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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 253 records · Page 14
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Multifunctional transitional metal-based phosphide nanoparticles towards improved polysulfide confinement and redox kinetics for highly stable lithium-sulfur batteries

The shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) are the major issues impeding the practical applications of lithium-sulfur batteries (LSBs). Herein, a highly-efficient Ni 2 P electrocatalyst supported on N, P co-doped graphene (Ni 2 P@NPG) is developed via a simple “recrystallization-self-assembly” method to address the above issues. Here, the ultrafine Ni 2 P nanoparticles ensure abundant adsorption-diffusion-conversion interfaces for accelerating LiPSs transformation and Li 2 S deposition, which extremely decreases the accumulation of LiPSs in the electrolyte and therefore prevents the migration of LiPSs. Their superior catalytic performance is demonstrated by reduced Gibbs free energy changes of rate-limiting step based on the systematic theoretical calculations and the reduced shuttle effect is tested by the three-dimensional reconstructions of Raman depth profiles. Benefiting from these synergistic effects, the LSBs with Ni 2 P@NPG modified separators present a superior cycling performance with an average capacity decay rate of 0.048 % per cycle at 1C around the 400 cycles and a high-rate capacity of 731 mAh/g at 2C. Even with a high-sulfur loading of 3.53 mg cm –2 , the cell can still contain a reversible capacity of 809 mAh/g at 0.2C with a remarkable columbic efficiency of 98.4 %.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Horizons of modern molecular dynamics simulation in digitalized solid freeform fabrication with advanced materials

Our ability to shape and finish a component by combined methods of fabrication including (but not limited to) subtractive, additive and/or no theoretical mass-loss/addition during the fabrication is now popularly known as solid free form fabrication. Fabrication of a telescope mirror is a typical example where grinding and polishing processes are first applied to shape the mirror and thereafter an optical coating is usually applied to enhance its optical performance. The area of nanomanufacturing cannot grow without a deep knowledge of the fundamentals of materials and consequently, the use of computer simulations is becoming ubiquitous. This article is intended to introduce the most recent advances in the computation benefit specific to the area of solid free form fabrication as these systems are traversing through the journey of digitalisation and Industry-4.0. Specifically, this article demonstrates that the application of the latest materials modelling approaches, based on techniques such as molecular dynamics, are enabling breakthroughs in applied precision manufacturing techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Tailoring copper current collector roughness and crystallographic orientation to improve lithium plating

Secondary lithium metal batteries are of great interest due to a high theoretical energy density, but rechargeability is limited by the formation of lithium dendrites that lead to internal short circuits and catastrophic cell failure. Mitigating dendrites through uniform current distribution at the current collector is a promising solution to enabling long cycle life of lithium metal electrodes. Here, the impact of copper crystal orientation and roughness on electrochemically deposited lithium morphology is studied. For 50 cycles, the capacity retention from greatest to least followed polycrystalline copper 95 ± 1 % (MC-PC) ≥ 94.55 ± 0.01 % Cu (110) > 93.0 ± 0.4 % Cu(111) > 75.8 ± 0.1 % Cu(100). Cu(100) performed the worst in all cases with shorts occurring frequently before reaching 50 cycles. Cryo-scanning electron microscopy images showed that after 50 cycles, MC-PC Cu had the best lithium morphology, but at early cycles, Cu(111) formed the densest lithium layer. MC-PC Cu had the most uniform lithium nucleation which may have been caused by increased roughness relative to the single crystal samples. When polycrystalline Cu (F-PC) roughness was systematically controlled, the cumulative Coulombic efficiency increased from about 0.3–0.5 with increasing roughness from an Ra of about 10–40 nm. Lastly, plating rates were studied. Slower rates of 0.25 mA/cm 2 exhibited denser lithium morphology in all cases as compared to 0.5 and 1.0 mA/cm 2 , but the relative porosity of Li deposited on the different current collectors depended on the rate applied.

