arXiv:1403.4644 · Physical Review Letters

Coherent Amplification of Ultrafast Molecular Dynamics in an Optical Oscillator

Igal Aharonovich, Avi Pe’er

Published Feb 18, 2016• 2 citations

Abstract

Optical oscillators present a powerful optimization mechanism. The inherent competition for the gain resources between possible modes of oscillation entails the prevalence of the most efficient single mode. We harness this "ultrafast" coherent feedback to optimize an optical field in time, and show that, when an optical oscillator based on a molecular gain medium is synchronously pumped by ultrashort pulses, a temporally coherent multimode field can develop that optimally dumps a general, dynamically evolving vibrational wave packet, into a single vibrational target state. Measuring the emitted field opens a new window to visualization and control of fast molecular dynamics. The realization of such a coherent oscillator with hot alkali dimers appears within experimental reach.

DOI: 10.1103/physrevlett.116.073603

Related papers

Visualizing fast molecular dynamics by coherent feedback in an optical oscillator

Avi Pe’er, Igal Aharonobich

We exploit the inherent mode competition in a laser resonator to solve in real time the major coherent control problem — how to shape a pulse that will dump a general wave-packet in to a single target state.

Jan 1, 20150 citations

A Coherent Raman Oscillator Pumped by a Frequency Comb

Igal Aharonovich, Avi Pe

Free induction decay is the coherent emission of light that follows the excitation of a medium by a short pulse. During the coherence time of the medium (T2), all atoms/molecules oscillate ’in unison’, forming a macroscopic dipole that emits light as a large coherent antenna, ’broadcasting’ information on the quantum state of the atoms/molecules and its dynamical evolution. We present an optical oscillator, where the coherent dipole emission from a dynamical wave-packet, is amplified beyond the lasing threshold. By placing a molecular medium in an optical cavity that is synchronously pumped by a frequency comb laser, emission from the excitation of one pump pulse can return to the medium with subsequent pump pulses, allowing stimulated amplification. When threshold is crossed, a broadband coherent oscillation is achieved, bearing information on the coherent wave-packet dynamics inside the medium. We analyze theoretically this coherent Raman oscillator and simulate thoroughly it’s dynamics under most realistic conditions for a model system of Alkali dimers (Li2,K2) in a hot gas cell (100−300 ◦ C), showing that the oscillation condition is well within reach. If realized, this coherent Raman oscillator can open avenues for precise measurement of vibrational dynamics in molecules.

Mar 18, 20140 citations

Nanoscale Coherent Control. Ultrafast dynamics of single molecules, individual light harvesting complexes and discrete nanoantennas at room temperature.

Daan Brinks

Ultrafast pulses allow observation of molecular dynamics with femtosecond time resolution through pump probe experiments. However, averaging over an ensemble of molecules tends to wash out phase sensitive information, necessary to probe quantum effects, due to the intrinsic inhomogeneity in molecular conformations, orientations and interactions that lead to unique potential energy landscapes for each molecule. It is therefore important to go beyond the ensemble average when looking at quantum dynamics of organic systems at room temperature, and resolve the behaviour of specific molecules on an individual basis. In this thesis, we show the creation, manipulation and observation of ultrafast coherent effects in single molecules at room temperature, and resolve a certain measure of environmental influence on the specific dynamics of each molecule. Moreover, we apply this insight to investigate a functional light harvesting biosystem, and lay the basis for a technique that has the time and space resolution required to observe these systems in vivo. In chapter 1, we introduce the concepts and techniques the research in this thesis is built on. In chapter 2, we treat the possibility of controlling ultrafast pulses at the high-NA diffraction limit, and come to conclusions about the procedure to follow there that hold for all pulse-shaping experiments. We show in proof of principle experiments that we can control the ultrafast characteristics of optical pulses in nanometric excitation volumes. In chapters 3 and 4 we report the creation, detection and control of ultrafast quantum dynamics in single organic molecules at room temperature. We show that manipulation of superposition states is possible in these systems within a coherence dephasing time of ~50 fs. This leads to the first observation of rabi-oscillations in room temperature single molecules, to ultrafast operation of an organic qubit, and to the creation of non-stationary superposition states (vibrational wavepackets). We probe the influence of the local environment on the composition and dynamics of these wavepackets and show we can optimize the state preparation protocol for each individual molecule in its own nanoenvironment, leading to high fidelity coherent control. In these chapters we lay out the proof of principle work of detecting the quantumdynamics of a complex system in interaction with its environment at room temperature. In chapter 5 we discuss application of these techniques to the investigation of long lived coherence in photosynthetic systems. We show that electronic coherence between different rings of the LH2 system persists to time scales of 100s of femtoseconds at room temperature. Moreover we show that the energy transfer pathways in LH2 adapt to environmentally induced changes in the molecule and that the nature of the transfer remains coherent for each pathway, providing strong evidence that coherent energy transfer is the optimum process for energy transfer in photosynthesis. Finally, in chapter 6 we take the technical development one step further and report on the creation of a framework based on plasmonic antennas that allows for control of the amplitude-phase characteristics in nanometric sized hotspot fields. We show for the first time that the ultrafast characteristics of plasmonic hotspots can directly be engineered through design of the plasmonic system and experimentally demonstrate two much-anticipated examples: a sub-diffraction resolution phase shaper and an ultrafast plasmonic switch for pump probe experiments. The results presented in this thesis form the first creation and observation of ultrafast coherent dynamics in individual molecular systems at room temperature. This is a necessary step to be able to do true quantum tomography in complex systems, resolve the influence of the environment on molecular dynamics, and investigate the physics that determines evolutionary optimization and functionality in biomolecules.

