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DOE OSTI2020

Photoinduced charge transfer in transition metal dichalcogenide heterojunctions – towards next generation energy technologies

Increasing interest in using two-dimensional transition metal dichalcogenides (2D TMDCs) in optical energy conversion technologies creates a demand for improving the yields and lifetimes of photogenerated charge carriers. Despite inherently fast photocarrier decay in neat 2D TMDCs, the unique photophysics in these quantum-confined systems motivates continued effort to control the evolution of photoexcited states and create functional devices. Here, an intriguing strategy to accomplish this goal is to employ TMDCs in heterojunctions with appropriate semiconductors, where energy level offsets drive photoinduced charge transfer (PCT) across material interfaces. PCT in TMDC-based systems can be optimized for many different applications, such as driving free carriers to photocatalytic sites for redox reactions like water splitting, extracting charge to perform work in photovoltaics or photodetectors, and manipulating the spin and momentum valley electronic degrees of freedom for quantum computing systems. Here, we review recent strides in optimizing PCT for such applications through greater fundamental understanding of the photophysics that occurs at TMDC/semiconductor interfaces. After giving an overview of isolated TMDC properties, synthetic methods, and the basics of PCT, we discuss TMDCs in heterojunctions with several classes of materials, including other TMDCs, small molecule semiconductors, polymers, single-walled carbon nanotubes, quantum dots, perovskites, and electrolytes. In addition to highlighting the unique benefits of each materials category, we also identify parallels across common themes, such as the roles of charge-transfer states, spin, electronic coupling, delocalization, interfacial atomic morphology, and the precise design of energy landscapes to direct charge and energy motion. We hope to capture a broad range of the valuable work in this fast-paced field to inspire new research directions for employing PCT in targeted TMDC-based systems.

30 DIRECT ENERGY CONVERSION↗

NASA NTRS2019

Investigation of Transient Gas Phase Column Density Due to Droplet Evaporation

A NASA robotic refueling mission experiment on board the International Space Station (ISS) was designed to repeatedly transfer simulated cryogenic propellant between two dewars. After each metered transfer, the cryogen was to be vented overboard via sublimation or evaporation. ISS payload providers must conduct analyses to demonstrate that any planned gaseous venting generate no more than a certain level of material that may interfere with optical measurements from other payloads that may be located nearby. This requirement is expressed in terms of a maximum column number density (CND). For the experiment under consideration, fluid droplets likely would accompany any such vapor. Earlier related studies led to development of analytical expressions for column density along general paths for a number of practical cases under steady conditions, including droplet evaporation. These expressions are not appropriate for rapid evaporation of small droplets however, since the droplets cannot sustain mass flow rates consistent with steady conditions. In this work, analytical expressions are developed for estimating column density near a rapidly evaporating droplet along general paths. The influence for instantaneous evaporation is created first as a limiting case, where it is found the peak value occurs at the time it takes a wave of vapor to reach the closest point along the optical path traveling at its most probable thermal speed. Next, the case for finite-period evaporation is evaluated for constant conditions. Compared to the instantaneous case, peak column density occurs shortly after droplet extinction, but at a lower intensity. A new mathematical function is discovered that solves the integrals associated with this case. Finally, ways to account for droplet motion and changes in evaporation rate with size and temperature are discussed in this framework.