Copper↗
DOE OSTI2025

Particle-based modelling of axisymmetric tandem mirror devices

In this work, we describe the use of a 1D-2V quasi-neutral hybrid electrostatic PIC with Monte-Carlo Coulomb collisions and non-uniform magnetic field to model the parallel transport and confinement in an axisymmetric tandem mirror device. End-plugs, based on simple-mirrors, are positioned at each end of the device and fueled with neutral beams (25 and 100 keV) to produce a sloshing ion population and increase the density of the end-plugs relative to the central cell. Results show the formation of a potential difference barrier between the central cell and the end-plugs. This potential confines a large fraction of the low energy thermal ions in the central cell which would otherwise be lost in a simple mirror, demonstrating the advantage of the beam-driven tandem mirror configuration relative to simple mirrors. In addition, we explore the effect of end-plug electron temperature on the confinement time of the device and compare it with theoretical estimates. Finally, we discuss the limitations of the code in its present form and describe the next logical steps to improve its predictive capability such as a fully nonlinear Fokker–Planck collision operator, multiply nested flux surface solutions and modeling the exhaust region up to the wall.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Control of Catalyst Isomers Using an N -Phenyl-Substituted RN(CH 2 CH 2 P i Pr 2 ) 2 Pincer Ligand in CO 2 Hydrogenation and Formic Acid Dehydrogenation

A novel pincer ligand, i Pr PN Ph P [PhN- (CH 2 CH 2 P i Pr 2 ) 2 ], which is an analogue of the versatile MACHO ligand, iPr PN H P [HN(CH 2 CH 2 P i Pr 2 ) 2 ], was synthesized and characterized. The ligand was coordinated to ruthenium, and a series of hydride-containing complexes were isolated and characterized by NMR and IR spectroscopies, as well as X-ray diffraction. Comparisons to previously published analogues ligated by iPr PN H P and iPr PN Me P [CH 3 N(CH 2 CH 2 P i Pr 2 ) 2 ] illustrate that there are large changes in the coordination chemistry that occur when the nitrogen substituent of the pincer ligand is altered. For example, ruthenium hydrides supported by the iPr PN Ph P ligand always form the syn isomer (where syn/anti refer to the relative orientation of the group on nitrogen and the hydride ligand on ruthenium), whereas complexes supported by iPr PN H P form the anti isomer and complexes supported by iPr PN Me P form a mixture of syn and anti isomers. We evaluated the impact of the nitrogen substituent of the pincer ligand in catalysis by comparing a series of iPr PN R P (R = H, Me, Ph)-ligated ruthenium hydride complexes as catalysts for formic acid dehydrogenation and carbon dioxide (CO 2 ) hydrogenation to formate. The iPr PN Ph P-ligated species is the most active for formic acid dehydrogenation, and mechanistic studies suggest that this is likely because there are kinetic advantages for catalysts that operate via the syn isomer. In CO 2 hydrogenation, the iPr PN Ph P-ligated species is again the most active under our optimal conditions, and we report some of the highest turnover frequencies for homogeneous catalysts. Experimental and theoretical insights into the turnover-limiting step of catalysis provide a basis for the observed trends in catalytic activity. Additionally, the stability of our complexes enabled us to detect a previously unobserved autocatalytic effect involving the base that is added to drive the reaction. Overall, by modifying the nitrogen substituent on the MACHO ligand, we have developed highly active catalysts for formic acid dehydrogenation and CO 2 hydrogenation and also provided a framework for future catalyst development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Mapping charge excitations in generalized Wigner crystals

Transition metal dichalcogenide-based moiré superlattices exhibit strong electron-electron correlations, thus giving rise to strongly correlated quantum phenomena such as generalized Wigner crystal states. Evidence of Wigner crystals in transition metal dichalcogenide moire superlattices has been widely reported from various optical spectroscopy and electrical conductivity measurements, while their microscopic nature has been limited to the basic lattice structure. Theoretical studies predict that unusual quasiparticle excitations across the correlated gap between upper and lower Hubbard bands can arise due to long-range Coulomb interactions in generalized Wigner crystal states. However, the microscopic proof of such quasiparticle excitations is challenging because of the low excitation energy of the Wigner crystal. Here, in this study, we describe a scanning single-electron charging spectroscopy technique with nanometre spatial resolution and single-electron charge resolution that enables us to directly image electron and hole wavefunctions and to determine the thermodynamic gap of generalized Wigner crystal states in twisted WS 2 moiré heterostructures. High-resolution scanning single-electron charging spectroscopy combines scanning tunnelling microscopy with a monolayer graphene sensing layer, thus enabling the generation of individual electron and hole quasiparticles in generalized Wigner crystals. We show that electron and hole quasiparticles have complementary wavefunction distributions and that thermodynamic gaps of ~50 meV exist for the 1/3 and 2/3 generalized Wigner crystal states in twisted WS 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2022

