Motional Narrowing Research Articles

Theory and quantum dynamics simulations of exciton-polariton motional narrowing.

The motional narrowing effect has been extensively studied for cavity exciton-polariton systems in recent decades both experimentally and theoretically, which is featured by (1) the subaverage behavior and (2) the asymmetric linewidths for the upper polariton and the lower polariton. However, a minimal theoretical model that is clear and adequate to address all these effects as well as the linewidth scaling relations remains missing. In this work, based on the single mode 1D Holstein-Tavis-Cummings (HTC) model, we studied the motional narrowing effect of the polariton linear absorption spectra via both semi-analytic derivations and numerically exact quantum dynamics simulations using the hierarchical equations of motion approach. The results reveal that under collective light-matter coupling between a cavity mode and N molecules, the polariton linewidth scales as 1/N under the slow limit, while scales as 1/N under the fast limit, due to the polaron decoupling effect. Furthermore, by varying the detunings, the polariton linewidths exhibit significant motional narrowing, covering both characters mentioned above. Our analytic linewidth expressions [Eqs. (34) and (35)] agree well with the numerical exact simulations in all the parameter regimes we explored. These results indicate that the physics of motional narrowing is adequately accounted for by the single-mode 1D HTC model. We envision that both the numerical results and the analytic polariton linewidths expression presented in this work will offer great theoretical value for providing a better understanding of the exciton-polariton motional narrowing based on the HTC model.

Solid-State Lithium Batteries with in-Situ Polymerized Acrylate-Based Electrolytes Capable of Electrochemically Stable Operation at 100 ℃

In-situ polymerized acrylate-based polymers are very appealing as solid polymer electrolytes (SPEs) in lithium (Li) batteries due to the drop-in compatibility of such in-situ polymerization with conventional battery production, the ease of acrylate polymerization and their inexpensive, facile SPE chemistry. We identified, however, that such SPEs suffer from either a low cationic transference number with dual ion conducting salts (0.12-0.2) or a low ionic conductivity with single Li-ion conducting (SLIC) salts (6·10-6 S cm-1). In this project we overcame these limitations and developed significantly improved SPE with ionic conductivity of up to 2·10-4 Scm-1 and a relatively high Li-ion transference number of 0.4. With a significantly reduced fraction of mobile anions in the hybrid SPE, in-situ polymerized SPE cells with an LiFePO4 (LFP) cathode achieve a stable performance for over 100 cycles at temperatures as high as 100 °C, which is unattainable with conventional Li salts or electrolytes. Furthermore, the motional narrowing observed in the line-shapes of solid-state nuclear magnetic resonance (SS-NMR) spectra provided additional insights of the differences in Li nucleus environments and revealed a reduced activation energy for the hybrid salt SPEs due to their more open structure. This study opens the path for the fabrication of high-performance solid polymer lithium batteries capable of operating at high temperatures using commercial battery fabrication equipment. We expect that further tuning of the acrylate based SPE composition may allow further increases in its conductivity without sacrifices in its electrochemical stability or mechanical properties.

Motional narrowing of molecular vibrations strongly coupled to surface lattice resonances

Motional narrowing of molecular vibrations strongly coupled to surface lattice resonances

Motion of Two-Dimensional Excitons in Momentum Space Leads to Pseudospin Distribution Narrowing on the Bloch Sphere.

Motional narrowing implies narrowing induced by motion; for example, in nuclear magnetic resonance, the thermally induced random motion of the nuclei in an inhomogeneous environment leads to a counterintuitive narrowing of the resonance line. Similarly, the excitons in monolayer semiconductors experience magnetic inhomogeneity: the electron-hole spin-exchange interaction manifests as an in-plane pseudomagnetic field with a periodically varying orientation inside the exciton band. The excitons undergo random momentum scattering and pseudospin precession repeatedly in this inhomogeneous magnetic environment, typically resulting in fast exciton depolarization. On the contrary, we show that such magnetic inhomogeneity averages out at high scattering rates due to motional narrowing. Physically, a faster exciton scattering leads to a narrower pseudospin distribution on the Bloch sphere, implying a nontrivial improvement in exciton polarization. The in-plane nature of the pseudomagnetic field enforces a contrasting scattering dependence between the circularly and linearly polarized excitons, providing a spectroscopic way to gauge the sample quality.

Motional Narrowing Effects in the Excited State Spin Populations of Mn-Doped Hybrid Perovskites.

