Femtosecond Coherence and Quantum Control of Single Molecules at Room Temperature

Abstract

Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing interest in the possibility of organic quantum computing. Since biological systems are intrinsically heterogeneous, clear relations between structural and quantum-mechanical properties can only be obtained by investigating individual assemblies. However, single-molecule techniques to access ultrafast coherences at physiological conditions were not available so far. Here we show by employing femtosecond pulse-shaping techniques that quantum coherences in single organic molecules can be created, probed, and manipulated at ambient conditions even in highly disordered solid environments. We find broadly distributed coherence decay times for different individual molecules giving direct insight into the structural heterogeneity of the local surroundings. Most importantly, we induce Rabi-oscillations and control the coherent superposition state in a single molecule, thus performing a basic femtosecond single-qubit operation at room temperature.

References in corpus (3)

• Quantum Computing
• Efficient coupling of photons to a single molecule and the observation of its resonance fluorescence
• Coherent State Preparation and Observation of Rabi Oscillations in a Single Molecule

Cited by in corpus (9)

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• Two-Dimensional Electronic Spectroscopy Using Incoherent Light: Theoretical Analysis
• Optical tracing of multiple charges in single-electron devices
• Long-lived oscillatory incoherent electron dynamics in molecules: trans-polyacetylene oligomers
• Plasmon-assisted quantum control of distant emitters
• Generation and quantum control of giant plasmon pulses by transient quantum coherence