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Physical Review Letters

Pump-Probe Experiments with a Single Molecule: ac-Stark Effect and Nonlinear Optical Response

Philippe Tamarat, Brahim Lounis, J. Bernard, Michel Orrit, S. Kummer, R. Kettner, S. Mais, Th. Basché

Published Aug 21, 1995• 97 citations
Publisher

Abstract

We have measured the ac-Stark effect on single terrylene molecules in $p$-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.

DOI
10.1103/physrevlett.75.1514

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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.
The dynamic Stark effect (Autler-Townes splitting and radiative shift) of a J = 0 ↔ J = 1 optical transition have been investigated. The barium atomic beam is illuminated by a strong pump beam, resonant or slightly non-resonant with the BaI resonance line (λ = 5 535 Å) ; the fluorescence induced by a weak probe beam is detected versus the probe frequency. With linear polarizations for the two beams one deals either with a two-level (parallel polarizations) or with a three-level system (perpendicular polarizations). In the latter case and for small detunings of the pump beam, the Autler-Townes doublet has been observed. For large detunings of the pump beam a single, shifted resonance has been obtained with both polarization settings. In the three-level case the observation of the passage from the Autler-Townes situation to the light-shift situation, is reported. The corresponding calculations are presented; a particular attention is paid to the case of large detunings for the pump beam (light-shift situation). The evolution calculated for the resonance curve (position and relative intensities of the peaks) when the relative polarization directions are changed is consistent with the experimental data.
In recent years, coherent effects in atomic and molecular systems have been studied extensively, especially in several new classes of effects, such as lasing without inversion (LWI), electromagnetically induced transparency (EIT), coherent population trapping (CPT), AC Stark effect and Autler-Townes (AT) splitting in multilevel systems. The AC stark effect and Autler-Townes splitting in molecules have only been investigated recently. We demonstrate AC stark effect and Autler-Townes (AT) splitting in a lithium molecule using cw multi-photon spectroscopy. The excited upper level of the G1PigG^{1}\\Pi_{g}G1Pig​ is prepared by the optical-optical double resonance (OODR) excitation. The OODR line is split in the presence of a third coupling laser, which couples the upper level to an another intermediate level when the coupling laser is on or near resonance transition. The AT line shape consists of the superposition of ∣MJ∣|M_{J}|∣MJ​∣ components which have been resolved for G1Pig(v=12,J=3,f)G^{1}\\Pi_{g}(v=12, J=3,f)G1Pig​(v=12,J=3,f). We find that the AT splittingis linearly proportional to ∣MJ∣|M_{J}|∣MJ​∣, which allows the excitation of molecules with a selected ∣MJ∣|M_{J}|∣MJ​∣ level. The AC Stark shift of the OODR line is observed when the coupling laser is detuned from the resonance transition.
This paper describes an extension of the familiar coherence effects from atomic systems to the molecular regime. Such effects are inherent in the interaction of multiple laser fields with molecular systems. We have observed Autler–Townes splitting and the AC Stark shift in diatomic Lithium using the continuous wave all-optical triple resonance (AOTR) techniques. By using the Autler–Townes effect, we have partially resolved the magnetic sublevels of a molecular rovibrational level in a Doppler broadened sample, allowing all-optical alignment of the angular momentum in excited states of nonpolar molecules. The Autler–Townes effect in a molecular system extends the rovibrational state selectivity of the AOTR excitation technique to magnetic sublevels. PACS Nos.: 33.40tf, 42.50Hz
Fluorescence excitation spectra of single terrylene molecules in p-terphenyl crystals were investigated at low temperatures. The line shifts due to hydrostatic pressure and external electric fields were measured, with the electric field strength oriented either parallel or perpendicular to the k vector of the laser light. A linear Stark effect was found for most molecules, indicating local environments of low symmetry. In sites X1 and X3 (and XY, a photoproduct state), spectral hole burning was observed. Whereas the holes are stable in sites X1 and XY, they decay with a time constant of some minutes in X3. Pressure experiments were performed on the stable hole spectra in sites X1 and XY. In weakly doped samples, holes composed of very few molecular lines were generated with halfwidths distinctly narrower than twice the homogeneous linewidth.
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.
The dynamic Stark effect is investigated in a J=0\ensuremath{\rightarrow}1\ensuremath{\rightarrow}0 three-level ladder system in an atomic beam of natural barium. This system is free of hyperfine structure, which has complicated previous experiments of this type. An intense, actively stabilized cw dye laser was tuned to resonance with the transition between the upper two levels, and a similar, but much less intense, probe laser was scanned through resonance with the transition connecting the lower two levels. Fluorescence arising from transitions out of the middle and upper levels was separately recorded as a function of probe-laser frequency. This allowed us to observe the effects of the strong laser on both the levels which it coupled. The smooth transition from an Autler-Townes doublet to a single light-shifted peak was observed, as well as effects related to coherent population trapping. The resulting profiles were found to be in excellent agreement with theoretical predictions. With a theoretical model extended to incorporate the contributions of the five most abundant isotopes of barium, and other nonideal features of the experiment, it was possible to account for every detail of the observed profiles. Comparing the experimental results with theory also yielded a measurement for the absorption f value for the 6s6p 1{\mathrm{}}^{1}1P1{P}_{1}P1​\ensuremath{\rightarrow}6p2{p}^{2}p2 3P0^{3}P_{0}3P0​ (608.3 nm) transition in 138Ba^{138}\mathrm{Ba}138Ba.