Controlling the Future of Matter

Kohler, Bern; Krause, Jeffrey L.; Ráksi, F.; Wilson, Kent R.; Yakovlev, Vladislav V.; Whitnell, Robert M.; Yan, YiJing

doi:10.1021/ar00051a006

Cited by 164 publications

(80 citation statements)

References 47 publications

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“…[11][12][13][14][15] A number of methods based on formal control theory, first introduced by Rabitz and co-workers, [16][17][18] have been presented to determine the coherent temporal-spectral shape of light field that best drives a quantum system to a desired target. [19][20][21][22][23][24][25][26][27][28] Experimental demonstrations of the optimal control scheme have been carried out for manipulating the excited state wave packet focusing dynamics and photodissociation product. [29][30][31] Recently, Yan and co-workers [32][33][34][35][36] have further developed the theory of optimal control via a pair of phase-unlocked coherent fields.…”

Section: Introductionmentioning

confidence: 99%

Pump-dump control and the related transient absorption spectroscopies

Shen

Yan

Cheng

et al. 1999

The Journal of Chemical Physics

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We combine theories of optimal pump-dump control and the related transient probe absorption spectroscopy in order to elucidate the relation between these two optical processes and the possibility of experimental realization. In the weak response regime, we identify the globally optimal pair of pump-dump control fields, and further propose a second-order difference detection scheme to monitor the wave packets dynamics that is jointly controlled by both the pump and dump fields. The globally optimal solution serves also as the initial input for the iterative search for the optimal control fields in the strong response regime. We use a model I 2 molecule to demonstrate numerically the pump-dump control and the detection of a highly vibrationally excited wave packet focusing dynamics on the ground X surface in both the weak and strong response regimes. The I 2 B surface serves as the intermediate to assist the pump-dump control and the optical detection processes. Demonstrated in the strong response regime are the optimal pair of pump-dump molecular-pulses that invert nearly total population onto the predefined target region within a half period of vibration motion.

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Section: Introductionmentioning

confidence: 99%

Pump-dump control and the related transient absorption spectroscopies

Shen

Yan

Cheng

et al. 1999

The Journal of Chemical Physics

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“…Particularly in correlated electronic systems, where the phase state is determined by the interactions between charges, orbitals, spins, and the crystal lattice, 1 these optically driven lattice distortions lead to colossal rearrangements in the electronic and magnetic properties, opening up many opportunities for applications in ultrafast data processing and storage. Especially attractive is the ability to switch the functionality of these solids at high speeds, while minimizing heating and dissipation.These advances are related to previous work aimed at driving chemical reactions by the coherent control of specific molecular vibrations, 2,3 in what is often referred to as "bond selective chemistry". However, bond selective chemistry has been often severely limited by the large atomic motions needed to break or make chemical bonds.…”

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confidence: 92%

Mode-Selective Control of the Crystal Lattice

2015

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CONSPECTUS: Driving phase changes by selective optical excitation of specific vibrational modes in molecular and condensed phase systems has long been a grand goal for laser science. However, phase control has to date primarily been achieved by using coherent light fields generated by femtosecond pulsed lasers at near-infrared or visible wavelengths. This field is now being advanced by progress in generating intense femtosecond pulses in the mid-infrared, which can be tuned into resonance with infrared-active crystal lattice modes of a solid. Selective vibrational excitation is particularly interesting in complex oxides with strong electronic correlations, where even subtle modulations of the crystallographic structure can lead to colossal changes of the electronic and magnetic properties. In this Account, we summarize recent efforts to control the collective phase state in solids through mode-selective lattice excitation. The key aspect of the underlying physics is the nonlinear coupling of the resonantly driven phonon to other (Raman-active) modes due to lattice anharmonicities, theoretically discussed as ionic Raman scattering in the 1970s. Such nonlinear phononic excitation leads to rectification of a directly excited infrared-active mode and to a net displacement of the crystal along the coordinate of all anharmonically coupled modes. We present the theoretical basis and the experimental demonstration of this phenomenon, using femtosecond optical spectroscopy and ultrafast X-ray diffraction at a free electron laser. The observed nonlinear lattice dynamics is shown to drive electronic and magnetic phase transitions in many complex oxides, including insulator−metal transitions, charge/orbital order melting and magnetic switching in manganites. Furthermore, we show that the selective vibrational excitation can drive high-T C cuprates into a transient structure with enhanced superconductivity. The combination of nonlinear phononics with ultrafast crystallography at X-ray free electron lasers may provide new design rules for the development of materials that exhibit these exotic behaviors also at equilibrium. ■ INTRODUCTIONCoherent optical excitation of infrared-active lattice vibrations in solids is emerging as a new tool to control the crystal structure of solids directly and to drive phase transitions dynamically. Particularly in correlated electronic systems, where the phase state is determined by the interactions between charges, orbitals, spins, and the crystal lattice, 1 these optically driven lattice distortions lead to colossal rearrangements in the electronic and magnetic properties, opening up many opportunities for applications in ultrafast data processing and storage. Especially attractive is the ability to switch the functionality of these solids at high speeds, while minimizing heating and dissipation.These advances are related to previous work aimed at driving chemical reactions by the coherent control of specific molecular vibrations, 2,3 in what is often referred to as "bond selective chemistry...

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“…Advancement in generating tailored light pulses has made it possible to steer matter towards a specific goal, namely, to control its future [1][2][3][4][5][6][7].…”

Section: Introductionmentioning

confidence: 99%

Coherent optimal control of multiphoton molecular excitation

Dey¹

2001

J. Phys. B: At. Mol. Opt. Phys.

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We give a framework for molecular multiphoton excitation process induced by an optimally designed electric field. The molecule is initially prepared in a coherent superposition state of two of its eigenfunctions. The relative phase of the two superposed eigenfunctions has been shown to control the optimally designed electric field which triggers the multiphoton excitation in the molecule. This brings forth flexibility in designing the optimal field in the laboratory by suitably tuning the molecular phase and hence by choosing the most favorable interfering routes that the system follows to reach the target.We follow the quantum fluid dynamical formulation for designing the electric field with application to HBr molecule.

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Controlling the Future of Matter

Cited by 164 publications

References 47 publications

Pump-dump control and the related transient absorption spectroscopies

Pump-dump control and the related transient absorption spectroscopies

Mode-Selective Control of the Crystal Lattice

Coherent optimal control of multiphoton molecular excitation

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