Ultrafast Coherent Control of Condensed Matter with Attosecond Precision

Coherent control is a technique to manipulate wave functions of matter with light. Coherent control of isolated atoms and molecules in the gas phase is well-understood and developed since the 1990s, whereas its application to condensed matter is more difficult because its coherence lifetime is shorter. We have recently applied this technique to condensed matter samples, one of which is solid para-hydrogen ( p-H₂). Intramolecular vibrational excitation of solid p-H₂ gives an excited vibrational wave function called a "vibron", which is delocalized over many hydrogen molecules in a manner similar to a Frenkel exciton. It has a long coherence lifetime, so we have chosen solid p-H₂ as our first target in the condensed phase. We shine a time-delayed pair of femtosecond laser pulses on p-H₂ to generate vibrons. Their interference results in modulation of the amplitude of their superposition. Scanning the interpulse delay on the attosecond time scale gives a high interferometric contrast, which demonstrates the possibility of using solid p-H₂ as a carrier of information encoded in the vibrons. In the second example, we have controlled the terahertz collective phonon motion, called a "coherent phonon", of a single crystal of bismuth. We employ an intensity-modulated laser pulse, whose temporal envelope is modulated with terahertz frequency by overlap of two positively chirped laser pulses with their adjustable time delay. This modulated laser pulse is shined on the bismuth crystal to excite its two orthogonal phonon modes. Their relative amplitudes are controlled by tuning the delay between the two chirped pulses on the attosecond time scale. Two-dimensional atomic motion in the crystal is thus controlled arbitrarily. The method is based on the simple, robust, and universal concept that in any physical system, two-dimensional particle motion is decomposed into two orthogonal one-dimensional motions, and thus, it is applicable to a variety of condensed matter systems. In the third example, the double-pulse interferometry used for solid p-H₂ has been applied to many-body electronic wave functions of an ensemble of ultracold rubidium Rydberg atoms, hereafter called a "strongly correlated ultracold Rydberg gas". This has allowed the observation and control of many-body electron dynamics of more than 40 Rydberg atoms interacting with each other. This new combination of ultrafast coherent control and ultracold atoms offers a versatile platform to precisely observe and manipulate nonequilibrium dynamics of quantum many-body systems on the ultrashort time scale. These three examples are digested in this Account.