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Physical Review Letters

Single Molecules Driven by Strong Resonant Fields: Hyper-Raman and Subharmonic Resonances

Brahim Lounis, Fedor Jelezko, Michel Orrit

Published May 12, 1997• 51 citations
Publisher

Abstract

We present pump-probe experiments on single molecules in a solid matrix, with strong laser fields and a new host-guest system, dibenzanthanthrene in a naphthalene crystal. Besides strong light-shifts of the lines, we observe the hyper-Raman resonance, for the first time in condensed matter. For strong pump and probe, we also observe subharmonic resonances due to a''kicked pendulum'' motion of the Bloch vector. Since our results agree with Bloch's equations without any adjustable parameter, they provide a stringent test of the optical two-level model as applied to single molecules in solids.

DOI
10.1103/physrevlett.78.3673

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Angewandte Chemie International Edition in English•Apr 1, 1993•192 citations
We present pump-probe experiments on single molecules in a solid matrix, with strong laser fields and a new host-guest system, dibenzanthanthrene in a naphthalene crystal. Besides strong light-shifts of the lines, we observe the hyper-Raman resonance, for the first time in condensed matter. For strong pump and probe, we also observe subharmonic resonances due to a''kicked pendulum'' motion of the Bloch vector. Since our results agree with Bloch's equations without any adjustable parameter, they provide a stringent test of the optical two-level model as applied to single molecules in solids.
We report on a new crystalline host–guest system for single molecule spectroscopy; dibenzanthanthrene (DBATT) in a naphthalene crystal. As compared to DBATT in an n-hexadecane Shpol’skii matrix (a combination studied earlier), this system is shifted to the red (618.7 nm), has a lower triplet yield and shorter triplet lifetimes. Thanks to the narrow lines of this system (20 MHz), to its high photostability and to the absence of spectral diffusion, even in strained crystals, we could measure line shapes and widths with great accuracy. As an illustration of the potential of this new system for quantum optical experiments, we present pump–probe experiments with strong laser fields. The experiments are in very good agreement with calculations based on Bloch’s equations, demonstrating the validity of these equations for single molecules in solids under intense resonant fields.
Single molecules in a crystal at low temperature are driven simultaneously by a laser and by the electric field of an rf. At weak rf power, we observe Rabi transitions within doublets of dressed states, the first such observation in condensed matter in the optical domain. At higher rf power, resonances involving several rf photons appear. The interplay between rf and laser dynamics induces shifts and broadenings that are in excellent agreement with calculations from optical Bloch equations. We also directly display the Rabi and multi-rf-photon resonances by recording the fluorescence signal versus the rf frequency.
Experiments with single quantum systems are at the frontier of modern physics. Probing single molecules allows for very precise control of light-matter interaction and for quantum optical studies. Moreover, a single guest molecule in a solid host matrix is a very sensitive probe of local dynamics in its nano-environment. Fluorescence excitation spectroscopy on single molecules is a powerful tool for spectroscopic characterizations at highest resolution, as information can be revealed that is not accessible in experiments on ensembles of molecules. The detection of the fluorescence signal of a single absorber is achieved by exploiting the high spectral selectivity given by the ratio (10 10) of homogeneous to inhomogeneous linewidths of optical transitions at cryogenic temperatures (zero-phonon transitions). Two-photon fluorescence excitation, a fundamental nonlinear optical process, was observed on a single quantum system [1]. Single diphenyl-octatetraene molecules trapped in an n-tetradecane matrix were excited from the 1Ag ground to the lowest excited singlet state by simultaneous absorption of two photons using a single-mode cw laser. Excited molecules were observed through weak one-photon emission resulting from a symmetry breaking induced by the crystal field. The fundamental principles and the experimental technique of single molecule spectroscopy will be introduced briefly and some particular single molecule experiments presented. This work was done in collaboration with T. Plakhotnik, A. Renn and U.P. Wild
We have measured the ac-Stark effect on single terrylene molecules in ppp-terphenyl crystals at superfluid helium temperatures. With the pump beam far enough from resonance, the molecular transition shifts as expected, i.e., proportional to the pump intensity and to the inverse pump detuning. Experiments closer to resonance with stronger beams show Autler-Townes-like structures that can be well reproduced by means of Bloch equations with two intense laser fields. These experiments are a demonstration of nonlinear optical effects with the localized electronic states of a single molecule trapped in a solid.
Optical spectroscopy of single impurity molecules in low-temperature solids provides an exquisitely sensitive probe of the structure and dynamics of the specific local environment around the single molecule, unobscured by ensemble averaging. Effects such as spectral diffusion, perturbations by external fields, changes in molecular photophysics, optical switching, dynamics due to amorphous system physics, magnetic resonance of a single molecular spin, and perturbations due to nearby charge transport have all been observed. Because properly chosen single molecules act as two- and three-level quantum systems, a variety of quantum optical effects may be observed, such as photon antibunching, optical Stark effect, and single-photon emission on command. When they carry spin in their ground and excited states, single molecules and other nano-objects open many more experiments in quantum optics and nanophysics, because they are sensitive to magnetic interactions and can serve as readouts for spin systems with long coherence times. As a new class of nanoscale experiments, the ability to optically pump and probe single 2–3-nm-sized molecules in complex systems provides a new window into the local dynamics and heterogeneity of solids.
Abstract Optical spectroscopy of a single impurity molecule provides the first truly local probe of host–guest interactions in doped solids. In conventional optical high‐resolution experiments with many molecules only ensemble averages of the microscopic parameters can be obtained. In the single‐molecule regime, the exquisite sensitivity of an individual dopant molecule to both the local environment and to external perturbations has been exploited in recent experiments to reveal a wealth of fascinating novel phenomena such as spectral diffusion in crystals and polymers, optical modification of a single impurity molecule (spectral hole‐burning), local field measurements at the site of a single impurity molecule, and quantum optics in a solid.