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arXiv:2606.22530

Liouvillian Geometry of Multidimensional Spectra: Pathway Transport and Observational Holonomy in Open Quantum Systems

Eric R. Bittner, Carlos Silva-Acuña, Hao Li

quant-phSubmitted Jun 21, 2026• Announced Jun 23, 2026• 0 citations• Revised Aug 21, 2026 (v2)
v1 · Jun 21, 2026v2 · Aug 21, 2026
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Abstract

Liouville pathways provide the conceptual foundation for interpreting multidimensional spectroscopies and are commonly represented as independent contributions to the nonlinear response. In open quantum systems, however, the effective reduced Liouvillian need not preserve this observational pathway decomposition. Environmental interactions can transport amplitude between pathway sectors during the free-evolution intervals, generating measurable signatures in the nonlinear spectroscopic response.} We develop a geometric framework in which pathway transport is governed by a Liouvillian connection, its associated curvature, and the resulting observational holonomy. The framework applies to open quantum systems in which the environment selects a pointer basis distinct from the observational basis used to construct the spectroscopic response. This basis incompatibility induces transport among Liouville pathways, generating characteristic spectral distortions and a nontrivial Liouvillian curvature. Using a Duhamel expansion of the Liouvillian propagator, we derive a reconstruction procedure that identifies the transport operators responsible for the observed redistribution of pathway weight, accurate throughout the full range of basis misalignment. This perspective reframes spectral features as determined not only by which pathways exist but by how amplitude is transported among them. Spectral distortions, peak shifts, and otherwise-forbidden pathway contributions become geometric signatures of a curved Liouville-space manifold rather than phenomenological broadening corrections, identifying pathway geometry as a complementary layer of organization in nonlinear spectroscopy.

