What do you think of when you think of Regina Spektor? Maybe it's her Grammy-nominated theme song for Orange Is the New Black, or the dozens of dramatic TV scenes that have used her music as a soundtrack (Grey's Anatomy, Weeds, Veronica Mars). Or perhaps you remember that Chance The Rapper cut her, regretfully, from Coloring Book's “Same Drugs.”

A common thread through most of these memories is Spektor's signature whimsy, honed through lyrics about making computers out of macaroni or finding human teeth down on Delancey. As that Orange theme showed, she can even make a women's prison sound kind of sweet and charming. This quality has led to years of critics and fans labeling Spektor “quirky,” and it's true that her music can be a little precious. There's a childlike core to her work that isn't so much weird or inappropriate as it is deeply, unabashedly earnest. But what's remarkable about Spektor's musical universe — grounded by her classical piano and tinkering indie-pop instrumentals, unfurling like a children's storybook — is just how wholly distinctive it is.

Given this background, Spektor's latest album, Remember Us to Life, feels surprisingly somber. On her first full-length release since 2012, she seems to take the inklings of dreary existentialism that merely slipped into past albums and bring them to the fore. “This is how I feel right now / Obsolete manuscript, no one reads and no one needs,” Spektor sings softly on the gorgeous, restrained “Obsolete,” with her reverbed piano backed by New Agey synths more suitable for a Cocteau Twins track than a Spektor song. On the excellent “Tornadoland,” she sings, “Everybody's time has come / It's everybody's moment except yours,” her lyrics weighted with paranoia as she bangs out a scale while her piano and a string section follows in an ominous frenzy. With her piano arrangements backed by an extensive orchestra, Remember Us to Life plays like a grander chamber-pop display of Spektor's musical talents than the more minimalist, sweeter instrumentals of her last album, What We Saw from the Cheap Seats.

That's not to say all of Remember Us to Life is so straitlaced, but even the record's more imaginative fables feel particularly dark. On “Grand Hotel,” which details what sounds like a Wes Anderson–directed trip through a hotel's winding halls to a lake house, Spektor warns that “Under the floorboards, there’s a deep well / That leads to a spring that sprung up in Hell,” where old devils used to dance. Elsewhere, though, the Brothers Grimm vibe doesn't always land. “Small Bill$,” which sounds like a villain's musical number ripped from a Disney animated film, tells the story of a man who spent all his fortune on weed, chocolate, and Coca-Cola, which sounds like it’s intended to be seriously anti-consumerist but instead rings a bit silly. On the over-the-top “The Trapper and the Furrier,” a sibling to Spektor's “Ballad of a Politician,” she calls out lawyers and pharmacists who turn a blind eye to the needy. “What a strange, strange world we live in ... Those who don’t have lose, those who got get given / More, more, more, more,” she sings, wailing “more, more, more, more” loudly as cellos throb cartoonishly in the background.

But even at its most high-flying, Remember Us to Life is never quite cute, never really light. Spektor's voice doesn't try on weird accents or vocal tics. Even her twistiest lyrical riddles have a way of curdling a song's mood. “Enjoy your youth / Sounds like a threat,” she sings as a footnote to the the deceptively cheery and plucky “Older and Taller.” But whether she's doling out great, direct ballads like the synth-laden Begin to Hope throwback “Bleeding Heart” or the album's more oddball cuts, Spektor comes across as a much wiser songwriter, frequently outlining how time can reveal once-hidden truths and fears. While the wordy idiosyncrasies of her songwriting still shine through, this is Spektor at her most mature.