The ability to control dynamics of quantum states by optical interference, and subsequent electrical read-out, is crucial for solid state quantum technologies. Ramsey interference has been successfully observed for spins in silicon and nitrogen vacancy centres in diamond, and for orbital motion in InAs quantum dots. Here we demonstrate terahertz optical excitation, manipulation and destruction via Ramsey interference of orbital wavepackets in Si:P with electrical read-out. We show milliradian control over the wavefunction phase for the two-level system formed by the 1s and 2p states. The results have been verified by all-optical echo detection methods, sensitive only to coherent excitations in the sample. The experiments open a route to exploitation of donors in silicon for atom trap physics, with concomitant potential for quantum computing schemes, which rely on orbital superpositions to, for example, gate the magnetic exchange interactions between impurities.
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http://dx.doi.org/10.1038/ncomms7549 | DOI Listing |
J Phys Chem A
August 2024
School of Chemistry, Indian Institute of Science Education and Research Thiruvananthapuram, Maruthamala PO, Vithura, Thiruvananthapuram, Kerala 695551, India.
Gas phase excited-state quantum wavepacket dynamics simulations of the thiotropolone demonstrate the ultrafast triplet formation upon photoexcitation to the dipole-allowed S state. The dominant relaxation pathway of the S-T intersystem crossing, facilitated by the strong spin-orbit coupling and narrow energy gap, competes with the S to S/S internal conversion. The wavepacket populated in T via the former pathway decays to lower triplet states.
View Article and Find Full Text PDFNat Commun
June 2024
School of Optical-Electrical and Computer Engineering, University of Shanghai for Science and Technology, Shanghai, China.
J Phys Chem A
April 2024
Laboratoire de Chimie Quantique, Institut de Chimie Strasbourg, UMR-7177 CNRS, Université de Strasbourg, 1 Rue Blaise Pascal BP 296/R8, F-67008 Strasbourg, France.
The ultrafast nonadiabatic excited state dynamics of (PTZ-N-benzyl-acetylide) (-bis-trimethylphosphine) Pt(II) (acetylide-NDI-bis-methyl) , representative of a series of Pt(II) donor-bridge-acceptor assemblies experimentally studied by the Weinstein group, University of Sheffield, is investigated by means of wavepacket propagations based on the multiconfiguration time-dependent Hartree (MCTDH) method. On the basis of electronic structure data obtained at the time-dependent density functional theory (TD-DFT) level, the subpicosecond decay is simulated by solving an 11 electronic states multimode problem, up to 18 vibrational normal modes, including both spin-orbit coupling (SOC) and vibronic coupling. A careful analysis of the results, within the diabatic representation, provides the key features of the spin-vibronic mechanism at work in this complex, distinguishing between the spin-orbit and vibronically activated ultrafast processes within the excited states manifold.
View Article and Find Full Text PDFPhys Chem Chem Phys
February 2024
Wilhelm-Ostwald-Institut für Physikalische und Theoretische Chemie, Universität Leipzig, Linnéstr. 2, 04103, Leipzig, Germany.
Vibrational wave-packet dynamics on the ground electronic state of the neutral silver pentamer (Ag) are studied by femtosecond (fs) pump-probe spectroscopy using the 'negative ion - to neutral - to positive ion' (NeNePo) excitation scheme. A vibrational wave packet is prepared on the A state of Ag photodetachment of mass-selected, cryogenically cooled Ag anions using a fs pump pulse. The temporal evolution of the vibrational wave packet is then probed by an ultrafast probe pulse resonant multiphoton ionization to Ag.
View Article and Find Full Text PDFJ Chem Phys
February 2024
Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA.
We show that standard Ehrenfest dynamics does not conserve linear and angular momentum when using a basis of truncated adiabatic states. However, we also show that previously proposed effective Ehrenfest equations of motion [M. Amano and K.
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