TBA

TBA

The role of quantum mechanical coherences or coherent superposition states in excited state processes has received considerable attention in the last two decades owing much to advances in ultrafast laser spectroscopy. The existence of coherence effects shows promise for enhancing the efficiency and robustness of functionally relevant processes, even when confronted with strong energy disorder and environmental fluctuations. Therefore, an in-depth understanding of coherence propels us to push the frontier to the grand challenge of using optical control of coherence to improve functions or create new ones in molecular and material systems. In this frontier, the role of electronic and vibrational interplay, or more specifically the role of vibrations in directing electronic dynamics, has emerged as the leading principle, where two energetically disparate quantum degrees of freedom work in-sync to dictate the trajectory of an excited state reaction. Moreover, with the vibrational degree being directly related to the structural composition of molecular or material systems, new molecular designs could be inspired by tailoring certain structural elements.

In this talk, I envision acquainting the quantum world of molecules to physicists. I will summarize essential aspects concerning the interplay of electronic and vibrational dynamics afforded from state-of-the-art ultrafast laser spectroscopy in three exemplary processes: photo-induced electron transfer, singlet-triplet intersystem crossing, and intramolecular vibrational energy-driven energy flow in molecular systems. More precisely, I will showcase crucial experimental signatures that offer deeper insights into the complex electronic-vibrational trajectories encompassing excited states. I will discuss rapid decoherence—loss of phase and amplitude correlations—of vibrational coherences along promoter vibrations in comparison to spectator coherences in a near-ballistic (~30-femtosecond time constant) electron transfer reaction in the Marcus-inverted region and during a sub-picosecond intersystem crossing dynamics in a series of binuclear platinum complexes. The rapid decoherence depicts the vibration-driven reactive pathways from Franck-Condon state to the curve crossing region. I will also discuss the generation of new vibrational coherences induced by impulsive reaction dynamics—not by the laser pulse—in these systems which informs on specific energy dissipation pathways and thereby on the progression of the reaction trajectory in the vicinity of the curve crossing on the product side. While the decoherence or impulsive generation of vibrational wavepackets has emerged as a prominent indicator of the interplay of electronic dynamics and vibrations, the other property of vibrational coherences, amplitude, also relays how energy can flow from one vibration to another vibration in the electronic excited state. 

From these studies, we learn that superposition states along vibrations that are part of the complex reactive trajectories are extremely sensitive to electronic dynamics. Thus, vibrational superposition states act as quantum mechanical windows for visualizing the interplay of electronic and vibrational dynamics. This frontier could change the outlook on how vibrations might soon become a control element in the hands of a chemist, influencing the outcome of a reaction.

The role of quantum mechanical coherences or coherent superposition states in excited state processes has received considerable attention in the last two decades owing much to advances in ultrafast laser spectroscopy. The existence of coherence effects shows promise for enhancing the efficiency and robustness of functionally relevant processes, even when confronted with strong energy disorder and environmental fluctuations. Therefore, an in-depth understanding of coherence propels us to push the frontier to the grand challenge of using optical control of coherence to improve functions or create new ones in molecular and material systems. In this frontier, the role of electronic and vibrational interplay, or more specifically the role of vibrations in directing electronic dynamics, has emerged as the leading principle, where two energetically disparate quantum degrees of freedom work in-sync to dictate the trajectory of an excited state reaction. Moreover, with the vibrational degree being directly related to the structural composition of molecular or material systems, new molecular designs could be inspired by tailoring certain structural elements.

In this talk, I envision acquainting the quantum world of molecules to physicists. I will summarize essential aspects concerning the interplay of electronic and vibrational dynamics afforded from state-of-the-art ultrafast laser spectroscopy in three exemplary processes: photo-induced electron transfer, singlet-triplet intersystem crossing, and intramolecular vibrational energy-driven energy flow in molecular systems. More precisely, I will showcase crucial experimental signatures that offer deeper insights into the complex electronic-vibrational trajectories encompassing excited states. I will discuss rapid decoherence—loss of phase and amplitude correlations—of vibrational coherences along promoter vibrations in comparison to spectator coherences in a near-ballistic (~30-femtosecond time constant) electron transfer reaction in the Marcus-inverted region and during a sub-picosecond intersystem crossing dynamics in a series of binuclear platinum complexes. The rapid decoherence depicts the vibration-driven reactive pathways from Franck-Condon state to the curve crossing region. I will also discuss the generation of new vibrational coherences induced by impulsive reaction dynamics—not by the laser pulse—in these systems which informs on specific energy dissipation pathways and thereby on the progression of the reaction trajectory in the vicinity of the curve crossing on the product side. While the decoherence or impulsive generation of vibrational wavepackets has emerged as a prominent indicator of the interplay of electronic dynamics and vibrations, the other property of vibrational coherences, amplitude, also relays how energy can flow from one vibration to another vibration in the electronic excited state. 

From these studies, we learn that superposition states along vibrations that are part of the complex reactive trajectories are extremely sensitive to electronic dynamics. Thus, vibrational superposition states act as quantum mechanical windows for visualizing the interplay of electronic and vibrational dynamics. This frontier could change the outlook on how vibrations might soon become a control element in the hands of a chemist, influencing the outcome of a reaction.

