Spectroscopic measurements in quantum systems are subject to selection rules, usually based on space-time symmetries, that allow or disallow transitions between states. In many-body systems, in addition to the single-particle states, there emerge new ones due to collective excitations of the system. Here we demonstrate the existence of a ``fragile'' selection rule that emerges as a manifestation of many-body effects and outlines the conditions for collective excitations to couple to a given spectroscopic probe beyond the usual symmetry considerations. As an example, we apply the rule to Raman spectroscopy of multiband superconductors and settle some unresolved features in experiments, one of them being the spectral weight distribution between the pair-breaking excitations and the collective modes.
Superconducting qubits acting as artificial two-level atoms allow for controlled variation of the symmetry properties which govern the selection rules for single and multiphoton excitation. We spectroscopically analyze a superconducting qubit-resonator system in the strong coupling regime under one- and two-photon driving. Our results provide clear experimental evidence for the controlled transition from an operating point governed by dipolar selection rules to a regime where one- and two-photon excitations of the artificial atom coexist. We find that the vacuum coupling between qubit and resonator can be straightforwardly extracted from the two-photon spectra where the detuned two-photon drive does not populate the relevant resonator mode significantly.
Creation and manipulation of non-classical states of light is rapidly becoming the focus of modern attosecond science. Here, we demonstrate numerically how interaction with such states can trigger the emergence of a many-body system with spontaneously broken symmetry by considering a modification of the well-known problem of superradiance encountered already by Dicke. Similarly to him, we investigate photon emission by ensembles of indistinguishable atoms. In contrast to him, however, we leverage symmetry-based selection rules to suppress emission of single photons by single atoms. A steady state is therefore only reached following a spontaneous transition into a collective symmetry-broken state of atoms and photonic modes. This transition permanently locks the atomic dipoles to the quantum field experienced by the system at a particular instant, transforming the entire setup into a potent quantum sensor reproducing the phase of the recorded quantum fluctuation.
A single quantum of excitation of a mechanical oscillator is a textbook example of the principles of quantum physics. Mechanical oscillators, despite their pervasive presence in nature and modern technology, do not generically exist in an excited Fock state. In the past few years, careful isolation of GHz-frequency nano-scale oscillators has allowed experimenters to prepare such states at milli-Kelvin temperatures. These developments illustrate the tension between the basic predictions of quantum mechanics that should apply to all mechanical oscillators existing even at ambient conditions, and the complex experiments in extreme conditions required to observe those predictions. We resolve the tension by creating a single Fock state of a vibration mode of a crystal at room temperature using a technique that can be applied to any Raman-active system. After exciting a bulk diamond with a femtosecond laser pulse and detecting a Stokes-shifted photon, the 40~THz Raman-active internal vibrational mode is prepared in the Fock state
∣1> with
98.5% probability. The vibrational state is read out by a subsequent pulse, which when subjected to a Hanbury-Brown-Twiss intensity correlation measurement reveals the sub-Poisson number statistics of the vibrational mode. By controlling the delay between the two pulses we are able to witness the decay of the vibrational Fock state over its
3.9 ps lifetime at room temperature. Our technique is agnostic to specific selection rules, and should thus be applicable to any Raman-active medium, opening a new generic approach to the experimental study of quantum effects related to vibrational degrees of freedom in molecules and solid-state systems.