Domain wall enabled steep slope switching in MoS2 transistors towards hysteresis-free operation

Abstract The device concept of ferroelectric-based negative capacitance (NC) transistors offers a promising route for achieving energy-efficient logic applications that can outperform the conventional semiconductor technology, while viable operation mechanisms remain a central topic of debate. In this work, we report steep slope switching in MoS 2 transistors back-gated by single-layer polycrystalline PbZr 0.35 Ti 0.65 O 3 . The devices exhibit current switching ratios up to 8 × 10 6 within an ultra-low gate voltage window of $$V_{{{\mathrm{g}}}} = \pm \! 0.5$$ V g = ± 0.5 V and subthreshold swing (SS) as low as 9.7 mV decade −1 at room temperature, transcending the 60 mV decade −1 Boltzmann limit without involving additional dielectric layers. Theoretical modeling reveals the dominant role of the metastable polar states within domain walls in enabling the NC mode, which is corroborated by the relation between SS and domain wall density. Our findings shed light on a hysteresis-free mechanism for NC operation, providing a simple yet effective material strategy for developing low-power 2D nanoelectronics.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Investigation of SiO x anode fading mechanism with limited capacity cycling

Silicon suboxide (SiO x ) is one of the promising anode materials for the next-generation lithium-ion batteries. However, SiO x has a severe capacity fading problem during cycling. It is thus desired to investigate the detailed fading mechanisms of SiO x anode materials. In this study, limited capacity cycling was employed to examine the electrochemical behaviors of the SiO x anode, and the lithiation/delithiation cycling was limited within a range of 10% theoretical capacity. This strategy minimizes the volume variation of SiO x materials upon charging/discharging, which helps to reveal their decay factors other than volume fluctuation. It is demonstrated that the instability of the SiO x surface during cycling was likely a parallel factor of active material fading, which seems to cause unfavored electrode interface rearrangements with lowered electric conductivity.

electric vehicles↗
DOE OSTI2020

Encoding an Oscillator into Many Oscillators

An outstanding challenge for quantum information processing using bosonic systems is Gaussian errors such as excitation loss and added thermal noise errors. Thus, bosonic quantum error correction is essential. Most bosonic quantum error correction schemes encode a finite-dimensional logical qubit or qudit into noisy bosonic oscillator modes. In this case, however, the infinite-dimensional bosonic nature of the physical system is lost at the error-corrected logical level. On the other hand, there are several proposals for encoding an oscillator mode into many noisy oscillator modes. However, these oscillator-into-oscillators encoding schemes are in the class of Gaussian quantum error correction. Therefore, these codes cannot correct practically relevant Gaussian errors due to the established no-go theorems that state that Gaussian errors cannot be corrected by using only Gaussian resources. Here, we circumvent these no-go results and show that it is possible to correct Gaussian errors by using Gottesman-Kitaev-Preskill (GKP) states as non-Gaussian resources. In particular, we propose a non-Gaussian oscillator-into-oscillators code, namely the GKP two-mode squeezing code, and demonstrate that it can quadratically suppress additive Gaussian noise errors in both the position and momentum quadratures except for a small sublogarithmic correction. Furthermore, we demonstrate that our GKP two-mode squeezing code is near optimal in the weak noise limit by proving via quantum information theoretic tools that quadratic noise suppression is optimal when we use two physical oscillator modes. Lastly, in this work we show that our non-Gaussian oscillator encoding scheme can also be used to correct excitation loss and thermal noise errors, which are dominant error sources in many realistic bosonic systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Implanted Guard Ring Edge Termination With Avalanche Capability for Vertical GaN Devices

