arXiv subjects
Publications and source records attributed to Steven Chu.
George Smoot (1945-2025) was a major figure in observational cosmology, particularly through his role in the precision measurement of the CMB dipole and the discovery of the primordial CMB temperature anisotropy as part of the COBE team. This collection of 33 essays from collaborators, colleagues, students, and friends offers varied insights into the work, career, and life of George Smoot.
Developing new fluorophores for advanced imaging techniques requires exploring new chemical space. While generative AI approaches have shown promise in designing novel dye scaffolds, prior efforts often produced synthetically intractable candidates due to a lack of reaction constraints. Here, we developed SyntheFluor-RL, a generative AI model that employs known reaction libraries and molecular building blocks to create readily synthesizable fluorescent molecule scaffolds via reinforcement learning. To guide the generation of fluorophores, SyntheFluor-RL employs a scoring function built on multiple graph neural networks (GNNs) that predict key photophysical properties, including photoluminescence quantum yield, absorption, and emission wavelengths. These outputs are dynamically weighted and combined with a computed pi-conjugation score to prioritize candidates with desirable optical characteristics and synthetic feasibility. SyntheFluor-RL generated 11,590 candidate molecules, which were filtered to 19 structures predicted to possess dye-like properties. Of the 19 molecules, 14 were synthesized and 13 were experimentally confirmed. The top three were characterized, with the lead compound featuring a benzothiadiazole chromophore and exhibiting strong fluorescence (PLQY = 0.62), a large Stokes shift (97 nm), and a long excited-state lifetime (11.5 ns). These results demonstrate the effectiveness of SyntheFluor-RL in the identification of synthetically accessible fluorophores for further development.
The practical implementation of lithium-metal anodes has been hindered by uncontrollable dendrite formation and interfacial instability. This study presents a defect-engineering approach of a chemically stable and electrically insulating interfacial layer of hexagonal boron nitride (h-BN) that markedly enhances ionic conductivity through argon ion irradiation. Initially, the electrochemical performance from commercially available, large-area chemical vapor deposition (CVD)-grown h-BN films with industrial-scale argon ion implantation motivated our subsequent detailed investigations using lab-scale exfoliated single-crystal h-BN flakes. Integration of these exfoliated flakes into a hybrid microfluidic-microelectronic chip provided direct evidence that controlled vacancy defects transform h-BN into an efficient lithium-ion conductor while preserving its intrinsic electrical insulation. Experimental validation confirmed improved lithium-metal anode stability, achieving dendrite-free cycling with Li plating/stripping Coulombic efficiencies exceeding 99.5% about 1000 cycles. Further assemble of irradiated h-BN in lithium-sulfur batteries effectively mitigates the polysulfide shuttle effect, sustaining over 97% specific capacity around 300 cycles. These results establish a robust, scalable interface-engineering route for next-generation lithium-metal batteries that combine high ionic transport with excellent electrical insulation.
The development of reversible metal anodes is a key challenge for advancing aqueous battery technologies, particularly for scalable and safe stationary energy storage applications. Here we demonstrate a strategy to realize epitaxial electrodeposition of iron (Fe) on single-crystal copper (Cu) substrates in aqueous electrolytes. We compare the electrodeposition behavior of Fe on polycrystalline and single-crystalline Cu substrates, revealing that the latter enables highly uniform, dense, and crystallographically aligned Fe growth. Comprehensive electron backscatter diffraction (EBSD) and X-ray diffraction (XRD) analysis confirms the formation of Fe with specific out-of-plane and in-plane orientations, including well-defined rotational variants. Our findings highlight that epitaxial electrodeposition of Fe can suppress dendritic growth and significantly enhance Coulombic efficiency during plating/stripping cycles. This approach bridges fundamental crystallography with practical electrochemical performance, providing a pathway toward high-efficiency aqueous batteries utilizing Earth-abundant materials.
Capture of anthropogenic CO2 is critical for mitigating climate change, and reducing the energy cost is essential for wide-scale deployment. Solubility of inorganic carbon in aqueous solutions depends on the pH, and electrochemical modulation of the pH has been investigated as a means of CO2 capture and release. However, reported methods incur unavoidable energy costs due to thermodynamic penalties. In this study, we introduce a pH-independent redox chemistry that greatly lowers the thermodynamic energy costs by changing the pH without directly changing the [H+]. We show that the redox reaction of TEMPO molecules modulates the pH for capture and release of CO2 in a flow cell with an energy cost as low as 2.6 kJ/mol of CO2 corresponding to 0.027 eV/molecule. A molecular model, supported by MD and DFT simulations, is proposed of how the pH is decreased by 7.6 while largely avoiding the entropic energy cost associated with increasing the [H+]. We believe that this work showcases the potential of pH-independent redox chemistries for practical and cost-effective CO2 capture.
