally, in a comparison of force fields, AMBER ff14SB outperforms CHARMM36m in accurately capturing these fast time scale motions, and we suggest that the origin of this performance gap is likely attributed to differences in side chain torsional parametrization and not due to differences in the global protein conformations sampled by the force fields. This study provides insight into obtaining accurate and reproducible Saxis2 values from molecular simulations and underscores the necessity of using replica simulations to compute equilibrium properties.

Mono- and Bichromophores Formed from Perylene Monoimide Diesters: Competition between Intramolecular Charge Transfer and Intermolecular Singlet Exciton Fission.

Perylene monoimide diesters and the corresponding phenyl-linked bichromophores are strongly fluorescent in dilute solution with minimal triplet population after relaxation of the initial Franck-Condon state. The monomer forms nonemissive face-to-face dimers in solution, wherein illumination leads to formation of a spin-correlated, triplet pair with a yield of ca. 13% and with a time constant of 4 ± 1 ps. The triplet pair, which is localized on the aggregate, cannot separate and decays with a mean lifetime of 80 ± 10 ps. The relaxed S1 state of the weakly coupled, phenyl-linked bichromophores establishes an equilibrium with an intramolecular charge-transfer state over a hundred picoseconds or so, depending on the solvent and the geometry of the linkage. This equilibrium mixture, being dominated by the relaxed S1 state, decays on the nanosecond time scale in solution at room temperature without implication of a triplet state. Self-association occurs at higher concentration and, for the para-bridged bichromophore, leads to inefficient triplet formation in tetrahydrofuran at room temperature.

Slow Equilibrium Relaxation in a Chiral Magnet Mediated by Topological Defects.

We performed a pump-probe experiment on the chiral magnet Cu_{2}OSeO_{3} to study the relaxation dynamics of its noncollinear magnetic orders, employing a millisecond magnetic field pulse as the pump and resonant elastic x-ray scattering as the probe. Our findings reveal that the system requires ∼0.2 s to stabilize after the perturbation applied to both the conical and skyrmion lattice phase, which is significantly slower than the typical nanosecond timescale observed in micromagnetics. This prolonged relaxation is attributed to the formation and slow dissipation of local topological defects, such as emergent monopoles. By unveiling the experimental lifetime of these emergent singularities in a noncollinear magnetic system, our study highlights a universal relaxation mechanism in solitonic textures within the slow dynamics regime, offering new insights into topological physics and advanced information storage solutions.

Molecular dynamics simulations of nanoparticle sintering in additive nanomanufacturing: insights from sintering mechanisms

The sintering behavior of nanoparticles (NPs), which determines the quality of additively nanomanufactured products, differs from conventional understanding established for microparticles. As NPs have a high surface-to-volume ratio, they are subjected to a higher influence from surface tension and a lower melting point than microparticles, resulting in variations in both crystallographic defect-mediated and surface diffusion mechanisms. Meanwhile, the interplay between these controlling mechanisms in NPs has not been well understood, primarily because sintering occurs on the nanosecond timescale, making it an exceptionally transient process. In this work, sintering of both equal and unequal sized Ag and Cu NP doublets with and without misorientation (both tilt and twist) is modeled through molecular dynamics (MD) simulations. The formation and evolution of crystallographic defects, such as vacancies, dislocations, stacking faults, twin boundaries, and grain boundaries, during sintering are investigated. The influence of these defects on plastic deformation and diffusion mechanisms, such as volume diffusion and grain boundary (GB) diffusion, is discussed to elucidate the responsible sintering mechanisms. The surface diffusion mechanism is visualized by using detailed atomic trajectories generated during the sintering process. Finally, the overall effectiveness of all diffusion sintering mechanisms is quantified. This study provides first insights into the complexity and dynamics of NP sintering mechanisms which can aid in the development of accurate predictive models.