Edge termination is the key building block in power devices to enable near-ideal, avalanche breakdown voltage (BV). Here, this work presents the design, fabrication, and physics of a GaN guard ring (GR) edge termination formed by selective-area nitrogen implantation through an epitaxial p-GaN layer. The fabrication of this termination only includes a single implantation step that does not require precise control of implant depth, rendering a large process latitude. The selective-area implantation produces p-GaN rings that are separated by the implanted, semi-insulating regions. The number and spacing of the p-type rings are found to determine the BV of the vertical GaN p-n diode. The 16-ring structure enables a BV of 1800 V, being 88% of the theoretical 1-D parallel-plane limit. Avalanche characteristics are observed in devices with a large variety of GR designs. Finally, we present a comprehensive survey on the efficiency, fabrication complexity, real estate, and avalanche capability of various edge termination techniques that have been reported in vertical GaN devices. The high efficiency (among the highest reported in avalanche-capable GaN terminations), simple and robust fabrication process, and uniform avalanche capability make this implanted GR a promising edge termination for high-voltage GaN devices.

42 ENGINEERING↗
DOE OSTI2022

Physics Guided Simulation of Electrostatic Discharge: Technical Report

Triboelectrically-charged objects may create threshold sparks, electrostatic discharge (ESD) events, to equilibrate charge between themselves and other relatively charged objects. ESD events exhibit many complex physical phenomena. They are a nexus of several fields of physics with disparate characteristic scales: plasma physics, chemical kinetics, hydrodynamics, circuit models, etc. These scales can span many orders of magnitude from the varied collisions thermalizing information within a plasma on the $\mathcal{O}(fs/ps)$ to the physical size of the plasma channel on the $\mathcal{O}(100µm)$, to the speed of a nonlinear hydrodynamic wave propagating at $\mathcal{O}(µm, ns)$. These threshold ESD events may occur in situations of programmatic importance, delivering energy and power profiles to a “victim load” generating deleterious consequences. To predict and mitigate these consequences we must answer questions about the spark’s energy budget: how much energy goes into producing the spark channel; how much gets radiated away; how much energy is advected away into the hydrodynamics; and how much energy is delivered to a victim load. An ESD simulation toolset has been created and evolved in order to answer these questions. An appropriate, physics guided implementation for simulation can be done by gaining insight into its constituent physics and leveraging that intuition to choose a suitable numerical operator. We examine in detail the chemical kinetics, circuit discharge, and hydrodynamics to deter mine dominant regimes, values, timescales, and interactions to uncover the underlying physical dynamics. We also examine and propose model reduction schemes for high-dimensional chemical kinetics. We use past and current work with experimentally validated and theoretically-verified hydrodynamics to calculate applicability limits of the non-ionizing strong shock limit. We quantify the energy budget from a hydrodynamic perspective and demonstrate that a significant fraction of the stored energy is “earmarked” for hydrodynamic advection as an energy terminus. Lastly, we combine the constituent physics of an ESD event (chemical kinetics, circuit model, and hydrodynamics) into a cohesive, actionable toolset and obtain promising results from an isothermal test case. We then propose a viable, modular evolution of the ESD toolset based upon the performed examination of the physics uncovering dominant physical scales and the stiffness of the compositional differential system.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Recent Developments of Tin (II) Sulfide/Carbon Composites for Achieving High-Performance Lithium Ion Batteries: A Critical Review

The ever-increasing worldwide energy demand and the limited resources of fossil have forced the urgent adoption of renewable energy sources. Additionally, concerns over CO 2 emissions and potential increases in fuel prices have boosted technical efforts to make hybrid and electric vehicles more accessible to the public. Rechargeable batteries are undoubtedly a key player in this regard, especially lithium ion batteries (LIBs), which have high power capacity, a fast charge/discharge rate, and good cycle stability, while their further energy density improvement has been severely limited, because of the relatively low theoretical capacity of the graphite anode material which is mostly used. Among various high-capacity anode candidates, tin (II) sulfide (SnS 2 ) has been attracted remarkable attention for high-energy LIBs due to its enormous resource and simplicity of synthesis, in addition to its high theoretical capacity. However, SnS 2 has poor intrinsic conductivity, a big volume transition, and a low initial Coulombic efficiency, resulting in a short lifespan. SnS 2 /carbon composites have been considered to be a most promising approach to addressing the abovementioned issues. Therefore, this review summarizes the current progress in the synthesis of SnS 2 /carbon anode materials and their Li-ion storage properties, with special attention to the developments in Li-based technology, attributed to its immense current importance and promising prospects. Finally, the existing challenges within this field are presented, and potential opportunities are discussed.

