Coherent control is based on optical manipulation of the amplitudes and phases of wave functions. It is expected to be a key technique to develop novel quantum technologies such as bond-selective chemistry and quantum computing, and to better understand the quantum worldview founded on wave-particle duality. We have developed high-precision coherent control by imprinting optical amplitudes and phases of ultrashort laser pulses on the quantum amplitudes and phases of molecular wave functions. The history and perspective of coherent control and our recent achievements are described.
Coherent control is based on optical manipulation of the amplitudes and phases of wave functions. It is expected to be a key technique to develop novel quantum technologies such as bond-selective chemistry and quantum computing, and to better understand the quantum worldview founded on wave-particle duality. We have developed high-precision coherent control by imprinting optical amplitudes and phases of ultrashort laser pulses on the quantum amplitudes and phases of molecular wave functions. The history and perspective of coherent control and our recent achievements are described.
Coherent control is a technique to manipulate the amplitudes and phases of wave functions by exploiting the coherent property of light. It is of great importance for the development of quantum technologies including quantum information processing and chemical reaction control as well as for addressing fundamental problems in quantum mechanics such as the quantum–classical boundary. In this chapter, we describe the development and applications of coherent control based on wave-packet interferometry with attosecond precision, which has been made possible by tuning the delay between two laser pulses on the attosecond time scale. This technique has been applied to several different hierarchies from simple to complex quantum systems: (i) isolated iodine molecules in the gas phase, (ii) molecular crystals of para-hydrogen, and (iii) single crystals of bismuth. In system (i), we have controlled and visualized the interference of vibrational wave packets in the isolated iodine molecules, and that wave-packet interference has been utilized to develop a molecular computer, which executes ultrafast Fourier transform. In system (ii), we have manipulated vibrational wave-functions delocalized in a para-hydrogen crystal. The long coherence lifetime of para-hydrogen crystals is a promising resource to preserve quantum information in bulk solids. In system (iii), we have controlled the excitation ratio of two orthogonal coherent phonon modes, whose coherent superposition has allowed for active control of ultrafast two-dimensional atomic motions in a single crystal of bismuth. Those atomic motions have been visualized by density functional theory calculations. Finally, the coherent control of an ensemble of ultracold Rydberg atoms is briefly discussed as future perspectives for exploring the quantum–classical boundary.
Whenever scientific tools are significantly advanced; new discoveries soon follow. My thesis work relies on advances in ultrafast laser technology that allow precise control over the shape of sub 20-fs laser pulses. This laser system enabled many new experiments that yielded significant advances in attosecond science, atomic physics; extreme nonlinear optics, quantum chemistry, coherent control, molecular physics, ultrafast optical phase modulation, EUV coherent imagines, and EUV radiation sources. By using an automated learning control algorithm coupled to our deformable mirror pulse shaper; we have demonstrated the control of a process on an attosecond time-scale for the first time. We demonstrate the manipulation of the phase of an electron wave packet, allowing us to tailor the EUV spectrum generated by high-order harmonic generation. These optimal fields were discovered by a learning algorithm that both found an unknown optimal solution; but also discovered an unknown phase-matching mechanism that occurs in the interaction of a single atom and light pulse. We control molecular vibrational and rotational coherences with the same learning algorithm; demonstrating selective control in room temperature molecules at atmospheric pressures. Moreover, we demonstrate that modifications to the algorithm can help automatically uncover the physics of the control mechanism found by the learning algorithm. We also demonstrate a new pulse-compression technique using rotational phase modulation, where optical pulses were compressed by an order of magnitude after phase modulation by a molecular rotational coherence and subsequent propagation through a transparent window. This technique will enable efficient pulse compression in the deep-UV. Finally, we measure the coherence of EUV light generated by high-harmonic upconversion of a femtosecond laser. In phase-matched hollow-fiber geometry, the EUV light exhibits the highest inherent spatial coherence of any source in this region of the spectrum. We use this source to demonstrate the coherent image with first table-top EUV radiation. Since this source exhibits full spatial coherence at very short wavelength, this light source represents has smallest inherent effective source-size of any light source yet created. We also demonstrate that the spectrum of an optical field can be determined by measuring the interference of a double-slit pattern.
