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In this Festschrift contribution in honor of Prof. Maurizio Persico, we present a systematic derivation and comprehensive assessment of several integrators for quantum-classical time-dependent Schrodinger (TD-SE) and Liouville (QCLE) equations. We construct a systematic formalism that naturally accounts for trivial state crossing effects and helps solve related phenomena that often pose significant numerical problems in nonadiabatic molecular dynamics simulations. Our derivations generalize and extend the local diabatization approach pioneered by Prof. Persico and co-workers, leading to several new integrators for TD-SE. Further, we extend this formalism to the QCLE integration. We generalize the symmetric splitting integrator proposed by one of us earlier, and demonstrate how it can be applied to integrate both TD-SE and QCLE. We provide detailed discussion of the algorithms and their implementation in the Libra software, and we present their comprehensive assessment with several well-designed model problems.

We investigated the magnetic effect of Mn2+ ions on an exciton of Mn-doped CsPbI3 quantum dots (QDs), where we looked for the signatures of an exciton magnetic polaron known to produce a large effective magnetic field in Mn-doped CdSe QDs. In contrast to Mn-doped CdSe QDs that can produce ∼100 T of magnetic field upon photoexcitation, manifested as a large change in the energy and relaxation dynamics of a bright exciton, Mn-doped CsPbI3 QDs exhibited little influence of a magnetic dopant on the behavior of a bright exciton. However, a μs-lived dark exciton in CsPbI3 QDs showed 40% faster decay in the presence of Mn2+, equivalent to the effect of ∼3 T of an external magnetic field. While further study is necessary to fully understand the origin of the large difference in the magneto-optic property of an exciton in two systems, we consider that the difference in antiferromagnetic coupling of the dopants is an important contributing factor.

Multiple applied studies of slow nonadiabatic processes in nanoscale and condensed matter systems have adopted the "repetition" approximation in which long trajectories for such simulations are obtained by concatenating shorter trajectories, directly available from ab initio calculations, many times. Here, we comprehensively assess this approximation using model Hamiltonians with parameters covering a wide range of regimes. We find that state transition time scales may strongly depend on the length of the repeated data, although the convergence is not monotonic and may be slow. The repetition approach may under- or overestimate the time scales by a factor of ≤7-8, does not directly depend on the dispersion of energy gap and nonadiabatic coupling (NAC) frequencies, but may depend on the magnitude of the NACs. We suggest that the repetition-based nonadiabatic dynamics may be inaccurate in simulations with very small NACs, where intrinsic transition times are on the order of ≥100 ps.

Hot electrons play a crucial role in enhancing the efficiency of photon-to-current conversion or photocatalytic reactions. In semiconductor nanocrystals, energetic hot electrons capable of photoemission can be generated via the upconversion process involving the dopant-originated intermediate state, currently known only in Mn-doped cadmium chalcogenide quantum dots. Here, we report that Mn-doped CsPbBr

Using a recently developed many-body nonadiabatic molecular dynamics (NA-MD) framework for large condensed matter systems, we study the phonon-driven nonradiative relaxation of excess electronic excitation energy in cubic and tetragonal phases of the lead halide perovskite CsPbI3. We find that the many-body treatment of the electronic excited states significantly changes the structure of the excited states' coupling, promotes a stronger nonadiabatic coupling of states, and ultimately accelerates the relaxation dynamics relative to the single-particle description of excited states. The acceleration of the nonadiabatic dynamics correlates with the degree of configurational mixing, which is controlled by the crystal symmetry. The higher-symmetry cubic phase of CsPbI3 exhibits stronger configuration mixing than does the tetragonal phase and subsequently yields faster nonradiative dynamics. Overall, using a many-body treatment of excited states and accounting for decoherence dynamics are important for closing the gap between the computationally derived and experimentally measured nonradiative excitation energy relaxation rates.