Multidimensional spectroscopy has become an established tool for disentangling microscopic processes that remain unresolved in conventional linear spectroscopy. Its extension to the terahertz regime now enables analogous questions to be addressed for low-energy collective excitations in quantum materials and synthetic many-body systems. Unlike isolated few-level systems, however, these collective modes generally cannot be described within the standard framework of nonlinear spectroscopy based on a few-level description. Their response is instead governed by their extended nature, interplay of interactions, fluctuations, disorder, dissipation, and coupling to additional degrees of freedom. This thesis develops a theoretical framework for computing and interpreting multidimensional nonlinear spectroscopy in quantum many-body systems. Using real-time nonequilibrium field theory, we formulate nonlinear susceptibilities diagrammatically in terms of propagators, interaction vertices, and self-energies, with particular emphasis on the third-order susceptibility relevant to infrared-active collective excitations. This approach places the established concepts and capabilities of multidimensional spectroscopy within a systematic many-body field-theoretical framework. Furthermore, this formulation makes it possible to move beyond the established probing capabilities, extending multidimensional spectroscopy beyond few-level descriptions and revealing new signatures and functionalities specific to interacting many-body systems. At the same time, it provides a controlled framework for constructing approximations that preserve the underlying symmetries and conservation laws of the system while remaining amenable to both analytical and numerical calculations. By incorporating quantum and thermal fluctuations within the random-phase approximation, we demonstrate that two-dimensional spectra can reveal the growth of fluctuations, identify field-theoretical bound states, and characterize their coupling to many-body continua. We further develop a diagrammatic description of rephasing in extended bosonic systems in the presence of static disorder. We identify the disorder vertex corrections responsible for echo formation and show how echo spectroscopy separates disorder-induced broadening from intrinsic relaxation. This framework is extended to coupled modes and strongly interacting regimes, where interactions can either enhance or suppress rephasing. A further result is the identification of a nonrephasing four-wave-mixing signal that is critically enhanced near a phase transition, in contrast to simpler nonlinear protocols like third-harmonic generation. We apply this framework to electromagnons in NiI
2, Josephson plasmons in La
2−xSr
xCuO
4, and the low-energy collective excitations in coupled one-dimensional Bose-Einstein condensates. Across these systems, we show how multidimensional spectroscopy can disentangle disorder from intrinsic relaxation, reveal the effects of interactions and fluctuations, identify coupling between collective modes and continua, and extract microscopic information that remains obscured in conventional spectroscopy. Taken together, the results of this thesis provide a diagrammatic framework for calculating and interpreting multidimensional nonlinear spectroscopic signals in many-body systems, while establishing this technique as a selective probe of collective dynamics across a broad range of quantum materials and synthetic platforms.
Understanding the emergence of collective organizational phenomena is a major goal in many fields of physics from condensed matter to cosmology. Using a recently introduced manybody perturbation formalism for fermions, we propose a mechanism for the emergence of collective behavior, specifically superfluidity, driven by quantum statistics and the enforcement of the Pauli principle through the selection of normal modes. The method, which is called symmetry invariant perturbation theory (SPT), uses group theory and graphical techniques to solve the manybody Schrodinger equation through first order exactly. The solution at first order defines collective coordinates in terms of five N-body normal modes, identified as breathing, center of mass, single particle angular excitation, single particle radial excitation and phonon. A correspondence is established "on paper" that enforces the Pauli principle through the assignment of specific normal mode quantum numbers. Applied in the unitary regime, this normal mode assignment yields occupation only in an extremely low frequency N-body phonon mode at ultralow temperatures. A single particle radial excitation mode at a much higher frequency creates a gap that stabilizes the superfluidity at low temperatures. Coupled with the corresponding values for the frequencies at unitarity obtained by this manybody calculation, we obtain good agreement with experimental thermodynamic results including the lambda transition in the specific heat. Our results suggest that the emergence of collective behavior in macroscopic systems is driven by the Pauli principle and its selection of the correct collective coordinates in the form of N-body normal modes.
The efficient probing of spectral features is important for characterising and understanding the structure and dynamics of quantum materials. In this work, we establish a framework for probing the excitation spectrum of quantum many-body systems with quantum simulators. Our approach effectively realises a spectral detector by processing the dynamics of observables with time intervals drawn from a defined probability distribution, which only requires native time evolution governed by the Hamiltonian without ancilla. The critical element of our method is the engineered emergence of frequency resonance such that the excitation spectrum can be probed. We show that the time complexity for transition energy estimation has a logarithmic dependence on simulation accuracy and how such observation can be guaranteed in certain many-body systems. We discuss the noise robustness of our spectroscopic method and show that the total running time maintains polynomial dependence on accuracy in the presence of device noise. We further numerically test the error dependence and the scalability of our method for lattice models. We present simulation results for the spectral features of typical quantum systems, either gapped or gapless, including quantum spins, fermions and bosons. We demonstrate how excitation spectra of spin-lattice models can be probed experimentally with IBM quantum devices.