Spin-orbit coupling in the electronic states of solution-processed hybrid metal halide perovskites forms complex spin-textures in the band structures and allows for optical manipulation of the excited state spin-polarizations. Here, we report that motional narrowing acts on the photoexcited spin-polarization in CH3NH3PbBr3 thin films, which are doped at percentage-level with Mn2+ ions. Using ultrafast circularly polarized broadband transient absorption spectroscopy at cryogenic temperatures, we investigate the spin population dynamics in these doped hybrid perovskites and find that spin relaxation lifetimes are increased by a factor of 3 compared to those of undoped materials. Using quantitative analysis of the photoexcitation cooling processes, we reveal increased carrier scattering rates in the doped perovskites as the fundamental mechanism driving spin-polarization-maintaining motional narrowing. Our work reports transition-metal doping as a concept to extend spin lifetimes of hybrid perovskites.

Motional Narrowing through Photonic Exchange: Rational Suppression of Excitonic Disorder from Molecular Cavity Polariton Formation.

Maximizing the coherence between the constituents of molecular materials remains a crucial goal toward the implementation of these systems into everyday optoelectronic technologies. Here we experimentally assess the ability of strong light-matter coupling in the collective limit to reduce energetic disorder using porphyrin-based chromophores in Fabry-Pérot (FP) microresonator structures. Following characterization of cavity polaritons formed from chemically distinct porphyrin dimers, we find that the peaks corresponding to the lower polariton (LP) state in each sample do not possess widths consistent with conventional theories. We model the behavior of the polariton peak widths effectively using the results of spectroscopic theory. We correlate differences in the suppression of excitonic energetic disorder between our samples with microscopic light-matter interactions and propose that the suppression stems from photonic exchange. Our results demonstrate that cavity polariton formation can suppress disorder and show researchers how to design coherence into hybrid molecular material systems.

Spin-EPR-pair separation by conveyor-mode single electron shuttling in Si/SiGe

Long-ranged coherent qubit coupling is a missing function block for scaling up spin qubit based quantum computing solutions. Spin-coherent conveyor-mode electron-shuttling could enable spin quantum-chips with scalable and sparse qubit-architecture. Its key feature is the operation by only few easily tuneable input terminals and compatibility with industrial gate-fabrication. Single electron shuttling in conveyor-mode in a 420 nm long quantum bus has been demonstrated previously. Here we investigate the spin coherence during conveyor-mode shuttling by separation and rejoining an Einstein-Podolsky-Rosen (EPR) spin-pair. Compared to previous work we boost the shuttle velocity by a factor of 10000. We observe a rising spin-qubit dephasing time with the longer shuttle distances due to motional narrowing and estimate the spin-shuttle infidelity due to dephasing to be 0.7% for a total shuttle distance of nominal 560 nm. Shuttling several loops up to an accumulated distance of 3.36 μm, spin-entanglement of the EPR pair is still detectable, giving good perspective for our approach of a shuttle-based scalable quantum computing architecture in silicon.

Investigation of J-Aggregates of 2,3,7,8,12,13,17,18-Octabromo-5,10,15,20-tetrakis(4-sulfonatophenyl) Porphyrin in Aqueous Solutions.

The highly distorted water-soluble 2,3,7,8,12,13,17,18-octabromo-5,10,15,20-tetrakis(4-sulfonatophenyl)porphyrin (Br8TPPS44-) is readily protonated under acidic pH, forming the diacid H2Br8TPPS42- and subsequently the zwitterionic H4Br8TPPS4, which eventually evolves into J-aggregates. These latter species exhibit a relevant bathochromic shift with respect to the monomer with a quite sharp band due to motional narrowing. The depolarization ratio measured in resonant light scattering spectra allows estimating a tilt angle of ~20° of the porphyrins in the J-aggregate. The kinetic parameters are obtained by applying a model based on the initial slow nucleation step, leading to a nucleus containing m monomers, followed by fast autocatalytic growth. The kc values for this latter step increase on decreasing the acid concentration and on increasing the porphyrin concentration, with a strong power-law dependence. No spontaneous symmetry breaking or transfer of chirality from chiral inducers is observed. Both Atomic Force Microscopy (AFM) and Dynamic Light Scattering (DLS) point to the presence, in both the solid and solution phases, of globular-shaped aggregates with sizes close to 130 nm. Density functional theory (DFT) calculations performed on simplified models show that (i) upon protonation, the saddled conformation of the porphyrin ring is slightly altered, and a further rotation of the aryl rings occurs, and (ii) the diacid species is more stable than the parent unprotonated porphyrin. Time-dependent DFT analysis allows comparing the UV/Vis spectra for the two species, showing a consistent red shift upon protonation, even if larger than the experimental one. The simulated Raman spectrum agrees with the experimental spectrum acquired on solid samples.