Understanding the chemical state of individual ions in solutions is crucial for advancing knowledge of complex systems. However, sensing systems at the single-ion level in liquid environments remains a significant challenge. A strategy is introduced that leverages the optical emission properties of point defects in hexagonal boron nitride (h-BN) as single ion sensors. The interaction of optically active h-BN defects with ions in solution leads to distinct spectral shifts, enabling precise visualization and analyzing of individual ions. Using Li+ ions in organic electrolytes as a model, spectral shifts exceeding 10 nm were observed upon ion addition. Application of an external electric field further enhanced these shifts to over 40 nm, enabling real-time monitoring of electrical field induced local perturbations of Li+ ions. Through this approach, individual point defects were shown to spectroscopically distinguish ions of varying charges (e.g., Na+, Mg2+, and Al3+) based on their local electrical field, each producing a distinct spectral shift. This platform allows direct sensing of ions and their chemical states in liquid environments, providing insights into subtle interfacial changes at the single-ion level, with measurable spectral shifts detectable at millisecond temporal resolution and at concentrations down to 10 micromolar range. This capability presents potential applications in various fields involving ions in liquids that include battery technology and environmental science.
Electron microscopy (EM) has been instrumental in our understanding of biological systems ranging from subcellular structures to complex organisms. Although EM reveals cellular morphology with nanoscale resolution, it does not provide information on the location of proteins within a cellular context. An EM-based bioimaging technology capable of localizing individual proteins and resolving protein-protein interactions with respect to cellular ultrastructure would provide important insights into the molecular biology of a cell. Here, we report on the development of luminescent nanoprobes potentially suitable for labeling biomolecules in a multicolor EM modality. In this approach, the labels are based on lanthanide-doped nanoparticles that emit light under electron excitation in a process known as cathodoluminescence (CL). Our results suggest that the optimization of nanoparticle composition, synthesis protocols and electron imaging conditions could enable high signal-to-noise localization of biomolecules with a sub-20-nm resolution, limited only by the nanoparticle size. In ensemble measurements, these luminescent labels exhibit narrow spectra of nine distinct colors that are characteristic of the corresponding rare-earth dopant type.
We demonstrate cavity-enhanced Raman emission from a single atomic defect in a solid. Our platform is a single silicon-vacancy center in diamond coupled with a monolithic diamond photonic crystal cavity. The cavity enables an unprecedented frequency tuning range of the Raman emission (100 GHz) that significantly exceeds the spectral inhomogeneity of silicon-vacancy centers in diamond nanostructures. We also show that the cavity selectively suppresses the phonon-induced spontaneous emission that degrades the efficiency of Raman photon generation. Our results pave the way towards photon-mediated many-body interactions between solid-state quantum emitters in a nanophotonic platform.
Quantum emitters are an integral component for a broad range of quantum technologies including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single photon generation and photon mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime where the excited state lifetime is dominated by spontaneous emission into the cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited state energy decay occurring through spontaneous emission into the cavity mode. We also demonstrate the largest to date coupling strength ($g/2\pi=4.9\pm0.3 GHz$) and cooperativity ($C=1.4$) for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.
Arrays of identical and individually addressable qubits lay the foundation for the creation of scalable quantum hardware such as quantum processors and repeaters. Silicon vacancy centers in diamond (SiV) offer excellent physical properties such as low inhomogeneous broadening, fast photon emission, and a large Debye-Waller factor, while the possibility for all-optical ultrafast manipulation and techniques to extend the spin coherence times make them very promising candidates for qubits. Here, we have developed arrays of nanopillars containing single SiV centers with high yield, and we demonstrate ultrafast all-optical complete coherent control of the state of a single SiV center. The high quality of the chemical vapor deposition (CVD) grown SiV centers provides excellent spectral stability, which allows us to coherently manipulate and quasi-resonantly read out the state of individual SiV centers on picosecond timescales using ultrafast optical pulses. This work opens new opportunities towards the creation of a scalable on-chip diamond platform for quantum information processing and scalable nanophotonics applications.
