arXiv subjects

Liang Z. Tan

Publications and source records attributed to Liang Z. Tan.

At least 19 recordsLinked to original sources

arXiv2026

Room-temperature quantum-sensing molecular crystals grown in minutes

Quantum sensing increasingly demands materials combining room-temperature optical spin addressability and coherent control with rapid, accessible fabrication. Yet semiconductor platforms require costly materials and specialized processing, while molecular systems often depend on bespoke synthesis or involved crystal growth. Here we apply microspacing in-air sublimation (MAS) to rapidly fabricate quantum-sensing materials within minutes. Microgram quantities of commercially available precursors crystallize on glass, in air and without vacuum or inert-gas handling. Monitored in situ, growth yields optically clear, stoichiometric single crystals of excellent quality, including plates and needles with intrinsic optical waveguiding. Donor-acceptor charge-transfer co-crystals pairing anthracene or biphenyl with tetracyanobenzene, together with localized-exciton pentacene:pentacenequinone (P:PQ), exhibit room-temperature optically detected magnetic resonance (ODMR). Charge-transfer ODMR resonances reach linewidths below $4\mathrm{MHz}$, consistent with motional narrowing of mobile triplet excitons, while P:PQ supports coherent ensemble spin control with $T_2=0.56μ\mathrm{s}$. Functionality across chemically and electronically distinct pairs establishes MAS as an accessible screen for molecular quantum-sensing materials, connecting molecular crystal engineering with low-cost, chemically tunable thin triplet-spin layers and waveguiding sensor geometries for quantum sensing and microscopy.

quant-ph↗

arXiv2026

Dense pentacene cocrystal demonstrates room-temperature coherent control

Maximizing the number of addressable spins within a fixed volume can improve ensemble quantum sensor sensitivity, but dense packing usually increases dipolar interactions and excited-state transport, shortening coherence and suppressing optical readout. Here we report a 2:1 cocrystal of 6,13-dihydropentacene and pentacene (DHP/Pc) containing 33.3 mol% pentacene ($3.3\times10^{5}$ ppm; $9.51\times10^{20}$ cm$^{-3}$), a volumetric spin-site density more than two orders of magnitude above previous benchmarks, NV-diamond and pentacene-doped p-terphenyl (PDP). Despite this density, DHP/Pc exhibits microsecond spin coherence, room-temperature optically detected magnetic resonance and coherent control. Time-resolved measurements indicate that the long-lived triplet population is generated predominantly by intersystem crossing and exhibits strong, non-thermal sublevel polarization. Density-functional theory calculations further suggest that the native cocrystal geometry weakens electronic coupling between neighboring pentacenes, while the higher DHP triplet energy creates a barrier to triplet migration. These results identify molecular packing and coformer triplet energetics as complementary design parameters for preserving coherence in high spin-site density systems, demonstrating cocrystallization as a promising route to dense, optically addressable spin materials for room-temperature ensemble quantum sensing.

quant-ph↗

arXiv2026

Vortex-enhanced photovoltaic current in disordered topological materials

In disordered topological materials, real-space crystalline defects interplay with momentum-space wave function singularities to \textit{enhance} the bulk photovoltaic current. What's singular is the interband Berry phase, or equivalently the phase of the \textit{optical} dipole matrix element, which has a \textit{vortex} structure in momentum space. Such \textit{optical vorticity} is guaranteed to exist in all topological materials associated with nontrivial Chern numbers. These vortices enhance electron-impurity skew scattering, which manifests as a ballistic photovoltaic current that is sensitive to (a) the topological material class, (b) the symmetry class of crystalline defects, and (c) the light polarization. This sensitivity manifests in two ways: firstly, by (a-c)-dependent frequency exponents for the photovoltaic current $\propto ω^{\text{exponent}}$ in topological semimetals, with $ω$ the frequency of the light source. Secondly, by (a-c)-dependent constraints of the bulk photovoltaic tensor, which are explainable only by emergent, \textit{magnetic} symmetries of \textit{time-reversal-invariant} topological materials. These ideas are concretized by case studies on multifold fermions, 3D $m$-order Weyl semimetals and 2D $n$-order Dirac systems, which include $n$-layer rhombohedral graphene, transition metal dichalcogenides, and topological surface states. Theoretical guidance is provided for a tri-pronged experimental program that combines frequency-tuned photoconductivity measurements, defect characterization and defect engineering.