In this work, we report a new methodology for nonadiabatic molecular dynamics calculations within the extended tight-binding (xTB) framework. We demonstrate the applicability of the developed approach to finite and periodic systems with thousands of atoms by modeling "hot" electron relaxation dynamics in silicon nanocrystals and electron-hole recombination in both a graphitic carbon nitride monolayer and a titanium-based metal-organic framework (MOF). This work reports the nonadiabatic dynamic simulations in the largest Si nanocrystals studied so far by the xTB framework, with diameters up to 3.5 nm. For silicon nanocrystals, we find a non-monotonic dependence of "hot" electron relaxation rates on the nanocrystal size, in agreement with available experimental reports. We rationalize this relationship by a combination of decreasing nonadiabatic couplings related to system size and the increase of available coherent transfer pathways in systems with higher densities of states. We emphasize the importance of proper treatment of coherences for obtaining such non-monotonic dependences. We characterize the electron-hole recombination dynamics in the graphitic carbon nitride monolayer and the Ti-containing MOF. We demonstrate the importance of spin-adaptation and proper sampling of surface hopping trajectories in modeling such processes. We also assess several trajectory surface hopping schemes and highlight their distinct qualitative behavior in modeling the excited-state dynamics in superexchange-like models depending on how they handle coherences between nearly parallel states.

Hot electrons play a crucial role in enhancing the efficiency of photon-to-current conversion or photocatalytic reactions. In semiconductor nanocrystals, energetic hot electrons capable of photoemission can be generated via the upconversion process involving the dopant-originated intermediate state, currently known only in Mn-doped cadmium chalcogenide quantum dots. Here, we report that Mn-doped CsPbBr3 nanocrystals are an excellent platform for generating hot electrons via upconversion that can benefit from various desirable exciton properties and the structural diversity of metal halide perovskites (MHP). 2-dimensional Mn-doped CsPbBr$_3$ nanoplatelets are particularly advantageous for hot electron upconversion due to the strong exciton-dopant interaction mediating the upconversion process. Furthermore, nanoplatelets reveal evidence for the hot electron upconversion via long-lived dark exciton in addition to bright exciton that may enhance the upconversion efficiency. This study not only establishes the feasibility of hot electron upconversion in MHP host but also demonstrates the potential merits of 2-dimensional MHP nanocrystals in hot electron upconversion.

We present a new state tracking algorithm based on a stochastic state reassignment that reflects the quantum mechanical interpretation of the state time-overlaps. We assess the new method with a range of model Hamiltonians and demonstrate that it yields the results generally consistent with the deterministic min-cost algorithm. However, the stochastic state tracking algorithm reduces magnitudes of the state population fluctuations as the quantum system evolves toward its equilibrium. The new algorithm facilitates the thermalization of quantum state populations and suppresses the population revivals and oscillations near the equilibrium in many-state systems. The new stochastic algorithm has a favorable computational scaling, is easy to implement due to its conceptual transparency, and treats various types of state identity changes (trivial or avoided crossings and any intermediate cases) on equal footing.

Synergy of nonadiabatic molecular dynamics with real-time time-dependent density functional theory has led to significant progress in modeling excited-state dynamics in nanoscale and condensed matter systems over the past decade. Nonadiabatic coupling (NAC) is the central quantity in such simulations, and its accurate and efficient evaluation is an enduring challenge in time-dependent Kohn-Sham theory, particularly in conjunction with planewave basis sets and projector augmented-wave (PAW) pseudopotentials because of the complexity of the PAW "all-electron" wave function. We report a method for rigorous evaluation of the NAC with PAW wave functions and demonstrate an efficient approximation to the rigorous NAC that gives comparable accuracy. As a validation, we intensely examine the NAC matrix elements calculated using both pseudo- and all-electron wave functions under the PAW formalism in six representative systems. The approximate NAC obtained with pseudowave functions is close to the exact all-electron NAC, with the largest deviations observed when subshell d-electrons are involved in the transitions. The developed approach provides a rigorous and convenient methodology for the numerical computation of NAC in the Kohn-Sham theory framework.