Generating field-free (non-stationary) orientation of molecules in space has been a longstanding goal in the field of quantum control of molecular rotation, which has significant applications in physical chemistry, chemical physics, strong-field physics, and quantum information science. In this Perspective, we review and examine several representative control schemes developed in recent years and implemented in theoretical and experimental areas for generating field-free orientation of molecules. By conducting numerical simulations of different control schemes on the same molecular system, we demonstrate that quantum coherent control, specifically targeting a limited number of the lowest-lying rotational levels to achieve an optimal superposition, can result in a high degree of orientation. To this end, we provide an overview of our latest developed analytical method, which enables the precise design of terahertz field parameters through resonant excitation. This design approach facilitates the attainment of desired field-free orientations by optimizing the amplitudes and phases of rotational wave functions for the selected rotational levels. Finally, we outlook the significance of such progress in multiple frontier research fields, highlighting its potential applications in ultracold physics, quantum computation, quantum simulation, and quantum metrology.
Summary form only given. The developments with coherent control (CC) techniques in optical spectroscopy have recently demonstrated population control and coherence manipulations when the induced optical phase is explored with phase-locked laser pulses. These and other developments have been guiding the new research field of quantum control including the recent applications to semiconductors and nanostructures. We study the influence of inhomogeneous broadening in semiconductors on CC results. Photoluminescence (PL) and the coherent emission in four-wave mixing (FWM) is recorded after resonant excitation with phase-locked laser pulses. The sample is a narrow GaAs single quantum well.
T hink about coherent systems, and odds are that the first example to cross your mind will be a laser: a device that emits monochromatic light homogenized so that the photons propagate with their phase in lockstep. The well-defined wavefront of the laser beam makes it possible to focus the light to spot sizes on the order of the wavelength of the light without the aberrations usually observed with the random wavefront of incoherent light. The well-defined phase also provides a medium capable of storing and carrying information more efficiently than the intensity-modulated signals typical of incoherent sources. These useful properties of coherence have made lasers almost ubiquitous in science and technology, and that “almost” is shrinking by the day.
In general, coherence comes about when individual components of a system act in unison, either in phase or with a fixed phase difference between the components. More accurately, the system can be described as a local oscillator whose wavefunction contains phase and amplitude terms that define how the system evolves in space and time. The collection of articles in this special issue describes the recent progress and developments of coherence in optical, atomic, and semiconductor systems, and how manipulating that coherence may lead to useful applications and to experimental systems for studying the elements of quantum mechanics.
Since the first demonstration of the laser in 1960, progress in improving the extent of the spatial and temporal coherence of laser light has been steady. Psaltis (p. [1359][1]) reviews developments in optical coherence and highlights examples of the key role coherence has played in applications in imaging, communication, and information processing and storage. Just as lasers revolutionized the field of optics, many researchers have high expectations that other coherent systems will provide similar advances in their respective fields. Exploiting the fundamental tenet of quantum mechanics whereby particles have the properties of waves, Kasevich (p. [1363][2]) reviews coherence effects in collections of cold atoms and describes how the shorter wavelengths associated with atoms and the recent accessibility of bright coherent atom sources may lead to precision measurements beyond anything currently available to the optical regime. For integration and potential applications, the ideal system would be based in semiconductors. Snoke (p. [1368][3]) describes recent work toward the formation of coherent semiconductor systems.
With coherence in the atomic and optical systems generally comprising macroscopic systems, Mabuchi and Doherty (p. [1372][4]) look at coherence effects at the quantum limit, probing the interactions between single atoms and single photons confined to high-quality cavities. In addition to providing invaluable information on the limits of quantum mechanics, such effects might also shed new light on information science in the quantum regime.
The section opens with a pair of News features by staff writers Charles Seife and Robert Service. Seife presents a smattering of common applications that scientists and engineers have found for coherent waves, whether in light, sound, or subatomic particles. Service describes efforts to create new coherent sources of the type of radiation known as “hard” x-rays—a long-sought range of high frequencies with enormous potential for scientific research, technology, and medicine.
[1]: /lookup/doi/10.1126/science.1078823
[2]: /lookup/doi/10.1126/science.1079430
[3]: /lookup/doi/10.1126/science.1078082
[4]: /lookup/doi/10.1126/science.1078446