25 ENERGY STORAGE↗
DOE OSTI2022

3D Hydrodynamics of Pre-supernova Outbursts in Convective Red Supergiant Envelopes

Eruptive mass loss likely produces the energetic outbursts observed from some massive stars before they become core-collapse supernovae (SNe). The resulting dense circumstellar medium may also cause the subsequent SNe to be observed as Type IIn events. The leading hypothesis of the cause of these outbursts is the response of the envelope of the red supergiant (RSG) progenitor to energy deposition in the months to years prior to collapse. Early theoretical studies of this phenomenon were limited to 1D, leaving the 3D convective RSG structure unaddressed. Using FLASH's hydrodynamic capabilities, we explore the 3D outcomes by constructing convective RSG envelope models and depositing energies less than the envelope binding energies on timescales shorter than the envelope dynamical time deep within them. We confirm the 1D prediction of an outward-moving acoustic pulse steepening into a shock, unbinding the outermost parts of the envelope. However, we find that the initial 2–4 km s -1 convective motions seed the intrinsic convective instability associated with the high-entropy material deep in the envelope, enabling gas from deep within the envelope to escape and increasing the amount of ejected mass compared to an initially "quiescent" envelope. The 3D models reveal a rich density structure, with column densities varying by ≈10× along different lines of sight. Our work highlights that the 3D convective nature of RSG envelopes impacts our ability to reliably predict the outburst dynamics, the amount, and the spatial distribution of the ejected mass associated with deep energy deposition.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Propagation of radio frequency waves through turbulent plasmas

The practical and economic viability of tokamak fusion reactors depends, in a significant way, on the efficiency of radio frequency (RF) waves to deliver energy and momentum to the plasma in the core of the reactor. The RF electromagnetic waves, excited by antenna structures placed near the wall of a tokamak, have to propagate through the turbulent edge plasma along their path to the core of the fusion device. In present day experiments, the radial width of the edge region and scrape-off layer is of the order of a few centimeters. In ITER, and in future fusion reactors, this width will be of the order of tens of centimeters. Any effects on RF waves due to plasma turbulence have to be properly understood in order to optimize the delivery of RF energy and momentum into the core. This paper is on a multi-pronged, theoretical and computational, approach that is being pursued to quantify the effect of edge plasma turbulence on the propagation of RF waves. The theoretical and analytical models are based on solutions of the Faraday-Ampere equation in a magnetized plasma and on the Kirchhoff tangent plane approximation. An effective medium approach has been developed so as to approximate the permittivity of a turbulent plasma by analytical expressions. The computations are being carried out with a newly developed code ScaRF that is based on the finite difference finite domain technique for solving Maxwell's equations. The plasma permittivity can be assigned as desired. The code is being used to validate the analytical and theoretical models and to evaluate their limitations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Probing how Ti- and Nb-substitution affect the stability and improve the electrochemical performance of β- and ε-LiVOPO 4

LiVOPO 4 is a promising next-generation multi-electron cathode material, boasting a theoretical capacity of 305 mA h g -1 , significantly higher than any commercially used Li-ion battery cathode material. However, the material still faces several limitations, including the difficulty in attaining the full theoretical capacity at higher rates and capacity fade over several cycles. Here, in this paper, we show that Ti- and Nb-substitution can be used to improve the thermal stability and electrochemical performance of LiVOPO 4 . We show through in situ heating with XRD and a novel gradient heating technique that both Ti- and Nb-substitution cause β-LiVOPO 4 to be stabilized relative to ε-LiVOPO 4 . This is due to transition-metal substitution, which increases the O-vacancy formation energies, pushing the β → ε transition to higher temperatures. We show that it is still possible to synthesize pure-phase ε-LiVOPO 4 through the use of high temperatures to generate these O-vacancies. We show that even 1% of Ti- or Nb-substitution can improve the initial capacity and long term cycling capability of LiVOPO 4 by improving the high-voltage capacity and reducing the capacity fade in both the high- and low-voltage regions. This is due to the overall improved Li + ion diffusion which is caused by an improved charge-transfer resistance during cycling.