The results of growing multilayered nitrogen-doped nanostructures that have the form of periodically arranged nanometer-thick nitrogen-containing layers in a single-crystal CVD diamond are presented. The possibility of creating nitrogen-doped diamond layers with extremely sharp boundaries (less than 1 nm) is demonstrated. The photoluminescence study have shown that multilayered structures make it possible to obtain a higher radiation intensity of practically important NV – sites at a spin coherence time close to that for uniformly doped layers with the same concentration of nitrogen.

Nitrogen-vacancy centers possessing nuclear spins are promising candidates for a novel nuclear spin gyroscope. Preparation of a nuclear spin state is a crucial step to implement a sensor that utilizes a nuclear spin. In a low magnetic field, such a preparation utilizes population transfer, from polarized electronic spin to nuclear spin, using microwave pulses. The use of the narrowband microwave pulse proposed earlier is inefficient when magnetic transitions are not well resolved, particularly when applied to diamond with a natural abundance of carbon atoms or dense ensembles of nitrogen-vacancy centers. In this study, the authors performed optimization of the pulse shape for 3 relatively easily accessible pulse shapes. The optimization was done for a range of magnetic transition linewidths, corresponding to the practically important range of nitrogen concentrations (5-50 ppm). It was found that, while at low nitrogen concentrations, optimized pulse added very little to simple square shape pulse, and in the case of dense nitrogen-vacancy ensembles, with a rather wide magnetic transition width of 1.5 MHz optimal pulses, a factor of 15% improvement in the population of the target state was observed.

Integrated photonics will play a key role in quantum systems as they grow from few-qubit prototypes to tens of thousands of qubits. The underlying optical quantum technologies can only be realized through the integration of these components onto quantum photonic integrated circuits (QPICs) with accompanying electronics. In the last decade, remarkable advances in quantum photonic integration have enabled table-top experiments to be scaled down to prototype chips with improvements in efficiency, robustness, and key performance metrics. These advances have enabled integrated quantum photonic technologies combining up to 650 optical and electrical components onto a single chip that are capable of programmable quantum information processing, chip-to-chip networking, hybrid quantum system integration, and high-speed communications. In this roadmap article, we highlight the status, current and future challenges, and emerging technologies in several key research areas in integrated quantum photonics, including photonic platforms, quantum and classical light sources, quantum frequency conversion, integrated detectors, and applications in computing, communications, and sensing. With advances in materials, photonic design architectures, fabrication and integration processes, packaging, and testing and benchmarking, in the next decade we can expect a transition from single- and few-function prototypes to large-scale integration of multi-functional and reconfigurable devices that will have a transformative impact on quantum information science and engineering., JPhys Photonics, 4 (1), ISSN:2515-7647

We investigated the magnetic effect of Mn

The dynamics of electron–hole recombination in pristine and defect-containing monolayer black phosphorus (ML-BP) has been studied computationally by several groups relying on the one-particle description of electronic excited states. Our recent developments enabled a more sophisticated and accurate treatment of excited states dynamics in systems with pronounced excitonic effects, including 2D materials such as ML-BP. In this work, I present a comprehensive characterization of optoelectronic properties and nonadiabatic dynamics of the ground state recovery in pristine and divacancy-containing ML-BP, relying on the linear-response time-dependent density functional theory description of excited states combined with several trajectory surface hopping methodologies and decoherence correction schemes. This work presents a revision and new implementation of the decoherence-induced surface hopping methodology. Several popular algorithms for nonadiabatic dynamics algorithms are assessed. The kinetics of nonradiative relaxation of lower-lying excited states in ML-BP systems is revised considering the new methodological developments. A general mechanism that explains the sensitivity of the nonradiative dynamics to the presence of divacancy defect in ML-BP is proposed. According to this mechanism, the excited states’ relaxation may be inhibited by the presence of energetically close higher-energy states if electronic decoherence is present in the system.