Degradation induced by charge relaxation in silicone gels under the ultra‐fast pulsed electric field

AbstractThe insulating properties of silicone gel used for silicon carbide‐insulated gate bipolar transistors encapsulation may deteriorate seriously under ultra‐fast pulsed electric fields. The essence of insulation degradation lies in the deterioration of materials caused by dynamic phenomena at microscopic scale, such as charge trapping and detrapping. Different from the steady‐state operating condition, insulating materials exhibit a sharp decrease in their insulating properties when subjected to a rapidly changing electric field. To investigate the insulation failure of silicone gel materials under an ultra‐fast pulsed electric field, Marcus hopping mechanism for charge response is proposed. By calculating the relaxation time with different defects, we characterise the degradation of the materials. According to the force analysis of space charge, the authors establish a relationship between insulation failures and charge relaxation time. Combined with the experimental results on electrical treeing in silicone gel, the feasibility of the theory is verified. The experimental phenomenon can be well explained, that is, the initial voltage of the electrical trees decreased sharply with shortening the edge time of the pulsed electric field, especially on the nanosecond time scale.

Investigation on the vibrational relaxation and ultrafast electronic dynamics of S1 state in 2,4-difluoroanisole.

Intramolecular vibrational energy redistribution (IVR) has a profound impact on dynamic processes. We have studied two types of IVR processes, restricted and dissipative, and ultrafast dynamics of the S1 state of 2,4-difluoroanisole using time-resolved photoelectron spectroscopy and time-of-flight mass spectroscopy. The restricted IVR occurs in the intermediate regime of 219cm-1 vibrational level, and the dissipative IVR occurs in the statistical regime of 1200cm-1. The lifetimes of IVR processes are measured to be 90 and 11ps, respectively, depending on the internal energies of the S1 state and differ by a factor of eight. Similar subsequent dynamics were observed at two vibrational levels in the S1 state. The population undergoes IVR following the initial excitation and subsequently leaks into a triplet state, accompanied by intersystem crossing within ∼400ps followed by a slower nonradiative relaxation of the triplet state on the nanosecond time scale. Furthermore, the values of 3s and 3px Rydberg states of 2,4-difluoroanisole were experimentally determined to be 5.02 and 6.28eV.

Bimetallic AgCo Nanoparticle Synthesis via Combinatorial Nanosecond Laser‐Induced Dewetting of Thin Films

Herein, a combinatorial approach is developed to conduct high‐throughput studies on the nanosecond pulsed laser‐induced dewetting phenomenon of bilayer Ag–Co metallic thin films. Laser irradiation results in the spontaneous rupture of these films in nanosecond timescale, forming bimetallic nanoparticles (NPs) through intermediate stages of hole formation and bicontinuous nanostructures. This approach utilizes bilayer thin films with thickness gradients in both Ag and Co layers (referred to as bigradient samples) while maintaining a constant overall thickness. The laser irradiation on such bigradient bilayer films facilitates control on Ag and Co ratio in the thin films, thus enabling material libraries of Ag–Co NPs covering a large compositional variation. The evolution of NPs with a correlation between NP diameter and interparticle spacings is further studied. The study reveals monotonic increase in NP size and interparticle spacing in Co/Ag bilayer arrangement, while an increase and subsequent decrease in the NP size is observed at 50% Ag in Ag/Co bigradient films. A transition from intermediate stage hole formation to bicontinuous nanostructures with changing composition is also observed. These changes in intermediate stage morphologies and dewetting mechanism are attributed to variation of the free energy of the bilayer system dominated by intermolecular interaction forces.

Molecular Interactions of the Pioneer Transcription Factor GATA3 With DNA.

The GATA3 transcription factor is a pioneer transcription factor that is critical in the development, proliferation, and maintenance of several immune cell types. Identifying the detailed conformational dynamics and interactions of this transcription factor, as well as its clinically important population variants will allow us to unravel its mode of action. In this study, we analyze the molecular interactions of the GATA3 transcription factor bound to dsDNA as well as three clinically important population variants by atomistic molecular dynamics simulations. We identify the effect of the variants on the DNA conformational dynamics and delineate the differences compared to the wildtype transcription factor that could be related to impaired function. We highlight the structural plasticity in the binding of the GATA3 transcription factor and identify important DNA-protein contacts. Although the DNA-protein contacts are persistent and appear to be stable, they exhibit nanosecond timescale fluctuations and several binding/unbinding events. Further, we identify differential DNA binding in the three variants and show that the N-terminal binding is reduced in two of the variants. Our results indicate that reduced minor groove width and DNA diameter are important hallmarks for the binding of GATA3. Our work is an important step towards understanding the functional dynamics of the GATA3 protein and its clinically significant population variants.

