Electronic Coherence Times Research Articles

Coherent control of the orbital occupation driving the insulator-to-metal Mott transition in V2O3

Managing light-matter interactions on timescales faster than the loss of electronic coherence is key for achieving full quantum control of the final products in solid-solid transformations. In this Letter, we demonstrate coherent optical control of the orbital occupation that determines the insulator-to-metal transition in the prototypical Mott insulator ${\mathrm{V}}_{2}{\mathrm{O}}_{3}$. Selective excitation of a specific interband transition with two phase-locked light pulses manipulates the occupation of the correlated bands in a way that depends on the coherent evolution of the photoinduced superposition of states. A comparison between experimental results and numerical solutions of the optical Bloch equations provides an electronic coherence time on the order of 5 fs. Temperature-dependent experiments suggest that the electronic coherence time is enhanced in the vicinity of the insulator-to-metal transition critical temperature, thus highlighting the role of fluctuations in determining the electronic coherence. These results open different routes to selectively switch the functionalities of quantum materials and coherently control solid-solid electronic transformations.

Coherent Control of a Nuclear Spin via Interactions with a Rare-Earth Ion in the Solid State

Individually addressed Er$^{3+}$ ions in solid-state hosts are promising resources for quantum repeaters, because of their direct emission in the telecom band and compatibility with silicon photonic devices. While the Er$^{3+}$ electron spin provides a spin-photon interface, ancilla nuclear spins could enable multi-qubit registers with longer storage times. In this work, we demonstrate coherent coupling between the electron spin of a single Er$^{3+}$ ion and a single $I=1/2$ nuclear spin in the solid-state host crystal, which is a fortuitously located proton ($^1$H). We control the nuclear spin using dynamical decoupling sequences applied to the electron spin, implementing one- and two-qubit gate operations. Crucially, the nuclear spin coherence time exceeds the electron coherence time by several orders of magnitude, because of its smaller magnetic moment. These results provide a path towards combining long-lived nuclear spin quantum registers with telecom-wavelength emitters for long-distance quantum repeaters.

Hyperfine interactions and coherent spin dynamics of isotopically purified 167Er3+ in polycrystalline Y2O3

167Er3+ doped solids are a promising platform for quantum technology due to erbium’s telecom C-band optical transition and its long hyperfine coherence times. We experimentally study the spin Hamiltonian and dynamics of 167Er3+ spins in Y2O3 using electron paramagnetic resonance (EPR) spectroscopy. The anisotropic electron Zeeman, hyperfine and nuclear quadrupole matrices are fitted using data obtained by X-band (9.5 GHz) EPR spectroscopy. We perform pulsed EPR spectroscopy to measure spin relaxation time T 1 and coherence time T 2 for the 3 principal axes of an anisotropic g tensor. Long electronic spin coherence time up to 24.4 μs is measured for lowest g transition at 4 K, exceeding previously reported values at much lower temperatures. Measurements of decoherence mechanism indicates T 2 limited by spectral diffusion and instantaneous diffusion. Long spin coherence times, along with a strong anisotropic hyperfine interaction makes 167Er3+:Y2O3 a rich system and an excellent candidate for spin-based quantum technologies.

Attosecond-Resolved Coherent Control of Lattice Vibrations in Thermoelectric SnSe.

Manipulating lattice vibrations is the cornerstone to achieving ultralow thermal conductivity in thermoelectrics. Although spatial control by novel material designs has been recently reported, temporal manipulation, which can shape thermoelectric properties under nonequilibrium conditions, remains largely unexplored. Here, taking SnSe as a representative, we have demonstrated that in the ultrafast pump-pump-probe spectroscopy, electronic and lattice coherences inherited from optical excitations can be exploited independently to manipulate phonon oscillations in a highly selective manner. Specifically, when the pump-pump delay time (tmod) is in the electronic coherence time range, the amplitude, frequency, and lifetime of all phonon modes are simultaneously following the optical cycle. While extending tmod into the lattice coherence time range, the amplitude of each coherent phonon mode can be selectively manipulated according to its intrinsic period without changing the frequency and lifetime. This work opens up exciting avenues to temporally and discriminatorily manipulate phononic processes in thermoelectric materials.