R-Type Ferrites (RTF) constitute a large isostructural class of transition element oxides featuring quasi-two-dimensional Kagome sublattices.  We review a decade of experiments covering a large range of compositional variations, ATM₅O₁₁ (A= alkali earth, T= 3d element, M= Ru and 3d elements).  The physical properties of RTF are remarkably sensitive to atomic disorder, and crucial roles for spin-orbit interactions and magnetic frustration are indicated.  The availability of single-crystal samples has revealed a startling panorama of RTF ground states and exotic physical properties:  

Disordered iron-bearing RTF are narrow-gap semiconductors with colinear ferrimagnetic order well above 300 K with T_C proportional to the semiconducting gap, and properties suitable for spin injection applications.  In contrast, disordered Co- and Mn-bearing RTF exhibit canted, “all-in/all-out” ordering substantially below 300 K in the frustrated Kagome sublattice.  Atomically ordered RTF (T= Ni, Zn, M= Ru) do not order to below 4 K, and display spin fluctuations and unusual non-Fermi-liquid behavior.  Many RTF compositions display large anomalous topological Hall effects that involve Berry phase effects in the magnetization textures.  

In spite of the wide variations of ground states and physical properties, the lattice parameters of RTF vary by as little as 0.1%, which suggests fabrication of epitaxial RTF heterostructures with unique physical properties may be feasible for a range of applications.

*Research supported by U.S. DoE Grant #DE-FG02-97ER45653 and the Kentucky Science and Engineering Foundation.  
 

R-Type Ferrites (RTF) constitute a large isostructural class of transition element oxides featuring quasi-two-dimensional Kagome sublattices.  We review a decade of experiments covering a large range of compositional variations, ATM₅O₁₁ (A= alkali earth, T= 3d element, M= Ru and 3d elements).  The physical properties of RTF are remarkably sensitive to atomic disorder, and crucial roles for spin-orbit interactions and magnetic frustration are indicated.  The availability of single-crystal samples has revealed a startling panorama of RTF ground states and exotic physical properties:  

Disordered iron-bearing RTF are narrow-gap semiconductors with colinear ferrimagnetic order well above 300 K with T_C proportional to the semiconducting gap, and properties suitable for spin injection applications.  In contrast, disordered Co- and Mn-bearing RTF exhibit canted, “all-in/all-out” ordering substantially below 300 K in the frustrated Kagome sublattice.  Atomically ordered RTF (T= Ni, Zn, M= Ru) do not order to below 4 K, and display spin fluctuations and unusual non-Fermi-liquid behavior.  Many RTF compositions display large anomalous topological Hall effects that involve Berry phase effects in the magnetization textures.  

In spite of the wide variations of ground states and physical properties, the lattice parameters of RTF vary by as little as 0.1%, which suggests fabrication of epitaxial RTF heterostructures with unique physical properties may be feasible for a range of applications.

*Research supported by U.S. DoE Grant #DE-FG02-97ER45653 and the Kentucky Science and Engineering Foundation.  
 

Two-dimensional (2D) van der Waals (vdW) materials are thin layers of crystals that are held together by the weak vdW forces. The recent discovery of long-range magnetic order in 2D vdW materials has triggered a renaissance in the study of 2D magnetism for both fundamental science and technological advances. In this talk, I will present our recent work on chromium

chalcogenides, a family of 2D self-intercalated vdW magnets which possess a broad spectrum of intriguing magnetic properties, including high temperature ferromagnetism, topological spin textures, and giant anomalous Hall conductivity. I will discuss the bottom-up synthesis of these 2D magnets, the correlation between their structural phases and emergent magnetism, as well as the new opportunities that they may offer and the challenges that need to be overcome for

spintronic applications.

Two-dimensional (2D) van der Waals (vdW) materials are thin layers of crystals that are held together by the weak vdW forces. The recent discovery of long-range magnetic order in 2D vdW materials has triggered a renaissance in the study of 2D magnetism for both fundamental science and technological advances. In this talk, I will present our recent work on chromium

chalcogenides, a family of 2D self-intercalated vdW magnets which possess a broad spectrum of intriguing magnetic properties, including high temperature ferromagnetism, topological spin textures, and giant anomalous Hall conductivity. I will discuss the bottom-up synthesis of these 2D magnets, the correlation between their structural phases and emergent magnetism, as well as the new opportunities that they may offer and the challenges that need to be overcome for

spintronic applications.

Chern insulator ferromagnets are a fascinating area of research in condensed matter physics. These materials exhibit a quantized anomalous Hall effect, which has been observed experimentally in various systems including magnetically-doped topological insulator (MTI) thin films and bilayer graphene moiré superlattices. Chern insulator ferromagnets are classified into two categories, spin or orbital, based on the origin of their orbital magnetization. In the case of spin Chern insulator (e.g. MTIs), the orbital magnetization arises from spontaneous spin-polarization combined with spin-orbit interactions. In contrast, orbital Chern insulators (e.g. graphene-based moiré superlattices) exhibit spontaneous orbital currents that give rise to the orbital magnetization. Understanding the differences between these two types of Chern insulators is crucial for developing new materials with interesting properties. In this talk, I will emphasise the curious magnetic properties of orbital Chern insulator using magic-angle twisted bilayer graphene as an example.

Chern insulator ferromagnets are a fascinating area of research in condensed matter physics. These materials exhibit a quantized anomalous Hall effect, which has been observed experimentally in various systems including magnetically-doped topological insulator (MTI) thin films and bilayer graphene moiré superlattices. Chern insulator ferromagnets are classified into two categories, spin or orbital, based on the origin of their orbital magnetization. In the case of spin Chern insulator (e.g. MTIs), the orbital magnetization arises from spontaneous spin-polarization combined with spin-orbit interactions. In contrast, orbital Chern insulators (e.g. graphene-based moiré superlattices) exhibit spontaneous orbital currents that give rise to the orbital magnetization. Understanding the differences between these two types of Chern insulators is crucial for developing new materials with interesting properties. In this talk, I will emphasise the curious magnetic properties of orbital Chern insulator using magic-angle twisted bilayer graphene as an example.