Computational screening of the effects of mutations on protein-protein off-rates and dissociation mechanisms by τRAMD

The dissociation rate, or its reciprocal, the residence time (τ), is a crucial parameter for understanding the duration and biological impact of biomolecular interactions. Accurate prediction of τ is essential for understanding protein-protein interactions (PPIs) and identifying potential drug targets or modulators for tackling diseases. Conventional molecular dynamics simulation techniques are inherently constrained by their limited timescales, making it challenging to estimate residence times, which typically range from minutes to hours. Building upon its successful application in protein-small molecule systems, τ-Random Acceleration Molecular Dynamics (τRAMD) is here investigated for estimating dissociation rates of protein-protein complexes. τRAMD enables the observation of unbinding events on the nanosecond timescale, facilitating rapid and efficient computation of relative residence times. We tested this methodology for three protein-protein complexes and their extensive mutant datasets, achieving good agreement between computed and experimental data. By combining τRAMD with MD-IFP (Interaction Fingerprint) analysis, dissociation mechanisms were characterized and their sensitivity to mutations investigated, enabling the identification of molecular hotspots for selective modulation of dissociation kinetics. In conclusion, our findings underscore the versatility of τRAMD as a simple and computationally efficient approach for computing relative protein-protein dissociation rates and investigating dissociation mechanisms, thereby aiding the design of PPI modulators.

Formation mechanism and luminescence properties of silicon carbide nanowires with core-shell structure

For the preparation of SiC nanowires (SiC NWs) by carbothermal reduction, it is of great significance to study the formation mechanism of sic nanowires for process optimization and the controllable preparation. Although first-principles molecular dynamics (FPMD) can simulate systems of hundreds of atoms on a picosecond time scale, the results of FPMD are still insufficient to elucidate the formation mechanism of core-shell SiC nanowires. To make up this deficiency, this article has conducted Deep Potential Molecular Dynamics (DPMD) simulation on nanoseconds timescales with near FPMD accuracy for systems containing thousands of atoms, the results more concretively show the formation process of core-shell SiC nanowires. DPMD simulation results show when CO molecules react with SiO molecules, CO molecules are wrapped by SiO molecules to form agglomerates, SiO molecules in the agglomerates that can come into contact with the wrapped CO molecules will react with wrapped CO molecules to form the SiC core, and SiO molecules that in the outer layer of the agglomerates will disproportionate into the amorphous SiO2 shell. Furthermore, the formation mechanism of SiC nanowires was validated in combination with thermodynamics and experimental methods. Thermodynamic results show that vacuum conditions are favorable for the formation of SiO and CO and lower the temperature of SiC preparation. Finally, the core-shell structure of SiC NWs with good luminescence properties were successfully prepared by carbothermal reduction method using carbon black and silicon dioxide as raw materials under the pressure of less than 5 kPa.

Kernel-Based Minimal Distributed Charges: A Conformationally Dependent ESP-Model for Molecular Simulations.

A kernel-based method (kernelized minimal distributed charge model (kMDCM)) to represent the molecular electrostatic potential (ESP) in terms of off-center point charges is introduced. The positions of the charges adapt to the molecular geometry and allow the description of intramolecular charge flow. Using Gaussian kernels and atom-atom distances as the features, the ESPs for water and methanol are shown to improve by at least a factor of 2 compared with point charge models fit to an ensemble of structures. The conformationally fluctuating molecular dipole moment of water is reproduced almost twice as accurately using kMDCM compared with static PCs, despite not fitting to the dipole directly. The role of hyperparameters in the kernelization is investigated and their implication on model performance and simulation stability is discussed. Combining kMDCM for the electrostatics and reproducing kernels for the bonded terms allows energy-conserving simulations of 2000 water molecules with periodic boundary conditions on the nanosecond time scale. These MD simulations sample geometries outside the training set but remain stable, which demonstrates the robustness of the model and its implementation.

