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Bulk heterojunction (BHJ) organic solar cells have made remarkable inroads towards 20% efficiency, yet nonradiative recombination losses ({\Delta}Vnr) remain high compared to silicon and perovskite photovoltaics. Interfaces buried within BHJ blends hold the key to recombination losses but access to their energetic landscape underpinning charge transfer (CT) states and their disorder remain elusive. Here, we reveal the energetic landscape and CT state manifold of modern BHJs with both spatial and energetic resolutions and link the offset between singlet (ES1) and CT energy (ES1-CT) and interfacial energetic disorder with {\Delta}Vnr. We do so by locally mapping the energy distributions of modern PM6-based BHJs with IT4F, Y6 and PC71BM acceptors and combine it, for the first time, with sensitive EQE measurements, to visualize and quantify donor (D) and acceptor (A) energetics at interfaces and associated them with CT states within a modified Marcus framework. A key new ability is the identification of the specific BHJ interfaces associated with the CT manifold, including where the lowest energy CT states reside. Moreover, we quantify energy levels and electronic disorders directly at these and other interfaces and connect these contributions to the energy losses. We delineate the influences of S1-CT offset and interfacial energetic disorder on {\Delta}Vnr across morphologically varied BHJs. Our results show both factors influencing energy losses in different ways. We demonstrate that PM6:Y6 can achieve low {\Delta}Vnr by forming a nominally sharp D/A interface with exceptionally low interfacial disorder via judicious processing combined with a low S1 to CT offset. This provides a design rule to minimize {\Delta}Vnr for modern NFAs: sharp D/A interfaces with low S1 to CT offset exhibiting minimal interfacial disorder., Comment: Manuscript: 30 pages, 4 figures, 2 tables Supplementary information: 41 pages, 24 figures, 7 tables

Strong nonradiative recombination has been observed in quasi-one-dimensional antimony selenide, which runs counter to the simple intuition that claims high defect tolerance exists in semiconductors with antibonding state in the valence band and bonding state in the conduction band. Here we reveal such a defect intolerance actually stems from the richness of structural metastability and vibrational anharmonicity owing to the low-symmetry atomic structure. Taking the deep defect V$_{\rm Se}$ as a benchmark, we show the defect with its ground-state configuration alone does not act as a recombination center. Instead, we identify three different configurations with different formation energies, such richness of metastability offers a higher probability to accomplish a rapid recombination cycle. Another contributing factor is the anharmonicity in the potential energy surfaces that is caused by the large atomic relaxation, which elevates the total capture coefficient by 2-3 orders of magnitude compared with harmonic approximation. Therefore, the unique properties from both crystals and phonons in quasi-one-dimensional system enhance the nonradiative recombination, making the traditional intuition of defect tolerance invalid. These results highlight the importance of the correct identification of metastable defects and phonon anharmonicity in the nonradiative recombination in low-symmetry semiconductors.

The diffuse supernova neutrino background (DSNB) is the constant flux of neutrinos and antineutrinos emitted by all past core collapses in the observable Universe. We study the potential to extract information on the neutrino lifetime from the upcoming observation of the DSNB flux. The DSNB flux has a unique sensitivity to neutrino nonradiative decay for $\tau / m \in \left[ 10^9, 10^{11}\right]$~s/eV. To this end, we integrate, for the first time, astrophysical uncertainties, the contribution from failed supernovae, and a three-neutrino description of neutrino nonradiative decay. We present our predictions for future detection at the running Super-Kamiokande + Gd and the upcoming Hyper-Kamiokande, JUNO, and DUNE experiments. Finally, our results show the importance of identifying the neutrino mass ordering to restrict the possible decay scenarios for the impact of nonradiative neutrino decay on the DSNB., Comment: Submitted to Proceedings of Science, XVIII International Conference on Topics in Astroparticle and Underground Physics (TAUP2023). 6 pages, 4 figures

Exciton excited states in the quantum well are studied via their effect on the nonradiative broadening of the ground exciton resonance. Dependence of the nonradiative broadening of the ground exciton state on the photon energy of additional laser excitation was measured. Applying magnetic field up to 6 T, we could trace the formation of Landau levels and evolution of the exciton states of size quantization in a 14-nm GaAs/AlGaAs quantum well. Sensitivity of the technique allowed for observation of the second exciton state of size quantization, unavailable for conventional reflectance and photoluminescence spectroscopy. Our interpretation is supported by the numerical calculation of the exciton energies of the heavy-hole and light-hole subsystems. The numerical problems were solved using the finite-difference method on the nonuniform grid. The ground Landau level of the free electron-hole pair was observed and numerically analysed. In addition to energies of the excited states, electron hole distances and exciton-light interaction constant was investigated using the obtained in the numerical procedure exciton wave functions.