We develop a new express methodology for modeling excited-state dynamics occurring in dense manifolds of electronic states in atomistic systems. The approach leverages a modified Landau-Zener formula, the neglect of a back-reaction approximation, and the highly efficient density functional tight-binding method. We study the hot electron dynamics in a series of H- and F-terminated silicon nanocrystals (NCs) containing up to several hundred atoms. We explain the slower electron cooling dynamics in F-terminated NCs by the larger energy gaps between the adjacent electronic states in these systems as well as their slower fluctuations. We conclude that both the mass and chemical identity of the surface termination groups equally influence the electron dynamics, on average. However, the mass effect becomes dominant for higher-energy excitations. We find that the electron decay dynamics in F-terminated NCs has a greater sensitivity to the mass of the surface ligands than do the H-terminated NCs and explain this observation by the details of the electron-phonon coupling in the systems. We find that in the H-terminated NCs, electronic transitions in the cooling process occur predominantly between the surface states, whereas in F-terminated Si NCs, both surface and NC core states are coupled to the nuclear vibrations. We find that electron energy relaxation is accelerated in larger NCs and attribute this effect to the higher densities of states and smaller energy gaps in these systems.

Nanocars are artificial molecular machines with chassis, axles, and wheels designed for nanoscale transport at materials’ surfaces. Understanding the dependence of surface dynamics of nanocars on the substrate’s physicochemical properties is critical to the design of the transport properties of such man-made nanoscale devices. Among the multitude of potential substrates for the nanotransporters, graphene exhibits intrinsic ripples on its surface, which may affect the surface dynamics of nanocars. In this work, we report our molecular dynamics study of motion of C60, a popular nanocar wheel, on the graphitic substrates with systematically controllable surface ripples. We find that surface ripples increase the amplitude of fullerene fluctuation in the direction normal to surface, which leads to decrease of the desorption temperature from 650 K on a double-layer graphite system with less ripples to 550 K on single-layer graphene with more ripples. The surface diffusion of C60 follows the rare hops mechanism ...

Accurate, high spatial resolution thermal measurements have provided fundamental insights into many fields of study; however, existing thermometer technology often suffers from one or more limitati...

Creation of localized NV center ensembles, produced by irradiation of CVD diamond with nitrogen doped delta-layer with 200 keV electron beam and the subsequent annealing is demonstrated. Results of optical measurements of activated areas at different irradiation doses are presented. Issues concerning defect formation in diamond lattice during the electron beam impact are discussed.

Recent studies demonstrated anomalous temperature shifts for some Fano-Feshbach resonances of thulium atoms. These anomalies were explained by the variation in light intensity in the optical dipole trap, which accompanied changes in temperature. In addition, a temperature-related transformation of the statistics of the inter-resonance spacing was demonstrated [Aikawa et al., Phys. Rev. Lett. 108, 210401 (2012)]. Here, we analyze the shifts of isolated $s$- and $d$-type Fano-Feshbach resonances of ultracold thulium atoms with temperature for a fixed depth of an optical dipole trap. The measurements are consistent with the three-body recombination-based theory of the temperature-related resonance shift and enable the extraction of the resonance parameters, particularly the magnetic moments of closed channel states. This parameter and the known polarizability of the open channel enable us to separate the contributions of the temperature and Stark shift to the overall shift of the resonances and show the dominant role of the Stark effect in the overall shift.

In this work, we report a new nonadiabatic molecular dynamics methodology that incorporates many-body (MB) effects in the treatment of electronic excited states in extended atomistic systems via linear-response time-dependent density functional theory (TD-DFT). The nonradiative dynamics of excited states in Si75H64 and Cd33Se33 nanocrystals is studied at the MB (TD-DFT) and single-particle (SP) levels to reveal the role of MB effects. We find that a MB description of the excited states qualitatively changes the structure of coupling between the excited states, leading to larger nonadiabatic couplings and accelerating the dynamics by a factor of 2-4. The dependence of excited state dynamics in these systems on the surface hopping/decoherence methodology and the choice of the dynamical basis is investigated and analyzed. We demonstrated that the use of special "electron-only" or "hole-only" excitation bases may be advantageous over using the full "electron-hole" basis of SP states, making the computed dynamics more consistent with the one obtained at the MB level.