Woronowicz, M. S.↗

NASA NTRS1999

Cloud Thickness from Diffusion of Lidar Pulses in Clouds

Measurements of the distribution of reflected light from a laser beam incident on an aqueous suspension of particles or "cloud" with known thickness and particle size distribution are reported. The distribution is referred to as the "cloud radiative Green's function", G. In the diffusion domain, G is sensitive to cloud thickness, allowing that important quantity to be retrieved. The goal of the laboratory simulation is to provide preliminary estimates of sensitivity of G to cloud thickness,for use in the optimal design of an offbeam Lidar instrument for remote sensing of cloud thickness (THOR, Thickness from Offbeam Returns). These clouds of polystyrene microspheres suspended in water are analogous to real clouds of water droplets suspended in air. The microsphere size distribution is roughly lognormal, from 0.5 microns to 25 microns, similar to real clouds. Density of suspended spheres is adjusted so mean-free-path of visible photons is about 10 cm, approximately 1000 times smaller than in real clouds. The light source is a ND:YAG laser at 530 nm. Detectors are flux and photon-counting Photomultiplier Tube (PMTS), with a glass probe for precise positioning. A Labview 5 VI controls positioning, and data acquisition, via an NI Motion Control board connected to a stepper motor driving an Edmund linear slider, and a 16-channel 16-bit NI-DAQ board. The stepper motor is accurate to 10 microns, and step size is selectable from the VI software. Far from the incident beam, the rate of exponential increase as the direction of the incident beam is approached scales as expected from diffusion theory, linearly with the cloud thickness, and inversely as the square root of the reduced optical thickness, and is independent of particle size. Near the beam the signal begins to increase faster than exponential, due to single and low-order scattering near the backward direction, and here the distribution depends on particle size. Results are being used to verify 3D Monte Carlo radiative transfer simulations, used to estimate signal-to-noise ratios for remotely sensed off beam returns, for both homogeneous and inhomogeneous clouds. Signal-to-noise estimates show that unfiltered observations are straight forward at night, while narrow band pass filters are being studied for day.

Cahalan, Robert F.↗

NASA NTRS2014

Improving Sensorimotor Adaptation Following Long Duration Space Flight by Enhancing Vestibular Information Transfer

Crewmember adapted to the microgravity state may need to egress the vehicle within a few minutes for safety and operational reasons after gravitational transitions. The transition from one sensorimotor state to another consists of two main mechanisms: strategic and plastic-adaptive and have been demonstrated in astronauts returning after long duration space flight. Strategic modifications represent "early adaptation" - immediate and transitory changes in control that are employed to deal with short-term changes in the environment. If these modifications are prolonged then plastic-adaptive changes are evoked that modify central nervous system function, automating new behavioral responses. More importantly, this longer term adaptive recovery mechanism was significantly associated with their strategic ability to recover on the first day after return to Earth G. We are developing a method based on stochastic resonance to enhance information transfer by improving the brain's ability to detect vestibular signals (Vestibular Stochastic Resonance, VSR) especially when combined with balance training exercises such as sensorimotor adaptability (SA) training for rapid improvement in functional skill, for standing and mobility. This countermeasure to improve detection of vestibular signals is a stimulus delivery system that is wearable/portable providing low imperceptible levels of white noise based binaural bipolar electrical stimulation of the vestibular system (stochastic vestibular stimulation). To determine efficacy of vestibular stimulation on physiological and perceptual responses during otolith-canal conflicts and dynamic perturbations we have conducted a series of studies: We have shown that imperceptible binaural bipolar electrical stimulation of the vestibular system across the mastoids enhances balance performance in the mediolateral (ML) plane while standing on an unstable surface. We have followed up on the previous study showing VSR stimulation improved balance performance in both ML and anteroposterior planes while stimulating in the ML axis only. We have shown the efficacy of VSR stimulations on enhancing physiological and perceptual responses of whole-body orientation during low frequency perturbations (0.1 Hz) on the ocular motor system using a variable radius centrifuge on both physiological (using eye movements) and perceptual responses (using a joystick) to track imposed oscillations. The variable radius centrifuge provides a selective tilting sensation that is detectable only by the otolith organs providing conflicting information from the canal organs of the vestibular system (intra-vestibular conflict). These results indicate that VSR can improve performance in sensory conflict scenarios like that experienced during space flight. We have showed the efficacy of VSR stimulation to improve balance and locomotor control on subjects exposed to continuous, sinusoidal lateral motion of the support surface while walking on a treadmill while viewing perceptually matched linear optic flow. We have shown the safety of short term continuous use of up to 4 hours of VSR stimulation and its efficacy in improving balance and locomotor function in Parkinson's Disease patients. This technique for improving vestibular signal detection may thus provide additional information to improve strategic abilities. We hypothesize that VSR stimulation will act synergistically with SA training to improve adaptability by increased utilization of vestibular information and therefore serve to optimize and personalize the SA countermeasure prescription. This forms the basis of its usefulness both as a training modality and further help in significantly reducing the number of days required to recover functional performance to preflight levels after long duration space flight.