Oct 19, 20120 citations

Coherent amplification without inversion of femtosecond optical pulses

John N. Sweetser, Thomas J. Dunn, Ian A. Walmsley

Recent progress has been made in the theoretical and experimental study of the amplification of optical signals without population inversion (AWI) of the participating electronic levels. Induced coherence among appropriate levels in the active medium is the necessary condition for obtaining AWI. Similarly, the generation of wave packet states in atoms and molecules also relies on the coherent superposition of several states. It is feasible, therefore, that AWI is possible in a system which has been excited into a wave packet state. We have thus demonstrated experimentally such amplification in an extended sample of sodium dimers and we term this process wave packet amplification (WPA). An important characteristic of WPA is that the gain is doubly phase-sensitive—it is modulated at both the wave packet oscillation period and the optical period. The former time-dependence is a result of the periodic revivals of the pump-induced electronic polarization and the latter optical phase-sensitivity is a manifestation of the coherent nature of the molecular wave packet. The experiments to be described use a time-resolved upconversion method to detect the change in energy of a 50 fs probe pulse after it passes through a sodium heat pipe that has been pumped with another 50 fs pulse. The maximum saturated energy gain in this system is four and corresponds to all of the available energy being transferred from the wave packet to the probe pulse.

Annual Meeting Optical Society of AmericaJan 1, 19930 citations

Demonstrating coherent control in R85b2 using ultrafast laser pulses: A theoretical outline of two experiments

Hugo E. L. Martay, David J. McCabe, Duncan G. England +3 more

Calculations relating to two experiments that demonstrate coherent control of preformed rubidium-85 molecules in a magneto-optical trap using ultrafast laser pulses are presented. The two experiments are a step toward the stabilization of ultracold rubidium dimers using ultrafast lasers. In the first experiment, it is shown that preassociated molecules in an incoherent mixture of states can be made to oscillate coherently using a single ultrafast pulse. A mechanism that can transfer molecular population to more deeply bound vibrational levels is used in the second. Optimal parameters of the control pulse are presented for the application of the mechanism to molecules in a magneto-optical trap. The calculations make use of an experimental determination of the initial state of molecules photoassociated by the trapping lasers in the magneto-optical trap and use shaped pulses consistent with a standard ultrafast laser system. The experiment's purpose is to demonstrate and evaluate the use of ultrafast shaped pulses to manipulate ultracold rubidium dimers with a view to the eventual stabilization of the molecules.

arXiv:0904.0225Physical Review ASep 3, 200910 citations

Coherent control of electronic and vibrational wave packets using phase-locked optical pulses

Elizabeth Durrell Boleat

Experimental and theoretical work is presented on the control of wave packet dynamics in atomic and molecular systems. Using sequences of phase-locked optical pulses, the link between optical phase and quantum mechanical phase is explored in the Na atom and Naj dimer, representing a step towards the logical engineering of quantum states in more complicated systems. A novel apparatus, constructed to study and control the vibrational dynamics of vibrational wave packets on the Na ionic potential surface, is described in chapter 3. Theoretical simulations for proposed experiment are presented in chapter 4. Control is achieved by exploiting the phase-evolution of the constituent vibrational quantum states within the wave packet superposition. The phase relationship and the accumulated phase difference between the various components of the wave packet is determined, and a sequence of phase-locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi-pulse response of the time-dependent vibrational state populations. In chapter 5, the quantum interference between Rydberg electron wave packets in the Na atom is investigated using pairs of phase-locked wave packets, allowing manipulation of the total orbital angular momentum of Na Rydberg atoms. Initially the wave packet is composed of a superposition of s and d Rydberg series. Exploitation of the difference between the quantum defects of the two series allows specific angular momentum compositions within the resultant wave packet to be engineered. Experimentally, this final quantum state distribution is analysed in the frequency domain using state selective field ionisation, and in the time domain using the optical Ramsey method. The theoretical calculations show how the phase difference between pairs of optical pulses is linked to the corresponding Rydberg frequency spectrum, therefore enabling the control of the quantum state composition of the wave packets.

Jan 1, 20050 citations