Nuclear induction lineshape modeling via hybrid SDE and MD approach.

The temperature dependence of the nuclear free induction decay in the presence of a magnetic-field gradient was found to exhibit motional narrowing in gases upon heating, a behavior that is opposite to that observed in liquids. This has led to the revision of the theoretical framework to include a more detailed description of particle trajectories since decoherence mechanisms depend on histories. In the case of free diffusion and single components, the new model yields the correct temperature trends. The inclusion of boundaries in the current formalism is not straightforward. We present a hybrid SDE-MD (stochastic differential equation - molecular dynamics) approach whereby MD is used to compute an effective viscosity and the latter is fed to the SDE to predict the line shape. The theory is in agreement with the experiments. This two-scale approach, which bridges the gap between short (molecular collisions) and long (nuclear induction) timescales, paves the way for the modeling of complex environments with boundaries, mixtures of chemical species, and intermolecular potentials.

Electron Spin Decoherence Dynamics in Magnetic Manganese Hybrid Organic-Inorganic Crystals: The Effect of Lattice Dimensionality.

Organic-inorganic metal hybrids with their tailorable lattice dimensionality and intrinsic spin-splitting properties are interesting material platforms for spintronic applications. While the spin decoherence process is extensively studied in lead- and tin-based hybrids, these systems generally show short spin decoherence lifetimes, and their correlation with the lattice framework is still not well-understood. Herein, we synthesized magnetic manganese hybrid single crystals of (4-fluorobenzylamine)2MnCl4, ((R)-3-fluoropyrrolidinium)MnCl3, and (pyrrolidinium)2MnCl4, which represent a change in lattice dimensionality from 2D and 1D to 0D, and studied their spin decoherence processes using continuous-wave electron spin resonance spectroscopy. All manganese hybrids exhibit nanosecond-scale spin decoherence time τ2 dominated by the symmetry-directed spin exchange interaction strengths of Mn2+-Mn2+ pairs, which is much longer than lead- and tin-based metal hybrids. In contrast to the similar temperature variation laws of τ2 in 2D and 0D structures, which first increase and gradually drop afterward, the 1D structure presents a monotonous rise of τ2 with the temperatures, indicating the strong correlation of spin decoherence with the lattice rigidity of the inorganic framework. This is also rationalized on the basis that the spin decoherence is governed by the competitive contributions from motional narrowing (prolonging the τ2) and electron-phonon coupling interaction (shortening the τ2), both of which are thermally activated, with the difference that the former is more pronounced in rigid crystalline lattices.

Observation of ~100% valley-coherent excitons in monolayer MoS2 through giant enhancement of valley coherence time

In monolayer transition metal dichalcogenide semiconductors, valley coherence degrades rapidly due to a combination of fast scattering and inter-valley exchange interaction. This leads to a sub-picosecond valley coherence time, making coherent manipulation of exciton a highly challenging task. Using monolayer MoS2 sandwiched between top and bottom graphene, here we demonstrate fully valley-coherent excitons by observing ~100% degree of linear polarization in steady state photoluminescence. This is achieved in this unique design through a combined effect of (a) suppression in exchange interaction due to enhanced dielectric screening, (b) reduction in exciton lifetime due to a fast inter-layer transfer to graphene, and (c) operating in the motional narrowing regime. We disentangle the role of the key parameters affecting valley coherence by using a combination of calculation (solutions of Bethe-Salpeter and Maialle-Silva-Sham equations) and a careful choice of design of experiments using four different stacks with systematic variation of screening and exciton lifetime. To the best of our knowledge, this is the first report in which the excitons are found to be valley coherent in the entire lifetime in monolayer semiconductors, allowing optical readout of valley coherence possible.