cond-mat.str-el↗

arXiv2026

Radiative electronic bound states in the continuum from defects in semiconductors

Continuum-buried defect states in semiconductors are generally expected to be optically inactive due to their strong coupling to continuum bands. Here, we show that such defects can instead host radiative electronic bound states in the continuum (BICs), using the silicon G-center as a prototypical example. Hybrid-functional first-principles calculations with a Hubbard $U$ correction reveal that a localized defect state, initially buried below the valence band maximum (VBM) in the ground state, undergoes exchange-driven energy-level reordering under optical excitation and shifts above the VBM. This exchange-induced transition suppresses nonradiative decay and enables robust radiative emission. By computing temperature-dependent nonradiative lifetimes and comparing them with experimental photoluminescence (PL) lifetimes, we quantitatively reproduce the observed temperature dependence of the emission. These results uncover a stabilization mechanism for continuum-embedded defect states and establish electronic BICs as a general paradigm for designing defect-based optical systems, including quantum emitters and qubits.

cond-mat.mtrl-sci↗

arXiv2026

Non-magnetic insulating phase induced by Jahn-Teller effect in RNiO$_3$

We propose a three-dimensional multi-orbital tight-binding model for rare-earth nickelates RNiO$_3$ that treats charge, spin, orbital, and lattice degrees of freedom on equal footing. All model parameters, including the on-site interactions $U$ and $J$ and the electron-phonon (el-ph) coupling to the breathing mode, are extracted from hybrid-functional DFT calculations for the small-bandwidth nickelate LuNiO$_3$. The model describes three competing insulating phases governed by the interplay of $U{-}3J$ and el-ph coupling to the breathing and Jahn--Teller (JT) modes. For large $U{-}3J$, the insulating state is stabilized by local JT distortions on high-spin Ni$^{3+}$ sites. For smaller $U{-}3J$, the system undergoes charge disproportionation, $2\mathrm{Ni}^{3+}\rightarrow\mathrm{Ni}^{2+}+\mathrm{Ni}^{4+}$, resulting in the spin-polarized charge-ordered state observed experimentally below the Néel temperature in small-bandwidth RNiO$_3$. When the JT energy on the Ni$^{2+}$ site exceeds Hund's exchange $3J$, a distinct charge- and orbital-ordered insulating phase emerges in which the two $e_g$-electrons occupy the same orbital with opposite spin. The stability of this phase is further confirmed by self-consistent calculations within the full three-dimensional tight-binding model. This newly predicted metastable state, characterized by JT distortions in a nonmagnetic charge-ordered RNiO$_3$ phase, shows that the onset of magnetic order is not required for the metal-insulator transition in RNiO$_3$.

cond-mat.str-el↗

arXiv2026

Dynamics of ballistic photocurrents driven by Coulomb scattering

First principles real-time time dependent density functional theory (rt-TDDFT) calculations reveal the existence of ballistic photocurrents generated by Coulomb scattering, which has not previously been considered as a mechanism for the bulk photovoltaic effect. With monolayer GeS as an example, it is predicted that ballistic currents can be comparable to shift currents under experimentally accessible conditions.

cond-mat.mes-hall↗

arXiv2026

Strong-field Driven Sub-cycle Band Structure Modulation and Dephasing Control

Over the past decade, ultrafast electron dynamics in the solid state have been extensively studied using various strong light-matter interaction techniques, such as high-harmonic generation. These studies lead to multiple interpretations of light-matter interaction in the strong-field regime, with exact mechanisms not yet fully understood. It is well known that strong-field interaction with a crystalline solid leads to significant modification of its band structure and, hence, its optical properties on ultrafast timescales. In this work, we present measurements of ultrafast electric-field observables in magnesium oxide using a non-resonant nonlinear optical interaction. Using field observables, we show that strong laser fields modulate the band structure on sub-cycle timescales, thereby altering the material's nonlinear optical response. We perform time-dependent perturbation theory calculations using a field-dependent dispersion relation and non-perturbative semiconductor Bloch equation calculations, both of which agree with experimental observations. Furthermore, we directly extract dephasing times from the real-time signal electric field envelope and show sub-cycle control of dephasing times. Our work offers a new perspective on strong-field-driven electron dynamics in solids through electric-field observables. The demonstrated attosecond modulation of the nonlinear response could have important implications for quantum light generation and quantum spectroscopy using nonlinear optical processes.

