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Register a new userQuantum process tomography of entangled photons as a probe of intermediates of singlet fission in a tetracene derivative
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Spin-entaglement has been proposed and extensively used in the case of correlated triplet pairs which are intermediate states in singlet fission process in select organic semiconductors. Here, we employ quantum process tomography of polarization entangled photon-pairs resonant with the excited state absorption of these states to investigate the nature of the inherent quantum correlations and to explore for an unambiguous proof for the existence of exciton entanglement.
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In this work we study singlet fission in tetracene para-dimers, covalently linked by a phenyl group. In contrast to most previous works, 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 molecules 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 $t_0 approx 35 text{fs}$ 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 for the energy transfer between excitonic and vibrational system. Notably, the oscillation frequency of these modes coincides with the observed electronic coherence time $t_0$. We extended 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 $t_0$ is mainly unaffected.
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.
Singlet fission in tetracene generates two triplet excitons per absorbed photon. If these triplet excitons can be effectively transferred into silicon (Si) then additional photocurrent can be generated from photons above the bandgap of Si. This could alleviate the thermalization loss and increase the efficiency of conventional Si solar cells. Here we show that a change in the polymorphism of tetracene deposited on Si due to air exposure, facilitates triplet transfer from tetracene into Si. Magnetic field-dependent photocurrent measurements confirm that triplet excitons contribute to the photocurrent. The decay of tetracene delayed photoluminescence was used to determine a triplet transfer time of 215 ns and a maximum yield of triplet transfer into Si of ~50 %. Our study suggests that control over the morphology of tetracene during deposition will be of great importance to boost the triplet transfer yield further.
The realization of a future quantum Internet requires processing and storing quantum information at local nodes, and interconnecting distant nodes using free-space and fibre-optic links. Quantum memories for light are key elements of such quantum networks. However, to date, neither an atomic quantum memory for non-classical states of light operating at a wavelength compatible with standard telecom fibre infrastructure, nor a fibre-based implementation of a quantum memory has been reported. Here we demonstrate the storage and faithful recall of the state of a 1532 nm wavelength photon, entangled with a 795 nm photon, in an ensemble of cryogenically cooled erbium ions doped into a 20 meter-long silicate fibre using a photon-echo quantum memory protocol. Despite its currently limited efficiency and storage time, our broadband light-matter interface brings fibre-based quantum networks one step closer to reality. Furthermore, it facilitates novel tests of light-matter interaction and collective atomic effects in unconventional materials.
An ideal source of entangled photon pairs combines the perfect symmetry of an atom with the convenient electrical trigger of light sources based on semiconductor quantum dots. We create a naturally symmetric quantum dot cascade that emits highly entangled photon pairs on demand. Our source consists of strain-free GaAs dots self-assembled on a triangular symmetric (111)A surface. The emitted photons strongly violate Bells inequality and reveal a fidelity to the Bell state as high as 86 (+-2) % without postselection. This result is an important step towards scalable quantum-communication applications with efficient sources.
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