Zero-field quantum beats and spin decoherence mechanisms in CsPbBr3 perovskite nanocrystals

Coherent optical manipulation of exciton states provides a fascinating approach for quantum gating and ultrafast switching. However, their coherence time for incumbent semiconductors is highly susceptible to thermal decoherence and inhomogeneous broadening effects. Here, we uncover zero-field exciton quantum beating and anomalous temperature dependence of the exciton spin lifetimes in CsPbBr3 perovskite nanocrystals (NCs) ensembles. The quantum beating between two exciton fine-structure splitting (FSS) levels enables coherent ultrafast optical control of the excitonic degree of freedom. From the anomalous temperature dependence, we identify and fully parametrize all the regimes of exciton spin depolarization, finding that approaching room temperature, it is dominated by a motional narrowing process governed by the exciton multilevel coherence. Importantly, our results present an unambiguous full physical picture of the complex interplay of the underlying spin decoherence mechanisms. These intrinsic exciton FSS states in perovskite NCs present fresh opportunities for spin-based photonic quantum technologies.

Blueprint of a Scalable Spin Qubit Shuttle Device for Coherent Mid-Range Qubit Transfer in Disordered Si/SiGe/SiO2

Silicon spin qubits stand out due to their very long coherence times, compatibility with industrial fabrication, and prospect to integrate classical control electronics. To achieve a truly scalable architecture, a coherent mid-range link that moves the electrons between qubit registers has been suggested to solve the signal fan-out problem. Here, we present a blueprint of such a link of 10 μm length, called a spin qubit shuttle, which is based on connecting an array of gates into a small number of sets. To control these sets, only a few voltage control lines are needed and the number of these sets and thus the number of required control signals is independent of the length of this link. We discuss two different operation modes for the spin qubit shuttle: a qubit conveyor, i.e., a potential minimum that smoothly moves laterally, and a bucket brigade, in which the electron is transported through a series of tunnel-coupled quantum dots by adiabatic passage. We find the former approach more promising considering a realistic Si/SiGe device, including potential disorder from the charged defects at the Si/SiO2 layer, as well as typical charge noise. Focusing on the qubit transfer fidelity in the conveyor shuttling mode, we discuss in detail motional narrowing, the interplay between orbital and valley excitation and relaxation in the presence of g factors that depend on orbital and valley state of the electron, and effects from spin hotspots. We find that a transfer fidelity of 99.9% is feasible in Si/SiGe at a speed of approximately 10m/s, if the average valley splitting and its inhomogeneity stay within realistic bounds. Operation at low global magnetic field approximately equal to 20mT and material engineering towards high valley splitting is favorable for reaching high fidelities of transfer.12 MoreReceived 10 March 2022Revised 18 October 2022Accepted 15 February 2023DOI:https://doi.org/10.1103/PRXQuantum.4.020305Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.Published by the American Physical SocietyPhysics Subject Headings (PhySH)Research AreasQuantum information with solid state qubitsQuantum transportSpin coherenceSpin relaxationSurface & interfacial phenomenaPhysical SystemsQuantum dotsSemiconductor compoundsCondensed Matter, Materials & Applied PhysicsQuantum Information

Coherent exciton coupling in fluorescent protein dimers probed by two-photon polarization ratio

Coherent excitonic coupling of two chromophores in a dimer of a GFP-analogue, VenusA206, was discovered previously by using circular dichroism and a combination of photon antibunching and fluorescence correlation spectroscopy. To further elucidate this effect, here we use a new approach based on the measurements of two-photon polarization ratio (Ω) as a function of excitation wavelength. Theoretically, Ω depends on the angle between the vectors of absorption transition dipole moment and permanent dipole moment change upon excitation. Generally, excitonic coupling of two chromophores should provide a change of this angle. We measured Ω for the tandem dimer of Venus (tdV) with two chromophores per protein chain and, as a control - for the tandem dimer with one of the chromophores knocked out by point mutation (tdVx). Compared to tdVx, we observe in tdV a significant increase of Ω in the red side of the pure electronic transition and a significant decrease of Ω in the blue side. At the same time, the two-photon absorption spectra of the two systems virtually coincide. Our observations are consistent with a model where only a minority of dimers are coupled coherently and the two permanent dipoles are oriented in an oblique head-to-head arrangement with an angle ∼400 between them. For multiphoton microscopy applications, it is interesting to investigate if the coherently coupled GFP dimer can provide a cooperative enhancement of the two-photon cross section, i.e., absorb stronger than two uncoupled monomers. This possibility can come from the “motional narrowing” of excitonic transition and will be discussed.