High-resolution thermal and magnetic vector gradient imaging is demonstrated using diamond quantum sensors in a microstructured fiber probe platform. These sensors are capable of in situ magnetic field and temperature measurements with 160 pT / Hz and 25 mK / Hz sensitivities.

The fine structure of the band edge exciton and the dark exciton photoluminescence (PL) are topics of significant interest in the research of semiconducting metal halide perovskite nanocrystals, with several conflicting reports on the level ordering of the bright and dark states and the accessibility of the emitting dark states. Recently, we observed the intense dark exciton PL in strongly confined CsPbBr3 nanocrystals at cryogenic temperatures, in contrast to weakly confined nanocrystals lacking dark exciton PL, which was explained by the confinement enhanced bright-dark exciton splitting. In this work, we investigated the size-dependence of the dark exciton photoluminescence properties in CsPbBr3 and CsPbI3 quantum dots in the strongly confined regime, showing the clear role of confinement in determining the bright-dark energy splitting (ΔEBD) and the dark exciton lifetime (τD). We observe the increase in both ΔEBD and τD with increasing quantum confinement in CsPbBr3 and CsPbI3 QDs, consistent with the earlier predictions on the size-dependence of ΔEBD and τD. Our results show that quantum confinement plays a crucial role in determining the accessibility to the dark exciton PL and its characteristics in metal halide perovskite nanocrystals.

Organic-inorganic perovskites have shown great promise towards their application in optoelectronics. The success of this class of material is dictated by the complex interplay between various underlying microscopic phenomena. The structural dynamics of organic cations and the inorganic sublattice after photoexcitation is hypothesized to have a direct effect on the material properties, thereby affecting the overall device performance. Here, we use two-dimensional (2D) electronic spectroscopy to reveal impulsively excited vibrational modes of methylammonium (MA) lead iodide perovskite, which drive the structural distortion after photoexcitation. The vibrational analysis of the measured data allows us to directly monitor the time evolution of the librational motion of the MA cation along with the vibrational coherences of inorganic sublattice. Wavelet analysis of the observed vibrational coherences uncovers the interplay between these two types of phonons. It reveals the coherent generation of the librational motion of the MA cation within ~300 fs, which is complemented by the coherent evolution of the skeletal motion of the inorganic sublattice. We have employed time-dependent density functional theory (TDDFT) to study the atomic motion of the MA cation and the inorganic sublattice during the process of photoexcitation. The TDDFT calculations support our experimental observations of the coherent generation of librational motions in the MA cation and highlight the importance of the anharmonic interaction between the MA cation and the inorganic sublattice. Our calculations predict the transfer of the photoinduced vibrational coherence from the MA cation to the inorganic sublattice, which drives the skeleton motion to form a polaronic state leading to long lifetimes of the charge carriers. This work may lead to novel design principles for next generation of solar cell materials.

A rotation sensor is one of the key elements of inertial navigation systems and compliments most cell phone sensor sets used for various applications. Currently, inexpensive and efficient solutions are mechanoelectronic devices, which nevertheless lack long-term stability. Realization of rotation sensors based on spins of fundamental particles may become a drift-free alternative to such devices. Here, we carry out a proof-of-concept experiment, demonstrating rotation measurements on a rotating setup utilizing nuclear spins of an ensemble of nitrogen vacancy centers as a sensing element with no stationary reference. The measurement is verified by a commercially available microelectromechanical system gyroscope.

Recently, the thulium atom was cooled down to the Bose-Einstein condensation temperature, thus opening a pathway to quantum simulation with this atom. However, successful simulations require instruments to control and readout states of the atom as well as the ability to control the interaction between either different species or different states of the same type of species. In this paper, we provide an experimental demonstration of high-fidelity (over 93%) manipulation of the ground state magnetic sublevels of thulium, which utilizes a simple and efficient design of a microwave (MW) antenna. The coherence time and dephasing rate of the energetically highest hyperfine level of the ground state were also examined.

