Optical Control of Quantum Phases

Exposing solids to sub-picosecond (ps) electromagnetic pulses with electric field strengths as high as 1 V/Å can cause large transient changes to the electronic and structural degrees of freedom, leading to the modification of the equilibrium electronic phase – enhancing or suppressing electronic orders including superconductivity, orbital order, magnetism, and topological order. The transient state can form completely new electronic phases – “hidden” phases not observed at equilibrium. Light-induced transformations typically impact nano-scale regions, leading to a spatially non-uniform and non-equilibrium state of matter. Therefore, the optical excitation, together with the optical interrogation of transient properties, must be carried out locally. In our group we devised and deployed instrumentation needed to carry out nano-scale and time-resolved pump-probe studies.

Programable hyperbolic polaritons in Van der Waals semiconductors
Sternbach et al. Science, 371, 617 (2021). Article [293]

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In materials hosting both strong anisotropy and strong dipole active resonances non-intuitive optical properties can emerge. Chief among them are sub-diffractional polaritonic wave packets that can travel as conical rays with hyperbolic dispersion throughout the materials’ bulk. In our work, we utilized femtosecond photoexcitation to agitate the vdW semiconductor WSe2 and interrogated these crystals in the transient state. Our time-resolved nano-imaging data reveals key signatures of on-demand hyperbolic exciton-polaritons, appearing on the sub-picosecond timescale. These hyperbolic polaritons travel throughout the bulk of WSe2 with tunable trajectories rooted in the electronic process governing their transient electrodynamics.

Ultrafast optical switching of infrared plasmon polaritons in high-mobility graphene
Ni et al. Nature Photonics 10, 244 (2016) . Article [225]

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pic6Graphene is emerging as one of the most capable candidates for plasmonic media for infrared wavelengths. Here we visualize and elucidate the properties of non-equilibrium photo-induced plasmons in a high-mobility graphene monolayer4.We activate plasmons with femtosecond optical pulses in a specimen of graphene that otherwise lacks infrared plasmonic response at equilibrium. In combination with static nano-imaging results on plasmon propagation, our infrared pump–probe nano-spectroscopy investigation reveals new aspects of carrier relaxation in heterostructures based on high-purity graphene.

Cooperative photoinduced metastable phase control in strained manganite films
(with R.A. Averitt) Zhang et al. Nature Materials 15, 956 (2016) . Article [229]

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picture62A major challenge in quantum materials is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers, enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase, where a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is cooperative and ultrafast, requiring a critical absorbed photon density to activate local charge excitations that mediate magnetic–lattice coupling.

Ultrafast Dynamics of Surface Plasmons in InAs by Time-Resolved IR Nanospectroscopy
Wagner et al. Nano Letters 14, 4529 (2014). Article [196]

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picture63We report on time-resolved mid-infrared (mid-IR) near field spectroscopy of the narrow bandgap semiconductor InAs. The dominant effect we observed pertains to the dynamics of photoexcited carriers and associated surface plasmons. A novel combination of pump− probe techniques and near-field nanospectroscopy accesses high momentum plasmons and demonstrates efficient, subpicosecond photomodulation of the surface plasmon dispersion with subsequent tens of picoseconds decay under ambient conditions. The photoinduced change of the probe intensity due to plasmons in InAs is found to exceed that of other mid-IR or near-IR media by 1− 2 orders of magnitude.