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Optics and Spectroscopy

Stochastic theory of optically detected coherent phenomena in the triplet state of single molecules

Alexander P. Nizovtsev, S. Ya. Kilin, P. R. Berman, Christian von Borczyskowski, Jörg Wrachtrup

Published Jun 1, 1997• 0 citations
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The on-demand manipulation of triplet states in closed-shell single molecules is still out of reach due to a lack of information about the energy of those triplet states. Yet, the access to triplet states would open up a route toward an all-optical single-molecule photonic switch/transistor and, moreover, would provide a way of performing coherent spin operations from the spinless ground state. In this work, we take an important step toward those aims by measuring the triplet energy from the weak phosphorescence signal of perdeuterated perylene, embedded as a guest molecule in a dibenzothiophene host matrix, which well preserves the coherence properties of the perylene guest. We find that perylene’s phosphorescence can be enhanced in this host matrix, when acting as an intermediary for the generation of triplet excitons. The triplet energy that we find can be used to significantly narrow down the search for the ultraweak spin-forbidden transitions from the ground singlet to the triplet states of a single molecule.

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In this article, we address fluorescence of single molecule inside a plasmonic picocavity by proposing a semi-classical theory via combining the macroscopic quantum electrodynamics theory and the open quantum system theory. To gain insights into the experimental results [Nat. Photonics, 14, 693 (2020)], we have further equipped this theory with the classical electromagnetic simulation of the pico-cavity, formed by single atom decorated silver STM tip and a silver substrate, and the time-dependent density functional theory calculation of zinc phthalocyanine molecule. Our simulations not only reproduce the fluorescence spectrum as measured in the experiment, confirming the influence of extreme field confinement afforded by the picocavity, but also reveal Rabi oscillation dynamics and Mollow triplets spectrum for moderate laser excitation. Thus, our study highlights the possibility of coherently manipulating the molecular state and exploring non-linear optical phenomena with the plasmonic picocavity.

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Optical spectroscopy of single molecules: application to nonlinear and quantum optics

Ch. Brunel, Philippe Tamarat, Brahim Lounis +1 more

Journal of Luminescence•May 1, 2000•3 citations
The on-demand manipulation of triplet states in closed-shell single molecules is still out of reach due to a lack of information about the energy of those triplet states. Yet, the access to triplet states would open up a route toward an all-optical single-molecule photonic switch/transistor and, moreover, would provide a way of performing coherent spin operations from the spinless ground state. In this work, we take an important step toward those aims by measuring the triplet energy from the weak phosphorescence signal of perdeuterated perylene, embedded as a guest molecule in a dibenzothiophene host matrix, which well preserves the coherence properties of the perylene guest. We find that perylene’s phosphorescence can be enhanced in this host matrix, when acting as an intermediary for the generation of triplet excitons. The triplet energy that we find can be used to significantly narrow down the search for the ultraweak spin-forbidden transitions from the ground singlet to the triplet states of a single molecule.
In this article, we address fluorescence of single molecule inside a plasmonic picocavity by proposing a semi-classical theory via combining the macroscopic quantum electrodynamics theory and the open quantum system theory. To gain insights into the experimental results [Nat. Photonics, 14, 693 (2020)], we have further equipped this theory with the classical electromagnetic simulation of the pico-cavity, formed by single atom decorated silver STM tip and a silver substrate, and the time-dependent density functional theory calculation of zinc phthalocyanine molecule. Our simulations not only reproduce the fluorescence spectrum as measured in the experiment, confirming the influence of extreme field confinement afforded by the picocavity, but also reveal Rabi oscillation dynamics and Mollow triplets spectrum for moderate laser excitation. Thus, our study highlights the possibility of coherently manipulating the molecular state and exploring non-linear optical phenomena with the plasmonic picocavity.
Optical interfaces that connect long-lived spin qubits to photons are a central requirement for quantum networking and distributed quantum information processing. Currently, solid-state atomic defects are leading candidates due to their inherent spin and optical coherence. Building on these advancements, synthetically tailored molecular systems represent a fundamental change in the field, utilizing precise atomic control and consistent bottom-up assembly. However, the lack of a robust spin-photon interface combining bright fluorescence, high spectral stability, and the persistent spin lifetimes inherent to ground-state systems has prohibited the detection of individual molecular qubits. Here we show that a triplet ground state carbene molecule, embedded within a structurally matched host crystal, functions as a robust spin-photon interface with single-molecule addressability. The system exhibits narrow zero-phonon lines, spectral stability over more than an hour, spin-selective optical transitions and single-molecule optically detected magnetic resonance. Coherent control yields millisecond-scale dynamical-decoupling coherence and tens-of-milliseconds spin relaxation at a temperature of 4.5 K. These results establish molecular qubits as a viable platform for single-emitter quantum optics while preserving the advantages of bottom-up chemical design and processable materials.