Remarkable advancements in the ability to create, manipulate, and measure quantum systems are paving the way to build next generations of devices based on quantum physics. Quantum technologies in Russia are on the list of strategically important cross-cutting directions in the framework of the National Technology Initiative programs and the Digital Economy National Program. The broad focus includes quantum computing and simulation, quantum communications, quantum metrology and sensing. This paper reviews existing research on quantum science and technologies in Russia and summarizes the main goals for the next few years that form the basis of an upcoming major national initiative.

Recent time-resolved transient absorption studies demonstrated that the rate of photoinduced interfacial charge transfer (CT) from Zn-phthalocyanine (ZnPc) to single-layer graphene (SLG) is faster than to double-layer graphene (DLG), in contrast to the expectation from Fermi's golden rule. We present the first time-domain non-adiabatic molecular dynamics (NA-MD) study of the electron injection process from photoexcited ZnPc molecules into SLG and DLG substrates. Our calculations suggest that CT occurs faster in the ZnPc/SLG system than in the ZnPc/DLG system, with 580 fs and 810 fs being the fastest components of the observed CT timescales, respectively. The computed timescales are in close agreement with those reported in the experiment. The computed CT timescales are determined largely by the magnitudes of the non-adiabatic couplings (NAC), which we find to be 4 meV and 2 meV, for the ZnPc/SLG and ZnPc/DLG systems, respectively. The transitions are driven mainly by the ZnPc out-of-plane bending mode at 1100 cm−1 and an overtone of fundamental modes in graphene at 2450 cm−1. We find that dephasing occurs on the timescale of 20 fs and is similar in both systems, so decoherence does not notably change the qualitative trends in the CT timescales. We highlight the importance of proper energy level alignment for capturing the qualitative trends in the CT dynamics observed in experiment. In addition, we illustrate several methodological points that are important for accurately modeling nonadiabatic dynamics in the ZnPc/FLG systems, such as the choice of surface hopping methodology, the use of phase corrections, NAC scaling, and the inclusion of Hubbard terms in the density functional and molecular dynamics calculations.

The sensitivity of the nitrogen-vacancy (NV) color centers in diamond-based magnetometers strongly depends on the number of NV centers involved in the measurement. Unfortunately, an increasing concentration of NV centers leads to a decrease in their dephasing and coherence times if the nitrogen content exceeds a certain threshold level (approximately 10 17 c m - 3 or 0.6 ppm). Here, we demonstrate that this increased dephasing can be efficiently compensated for by optimizing the electron irradiation dose in postprocessing procedures in the vicinity of the threshold concentration, thus extending the range of possible useful concentrations of NV centers in diamonds with a natural carbon content.

All-optical thermometry presents a promising avenue of investigation for sensitive biological and electronic systems, with methods free of radio-frequency interference of particular importance. In this work, an all-optical scanning fiber thermometer is tested and shown to possess $5\phantom{\rule{0.2em}{0ex}}\ensuremath{\mu}\mathrm{m}$ spatial and $20\phantom{\rule{0.2em}{0ex}}\mathrm{mK}/\sqrt{\mathrm{Hz}}$ temperature resolution. This probe is then used to generate noncontact scanning thermal images of active circuit elements with microscale thermal features.

Properties of silicon-vacancy (SiV) colour centres in ultra-nanosize diamonds are studied. Nanodiamonds are obtained at a high temperature and pressure, which induced transformations in mixtures of organic and hetero-organic compounds without metal-catalysts. The size distribution of grown nanodiamonds is determined by the methods of transmission electron microscopy and atomic-force microscopy, as well as by using the model of phonon spatial localisation. In addition, Raman spectra of various nanodiamonds and luminescence properties of SiV-centres are investigated.

Bose-Einstein condensation (BEC) is a powerful tool for a wide range of research activities, a large fraction of which is related to quantum simulations. Various problems may benefit from different atomic species, but cooling down novel species interesting for quantum simulations to BEC temperatures requires a substantial amount of optimization and is usually considered to be a difficult experimental task. In this work, we implemented the Bayesian machine learning technique to optimize the evaporative cooling of thulium atoms and achieved BEC in an optical dipole trap operating near 532 nm. The developed approach could be used to cool down other novel atomic species to quantum degeneracy without additional studies of their properties.

