arXiv subjects

Lucas Borges

Publications and source records attributed to Lucas Borges.

7 recordsLinked to original sources

arXiv2025

Selective excitation of molecular vibrations via a two-mode cavity Raman scheme

The experimental realization of strong light-matter coupling with molecules initiated the rapidly evolving field of molecular polaritonics. Most studies focus on how exciton polaritons, which combine electronic excitations with confined light modes, alter photochemistry. In this paper, we investigate their use in selectively exciting molecular vibrational states in the ground state. Selectively exciting molecules to high vibrational states with infrared lasers to catalyze ground-state chemical reactions is a challenging task. Here, we propose a two-cavity mode setup in the electronic strong coupling regime inspired by the process of Stimulated Raman Adiabatic Passage (STIRAP) to selectively populate excited vibrational states. One cavity mode actively pumps the molecular system, while the other provides a highly effective and tunable decay channel via photon leakage. We demonstrate the ability to selectively populate vibrational states for coherent and incoherent light sources using a molecular model system. Our initial findings show high efficiency and suggest a possible route to steering and controlling chemical reactions in the electronic ground state based on electronic strong coupling.

physics.chem-ph↗

arXiv2025

A competitive NISQ and qubit-efficient solver for the LABS problem

Pauli Correlation Encoding (PCE) is as a qubit-efficient variational approach to combinatorial optimization problems. The method offers a polynomial reduction in qubit count and a super-polynomial suppression of barren plateaus. Here, we extend the PCE-based framework to solve the Low Autocorrelation Binary Sequences (LABS) problem, a notoriously hard problem often used as a benchmark for classical and quantum solvers. To illustrate this,we simulate two variants of the PCE quantum solver for LABS instances of up to $N=45$ binary variables: one with commuting and one with maximally non-commuting sets of Pauli operators. The simulations use $4$ qubits and a circuit Ansatz with a total of $30$ two-qubit gates. We benchmark our method against the state-of-the-art classical solver and other quantum schemes. We observe improved scaling in the total time to reach the exact solution, outperforming the best-performing classical heuristic while using only a fraction of the quantum resources required by other quantum approaches. In addition, we perform proof-of-principle demonstrations on IonQ's Forte quantum processor, showing that the final solution is resilient to noise. Our findings point at PCE-based solvers as a promising quantum-inspired classical heuristic for hard problems as well as a tool to reduce the resource requirements for actual quantum algorithms.

quant-ph↗

arXiv2025

The role of dark polariton states for electronic strong coupling in molecules

Polaritonic chemistry investigates the possible modification of chemical and photochemical reactions by means of strong light-matter coupling in optical cavities, as demonstrated in numerous experiments over the last few years. These experiments are typically interpreted in terms of the Jaynes-Cummings or Tavis-Cummings models under the assumption that the molecular ensemble is only excited by a single photon. In such a model, two polariton states compete with an overwhelming number of dark states, inhibiting polaritonic reactions entropically. We analyze the higher excitation manifolds of the Tavis-Cummings model along with a three-level system that resembles photochemical reactions. We demonstrate that allowing for more than a single excitation makes the reaction of the involved polaritons entropically more favorable.

quant-ph↗

arXiv2024

Partition function estimation with a quantum coin toss

Estimating quantum partition functions is a critical task in a variety of fields. However, the problem is classically intractable in general due to the exponential scaling of the Hamiltonian dimension $N$ in the number of particles. This paper introduces a quantum algorithm for estimating the partition function $Z_\beta$ of a generic Hamiltonian $H$ up to multiplicative error based on a quantum coin toss. The coin is defined by the probability of applying the quantum imaginary-time evolution propagator $f_\beta[H]=e^{-\beta H/{2}}$ at inverse temperature $\beta$ to the maximally mixed state, realized by a block-encoding of $f_\beta[H]$ into a unitary quantum circuit followed by a post-selection measurement. Our algorithm does not use costly subroutines such as quantum phase estimation or amplitude amplification; and the binary nature of the coin allows us to invoke tools from Bernoulli-process analysis to prove a runtime scaling as $\mathcal{O}(N/{Z_\beta})$, quadratically better than previous general-purpose algorithms using similar quantum resources. Moreover, since the coin is defined by a single observable, the method lends itself well to quantum error mitigation. We test this in practice with a proof-of-concept 9-qubit experiment, where we successfully mitigate errors through a simple noise-extrapolation procedure. Our findings offer an interesting alternative for quantum partition function estimation relevant to early-fault quantum hardware.

quant-ph↗

arXiv2024

Extending the Tavis-Cummings model for molecular ensembles -- Exploring the effects of dipole self energies and static dipole moments

Strong coupling of organic molecules to the vacuum field of a nanoscale cavity can be used to modify their chemical and physical properties. We extend the Tavis-Cummings model for molecular ensembles and show that the often neglected interaction terms arising from the static dipole moment and the dipole self-energy are essential for a correct description of the light-matter interaction in polaritonic chemistry. On the basis of a full quantum description, we simulate the excited-state dynamics and spectroscopy of MgH$^+$ molecules resonantly coupled to an optical cavity. We show that the inclusion of static dipole moments and the dipole self-energy is necessary to obtain a consistent model. We construct an efficient two-level system approach that reproduces the main features of the real molecular system and may be used to simulate larger molecular ensembles.

physics.chem-ph↗

arXiv2024

Towards large-scale quantum optimization solvers with few qubits

We introduce a variational quantum solver for combinatorial optimizations over $m=\mathcal{O}(n^k)$ binary variables using only $n$ qubits, with tunable $k>1$. The number of parameters and circuit depth display mild linear and sublinear scalings in $m$, respectively. Moreover, we analytically prove that the specific qubit-efficient encoding brings in a super-polynomial mitigation of barren plateaus as a built-in feature. This leads to unprecedented quantum-solver performances. For $m=7000$, numerical simulations produce solutions competitive in quality with state-of-the-art classical solvers. In turn, for $m=2000$, an experiment with $n=17$ trapped-ion qubits featured MaxCut approximation ratios estimated to be beyond the hardness threshold $0.941$. To our knowledge, this is the highest quality attained experimentally on such sizes. Our findings offer a novel heuristics for quantum-inspired solvers as well as a promising route towards solving commercially-relevant problems on near term quantum devices.

quant-ph↗

arXiv2022

Fourier-based quantum signal processing

Implementing general functions of operators is a powerful tool in quantum computation. It can be used as the basis for a variety of quantum algorithms including matrix inversion, real and imaginary-time evolution, and matrix powers. Quantum signal processing is the state of the art for this aim, assuming that the operator to be transformed is given as a block of a unitary matrix acting on an enlarged Hilbert space. Here we present an algorithm for Hermitian-operator function design from an oracle given by the unitary evolution with respect to that operator at a fixed time. Our algorithm implements a Fourier approximation of the target function based on the iteration of a basic sequence of single-qubit gates, for which we prove the expressibility. In addition, we present an efficient classical algorithm for calculating its parameters from the Fourier series coefficients. Our algorithm uses only one qubit ancilla regardless the degree of the approximating series. This contrasts with previous proposals, which required an ancillary register of size growing with the expansion degree. Our methods are compatible with Trotterised Hamiltonian simulations schemes and hybrid digital-analog approaches.

quant-ph↗