physics.optics↗

arXiv2026

Optical control of spin-splitting in an altermagnet

Manipulating and controlling the band structure and the spin-splitting in the newly discovered class of magnetic materials known as 'altermagnets' is highly desirable for their application in spintronics. Based on real-time simulations for an interacting multiband tight-binding model, we propose optical excitations as an effective way to selectively control the spin-splitting of an altermagnet. The consistent treatment of electronic interactions and electron-phonon coupling in the model allows for a systematic study of the effect of these interactions on the spin-splitting of the altermagnet in the ground as well as in the excited-state. Our simulations reveal that optical excitations modify the band structure and thus lead to significant changes in the spin-splitting within 50 fs. The relative spin-splitting in the conduction band grows up to four times in the optically excited altermagnet. We disentangle the roles of Coulomb $U$ and $J$ in the enhancement of the spin-splitting in the photoexcited state. Our study elucidates the potential for exploiting optical control of spin-splitting gaps to obtain desirable properties in altermagnets on the fastest possible timescales.

cond-mat.str-el↗

arXiv2025

Terahertz field-induced giant symmetry modulations in a van der Waals antiferromagnet

Strong-field terahertz (THz) excitations enable dynamic control over electronic, lattice and symmetry degrees of freedom in quantum materials. Here, we uncover pronounced terahertz-induced symmetry modulations and coherent phonon dynamics in the van der Waals antiferromagnet MnPS3, in which inversion symmetry is broken by its antiferromagnetic spin configuration. Time-resolved second harmonic generation measurements reveal long-lived giant oscillations in the antiferromagnetic phase, with amplitudes comparable to the equilibrium signal, driven by phonons involving percent-level atomic displacements relative to the equilibrium bond lengths. The temporal evolution of the rotational anisotropy patterns indicate a dynamic breaking of mirror symmetry, modulated by two vibrational modes at 1.7 THz and 4.5 THz, with the former corresponding to a hidden mode not observed in equilibrium spectroscopy. We show that these effects arise in part from a field-induced charge rearrangement mechanism that lowers the local crystal symmetry, and couples to the phonon modes. A long-lived field-driven response was uncovered with a complex THz polarization dependence which, in comparison to theory, indicates evidence for an antiferromagnetic-to-ferrimagnetic transition. Our results establish an effective field-tunable pathway for driving excitations otherwise weak in equilibrium, and for manipulating magnetism in low-dimensional materials via dynamical modulation of symmetry.

cond-mat.str-el↗

arXiv2025

Carrier Localization and Spontaneous Formation of Two-Dimensional Polarization Domain in Halide Perovskites

Halide perovskites are known for their rich phase diagram and superior performance in diverse optoelectronics applications. The latter property is often attributed to the long electron-hole recombination time, whose underlying physical mechanism has been a long-standing controversy. In this Letter, we investigate the transport and localization properties of electron and hole carriers in a prototypical halide perovskite (CsPbBr$_3$), through \textit{ab initio} tight-binding nonadiabatic dynamics approach for large-scale (tens of nm size) supercell calculations, to simulate electron and ion dynamics on the same footing. We found distinct structural, lattice polarization, and electron-phonon coupling properties at low (below 100 K) and high temperatures, consistent with experimental observations. In particular, at low temperature we find spontaneous formation of polar grain boundaries in the nonpolar bulk systems, which result in two-dimensional polarization patterns that serve to localize and separate electrons and holes. We reveal phonon-assisted variable-range hopping mostly responsible for low-temperature transport, and their characteristic frequency correlates with temperature-dependent phonon power spectrum and energy oscillation frequency in nonadiabatic dynamics. We answer the critical questions of long electron-hole recombination lifetime at low temperature and offer the correlation among polarization domains, electron-phonon couplings, and photocarrier dynamics.

cond-mat.mtrl-sci↗

arXiv2025

Interplay between ultrafast electronic and librational dynamics in liquid nitrobenzene probed with two-color four-wave mixing