Highly Sensitive and High-Throughput Magnetic Resonance Thermometry of Fluids Using Superparamagnetic Nanoparticles

Magnetic resonance imaging (MRI) enables noninvasive three-dimensional thermometry, which has potential applications in biological tissues and engineering systems. In biological tissues, where MRI is routinely used to monitor temperature during thermal therapies, ${T}_{1}$ or ${T}_{2}$ contrast in water are relatively insensitive to temperature, and techniques with greater temperature sensitivity, such as chemical shift or diffusion imaging, suffer from motional artifacts and long scan times. MR thermometry is not well developed for nonbiological or engineering systems. We describe an approach for highly sensitive and high-throughput MR thermometry that is not susceptible to motional artifacts and could be applied to various biological systems and engineering fluids. We use superparamagnetic iron-oxide nanoparticles (SPIONs) to spoil ${T}_{2}$ of water protons. Motional narrowing results in proportionality between ${T}_{2}$ and the diffusion constant, dependent only on the temperature in a specific environment. Our results show, for pure water, the nuclear magnetic resonance linewidth and ${T}_{2}$ follow the same temperature dependence as the self-diffusion constant of water. Thus, a ${T}_{2}$ mapping is a diffusion mapping in the presence of SPIONs, and ${T}_{2}$ is a thermometer. For pure water, a ${T}_{2}$ mapping of a 64 \ifmmode\times\else\texttimes\fi{} 64 image (voxel size = 0.5 mm \ifmmode\times\else\texttimes\fi{} 0.5 mm \ifmmode\times\else\texttimes\fi{} 3 mm) in a 9.4 T MRI scanner resulted in a temperature resolution of 0.5 K for a scan time of 2 min. This indicates a highly sensitive and high-throughput MR thermometry technique that potentially has a range of applications from thermal management fluids to biological tissues.

Study on Anhydrous Proton Conduction in Imidazole–Collagen Composite

Recently, hydrogen-fuel cells have attracted attention as an environmentally friendly next-generation energy device. Very recently, biomaterials such as collagen and chitin have realized proton conductivity via water bridges under humidity condition, and the fabrication of fuel cells using biomaterials is possible. However, the fuel cell electrolyte via water has demerits, such as the complication of fuel cell instruments and the operating temperature limit. Therefore, fuel cell electrolytes without humidified conditions are desired. In the present work, we have synthesized an anhydrous proton conductor using imidazole and collagen, which are biomaterials, and investigated the anhydrous proton conductivity in imidazole–collagen composites. It was found that an imidazole–collagen composite is a high-proton conductor above 10−3 S/m and above 200 °C without the humidified condition compared with other anhydrous bio-proton conductors such as the hydroxyapatite–collagen composite. Moreover, the motional narrowing of the 1H-NMR line width reveals that the proton conductivity is realized in the temperature region from 120 to 200 °C. In addition, the DTA measurement and the impedance analyses reveal that the imidazole–collagen composite film undergoes the phase transition at 120 °C. Furthermore, the proton conductivity in the imidazole–collagen composite strongly depends on n, which is the imidazole concentration per collagen molecule and takes a maximum at n = 2.0. In addition, the proton conductivity perpendicular to the collagen fiber is approximately ten times higher than that parallel to the collagen fiber. From these results, it can be deduced that the proton conductivity in the imidazole–collagen composite is caused by breaking and rearranging the hydrogen bonds of the collagen side chain with the imidazole molecule formed between the collagen fibers.

Interplay between disorder and collective coherent response: Superradiance and spectral motional narrowing in the time domain

The interplay between static and dynamic disorder and collective optical response in molecular ensembles is an important characteristic of nanoplasmonic and nanophotonic molecular systems. Here we investigate the cooperative superradiant response of a molecular ensemble of quantum emitters under the influence of environmental disorder, including inhomogeneous broadening (as induced by static random distribution of the molecular transition frequencies) and motional narrowing (as induced by stochastic modulation of these excitation energies). The effect of inhomogeneous broadening is to destroy the coherence of the collective molecular excitation and suppress superradiant emission. However, fast stochastic modulation of the molecular excitation energy can effectively restore the coherence of the quantum emitters and lead to a recovery of superradiant emission, which is an unexpected manifestation of motional narrowing. For a light scattering process as induced by an off-resonant incident pulse, stochastic modulation leads to inelastic fluorescence emission at the average excitation energy at long times and suggests that dynamic disorder effects can actually lead to collective excitation of the molecular ensemble.