Quantum dynamics simulation of intramolecular singlet fission in covalently linked tetracene dimer.

In this work, we study singlet fission in tetracene para-dimers, covalently linked by a phenyl group. In contrast to most previous studies, we account for the full quantum dynamics of the combined excitonic and vibrational system. For our simulations, we choose a numerically unbiased representation of the molecule's wave function, enabling us to compare with experiments, exhibiting good agreement. Having access to the full wave function allows us to study in detail the post-quench dynamics of the excitons. Here, one of our main findings is the identification of a time scale t0 ≈ 35fs dominated by coherent dynamics. It is within this time scale that the larger fraction of the singlet fission yield is generated. We also report on a reduced number of phononic modes that play a crucial role in the energy transfer between excitonic and vibrational systems. Notably, the oscillation frequency of these modes coincides with the observed electronic coherence time t0. We extend our investigations by also studying the dependency of the dynamics on the excitonic energy levels that, for instance, can be experimentally tuned by means of the solvent polarity. Here, our findings indicate that the singlet fission yield can be doubled, while the electronic coherence time t0 is mainly unaffected.

Electronic Coherence and Coherent Dephasing in the Optical Control of Electrons in Graphene.

Electronic coherence is of utmost importance for the access and control of quantum-mechanical solid-state properties. Using a purely electronic observable, the photocurrent, we measure a lower bound of the electronic coherence time of 22 ± 4 fs in graphene. The photocurrent is ideally suited to measure electronic coherence, as it is a direct result of coherent quantum-path interference, controlled by the delay between two ultrashort two-color laser pulses. The maximum delay for which interference between the population amplitude injected by the first pulse interferes with that generated by the second pulse determines the electronic coherence time. In particular, numerical simulations reveal that the experimental data yields a lower bound on the electronic coherence time, masked by coherent dephasing due to the broadband absorption in graphene. We expect that our results will significantly advance the understanding of coherent quantum control in solid-state systems ranging from excitation with weak fields to strongly driven systems.

On-the-Fly AbInitio Semiclassical Evaluation of Electronic Coherences in Polyatomic Molecules Reveals a Simple Mechanism of Decoherence.

Irradiation of a molecular system by an intense laser field can trigger dynamics of both electronic and nuclear subsystems. The lighter electrons usually move on much faster, attosecond timescale but the slow nuclear rearrangement damps ultrafast electronic oscillations, leading to the decoherence of the electronic dynamics within a few femtoseconds. We show that a simple, single-trajectory semiclassical scheme can evaluate the electronic coherence time in polyatomic molecules accurately by demonstrating an excellent agreement with full-dimensional quantum calculations. In contrast to numerical quantum methods, the semiclassical one reveals the physical mechanism of decoherence beyond the general blame on nuclear motion. In the propiolic acid, the rate of decoherence and the large deviation from the static frequency of electronic oscillations are quantitatively described with just two semiclassical parameters-the phase space distance and signed area between the trajectories moving on two electronic surfaces. Because it evaluates the electronic structure on the fly, the semiclassical technique avoids the "curse of dimensionality" and should be useful for preselecting molecules for experimental studies.

Narrow Optical Line Widths in Erbium Implanted in TiO2.

Atomic and atomlike defects in the solid state are widely explored for quantum computers, networks, and sensors. Rare earth ions are an attractive class of atomic defects that feature narrow spin and optical transitions that are isolated from the host crystal, allowing incorporation into a wide range of materials. However, the realization of long electronic spin coherence times is hampered by magnetic noise from abundant nuclear spins in the most widely studied host crystals. Here, we demonstrate that Er3+ ions can be introduced via ion implantation into TiO2, a host crystal that has not been studied extensively for rare earth ions and has a low natural abundance of nuclear spins. We observe efficient incorporation of the implanted Er3+ into the Ti4+ site (>50% yield) and measure narrow inhomogeneous spin and optical line widths (20 and 460 MHz, respectively) that are comparable to bulk-doped crystalline hosts for Er3+. This work demonstrates that ion implantation is a viable path to studying rare earth ions in new hosts and is a significant step toward realizing individually addressed rare earth ions with long spin coherence times for quantum technologies.

