The primary consideration in developing new material platforms for quantum applications is to optimize coherence. Despite its importance, decoherence processes remain challenging to experimentally interrogate and quantify. In this Perspective, we first introduce the concept of decoherence in quantum systems and conventional techniques to assess decoherence at optical frequencies. We then introduce multidimensional coherent spectroscopy as a unique probe capable of revealing the full complexity of decoherence dynamics in realistic circumstances. To contextualize the techniques discussed here, demonstrative examples in two prototypical quantum systems, namely colloidal nanocrystals and vacancy centers in diamond, are provided.
The primary consideration in developing new material platforms for quantum applications is to optimize coherence. Despite its importance, decoherence processes remain challenging to experimentally interrogate and quantify. In this Perspective, we first introduce the concept of decoherence in quantum systems and conventional techniques to assess decoherence at optical frequencies. We then introduce multidimensional coherent spectroscopy as a unique probe capable of revealing the full complexity of decoherence dynamics in realistic circumstances. To contextualize the techniques discussed here, demonstrative examples in two prototypical quantum systems, namely colloidal nanocrystals and vacancy centers in diamond, are provided.
Quantum materials displaying intriguing magnetic and electronic properties could be key to the development of future technologies. However, it is poorly understood how the macroscopic behavior emerges in complex materials with strong electronic correlations. While measurements of the dynamics of excited electronic populations have been able to give some insight, they have largely neglected the intricate dynamics of quantum coherence. Here, we apply multidimensional coherent spectroscopy to a prototypical cuprate and report unprecedented coherent dynamics persisting for ~500 fs, originating directly from the quantum superposition of optically excited states separated by 20 to 60 meV. These results reveal that the states in this energy range are correlated with the optically excited states at ~1.5 eV and point to nontrivial interactions between quantum many-body states on the different energy scales. In revealing these dynamics and correlations, we demonstrate that multidimensional coherent spectroscopy can interrogate complex quantum materials in unprecedented ways.
Abstract Optical multidimensional coherent spectroscopy provides information about the structure and excitation dynamics in a broad range of material systems. This book focuses on systems of interest in physics, including atomic vapors, semiconductor nanostructures and two-dimensional materials. An introduction to ultrafast spectroscopy and the fundamental concepts of multidimensional coherent spectroscopy applies to all material systems. Relevant experimental implementations, including phase-stabilized crossed-beams, frequency-tagged fully-collinear, three-dimensional and frequency-comb based methods. The use of the method to study atomic vapors, semiconductor quantum wells, semiconductor quantum dots and two-dimensional materials are described in separate chapters. The final chapters survey the use of the method in some other areas and speculate on future directions.
Quantum entanglement, a hallmark of quantum mechanics, offers unprecedented opportunities to revolutionize spectroscopic techniques. This paper explores the theoretical underpinnings and experimental prospects of quantum entanglement-enhanced spectroscopy for the precise probing of coherent dynamics in complex chemical systems. Traditional spectroscopic methods often face limitations in resolution, sensitivity, and the ability to distinguish subtle quantum phenomena due to their reliance on classical light sources. By harnessing entangled photons, it is possible to overcome these limitations, enabling sub-shot-noise measurements, enhanced spectral resolution beyond the diffraction limit, and access to non-classical correlations within molecular systems. We delve into how entangled light can be generated and engineered to interact with molecular ensembles, facilitating the study of processes such as exciton transport, charge transfer, and vibrational energy redistribution with extraordinary fidelity. The methodology section outlines conceptual experimental setups, including entangled two-photon absorption spectroscopy and quantum Ramsey interferometry, discussing the benefits of these approaches over their classical counterparts. We present hypothetical results demonstrating how entanglement can resolve overlapping spectral features, extend coherence lifetimes, and provide unique insights into the quantum pathways governing chemical reactions. The discussion addresses the challenges associated with maintaining entanglement in noisy chemical environments and outlines strategies for mitigating decoherence. Ultimately, entanglement-enhanced spectroscopy represents a transformative paradigm for chemical physics, promising a deeper understanding of fundamental quantum processes that dictate reactivity and function in biological and material sciences.
Defects in solid-state materials play a central role in determining coherence, stability, and performance in quantum technologies. Although narrowband techniques can probe specific resonances with high precision, a broadband spectroscopic approach captures the full spectrum of defect properties and dynamics. Two-level system (TLS) defects in amorphous dielectrics are a particularly important example because they are major sources of decoherence and energy loss in superconducting quantum devices. However, accessing and characterizing their collective dynamics remains far more challenging than probing individual TLS defects. Building on our previously developed Broadband Cryogenic Transient Dielectric Spectroscopy (BCTDS) technique, we study the coherent control and time-resolved dynamics of TLS defect ensembles over a wide frequency range of 3-5 GHz without requiring full device fabrication, revealing quantum interference effects, memory-dependent dynamics, and dressed-state evolution within the TLS defect bath. The spectral response reveals distinct V-shaped structures corresponding to the bare eigenmode frequencies. Using these features, we extract a TLS defect spectral density of 84 GHz^-1 for a silicon sample, across a 4.1-4.6 GHz span. Furthermore, we systematically investigate amplitude- and phase-controlled interference fringes for multiple temperatures and inter-pulse delays, providing direct evidence of coherent dynamics and control. A driven minimal spin model with dipole-dipole interactions that qualitatively capture the observed behavior is presented. Our results establish BCTDS as a versatile platform for broadband defect spectroscopy, offering new capabilities for diagnosing and mitigating sources of decoherence, engineering many-body dynamics, and exploring non-equilibrium phenomena in disordered quantum systems.
Abstract Multi-dimensional coherent spectroscopy on a variety of materials and systems relevant to physics and materials science is discussed. This chapter provides a summary of results from material systems not already covered in previous chapters of the book. These include semiconductor carbon nanotubes, color centers in diamond, and perovskite materials. The technique elucidates several important features in each of these systems, including the homogeneous linewidths and dephasing processes, population relaxation channels and mechanisms, carrier redistribution dynamics, and coherent phonon interactions.
Multidimensional coherent spectroscopy (MDCS) has been established in quantum chemistry as a powerful tool for studying the nonlinear response and nonequilibrium dynamics of molecular systems. More recently, the technique has also been applied to correlated electron materials, where the interplay of localized and itinerant states makes the interpretation of the spectra more challenging. Here we use the Keldysh contour representation of effective models and nonequilibrium dynamical mean field theory to systematically study the MDCS signals of prototypical correlated lattice systems. By analyzing the current induced by sequences of ultrashort laser pulses we demonstrate the usefulness of MDCS as a diagnostic tool for excitation pathways and coherent processes in correlated solids. We also show that this technique allows to extract detailed information on the nature and evolution of photo-excited nonequilibrium states.