Rapid water dynamics structures the OH-stretching spectra of solitary water in ionic liquids and dipolar solvents.

In a recent study [J. Phys. Chem. B 126, 4584-4598 (2022)], we have used infrared spectroscopy to investigate the solvation and dynamics of solitary water in ionic liquids and dipolar solvents. Complex shapes observed for water OH-stretching bands, common to all high-polarity solvents, were assigned to water in several solvation states. In the present study, classical molecular dynamics simulations of a single water molecule in four ionic liquids and three dipolar solvents were used to test and refine this interpretation. Consistent with past assignments, simulations show solitary water usually donates two hydrogen bonds to distinct solvent molecules. Such symmetrically solvated water produces the primary pair of peaks identified in the OH spectra of water in nearly all solvents. We had further proposed that additional features flanking this main peak are due to asymmetric solvation states, states in which only one OH group makes a hydrogen bond to solvent. Such states were found in significant concentrations in all of the systems simulated. Simulations of the OH stretching spectra using a semiclassical description and the vibrational map developed by Auer and Skinner [J. Chem. Phys. 128, 224511-224512 (2008)] provided semi-quantitative agreement with experiment. Analysis of species-specific spectra confirmed assignment of the additional features in the experimental spectra to asymmetrically solvated water. The simulations also showed that rapid water motions cause a marked motional narrowing compared with the inhomogeneous limit. This narrowing is largely responsible for making the additional features due to minority solvation states manifest in the spectra.

Anhydrous Proton Conductivity in HAp-Collagen Composite

It is well known that a proton conductor is needed as an electrolyte of hydrogen fuel cells, which are attracting attention as an environmentally friendly next-generation device. In particular, anhydrous proton-conducting electrolytes are highly desired because of their advantages, such as high catalytic efficiency and the ability to operate at high temperatures, which will lead to the further development of fuel cells. In this study, we have investigated the proton-conducting properties of the hydroxyapatite (HAp)-collagen composite without external humidification conditions. It was found that, by injecting HAp into collagen, the electrical conductivity becomes higher than that of the HAp or the collagen. Moreover, the motional narrowing of the proton NMR line is observed above 130 °C. These results indicate that the electrical conductivity observed in the HAp-collagen composite is caused by mobile protons. Furthermore, we measured the proton conduction of HAp-collagen composite films with different HAp contents and investigated the necessity of the appearance of proton conductivity in HAp-collagen composites. HAp content (n = 0–0.38) is the number of HAp per collagen peptide representing Gly-Pro-Hyp. These results indicate that injection of HAp into collagen decreases the activation energy of proton conduction which becomes almost constant above a HAp content n of 0.3. It is deduced that the proton-conduction pathway in the HAp-collagen composite is fully formed above n = 0.3. Furthermore, these results indicate that the value of the activation energy of proton conductivity was lowered, accompanied by the formation of the HAp-collagen composite, and saturated at n > 0.3. From these results, the HAp-collagen composite forms the proton-conduction pathway n > 0.3 and becomes the proton conductor with no external humidification in the condition of n > 0.3 above 130 °C.

Electrically Tunable Localized versus Delocalized Intralayer Moiré Excitons and Trions in a Twisted MoS2 Bilayer.

Moiré superlattice (mSL)-induced sub-bands in twisted van der Waals homo- and heterostructures govern their optical and electrical properties, rendering additional degrees of freedom such as twist angle. Here, we demonstrate the moiré superlattice effects on the intralayer excitons and trions in a twisted bilayer of MoS2 of H-type stacking at marginal twist angles. We identify the emissions from localized and delocalized sub-bands of intralayer moiré excitons and show their electrical modulation by the corresponding trion formation. The electrical control of the oscillator strength of the moiré excitons also results in the strong tunability of resonant Raman scattering. We find that the gate-induced doping significantly modulates the electronic moiré potential; however, leaves the excitonic moiré confinement unaltered. This effect, coupled with variable moiré trap filling by tuning the optical excitation density, allows us to delineate the different phases of localized and delocalized moiré trions. We demonstrate that the moiré excitons exhibit strong valley coherence that changes in a striking nonmonotonic W-shape with gating due to motional narrowing. These observations from the simultaneous electrostatic control of quasiparticle-dependent moiré potential will lead to exciting effects of tunable many-body phenomena in moiré superlattices.