We present an experimental and theoretical study of the interplay between ultrafast electron dynamics and librational dynamics in liquid nitrobenzene. A femtosecond ultraviolet pulse and two femtosecond near infrared pulses interact with nitrobenzene molecules, generating a four-wave mixing nonlinear signal that is measured in the Optical Kerr Effect geometry. The near infrared nonlinear signal is measured to be non-zero only at negative time delays, corresponding to the near infrared pulses arriving earlier than the ultraviolet pulse. We perform time-dependent Quantum Master Equation calculations, which include a classical libration model, to simulate the experiment. The simulations support the conclusion that the near infrared pulses launch librational motion, while simultaneously creating electronic coherences that result in a libration-modulated electronic nonlinear response. Furthermore, we conclude that the measured nonlinear optical signal corresponds to a non-parametric process that leaves the molecules in an excited electronic state. This work provides new insight into ultrafast nonlinear optical interactions in liquids and is an important step towards probing ultrafast electronic coherences in large molecules in the liquid phase.

physics.chem-ph↗

arXiv2025

Molecular Axis Distribution Moments in Ultrafast Transient Absorption Spectroscopy: A Path Towards Ultrafast Quantum State Tomography

In ultrafast experiments with gas phase molecules, the alignment of the molecular axis relative to the polarization of the interacting laser pulses plays a crucial role in determining the dynamics following this light-matter interaction. The molecular axis distribution is influenced by the interacting pulses and is intrinsically linked to the electronic coherences of the excited molecules. However, in typical theoretical calculations of such interactions, the signal is either calculated for a single molecule in the molecular frame or averaged over all possible molecular orientations to compare with the experiment. This averaging leads to the loss of information about anisotropy in the molecular-axis distribution, which could significantly affect the measured experimental signal. Here, we calculate the laboratory frame transient electronic first-order polarization ($P^{(1)}$) spectra in terms of separated molecular frame and laboratory frame quantities. The laboratory frame polarizations are compared with orientation-averaged Quantum Master Equation (QME) calculations, demonstrating that orientation-averaging captures only the isotropic contributions. We show that our formalism allows us to also evaluate the anisotropic contributions to the spectrum. Finally, we discuss the application of this approach to achieve ultrafast quantum state tomography using transient absorption spectroscopy and field observables in nonlinear spectroscopy.

physics.chem-ph↗

arXiv2024

Coactive-Staggered Feature in Weyl Materials for Enhancing the Anomalous Nernst Conductivity

Power generation through the anomalous Nernst effect in topological Weyl materials has several advantages over conventional thermoelectrics due to the transverse geometry. However, the magnitude of the anomalous Nernst conductivity (ANC) in most known materials is too small to be of practical use, and there exist few guiding principles for finding materials with optimal thermoelectric properties. This work shows that the ANC is maximal when there is a ``coactive-staggered" feature in the anomalous Hall conductivity (AHC). It is shown that a minimal arrangement of two Weyl pairs leads to such a feature, and tuning the separations between the pairs controls the temperature at which the ANC is maximal. Several methods are proposed for creating such arrangements of Weyl points starting from Dirac semimetal materials. It is also demonstrated how an existing coactive-staggered AHC in a Heusler material can be exploited, by collectively tuning the positions of the Weyl points through strain to further enhance the ANC. A modest 20% amplification of the ANC is achieved, even with relatively minor changes in Weyl point positions.

cond-mat.mtrl-sci↗

arXiv2024

Factors influencing quantum evaporation of helium from polar semiconductors from first principles

While there is much indirect evidence for the existence of dark matter (DM), to date it has evaded detection. Current efforts focus on DM masses over $\sim$GeV -- to push the sensitivity of DM searches to lower masses, new DM targets and detection schemes are needed. In this work, we focus on the latter - a novel detection scheme recently proposed to detect ~10-100 meV phonons in polar target materials. Previous work showed that well-motivated models of DM can interact with polar semiconductors to produce an athermal population of phonons. This new sensing scheme proposes that these phonons then facilitate quantum evaporation of $^3$He from a van der Waals film deposited on the target material. However, a fundamental understanding of the underlying process is still unclear, with several uncertainties related to the precise rate of evaporation and how it can be controlled. In this work, we use \textit{ab initio} density functional theory (DFT) calculations to compare the adsorption energies of helium atoms on a polar target material, sodium iodide (NaI), to understand the underlying evaporation physics. We explore the role of surface termination, monolayer coverage and elemental species on the rate of He evaporation from the target material. Using this, we discuss the optimal target features for He-evaporation experiments and their range of tunability through chemical and physical modifications such as applied field and surface termination.