25 ENERGY STORAGE↗
DOE OSTI2026

Observation of Synchronization between Two Quantum van der Pol Oscillators in Trapped Ions

Synchronization is a hallmark of collective behavior that emerges when nonlinear systems interact, spanning scales from mechanical oscillators to planetary orbits. As a universal phenomenon, it underpins the study of complex systems and has far-reaching technological implications. While classical synchronization has a long and rich history, it has not been observed experimentally between multiple quantum limit-cycle oscillators despite a decade of theoretical investigations. We realize synchronization between two quantum van der Pol oscillators by engineering dissipation in a mixed-isotope trapped-ion quantum simulator. The synchronized state is encoded in a fixed relative phase between the oscillators that is inaccessible to individual measurements and revealed only through joint readout of both oscillators, in stark contrast to the system in the (deterministic) classical limit where synchronization can be observed via individual phase measurements. We further show that the relative phase can be precisely controlled and that the chain of two oscillators can synchronize to an external field, suggesting applications in sensing. Our results provide a promising pathway for studying more complex synchronized quantum dynamics beyond two oscillators, where a theoretical treatment becomes increasingly challenging, and it remains to be understood whether genuinely quantum features persist in such cases.

Liu, Jiarui↗
DOE OSTI2025

Time-domain theory of transient heat conduction in the local limit

Ultrafast and nanoscale heat conduction demands a unified theoretical framework that rigorously bridges macroscopic transport equations with microscopic material properties derived from statistical physics. Existing empirical generalizations of Fourier's law often lack a solid microscopic foundation, failing to connect observed non-Fourier behavior with underlying atomic-scale mechanisms. In this work, we present a time-domain theory of transient heat conduction rooted in Zwanzig's statistical theory of irreversible processes. Central to this framework is the time-domain transport function $\overleftrightarrow{𝑍}$⁡(𝑡) defined through equilibrium time-correlation functions of heat fluxes. This function generalizes the conventional concept of steady-state thermal conductivity, governing the transition of conduction dynamics from onset second sound type wave propagation at finite speeds to diffusion-dominated behavior across broad temporal and spatial scales. Unlike phonon hydrodynamic models that rely on mesoscopic constructs such as phonon drift velocity, our approach provides a quantitative and microscopic description of intrinsic memory effects in transient heat fluxes and applies universally to bulk materials at any temperature or length scale. By integrating atomistic-scale first-principles calculations with continuum-level macroscopic equations, this framework offers a robust foundation for numerical simulations of transient temperature fields. Furthermore, it facilitates the interpretation and design of transient thermal grating experiments using nanometer-scale heat sources and ultrafast laser systems in the extreme ultraviolet and x-ray wavelength ranges, advancing our understanding of heat dissipation dynamics.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2021

Localization of Nonblinking Point Sources Using Higher-Order-Mode Detection and Optical Heterodyning: Developing a Strategy for Extending the Scope of Molecular, Super-resolution Imaging

While the stochastic, “blinking” nature of fluorescent systems has enabled the super-resolution of their localization by the fitting of their point-spread functions (PSFs), this strategy cannot be exploited for similar resolution of “nonblinking” systems, such as those that might be encountered in a coherent Raman experiment. An alternative method for subdiffraction-limited imaging lies in the exploitation of optical heterodyning. For example, if a Gaussian PSF (a TEM00 mode) of a point emitter is displaced with respect to the origin of the optical system, photons in the higher-order TEM modes carry information about that displacement. Information concerning the displacement can be extracted from photons in these higher-order modes. These photons can be collected by optical heterodyning, which exploits the large gain in a detector’s response to an optical signal from an emitter coupled to a local oscillator, which is prepared in the TEM of interest, e.g., TEM10. We have generalized and developed the heterodyning technique to localize point emitters via the detection of higher-order spatial modes. We have developed a theoretical approach to find a practical estimation limit of the localization parameters using a realistic model that accounts for shot noise, background noise, and Gaussian noise. To demonstrate the applicability of the method, we designed experiments in which a laser is a surrogate for one and two point emitters. Using the Fisher information and its accompanying Cramér-Rao lower bound, we demonstrate super-resolution localization in these cases: we show that objects can be localized to roughly 2–3 orders of magnitude of their point-spread function’s size for a given optical system. Finally and most importantly, it is suggested that the results will ultimately be generalizable to multiple emitters and, most importantly, to “nonblinking” molecular systems, which will be essential for broadening the scope of super-resolution measurements beyond the limits of fluorescence-based techniques.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