Magnetic fields are one of the main tools for controlling the interaction of ultracold atoms using the so-called Feshbach resonances. However, the accurate knowledge of magnetic fields within the high-vacuum chamber is significantly complicated due to the inexact knowledge of the setup geometry, the presence of magnetic parts, and other. In this paper, we demonstrate precision calibration of magnetic fields in the high-vacuum setup using microwave spectroscopy of the ground state of ultracold thulium atoms.

In this work, we study the role of spin–orbit coupling (SOC) in nonradiative relaxation of hot electrons and holes in methylammonium lead perovskite, MAPbI3. For this purpose, we have developed the nonadiabatic molecular dynamics method with two-component spinor wave functions that are solutions of the relativistic Kohn–Sham (KS) equations. We find that SOC enhances contributions of Pb(px) and Pb(py) orbitals to the conduction and valence bands. As a result, the KS orbitals become more sensitive to nuclear motions, leading to the increased nonadiabatic couplings. Consequently, SOC greatly speeds up the electron and hole relaxation, making the computed relaxation time scales consistent with available experiments. We suggest that the fast hot carrier relaxation facilitated by the SOC allows rapid transition into the long-lived triplet state that extends charge-carrier lifetime and helps achieve high-efficiency perovskite solar cells.

A microwave antenna configuration shaped as coaxial resonant coils is proposed for exciting magnetic dipole transitions of the optical ground state of the nitrogen—vacancy color center in diamond. The field within the antenna is simulated, field amplitudes are experimentally measured.

NV centers in diamond recommend themselves as good sensors of environmental fields as well as detectors of diamond impurities. In particular, C-centers, often also called ${{p}_{1}}$-centers, can be detected via double electron-electron resonance. This resonance can be used to measure the C-center concentration. Here, we measured the concentration of C-centers in several diamond plates and investigated the influence of the free precession time of the NV center on the observed contrast in the measured double electron-electron resonance spectrum. The dependence of the resonance amplitudes and widths on the concentration of C-centers as well as the length of the combined C-center driving and NV-center $\pi$-pulse is also discussed. The optimal contrast-free precession time was determined for each C-center concentration, showing a strong correlation with both the concentration of C-centers and the NV-center ${{T}_{2}}$ time.

We present high-resolution, all-optical thermometry based on ensembles of germanium-vacancy (GeV) color center in diamond and implement this method of thermometry in the fiber-optic format. Due to the unique properties of diamond, an all-optical approach using this method opens a way to produce back-action-free temperature measurements with resolution below 0.1 K in a wide range of temperatures.

We report a study on the non-adiabatic molecular dynamics (NA-MD) of the charge transfer (CT) process in the boron subphtalocyanine chloride (SubPc)/fullerene (C60) interface using our newly implemented Libra-X software package, which is based on an interface of the Libra NA-MD library and the GAMESS electronic structure software. In particular, we address the following aspects of the simulation protocol: (a) the choice of the potential used to treat interatomic interactions and its effect on the structures of the complex and CT rates; (b) the choice of the electronic structure methodology used; and (c) the choice of the trajectory surface hopping (TSH) methodology used. From our analysis of the electronic structure, we suggest that the distortion of the SubPc conical structure affects orbital localization and that the “breathing” motion of SubPc drives the CT process in SubPc/C60. This study illustrates that the choice of the TSH methodology and electronic decoherence are crucial for the CT simulation. We extend our analysis of CT in SubPc/(C60)n models by increasing the number of C60 molecules up to n = 4. We find that the details of the interfacial SubPc/(C60)n geometry determine the CT rate. Finally, we find the computed CT timescale to be in the range of 2.2–5.0 ps, which is in agreement with the experimentally determined timescale in the order of magnitude of ∼10 ps. The developed open-source Libra-X package is freely available on the Internet at https://github.com/Quantum-Dynamics-Hub/Libra-X.