Lewis Base Passivation of Hybrid Halide Perovskites Slows Electron-Hole Recombination: Time-Domain Ab Initio Analysis.

Nonradiative electron-hole recombination plays a key role in determining photon conversion efficiencies in solar cells. Experiments demonstrate significant reduction in the recombination rate upon passivation of methylammonium lead iodide perovskite with Lewis base molecules. Using nonadiabatic molecular dynamics combined with time-domain density functional theory, we find that the nonradiative charge recombination is decelerated by an order of magnitude upon adsorption of the molecules. Thiophene acts by the traditional passivation mechanism, forcing electron density away from the surface. In contrast, pyridine localizes the electron at the surface while leaving it energetically near the conduction band edge. This is because pyridine creates a stronger coordinative bond with a lead atom of the perovskite and has a lower energy unoccupied orbital compared with thiophene due to the more electronegative nitrogen atom relative to thiophene's sulfur. Both molecules reduce two-fold the nonadiabatic coupling and electronic coherence time. A broad range of vibrational modes couple to the electronic subsystem, arising from inorganic and organic components. The simulations reveal the atomistic mechanisms underlying the enhancement of the excited-state lifetime achieved by the perovskite passivation, rationalize the experimental results, and advance our understanding of charge-phonon dynamics in perovskite solar cells.

Nonadiabatic Vibrational Damping of Molecular Adsorbates: Insights into Electronic Friction and the Role of Electronic Coherence.

We present a perturbation approach rooted in time-dependent density-functional theory to calculate electron-hole (e-h) pair excitation spectra during the nonadiabatic vibrational damping of adsorbates on metal surfaces. Our analysis for the benchmark systems CO on Cu(100) and Pt(111) elucidates the surprisingly strong influence of rather short electronic coherence times. We demonstrate how in the limit of short electronic coherence times, as implicitly assumed in prevalent quantum nuclear theories for the vibrational lifetimes as well as electronic friction, band structure effects are washed out. Our results suggest that more accurate lifetime or chemicurrentlike experimental measurements could characterize the electronic coherence.

Nuclear spin cooling by electric dipole spin resonance and coherent population trapping

Nuclear spin fluctuation suppression is a key issue in preserving electron coherence for quantum information/computation. We propose an efficient way of nuclear spin cooling in semiconductor quantum dots (QDs) by the coherent population trapping (CPT) and the electric dipole spin resonance (EDSR) induced by optical fields and ac electric fields. The EDSR can enhance the spin flip-flop rate and may bring out bistability under certain conditions. By tuning the optical fields, we can avoid the EDSR induced bistability and obtain highly polarized nuclear spin state, which results in long electron coherence time. With the help of CPT and EDSR, an enhancement of 1500 times of the electron coherence time can been obtained after a 500ns preparation time.

Dynamic nuclear polarization enhanced magnetic field sensitivity and decoherence spectroscopy of an ensemble of near-surface nitrogen-vacancy centers in diamond

We perform pulsed optically detected electron spin resonance to measure the DC magnetic field sensitivity and electronic spin coherence time T2 of an ensemble of near-surface, high-density nitrogen-vacancy centers engineered to have a narrow magnetic resonance linewidth. Combining pulsed spectroscopy with dynamic nuclear polarization, we obtain the photon-shot-noise-limited DC magnetic sensitivity of 35 nT Hz−0.5. We find that T2 is controlled by instantaneous diffusion, enabling decoherence spectroscopy on residual nitrogen impurity spins in the diamond lattice and a quantitative determination of their density. The demonstrated high DC magnetic sensitivity and decoherence spectroscopy are expected to broaden the application range for two-dimensional magnetic imaging.

Optical nuclear spin polarization in quantum dots**Project partially supported by the National Natural Science Foundations of China (Grant Nos. 11374039 and 11174042) and the National Basic Research Program of China (Grant Nos. 2011CB922204 and 2013CB632805).