We discuss the progress in integration of nanodiamonds with photonic devices for quantum optics applications. Experimental results in GaP, SiO2 and SiC-nanodiamond platforms show that various regimes of light and matter interaction can be achieved by engineering color center systems through hybrid approaches. We present our recent results on the growth of color center-rich nanodiamond on prefabricated 3C-SiC microdisk resonators. These hybrid devices achieve up to five-fold enhancement of diamond color center light emission and can be employed for integrated quantum photonics.
Optical coherence tomography (OCT) is a powerful biomedical imaging technology that relies on the coherent detection of backscattered light to image tissue morphology in vivo. As a consequence, OCT is susceptible to coherent noise (speckle noise), which imposes significant limitations on its diagnostic capabilities. Here we show a method based purely on light manipulation that is able to entirely remove the speckle noise originating from turbid samples without any compromise in resolution. We refer to this method as Speckle-Free OCT (SFOCT). Using SFOCT, we succeeded in revealing small structures that are otherwise hidden by speckle noise when using conventional OCT, including the inner stromal structure of a live mouse cornea, the fine structures inside the mouse pinna, sweat ducts, and Meissners corpuscle in the human fingertip skin. SFOCT has the potential to markedly increase OCTs diagnostic capabilities of various human diseases by revealing minute features that correlate with early pathology.
We show that Wolf et al.'s 2011 analysis in Class. Quant. Grav. v28, 145017 does not support their conclusions, in particular that there is "no redshift effect" in atom interferometers except in inconsistent dual Lagrangian formalisms. Wolf et al. misapply both Schiff's conjecture and the results of their own analysis when they conclude that atom interferometers are tests of the weak equivalence principle which only become redshift tests if Schiff's conjecture is invalid. Atom interferometers are direct redshift tests in any formalism.
We investigate leading order deviations from general relativity that violate the Einstein equivalence principle in the gravitational standard model extension. We show that redshift experiments based on matter waves and clock comparisons are equivalent to one another. Consideration of torsion balance tests, along with matter wave, microwave, optical, and M\"ossbauer clock tests, yields comprehensive limits on spin-independent Einstein equivalence principle-violating standard model extension terms at the $10^{-6}$ level.
We review matter wave and clock comparison tests of the gravitational redshift. To elucidate their relationship to tests of the universality of free fall (UFF), we define scenarios wherein redshift violations are coupled to violations of UFF ("type II"), or independent of UFF violations ("type III"), respectively. Clock comparisons and atom interferometers are sensitive to similar effects in type II and precisely the same effects in type III scenarios, although type III violations remain poorly constrained. Finally, we describe the "Geodesic Explorer," a conceptual spaceborne atom interferometer that will test the gravitational redshift with an accuracy 5 orders of magnitude better than current terrestrial redshift experiments for type II scenarios and 12 orders of magnitude better for type III.
We stand by our result [H. Mueller et al., Nature 463, 926-929 (2010)]. The comment [P. Wolf et al., Nature 467, E1 (2010)] revisits an interesting issue that has been known for decades, the relationship between test of the universality of free fall and redshift experiments. However, it arrives at its conclusions by applying the laws of physics that are questioned by redshift experiments; this precludes the existence of measurable signals. Since this issue applies to all classical redshift tests as well as atom interferometry redshift tests, these experiments are equivalent in all aspects in question.
Topologically-ordered matter is a novel quantum state of matter observed only in a small number of physical systems, notably two-dimensional electron systems exhibiting fractional quantum Hall effects. It was recently proposed that a simple form of topological matter may be created in interacting systems of rotating ultra-cold atoms. We describe ensemble measurements on small, rotating clusters of interacting bosonic atoms, demonstrating that they can be induced into quantum ground states closely analogous to topological states of electronic systems. We report measurements of inter-particle correlations and momentum distributions of Bose gases in the fractional quantum Hall limit, making comparison to a full numerical simulation. The novel experimental apparatus necessary to produce and measure properties of these deeply entangled quantum states is described.
We present atom-interferometer tests of the local Lorentz invariance of post-Newtonian gravity. An experiment probing for anomalous vertical gravity on Earth, which has already been performed by us, uses the highest-resolution atomic gravimeter so far. The influence of Lorentz violation in electrodynamics is also taken into account, resulting in combined bounds on Lorentz violation in gravity and electrodynamics. Expressed within the standard model extension or Nordtvedt's anisotropic universe model, we limit twelve linear combinations of seven coefficients for Lorentz violation at the part per billion level, from which we derive limits on six coefficients (and seven when taking into account additional data from lunar laser ranging). We also discuss the use of horizontal interferometers, including atom-chip or guided-atom devices, which potentially allow the use of longer coherence times in order to achieve higher sensitivity.