CO2 and NO2 formation on amorphous solid water

Context. The dynamics of molecule formation, relaxation, diffusion, and desorption on amorphous solid water (ASW) is studied in a quantitative fashion. Aims. The formation probability, stabilization, energy relaxation, and diffusion dynamics of CO2 and NO2 on cold ASW following atom+diatom recombination reactions are characterized quantitatively. Methods. Accurate machine-learned energy functions combined with fluctuating charge models were used to investigate the diffusion, interactions, and recombination dynamics of atomic oxygen with CO and NO on ASW. Energy relaxation to the ASW and into water internal degrees of freedom were determined from the analysis of the vibrational density of states. The surface diffusion and desorption energetics were investigated with extended and nonequilibrium MD simulations. Results. The reaction probability is determined quantitatively and it is demonstrated that surface diffusion of the reactants on the nanosecond time scale leads to recombination for initial separations of up to 20 Å. After recombination, both CO2 and NO2 stabilize by energy transfer to water internal and surface phonon modes on the picosecond timescale. The average diffusion barriers and desorption energies agree with those reported from experiments, which validates the energy functions. After recombination, the triatomic products diffuse easily, which contrasts with the equilibrium situation, in which both CO2 and NO2 are stationary on the multinanosecond timescale.

Oxide Derivatives of Nb2CTx MXene and Their Application as Electron Transport Layers in Perovskite Solar Cells: Unraveling the Oxidation Process and Functionalization.

In the realm of photovoltaic research, 2D transition metal carbides (MXenes) have gained significant interest due to their exceptional photoelectric capabilities. However, the instability of MXenes due to oxidation has a direct impact on their practical applications. In this work, the oxidation process of Nb2CTx MXene in aqueous systems is methodically simulated at the atomic level and nanosecond timescales, which elucidates the structural variations influenced by the synergistic effects of water and dissolved oxygen, predicting a transition from metal to semiconductor with 44% C atoms replaced by O atoms in Nb2CTx. Moreover, Nb2CTx with varying oxidation degrees is utilized as electron transport layers (ETLs) in perovskite solar cells (PSCs). Favorable energy level alignments with superior electron transfer capability are achieved by controlled oxidation. By further exploring the composites of Nb2CTx to its derivatives, the strong interaction of the nano-composites is demonstrated to be more effective for electron transport, thus the corresponding PSC achieves a better performance with long-term stability compared with the widely used ETLs like SnO2. This work unravels the oxidation dynamics of Nb2CTx and provides a promising approach to designing ETL by exploiting MXenes to their derivatives for photovoltaic technologies.

An unusual CAr^CNHC- and bidentate NAr^CNHC-cyclometalated Re(I)-NHC complexes with quinoline-functionalized ligands: Syntheses, structures, and blue-luminescent properties

An unusual CAr^CNHC-cyclometalated rhenium(I) tetracarbonyl complexes fac- (CAr^CNHC)Re(CO)4 (13) (the first report) and six NAr^CNHC-cyclometalated rhenium(I) tricarbonyl iodide/chloride complexes with quinoline-functionalized N-heterocyclic carbenes (NHC), fac-Re(CO)3(LNHC)I / fac-Re(CO)3(LNHC)Cl (LNHC = 1-(quinolin-8-yl)-3-methyl-1H-imidazol-2-ylidene (4, 10); 1-(quinolin-8-yl)-4-methyl-1H-1,2,4-triazoline-5-ylidene (5, 11); 1-(quinolin-8-yl)-3-benzyl-1H-imidazol-2-ylidene (6, 12) have been synthesized under controllable reaction conditions and characterized by their 1H NMR, 13C NMR, ESI–MS, IR spectra, and single-crystal X-ray diffraction analysis. X-ray crystallography revealed that the Re(I)-NHC complex 13 is a rare five-member bidentate CAr^CNHC-cyclometalated structure containing the coplanar system of quinoline and imidazole ring with a dihedral angle of 7.6°. The density functional theory (DFT) calculations also indicated that the blue shift of 50 nm for the MLCT absorption band of 13 is in good agreement with the coplanar five-member cyclometalated structure and the Re(I)-NHC complex 10 is a thermodynamic product. Seven Re(I)-NHC complexes exhibit photoluminescence emission in the blue region (410–470 nm) with relatively short decay lifetime on the nanosecond time scale, and high quantum yields of the Re(I)-NHC complexes 5 (Φ = 0.558) and 6 (Φ = 0.629) based-triazole were calculated by using [Ru(bpy)3](PF6)2 in degassed acetonitrile solution (Φstd = 0.062) as standard, due to the coordination of quinoline rings, NHC ligands to Re(I) center.