Hyperfine interaction between electron spin and randomly oriented nuclear spins is a key issue of electron coherence for quantum information/computation. We propose an efficient way to establish high polarization of nuclear spins and reduce the intrinsic nuclear spin fluctuations. Here, we polarize the nuclear spins in semiconductor quantum dot (QD) by the coherent population trapping (CPT) and the electric dipole spin resonance (EDSR) induced by optical fields and ac electric fields. By tuning the optical fields, we can obtain a powerful cooling background based on CPT for nuclear spin polarization. The EDSR can enhance the spin flip–flop rate which may increase the cooling efficiency. With the help of CPT and EDSR, an enhancement of 1300 times of the electron coherence time can be obtained after a 10-ns preparation time.

Collective non-perturbative coupling of 2D electrons with high-quality-factor terahertz cavity photons

Nonperturbative coupling of light with condensed matter in an optical cavity is expected to reveal a host of coherent many-body phenomena and states. In addition, strong coherent light-matter interaction in a solid-state environment is of great interest to emerging quantum-based technologies. However, creating a system that combines a long electronic coherence time, a large dipole moment, and a high cavity quality ($Q$) factor has been a challenging goal. Here, we report collective ultrastrong light-matter coupling in an ultrahigh-mobility two-dimensional electron gas in a high-$Q$ terahertz photonic-crystal cavity in a quantizing magnetic field, demonstrating a cooperativity of $\sim$360. The splitting of cyclotron resonance (CR) into the lower and upper polariton branches exhibited a $\sqrt{n_\mathrm{e}}$-dependence on the electron density ($n_\mathrm{e}$), a hallmark of collective vacuum Rabi splitting. Furthermore, a small but definite blue shift was observed for the polariton frequencies due to the normally negligible $A^2$ term in the light-matter interaction Hamiltonian. Finally, the high-$Q$ cavity suppressed the superradiant decay of coherent CR, which resulted in an unprecedentedly narrow intrinsic CR linewidth of 5.6 GHz at 2 K. These results open up a variety of new possibilities to combine the traditional disciplines of many-body condensed matter physics and cavity-based quantum optics.

Quantum charge pumping in graphene-based devices: When lattice defects do help

Quantum charge pumping, the quantum coherent generation of a dc current at zero bias through time-dependent potentials, provides outstanding opportunities for metrology and the development of nanodevices. The long electronic coherence times and high quality of the crystal structure of graphene may provide suitable building blocks for such quantum pumps. Here, we focus in adiabatic quantum pumping through graphene nanoribbons in the Fabry-Pérot regime highlighting the crucial role of defects by using atomistic simulations. We show that even a single defect added to the pristine structure may produce a two orders of magnitude increase in the pumped charge.

Magnetization and spin dynamics of the spinS=12hourglass nanomagnet Cu5(OH)2(NIPA)4·10H2O

We report a combined experimental and theoretical study of the spin S=1/2 nanomagnet Cu5(OH)2(NIPA)4*10H2O (Cu5-NIPA). Using thermodynamic, electron spin resonance and 1H nuclear magnetic resonance measurements on one hand, and ab initio density-functional band-structure calculations, exact diagonalizations and a strong coupling theory on the other, we derive a microscopic magnetic model of Cu5-NIPA and characterize the spin dynamics of this system. The elementary five-fold Cu2+ unit features an hourglass structure of two corner-sharing scalene triangles related by inversion symmetry. Our microscopic Heisenberg model comprises one ferromagnetic and two antiferromagnetic exchange couplings in each triangle, stabilizing a single spin S=1/2 doublet ground state (GS), with an exactly vanishing zero-field splitting (by Kramer's theorem), and a very large excitation gap of \Delta~68 K. Thus, Cu5-NIPA is a good candidate for achieving long electronic spin relaxation (T1) and coherence (T2) times at low temperatures, in analogy to other nanomagnets with low-spin GS's. Of particular interest is the strongly inhomogeneous distribution of the GS magnetic moment over the five Cu2+ spins. This is a purely quantum-mechanical effect since, despite the non-frustrated nature of the magnetic couplings, the GS is far from the classical collinear ferrimagnetic configuration. Finally, Cu5-NIPA is a rare example of a S=1/2 nanomagnet showing an enhancement in the nuclear spin-lattice relaxation rate 1/T1 at intermediate temperatures.

