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Hot electron processes at metallic heterojunctions are central to optical-to-chemical or electrical energy transduction. Ultrafast nonlinear photoexcitation of graphite (Gr) has been shown to create hot thermalized electrons at temperatures corresponding to the solar photosphere in less than 25 fs. Plasmonic resonances in metallic nanoparticles are also known to efficiently generate hot electrons. Here we deposit Ag nanoclusters (NC) on Gr to study the ultrafast hot electron generation and dynamics in their plasmonic heterojunctions by means of time-resolved two-photon photoemission (2PP) spectroscopy. By tuning the wavelength of p-polarized femtosecond excitation pulses, we find an enhancement of 2PP yields by 2 orders of magnitude, which we attribute to excitation of a surface-normal Mie plasmon mode of Ag/Gr heterojunctions at 3.6 eV. The 2PP spectra include contributions from (i) coherent two-photon absorption of an occupied interface state (IFS) 0.2 eV below the Fermi level, which electronic structure calculations assign to chemisorption-induced charge transfer, and (ii) hot electrons in the π*-band of Gr, which are excited through the coherent screening response of the substrate. Ultrafast pump–probe measurements show that the IFS photoemission occurs via virtual intermediate states, whereas the characteristic lifetimes attribute the hot electrons to population of the π*-band of Gr via the plasmon dephasing. Our study directly probes the mechanisms for enhanced hot electron generation and decay in a model plasmonic heterojunction.

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Experimental methods for ultrafast microscopy are advancing rapidly. Promising methods combine ultrafast laser excitation with electron-based imaging or rely on super-resolution optical techniques to enable probing of matter on the nano–femto scale. Among several actively developed methods, ultrafast time-resolved photoemission electron microscopy provides several advantages, among which the foremost are that time resolution is limited only by the laser source and it is immediately capable of probing of coherent phenomena in solid-state materials and surfaces. Here we present recent progress in interference imaging of plasmonic phenomena in metal nanostructures enabled by combining a broadly tunable femtosecond laser excitation source with a low-energy electron microscope.

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Strontium titanate is a bulk insulator that becomes superconducting at remarkably low carrier densities. Even more enigmatic properties become apparent at the strontium titanate/lanthanum aluminate (STO/LAO) interface and it is important to disentangle the effects of reduced dimensionality from the poorly-understood pairing mechanism. Recent experiments measuring the surface photoemission spectrum[1] and bulk tunneling spectrum[1] have found a cross-over, as a function of carrier density, from a polaronic regime with substantial spectral weight associated with strongly coupled phonons, to a more conventional weakly coupled Fermi liquid. Interestingly, it is only the polaronic state that becomes superconducting at low temperatures, although the properties of the superconducting phase itself appear entirely conventional. We interpret these results in a simple analytical model that extends an Engelsberg-Schrieffer theory of electrons coupled to a single longitudinal optic phonon mode to include the response of the electron liquid, and in particular phonon-plasmon hybridization. We perform a Migdal-Eliashberg calculation within our model to obtain this material's unusual superconducting phase diagram.

[1] Z. Wang et al, Nat. Mater. (2016)
[2] A.G. Swartz et al, arXiv:1608.05621

In this talk, I am going to present some of the work that I have done during my PhD. In the first part I will mostly focus on building a low-temperature Andreev reflection spectroscopy probe (which is basically a simpler version of an STM). In the second part, I will briefly talk about the observation of a new phase of matter, tip-induced superconductivity (TISC), that emerges only under mesoscopic metallic point contacts on topologically non-trivial semimetals like a 3-D Dirac semimetal Cd3As2, and a Weyl semimetal, TaAs and comment on the possible mechanism that might lead to the emergence of such a surprising phase of matter. All these experiments were done using our home-built low-temperature probe.
If time permits, I will also talk about some experiments that we did using various scanning probe based microscopic techniques, e.g., piezo-response force microscopy (PFM) and ferroelectric lithography. I will show how certain “artifacts” can limit the application of PFM in the investigation of ferroelectric materials, and how, under certain circumstances, such “artifacts” can actually turn out to be useful.

[1] L. Aggarwal, A. Gaurav, G. S. Thakur, Z. Haque, A. K. Ganguli & G. Sheet, Unconventional Superconductivity at Mesoscopic Point-contacts on the 3-Dimensional Dirac Semi-metal Cd3As2.” Nature Materials 15, 32 (2016).
[2] L. Aggarwal, S. Gayen, S. Das, R. Kumar, V. Sϋß, C. Shekhar, C. Felser & G. Sheet, “Mesoscopic superconductivity and high spin-polarization coexisting at metallic point contacts on Weyl semimetal TaAs.” Nature Communications, 8, 13974 (2017).
[3] J. S. Sekhon, L. Aggarwal & G. Sheet, “Voltage induced local hysteretic phase switching in silicon.” Applied Physics Letters 104, 162908 (2014). 

The two-dimensional diffusive metal stabilized at the interface of SrTiO3 and the Mott Insulator perovskite LaTiO3[1-2] has challenged many notions related to the formation and electronic behavior of the two-dimensional electron gas (2DEG) at the well studies LaAlO3-SrTiO3 interface. Here we discuss specifically the stability of the superconducting phase[3] at LaTiO3 – SrTiO3 interface, the nature of the superconductor – normal metal quantum phase transition (T=0 limit) driven by magnetic field, significance of the field vis-à-vis the Chandrasekhar - Clogston limit for depairing, and how the transition is initiated when the extent of Coulomb interaction amongst charge carriers is modulated by electrostatic gating[4]. The nature of the superconducting condensate is highlighted in the light of the Ti - t2g orbital driven bands and their filling in the presence of a strong Rashba spin – orbit interaction (SOI). Towards the end of the talk, we will discuss the prominent effects of Rashba SOI on normal state quantum transport and how it renormalizes a Kondo-like electronic behavior in range of temperature Tc< T < 5K[5-7]. The prominence of the Ti 3d0 and Ti 3d1 correlated electron physics in these systems will be demonstrated further from our recent studies of 2DEG in ion irradiated SrTiO3 crystals[8,9].
1. Advanced Materials 22, 4448(2010). 2. Phys. Rev. B 86, 075127(2012).
3. Nature Communications, 1, 89(2010). 4. Nature Materials 12, 542(2013).
5. Phys. Rev. B (Rapid Communication) 90, 081107(2014). 6. Phys. Rev. B 90, 075133(2014). 7. Phys. Rev. B 94, 115165 (2016).
8. Phys. Rev. B 91, 205117(2015). 9. Phys. Rev. B 92, 235115 (2015).