Tracking surface charge dynamics on single nanoparticles

Dagar, Ritika; Zhang, Wenbin; Rosenberger, Philipp; Linker, Thomas M.; Sousa-Castillo, Ana; Neuhaus, Marcel; Mitra, Sambit; Biswas, Shubhadeep; Feinberg, Alexandra; Summers, Adam M.; Nakano, Aiichiro; Vashishta, Priya; Shimojo, Fuyuki; Wu, Jian; Vera, Cesar Costa; Maier, Stefan A.; Cortés, Emiliano; Bergues, Boris; Kling, Matthias F.

doi:10.1126/sciadv.adp1890

DOE OSTI · 2375506

Tracking surface charge dynamics on single nanoparticles

Dagar, Ritika·Zhang, Wenbin·Rosenberger, Philipp·Linker, Thomas M.·Sousa-Castillo, Ana·Neuhaus, Marcel·Mitra, Sambit·Biswas, Shubhadeep·Feinberg, Alexandra·Summers, Adam M.·Nakano, Aiichiro·Vashishta, Priya·Shimojo, Fuyuki·Wu, Jian·Vera, Cesar Costa·Maier, Stefan A.·Cortés, Emiliano·Bergues, Boris·Kling, Matthias F.

View original source ↗Read source document ↗Export metadata ↓

Abstract

Surface charges play a fundamental role in physics and chemistry, in particular in shaping the catalytic properties of nanomaterials. However, tracking nanoscale surface charge dynamics remains challenging due to the involved length and time scales. Here, we demonstrate time-resolved access to the nanoscale charge dynamics on dielectric nanoparticles using reaction nanoscopy. We present a four-dimensional visualization of the spatiotemporal evolution of the charge density on individual SiO 2 nanoparticles under strong-field irradiation with femtosecond-nanometer resolution. The initially localized surface charges exhibit a biexponential redistribution over time. Our findings reveal the influence of surface charges on surface molecular bonding through quantum dynamical simulations. We performed semi-classical simulations to uncover the roles of diffusion and charge loss in the surface charge redistribution process. Understanding nanoscale surface charge dynamics and its influence on chemical bonding on a single-nanoparticle level unlocks an increased ability to address global needs in renewable energy and advanced health care.

Explore related subjects

74 ATOMIC AND MOLECULAR PHYSICS 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Keep this discovery

Explore connections, maps & timelines

BibTeX RIS

Dagar, Ritika, Zhang, Wenbin, Rosenberger, Philipp, Linker, Thomas M., Sousa-Castillo, Ana, Neuhaus, Marcel, Mitra, Sambit, Biswas, Shubhadeep, Feinberg, Alexandra, Summers, Adam M., Nakano, Aiichiro, Vashishta, Priya, Shimojo, Fuyuki, Wu, Jian, Vera, Cesar Costa, Maier, Stefan A., Cortés, Emiliano, Bergues, Boris, Kling, Matthias F.. 2024-08-09. Tracking surface charge dynamics on single nanoparticles. https://doi.org/10.1126/sciadv.adp1890

Cite the original work for its findings. Save a collection to share your selection of sources.

KEEP EXPLORING

Related reports

DOE OSTI2026

Geometric decoherence time in Lindbladian dynamics

The onset of decoherence in open many-body systems lacks a dynamical timescale grounded in the loss of bipartite entanglement. Here, we introduce the geometric decoherence time, defined as the earliest moment the monotone relation between logarithmic negativity and Rényi-$\frac{1}{2}$ entropy—exactly equal across any bipartition for pure states—breaks down under open-system evolution, signaling entropy growth without accompanying entanglement growth. We establish this criterion in both single-particle Gaussian dynamics and many-body Lindbladian evolution. We show that quantum mutual information provides a complementary long-time diagnostic: Its asymptotic vanishing is equivalent to factorization of the steady state across the bipartition, a condition strictly stronger than separability, and whenever a product steady state is approached exponentially in trace norm, negativity and mutual information share the same decay rate. In the presence of a strong symmetry, this tracking can fail—residual classical correlations can survive after entanglement has vanished. In the Kitaev chain with balanced gain and loss, we derive a closed-form solution and show that the topological phase sustains longer coherence times than the trivial phase at identical dissipation, with a local minimum at the chiral-symmetric point. In the interacting XXZ chain, exact many-body evolution shows that local 𝑍 dephasing preserves residual classical correlations, whereas gain and loss restore the mutual-information tracking of negativity. Furthermore, our results establish the geometric decoherence time as a dynamical scale tracking the onset of decoherence.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2026

Restricted Partition Function Semiclassical Transition State Theory (RPF-SCTST): Applications to Reactions Involving Hydrogen Cyanide, Hydrogen Peroxide, and Formaldehyde Oxide

We demonstrate the efficiency of the numerical calculation of thermal semiclassical transition state theory (SCTST) rates across several representative chemical reactions using the restricted partition function (RPF)─viz a function that depends only on the imaginary action associated with a reaction. Here, we treat the potential energy surfaces (PESs) through fourth order expansions around the saddle point and integrate the Hamiltonian up to second order in employing vibrational perturbation theory. We apply this formalism to uni- and bimolecular reactions with different─though relatively high─barrier heights to uncover the influence of the barrier properties, minimal energies, and separability of the rotational motion on rate constants and tunneling corrections. Although all modes are coupled within the RPF, we found in our numerical examples that the rotational component in the absence of significant rotational distortions can be separated from the vibrational contributions. Moreover, a classical treatment of the rotational contribution is adequate over the temperature range from approximately 100 to 1000 K. We also found that the choice of DFT basis set can lead to variations in rate constants of up to an order of magnitude. Lastly, different schemes for counting eligible energy levels result in rate constants that differ by no more than a factor of 2, with the remaining discrepancies attributed to the treatment of near-convergent levels in perturbation theory.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2026

Seniority eigenstate configuration interaction

Zero-seniority methods have shown great promise for the description of strongly correlated electronic systems. Other seniority sectors have been much less explored, and in particular, the maximal seniority sector and zero seniority have the same underlying algebraic structure. We introduce a seniority eigenstate configuration interaction in which the wave function is constrained to have good fixed local seniority for each paired orbital, by which we mean we partition orbitals into a pairing set with seniority zero, and a spin set with seniority one. Here, we show how to build the effective Hamiltonian for this ansatz, and demonstrate that high-seniority wave functions have unexpectedly excellent accuracy for strongly correlated fermionic systems, with accuracy competitive with or better than seniority zero for the Hubbard model and for the dissociation of the nitrogen molecule.

74 ATOMIC AND MOLECULAR PHYSICS↗