Charge and Spin Transfer Dynamics in a Weakly Coupled Porphyrin Dimer.

The dynamics of electron and spin transfer in the radical cation and photogenerated triplet states of a tetramethylbiphenyl-linked zinc-porphyrin dimer were investigated, so as to test the relevant parameters for the design of a single-molecule spin valve and the creation of a novel platform for the photogeneration of high-multiplicity spin states. We used a combination of multiple techniques, including variable-temperature continuous wave EPR, pulsed proton electron-nuclear double resonance (ENDOR), transient EPR, and optical spectroscopy. The conclusions are further supported by density functional theory (DFT) calculations and comparison to reference compounds. The low-temperature cw-EPR and room-temperature near-IR spectra of the dimer monocation demonstrate that the radical cation is spatially localized on one side of the dimer at any point in time, not coherently delocalized over both porphyrin units. The EPR spectra at 298 K reveal rapid hopping of the radical spin density between both sites of the dimer via reversible intramolecular electron transfer. The hyperfine interactions are modulated by electron transfer and can be quantified using ENDOR spectroscopy. This allowed simulation of the variable-temperature cw-EPR spectra with a two-site exchange model and provided information on the temperature-dependence of the electron transfer rate. The electron transfer rates range from about 10.0 MHz at 200 K to about 53.9 MHz at 298 K. The activation enthalpies Δ‡H of the electron transfer were determined as Δ‡H = 9.55 kJ mol-1 and Δ‡H = 5.67 kJ mol-1 in a 1:1:1 solvent mixture of CD2Cl2/toluene-d8/THF-d8 and in 2-methyltetrahydrofuran, respectively, consistent with a Robin-Day class II mixed valence compound. These results indicate that the interporphyrin electronic coupling in a tetramethylbiphenyl-linked porphyrin dimer is suitable for the backbone of a single-molecule spin valve. Investigation of the spin density distribution of the photogenerated triplet state of the Zn-porphyrin dimer reveals localization of the triplet spin density on a nanosecond time scale on one-half of the dimer at 20 K in 2-methyltetrahydrofuran and at 250 K in a polyvinylcarbazole film. This establishes the porphyrin dimer as a molecular platform for the formation of a localized, photogenerated triplet state on one porphyrin unit that is coupled to a second redox-active, ground-state porphyrin unit, which can be explored for the formation of high-multiplicity spin states.

Accelerating QM/MM simulations of electrochemical interfaces through machine learning of electronic charge densities.

A crucial aspect in the simulation of electrochemical interfaces consists in treating the distribution of electronic charge of electrode materials that are put in contact with an electrolyte solution. Recently, it has been shown how a machine-learning method that specifically targets the electronic charge density, also known as SALTED, can be used to predict the long-range response of metal electrodes in model electrochemical cells. In this work, we provide a full integration of SALTED with MetalWalls, a program for performing classical simulations of electrochemical systems. We do so by deriving a spherical harmonics extension of the Ewald summation method, which allows us to efficiently compute the electric field originated by the predicted electrode charge distribution. We show how to use this method to drive the molecular dynamics of an aqueous electrolyte solution under the quantum electric field of a gold electrode, which is matched to the accuracy of density-functional theory. Notably, we find that the resulting atomic forces present a small error of the order of 1 meV/Å, demonstrating the great effectiveness of adopting an electron-density path in predicting the electrostatics of the system. Upon running the data-driven dynamics over about 3ns, we observe qualitative differences in the interfacial distribution of the electrolyte with respect to the results of a classical simulation. By greatly accelerating quantum-mechanics/molecular-mechanics approaches applied to electrochemical systems, our method opens the door to nanosecond timescales in the accurate atomistic description of the electrical double layer.