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Register a new userClock Transitions Guard Against Spin Decoherence in Singlet Fission
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Short coherence times present a primary obstacle in quantum computing and sensing applications. In atomic systems, clock transitions (CTs), formed from avoided crossings in an applied Zeeman field, can substantially increase coherence times. We show how CTs can dampen intrinsic and extrinsic sources of quantum noise in molecules. Conical intersections between two periodic potentials form CTs in electron paramagnetic resonance experiments of the spin-polarized singlet fission photoproduct. We report on a pair of CTs for a two-chromophore molecule in terms of the Zeeman field strength, molecular orientation relative to the field, and molecular geometry.
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In many important situations the dominant dephasing mechanism in cryogenic rare-earth-ion doped systems is due to magnetic field fluctuations from spins in the host crystal. Operating at a magnetic field where a transition has a zero first-order-Zeeman (ZEFOZ) shift can greatly reduce this dephasing. Here we identify the location of transitions with zero first-order Zeeman shift for optical transitions in Pr3+:YAG and for spin transitions in Er3+:Y2SiO5. The long coherence times that ZEFOZ would enable would make Pr3+:YAG a strong candidate for achieving the strong coupling regime of cavity QED, and would be an important step forward in creating long-lived telecommunications wavelength quantum memories in Er3+:Y2SiO5. This work relies mostly on published spin Hamiltonian parameters but Raman heterodyne spectroscopy was performed on Pr3+:YAG to measure the parameters for the excited state.
We present a novel method for engineering an optical clock transition that is robust against external field fluctuations and is able to overcome limits resulting from field inhomogeneities. The technique is based on the application of continuous driving fields to form a pair of dressed states essentially free of all relevant shifts. Specifically, the clock transition is robust to magnetic shifts, quadrupole and other tensor shifts, and amplitude fluctuations of the driving fields. The scheme is applicable to either a single ion or an ensemble of ions, and is relevant for several types of ions, such as $^{40}mathrm{Ca}^{+}$, $^{88}mathrm{Sr}^{+}$, $^{138}mathrm{Ba}^{+}$ and $^{176}mathrm{Lu}^{+}$. Taking a spherically symmetric Coulomb crystal formed by 400 $^{40}mathrm{Ca}^{+}$ ions as an example, we show through numerical simulations that the inhomogeneous linewidth of tens of Hertz in such a crystal together with linear Zeeman shifts of order 10~MHz are reduced to form a linewidth of around 1~Hz. We estimate a two-order-of-magnitude reduction in averaging time compared to state-of-the art single ion frequency references, assuming a probe laser fractional instability of $10^{-15}$. Furthermore, a statistical uncertainty reaching $2.9times 10^{-16}$ in 1~s is estimated for a cascaded clock scheme in which the dynamically decoupled Coulomb crystal clock stabilizes the interrogation laser for an $^{27}mathrm{Al}^{+}$ clock.
Despite the importance of isotopically purified samples in current experiments, there have been few corresponding studies of spin qubit decoherence using full quantum bath calculations. Isotopic purification eliminates the well-studied nuclear spin baths which usually dominate decoherence. We model the coherence of electronic spin qubits in silicon near so called Clock Transitions (CT) where experiments have electronic $T_{2e}$ times of seconds. Despite the apparent simplicity of the residual decoherence mechanism, this regime is not well understood: the state mixing which underpins CTs allows also a proliferation of contributions from usually forbidden channels (direct flip-flops with non-resonant spins); in addition, the magnitude and effects of the corresponding Overhauser fields and other detunings is not well quantified. For purely magnetic detunings, we identify a regime, potentially favourable for quantum computing, where forbidden channels are completely suppressed but spins in resonant states are fully released from Overhauser fields and applied magnetic field gradients. We show by a general argument that the enhancement between this regime and the high field limit is $< 8$, regardless of density, while enhancements of order 50 are measured experimentally. We propose that this discrepancy is likely to arise from strains of exclusively non-magnetic origin, underlining the potential of CTs for isolating and probing different types of inhomogeneities. We also identify a set of fields, Dipolar Refocusing Points (DRPs), where the Hahn echo fully refocuses the effect of the dipolar interaction.
Singlet fission is a process whereby two triplet excitons can be produced from one photon, potentially increasing the efficiency of photovoltaic devices. Endothermic singlet fission is desired for maximum energy conversion efficiency, and such systems have been shown to form an excimer-like state with multi-excitonic character prior to the appearance of triplets. However, the role of the excimer as an intermediate has, until now, been unclear. Here we show, using 5,12-bis((triisopropylsilyl)ethynyl)tetracene in solution as a prototypical example, that, rather than acting as an intermediate, the excimer serves to trap excited states, to the detriment of singlet fission yield. We clearly demonstrate that singlet fission and its conjugate process, triplet-triplet annihilation, occur at a longer intermolecular distance than an excimer intermediate would impute. These results establish that an endothermic singlet fission material must be designed that avoids excimer formation, thus allowing singlet fission to reach its full potential in enhancing photovoltaic energy conversion.
Singlet exciton fission (SEF) is a key process in the development of efficient opto-electronic devices. An aspect that is rarely probed directly, and yet has a tremendous impact on SEF properties, is the nuclear structure and dynamics involved in this process. Here we directly observe the nuclear dynamics accompanying the SEF process in single crystal pentacene using femtosecond electron diffraction. The data reveal coherent atomic motions at 1 THz, incoherent motions, and an anisotropic lattice distortion representing the polaronic character of the triplet excitons. Combining molecular dynamics simulations, time-dependent density functional theory and experimental structure factor analysis, the coherent motions are identified as collective sliding motions of the pentacene molecules along their long axis. Such motions modify the excitonic coupling between adjacent molecules. Our findings reveal that long-range motions play a decisive part in the disintegration of the electronically correlated triplet pairs, and shed light on why SEF occurs on ultrafast timescales.
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