Excitons and free charge carriers with large wave vectors form a nonradiative reservoir, which can strongly affect properties of bright excitons due to the exciton-exciton and exciton-carrier interactions. In the present work, the dynamics of quasiparticles in the reservoir at different areal densities is experimentally studied in a GaAs/AlGaAs quantum well using a time-resolved reflectance spectroscopy of nonradiative broadening of exciton resonances. The population of the reservoir is controlled either by the excitation power or by the temperature of the structure under study. The dynamics is quantitatively analyzed in the framework of the model developed earlier [Kurdyubov et al., Phys. Rev. B {\bf 104}, 035414 (2021)]. The model considers several dynamic processes, such as scattering of photoexcited excitons into the reservoir, dissociation of excitons into free charge carriers and the reverse process, carrier-induced exciton scattering into the light cone depleting the reservoir, thermally activated nonradiative losses of charge carriers. We have found that competition of these processes leads to highly nonlinear dynamics of reservoir excitons, although their density is far below the exciton Mott transition densities. Characteristic rates of the processes and their dependencies on the excitation power and the temperature are determined., Comment: Submitted to PRB

There is increasing interest in filling the gap of miniaturized terahertz/mid-infrared radiation sources and, particularly, in incorporating these sources into micro/nanophotonic circuits. By using rigorous electromagnetic methods, we investigate the lasing conditions and the electric-tunability of radiative and non radiative propagating surface-plasmon modes in cylinders made of active materials coated with a graphene layer. A detailed analysis of the lasing condition of different surface-plasmon modes shows that there is an abrupt change in the gain required when modes become nonradiative. Although radiative modes, subject to both radiation and ohmic losses, are expected to require more gain compensation than nonradiative modes, we find that, counterintuitively, gain compensation is greater for nonradiative modes. This is explained in terms of a change in the distribution of fields that occurs when the character of modes switches from plasmonic to photonic. Finally, we assess the feasibility of our proposal by using a realist gain medium and showing that a relatively low population inversion is required for the stimulated emission of the studied system., Comment: to appear in JosaB

The description of carrier dynamics in spatially confined semiconductor nanocrystals (NCs), which have enhanced electron-hole and exciton-phonon interactions, is a great challenge for modern computational science. These NCs typically contain thousands of atoms and tens of thousands of valence electrons with a discrete spectrum at low excitation energies, similar to atoms and molecules, that converges to the continuum bulk limit at higher energies. Computational methods developed for molecules are limited to very small nanoclusters, and methods for bulk systems with periodic boundary conditions are not suitable due to the lack of translational symmetry in NCs. This perspective focuses on our recent efforts in developing a unified atomistic model based on the semiempirical pseudopotential approach, which is parametrized by first-principles calculations and validated against experimental measurements, to describe two of the main nonradiative relaxation processes of quantum confined excitons: exciton cooling and Auger recombination. We focus on the description of both electron-hole and exciton-phonon interactions in our approach and discuss the role of size, shape, and interfacing on the electronic properties and dynamics for II-VI and III-V semiconductor NCs.

Combined studies on fluorescence quantum yield in coenzymes NADH and FAD in water-methanol, water-ethanol and water-propylene glycol mixtures and on time-resolved fluorescence of the same molecules under excitation at 450 and 355~nm by means of the TCSPC method have been carried out. The dependence of quantum yield in NADH on alcohol concentration was found to be similar in methanol and ethanol and different from that in propylene glycol. The behavior of quantum yield in FAD was found to be almost independent of the type of alcohol and exhibited a dramatic 5--6 times increase with alcohol concentration. A model describing molecular excited state relaxation dynamics in pico- and nanosecond time domain was developed on the basis on the quantum mechanical theory and used for analysis of the experimental results. In particular, the model provided a new insight into the nature of the Decay Associated Spectra (DAS) phenomenon. The analysis of the role of pico- and nanosecond quenching in NADH suggested that the picosecond decay in methanol and ethanol likely does not occur through electron transfer in the stacking configuration of the nicotinamide and adenine moieties, but through other mechanisms. However in propylene glycol the picosecond quenching in NADH depended strongly on propylene glycol concentration and sharp increase of the measured quantum yield was associated with the contribution of both picosecond and nanosecond quenching mechanisms. The picosecond quenching to FAD was found to depend significantly on the any alcohol concentration suggesting that it gives a profound contribution to the rise of the measured quantum yield with alcohol concentration. This conclusion supports the established mechanism of the fluorescence quenching in FAD through electron transfer reaction in the $\pi$-stacked conformation between isoalloxazine and adenine moieties., Comment: 16 pages, 4 figures

Most optoelectronic devices operate at high photocarrier densities, where all semiconductors suffer from enhanced nonradiative recombination. Nonradiative processes proportionately reduce photoluminescence (PL) quantum yield (QY), a performance metric that directly dictates the maximum device efficiency. Although transition-metal dichalcogenide (TMDC) monolayers exhibit near-unity PL QY at low exciton densities, nonradiative exciton-exciton annihilation (EEA) enhanced by van-Hove singularity (VHS) rapidly degrades their PL QY at high exciton densities and limits their utility in practical applications. Here, by applying small mechanical strain (< 1%), we circumvent VHS resonance and drastically suppress EEA in monolayer TMDCs, resulting in near-unity PL QY at all exciton densities despite the presence of a high native defect density. Our findings can enable light-emitting devices that retain high efficiency at all brightnesses.

For more than 50 years, an elegant energy gap (EG) law developed by Englman and Jortner [Mol. Phys. {\bf 18}, 145 (1970)] has served as a key theory to understand and model nearly exponential dependence of nonradiative transition rates on the difference of energy between the initial and final states. This work revisits the theory, clarifies key assumptions involved in the rate expression, and provides a generalization for the cases where the effects of temperature dependence and low frequency modes cannot be ignored. For a specific example where the low frequency vibrational and/or solvation responses can be modeled as an Ohmic spectral density, a simple generalization of the EG law is provided. Test calculations demonstrate that this generalized EG law brings significant improvement over the original EG law. Both the original and generalized EG laws are also compared with stationary phase approximations developed for electron transfer theory, which suggests the possibility of a simple interpolation formula valid for any value of EG., Comment: 10 pages, 4 figures, accepted for publication in the Journal of Chemical Physics