hep-ph↗

arXiv2024

Electrically Switchable Circular Photogalvanic Effect in Methylammonium Lead Iodide Microcrystals

We investigate the circular photogalvanic effect (CPGE) in single-crystalline methylammonium lead iodide microcrystals under a static electric field. The external electric field can enhance the magnitude of the helicity dependent photocurrent (HDPC) by two orders of magnitude and flip its sign, which we attribute to magnetic shift currents induced by the Rashba-Edelstein effect. This HDPC induced by the static electric field may be viewed as an unusually strong third-order photoresponse, which produces a current two orders of magnitude larger than second-order injection current. Furthermore, the HDPC is highly nonlocal and can be created by photoexcitation out of the device channel, indicating a spin diffusion length up to 50 $μ$m at 78 K.

cond-mat.mes-hall↗

arXiv2023

Ultrafast Field-Resolved Nonlinear Optical Spectroscopy in the Molecular Frame

We resolve the real-time electric field of a femtosecond third-order nonlinear optical signal in the molecular frame. The electric field emitted by the induced third-order polarization from impulsively pre-aligned gas-phase molecules at room temperature, in a degenerate four-wave mixing (DFWM) scheme, is measured using a spectral interferometry technique. We show that by measuring both the amplitude and phase of the emitted femtosecond pulse, information related to electronic symmetries can be accessed. The nonlinear signal is measured around a rotational revival to extract its molecular-frame angle dependence from pump-probe time delay scans. By comparing these measurements for two linear molecules, carbon dioxide (CO2) and Nitrogen (N2), we show that the measured second-order phase parameter (temporal chirp) of the signal is sensitive to the valence electronic symmetry of the molecules, whereas the amplitude of the signal does not show such sensitivity. We compare these measurements to theoretical calculations of the chirp observable in the molecular frame. This work is an important step towards using field-resolved nonlinear optical measurements to study ultrafast dynamics in electronically excited molecules.

physics.optics↗

arXiv2023

Correlated Anharmonicity and Dynamic Disorder Control Carrier Transport in Halide Perovskites

Halide pervoskites are an important class of semiconducting materials which hold great promise for optoelectronic applications. In this work we investigate the relationship between vibrational anharmonicity and dynamic disorder in this class of solids. Via a multi-scale model parameterized from first-principles calculations, we demonstrate that the non-Gaussian lattice motion in halide perovskites is microscopically connected to the dynamic disorder of overlap fluctuations among electronic states. This connection allows us to rationalize the emergent differences in temperature-dependent mobilities of prototypical MAPbI$_3$ and MAPbBr$_3$ compounds across structural phase-transitions, in agreement with experimental findings. Our analysis suggests that the details of vibrational anharmonicity and dynamic disorder can complement known predictors of electronic conductivity and can provide structure-property guidelines for the tuning of carrier transport characteristics in anharmonic semiconductors.

cond-mat.mtrl-sci↗

arXiv2023

Intrinsic Origin and Enhancement of Topological Responses in Ferrimagnetic Antiperovskite Mn4N

Using first-principles calculations we investigate the intrinsic origins of the anomalous Hall effect (AHE) and the anomalous Nernst effect (ANE) in antiperovskite ferrimagnet Mn4N. We predict that the AHE is significantly enhanced under both compressive and tensile strain, however, the ANE generally decreases under epitaxial strain, except for 1% compressive strain. We connect this behavior to the evolution of the Berry curvature with strain, suggesting similar strategies for achieving large AHE and ANE changes with modest amounts of strain. Finally, we find that the non-monotonic characteristics of the AHE and ANE stem from the formation and movement of new Weyl points at the periphery of the Brillouin Zone under compressive and tensile strains.

cond-mat.mtrl-sci↗