Mulavara, A. P.↗

DOE OSTI2026

Ultrafast solvent-to-solute proton transfer mediated by intermolecular coherent vibrations

Ultrafast photoinduced excited-state proton transfer (ESPT) plays a crucial role in protecting biomolecules and functional materials from photodamage. However, the influence of solute-solvent interactions on ESPT dynamics remains under active investigation. Here, we present an ultrafast spectroscopic study of ESPT in the photobase 2-(2´-pyridyl)benzimidazole (PBI) in methanol. Ultrafast absorption spectroscopy, supported by quantum chemical calculations, reveals three distinct kinetic steps: (1) a 2.2 ps solvent-to-solute proton transfer, (2) subsequent nonradiative relaxation to the ground state within 31 ps, producing a vibrationally hot ensemble with substantial excess kinetic energy, and (3) equilibration as this energy dissipates into the surrounding solvent bath over 186 ps. Femtosecond-resolved dynamics exhibit oscillatory signals indicative of coherent wavepacket motion on the S 1 potential energy surface. A phase flip in the excited-state absorption maximum confirms this assignment. Fourier analysis resolves two dominant periods (∼117 fs and ∼340 fs), corresponding to in-plane and out-of-plane vibrational modes coupled between PBI and the hydrogen-bonded methanol molecule. The rapid dephasing ( < 300 fs) suggests that the nuclear wavefunction evolves on an anharmonic potential energy surface while traversing the ESPT reaction coordinate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Chapter 14: Surface plasmon resonance enhanced artificial photosynthesis of chemical fuels for energy storage

Nanostructured noble metals such as Au, Ag, and Cu have interesting optical properties because of the oscillation motions of their surface electrons upon strong coupling with light under resonance conditions. This resonant oscillation motion of conduction electrons refers to surface plasmon resonance (SPR) and localized SPR (LSPR) when localized near the surface of a nanoparticle. The extinction spectrum of a solution of plasmonic nanoparticles has tunable wavelength responses from UV to NIR due to strong light scattering and absorption which are highly sensitive to the permittivity of the nanoparticles, their sizes and shapes, and chemical environment. Strong light scattering due to the LSPR of plasmonic nanoparticles creates a strong localized and far-field intensity capable of enhancing light absorption characteristics of a chromophore near a plasmonic surface. Engineering the chromophores’ radiative decay dynamics can be done by 1) increasing its radiative decay rate to increase its photoluminescence intensity and 2) increasing its nonradiative decay rates associated to direct charge transfer to the metal surface. Such interesting photophysical properties of a chromophore can be extended to other light-absorbing materials such as semiconductor thin films and nanostructures. This plasmonic effect on the photophysics of a light-absorbing material can be theoretically and experimentally validated. The phenomenon has also been applied to advanced optoelectronic devices such as organic light-emitting diodes (OLED)1 and organic photovoltaics (OPV).2-4 The local field created by the SPR can provide an intense EM field to enhance photoluminescence emission of an organic chromophore5-8 and Raman scattering of an organic molecule, and single-molecule Raman9-10 can be detected on specially designed LSPR substrate. (Figure 1 on SPR for energy) Recent studies suggest that LSPR can be incorporated in light-harvesting and conversion systems to increase energy conversion in a solar cell and photoelectrochemical cell and chemical transformations of CO2 to chemical fuels.11-12 Plasmonic active metals naturally exhibit catalytic activities for electrochemical fuel conversion that can be enhanced by engineering their structures to form unique catalytic structures such as symmetry-broken Au-Cu Janus nanocrystals.13 These studies are critical to addressing the global challenges of energy14-15 and CO2 emission from nonrenewable sources such as coal, petroleum, and natural gas.16-17 Electrochemical systems comprised of unique photonic structures and functions that enable efficient and affordable energy harvesting/conversion/storage are highly desired for providing safe and environment-friendly energy sources. This chapter reviews our recent work of LSPR enabled photoelectrochemical water splitting and recent advances in LSPR-enabled CO2 reduction and photochemical reactions reported in the literature. Scientific and technical challenges of applying LSPR to enhance these energy conversion and storage systems are discussed at the conclusion of this chapter.

Pan, Shanlin↗