Solid-state electronic spin coherence time approaching one second

Solid-state spin systems such as nitrogen-vacancy colour centres in diamond are promising for applications of quantum information, sensing and metrology. However, a key challenge for such solid-state systems is to realize a spin coherence time that is much longer than the time for quantum spin manipulation protocols. Here we demonstrate an improvement of more than two orders of magnitude in the spin coherence time (T₂) of nitrogen-vacancy centres compared with previous measurements: T₂≈0.6 s at 77 K. We employed dynamical decoupling pulse sequences to suppress nitrogen-vacancy spin decoherence, and found that T₂ is limited to approximately half of the longitudinal spin relaxation time over a wide range of temperatures, which we attribute to phonon-induced decoherence. Our results apply to ensembles of nitrogen-vacancy spins, and thus could advance quantum sensing, enable squeezing and many-body entanglement, and open a path to simulating driven, interaction-dominated quantum many-body Hamiltonians.

Sub-100 fs charge transfer in a novel donor–acceptor–donor triad organized in a smectic film

Ultrafast transient absorption spectroscopy is performed on a novel donor-acceptor-donor triad made of two identical bisthiophene derivatives as electron donors and a central perylenediimide moiety as electron acceptor. The triad is extended at both ends by covalently bound siloxane chains that confer self-organisation into thin smectic films at ambient temperature. When diluted in chloroform, selective excitation of the donor moiety leads to resonance energy transfer within 130 fs to the acceptor moiety, followed by the formation of a charge transfer (CT) state in ~3 ps. The CT state recombines entirely on a 55 ps time scale. In the liquid crystal films, excitonic intermolecular coupling leads to significant changes in the dynamics. Most remarkably, ultrafast intra- and intermolecular CT state formation occurs in about 60 fs, i.e. on a time scale comparable to electronic coherence times. While the intra-molecular CT states recombine on the same time scale as in solution or even faster, inter-molecular CT states live for about 1 ns. Last, triplet states of the perylenediimide moiety dominate the differential absorption after ~1 ns. We anticipate that the fast recombination of intra-molecular CT states and the triplet state formation may severely limit the photo-current in these materials.

Suppression of electron spin decoherence in a quantum dot

The dominant source of decoherence for an electron spin in a quantum dot is the hyperfine interaction with the surrounding bath of nuclear spins. The decoherence process may be slowed down by subjecting the electron spin to suitable sequences of external control pulses. We investigate the performance of a variety of dynamical decoupling protocols using exact numerical simulation. Emphasis is given to realistic pulse delays and the long-time limit, beyond the domain where available analytical approaches are guaranteed to work. Our results show that both deterministic and randomized protocols are capable to significantly prolong the electron coherence time, even when using control pulse separations substantially larger than what expected from the upper cutoff frequency of the coupling spectrum between the electron and the nuclear spins. In a realistic parameter range, the total width of such a coupling spectrum appears to be the physically relevant frequency scale affecting the overall quality of the decoupling.

Ultrafast dynamics of halogens in rare gas solids

We perform time resolved pump-probe spectroscopy on small halogen molecules ClF, Cl2, Br2, and I2 embedded in rare gas solids (RGS). We find that dissociation, angular depolarization, and the decoherence of the molecule is strongly influenced by the cage structure. The well ordered crystalline environment facilitates the modelling of the experimental angular distribution of the molecular axis after the collision with the rare gas cage. The observation of many subsequent vibrational wave packet oscillations allows the construction of anharmonic potentials and indicate a long vibrational coherence time. We control the vibrational wave packet revivals, thereby gaining information about the vibrational decoherence. The coherence times are remarkable larger when compared to the liquid or high pressure gas phase. This fact is attributed to the highly symmetric molecular environment of the RGS. The decoherence and energy relaxation data agree well with a perturbative model for moderate vibrational excitation and follow a classical model in the strong excitation limit. Furthermore, a wave packet interferometry scheme is applied to deduce electronic coherence times. The positions of those cage atoms, excited by the molecular electronic transitions are modulated by long living coherent phonons of the RGS, which we can probe via the molecular charge transfer states.