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Liouville pathways provide the conceptual foundation for interpreting multidimensional spectroscopies and are commonly represented as independent contributions to the nonlinear response. In open quantum systems, however, the effective reduced Liouvillian need not preserve this observational pathway decomposition. Environmental interactions can transport amplitude between pathway sectors during the free-evolution intervals, generating measurable signatures in the nonlinear spectroscopic response.} We develop a geometric framework in which pathway transport is governed by a Liouvillian connection, its associated curvature, and the resulting observational holonomy. The framework applies to open quantum systems in which the environment selects a pointer basis distinct from the observational basis used to construct the spectroscopic response. This basis incompatibility induces transport among Liouville pathways, generating characteristic spectral distortions and a nontrivial Liouvillian curvature. Using a Duhamel expansion of the Liouvillian propagator, we derive a reconstruction procedure that identifies the transport operators responsible for the observed redistribution of pathway weight, accurate throughout the full range of basis misalignment. This perspective reframes spectral features as determined not only by which pathways exist but by how amplitude is transported among them. Spectral distortions, peak shifts, and otherwise-forbidden pathway contributions become geometric signatures of a curved Liouville-space manifold rather than phenomenological broadening corrections, identifying pathway geometry as a complementary layer of organization in nonlinear spectroscopy.
We introduce the Spectral Autodiff Kernel Expansion (SAKE), a differentiable computational framework for transporting nonlinear spectroscopic response between neighboring quantum dynamical models. Rather than recomputing multidimensional spectra independently for each Hamiltonian or Liouvillian, SAKE constructs local transport expansions about a reference model by combining forward-mode automatic differentiation with Duhamel transport theory. Automatic differentiation generates first-, second-, and third-order derivatives of the parameter-dependent Liouvillian, which are assembled into a pathway transport operator that maps the nonlinear response of a reference model onto neighboring systems. The framework is validated for a four-level excitonic dimer possessing an su(2)×su(2)su(2)\times su(2)su(2)×su(2) symmetry by comparing second- and third-order transported pathway operators with exact projected transport matrices obtained from direct calculations. The third-order expansion accurately reproduces the projected transport operator and its associated pathway mixing. Beyond providing an efficient computational strategy, the transport operator reveals how coherent and dissipative perturbations redistribute amplitude among double-sided Feynman pathways, exposing mechanistic information that is not directly apparent from the nonlinear spectrum. SAKE thereby establishes a differentiable computational framework for nonlinear spectroscopy that supports efficient local parameter exploration, sensitivity analysis, and future inverse-design applications.
Abstract Standard quantum mechanics represents global phase with a single U(1) structure and typically treats phase transport as geometrically trivial unless additional external structure is introduced. In multi-carrier phase algebras, however, closed phase evolution can exhibit intrinsic holonomy, implying a nontrivial internal connection and curvature on the phase fiber. This article isolates the geometric junction at which internal (phase-fiber) curvature becomes operationally accessible as an effective curvature on the base manifold governing spatial transport. The mechanism is formulated in connection-theoretic terms: an internal transport law induces an effective base-level connection acting on multi-component amplitudes, whose curvature controls measurable departures from flat propagation. We highlight three observable channels—loop-dependent phase transport, interferometric shifts, and semiclassical deflections—through which internal holonomy can be tested without assuming a curved metric a priori. The resulting framework provides a compact geometric interpretation of how spatial curvature may emerge as a projection of internal phase holonomy, and it delineates the conditions under which this projection becomes experimentally distinguishable.
Complementarity relations constrain the distribution of coherence, predictability, and openness in quantum systems. Here we show that, in open quantum systems, these local constraints acquire a geometric interpretation through quasistatic transport. For a driven dissipative qubit, the complementarity variables define cylindrical coordinates on the Bloch sphere, while openness appears geometrically as a radial deficit associated with reduction from a larger Hilbert space. Quasistatic driving induces a work connection on the resulting steady-state manifold whose curvature determines the cyclic response. Hamiltonian-aligned dissipation produces an exact work connection and vanishing cyclic work, whereas fixed pointer-basis dissipation generates non-integrable transport, finite curvature, and holonomic response. The resulting curvature admits a phase-resolved representation on the triality manifold and develops perturbatively with pointer--Hamiltonian mismatch. In the weak-mismatch limit, the curvature is governed by a competition between coherence-preserving and pure-dephasing channels, producing symmetry-related positive- and negative-curvature sectors. These results establish a direct connection between complementarity, dissipation, and geometric thermodynamic response, and show that cyclic quasistatic work provides an operational probe of nonequilibrium quantum geometry.
We develop a geometry for transporting stationary-state response across the control space of an open quantum system. A physical model is represented by the ordered pair of its stationary state and dynamical generator. Embedding these pairs in a common ambient space induces a metric, a response one-form, and a closed two-form on the control manifold. The ambient space admits a canonical complex structure that exchanges state and generator directions, but the Liouvillian null-state condition restricts physical models to a submanifold that need not preserve this structure. For an amplitude-damped optical Bloch model, the metric and response two-form are compatible at the single point ω=0ω=0ω=0 and g/Γ=1/2g/Γ=1/\sqrt{2}g/Γ=1/2​; the physical manifold is non-Kähler elsewhere. The induced metric defines the Levi--Civita connection, geodesics, and parallel transport without requiring Kähler compatibility. We compute the connection by automatic differentiation through the stationary Liouvillian solve and recover the symbolic result to machine precision. A two-point calculation then shows that the resulting geodesic differs from linear interpolation in control space and follows a shorter path through the family of state--generator models. This geometry supplies the intrinsic derivative and transport structure needed to carry observable response, including multidimensional spectra, between admissible stationary models.
We develop a response-geometric framework for open quantum systems by decomposing the stationary-state response tensor into symmetric and antisymmetric sectors. The symmetric sector defines a metric-like response tensor governing local susceptibility, while the antisymmetric sector defines a curvature two-form associated with nonreciprocal response and geometric work. We show that the work curvature is precisely the antisymmetric component of the response tensor, establishing a fluctuation--response relation that extends the geometric structure of equilibrium thermodynamics to nonequilibrium steady states, and reveals a response geometry with both metric and symplectic sectors. In equilibrium, the antisymmetric sector vanishes by reciprocity, recovering the familiar metric geometry of thermodynamic response. Open quantum systems admit a broader structure in which reciprocal and nonreciprocal responses coexist on the same control manifold. We illustrate this with a driven dissipative qubit under pure dephasing, where finite curvature emerges from the misalignment between the Hamiltonian eigenbasis and the pointer basis selected by the environment, without requiring strong driving or engineered reservoirs. Comparison with the Bures metric shows that response geometry and information geometry characterize distinct properties of the stationary-state manifold: the former governs susceptibility and geometric work, the latter quantifies state distinguishability. Geometric work thus emerges as a measurable signature of nonreciprocal response in open quantum systems.
Quantum geometry is conventionally understood as a descriptive structure characterizing the space of quantum states. In this work, we examine an alternative but fully compatible interpretation in which geometric quantities—such as Berry curvature and the quantum metric—function effectively as constraint layers shaping the set of admissible dynamical trajectories. Without introducing new degrees of freedom or modifying established theoretical frameworks, we analyze how geometric terms enter semiclassical equations of motion and transport responses in quantum systems. In particular, anomalous velocity contributions and geometry-dependent transport coefficients indicate that geometry operates not merely as a passive descriptor, but as an active structural condition on system evolution. This shift from geometry as description to geometry as constraint does not alter the formalism, but reorganizes its interpretation, reducing conceptual fragmentation by unifying diverse geometry-dependent effects under a common structural principle. It highlights that the evolution of quantum systems is not only governed by dynamical variables, but also by the geometric structure that restricts the space of accessible trajectories. This perspective suggests that transport phenomena may be more fruitfully analyzed through constraint-space formulations rather than purely state-space descriptions. We clarify the scope and limits of this reinterpretation, emphasizing that it introduces no new physical interactions or ontological commitments. Instead, it provides a conceptually sharper and operationally informative framework for understanding the role of geometry in quantum dynamics and transport.